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Vibrational coherence of I2 in solid Kr.

M Karavitis¹, V A Apkarian

¹Department of Chemistry, University of California, Irvine, California 92697-2025, USA.

The Journal of Chemical Physics

|July 23, 2004

Summary

This study uses ultrafast spectroscopy to observe molecular vibrations in solid krypton. Researchers discovered a surprising local mode that is decoupled from lattice vibrations.

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Area of Science:

Physical Chemistry
Spectroscopy
Condensed Matter Physics

Background:

Understanding molecular dynamics in solid matrices is crucial for various applications.
Solid krypton provides a unique, weakly interacting environment for studying guest molecules.
Coherent anti-Stokes Raman scattering (CARS) is a powerful technique for probing vibrational states.

Purpose of the Study:

To investigate the coherent evolution of vibrational superposition states in I2 molecules isolated in solid Kr.
To precisely characterize molecular vibrational frequencies and dephasing rates.
To explore the coupling between molecular vibrations and the surrounding matrix environment.

Main Methods:

Time-resolved coherent anti-Stokes Raman scattering (TR-CARS) with 20 fs resolution.
Preparation of broadband vibrational superposition states (nu=1-6) on the ground electronic state of I2.
Monitoring coherent evolution for up to 1000 vibrational periods at 32 K.

Main Results:

Precise molecular vibration characterization: omega(e)=211.330(2) cm(-1), omega(e)x(e)=0.6523(6) cm(-1), omega(e)y(e)=2.9(1) x 10(-3) cm(-1).
Dephasing rates show strong vibrational quantum number (nu) dependence: gamma(nu)=8.5 x 10(-3)+4.9 x 10(-4)nu2+2.1 x 10(-6)nu4 ps(-1).
Observed signal modulation at omega(q)=41.56(3) cm(-1), indicating coupling to a local mode decoupled from lattice phonons.

Conclusions:

The observed local mode's decoupling from lattice phonons challenges conventional normal-mode analysis.
This finding suggests unique energy transfer pathways in solid matrices.
Ultrafast spectroscopy provides unprecedented insight into molecule-matrix interactions.

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