Probing Exciton Dynamics in the Frequency Domain Paul L. Raston and David T. Anderson Department of Chemistry, University of Wyoming, Laramie, WY 82071-3838.

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Presentation transcript:

Probing Exciton Dynamics in the Frequency Domain Paul L. Raston and David T. Anderson Department of Chemistry, University of Wyoming, Laramie, WY WF14 Dynamics Probed by Spectroscopy, 5:44 pm Wed, June 20 Math Annex nd International Symposium on Molecular Spectroscopy

Brief Outline Excitons in solid parahydrogen Vibrons and rovibrons in rare gas atom and halogen atom doped solid parahydrogen Probing exciton dynamics in these systems Conclusions and future directions

Vibrational excitation delocalized in solid pH Å hexagonal close-packed Q 1 (0) V(H 2 -H 2 )=V(r 1,r 2,R,  1,  2,  ) solidisolated 5 cm -1 vibron band VIBRON v,J= 0,0 1,0

Rotational excitation delocalized in solid 3.8 Å hexagonal close-packed S o (0) V(H 2 -H 2 )=V(r 1,r 2,R,  1,  2,  ) solidisolated 25 cm -1 roton band ROTON v,J= 0,0 0,2

Vibron dynamics in chemically doped solid para-H 2 Br pH Å hexagonal close-packed

Deposit crystals from the gas-phase S. Tam and M. E. Fajardo, Rev. Sci. Instrumen. 70, 1926 (1999). room temperature dopant (e.g., Br 2 ) vacuum shroud optical substrate T = 2.4 K IR beam atmosphere vacuum cryostat cold tip catalytic converter Fe(OH) 3 UV beam 355 nm

Vibrons in Rg atom doped solid para-H 2 para-H 2 Ne Ar Kr Xe Q 1 (0) V(Rg-H 2 )=V(r,R,  ) solidisolated 5 cm -1 vibron band

Vibrons in Br atom doped solid para-H 2 oH 2 Shifts are greater than for Xe Two peaks infer two different H 2 environments around Br( 2 P 3/2 ) V(Br---H 2 ) ab initio J. Klos, G. Chalasinski, and M. M. Szczesniak, JPC A 106, 7362 (2002).

Rg atom perturbed S 1 (0) rovibron band S 1 (0) V(H 2 -H 2 )=V(r 1,r 2,R,  1,  2,  ) solid v,J=0,0 v,J=1,2

Br atom perturbed S 1 (0) rovibron band Xe Br

pH 2 Study excitons using Br spin-orbit transition 1,2 2 P 3/2 2 P 1/2 h = cm -1  e =0.96 s gas-phasesolid parahydrogen Br 1.M. Fushitani, T. Momose, T. Shida, CPL 356, 375 (2002). 2.P. L. Raston and D. T. Anderson, JCP 126, (2007).

Br atom spin-orbit transition in solid para-H 2

Br spin-orbit transition induced excitons

Br spin-orbit + roton peak 25 cm -1

Br spin-orbit + vibron peak

Excitation energy above the barrier to reaction 7875 cm -1

Br spin-orbit + rovibron peak

Conclusions and future directions Inverse matrix isolation spectroscopy – use the matrix to tell you about the dopant Exciton line shapes reflect differences in atomic dopant species Exciton transitions build off Br spin-orbit transitions provide a new window into the exciton dynamics in a quantum solid Looking for theoretical collaborators to simulate exciton line shapes

Publications and funding Paul L. Raston and David T. Anderson, “Infrared-active vibron bands associated with rare gas atom dopants isolated in solid parahydrogen,” Low Temp. Phys. (in press). Paul L. Raston and David T. Anderson, “Infrared spectroscopic studies of the rare gas atom perturbed S 1 (0) rovibron band of solid parahydrogen,” JMS (in press). This research sponsored in part by the Chemistry Division of the National Science Foundation (CHE ). Sharron C. (Cassie) Kettwich 1 st year graduate student Paul L. Raston, Ph.D. 2007