Influence of surface morphology on D2 desorption kinetics from amorphous solid water -: art. no. 124701

被引:70
作者
Hornekær, L
Baurichter, A
Petrunin, VV
Luntz, AC
Kay, BD
Al-Halabi, A
机构
[1] Univ So Denmark, Dept Phys, DK-5230 Odense, Denmark
[2] Pacific NW Natl Lab, Fundamental Sci Directorate, Div Chem Sci, Richland, WA 99352 USA
[3] Gorlaeus Labs, Leiden Inst Chem, NL-2300 RA Leiden, Netherlands
关键词
D O I
10.1063/1.1874934
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The influence of surface morphology/porosity on the desorption kinetics of weakly bound species was investigated by depositing D-2 on amorphous solid water (ASW) films grown by low temperature vapor deposition under various conditions and with differing thermal histories. A broad distribution of binding energies of the D-2 monolayer on nonporous and porous ASW was measured experimentally and correlated by theoretical calculations to differences in the degree of coordination of the adsorbed H-2 (D-2) to H2O molecules in the ASW depending on the nature of the adsorption site, i.e., surface valleys vs surface peaks in a nanoscale rough film surface. For porous films, the effect of porosity on the desorption kinetics was observed to be a reduction in the desorption rate with film thickness and a change in peak shape. This can be partly explained by fast diffusion into the ASW pore structure via a simple one-dimensional diffusion model and by a change in binding energy statistics with increasing total effective surface area. Furthermore, the D-2 desorption kinetics on thermally annealed ASW films were investigated. The main effect was seen to be a reduction in porosity and in the number of highly coordinated binding sites with anneal temperature due to ASW restructuring and pore collapse. These results contribute to the understanding of desorption from porous materials and to the development of correct models for desorption from and catalytic processes on dust grain surfaces in the interstellar medium.
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页数:11
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共 59 条
[1]   Adsorption of CO on amorphous water-ice surfaces [J].
Al-Halabi, A ;
Fraser, HJ ;
Kroes, GJ ;
van Dishoeck, EF .
ASTRONOMY & ASTROPHYSICS, 2004, 422 (03) :777-791
[2]   Sticking of CO to crystalline and amorphous ice surfaces [J].
Al-Halabi, A ;
van Dishoeck, EF ;
Kroes, GJ .
JOURNAL OF CHEMICAL PHYSICS, 2004, 120 (07) :3358-3367
[3]  
Allen M. P., 1987, J COMPUTER SIMULATIO, DOI DOI 10.2307/2938686
[4]   Effect of porosity on the adsorption, desorption, trapping, and release of volatile gases by amorphous solid water [J].
Ayotte, P ;
Smith, RS ;
Stevenson, KP ;
Dohnálek, Z ;
Kimmel, GA ;
Kay, BD .
JOURNAL OF GEOPHYSICAL RESEARCH-PLANETS, 2001, 106 (E12) :33387-33392
[5]   TRAPPING AND RELEASE OF GASES BY WATER ICE AND IMPLICATIONS FOR ICY BODIES [J].
BARNUN, A ;
HERMAN, G ;
LAUFER, D ;
RAPPAPORT, ML .
ICARUS, 1985, 63 (03) :317-332
[6]   AMORPHOUS WATER ICE AND ITS ABILITY TO TRAP GASES [J].
BARNUN, A ;
DROR, J ;
KOCHAVI, E ;
LAUFER, D .
PHYSICAL REVIEW B, 1987, 35 (05) :2427-2435
[7]   A theory of water and ionic solution, with particular reference to hydrogen and hydroxyl ions [J].
Bernal, JD ;
Fowler, RH .
JOURNAL OF CHEMICAL PHYSICS, 1933, 1 (08) :515-548
[8]   IDENTIFICATION OF 2 DISTINCT STRUCTURAL AND DYNAMIC DOMAINS IN AN AMORPHOUS WATER CLUSTER [J].
BUCH, V .
JOURNAL OF CHEMICAL PHYSICS, 1990, 93 (04) :2631-2639
[9]   STICKING PROBABILITY OF H AND D ATOMS ON AMORPHOUS ICE - A COMPUTATIONAL STUDY [J].
BUCH, V ;
ZHANG, Q .
ASTROPHYSICAL JOURNAL, 1991, 379 (02) :647-652
[10]   SPECTRA OF DANGLING OH BONDS IN AMORPHOUS ICE - ASSIGNMENT TO 2-COORDINATED AND 3-COORDINATED SURFACE MOLECULES [J].
BUCH, V ;
DEVLIN, JP .
JOURNAL OF CHEMICAL PHYSICS, 1991, 94 (05) :4091-4092