Annealing of Amorphous Silicates

Laboratory Astrophysics group of the AIU Jena


Annealing is likely to occur in astrophysical environments:

· At the accretion disk stage of star formation:
Amorphous silicates (with the composition and structure inherited from the parent molecular cloud) entering an accretion disk slowly spiral inwards towards the protostar to form layers of progressively higher temperatures.
At sufficiently high temperature, diffusion processes start. This results in a conversion of the amorphous structure into an ordered lattice structure at different material-dependent temperature ranges.

· At the AGB stage of stellar evolution:
In cooling outflows of late-type red giants having an oxygen-rich elemental composition, silicates condense in a thermodynamic condensation sequence: e.g. Mg2SiO4   --> MgSiO3 --> Fe2SiO4[Tielens 1998].
 At the same time the dust is subject to the process of annealing. After particle condensation (but also at the same time), the silicates transform into the crystalline state - depending on the cooling rate of the outflow compared with the typical annealing time.


· Approach to understanding annealing processes:

1. Development of some degree of local order:
Due to thermally enhanced diffusion, the dust material gradually develops some order in the local arrangement of the atoms.
Lattice structure changes to a microcrystalline material.
Atom-size dependent diffusion leads to chemical fractionation, i.e. impurities may assemble at the surface or in inclusions.

2. Crystallization
If annealing lasts sufficiently long even crystallization may start at critical nuclei. Laboratory study reveils which kind of crystalline minerals forms from an amorphous silicate produced by laser ablation or pyrolysis.

3. Annealing time t:
Time of first indications for formation of an ordered structure. We found IR spectroscopy to be very sensitive to detect the presence of microcrystals. Therefore IR spectroscopy is used to determine activation energy and the constant w0 :

t -1 = w0 * e(-Ea/kT)

 with w0 = 2 * 1013 s-1 ... mean vibrational frequency of the  SiO4 tetrahedra,
        Ea ... activation energy of crystallization

4.  Short-range order:
 Time tanneal to form a local ordered structure of size d.

 d² = 6 D tanneal,
 D = 1/3  * a² * w0 * e(-Ea/kT) diffusion constant

Experiments indicated that silicate smoke annealed at T = 1000 K develops a local order of approx. 1 nm within one day. This can be seen fom IR spectra.
 

5. Stellar Outflows
Typical timescale for dust particle growth 107 s  (approx. 115 days).
Typical timescale for changes in the outflow temperature 108 s (approx. 3.1  years)

As model calculations of circumstellar shells around M stars proved, condensation of silicates starts at temperatures in the range of 1000 K; Mg-silicates subjected to this temperature would develop a short/long-range order of approx. 30 nm!
It can be seen from the calculated timescales that condensed silicates stay in a sufficient hot (for annealing) environment and can develop a lokal order.  The degree of crystallization of the silicates annealed in this temperature range has to be determined by laboratory study [model data from Gail & Sedlmayer 1998a].

 Annealing processes are most likely to take place in stellar outflows!



6. Protoplanetary accretion disk

·  Model: Solar-type star with accretion rate  10-7 Msun yr-1

In such a model conversion of the initially amorphous silicates into crystalline silicates starts at a distance of 1.5 AU at approx. 1000 K.
At 1 AU crystallization is completed.
With progressing crystallization a drop in opacity of the dust material could take place. This expected drop in opacity has to be proved experimentally.  [model data from Gail & Sedlmayer 1998b].

 Modelling of protoplanetary disks indicates that annealing processes have to be considered in disk dynamics!




Laboratory study:

The annealing experiments are performed in oxygen atmosphere at  1013 mbar in quarz glass box in a high temperature oven.
We focuse on the question:
Is there any difference in annealing kinetics between bulk samples and nanometer-sized samples?

1. Bulk: Thin glassy silicate splats (thickness 0.1 mm) produced by rapid cooling of a melt
2. Micrometre-sized grains: Ground splats with size-distribution 5 - 10 mm
3. Nanometer-sized grains: Magnesium silicate smoke produced by laser ablation
4. Amorphous SiO2: produced by sol-gel technique

Analytical methods:



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Last modified: Dirk Fabian, February 99