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Journal Articles

Time-resolved CARS study of molecular vibrational dissipation and dephasing in solid phase

Kumada, Takayuki; Karavitis, M.*; Goldschleger, I. U.*; Apkarian, V. A.*

Hoshasen Kagaku, (79), p.30 - 35, 2005/03

We should know how the high energy deposited by irradiation dissipates in materials in order to understand radiation chemical processes. In this study, we carried out TR-CARS (Time-Resolved Coherent Anti-Stokes Raman Scattering) study of molecular iodine in solid krypton to understand the mechanism of vibrational relaxation in solid phase. Decoherence of the vibrational state is due to energy dissipation below 10 K whereas pure dephasing plays an important role above. We also found that the dephasing is due to the scattering with local phonon mode with the energy of 40 K.

Journal Articles

Vibrational dissipation and dephasing of I$$_{2}$$(v = 1-19) in solid Kr

Karavitis, M.*; Kumada, Takayuki; Goldschleger, I. U.*; Apkarian, V. A.*

Physical Chemistry Chemical Physics, 7(5), p.791 - 796, 2005/02

 Times Cited Count:30 Percentile:69.48(Chemistry, Physical)

Energy dissipation and phase relaxation of the vibrational quantum states of iodine molecules in solid krypton have been studied in the temperature range between 7 and 45 K using a technique of time-resolved coherent anti-stokes Raman scattering (CARS) spectroscopy by a femto-second laser. The rate of energy dissipation was independent of tempeature, but proportional to the vibrational quantum number v. The pure dephasing rate exponentially increased with an increase in temperature and was proportional to v$$^{2}$$. The energy relaxation was found to take place by transfering the vibrational energy of iodine to four phonons in the krypton solid. The pure dephasing was induced by elastic scattering with phonon. It was suggested by a computer simulation that the phonon which induced the pure dephasing accompanied libration mode of iodine molecules.

Oral presentation

Time-resolved CARS study of vibrational coherence in solid phase

Kumada, Takayuki; Karavitis, M.*; Goldschleger, I.*; Apkarian, A.*

no journal, , 

We studied time-resolved CARS study of vibrational coherence in solid phase using iodine molecules in solid krypton. We observed the vibrational coherence of iodine molecules for 200 ps corresponding to about 1000 oscillations at 7 K. The rate of decoherence increases with increasing temperature and the number of vibrational quantum state.

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