institut für physikalische chemie & elektrochemie, lehrgebiet a columbus, oh, june 2006.ppt...
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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ROTATIONAL SPECTRAIN SERVICE OF PARTICLE PHYSICS
- ZEEMAN & HYPERFINE EFFECTS
Jens-Uwe Grabow, Lukas D. AlpheiGottfried-Wilhelm-Leibniz-Universität Hannover
Richard J Mawhorter, Alexander Baum, Zachary Glassmann, Benjamin GirodasPomona College, Claremont, CA
Trevor J SearsBrookhaven National Laboratory, Upton, NY
N.E. Shafer-RayUniversity of Oklahoma, Norman, OK
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Advantages of FT-microwave spectroscopy
Sample preparation for FT-MW Experiment
Precise FTMW Characterization
Future High Precision FTMW Investigation
Rotational Spectroscopy in the Time-Domain:Technique, Capabilities & Directions
non-volatile species: LASER-Ablation Source: CATS technique
high resolution & sensitivity: Resonator & Jet: COBRA instrument
electronic angular momentum species: in-situ generation: PbF, YbF, etc.
- Stark effect
- Zeeman effect
e-EDM sensitive species: Polarization direction: DREAM-FTMW machine
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Coaxial oriented Beam-Resonator Arrangement (COBRA):molecular excitation
)()(
)()(
tt
tt
bbba
abaa
0 baab
tMW pulse
1μs
before excitation pulse: dipole moments cancelEb
Ea
many two-level systems
single particle, Schrödinger equation:
iH
iH ,ensemble properties, von Neumann equation
wavefunction
density matrix
density matrix:
(no) coherence:
population: 0 bbaa
J.-U. Grabow, W. Stahl, Z. Naturforsch. 45a, 1043 (1990).
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Columbus, June 2013
Coaxial oriented Beam-Resonator Arrangement (COBRA):molecular response
E
t
T = 100μs
MW signal
after excitation pulse: oscillating macroscopic dipole moment
density matrix:
)()(
)()(
tt
tt
bbba
abaa
0, baabcoherence:
population: 0bbaa
Fourier Transform
Frequency Domain, Spectrum
Time Domain, FID
U. Andresen, H. Dreizler, J.-U. Grabow, W. Stahl, Rev.Sci.Instrum. 61, 3694 (1990).
J.-U. Grabow, W. Stahl, H. Dreizler, Rev.Sci.Instrum. 67, 4072 (1996).
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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COBRA chamber
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Fabry-Pérot Type Resonator: Spherical Reflectors
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Spherical Reflector: Transmit & Receive Antennae
supersonic-jet source
high-frequency antennae
low-frequency antennae
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Columbus, OH, June 2006 <Dateiname>.ppt
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TeSe: Electronic Data From Pure Rotational Spectra
125Te77SeJ‘ ← J 4 ← 3
Resolution:0.0000001 cm-1
Accuracy:0.00000001 cm-1
req = 235.904038(71) pm
Deike Banser, Melanie Schnell, Jens-Uwe Grabow, Emilio J. Cocinero, Alberto Lesarri, and Jose L. Alonso, Angew. Chem. Int. Ed. 2005, 44, 6311.
3
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Columbus, OH, June 2006 <Dateiname>.ppt
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MSe Multi-Isotopolog Potential Fits:Tracking down tiny effects of different origin
, ,
L. Bizzocchi, B.M. Giuliano, M. Hess, J.-U. Grabow, J. Chem. Phys. 126, 114305(2007).
B.M. Giuliano, L. Bizzocchi, S. Cooke, D. Banser, M. Hess, J. Fritzsche, J.-U. Grabow, PCCP 10, 2078(2008).
Born-Oppenheimer breakdown correction coefficients:
)24(92.12)(01 PbSePb
)16(915.1)(01 PbSeSe
)19(644.1)(01 SnSeSn
)10(841.1)(01 SnSeSe
)71(9787.20)(01 TeSeTe
)32(9541.20)(01 TeSeSe
1 3 1electronic state nuclear volume
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Columbus, OH, June 2006 <Dateiname>.ppt
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Symmetry leads to ±M-degeneracy of any molecule/atom that is not broken by an E-field along quantization axis.
The existence of an electron electric dipole moment would break this symmetry.
Major Difficulty:
A backgroundmagnetic field mimics an electron EDM.
What Would An
electron Electric Dipole Moment (e-EDM)
Do?
To search for an e-EDM look for
DU=U+M –U-M
in a strong (internal) E field at alternately parallel/anti-parallel B-fields.
A polar heavy atom diatomic in an electric field parallel or anti-parallel to an magnetic field:
• with a zero e−EDM the energy between states that differ only by MF is independent of the relative direction.
• a nonzero e−EDM would cause a small difference in this energy for the parallel and anti-parallel
configuration.
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Zentrum für Festkörperchemie
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Molecules with electronic angular momentum:
Heavy-metal fluorides
PbF
un-paired p electron: 2P1/2 ground state small g-factor
hfs due to F (and 207Pb) spin I = 1/2 large polarizabilityheavy Pb nucleus: relativistic effects candidate for e-EDM measurements @ reasonabe B-field control
\w linear Stark-effect (Eint~30 GV/cm) at moderate ext. fields
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Generation of PbF seeded supersonic jet:Coaxial Ablation Twin Source (CATS)
SF6(1%) / Ne @ ~500 kPa
Nd:YAG LASER I
Nd:YAG LASER II
supersonic
expansion
rotating/translating rods: elements, alloys, compounds
bulk material, compressed powder
elementary Pb
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Molecules with electronic angular momentum:
Zeeman-effect of 208PbF
-0.6 -0.4 -0.2 0 0.2 0.4 0.6 0.8
-0.15
-0.1
-0.05
0
0.05
0.1
0.15
0.2
Parallel ...
Splitting/MHz
B / gauss
Perpendicular Magnetic Field: ∆M = ± 1
Parallel Magnetic Field: ∆M = 0J, F = 1/2, 0 → 3/2, 1
J, F = 1/2, 1 → 3/2, 1
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Molecules with electronic angular momentum /w nuclear hfs:
Concept for a molecular spectroscopy e-EDM experiment
accidentally close-lying 207Pb19F states of opposite parity: complete polarizability (yielding ~30GV/cm effective internal fields) at moderate laboratory E fields (200V/cm)
2-spin system:
e-, F
3-spin system: e-, F, Pb
208Pb19F 207Pb19F
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Molecules with electronic angular momentum w/o nuclear hfs:
Concept for a molecular spectroscopy e-EDM experiment
WC:3Δ1electronic ground state
small g-factor
Systematically very
close-lying Λ-doublets
of opposite parity:
fields of E ~ 1 V/cm are
sufficient for complete
polarization (60 GV/cm).
from A. Leanhardt
Current limit (de =10.5 x 10-28 e cm-1):
would lead to e-EDM effect of 50 mHz
E = 0 E ≠ 0
J = 2
J = 1
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Where are we now?
accuracy reached with:
- standard COBRA-FTMW instrument
- <5 d after Pb rod was first inserted
measurement linewidth comparable to that in study of YbF:
J. Hudson, B. Sauer, M. Tarbutt, E. Hinds, Phys. Rev. Lett. 89 (2002) 23003.
Ai = -di + dci J(J+1)alternative interpretation of dci:
centrifugal correction to Ai
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Columbus, OH, June 2006 <Dateiname>.ppt
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Origin Of dc1 And dc2 ?Comparison to high level ab-initio calculations
in preparation
FS-RCCSD method
large basis sets
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Columbus, OH, June 2006 <Dateiname>.ppt
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Where are we now?
nuclear anapole moment
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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PbF: P-odd, T-odd effects
Current limit (from Tl atomic spectroscopy): de =10.5 x 10-28 e cm-1
J. J. Hudson, D. M. Kara, I. J. Smallman, B. E. Sauer, M. A. Tarbutt, E. A. Hinds, Nature 473 (2011) 493
corresponds to: WP,T κP,T+ Wd de = 17 mHz
nuclear anapole moment constants e-EDMV. V. Flambaum, I. B. Khriplovich, O. P. Sushkov, Phys. Lett. B 146 (1984) 367.
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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P-odd – Interaction Constant Wp:ab-initio calculations
A. Borschevsky, M. Ilias, V. A. Dzuba, K. Beloy, V. V. Flambaum, P. Schwerdtfeger, Phys. Rev. A 85, 052509 (2012)
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Molecules with electronic angular momentum:
Ytterbium Fluoride
YbF
un-paired s electron: 2S1/2 ground state small g-factor
hfs due to F spin I = ½ (171/173Yb: 1/2,5/2) large polarizabilityheavy Yb nucleus: relativistic effects
candidate for e-EDM measurements @ precise B-field controls electron penetrates nucleus: nuclear anapole moment sensitivity
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Generation of WC seeded supersonic jet:Coaxial Ablation Twin Source (CATS)
SF6(1%) / Ne @ ~500 kPa
or
pure Ne @ ~500 kPa
Nd:YAG LASER I
Nd:YAG LASER II
supersonic
expansion
rotating/translating rods: elements, alloys, compounds
bulk material, compressed powder
elementary Yb
or
YbF
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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COBRA-FTMW YbF Measurements
Measured 12 new and 4
previous* YbF lines:
• 1 170YbF lines
• 4 171YbF lines#
• 4 172YbF lines
• 4 174YbF lines
• 3 176YbF lines
# Spin ½ Yb nucleus
174YbF
*C.S. Dickinson, S.A. Coxon, N.R. Walker, M.C.L. Gerry , J. Chem. Phys. 115, 6979 (2001).
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Columbus, OH, June 2006 <Dateiname>.ppt
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YbF multi-isotopologue fit#+ results
174Yb19F V=0 V=1
Y01 / MHz 7256.444(80)
01 / MHz -0.145(80)
Y11 / MHz -44.9378(152)
Y02 / MHz -0.007159* -0.006904*
/ MHz -13.418163(310) -33.80950( 49)
D / MHz 0.00397552(309) 0.0043202( 37)
bF(F) / MHz 170.26361( 68) 168.8030(110)
c(F) / MHz 85.4035( 32) 86.7127(134)
cD(F) / MHz 0.001552( 70) 0.00216( 38)
CI(F) / MHz 0.014544(177) 0.01548( 66)* fixed to value taken from:
K.L. Dunfield, C. Linton, T.E. Clarke, J. McBride, A.G. Adam, J.R.D. Peers, J. Mol. Spectrosc. 174, 433 (1995).
+ including RF transitions taken from:
B. E. Sauer, J. Wang, and E. A. Hinds, J. Chem. Phys. 105, 7412 (1996).
# including v=1 transitions taken from:
C.S. Dickinson, S.A. Coxon, N.R. Walker, M.C.L. Gerry , J. Chem. Phys. 115, 6979 (2001).
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Columbus, OH, June 2006 <Dateiname>.ppt
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Diatomic Rotation - The quest for thee-EDM accelarated by Molecular Spectroscopy:
DREAM - FTMW
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Columbus, OH, June 2006 <Dateiname>.ppt
Zentrum für Festkörperchemie
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Acknowledgement
Aaron Leanhardt, U. Michigan
Feinmechanikwerkstatt des Instituts für Physikalische Chemie
W. Rogge
Deutsche
Forschungsgemeinschaft (DFG)
Deutscher Akademischer
Austauschdienst (DAAD)
Fonds der Chemischen Industrie
(FCI)
Land Niedersachsen