Phase coherent excitation mechanisms

A second type of relaxation mechanism, the spin-spm relaxation, will cause a decay of the phase coherence of the spin motion introduced by the coherent excitation of tire spins by the MW radiation. The mechanism involves slight perturbations of the Lannor frequency by stochastically fluctuating magnetic dipoles, for example those arising from nearby magnetic nuclei. Due to the randomization of spin directions and the concomitant loss of phase coherence, the spin system approaches a state of maximum entropy. The spin-spin relaxation disturbing the phase coherence is characterized by T. ... 

The phase of the signal oscillations gives hints about the specific mechanisms leading to the coherent excitation of the modes. At the time a vibration starts, the... 

In the following, we will discuss two basic - and in a sense complementary [44] - physical mechanisms to exert efficient control on the strong-field-induced coherent electron dynamics. In the first scenario, SPODS is implemented by a sequence of ultrashort laser pulses (discrete temporal phase jumps), whereas the second scenario utilizes a single chirped pulse (continuous phase variations) to exert control on the dressed state populations. Both mechanisms have distinct properties with respect to multistate excitations such as those discussed in Section 6.3.3. 

Vibrational echo experiments permit the use of optical coherence methods to study the dynamics of the mechanical degrees of freedom of condensed phase systems. Because vibrational transitions are relatively narrow, it is possible to perform vibrational echo experiments on well-defined transitions and from very low temperature to room temperature or higher. Further, vibrational echoes probe dynamics on the ground state potential surface. Therefore, the excitation of the mode causes a minimal perturbation of the solvent. 

Since the development of ultrashort lasers, nudear wavepacket dynamics of various matters have attracted continuing attention [1,2]. The research targets extend from gas phase molecules [3, 4] to molecules in solution [5, 6], and solids [7]. In general, an excitation of matter by an ultrashort pulse with sufficient bandwidth leads to the creation of coherence between vibrational (or vibronic) eigenstates [1]. The induced nuclear wavepacket then starts to evolve on a certain potential energy surface and the dynamics is probed by a suitable pump-probe spectroscopy. The direct time-domain observation of the nudear motion provides us with valuable information on photochemical reaction dynamics, vibrational excitation/relaxation mechanisms, electron-vibration (phonon) coupling, and so on. 

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