estudio quimica
DESCRIPTION
Estudio quimicaTRANSCRIPT
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âsijà ç µ·ø(ßá¿á³à³ÂmÁsÃlÄÁ¸Ã½µ·Áߪ¶Ãfµ¿àËm¸ÁËmµ³ÃÉâk¶Ã½Äðß³ÃÁ|È(µ³ÂmÁsó%à¬Á´\µ¿àµ·¶(ß\ÄÁsÃëvºª¶(¸³*Âm¶(á`Ëmá³ßªÁ$ä'ö7ºªÃ³ß¾i¶(ߪ¶(¸³á¿à¬¶(ß\ĶË`³¸³ à³ß\Ķ(ߪ¶(¸á³ Ëmá³ß`³¸½µ·Âª³ÂÂm¶ðÄÁà¬ÁsÃÈÁßèmµ ç ¸½µ·Âª³È(µ·Êß¯Ã½Ë D ±
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Estr = De
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1 − e−a(l−l0)]2 ` D ±VU R b
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a = w√
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w =√
(k/µ)±l0¶Ã*¶(á
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Estr =k
2(l − l0)
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Ebend =k
2(θ − θ0)
2 ` D ±VUH/bÂmÁߪÂm¶
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EvdW = εij
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r∗ijrij
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EvdW = εij
1,84 · 105e
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W (M/S) =
∫ 1
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dΩ [ρS(λ)Vint(q,Q,Ω)gs(Ω;λ)]` D ± G ]/b
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W (M/S) = ∆Gele + ∆Gcav + ∆Gdis + ∆Grep` D ± G Esb
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[
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K0 = RT
[
−ln (1 − y) +9
2
(
y
1 − y
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− 4πR3SP
3
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K1 = −3RT
RS
[
y
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(
y
1 − y
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+ 4πR2SP
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K2 =3RT
RS
[
y
1 − y+
3
2
(
y
1 − y
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− 4πRSP` D ± IH b
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Urep,ms = cmse−γmsrms
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∆Gdis−rep =∑
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∆Gele,i = ∆Gselfele,i + ∆Gcross
ele,i
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∆Gselfele,i =
1
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µsol =N∑
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∆Gsol,i(ri − r0) −∆Gsol
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ϑwz =µw
sol∣
∣µwsol
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1
MST Continuum Study of the Hydration Free Energies of Monovalent Ionic Species
Carles Curutchet,1 Axel Bidon-Chanal,1 Ignaci Soteras,1 Modesto Orozco,2*
and F. Javier Luque1*
1 Departament de Fisicoquímica. Facultat de Farmàcia. Universitat de Barcelona. Avgda. Diagonal 643. Barcelona 08028. Spain. 2 Departament de Bioquímica i Biología Molecular, Facultat de Química, Universitat de Barcelona, c/. Martí i Franqués 1, 08028, Barcelona, and Unitat de Modelització Molecular i Bioinformàtica, Institut de Recerca Biomèdica. Parc Científic de Barcelona, c/. Josep Samitier 1, 08028 Barcelona, Spain. Send correspondence to FJL (e-mail: [email protected]) or MO (e-mail: [email protected]) Abstract
In this study we revisit the protocol previously proposed within the framework of the
Miertus-Scrocco-Tomasi (MST) continuum model to define the cavity between solute
and solvent for predicting hydration free energies of univalent ions [Orozco, M.; Luque,
F. J. Chem. Phys. 1994, 182, 237]. The protocol relies on the use of a reduced cavity
(around 10-15% smaller than the cavity used for neutral compounds) around the atom(s)
bearing the formal charge. The suitability of this approach is examined here for a series
of 47 univalent ions for which accurate experimental hydration free energies are
available. Attention is also paid to the effect of the charge renormalization protocol used
to correct uncertainties arising from the electron density located outside the solute
cavity. The method presented here provides, with a minimum number of fitted
parameters, reasonable estimates of the hydration free energy of ions (average relative
error of 4.7%) and is able to reproduce solvation in water of both small and large ions.
Curutchet et al., October 2004, revised version
2
Introduction
The theoretical study of chemical systems in condensed phases has experienced
an extraordinary evolution in the last decades, leading to a number of computational
approaches that combine quantum mechanical (QM) or classical descriptions of the
solute with continuum or discrete representations of the solvent molecules.1 One of
these approaches is the self-consistent reaction field (SCRF) continuum model, where
the solute resides in a cavity carved into a continuum polarizable medium that simulates
the solvent.2 In spite of the rather crude description of the solvent, QM SCRF methods
have found a widespread acceptance due to several reasons. First, the availability of
well-defined formalisms developed to account for the mutual coupling between the
solute’s charge distribution and the solvent’s reaction field (see ref. 3 for a recent
review). Second, the ease of gaining insight into the solvent-induced changes in the
properties of the solute upon transfer from the gas phase to solution.2,4 Third, its low
computational cost, which is only slightly larger than the corresponding QM calculation
in the gas phase.
Though the preceding features have made QM SCRF methods very popular for
the study of molecules in solution, their chemical accuracy has mainly been restricted
by the uncertainty in the location of the boundary between solute and solvent.2 In the
last decade a large research effort has been spent to parametrize the solute cavity in
different SCRF methods, such as the multipolar expansion method developed at Nancy,5
the generalized Born SMx solvation models from Cramer and Truhlar,6 the Polarizable
Continuum model from Tomasi and coworkers7 and the related Miertus-Scrocco-
Tomasi (MST) version developed at Barcelona,8 or the conductor-like screening model
from Klamt and coworkers.9 As a result, the most refined QM SCRF methods predict
Curutchet et al., October 2004, revised version
3
the free energy of solvation of neutral molecules in a variety of solvents with an average
error clearly below 1 kcal/mol when solute cavities adjusted to the specific electrostatic
model are used.10
For ionic solutes, the uncertainty in the hydration free energies determined from
QM SCRF methods is larger (around 4-5 kcal/mol). The lower predictive accuracy for
ions arises not only for the intrinsic problems in representing the strong solute-solvent
interactions existing between water and ions, but also to the poor quality of most
experimental data. For neutral solutes the solvation free energy can be directly obtained
by measuring partition coefficients of solutes between gas phase and dilute aqueous
solutions in equilibrium. In this way the uncertainty of the measured partition
coefficient increases with increasing solvation free energy, and eventually the
concentration of solute molecules in the gas phase falls below the experimental
detection limits when the solvation free energy (in absolute terms) exceeds ~12
kcal/mol.11 This makes it necessary to determine the solvation free energy of ionic
species by indirect approaches based on the use of suitable thermodynamic cycles. For
example, Pearson12 determined the experimental solvation free energies for a number of
univalent ions using the relationships given by Eqs.1 and 2 for cations and anions,
respectively.
)AH(RTpK.)A(G)H(G)A(B)AH(G asolsolgsol+++ −++= 3032∆∆∆ (1)
)BH(RTpK.)BH(G)H(G)B(B)B(G asolsolgsol 3032++−−= +−− ∆∆∆ (2)
where Bg is the gas phase basicity and solG∆ denotes the free energy of solvation.
Note that according to Eqs. 1 and 2 the quality of the “experimental” solvation
free energies of cations, )AH(Gsol+∆ , and anions, )B(Gsol
−∆ , depend on the accuracy
Curutchet et al., October 2004, revised version
4
of different thermodynamic quantities, such as the gas phase basicity, the solvation free
energy of the conjugate neutral base, )A(G sol∆ , or acid, )BH(G sol∆ , the pKa constant,
and the solvation free energy of the proton, )H(G sol+∆ . It is also worth noting that
correction terms (not explicitly indicated in Eqs. 1 and 2) arising from the standard state
definition of the chemical species in the gas phase and in solution might be necessary.
Thus, solvation free energies can be defined for the hypothetical process of transferring
a species from a fixed position in the gas phase to a fixed position in the solution phase,
which is equivalent to using the same standard states (typically 1 M concentration) for
gas and solution phases.13 However, experimental data in the gas phase is generally
referred to an ideal gas at 1 atm. of pressure, so that a correction term of RTln(RT) must
be considered.
In his original work Pearson used an estimated )H(G sol+∆ value of -259.5
kcal/mol, which was also adopted by Florian and Warshel in the parametrization of their
Langevin dipole solvation model.14 However, the values of )H(Gsol+∆ used by other
authors vary considerably (from -252 to -263 kcal/mol)15. This range of error is similar
to that determined from theoretical calculations16 and introduces a noticeable range of
uncertainty in the “experimental” hydration free energy of ions. More recently,
Tissandier et al.,17 using a cluster-pair approximation and thermodynamic properties of
ion-water clusters, derived a value of )H(G sol+∆ =-264 kcal/mol. A very similar value
has recently been derived by Tuttle et al and by Coe and coworkers.18 Because this new
)H(G sol+∆ value is considerably more negative than the previous ones, it has a
significant effect on the absolute solvation free energies of ions and the corresponding
acidity/basicity constants.
Curutchet et al., October 2004, revised version
5
Pliego and Riveros have recently derived new experimental values for the
hydration free energies of 47 univalent ions using as reference the solvation free energy
of the proton derived by Tissandier et al.19 In light of the new reported values, the aim
of this work is to revisit the original parametrization of the MST model20 to predict the
corrected experimental hydration free energies for ions. In turn, this makes it necessary
to solve additional fundamental problems for a continuum description of solvation.
First, how should solute cavities be defined for ionic compounds, which are generally
characterized by a large anisotropy in the charge distribution? Second, how can errors in
the solvation free energy arising from the solute charge density lying outside the cavity
be corrected?
In our previous MST parametrization for ions,20 the van der Waals radii used to
built up the solute/solvent interface were scaled by a factor of 1.10-1.15, which is
around 10% smaller than that recommended for the hydration of neutral solutes.8
Moreover, the inaccuracies in the apparent surface charges due to the solute electron
density lying outside the cavity was treated by means of a simple uniform correction
procedure. However, owing to the small size of the ions examined in that study, the
strategy of reducing the whole cavity might not be appropriate for ionic compounds
having larger, more complex chemical structures, specially when there is high
anisotropy in the charge distribution along the molecule. Then, we explore here the
suitability of our original strategy, but limiting the reduction of the cavity to the atom(s)
that bear the formal charge in the ion. Furthermore, to reduce artefacts arising from the
solute charge density penetration, different charge renormalization procedures are tested
to determine their consistency in predicting the hydration free energies, particularly for
anions having diffuse charge distributions
Curutchet et al., October 2004, revised version
6
Methods
The MST continuum method. In the MST model the free energy of solvation is
determined as the sum of three contributions: electrostatic, cavitation, and van der
Waals. Following the formalism of the Polarizable Continuum model (PCM) originally
developed by Miertus, Scrocco and Tomasi,7 the electrostatic term (∆Gele) is determined
by using a set of apparent charges spread over the cavity surface (Eq. 3), which account
for the reaction field created in the solvent by the presence of the solute’s charge
distribution. The apparent charges are obtained by solving the Laplace equation with
suitable boundary conditions (Eq. 4).
∑=
=M
1j j
jR
r - r
q V (3)
where VR is the perturbation operator used to couple the solute’s charge distribution and
the solvent reaction field, M is the total number of surface elements, j, into which the
solute/solvent boundary is divided, and qj is the apparent charge at the j surface element,
which is centered at rj.
jT
jj )n
V( S
ε π 4
1-ε - q
∂∂
= (4)
where VT is the total electrostatic potential, which includes both solute and solvent
contributions, n is the unit vector normal to the surface element j, Sj is the area of the
surface element j, and ε is the solvent dielectric constant.
Curutchet et al., October 2004, revised version
7
The cavitation free energy is determined following Pierotti’s scaled particle
theory21 adapted to molecular shaped cavities by using the procedure proposed by
Claverie (Eq. 5).22 Thus, the cavitation free energy of atom i, ∆GC-P,i, is determined
weighting the contribution of the isolated atom, ∆GP,i, by the ratio between the solvent-
exposed surface of such an atom, Si, and the total surface of the molecule, ST (Eq. 5).
Finally, the van der Waals term (∆GvW) is computed using a linear relationship to the
solvent-exposed surface of each atom (Eq. 6).
iP
N
i T
icav G
S
S∆G ,
1
∆∑=
= (5)
where N is the number of atoms
i
N
iivdw S∆G ∑
==
1
ξ (6)
where ξi is the atomic surface tension, which is determined by fitting to the
experimental free energy of solvation.
Molecular-shaped GEPOL cavities23 are used to define the solute/solvent
interface for the calculation of electrostatic and non-electrostatic (cavitation, van der
Waals) terms. In the last parametrization of the MST model, a dual-cavity strategy was
used,24 so that nonelectrostatic contributions are determined by using a van der Waals
surface mainly built up from Pauling’s radii (in Å; polar hydrogen: 0.9, apolar
hydrogen: 1.2, C and N: 1.5, O: 1.4, F: 1.35, S: 1.75, and Cl: 1.80), whereas the
electrostatic term is determined by using a solvent-exposed surface created by scaling
the atomic radii by a solvent-dependent factor, λ, which adopts values of 1.25, 1.50,
1.60 and 1.80 for the solvation of neutral compounds in water, octanol, chloroform and
Curutchet et al., October 2004, revised version
8
carbon tetrachloride. Based on the comparison of the ∆Gele values determined from
MST and from Monte Carlo-Free Energy Perturbation (MC-FEP) calculations for seven
small ionic compounds,20 it was found necessary to further reduce the solute cavity by
around 10% to compute the hydration free energy of univalent ions. This reduction was
justified by the fact that due to strong electrostatic interactions solvent molecules are in
general closest to the atoms of charged molecules than in those of the neutral ones.
Charge normalization. Owing to the solute charge density that lies outside the cavity,
and to the numerical errors due to tessellation of the cavity surface (Eq. 4), the sum of
the apparent surface charges, ∑=j
jqQσ , in the MST (PCM) model do not satisfy the
relationship given by Eq. 7,7a,25 where QM denotes the total charge of the solute, and the
error in the charges is given by σσ∆ QQtheor −= , where Mtheor QQε
ε 1−−= .
MQQ
εε
σ1−−= (7)
The MST model8 takes into account the charge normalization by using the
expressions given in the original formalism7a (denoted in the following as the standard
correction (SC) approach), as noted in Eqs. 8a-b, where +σQ and −
σQ denote the sum of
positive and negative apparent charges, respectively.
[ ])2/(1' ++= σσ∆ Qqq jj for 0>jq (8a)
[ ])2/(1' −+= σσ∆ Qqq jj for 0<jq (8b)
Curutchet et al., October 2004, revised version
9
More elaborate treatments of the charge compensation have been developed by
the Pisa group.26 The most accurate procedure (denoted density-corrected (DC)
approach hereafter) relies on two main features. First, the introduction of separate
factors to correct the apparent charges induced by nuclei ( Zf ) and electrons ( ef ),
which makes possible to correct the numerical errors on the nuclear charges, which are
only affected by the discretization of the cavity (Eq. 9). Second, the explicit calculation
of the charge density outside the cavity (Qout), which is determined from the flux of the
solute electric field through the cavity surface (Eq. 10). Using this new approach the
solvent response induced by the electron charge density inside the cavity (Qin) is then
only affected by the numerical errors due to tessellation of the cavity (Eq. 11).
ZM
j
Zj
Z Qqfε
ε 1−−=∑ (9)
))(4
1()( dsnsEQQQQ sS M
eMin
eMout ⋅⋅+−=−−= ∫π
(10)
where )(sEM is the electric field created at each tessera of the cavity.
eMin
j
ej
e Qqf ,1
εε −−=∑ (11)
For the sake of completeness, let us note that an alternative procedure used by
other groups to alleviate the effects due to the charge density that lies outside the cavity,
where the continuous charge distribution obtained from quantum mechanical or density
functional calculations is replaced by a set of atomic point charges, often supplemented
by point dipoles, which are then used to evaluate the solvent reaction field by means of
finite-difference Poisson-Boltzmann or boundary element techniques.27 This approach,
Curutchet et al., October 2004, revised version
10
nevertheless, demands that the set of point charges accurately reproduces the charge
distribution of the solute, which then raises the question about the best procedure to
derive the atomic charges.28
Computational details. The set of compounds compiled by Pliego and Riveros19 has
been used to examine the suitability of our previous parametrization of the MST model
to predict the hydration free energy of univalent ions. In order to be consistent with our
previous work,20 all calculations have been performed at the HF/6-31+G(d) level.
Following the standard MST protocol,8,20 the gas phase geometry of the charged
molecules was fully optimized and subsequently used for calculations in solution. The
MST hydration free energies were determined by using a locally modified version of
Monstergauss.29 For the sake of comparison, computations were also performed by
using the Integral Equation Formalism30 of the Polarizable Continuum Model (IEF-
PCM), which has been claimed to be less sensitive to the inaccuracies arising in the
calculation of the electrostatic term. IEF-PCM calculations were performed by using the
code implemented in Gaussian03.31
Results and discussion
About the cavity definition for ionic species. Though the choice of the solute/solvent
boundary is a crucial parameter in the development of any QM SCRF method, the
definition of the solute cavity is even more delicate for ionic compounds, whose
electrostatic field strongly perturbs the solvent, thus making the solvent molecules in the
first hydration shells to exhibit properties clearly different from those of the bulk
solvent. In turn, hydration also changes the electron density distribution of ions,32
leading to differential trends in the electron rearrangement that takes place for cations
Curutchet et al., October 2004, revised version
11
and anions. Therefore, it can be questioned whether the hydration of ions can be
described in an effective way by means of a suitable refinement of the solute cavity in
continuum models, and whether or not such a refinement is well suited to reproduce the
solvent-induced change in different molecular properties of the solute.33
An attempt often considered to describe the solvation of ions consists of the
addition of an arbitrary number of solvent molecules to the solute, while the rest of the
solvent is treated as a continuum dielectric.34 This approach, however, raises some
problems, such as the increase in the computational task, the need to obtain appropriate
averages of the thermally accessible configurations or the treatment of the librational
motions originated from the weak interactions between solute and solvent molecules.
Moreover, by adding few solvent molecules, the conceptual problem of the solvation of
the solute alone is transformed into the solvation of the solute-solvent cluster. Finally,
the analysis of solute-solvent clusters for medium and large size molecules becomes
even more problematic and computationally more expensive. Because of these
considerations, we prefer here to limit the QM discrete description exclusively to the
solute. This choice, nevertheless, raises the delicate question about the suitability of
transferring the cavity definition optimized for the solvation of neutral solutes to ionic
compounds.
In the original MST parametrization,20 the optimum cavity for the hydration of
ions was defined by scaling the atomic radii by a factor of 1.10-1.15, which implies a
reduction with regard to the scaling factor of 1.25, i. e. the value optimized for the
hydration of neutral solutes.8 A similar correction was also adopted in the UAHF
parametrization of the PCM model,7c where the atomic radii are reduced depending on
the formal charge carried by atoms, though different correction factors are used for
cations and anions. Others authors have also proposed to exploit alternative
Curutchet et al., October 2004, revised version
12
relationships between the atomic charge and the effective atomic radius,35 or to use
modified set of atomic radii.36 An alternative approach for cavity size comes from the
use of isodensity contours of the electron density, which can be adjusted during the
SCRF calculation as the charge distribution of the solute is polarized by the solvent
reaction field.37 Here the electron density contour that leads to better agreement with the
experimental solvation free energy for ions is larger than that required for neutral
compounds.38
For our purposes here, we have decided to retain the original idea of reducing
the scaling factor (λ) that multiplies the atomic radii in order to build up the solute
cavity used to calculate the ∆Gele component. However, instead of reducing the whole
cavity of the solute, which might be appropriate for small size ions, the scaling down is
here limited to the heavy atom (and the hydrogen atoms attached to it) that bears the
formal charge. Thus, for alcohol cations and anions the reduction in the cavity only
affected the -OH2+ and -O- groups. In the case of ionized carboxylic acids, such a
reduction only affected the oxygen atoms in the –COO- group. Besides retaining the
simplicity of the original approach, this strategy allows us to exploit the same set of
scaling factors that modulate the cavity definition for the calculation of the electrostatic
component of the solvation free energy (see Methods), while introducing a minimum
number of parameters to describe the hydration of ionic species.
Refinement of the MST model for ions. The adjustment of the scaling factor λ used to
determine ∆Gele was performed with the aim to minimize the deviation of the calculated
hydration free energy, ∆Ghyd, from the experimental value for the series of monovalent
ions. Following our previous study,20 MST-HF/6-31+G(d) calculations were performed
by reducing progressively the scaling factor from λ=1.25 to λ=1.00. The ∆Gele values
Curutchet et al., October 2004, revised version
13
were calculated by using both SC (Eqs. 8a,b) and DC (Eqs. 10 and 11) charge
renormalization schemes. The cavity used to compute the ∆Gele term was built up by
using the set of atomic radii typically used in MST calculations (see Methods). Finally,
the non-electrostatic (cavitation and van der Waals) component, which was estimated by
using the standard atomic surface tensions determined for neutral molecules, was added
to the ∆Gele term to calculate ∆Ghyd. This computational strategy benefits from the fact
that the ∆Gele term is the dominant contribution to the hydration of ionic solutes, and
from the partial cancellation between cavitation and van der Waals components.
Figure 1 shows the profiles of the root mean square deviation (rmsd) and relative
error (in percentage) between experimental and calculated ∆Ghyd values determined for
different scaling factors. The smallest deviation is found for a scaling factor λ ranging
between 1.10 and 1.15, which implies a reduction in the size of the cavity around 90%
relative to that used for neutral molecules. It is also worth noting that such a range of
values is in agreement with the results found previously by comparing the ∆Gele values
determined from MST and MC-FEP calculations for a subset of small ions.20 The
results in Figure 1 also point out that both the rmsd and the relative error are further
reduced by near 1 kcal/mol when the DC charge renormalization scheme is considered.
This finding can be attributed to the larger efficiency of this method to account for the
anisotropies in the charge distribution of the ions.
Table 1 reports the electrostatic component of the hydration free energy
determined from MST calculations by using a scaling factor of 1.15 and the two charge
compensation schemes. For the sake of comparison, it also reports the values
determined by using the IEF-PCM formalism and the same cavity definition for the
univalent ions. Comparison of the MST and IEF results is shown in Figure 2. The
regression equations indicate that there is close agreement between MST and IEF
Curutchet et al., October 2004, revised version
14
results. Thus, the MST-SC ∆Gele values (Eq. 12) are around 3% larger than the IEF
ones, and such a difference is reduced to only 2% when the MST-DC results are
considered (Eq. 13). The most notable difference between the two charge normalization
schemes, nevertheless, is reflected in the correlation coefficient of the regression
equations, which is significantly larger when the MST-DC results are considered. This
finding points out not only the superiority of the DC charge normalization scheme, but
also the lower sensitivity of the IEF formalism to the errors arising from the penetration
of the charge density outside the solute cavity. Moreover, these results suggest that the
MST-DC optimized cavities can be considered to be transferable to the IEF-PCM
framework.
SC)(MSTG).(.(IEF)∆G eleele −±= ∆00909700 90.0=r 2191.F = (12)
)()005.0(979.0)( DCMSTGIEFG eleele −±= ∆∆ 97.0=r 8748.F = (13)
where r is the Pearson’s correlation coefficient and F stands for the Snedeckor’s
distribution parameter.
Considering the MST-DC results shown in Table 1, the rmsd between calculated
and experimental hydration free energies amounts to 5.8 kcal/mol (relative error of
5.9%). For the subset of 25 anions the rmsd is 4.7 kcal/mol, but it amounts to 6.9
kcal/mol for the 22 cations. Based on this finding, one might be tempted to use different
scaling factors to build up the solute cavity for anions and cations. However, the larger
rmsd found for cations mainly arises from deviations in protonated R-O-R’ (methanol,
ethanol, dimethyl ether, diethylether) and R-CO-R’ (acetone, methyl phenyl ketone,
methyl ethyl ester) groups, which have relative errors ≥ 10%. When these compounds
are excluded, the rmsd for the subset of cations (3.6 kcal/mol) is similar to that found
Curutchet et al., October 2004, revised version
15
for anions. It is not clear whether the notable deviation found for these compounds
might stem from short-range interactions with hydrating water molecules not properly
accounted for in the continuum model. Keeping in mind the limited availability of
accurate ∆Ghyd values for ionic compounds and the assumptions intrinsic to the
continuum method, it seems to us not justified, at least on the basis of present results, to
use different scaling factors for anions and cations, a procedure already used in the
context of solvation calculations of ion hydration carried out by using the Born
equation.39 Likewise, attempts to reduce these errors by distinct reshaping of solute
cavities seems not justified and might even yield to non-physical over-trained models.
An alternative strategy to reduce the difference between computed and
experimental data involves the adjustment of the atomic surface tensions, ξi (see Eq. 6),
which in the MST model are typically determined by fitting the experimental free
energies of solvation. Since steric terms are used in continuum models to account
implicitly for effects other than pure bulk electrostatic effects, the fitted parameters for
neutral and charged molecules might not be equal. Accordingly, one can expect that
restricting the refinement of the surface tensions only to the atom(s) bearing the formal
charge would suffice to improve the agreement between calculated and experimental
∆Ghyd values. From a practical point of view, caution is required owing to the limited
availability of data for certain atom types, which can lead to overtraining of the method.
Thus, the only statistically significant improvement was obtained when the surface
tension of the OH+ group was adjusted to -0.51 kcal mol-1 Å-2, which is near 4-fold
more negative than the corresponding value for neutral molecules (-0.14 kcal mol-1 Å-
2).8d With the only correction of this surface tension, the rmsd between calculated and
experimental ∆Ghyd values is 4.6 kcal/mol.
Curutchet et al., October 2004, revised version
16
The calculated ∆Ghyd and its electrostatic and non-electrostatic components
determined for the univalent anions are given in Table 2. With the exception of the
protonated R-O-R’ and R-CO-R’ groups (see above), the non-electrostatic term is
generally positive and only amounts, on average, to 3.9% of the hydration free energy.
Overall, there is satisfactory agreement between experimental and calculated ∆Ghyd
values, as noted in a relative error of 4.7%, and in the comparison of the regression
equation given in Eq. 14 (see Figure 3), specially keeping in mind the variety of
functional groups and sizes of the ionic compounds.
)DCMST(G).(.(exp)G hydhyd −∆±=∆ 00800191 940.r = 0351.F = (14)
Prediction of pKa values. Since the acidity/basicity of molecules is crucial to
understand chemical reactivity and intermolecular interactions, an intense research
effort has been devoted to check the reliability of theoretical methods, particularly QM
SCRF continuum methods, to predict accurately the pKa. Thus, Chen et al. were able to
predict the pKa values for several molecules by using a model where the reaction
potential was solved via finite-difference solutions to the Poisson-Boltzmann
equation.25c For a small series of imidazole derivatives, Topol et al. predicted pKa
values with an average absolute deviation of 0.8 units from experimental data by
combining results obtained from G2 or density functional calculations with SCRF
estimates of the hydration free energies.25d Schüürmann et al. estimated the acidities of
carboxylic acids by using the PCM-UAHF model at the SCF and MP2 levels, obtaining
good correlations for relative pKa values but not for the absolute ones, arguing that the
major sources of error stem from gas-phase calculations.40 Recently Shields and co-
workers predicted accurate absolute pKa’s for carboxylic acids41 and phenols42 using the
Curutchet et al., October 2004, revised version
17
C-PCM model along with state-of-the-art gas phase ab initio calculations. Chen and
MacKerell compared pKa differences in substituted pyridines by using semiempirical
and ab initio gas-phase free energies along with IPCM, SCIPCM and SM2 solvation
calculations, and relevant differences between the pKa values obtained at different
levels of theory were found.43 By using the SSC(V)PE model, Chipman checked
different isodensity thresholds to build up cavities in order to predict the pKa’s for
alcohols, acids and amines.38b This study showed that no single isodensity contour can
be applied to neutral compounds, anions and cations, and that good correlations can be
obtained only for compounds sharing the same acidic functional group. Other studies
also have pointed out the difficulty to predict absolute pKa values, which demand highly
accurate estimates of both the gas phase free energy difference between acid and base
partners and of the corresponding solvation free energies.44
To assess the performance of the MST parametrization for ionic compounds, we
have determined the pKa values for a series of carboxylic acids and substituted pyridines
by using the thermodynamic cycle shown in Figure 4 and Eq. 15. These compounds
were chosen because of the availability of experimental data for the gas phase
basicities.45,46 For consistency with the MST parametrization, the experimental
)H(G sol+∆ value determined by Tissandier17 was used. The hydration free energies of
the neutral species were calculated by using the HF/6-31G(d) version of the MST
model.8d Finally, to further compare the effect of the charge normalization scheme both
MST-SC and MST-DC calculations were performed for ionic compounds.
RTGKpK aqaa 303.2/log ∆=−= (15)
Curutchet et al., October 2004, revised version
18
Table 3 shows the results obtained for the two series of compounds, which
encompasses a range of pKa values larger than 5 units. Comparison of the results
obtained by using the two charge renormalization schemes supports the better
performance of the DC procedure. Thus, whereas both MST-SC and MST-DC methods
gives rise to similar relative pKa variations within the series of compounds (the rmsd
between calculated and experimental pKa differences varies between 0.4 and 1.2 pKa
units), the absolute pKa values determined from MST-DC computations agree better (in
absolute terms) with the experimental values, as noted in a rmsd (in pKa units) of 1.0
(MST-DC) and 2.4 (MST-SC) for carboxylic acids and of 1.9 (MST-DC) and 3.2
(MST-SC) for substituted pyridines.
Taking together the two series of compounds, the rmsd of the pKa values
predicted from MST-DC calculations amount to 1.6 pKa units. This uncertainty can be
mainly ascribed to the error in the hydration free energy of the ionic species, since the
difference between calculated and experimental hydration free energy for neutral
compounds (experimental ∆Ghyd available for acetic acid: -6.8 kcal/mol, pyridine: -4.7
kcal/mol, and 4-methylpyridine: -4.9 kcal/mol) is less than 0.5 kcal/mol. Chen and
McKerell reported rmsd values ranging from 1.22 to 4.14 pKa units depending on the
method used to compute the solvation free energy (see above). For carboxylic acids
alone, standard deviations of 0.4 pKa units have been reported by using Complete Basis
Set models in conjunction with C-PCM calculations.41 However, accurate estimates of
pKa values (i. e., with an error of half pKa unit) are typically obtained by means of an
empirical fitting of the experimental pKa values.44b-d In the absence of those empirical
adjustaments, the pKa values determined from MST-DC calculations compare
satisfactorily with the experimental ones, thus giving support to the computational
strategy used here to refine the MST method for the hydration of ionic compounds.
Curutchet et al., October 2004, revised version
19
Zwitterion-neutral equilibria. Because of the high anisotropy in the charge
distribution of zwitterions, the equilibrium between neutral and charge-separated forms
is particularly well suited to examine the effect of the charge renormalization scheme
within the framework of the MST model. To this end, we have examined the
equilibrium between neutral and zwitterionic forms of nicotinic and isonicotinic acids
(see Figure 5), a system that was previously studied by Nagy et al.47 In their study the
free energy of tautomerization in water was determined by adding the relative free
energies of hydration to the gas phase free energy difference between neutral and
zwitterionic species. This latter quantity was estimated from calculations carried out at
the MP2/6-311++G(d,p) level and subsequently corrected from zero-point energy,
thermal and entropy corrections determined at the MP2/6-31G(d). At this level, the
neutral forms are predicted to be favoured by 33-35 kcal/mol in the gas phase. To
determine the relative stability of tautomers in water, we adopted the relative gas phase
stabilities determined by Nagy et al., the hydration free energies of the neutral species
were determined from MST/HF6-31G(d) calculations,8d and those of the zwitterionic
compounds were obtained from both MST-SC and MST-DC calculations.
Table 4 reports the hydration free energies of the neutral and zwitterionic species
as well as the predicted tautomerization free energy (∆Gt) in water. As was found for
the calculated pKa values, the results obtained from MST-DC computations agree better
with the experimental data than those determined from MST-SC calculations. Thus,
whereas both neutral and zwitterionic forms of nicotinic acid are predicted to have
similar stability in water from MST-SC calculations, the neutral form is predicted to be
destabilized by around 2.8 kcal/mol according to MST-DC results, which agrees with
the observed preference of the zwitterion in aqueous solution by around 2.0 kcal/mol.
Curutchet et al., October 2004, revised version
20
With regard to the isonicotinic acid, the MST-SC method predicts again the neutral
form to be preferred in water, whereas the opposite trend is found from MST-DC
calculations, which predict the zwitterion to be more stable by 1.7 kcal/mol, in
agreement also with the experimental data.
Solvent reaction field in SC and DC schemes. The whole of the preceding results
support the better performance of the DC charge renormalization scheme for predicting
the hydration free energy of ionic compounds. This finding agrees with the results
obtained from the analysis of the fractional contributions of specific groups to the
hydration free energy within series of congeneric alkane derivatives,48 since the DC
scheme was found to yield consistently more transferable group contributions than the
SC scheme.
To gain further insight into the origin of the differences noticed between both SC
and DC charge renormalization schemes, we have compared a series of electrostatic
properties determined by using the wavefunction of the fully hydrated solute for a small
subset of charged monosubstituted alkane derivatives (CH3X and CH3(CH2)6X, with X
being NH3+, OH2
+, NH- and O-). This series of compounds is well suited to our purposes
because i) the enlargement of the side chain is expected to play a relatively small
perturbing effect on the hydration of the X unit, and ii) this allows us to concentrate
onto the differences in the solvent reaction field around the X group. To this end, we
have computed the rmsd between the electrostatic potential at selected points in four
layers around the molecule. For our purposes here, such a comparison was performed
by including exclusively those points generated by scaling the atomic radii of atoms in
the group X. Moreover, we have determined the well depth (Emin) of the molecular
interaction potential49 in the vicinity of the group X for the solutes interacting with
Curutchet et al., October 2004, revised version
21
classical probe particles O- (cations) and H+ (anions). Finally, the results are examined
in light of the solvent’s net apparent charge (Qσ) induced on the surface elements spread
on the portion of the cavity created from the group X. The results are shown in Table 5.
Not unexpectedly, there is close similarity in the results obtained from the two
charge renormalization schemes for CH3NH3+ and CH3OH2
+. However, there are
notable differences when the largest members of the congeneric series, CH3(CH2)6NH3+
and CH3(CH2)6OH2+, are considered. Thus, the electrostatic potential around the group
X is more positive when the DC scheme is used, which reflects the more negative
apparent charge induced on the cavity surface around the NH3+ and OH2
+ groups. In
fact, by enlarging the size of the side chain there is a reduction of 25-32% in Qσ(X)
when the SC scheme is used, which is notably larger than the 8-10% variation found for
the DC results.
For anions the differences between the two charge renormalization schemes are
clear even for the parent anions, CH3NH- and CH3O-, and tend to decrease as the size of
the ionic compound is enlarged. This is particularly true for the former anion, CH3NH-,
where the solvent apparent charge determined in the SC scheme (Qσ(NH-)=+0.91) is
sensibly larger than that obtained in the DC formalism (Qσ(NH-)=+0.78). A detailed
inspection of the results reveals that such a difference stems from the solvent reaction
field created in the portion of the cavity associated to the hydrogen atom. Thus, when
the DC scheme is used, the solvent reaction field is mainly concentrated in the surface
elements pertaining to the nitrogen atom, giving rise to an apparent charge of +0.80,
whereas the apparent charge on the portion of the cavity created by the hydrogen atom
is only -0.02. In contrast, when the SC scheme is considered, both nitrogen and
hydrogen atoms contribute markedly to the solvent reaction field, as noted in apparent
charges of +0.69 and +0.22, respectively. This different distribution of the reaction
Curutchet et al., October 2004, revised version
22
field in the surroundings of the NH group gives rise to differences in the electrostatic
properties of the solute (see Table 5), leading in turn to different solute-solvent
interaction energy.
In summary, the preceding results clearly point out that the explicit treatment of
anisotropy in the charge distribution leads to subtle, but nonnegligible differences in the
solvent reaction field, which in turn might modulate the calculation of the solvent-
induced change in solute’s properties, as noted in the case of the group contributions to
the solvation free energy.48
Concluding remarks
A satisfactory agreement between predicted and experimental hydration free
energies of univalent ions can be obtained by means of simple, conservative adjustment
in the definition of the cavity used to obtain the electrostatic contribution within the
framework of the MST model. Such a refinement implies a reduction in the cavity of
8% relative to the standard scaling used for neutral species, and is limited to the atom(s)
that bear the formal charge. This allows us to retain the original simplicity of the
approach and to exploit the same set of scaling factors that modulate the cavity
definition for the calculation of the electrostatic term in the MST model.
The results point out the need to account explicitly for the anisotropies in the
charge distribution of ionic species in order to correct the effects due to the solute’s
charge density that lies outside the cavity. The explicit consideration of the anisotropy
in the charge distribution of the ionic compounds leads to a subtle, but nonnegligible
improvement in the calculated electrostatic component of the hydration free energy.
Moreover, it also modulates the magnitude of the solvent reaction field, which in turn
influences the solvent-induced change in the solute’s properties. On the other hand, the
Curutchet et al., October 2004, revised version
23
IEF values are very close to and exhibit high correlation with the MST-DC results,
which are on average around 2% larger (in absolute value) than the hydration free
energies determined by using the IEF formalism. Therefore, these findings point out that
the optimized cavities should be largely transferible between the two computational
schemes.
The optimized MST-DC method leads to an average relative error of 4.7% in the
hydration free energy for the series of univalent ions containing a variety of functional
groups and molecular sizes. The basic strategy proposed here is still open to further
refinement, at least for the prediction of the hydration free energy, through the
adjustment of the atomic surface tensions used for the charged atoms. However, this
refinement would require the existence of a larger database of experimental values to
avoid overtrained models than can fail when applied to compounds very different to
those used in the parametrization of the model. In any case the robustness of the strategy
is supported by the results obtained for the absolute and relative pKas of carboxylic
acids and substituted pyridines, as well as for the tautomeric equilibrium between
neutral and zwitterionic forms of nicotinic and isonicotinic acids. These examples
suffice to point out that the MST model can be used confidently to measure the
magnitude of the solvent influence of chemically relevant properties and to use this
continuum method as an interpretative tool able to gain insight into the influence of
solvation on chemical processes of ionic species.
Acknowledgments
We are grateful to Prof. J. Tomasi for providing us with his original code of the
PCM model, which was modified by us to carry out the MST calculations. This work
has been supported by the Ministerio de Ciencia y Tecnología (BIO2003-06848 and
Curutchet et al., October 2004, revised version
24
SAF2002-04282), and the Centre de Supercomputació de Catalunya. C.C. is fellowship
from the Ministerio de Ciencia y Tecnología.
Curutchet et al., October 2004, revised version
25
Table 1. Electrostatic component of the free energy of hydration (kcal/mol)
determined at the HF/6-31+G(d) level from MST calculations using both SC and DC
charge normalization procedures and from IEF calculations.
Ion MST-SC MST-DC IEF
F- -101.7 -101.7 -98.4 Cl- -75.4 -75.4 -72.5 OCl- -74.6 -76.1 -73.5 OH- -106.4 -104.1 -98.7 HO2
- -92.6 -92.5 -89.4 NH2
- -102.5 -96.8 -90.3 CN- -74.8 -75.0 -71.6 HCC- -81.7 -81.9 -75.8 CH3O
- -90.3 -88.8 -84.7 CH3CH2O
- -89.8 -86.1 -81.4 C6H5O
- -77.0 -70.9 -66.1 HCOCH2
- -76.5 -73.5 -69.4 CH3COCH2
- -77.3 -73.0 -68.9 HCOO- -80.3 -79.8 -76.6 CH3COO- -82.8 -80.7 -76.9 CH2COOEt- -74.0 -70.0 -66.7 CH3CONH- -79.3 -76.4 -72.7 N3
- -72.6 -71.9 -68.9 CH2CN- -70.3 -69.6 -65.8 CH3CHCN- -69.2 -67.1 -64.1 CH2NO2
- -76.5 -73.5 -70.7 HS- -80.3 -76.5 -71.8 CH3S
- -78.4 -76.2 -71.4 C6H5S
- -74.9 -67.4 -63.2 CH3SO3
- -77.8 -76.4 -72.9 H3O
+ -105.2 -106.3 -107.6 CH3OH2
+ -83.8 -84.7 -86.3 CH3CH2OH2
+ -77.3 -79.1 -80.3 (CH3)2OH+ -68.5 -68.9 -69.6 (Et)2OH+ -59.2 -60.1 -61.4 NH4
+ -93.5 -93.7 -94.9 CH3NH3
+ -81.2 -81.3 -82.9 (CH3)2NH2
+ -70.7 -70.6 -72.4 (CH3)3NH+ -60.9 -60.7 -62.3 CH3CH2NH3
+ -76.1 -77.2 -78.9 (Et)3NH+ -52.4 -53.1 -54.1 n-PrNH3
+ -73.1 -75.6 -77.5 n-BuNH3
+ -71.2 -75.2 -76.7 C6H5NH3
+ -69.1 -76.1 -77.8 (CH3COCH3)H
+ -66.5 -67.6 -68.4 (PhCOCH3)H
+ -53.6 -56.8 -58.6
Curutchet et al., October 2004, revised version
26
(CH3COOEt)H+ -61.2 -63.1 -63.4 HCONH3
+ -78.4 -79.4 -80.4 CH3CONH3
+ -74.2 -74.7 -75.7 C5H5NH+ -59.5 -60.5 -61.8 (CH3)2SH+ -63.7 -63.5 -64.7 (CH3SOCH3)H
+ -63.3 -64.9 -65.7
Curutchet et al., October 2004, revised version
27
Table 2. Electrostatic and non-electrostatic contributions (kcal/mol) to the free energy
of hydration determined from MST-HF/6-31+G* calculations for the series of univalent
ions used in the parametrization. The electrostatic term was determined by using a
scaling factor of 1.15 and the DC charge renormalization scheme. The experimental
hydration free energies are also given.
Ion ∆Gele ∆Gn-ele ∆Ghyd(MST-DC) Expt. a
F- -101.7 1.7 -99.9 -105.0 Cl- -75.4 0.5 -74.8 -74.6 OCl- -76.1 2.4 -73.7 -80.7 OH- -104.1 0.1 -104.0 -105.0 HO2
- -92.5 2.3 -90.2 -97.3 NH2
- -96.8 0.3 -96.5 -92.2 CN- -75.0 2.9 -72.1 -67.6 HCC- -81.9 -0.8 -82.7 -76.1 CH3O
- -88.8 2.7 -86.0 -95.2 CH3CH2O
- -86.1 3.0 -83.1 -91.1 C6H5O
- -70.9 2.8 -68.1 -71.3 HCOCH2
- -73.5 2.5 -71.0 -75.7 CH3COCH2
- -73.0 2.6 -70.4 -75.6 HCOO- -79.8 4.1 -75.7 -76.2 CH3COO- -80.7 4.2 -76.5 -77.3 CH2COOEt- -70.0 4.0 -66.0 -66.4 CH3CONH- -76.4 2.5 -73.9 -80.1 N3
- -71.9 0.3 -71.6 -70.7 CH2CN- -69.6 3.6 -66.0 -65.7 CH3CHCN- -67.1 4.3 -62.8 -65.6 CH2NO2
- -73.5 4.2 -69.3 -75.9 HS- -76.5 1.8 -74.8 -71.6 CH3S
- -76.2 0.9 -75.3 -73.7 C6H5S
- -67.4 1.1 -66.3 -63.3 CH3SO3
- -76.4 6.1 -70.3 -71.7 H3O
+ -106.3 0.4 -105.9 -110.2 CH3OH2
+ -84.7 -6.9 -91.5 -93.1 CH3CH2OH2
+ -79.1 -6.6 -85.7 -88.4 (CH3)2OH+ -68.9 -3.2 -72.0 -79.8 (Et)2OH+ -60.1 -2.6 -62.6 -71.5 NH4
+ -93.7 0.6 -93.1 -85.2 CH3NH3
+ -81.3 1.2 -80.2 -76.5 (CH3)2NH2
+ -70.6 1.7 -68.9 -68.6 (CH3)3NH+ -60.7 2.3 -58.4 -61.2 CH3CH2NH3
+ -77.2 1.5 -75.8 -73.0 (Et)3NH+ -53.1 3.1 -50.0 -54.7 n-PrNH3
+ -75.2 2.0 -73.2 -70.9 n-BuNH3
+ -75.6 1.7 -73.9 -71.5
Curutchet et al., October 2004, revised version
28
C6H5NH3+ -76.1 1.4 -74.7 -72.8
(CH3COCH3)H+ -67.6 -5.6 -73.2 -76.8
(PhCOCH3)H+ -56.8 -5.2 -61.9 -65.1
(CH3COOEt)H+ -63.1 -4.0 -67.1 -68.5 HCONH3
+ -79.4 0.6 -78.7 -82.5 CH3CONH3
+ -74.7 0.8 -73.9 -73.8 C5H5NH+ -60.5 1.3 -59.2 -61.1 (CH3)2SH+ -63.5 2.6 -60.9 -64.5 (CH3SOCH3)H
+ -64.9 1.6 -63.3 -68.2 a Data taken from ref.19.
Curutchet et al., October 2004, revised version
29
Table 3. Calculated and experimental pKa values for series of substituted pyridines and
carboxylic acids. MST calculations have been performed by using both SC and DC
charge renormalization methods. Absolute and relative pKa values are given in plain and
in italics, respectively.
Compound ∆Ggasa ∆Gsol(A) ∆Gsol(AH+)
(SC) pKa
b
(SC) ∆Gsol(AH+)
(DC) pKa
b
(DC) pKa
(exp) c
Pyridine derivatives H 213.7 -4.9 -58.2 2.2
0.0 -59.2 2.9
0.0 5.2 0.0
p-CH3 218.0 -5.3 -54.9 2.6 0.4
-56.2 3.6 0.7
6.0 0.8
m-CH3 216.6 -5.2 -55.1 1.8 -0.4
-56.7 3.0 0.1
5.7 0.5
m-F 206.7 -3.5 -61.2 0.3 -1.9
-62.3 1.1 -1.8
3.0 -2.2
p-Cl 210.4 -3.9 -59.4 1.4 -0.9
-60.8 2.4 -0.5
3.8 -1.4
m-Cl 207.5 -4.0 -60.0 -0.3 -2.5
-61.4 0.7 -2.3
2.8 -2.4
o-OCH3 220.9 -4.9 -52.9 3.6 1.4
-54.5 4.8 -1.9
6.6 1.4
m-OCH3 216.7 -4.6 -54.2 1.7 -0.5
-55.9 2.9 0.0
4.8 -0.4
p-CN 202.5 -5.5 -64.4 -1.9 -4.1
-67.8 0.6 -2.3
1.9 -3.4
m-CN 201.7 -6.1 -65.5 -2.2 -4.4
-69.0 0.4 -2.5
1.4 -3.9
m-NO2 200.2 -5.4 -66.4 -2.1 -4.3
-69.8 0.4 -2.5
1.2 -4.0
mse d rmsd
-3.2 -0.2 3.2 0.4
-1.8 0.5 1.9 0.8
Carboxylic acids Formic 336.5 -7.1 -76.2 2.5
0.0 -75.7 2.9
0.0 3.8 0.0
Acetic 339.5 -6.8 -78.6 2.7 0.2
-76.5 4.3 1.4
4.8 1.0
Cyanoacetic 321.8 -9.4 -67.1 0.1 -2.4
-66.1 0.9 -2.0
2.5 -1.3
Chloroacetic 327.0 -8.3 -68.7 1.9 -0.6
-69.0 1.7 -1.2
2.9 -0.9
Pivalic 335.9 -4.7 -75.5 0.8 -1.7
-69.8 5.0 2.1
5.0 1.2
Curutchet et al., October 2004, revised version
30
mse rmsd
-2.2 -0.2 2.4 1.2
-0.8 -0.3 1.0 0.6
All compounds mse rmsd
-2.9 -0.2 3.0 0.7
-1.5 0.3 1.6 0.7
a Data taken from refs. 45 and 46. b A correction term of 1.9 kcal/mol was added to the gas phase free energy
difference to account for the change in standard states at 298.15 K. c Values taken from ref. 50. d rms: root-mean square deviation; mse: mean signed deviation.
Curutchet et al., October 2004, revised version
31
Table 4. Calculated and experimental free energies of tautomerization between neutral
and zwitterionic forms of nicotinic (NA) and isonicotinic (INA) acids. MST calculations
were performed by using both SC and DC charge renormalization methods.
Compound ∆Ggasa ∆Gsol(A) ∆Gsol(AH+)
(SC) ∆Gaq (SC)
∆Gsol(AH+) (DC)
∆Gaq (DC)
∆Gaq (exp.) a
NA (A)
(B)
33.3
33.5
-9.3
-9.0
-42.6
-42.6
0.0
0.0
-45.3
-45.3
-2.7
-2.7
-2.0
INA 35.1 -8.6 -42.1 1.6 -45.4 -1.7 -2.5
a Data taken taken from ref. 47
Cur
utch
et e
t al.,
Oct
ober
200
4, r
evis
ed v
ersi
on
32
Tab
le 5
. D
iffe
renc
es in
the
elec
tros
tati
c po
tent
ial c
ompu
ted
in la
yers
aro
und
the
mol
ecul
e, th
e w
ell d
epth
of
the
mol
ecul
ar in
tera
ctio
n po
tent
ial,
and
the
net a
ppar
ent c
harg
e in
duce
d on
the
cavi
ty s
urfa
ce f
or s
erie
s of
con
gene
ric
ioni
c co
mpo
unds
.
Com
poun
d X
rm
sd a in
laye
r E
min
b Q
σ(X
) c
x 1.
4 x
1.6
x 1.
8 x
2.0
MS
T-S
C
MS
T-D
C
MS
T-S
C
MS
T-D
C
CH
3NH
3+ N
H3+
0.0
0.0
0.0
0.0
-123
.8
-123
.8
-0.7
1 -0
.71
CH
3(C
H2)
6NH
3+ N
H3+
2.1
1.8
1.6
1.4
-118
.6
-121
.5
-0.5
3 -0
.65
CH
3OH
2+ O
H2+
0.5
0.4
0.3
0.3
-130
.1
-129
.7
-0.5
7 -0
.59
CH
3(C
H2)
6OH
2+ O
H2+
3.6
3.0
2.5
2.2
-127
.1
-127
.5
-0.3
9 -0
.53
CH
3NH
- N
H-
6.6
5.5
4.4
3.7
-187
.6
-192
.3
+0.
91
+0.
78
CH
3(C
H2)
6NH
- N
H-
1.6
1.3
1.1
0.9
-190
.6
-190
.6
+0.
79
+0.
72
CH
3O-
O-
0.9
0.8
0.6
0.5
-169
.6
-168
.5
+0.
81
+0.
77
CH
3(C
H2)
6O-
O-
0.6
0.5
0.5
0.4
-168
.2
-168
.2
+0.
76
+0.
75
Cur
utch
et e
t al.,
Oct
ober
200
4, r
evis
ed v
ersi
on
33
a rm
sd b
etw
een
the
elec
tros
tati
c po
tent
ials
com
pute
d fr
om th
e w
avef
unct
ions
det
erm
ined
fro
m M
ST
-SC
and
MS
T-D
C c
alcu
lati
ons
for
the
ioni
c
com
poun
ds. L
ayer
s de
fine
d by
sca
ling
the
van
der
Waa
ls r
adii
by
1.4,
1.6
, 1.8
and
2.0
.
b Min
imum
ene
rgy
of th
e m
olec
ular
inte
ract
ion
pote
ntia
l for
the
ioni
c co
mpo
unds
inte
ract
ing
wit
h cl
assi
cal p
robe
par
ticl
es O
- (ca
tion
s) a
nd H
+
(ani
ons)
.
c Net
app
aren
t cha
rge
spre
ad o
n th
e ca
vity
sur
face
of
the
grou
p X
det
erm
ined
fro
m b
oth
SC
and
DC
cha
rge
reno
rmal
izat
ion
sche
me.
Curutchet et al., October 2004, revised version
34
Legends to Figures
Figure 1. Representation of the change in the root-mean-square deviation (rmsd; solid
line) and the relative error (in percentage; dashed line) between the experimental
hydration free energies and the MST values obtained by varying the scaling factor used
to correct the atomic radii of charged atoms in the calculation of the electrostatic
component of the hydration free energy (see text for details). The electrostatic free
energy of solvation was determined by using both SC (black) and DC (white) charge
renormalization schemes (see text for details). The rmsd values are in kcal/mol.
5,0
6,0
7,0
8,0
9,0
10,0
1,00 1,05 1,10 1,15 1,20 1,25
Scaling Factor
rmsd
/rel
ativ
e er
ror
Curutchet et al., October 2004, revised version
35
Figure 2. Comparison of the electrostatic component of the free energy of hydration
(kcal/mol) determined from MST calculations by using a scaling factor of 1.15 and both
SC (black) and DC (white) charge renormalization schemes and IEF calculations at the
HF/6-31+G(d) level. The plots displays the ideal regression line y=cx with slope c equal
to unity.
40.0
60.0
80.0
100.0
120.0
40.0 60.0 80.0 100.0 120.0
-∆Gele(MST)
- ∆G
ele(
IEF
)
Curutchet et al., October 2004, revised version
36
Figure 3. Comparison of the experimental and calculated hydration free energies
(kcal/mol) for the series of univalent ions. Theoretical estimates were obtained from
MST-HF/6-31+G(d) calculations carried out by using a scaling factor of 1.15 and the
DC charge renormalization schemes. The plots displays the ideal regression line y=cx
with slope c equal to unity.
40,0
60,0
80,0
100,0
120,0
40,0 60,0 80,0 100,0 120,0
-∆Ghyd(MST-DC)
- ∆G
hyd
(exp
t)
Curutchet et al., October 2004, revised version
37
Figure 4. Thermodynamic cycle used for the calculation of the pKa values for the series
of substituted pyridines and carboxylic acids.
∆Ggas AH+ A- + H+ gas phase
∆Gsol(AH+) ∆Gsol(A-) ∆Gsol(H
+)
AH+ A- + H+ water ∆Gaq
Curutchet et al., October 2004, revised version
38
Figure 5. Representation of the neutral and zwitterionic species of nicotinic (top) and
isonicotinic (bottom) acids.
N
O
OH
N
OH
O
N
O
O
H
N
OHO
N
OO
H
-
+(A) (B)
+
-
Curutchet et al., October 2004, revised version
39
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Sargeant, E.P. and Dempsey, B. Ionisation Constants of Organic Acids in Aqueous
Solution; IUPAC no. 23; Pergamon Press: New York, 1979.
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Curutchet et al, November 2004
1
Development of distributed models of atomic polarizability for molecular simulations
Carles Curutchet,1 Ignacio Soteras,1 Axel Bidon-Chanal,1 Cristophe Chipot, 2* Modesto
Orozco,3* and F. Javier Luque1*
1 Departament de Fisicoquímica. Facultat de Farmàcia. Universitat de Barcelona. Avgda. Diagonal 643. Barcelona 08028. Spain. 2 Equipe de Dynamique des Assemblages Membranaires. Unité Mixte de Recherche CNRS/UHP 7565. Institut Nancéien de Chimie Moléculaire. Université Henri Poincaré – Nancy I. BP 239, 54506 Vanœuvre-lès-Nancy Cedex, France. 3 Departament de Bioquímica i Biología Molecular, Facultat de Química, Universitat de Barcelona, c/. Martí i Franqués 1, 08028, Barcelona, and Unitat de Modelització Molecular i Bioinformàtica, Institut de Recerca Biomèdica. Parc Científic de Barcelona, c/. Josep Samitier 1, 08028 Barcelona, Spain. Send correspondence to FJL (e-mail: [email protected]) or MO (e-mail: [email protected])
Abstract
This study is focused on the development of atomic distributed polarizability models for the treatment of induction effects in molecular simulations. Different models of dipolar polarizabilities are derived for a series of aromatic compounds from the OPEP (Optimal Partitioning of Electrical Properties) suite of programs. These models are obtained by fitting the induction energies computed in a grid surrounding the molecule by using a fast perturbational approach which permits to reproduce the induction energies determined at the MP2/Sadlej level of theory. Isotropic atomic dipole polarizability models are considered by imposing suitable restrains in the fitting procedure, and by exploring all-atom and united-atom models. The goodness of the distributed models is assessed by comparing the molecular polarizabilities recovered from the models and those obtained from MP2/Sadlej calculations. The behaviour of the models is further examined in the context of cation-π interactions by computing the polarization interaction energy of the aromatic systems with a sodium cation represented by a non-polarizable point charge, and by comparing them to MP2/Sadlej QM/MM calculations. In general, excellent results are obtained for isotropic all-atom models, with deviations around 1 kcal/mol. Energy profiles that characterize the approach of the sodium cation towards the center of the aromatic ring of benzene are also compared to QM/MM calculations and demonstrate the goodness of the models for different orientations. Finally, the transferability of the atomic polarizabilities within the series of benzene derivatives is also examined.
Curutchet et al, November 2004
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Introduction
The assumption that induction effects can be accounted for in an average sense
by means of a simple, appropriate parameterization is at the origin of the durable success of pairwise, additive potential energy functions for cost-effective statistical simulations of liquids. An important ingredient in the development of such nonpolarizable, effective force fields consists of increasing artificially the polarity of the participating molecules to compensate for missing, through-space intermolecular induction phenomena.1 A popular approach for implicit polarization is based upon the observation that, compared to the experimental gas-phase quantities, molecular dipole moments computed at the Hartree-Fock (HF) level of theory, using a split-valence 6-31G(d) basis set, are systematically exaggerated.2 In a number of instances where explicit nonadditivity effects can be neglected, intermolecular potentials parametrized with net atomic charges derived from the HF/6-31G(d) electrostatic potential provide a reasonable description of the properties of the liquid,3 although explicit, mutual polarization of the constituent molecules and their environment is clearly absent. The advantage of representing the system using pairwise, additive potential energy functions lies in the cost-effectiveness of the statistical simulation, avoiding the computationally demanding estimation of induced moments at the expense of sampling of the phase space. Such an implicit polarization approach is, however, not equivalent to a rigorous, atomic-level description of the molecular response to a nonuniform, external electric field, thus constituting the inherent limitation of the approach. This is particularly relevant in statistical simulations of ionic species or highly polarizing systems interacting with polarizable ones. Furthermore, explicit polarization has proven to be pivotal in those cases where intramolecular induction effects are sizable.4,5 The massive increase of computational resources witnessed in recent years, pushing back the limitations of statistical simulations, has allowed molecular assemblies of appreciable complexity to be tackled over realistic time-scales, using sophisticated potential energy functions. The generalized availability of such resources has inevitably contributed to the recent interest of nonadditive force fields, opening the way to the development of alternative approaches for modelling induction effects in chemical systems. To a large extent, the success of molecular simulations relying on polarizable potential energy functions is closely coupled to the ability of the modeller to design such functions. Arguably, the most popular scheme for constructing models of atomic polarizabilities is the one proposed by Applequist.6 In essence, his method is based on a self-consistent determination of parameters characterizing the atomic polarizability that see each other through screened dipole-dipole interactions. Just like its refined version devised by Thole,7 this heuristic approach implies a substantial component of arbitrariness in the parameterization of the model. In contrast, the partitioning scheme put forward by Stone,8-9 combining an earlier formulation of the susceptibility function of the charge density10 with the distributed multipole analysis (DMA) method,11 is clearly more rigorous. Rational models of distributed polarizabilities are derived from high-quality quantum mechanical (QM) calculations of the response of an isolated molecule to an external perturbation, thereby providing one and two-center charge-charge, charge-dipole, dipole-dipole, etc. parameters. A pivotal aspect of this approach concerns the partitioning of the response charge density into atomic and nonlocal contributions. Closely related, an alternative procedure supplying reasonably transferable, distributed polarizabilities12 relies on a topological partitioning of the
Curutchet et al, November 2004
3
molecular space into atomic regions, according to the theory of “atoms in molecules” (AIM) devised by Bader.13 The derived polarizability parameters have been shown to reproduce accurately, in a given region, the induced moments due to a local electrostatic potential and its successive derivatives experienced at another site. Inherently nonlocal,8,9,13 the resulting models include a plethora of terms that rapidly become cumbersome to handle, especially in the context of statistical simulations. For the latter, the number of polarizability components should be reduced significantly to yield compact and tractable sets of parameters, limited to low-order terms, e.g., charge flow and one-center dipole polarizabilities, capable of describing induction phenomena at a minimal cost. As a result, the above methods are not necessarily compatible with such requirements, and the quality of the generated models strongly depends on their level of sophistication. For instance, limiting the description to atomic dipole polarizabilities, accurate reproduction of molecular quantities beyond the order of the dipole is hopeless. Atomic point charges derived from the quantum mechanical electrostatic potential computed on a grid of points around the molecule14-16 are largely utilized for parameterizing the Coulomb part of all-purpose force fields. In the spirit of this approach, a number of schemes targeted at the construction of models of distributed polarizabilities have been devised, based on a least-squares fitting procedure to the induction energy.17-20 Their strength resides in the possibility to generate easily compact and flexible sets of polarizability parameters at any given order. Contrasting with the electrostatic potential, directly available from the wave function, the induction energy is somewhat more difficult to attain. In its most straightforward formulation, referred to as finite perturbation (FP),19 it can be estimated by considering the interaction of the molecule with a nonpolarizable point charge. Whereas potential derived charges imply a single QM calculation to map the entire space around the molecule, discretized in the form of a grid of Np points, evaluating induction energies for the same grid via FP would require Np distinct QM calculations, hence constituting the computational bottleneck of the approach. Clearly, the significant computational effort involved in the determination of induction energies, including usually intramolecular electron correlation and employing large basis sets to warrant an appropriate reproduction of the molecular polarizabilities, limits the applicability of FP to sufficiently small, prototypical systems. In light of these conclusions, two alternatives have been developed concurrently, aimed at a faster estimation of induction energies and relying essentially upon a single QM calculation – a sine qua non condition for the development of nonheuristic models of distributed polarizabilities. The first scheme, based on second-order perturbation theory (PT), allows the generation of large grids of induction energies derived from one QM calculation at the HF level.21,22 In essence, it relies upon an uncoupled form of the HF equations and provides only an approximation of the exact induction energy. Using adequately chosen scaling factors, this perturbative approach has been shown to yield induction energies in good agreement with the FP quantities.22 The second, more elaborate scheme consists of computing induction energies from fully distributed models of polarizabilities obtained within the framework of the AIM theory.12 The key feature of this approach lies in its ability to map grids of induction energies from a single QM calculation at a sophisticated level of approximation, followed by the topological partitioning of the electron density response into atomic regions.23
These two approaches have been compared in the evaluation of induction energy
grids and the derivation of distributed polarizability models at the MP2 level of theory
Curutchet et al, November 2004
4
and considering different choices of basis set24. The results pointed out that both strategies supply induction energies of comparable quality in terms of error with respect to the reference FP values for neutral molecules, provided that the PT HF/Saldej induction energy estimates are scaled appropriately to reproduce the MP2 quantities, this approach being more difficult to apply in the case of anions. Nevertheless, the strategy based on second-order perturbation theory constitutes a very appealing alternative due to its limited computational cost an ease of implementation. Moreover, this study showed the importance of sampling the space surrounding the molecule sufficiently far from the nuclei in the computed induction energy grids in order to obtain appropriate distributed models, and the suitability of the Sadlej26 basis set at the MP2 level of theory as an optimal compromise in terms of computational cost and agreement with experimental molecular polarizabilities.
The purpose of this study is to explore the strategy relying on the PT calculation
of induction energies for the derivation of distributed polarizability models able to introduce polarization effects in classical force fields in a systematic and well-defined way. As a test case, distributed models are derived for a series of aromatic compounds in order to explore the behaviour of this strategy in the context of cation-π interactions, where polarization effects play an important role25. The models are obtained by considering isotropic dipole atomic polarizabilities, and by exploring both united-atom and all-atom models, and the quality of the fitted parameters is assessed by comparing the molecular polarizabilities recovered from the models and those obtained from MP2/Sadlej calculations. The behaviour of the models are then examined in the context of cation-π interactions by computing the polarization interaction energy of the aromatic systems with a sodium cation represented by a non-polarizable point charge, and by comparing them to MP2/Sadlej QM/MM calculations. In addition, energy profiles that characterize the approach of the sodium cation towards the centre of the aromatic ring of benzene are also compared to QM/MM calculations to explore the goodness of the models for different orientations. Finally, the transferability of the atomic polarizabilities within the series of benzene derivatives is also examined.
Methods
A series of aromatic systems shown in Figure 1 were chosen in order to test the performance of the atomic distributed polarizability models in the prediction of polarization energies in cation-π complexes. The benzene derivatives were optimized at the MP2/6-31G(d,p) level of theory. Then, induction energy grids were generated by using the approach based on second-order perturbation theory. This approach permits the evaluation of the whole grid of induction energies from a single quantum chemical calculation, which was performed at the HF/Sadlej level of theory. Then, the induction energy estimates were scaled by a distance-dependent function in order to reproduce MP2/Sadlej estimates24. This choice is justified as the Sadlej26 basis set used at the MP2 level of theory offers a good compromise between computational cost and agreement with experimental molecular polarizabilities. The grids were constructed by taking about 1000 points going from 2 to 5 times the van der Waals atomic radii of the nearest atom, in order to sample the space surrounding the molecule sufficiently far from the nuclei. Molecular polarizabilities were also computed at the MP2/Sadlej level in order to assess the goodness of the distributed models.
Curutchet et al, November 2004
5
Figure 1. Aromatic structures considered in this study.
Isotropic dipole atomic components were fitted following different criteria in order to derive the distributed models, either by adopting an all-atom (AA) or united-atom (UA) approach. At the UA models, atomic polarizabilities were fitted for all atoms except for hydrogens. In order to test the transferability of the models, three different schemes were used for either AA or UA schemes. First, fitting to the induction energy grids was carried out without any restrain (no restrains - NR). Second, symmetric atoms were forced to share the same polarizability components (symmetry - S). Finally, all carbons and hydrogens pertaining to aromatic CH groups were forced to have the same components at each different system (atom type – AT). The atomic polaribilities obtained by using these three procedures were subsequently compared and used to discuss the transferability of these values between different aromatic systems.
The final behaviour of the models was analyzed by comparing the fitted
molecular polarizabilities with the pure QM estimates. In addition, polarization interaction energies between a sodium cation and the aromatic systems were computed both from the distributed models and from QM/MM calculations, where the sodium cation was simulated as a nonpolarizable point charge. The sodium cation was added at 2.47 Å above the aromatic ring for all systems (see ref. 25).The polarization energies derived from the isotropic distributed models were computed following the procedure proposed first by Applequist27, and subsequently refined by Thole7. On the other hand, QM/MM estimates were determined by two different approaches. First, by computing the full variational polarization interaction energy of the point charge with the aromatic system, and second, by using the second-order perturbational approach used to build up the induction energy grids, i.e., by computing perturbationally the HF/Sadlej polarization energy and then scaling it to reproduce MP2/Sadlej values. This final calculation also permits to analyze the performance of the fast second-order perturbational approach in comparison with the more costly variational calculation.
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Curutchet et al, November 2004
6
Finally, polarization energy profiles determined for the approach of the sodium cation to the aromatic ring of benzene were calculated using the isotropic all-atom symmetry (AA-S) model and from QM/MM MP2/Sadlej calculations, with the aim to investigate the behaviour of the model at different orientations of the cation.
Results and discussion
Table 1 shows the polarization energies obtained variationally for the cation-π complexes at the MP2/Sadlej level and the values obtained using the perturbational approach mentioned before. The polarization energies determined perturbatively are able to reproduce the variational results with a deviation of only 9% (r2=0.97) and a much lower computational cost, thus giving support to its use as a general strategy for the derivation of atomic polarizabilities adjusted to a given molecule.
Table 1. Variational and perturbational QM/MM MP2/Sadlej polarization interaction energies (kcal/mol) between the aromatic systems and the Na+ cation. Compound Variational Perturbational
1 -21.4 -23.8 2 -25.2 -28.3 3 -25.1 -27.6 4 -28.7 -30.4 5 -21.2 -23.7 6 -22.4 -24.9 7 -24.3 -26.5 8 -22.3 -25.2 9 -22.2 -25.3 10 -21.0 -23.5 11 -21.0 -23.7 12 -22.4 -23.4 13 -20.5 -21.3 14 -18.9 -20.9 15 -19.8 -22.3
msea 2.3 mue 2.3 rms 2.5
a mse: mean signed deviation (kcal/mol); mue: mean unsigned deviation (kcal/mol); rms: root-mean square deviation (kcal/mol)
The comparison of molecular polarizabilities obtained from the different models with the values determined variationally at the MP2/Sadlej level are shown in Table 2. A very close agreement is found when an all-atom description is used, as noted in mean deviations less than 1% when atom-type restraints are imposed in the fitting of atomic polarizabilities. When a united-atom description is used, the agreement between molecular polarizabilities recovered from the distributed models and computed variationally is slightly worse, even though the mean deviation is only 4%. At this point, it must be pointed out that the molecular polarizability was not used as an adjustable parameter in the fitting procedure to derive the distributed models, and so the agreement obtained gives strong support to the method.
Curutchet et al, November 2004
7
Table 2. Trace of the molecular polarizability (a.u.) obtained from the quantum mechanical calculation (MP2/Sadlej) and from different isotropic distributed models (All-atom/United-atom) obtained by imposing different kind of restrains: no restrains (NR), symmetry (S), atom type (AT). Compound All-atom United-atom QM NR S AT NR S AT
1 208.3 214.2 214.2 214.2 230.1 230.6 230.6 2 360.5 345.4 346.3 345.7 355.7 356.3 362.4 3 308.4 301.8 301.8 301.3 309.6 309.6 314.8 4 399.2 366.2 366.5 364.1 375.4 375.5 383.8 5 208.1 212.8 212.9 212.9 219.6 219.9 222.9 6 225.2 230.1 230.1 230.1 237.6 238.1 241.3 7 247.7 253.7 253.7 253.5 261.5 261.8 265.0 8 251.9 256.5 256.6 256.7 263.0 263.1 266.2 9 259.2 257.5 257.6 257.6 265.3 265.6 268.3 10 207.8 211.2 211.3 211.3 213.8 213.9 213.9 11 209.9 214.1 214.6 214.6 214.6 214.9 214.9 12 165.1 175.4 175.6 175.3 191.3 191.3 191.2 13 145.9 154.5 154.7 155.9 170.4 170.4 170.2 14 147.7 156.8 156.8 158.2 171.1 171.1 171.2 15 192.2 196.0 196.0 196.6 213.4 213.4 213.8
msea -0.6 -0.8 -0.7 -10.3 -10.6 -12.9 mue 8.1 8.1 8.5 14.2 14.3 14.9 rms 11.4 11.3 12.0 17.0 17.1 17.3
a mse: mean signed deviation (kcal/mol); mue: mean unsigned deviation (kcal/mol); rms: root-mean square deviation (kcal/mol)
Another parameter considered to asses the goodness of the fittings is the
deviation found between the induction energies computed quantum-mechanically and the values recovered from the distributed models along the grid points (see Table 3). In general, a good agreement is found for all the models, with small deviations ranging from 0.12·10-3 to 0.27·10-3 (in a.u.).
Table 3. Root-mean square deviation (10-3 a.u.) between the quantum mechanically and the recovered induction energies computed at the grids from different isotropic distributed models (All-atom/United-atom) obtained by imposing different kind of restrains: no restrains (NR), symmetry (S), atom type (AT). Compound All-atom United-atom NR S AT NR S AT
1 0.11 0.11 0.11 0.36 0.36 0.36 2 0.13 0.14 0.14 0.21 0.22 0.30 3 0.12 0.12 0.13 0.20 0.20 0.27 4 0.17 0.17 0.26 0.24 0.25 0.40 5 0.11 0.11 0.11 0.24 0.24 0.28 6 0.12 0.12 0.12 0.26 0.27 0.31 7 0.13 0.13 0.13 0.26 0.26 0.30 8 0.11 0.11 0.12 0.21 0.21 0.24 9 0.13 0.13 0.13 0.22 0.22 0.25 10 0.10 0.10 0.10 0.17 0.17 0.17 11 0.11 0.11 0.11 0.12 0.12 0.12 12 0.11 0.11 0.11 0.25 0.25 0.25 13 0.10 0.10 0.11 0.23 0.23 0.23 14 0.11 0.11 0.13 0.25 0.25 0.25 15 0.11 0.11 0.12 0.36 0.36 0.36
Mean 0.12 0.12 0.13 0.24 0.24 0.27
Curutchet et al, November 2004
8
In order to further investigate the behaviour of the models, the polarization energy of the aromatic systems interacting with the Na+ cation (placed at its optimum position to establish a cation-π interaction) was computed from the distributed models and compared to the variational MP2/Sadlej QM/MM calculations. Table 4 shows the results computed by neglecting the coupling between atomic induced dipoles, i. e., by considering only the electric field generated by the point charge of the sodium cation. On the other hand, Table 5 shows the results determined by computing the electric field generated by both the sodium cation and by the atomic induced dipoles following an iterative procedure, which usually converges in one or two cycles. The polarization energies of the different models with the Na+ cation show a good agreement, especially when an all-atom description is used. In this case, the differences between the polarization energies obtained at the QM and classical levels are lower than 2%, while this difference increases to 15% when united-atom models are considered. The results also indicate that the mutual coupling between the induced dipoles for the different cation-π complexes have a relalitively small effect in the computed induction energies. These results suggest, then, that the mutual coupling could be neglected, thus avoiding the self-consistent procedure that must be carried out to reach convergence between the induced dipoles, with the corresponding saving in computational cost specially for simulations of complex systems. Table 4. Polarization interaction energy (kcal/mol) between the Na+ cation and the aromatic systems determined from the variational quantum mechanical calculation and from different isotropic distributed models (All-atom/United-atom) obtained by imposing different kind of restrains (no restrains, symmetry, atom type). Energies computed without coupling between atomic induced dipoles. Compound All-atom United-atom QM NR S AT NR S AT
1 -21.4 -22.2 -22.3 -22.3 -29.1 -29.2 -29.2 2 -25.2 -23.2 -22.9 -23.6 -20.9 -20.7 -24.3 3 -25.1 -21.7 -21.7 -23.7 -21.8 -21.8 -24.0 4 -28.7 -24.1 -24.0 -23.0 -19.1 -19.1 -22.0 5 -21.2 -21.4 -21.5 -21.5 -24.2 -24.2 -25.6 6 -22.4 -22.5 -22.6 -22.6 -25.6 -25.7 -27.0 7 -24.3 -23.8 -23.9 -24.0 -26.5 -26.5 -27.6 8 -22.3 -22.4 -22.4 -22.4 -25.0 -25.0 -25.9 9 -22.2 -23.4 -23.4 -23.4 -23.5 -23.5 -24.1 10 -21.0 -20.6 -20.7 -20.7 -21.7 -21.7 -21.7 11 -21.0 -20.4 -20.5 -20.5 -20.4 -20.5 -20.5 12 -22.4 -21.6 -21.7 -21.5 -27.9 -27.9 -27.9 13 -20.5 -19.0 -19.1 -19.5 -25.0 -25.0 -25.0 14 -18.9 -19.3 -19.3 -19.8 -25.3 -25.3 -25.4 15 -19.8 -20.5 -20.5 -20.8 -27.4 -27.4 -27.4
msea 0.7 0.7 0.5 -1.8 -1.8 -2.7 mue 1.2 1.2 1.1 4.2 4.2 4.0 rms 1.8 1.8 1.8 5.1 5.1 4.8
a mse: mean signed deviation (kcal/mol); mue: mean unsigned deviation (kcal/mol); rms: root-mean square deviation (kcal/mol)
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Table 5. Polarization interaction energy (kcal/mol) between the Na+ cation and the aromatic systems determined from the variational quantum mechanical calculation and from different isotropic distributed models (All-atom/United-atom) obtanied by imposing different kind of restrains (no restrains, symmetry, atom type). Energies computed coupling atomic induced dipoles. Compound All-atom United-atom QM NR S AT NR S AT
1 -21.4 -22.5 -22.6 -22.6 -29.1 -29.2 -29.2 2 -25.2 -23.2 -22.7 -23.4 -20.9 -20.7 -24.3 3 -25.1 -21.8 -21.8 -23.8 -21.8 -21.8 -24.0 4 -28.7 -24.2 -24.1 -23.4 -19.1 -19.1 -22.0 5 -21.2 -22.0 -22.1 -21.9 -26.9 -26.9 -26.7 6 -22.4 -22.7 -22.8 -22.7 -25.6 -25.7 -27.0 7 -24.3 -23.9 -24.0 -24.1 -26.5 -26.5 -27.6 8 -22.3 -23.5 -23.5 -23.2 -28.3 -28.3 -27.7 9 -22.2 -23.7 -23.7 -23.8 -22.2 -22.1 -22.7 10 -21.0 -21.1 -21.2 -21.2 -23.0 -23.2 -23.2 11 -21.0 -21.0 -21.1 -21.1 -21.6 -21.7 -21.7 12 -22.4 -22.2 -22.2 -22.0 -27.9 -27.9 -27.9 13 -20.5 -19.6 -19.7 -19.9 -25.0 -25.0 -25.0 14 -18.9 -23.7 -23.7 -26.0 -33.0 -33.0 -33.0 15 -19.8 -21.2 -21.3 -21.2 -27.4 -27.4 -27.4
msea 0.0 0.0 -0.3 -2.8 -2.8 -3.5 mue 1.5 1.6 1.5 5.1 5.2 4.7 rms 2.2 2.3 2.6 6.4 6.5 6.1
a mse: mean signed deviation (kcal/mol); mue: mean unsigned deviation (kcal/mol); rms: root-mean square deviation (kcal/mol) Finally, the energy profiles that characterize the approach of the sodium cation to benzene were calculated from the isotropic all-atom symmetry (AA-S) model and from QM/MM calculations. As shown in Figure 2, approximation profiles were computed along three orientations: (i) along the middle of a C-C bond (x orientation), (ii) along the C-H bond (y orientation), and (iii) perpendicular to the center of the aromatic ring (z orientation). In all cases, polarization energies at the “hard particle radius” (defined as the point where dispersion and repulsion cancel each other, see ref. 25) and in points closer to and further away from the molecule were computed. The results given in Figure 3 show the good behaviour encountered for the model along these three orientations. Figure 2. Orientations of cation-aromatic interactions in this study. The z axis corresponds to the cation-π interaction.
x
y z
H HH
HH
H
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Figure 3. Polarization energy profiles that characterize the approach of Na+ to benzene determined from QM/MM MP2/Sadlej calculations and from the isotropic all-atom symmetry model of distributed polarizabilities. Distances (in Å) are referred in all cases to the hard sphere radius, the point where dispersion and repulsion cancel each other. Hard sphere radii are: 4.58 Å (x axis), 4.97 Å (y axis), and 3.24 Å (z axis). Profiles computed without coupling between atomic induced dipoles.
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In order to further investigate the transferability of atomic polarizability components between the different systems considered, the atomic polarizabilities obtained for the C and H atoms (all-atom) and the C-H group (united-atom) in the different distributed models are shown in Table 6. Table 6. Isotropic polarizability components (a.u.) for C and H pertaining to aromatic CH groups derived from different isotropic models. Mean values and standard deviations are given for the whole series of benzene derivatives considered in the study.
All-atom αC NR 10.2 6.8 S 10.4 5.9 AT 9.6 2.3 αH NR 3.5 1.1 S 3.4 0.9 AT 3.6 0.4
United-atom αC NR 19.1 8.8 S 19.1 8.4 AT 16.7 8.1 Inspection of the mean values obtained for the series of complexes shows that no relevant differences are found in the atomic polarizabilities obtained either without restraints or by imposing symmetry or atom-type equivalences. The atomic polarizability of C and H oscillates (in a.u.) between 9.6 and 10.4, and between 3.4 and 3.6, and for the C-H group adopts values between 16.7 and 19.1. However, it must be noted that notably large standard deviations are found, which suggests the existence of marked differences in the atomic polarizabilities obtained for these atoms in different molecules. This is clearly reflected in the results shown in Tables 7 (all-atom) and 8 (united-atom), where the mean atomic polarizabilities obtained for each compound are given. For instance, the C polarizability obtained without restraints oscillates between 4.0 and 18.2 (a.u.), while the C-H polarizability oscillates between 12.7 and 31.5. These results seriously question the assumption that distributed models of atomic polarizabilities can be transferable between structurally related molecules. Table 7. Isotropic polarizability components (a.u.) for C and H pertaining to aromatic CH groups derived from different all-atom isotropic models. For the atom-type model (AT) components derived for each aromatic system are given. In cases where diferent values can be found at each aromatic system, i.e. no restrains (NR) and symmetry (S) models, mean, maximum and minimum values, along with standard deviations are given for each compound. Atom-type No restrains Symmetry αC αC αC Mean Max Min Dev Mean Max Min Dev 1 8.2 8.1 8.9 5.8 1.1 8.2 8.2 8.2 0.0 2 10.8 11.5 23.8 -0.6 9.1 12.5 13.6 11.5 1.1 3 11.0 11.6 21.3 4.2 6.5 11.6 21.3 4.2 6.5 4 11.5 16.1 29.9 2.3 9.3 16.5 30.2 7.8 8.8 5 8.6 9.8 13.7 4.4 3.9 9.7 12.1 7.5 2.3 6 8.6 9.9 13.8 3.8 4.7 9.9 12.4 6.7 3.0 7 9.5 9.9 14.0 5.5 3.4 9.9 12.4 8.2 1.7 8 8.6 10.0 15.9 1.2 6.2 10.0 13.5 4.8 4.7 9 8.6 9.2 12.7 4.0 4.2 9.2 11.0 6.8 2.2 10 10.9 10.6 12.3 8.5 1.7 10.9 10.9 10.9 0.0 11 18.5 18.2 19.7 16.4 1.6 18.5 18.5 18.5 0.0 12 8.4 8.4 12.7 4.4 3.6 8.4 9.9 6.8 1.8 13 7.6 6.5 13.2 -0.7 6.8 6.6 12.3 0.9 6.6 14 7.2 4.0 6.9 -1.8 5.0 4.0 6.9 -1.8 5.0 15 6.8 5.3 19.2 -4.9 12.2 5.3 18.5 -4.0 12.0
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αH αH αH Mean Max Min Dev Mean Max Min Dev 1 3.7 3.8 4.7 3.5 0.5 3.7 3.7 3.7 0.0 2 3.5 3.5 6.1 1.4 1.6 3.1 3.2 2.9 0.2 3 3.4 3.3 5.3 0.9 1.5 3.3 5.3 0.9 1.5 4 3.9 2.6 5.0 0.4 1.4 2.5 3.6 0.4 1.3 5 3.6 3.4 4.5 3.0 0.6 3.4 3.6 3.2 0.2 6 3.8 3.6 4.6 2.9 0.6 3.6 3.7 3.2 0.2 7 3.7 3.7 4.5 3.0 0.6 3.7 4.0 3.2 0.3 8 3.7 3.5 4.9 2.7 0.9 3.5 4.0 2.9 0.5 9 3.6 3.6 4.7 3.0 0.7 3.5 3.7 3.3 0.2 10 3.2 3.3 3.8 2.9 0.4 3.2 3.2 3.2 0.0 11 2.1 2.2 2.8 1.6 0.6 2.1 2.1 2.1 0.0 12 3.7 3.6 4.7 2.8 0.8 3.6 4.2 3.1 0.6 13 3.5 3.7 5.6 2.1 1.7 3.7 5.0 2.3 1.6 14 3.8 4.4 5.6 3.4 1.2 4.4 5.6 3.4 1.2 15 4.0 4.1 5.6 2.2 1.6 4.1 5.4 2.3 1.6 Table 8. Isotropic polarizability components (a.u.) for C pertaining to aromatic CH groups derived from different united-atom isotropic models. For the atom-type model (AT) components derived for each aromatic system are given. In cases where diferent values can be found at each aromatic system, i.e. no restrains (NR) and symmetry (S) models, mean, maximum and minimum values, along with standard deviations are given for each compound. Atom-type No restrains Symmetry αC αC αC Mean Max Min Dev Mean Max Min Dev 1 12.8 12.8 15.9 10.5 2.1 12.8 12.8 12.8 0.0 2 18.9 22.0 33.6 10.1 8.4 22.2 29.0 15.3 7.3 3 18.4 21.4 32.6 10.5 8.9 21.4 32.6 10.5 8.9 4 19.9 24.2 36.5 16.1 8.0 24.1 34.8 16.3 7.7 5 14.9 19.0 31.3 6.0 11.2 19.0 29.7 8.8 10.5 6 15.1 19.7 36.1 3.2 13.4 19.6 31.8 7.6 12.1 7 16.2 20.7 34.5 5.3 13.3 20.7 33.1 8.1 12.5 8 15.0 18.8 29.6 7.6 10.5 18.8 29.3 8.5 10.4 9 15.9 19.1 28.8 9.7 8.4 19.1 27.4 12.0 7.8 10 21.9 21.8 25.7 17.7 3.9 21.9 21.9 21.9 0.0 11 31.5 31.5 31.9 31.1 0.4 31.5 31.5 31.5 0.0 12 13.5 14.0 15.5 12.2 1.5 14.0 15.1 12.8 1.4 13 12.8 13.0 13.8 12.4 0.7 13.0 13.6 12.4 0.7 14 12.9 12.6 13.3 12.1 0.6 12.6 13.3 12.1 0.6 15 12.7 12.4 17.3 6.8 4.5 12.4 17.1 6.8 4.6
Concluding remarks The procedure described in this study constitutes a promising alternative for the derivation of distributed models of atomic polarizabilities. The models obtained are able to reproduce either the polarization energies computed variationally or the global polarizability of the molecule. No relevant differences are found in the magnitude of the atomic polarizabilities due to the use of symmetry or atom type-based restraints compared to the values derived without imposing any restraint. On the other hand, marked differences are found in the values obtained for different molecules, thus difficulting the definition of a single set of atomic values transferable between molecules. These findings suggest that the procedure adopted can be an efficient alternative for the definition of distributed models of atomic polarizabilities.
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