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Physical Review Letters

Coherent Dynamics of the Localized Vibrational Modes of Hydrogen in CaF2

Jon‐Paul R. Wells, Chris W. Rella, Ian V. Bradley, Ian Galbraith, C. R. Pidgeon

Published May 22, 2000• 18 citations
Publisher

Abstract

We report the observation of giant quantum coherence effects in the localized modes of ionized hydrogen in synthetic fluorite. Infrared free induction decay experiments on the substitutional H- center show dramatic modulations at negative delay times due to interference between multiple vibrational levels. Spectrally resolving the degenerate four wave mixing signal allows unambiguous assignments of the participating vibrational states. The dependence of the signal intensity upon the delay path between the exciting free electron laser pulses can be accounted for in terms of the resonant third order polarization with a common dephasing time for the excited states.

DOI
10.1103/physrevlett.84.4998

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We report the observation of giant quantum coherence effects in the localized modes of ionized hydrogen in synthetic fluorite. Infrared free induction decay experiments on the substitutional H- center show dramatic modulations at negative delay times due to interference between multiple vibrational levels. Spectrally resolving the degenerate four wave mixing signal allows unambiguous assignments of the participating vibrational states. The dependence of the signal intensity upon the delay path between the exciting free electron laser pulses can be accounted for in terms of the resonant third order polarization with a common dephasing time for the excited states.
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The delayed or time-domain four-wave-mixing experiment is treated in the regime of intense near-resonant pulses. The interaction with the radiation during both pump and probe pulses is considered to all powers of the electric field amplitude. Analytical results are obtained for an effective four-level system. These include the dependence of the coherence amplitudes on the ratio of the pump-field intensities when there is a large vibrational discrepancy between ground and excited electronic states and a general solution for the unitary time development during the probe pulse. For the first time, delayed coherent anti-Stokes Raman scattering is detected from highly dilute (10-ppm) guest molecules. Illustrative examples are presented for the system of pentacene in benzoic acid at low temperature. Vibronic-free induction decay and the effect of field inhomogeneity across the beam profile are found to be essential for understanding the observed intensity and spectral distribution of the signal beam in the region of optimum pulse intensity.
The dynamics in the ground electronic state of the two intramolecular D-Cl stretching modes of (DCl)2 in nitrogen solid has been probed by degenerate four wave mixing experiments. Accumulated photon echoes on the "free" nu1 and "bonded" nu2 modes have been performed by means of the free electron laser of Orsay (CLIO). The analysis of the time-resolved signals provides information on the various processes responsible for the loss of vibrational coherence, in particular intra- and intermolecular vibrational energy transfer and pure dephasing. The influence of the weak hydrogen bond is clearly observed on the coherence times of the two stretching modes. Whatever the temperature, the homogeneous width of nu2 lines is almost twice that of nu1 lines. Contrary to the case of isolated DCl trapped in solid nitrogen, no obvious effect of the nitrogen lattice can be extracted from the temperature dependence of the coherence times.
The influence of the environment on vibrational dynamics, and especially on the vibrational dephasing time, is investigated for a simple system : DCl in a van der Waals solid (N2 lattice). Photon echo experiments are performed using the infrared free electron laser CLIO. In solid nitrogen, decay times of the third order polarization are in the picosecond range. In the case of the isolated DCl monomers in van der Waals interaction with the host, the observed signals are interpreted in term of a rapid spectral diffusion. The two different stretching modes of DCl dimers, perturbed in a different way by the weak hydrogen bond, exhibit different coherence times, reflecting the influence of the interaction strength between the molecules.
In this presentation the underlying theoretical analysis of the four wave mixing (FWM) efficiency is given for the resembling experiment of three-level quantum system (TLQS), where the transition from |1> to |3> correspond to a Raman active vibration mode and is forbidden in the dipole approximation. In this case quantum state |3> (vibration mode) is excited by combined resonance and, subsequently, quantum state |2> is driven by a (delayed) weak field. Notable, that during off-resonance FWM experiments significant excited state probability amplitude and, consequently, FWM exists only as long as the perturbing fields overlap. Actually, in this presentation we discuss efficiency of the FWM process, which exist for long (as compared to the pump and probe pulses) times, and appears dependent on the both electronic and nuclear excitations, stored in the TLQS. The induced material variables (coherences and populations) in the TLS were considered by means of the density matrix, and in order to account for Raman transition |1> → |3> we used an approach closely related to that exploited previously. Considerable impact of the created in TLQS electronic and nuclear coherences on the frequency conversion for specific (negative and positive) time delays will be demonstrated.