Nuclear phase coherence excitation mechanisms

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. 

Use of a surfactant allows solubilization of the polyoxometalate cluster K6[Vi5As6042(H20)] 8H20 (V15) in the organic solvent chloroform. Spin echo measurements revealed a phase memory time of Tm = 340 ns, which was attributed to resonances in the 5 = 3/2 excited state of the cluster [166]. No quantum coherence was detected in the pair of 5 = 1/2 ground states [151]. By measurement of the z-magnetization after a nutation pulse, and a delay to ensure decay of all coherences, Rabi oscillations were observed. From the analysis of the different possible decoherence mechanisms, it was concluded that decoherence is almost entirely caused by hyperfine coupling to the nuclear spins. 

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