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Chinese Physics Letters

Discovery of the Induced Superslow Optical Relaxation Processes in I 2

Hongjie Jiang, Yong Zhang, Jiahua Zhu, Shao-wu Fang, Liangen Ding, H.-R. Xia

Published Jun 1, 1996• 0 citations
Publisher

Abstract

We discover superslow optical processes with relaxation time as long as 250 ms in I 2 . The demonstration is performed by a series of experiments with novel considerations for I 2 interacting with phase modulated laser fields, monitored by both coherent and noncoherent detection with digital frequency scale and time scale simultaneously for comparison.

DOI
10.1088/0256-307x/13/6/010

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We discover superslow optical processes with relaxation time as long as 250 ms in I 2 . The demonstration is performed by a series of experiments with novel considerations for I 2 interacting with phase modulated laser fields, monitored by both coherent and noncoherent detection with digital frequency scale and time scale simultaneously for comparison.
The approaches to realize superslow relaxation receive growing attention for its correspondence to sharp optical resonance in frequency domain and to long term of information storage in time domain. Dephasing time as long as 2.6 mS was observed in the condensed matter of crystal under the temperature of 1.4K [1]. In RF ion trap Yb ion has been kept in its metastable excited state for 8 days [2]. Population trapping is one of the interested approaches recently. While most papers discussed it for Λ- or V-type three-level systems, Agarwarl et al has theoretically predicted the possibility of population trapping been established by frequency modulated laser field in two-level system [3]. The authors has demonstrated population trapping in high-lying state doublet and in intermediate state doublet via quantum interferences between two sum-frequency two-photon excitations in Y- and in rhomb-type four-level systems respectively [4].
A model of two-level weakly interacting quantum systems is used to demonstrate that the phase of molecular vibrations excited through stimulated Raman scattering can be controlled by the relative phase of time-separated laser pulses, allowing synchronization and amplitude control of coherence excitation in a medium. For transients with a phase relaxation time less than the field cycle, the field half-cycle can serve as a subfemtosecond probe of coherent vibrations. In this regime, the high-frequency field-induced modulation of molecular dipole moments gives rise to a detectable modulation of the optical response of a medium at the frequency $2\ensuremath{\omega}$, $\ensuremath{\omega}$ being the frequency of the laser field.
The pump and probe variant of the stimulated Raman gain technique permits the measurement of picosecond dephasing times with low-power, continuous-wave mode-locked lasers, but it suffers by its susceptibility to inevitable randomly induced fluctuations in the relative phases of the interacting laser fields. The resulting severe requirements on optical stability can be circumvented through application of a double-modulation–detection scheme that we have developed. It is based on rms detection of the T2 signal as generated through application of a low-frequency phase modulation of precise amplitude, additional to the commonly applied rf modulation with corresponding lock-in detection. A detailed description of the method and its experimental realization is presented. T2 measurements on the 656 cm−1 vibration of liquid CS2 illustrate its performance. In comparison with previous techniques, precision is improved by about a factor of 4. But more important is the fact that the technique permits to make a continuous recording of the T2 signal, while achieving at the same time a reduction in measurement time by an order of magnitude. Furthermore, optimization of the optical setup is possible, through direct monitoring of the dephasing signal at any delay. Automating the data taking and processing should be straightforward.