Energy Redistribution in I2-(CO2)n Collision on Silicon Surface

Yasumatsu, Hisato; Koizumi, Shi N.Ichi; Terasaki, Akira; Kondow, Tamotsu

doi:10.1021/jp982234z

Cited by 21 publications

(10 citation statements)

References 39 publications

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“…In particular, I 2 Ϫ has been studied in a wide variety of environments, including gas phase clusters, [3][4][5][6][7][8][9][10][11][12] liquid solutions, [13][14][15][16][17][18][19][20][21] and gas-surface collisions, [22][23][24][25] and these experiments have stimulated a variety of theoretical studies. These solvated molecular ions differ considerably from their neutral counterparts, since the interaction between the ion and the surrounding solvent, which can be as strong as the chemical bonding forces within the solute, depends sensitively on the solute charge distribution.…”

Section: Introductionmentioning

confidence: 99%

Simulation of UV photodissociation of I2−(CO2)n: Spin-orbit quenching via solvent mediated electron transfer

Delaney

Faeder

Parson

1999

The Journal of Chemical Physics

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We simulate the 395 nm photodissociation of I2− embedded in clusters of 6 to 22 CO2 molecules. In the isolated molecule, photodissociation at this wavelength leads exclusively to spin-orbit excited iodine (I*) plus I−. In the larger clusters we observe efficient electronic relaxation, leading both to dissociated products containing ground-state iodine and to recombined products containing I2−. The time scale and cluster size dependence of the spin-orbit quenching process agree well with experimental determinations of Sanov et al. (companion paper). The simulation trajectories show that spin-orbit quenching occurs by resonant charge transfer from solvated I− to a nascent I* atom. A model derived from the theory of electron transfer reactions in solution illustrates that this resonance arises when the I spin-orbit energy is compensated by the difference between the solvation energies of the ion and the neutral.

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Section: Introductionmentioning

confidence: 99%

Simulation of UV photodissociation of I2−(CO2)n: Spin-orbit quenching via solvent mediated electron transfer

Delaney

Faeder

Parson

1999

The Journal of Chemical Physics

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“…[26][27][28][29][30]32,33,[45][46][47] Kondow and co-workers examined collisions of I 2 -(CO 2 ) n cluster ions with solid surfaces and observed the wedge effect: the solvent CO 2 molecules sandwiched between the surface and the I 2waist in a collision split the I 2bond. [48][49][50][51] Several recent studies provided theoretical background for understanding the dissociation and recombination 38 The ab initio potentials have been scaled 38 to match the experimental I2well depth. 25,39 Arrows indicate the transitions studied in this work.…”

Section: Introductionmentioning

confidence: 99%

Photodissociation of I₂^-(OCS)_n Cluster Ions: Structural Implications

et al. 1998

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We report product distributions from the photodissociation of I 2 -(OCS) n (n ) 1-26) cluster ions at 790 and 395 nm and discuss implications concerning the structure of these clusters. The experimental results are paralleled by a theoretical investigation of I 2 -(OCS) n structures. The 790 and 395 nm transitions in I 2access dissociative excited states that correlate with the I -+ I( 2 P 3/2 ) and I -+ I*( 2 P 1/2 ) products, respectively. Photoabsorption by I 2 -(OCS) n clusters at 790 nm results in "uncaged" I -(OCS) k and "caged" I 2 -(OCS) k fragments. The 395 nm excitation leads, in general, to three distinct pathways: (1) I 2dissociation on the I -+ I*( 2 P 1/2 ) spin-orbit excited asymptote, competing with the solvent-induced spin-orbit relaxation of I*( 2 P 1/2 ) followed by either (2) I 2dissociation on the I -+ I( 2 P 3/2 ) asymptote or (3) I 2recombination. Pathways 1 and 2 result in a bimodal distribution of the uncaged I -(OCS) k fragments that energetically correlate with the two spin-orbit states of the escaping I atom. The I + Icaging efficiency is determined as a function of the number of solvent OCS molecules at both excitation wavelengths studied. At 790 nm, 100% caging of I 2is achieved for n g 17. For 395 nm excitation, addition of the 17th OCS molecule to I 2 -(OCS) 16 results in a steplike increase in the caging efficiency from 0.25 to 0.68. These results suggest that the first solvent shell around I 2is comprised of 17 OCS molecules. Results of theoretical calculations of the lowestenergy I 2 -(OCS) n cluster structures support this conclusion. The roles of different dominant electrostatic moments of OCS and CO 2 in defining the I 2 -(OCS) n and I 2 -(CO 2 ) n cluster structures are discussed, based on comparison of the photofragment distributions.

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“…33 The use of cluster ions in surface impact experiments allows for size selection and better control of the collision energy, and deposition, scattering, and dissociation of cluster ions have recently been studied. [34][35][36][37] Surface deposition of size-selected clusters is also being investigated for material processing applications, including the production of high-quality thin films. 38,39 Cluster impact with high kinetic energy is known to result in electron emission and dissociative ionization of cluster components.…”

Section: Introductionmentioning

confidence: 99%

Water Cluster Collisions with Graphite Surfaces: Angular-Resolved Emission of Large Cluster Ions

Andersson

Pettersson

1998

J. Phys. Chem. B

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We present experimental studies of negative cluster ions formed during scattering of (H 2 O) n (n j e 4600) from graphite surfaces. Angular distributions are measured using surface temperatures of 1280-1450 K and an incident cluster velocity of 1380 m/s. Large cluster ions are found to be emitted in sharply peaked distributions close to the tangential direction, except for normal incidence which produces distributions that are peaked in the surface normal direction. Time-of-flight measurements, combined with energy analysis of the emitted negative ions, are used to determine the final velocity and size of the cluster ions. The clusters are concluded to conserve 65-85% of their velocity parallel to the surface plane during a surface interaction, while the velocity component in the normal direction is 75-100 m/s independent of incident angle. The clusters undergo considerable fragmentation in surface contact, and 15-25% of a cluster survives as one unit for an initial cluster size of a few thousand molecules. The experimental findings are compared with results from earlier studies, and the detailed collision dynamics and conditions under which cluster charging takes place are discussed.

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Energy Redistribution in I₂^-(CO₂)_n Collision on Silicon Surface

Cited by 21 publications

References 39 publications

Simulation of UV photodissociation of I2−(CO2)n: Spin-orbit quenching via solvent mediated electron transfer

Simulation of UV photodissociation of I2−(CO2)n: Spin-orbit quenching via solvent mediated electron transfer

Photodissociation of I₂^-(OCS)_n Cluster Ions: Structural Implications

Water Cluster Collisions with Graphite Surfaces: Angular-Resolved Emission of Large Cluster Ions

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Energy Redistribution in I2-(CO2)n Collision on Silicon Surface

Cited by 21 publications

References 39 publications

Simulation of UV photodissociation of I2−(CO2)n: Spin-orbit quenching via solvent mediated electron transfer

Simulation of UV photodissociation of I2−(CO2)n: Spin-orbit quenching via solvent mediated electron transfer

Photodissociation of I2-(OCS)n Cluster Ions: Structural Implications

Water Cluster Collisions with Graphite Surfaces: Angular-Resolved Emission of Large Cluster Ions

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Product

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Energy Redistribution in I₂^-(CO₂)_n Collision on Silicon Surface

Photodissociation of I₂^-(OCS)_n Cluster Ions: Structural Implications