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原始惑星系円盤でのマグネシウムケイ酸塩気相成と蒸発 Vapor growth/evaporation of Mg-silicate under proto- planetary disk conditions: Experimental study Shogo Tachibana Dept. of Natural History Sciences, Hokkaido Univ. CPS seminar 3/6/2013 HOKKAIDO UNIVERSITY

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Page 1: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

原始惑星系円盤でのマグネシウムケイ酸塩気相成⻑⾧長と蒸発

Vapor growth/evaporation of Mg-silicate under proto-planetary disk conditions: Experimental study

Shogo TachibanaDept. of Natural History Sciences, Hokkaido Univ.

CPS seminar 3/6/2013

HOKKAIDO UNIVERSITY

Page 2: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Dense molecular

clouds

Blue supergiant

“Sher 25”

NGC3603

Starburstcluster

Proplyds

Giant pillars

Material Circulation in the Galaxy

Page 3: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Material Circulation in the Galaxy

Stars

SNe II SNe Ia

Interstellar Medium

Molecular Clouds

Journey

of Dust

2.1 Dust in the interstellar medium 9

AGB(M)

AGB(S)

AGB(C)

OB

RSG

LBV

WCL

Novae

SN

gas

ca

rb

on

d

u

st

silica

te

d

u

st

p

ec

u

liar

d

u

st

-10�8 10�7 10�6 10�5 10�4 10�3

Fig. 2.3. Dust production and gas mass return rate by di↵erent stellar types in solarmasses per year and kpc�2 in the galaxy at the solar cycle. Stars produce mainlysilicate or carbon dust; only in some cases a di↵erent kind of dust material is formed,probably iron or some iron alloy (peculiar dust). Many additional dust componentswith much smaller abundance are formed in most cases (Data from Tielens 1999;Zhukovska et al. 2008). Abbreviations of stellar types: AGB = Asymptotic GiantBranch stars of spectral types M, S, or C, OB = massive stars of spectral typesO and B on or close to the main sequence, RGB = massive stars on the RedGiant Branch, LBV = Luminous Blue Variables, WCL = Wolf-Rayet stars fromthe lower temperature range, Novae = mass ejecta from Novae, SN = mass ejectafrom SuperNovae.

fresh matter from intergalactic space (see Matteucci 2007, for more details

on the matter cycle). Presently the turn–around time of matter between

stars and the ISM in the solar vicinity of the Milky Way is of the order of

2.5Gyr, as follows from a local surface density of the ISM of 10±3 M� pc�2

(e.g. Dickey 1993) and a local star formation rate of 4± 1.5 M�Gyr�1 pc�2

(e.g. Rana 1991).The returned mass from the many di↵erent stellar sources is mixed on

rather short timescales with the interstellar matter by turbulent flows. The

result is an interstellar material with rather homogeneous elemental com-

2.1 Dust in the interstellar medium 9

AGB(M)

AGB(S)

AGB(C)

OB

RSG

LBV

WCL

Novae

SN

gas

ca

rb

on

d

u

st

silica

te

d

u

st

p

ec

u

liar

d

u

st

-10�8 10�7 10�6 10�5 10�4 10�3

Fig. 2.3. Dust production and gas mass return rate by di↵erent stellar types in solarmasses per year and kpc�2 in the galaxy at the solar cycle. Stars produce mainlysilicate or carbon dust; only in some cases a di↵erent kind of dust material is formed,probably iron or some iron alloy (peculiar dust). Many additional dust componentswith much smaller abundance are formed in most cases (Data from Tielens 1999;Zhukovska et al. 2008). Abbreviations of stellar types: AGB = Asymptotic GiantBranch stars of spectral types M, S, or C, OB = massive stars of spectral typesO and B on or close to the main sequence, RGB = massive stars on the RedGiant Branch, LBV = Luminous Blue Variables, WCL = Wolf-Rayet stars fromthe lower temperature range, Novae = mass ejecta from Novae, SN = mass ejectafrom SuperNovae.

fresh matter from intergalactic space (see Matteucci 2007, for more details

on the matter cycle). Presently the turn–around time of matter between

stars and the ISM in the solar vicinity of the Milky Way is of the order of

2.5Gyr, as follows from a local surface density of the ISM of 10±3 M� pc�2

(e.g. Dickey 1993) and a local star formation rate of 4± 1.5 M�Gyr�1 pc�2

(e.g. Rana 1991).The returned mass from the many di↵erent stellar sources is mixed on

rather short timescales with the interstellar matter by turbulent flows. The

result is an interstellar material with rather homogeneous elemental com-

AGBs (M)

(S)

(C)

OB

LBV

WCL

Novae

RSG

SNe

-8 -7 -6 -5 -4 -3 log MSun [kpc-1 y-1]

Gail & Hoppe (2010)

AGBs

PP

dis

ks

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Stars

SNe II SNe Ia

Interstellar Medium

Molecular Clouds

AGBs

PP

dis

ks

・・・・・・

・・

Evolvedstar

Dustformation

Acceleration

Mass-losswind

Material

SupplyRate

Dust: Key for the Galactic Chemical Evolution

Material Circulation in the Galaxy

Page 5: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Stars

SNe II SNe Ia

Interstellar Medium

Molecular Clouds

AGBs

PP d

isk

s

Dust: Building block of planets

Material Circulation in the Galaxy

Page 6: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

AA48CH02-Henning ARI 23 July 2010 15:10

20 30 40

20 30 40! (μm)

1.0

0.8

0.6

0.4

0.2

0

200

150

100

50

0

1.0

0.8

0.6

0.4

0.2

0

Forsterite

Enstatite

M.A

.C. *

B(1

00 K

)Fl

ux (

Jy)

M.A

.C. *

B(1

00 K

)

Figure 6Comparison of thecontinuum-subtractedspectrum of the objectAFGL 4106 with themass absorptioncoefficient of forsterite( purple line) andenstatite grains (redline) multiplied by aPlanck curve of 100 Kand normalized to 1.AFGL 4106 is adouble-linespectroscopic binary;the warmercomponent is likely apost-Red-Supergiant.After Jager et al.(1998).

They were generally attributed to amorphous silicates and could be well fitted with laboratorydata for amorphous silicates with olivine-type stoichiometry (e.g., Dorschner et al. 1995). Theobserved “amorphous” bands show a considerable variety of band positions and shapes, indicatingdifferent grain sizes, morphology, and chemical composition.

The Infrared Space Observatory (ISO) with its two spectrometers, covering a wavelength rangebetween 2 and 200 µm, led to breakthroughs in the characterization of AGB star spectra. Finally,the fingerprint spectra of cold crystalline sillicates could be detected (Waters et al. 1996). A forest ofnarrow features in the wavelength range between 20 and 70 µm could be attributed to olivines andpyroxenes ( Jager et al. 1998; Molster, Waters & Tielens 2002a). The analysis of the band positions,especially the 69-µm olivine band and the 40.5-µm pyroxene band, clearly indicates that thecrystalline silicates are Fe-poor and Mg-rich in composition (see Figure 6). The relative abundanceof crystalline silicates is in general quite modest (10%–15%), but sources with disk-like geometryoften show very strong bands owing to crystalline silicates (Molster, Waters & Tielens 2002a). Thecrystalline silicates are in general colder than the amorphous silicates, indicating that amorphoussilicates contain some Fe, leading to higher near-IR absorptivity (Molster et al. 2002b). This“dirtiness” of the amorphous silicates ( Jones & Merrill 1976) could be produced by Fe within the

30 Henning

Annu. R

ev. A

stro

. A

stro

phys.

2010.4

8:2

1-4

6. D

ow

nlo

aded

fro

m w

ww

.annual

revie

ws.

org

by U

niv

ersi

ty o

f T

okyo o

n 0

5/0

1/1

1. F

or

per

sonal

use

only

.

InfraredSpectroscopy

wavelength (micron)20 30 40

Flu

x (J

y)M

AC

* B

(100

K)M

AC

* B

(100

K)

AFGL4106

Forsterite

Enstatite

Presence of crystalline Mg-silicates

Astromineralogy

Jäger+ (1998)

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AA48CH02-Henning ARI 23 July 2010 15:10

They actually are thought to contain the most pristine material in the Solar System. Similarto cold crystals in protoplanetary disks, they must have formed through condensation and/orannealing processes together with transport processes, leading to an enhancement of the outerSolar System with crystalline silicates. We note that cometary silicate spectra show some diversitywith clear differences between Jupiter-family comet dust and dust in Oort-family comets (Kelley& Wooden 2009). Interestingly, the analysis of particles, returned by the Stardust mission fromcomet 81P/Wild 2, showed in the majority of cases the presence of olivine (Zolensky et al. 2006).The typical sizes range from submicrometer to over 10 µm with a wide compositional range inMg/(Mg+Fe) ratios.

Here, we note that HD 100456 is the only source among the observed Herbig Ae/Be starswhere the 69-µm olivine band could be detected through ISO observations, which then allowed aclear determination of the Fe content and provided direct evidence for Fe-poor forsterite grains.However, also the shorter wavelength bands, especially in high S/N Spitzer spectra, point to alow Fe content in the crystalline silicates and can be well fitted by enstatite and forsterite ( Juhaszet al. 2010, Watson et al. 2009). In HD 100456 the abundance of forsterite increases with diskradius (Bouwman et al. 2003), which is not expected in the present generation of one-zone diskdust chemistry models (Bockelee-Morvan et al. 2002, Wehrstedt & Gail 2002, Gail 2004).

Bouwman et al. (2003) speculated about the possibility of a local production of small forsteritegrains as the result of a collisional destruction process of a larger parent body as an explanationfor the strong crystal bands in HD 100456. A very similar spectrum with a very large crystallinityfraction has meanwhile been observed with Spitzer for the M-type star RECX5 (age about 8 Myr)(Bouwman et al. 2010; see Figure 8). Both objects share similar disk structures and composition,

5 10 15 20 25 30 35

! (μm)

0.00

0.02

0.04

0.06

0.08

Flu

x (J

y)

Hale-Bopp

Forsterite

RECX5

Figure 8Comparison of thespectrum of the diskaround the M-type starRECX5 (red line) andthe scaled emission ofthe comet Hale-Bopp(blue line) (Crovisieret al. 1997). Thepurple lower line is anemission spectrum fora distribution ofhollow forsteritespheres (compactequivalent radius of0.1 µm) at 200 K. AfterBouwman et al. (2010).

34 Henning

Annu. R

ev. A

str

o. A

str

ophys. 2010.4

8:2

1-4

6. D

ow

nlo

aded f

rom

ww

w.a

nnualr

evie

ws.o

rgby U

niv

ers

ity o

f T

okyo o

n 0

5/0

1/1

1. F

or

pers

onal

use o

nly

.

InfraredSpectroscopy

wavelength (micron)5 10 15 20 25 30 35

Flu

x (J

y)

REX5

Forsterite

Presence of crystalline Mg-silicates

Bouwman+ (2010)

Astromineralogy

Page 8: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

How did dust particles form in space?

Grain size, number density, mineral assemblages

Krot+ (2004)

Dust formation from gas

Nucleation and Growth

Page 9: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Grain size, number density, mineral assemblages

Krot+ (2004)

Dust formation from gasIf only a fraction

of gas condense,If all the colliding

gas condense,

slower growth

less amount of dust

diversity of dust species

How did dust particles form in space?

Page 10: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Growth kinetics of dust from vapor

Fe

Fe(g) → Fe(s)

Jnet =√ 2π mFekT

αc pFe – αe pFe(eq)

Jin

Jout

Jnet = Jin – Jout

αc : Condensation coefficient (Sticking probability of impinging atoms/molecules)

αe : Evaporation coefficient

Laboratory

Studies !

Page 11: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Evaporation experiments of minerals

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Evaporation experiments at low pressures

- Forsterite (Mg2SiO4): Hashimoto, 1990; Nagahara & Ozawa, 1996; Tsuchiyama+, 1999; Wang+, 1999; Kuroda & Hashimoto, 2002; Yamada+, 2006; Takigawa+, 2009; Ozawa+, 2012

- Olivine ((Mg0.9 Fe0.1)2SiO4): Ozawa & Nagahara, 2000

- Enstatite (MgSiO3): Tachibana+, 2002

- Silica (SiO2): Young+, 2002

- Silicate melts: e.g., Hashimoto, 1983; Nagahara & Ozawa, 1996;

Wang+, 2001; Yu+, 2003; Richter+, 2002, 2007

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Evaporation experiments at low pressures

- Forsterite (Mg2SiO4): Hashimoto, 1990; Nagahara & Ozawa, 1996; Tsuchiyama+, 1999; Wang+, 1999; Kuroda & Hashimoto, 2002; Yamada+, 2006; Takigawa+, 2009; Ozawa+, 2012

- Metallic iron : Tsuchiyama & Fujimoto, 1995; Tachibana+, 2011

- Troilite (FeS): Tachibana & Tsuchiyama, 1998

- Corundum (Al2O3): Takigawa, 2012, Ph.D. thesis

Page 14: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Evaporation experiments at low pressures

he

ate

r

thermocouple

H2 gas

continuous evacuation

vacuum gauge

ele

ctr

od

e

sampleWeight loss of sample due to isothermal heating in vacuum or at low hydrogen pressures

→ Evaporation rate

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Evaporation of Fe metal in vacuum

αe =1

Tachibana+ (2011) ApJ

1718 K 1347 K

Ideal evaporation

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Evaporation of forsterite at low hydrogen pressures

No. 1, 2009 ANISOTROPIC EVAPORATION OF FORSTERITE AND ITS EFFECTS ON IR SPECTRA L99

(a) (b) (c) (d)

Figure 2. Evaporation rates of forsterite along the three crystallographic axes in hydrogen gas. Evaporation rates in the vacuum are also plotted at 10!4 Pa forcomparison. Open circles, squares, and triangles represent average evaporation rates along the a-, b-, and c-axes, respectively, which were obtained by averagingmultiple experiments at the same conditions. The 2! standard deviation for multiple experiments is shown as an error bar. Solid and dashed curves are 1/10 and 1/100of the ideal maximum evaporation rates calculated from equilibrium vapor pressures and the kinetic theory of gases. (a) 1657"C, (b) 1535"C, (c) 1327"C, (d) 1153"C.

while that is Vc > Va # Vb at pH2 > 0.2 Pa (Figure 2(b)). Theanisotropy in the vacuum at these temperatures is consistent withprevious experiments (Ozawa et al. 1996; Yamada et al. 2006).

At 1327"C, Vb is larger than Va, and the anisotropy resultsin Vc > Vb > Va at pH2 = 0.2 Pa and Vb # Vc > Va

at pH2 = 2 Pa (Figure 2(c)). Vb is largest at 1153"C, andthe observed anisotropy is Vb > Vc # Va (Figure 2(d)).The anisotropy of forsterite evaporation in hydrogen gas issummarized as follows. (1) The anisotropy changes dependingboth on temperature and on pH2. (2) Temperature dependenceis more significant than pH2 dependence. (3) Vc is largest andVb is smallest at higher temperatures (1657 and 1535"C), whileVb is largest and Va is smallest at lower temperatures (1327and 1153"C). The temperature dependence of anisotropy andthe difference in anisotropy between that in hydrogen gas andthat in a vacuum may be explained by different thermodynamicand kinetic effects on surface structures and processes on anatomistic scale, details of which will be reported elsewhere.

4. IMPLICATION FOR A CRYSTALLOGRAPHICALLYANISOTROPIC SHAPE AND INFRARED SPECTRA

The experimental results indicate that circumstellar forsteritechanges its crystallographically anisotropic shape through evap-oration and that the crystallographic axis ratios (a/b, b/c, andc/a) can represent heating conditions because anisotropy inevaporation rates depends on temperature and hydrogen gaspressure. The change in crystallographically anisotropic shapeby evaporation at various temperatures and durations was eval-uated based on the present experimental results assuming aninitially spherical grain. We show the results of hydrogen pres-sure of 2 Pa as a typical value of protoplanetary disks (e.g.,Gail 2004). A sphere becomes a rod-like shape along the b-axis at temperature above #1600"C, a pancake-like shape alongthe c-axis at #1600 > T > 1400"C, a rod-like shape along thea-axis at 1400 > T > 1200"C, and a pancake-like shape alongthe b-axis below 1200"C. A grain elongated along the c-axisis hardly formed through evaporation, because the evaporation

rate along the c-axis is always larger than those along the a-and/or b-axes. If forsterite grains elongated along the c-axisare observed in circumstellar environments, they should not beformed by evaporation from a spherical grain but may suggestcondensation origin as formed in the condensation experimentsby Tsuchiyama (1998).

We then calculated IR spectra of forsterite corresponding tothe change in the crystallographically anisotropic shape pro-duced by evaporation at various conditions. A mass absorptioncoefficient for forsterite at 100 K, which was assumed to be ini-tially a sphere and evaporated at higher temperatures by 90 vol%,was evaluated by using a classical Lorentz vibration model inthe Rayleigh limit (Bohren & Huffman 1983; Sogawa et al.2006) with optical constants by Suto et al. (2006). A spectrumof a rod-like forsterite along the c-axis was also calculated forcomparison. Figure 3 compares the spectra of forsterite withinitially spherical grain, those evaporated at pH2 = 2 Pa and1540"C and 1150"C, respectively. The peak positions and rel-ative peak strengths vary depending on heated conditions, sug-gesting that detailed analysis of IR spectra would distinguishcrystallographically anisotropic shapes of forsterite. It furtherenables us to estimate the dust-forming conditions.

We apply the present results to the IR spectrum of proto-planetary disk, HD100546, which is reported to contain abun-dant crystalline forsterite (Malfait et al. 1998; Molster et al.2002; Bouwman et al. 2003; Lisse et al. 2007). The spectrumof HD100546 around 10 µm is mostly reproduced by the IRspectrum of grinded forsterite particles measured in laboratory(e.g., Malfait et al. 1998, Figure 4), which is presumed to be amodified CDEs (CDE2) model with quadratic weighting to em-phasize spherical grains (Fabian et al. 2001; Koike et al. 2006).As the age of HD100546 is #10 Myr, the crystalline silicatedusts in the disk may be secondarily produced by collisionaldestruction of small bodies (Bouwman et al. 2003), which arelikely to have a shape distribution similar to the CDE2 model.

The laboratory spectrum of forsterite, however, does notexplain the existence of double peaks at 10.1 and 11.2 µmeven if the effects of the present dust temperature and chemical

αe =

0.01

αe =

0.1

αe =0.01

αe =

0.1

1930 K 1803 K 1600 K 1430 K

αe =

0.1

αe =

0.1

Takigawa+ (2009) ApJLP(H2) [Pa]

Eva

po

ratio

n ra

te [

m/s

]circle: along the a-axis

square: along the b-axistriangle: along the c-axis

Anisotropic evaporation

w/ kinetic hindrance

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Evaporation coefficients

mineral αe references

corundum 0.1-0.01 Takigawa (2012, PhD thesis)

forsterite 0.1–0.01 e.g., Tsuchiyama+ (1998); Yamada+ (2006); Takigawa+ (2009)

enstatite 0.1 (as Fo) Tachibana+ (2002)

Metallic Fe 1–0.6 Tsuchiyama & Fujimoto (1995)Tachibana+ (2011)

troilite 0.1–10-3 Tachibana & Tsuchiyama (1998)

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Condensation experiments of minerals

Growth at low pressures

- good for understanding

kinetics if experimental

conditions are controlled

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he

ate

r

continuous evacuation

vacuum gauge

ele

ctr

od

e

gas source (Fe)

Growth of metallic

iron at controlled

T and PFe

substrate (Al2O3)@1235, 1340 K

Condensation of metallic iron in vacuum(Tachibana+, 2011)

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Condensation of metallic iron in vacuum

The Astrophysical Journal, 736:16 (8pp), 2011 July 20 Tachibana et al.

Figure 3. Secondary electron images of the surface (a) and the cross section (b)of metallic iron condensed at 1235 K for 48 hr.

-0.035

-0.03

-0.025

-0.02

-0.015

-0.01

-0.005

0

0.005

0 10 20 30 40 50 60

wei

ght c

hang

e (g

)

hour

Tsub

=1235 K

Tsource

=1630 K

Figure 4. Weight loss of metallic iron (gas source) due to evaporation at 1630 Kand the weight gain of the alumina substrate (1235 K) due to the condensationof metallic iron. The steady weight changes of the source and the substrateyield the incoming flux of iron onto the substrate and the condensation flux ofmetallic iron on the substrate, respectively.

atoms to break bonds with adjacent atoms, and condensationof incident metal atoms is also easier on a surface with manykink sites. The surface roughness (number of kinks), which thusaffects the kinetic hindrances for evaporation and condensation,may be reduced near equilibrium, where the number of atomsbreaking bonds at kink sites is balanced by the number of

0

5

10

15

20

0

0.2

0.4

0.6

0.8

1

-5 -4 -3 -2 -1 0 1 2 3 4 5Distance from the center (mm)

Direct incom

ing fluxThi

ckne

ss ( µ

m)

Figure 5. Thickness of condensed metallic iron (1235 K for 48 hr), shown inFigure 3, plotted against the distance from the center of the substrate (solidcircles). Error bars represent the standard deviations of the means. The spatialvariation of the direct incoming flux onto the substrate predicted by the fluxdistribution of vapor emerging from the tube (5.9 mm in diameter; Dayton1956), which is normalized to the flux at the center of the substrate, is alsoshown (dashed curve).

atoms being incorporated into the crystalline lattice, as longas the temperature of the surface is lower than the thermalroughening temperature. The kinetic hindrance for condensationis therefore expected to be larger near equilibrium than underlower saturation conditions.

k seems to have a weak temperature dependence; however,the mean value of k is !0.54 ± 0.15 (1! ). Thus, "e and "c atundersaturation (0 ! S <1) can empirically be expressed by

"e = "c = exp(1.44 ! 2595/T ) ! 0.54(p/peq)(p/peq < 1)(4)

over the temperature range from 1720 to 1350 K. The evap-oration rates calculated using Equation (4) are also shown inFigure 2.

4.2. Condensation Kinetics of Metallic Iron

A supersaturation ratio S (p/peq) at the surface of the substratewas calculated based on the direct incoming flux of iron onto thesubstrate that could be estimated from the flux distribution ofvapor emerging from the tube under molecular flow conditions(Dayton 1956) and the measured evaporation rate of the irongas source. The fraction of the flux onto the substrate relativeto the total evaporation flux of metallic iron from the tubewas calculated to range from 0.11 to 0.34 depending onthe distance between the substrate and the outlet of the tube.Note that the usage of the tube has the effect of focusinggas flux from the tube outlet (Dayton 1956) and that theestimated fraction of the flux onto the substrate against the totalevaporation flux here is much larger than that in the case withoutthe tube.

There might have been other indirect fluxes of iron ontothe substrate, which hit the substrate after colliding with theheat shields, and if they were present, the incoming flux ontothe substrate would be underestimated. However, the thicknessvariation of the condensed metallic iron layer agrees well withthe predicted spatial variation of direct flux onto the substrate(Figure 5), suggesting that the incoming flux of iron wasdominated by the direct flux from the outlet of the tube becausethe indirect iron gas flux would come from random directionsand its spatial variation would be uniform. We also found thatcondensation of metallic iron occurred on the molybdenum plateused to hold the Al2O3 substrate and on the heat shields at the

5

weight loss of gas source due to evaporation

weight gain of substrate due to condensation

Tachibana+ (2011)

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Condensates

Photo:

Growth steps on Fe metal condensed from vapor at 1235 K for 48 hr

1 micron

Tachibana+ (2011)

Page 22: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Condensates

Photo:

Growth steps on Fe metal condensed from vapor at 1235 K for 48 hr

1235 K, 48 hr

1 micron

Tachibana+ (2011)

Page 23: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

0

10

20

30

40

50

5 10 15 20 25 30 35 40

1235 K

1337 K

!=1

!=0.8

!=0.6

!=0.4

!=0.2

J con

d /

Jid

evap

(0)

Idealcondensation

1510 K 1630 K

Tgas

:1580 K

1580 K

!=0.4

1680 K1580 K

1680 K

Supersaturation ratio, S (=p/peq

)

αc=1

Tachibana+ (2011)

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Evaporation & Condensation coefficients

mineral αe αc

corundum 0.1-0.01 ~0.05 (Takigawa, 2012)

forsterite 0.1–0.01

enstatite 0.1 (as Fo)

Metallic Fe 1–0.6 ~1 (Tachibana+, 2011)

troilite 0.1–10-3 ~0.02

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Condensation of forsterite in low-pressure H2-H2O gas

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Evaporation of forsterite

Mg2SiO4(s) = 2Mg(g) + SiO(g) + 3O(g)

Free evaporation regime (FED)

Mg2SiO4(s) + 3H2(g) = 2Mg(g) + SiO(g) + 3H2O(g)

Hydrogen-reaction dominated regime (HRD) – Jevap proportional to pH2

1/2

pH2O/pH2-buffer dominated regime (HBD) – Jevap proportional to pH2O/pH2

Hashimoto (1990); Wang+ (1999); Yamada+ (2006); Takigawa+(1999); Ozawa+ (2012)

Nagahara & Ozawa (1996); Tsuchiyama+ (1998); Kuroda & Hashimoto (2002); Takigawa+ (2009)

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Tsuchiyama, Tachibana, Takahashi (1999)

Evaporation of forsterite

1573 K

1473 K

1373 K

1273 K

1173 K

2073 K1973 K1873 K1773 K1673 K

FED

HRD

HBD

solar composition α =1

Page 28: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

H2+H2Ohalogen lamp

gold mirror

vacuum gauge

Forsterite QMS

TMP+RP

continuous evacuation

Infrared vacuum furnace

Evaporation of forsterite in low-pressure H2-H2O gas

Pt mesh

silica tube

Page 29: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Evaporation of forsterite in low-pressure H2-H2O gas

ptotal=4x10-5 atm, T~1150°C (1423 K)

H2O/H2=0.0015

H2O/H2=0.016

Page 30: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Evaporation of forsterite in low-pressure H2-H2O gas

ptotal=4x10-5 atm, T~1150°C (1423 K)

HRD

HBD

αe=1

αe=0.1

αe=0.01

Page 31: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Evaporation of forsterite

confirmed for the first time

Mg2SiO4(s) = 2Mg(g) + SiO(g) + 3O(g)

Free evaporation regime (FED)

Mg2SiO4(s) + 3H2(g) = 2Mg(g) + SiO(g) + 3H2O(g)

Hydrogen-reaction dominated regime (HRD) – Jevap proportional to pH2

1/2

pH2O/pH2-buffer dominated regime (HBD) – Jevap proportional to pH2O/pH2

Hashimoto (1990); Wang+ (1999); Yamada+ (2006); Takigawa+(1999); Ozawa+ (2012)

Nagahara & Ozawa (1996); Tsuchiyama+ (1998); Kuroda & Hashimoto (2002); Takigawa+ (2009)

Page 32: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Evaporation of forsterite in low-pressure H2-H2O gas

Page 33: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

gas source:Forsterite

substrate:Forsterite~25 mm

Condensation of forsterite in low-pressure H2-H2O gas

~1% of gas evaporated from the gas source

~1900 K

Pressure: 4 Pa

H2O/H2=0.016Pt mesh

Page 34: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Condensation coefficient

#1 #2 #3 #4

Flux condensed on the substrate

Flux hitting the substrate surface

αc ≤ 0.08-0.17

1070 min 1250 min 790 min 1530 min

Tcond = ~1350 K

SiO/H2 = ~0.15 solar

H2O/H2 = ~16 solar

S = ~5

Page 35: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Evaporation & Condensation coefficients

mineral αe αc

corundum 0.1-0.01 ~0.05 (Takigawa, 2012)

spinel ~0.02

forsterite 0.1–0.01 ~0.1?

enstatite 0.1 (as Fo)

Metallic Fe 1–0.6 ~1 (Tachibana+, 2011)

troilite 0.1–10-3 ~0.02Growth (and evaporation)

of forsterite dust occurs less

efficiently than Fe metal

Page 36: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Application to cosmochemistry

Grain size, number density, mineral assemblages

Krot+ (2004)

AOA Formation

Page 37: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

0

4x103

8x103

1.2x104

9 10 11 12 15 17

CDE

LDE 2LDE 1

LDE 3

MA

C (c

m2 /

g)wavelength (�m)

16

HD100546 (Juhász et al. 2010)

25% LDE1 + 75% CDElaboratoryDHS

Takigawa & Tachibana, 2012

Anisotropy:

Probe for

high-T history

of dust

evap.

cond.

Application to infrared spectroscopy

Page 38: Vapor growth/evaporation of Mg-silicate under …cps/pub/seminar/fy2012/2013-03...2013/03/06  · Evaporation rates of forsterite along the three crystallographic axes in hydrogen

Summary &Conclusions

Understanding of dust formation kinetics is a key to understand dust forming environments

— experiments at controlled low-pressure “realistic” conditions combined with observation and modeling

Evaporation of forsterite controlled by pH2O/pH2 is confirmed; Kinetics is likely to be the same

Growth experiments of forsterite under controlled protosolar disk-like conditions are now being made; The growth efficiency is not as good as metallic iron