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Analytic Solution
Continuous Spectrum
Dynamic Range
Exponential Decay
Optical Pumping
Oscillations
Quantum Dynamics
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New mechanism for nontrivial intramolecular vibrational dynamics
New mechanism for nontrivial intramolecular vibrational dynamics,10.1140/epjd/e2009001865,European Physical Journal D,V. A. Benderskii,E. I. Kats
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New mechanism for nontrivial intramolecular vibrational dynamics
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V. A. Benderskii
,
E. I. Kats
We investigate the time evolution process of one selected (initially prepared by optical pumping) vibrational molecular state S, coupled to all other intramolecular vibrational states R of the same molecule, and also to its environment Q. Molecular states forming the first reservoir R are characterized by a discrete dense spectrum, whereas the environment reservoir Q states form a continuous spectrum. Assuming the equidistant reservoir R states we find the exact analytical solution of the quantum dynamic equations. SQ and RQ couplings yield to spontaneous decay of the S and R states, whereas SR exchange leads to recurrence cycles and Loschmidt echo at frequencies of SR transitions and double resonances at the interlevel reservoir R transitions. Due to these couplings the system S time evolution is not reduced to a simple exponential relaxation. We predict various regimes of the system S dynamics, ranging from
exponential decay
to irregular damped oscillations. Namely, we show that there are possible four dynamic regimes of the evolution: (i) independent of the environment Q
exponential decay
suppressing backward R  S transitions, (ii) Loschmidt echo regime, (iii) incoherent dynamics with multicomponent Loschmidt echo, when the system state is exchanged its energy with many states of the reservoir, (iv) cycle mixing regime, when long time
system dynamics
looks as a randomlike. We suggest applications of our results for interpretation of femtosecond vibration spectra of large molecules and nanosystems.
Journal:
European Physical Journal D  EUR PHYS J D
, vol. 54, no. 3, pp. 597605, 2009
DOI:
10.1140/epjd/e2009001865
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