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Physical Review A

Phase-dependent amplification in pump-probe experiments

Benjamin Fain, Vadim Khidekel, S. H. Lin

Published Feb 1, 1994• 2 citations
Publisher

Abstract

The pump pulse creates nonstationarity and coherence in the medium. The amplification (absorption) of the probe pulse in the nonstationary coherent medium belongs to phase-dependent Raman amplification (absorption). In this inversionless mechanism of amplification the phase is determined by the delay time between the pump and the probe pulses.

DOI
10.1103/physreva.49.1498

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Annual Meeting Optical Society of America•Jan 1, 1993•0 citations
The pump pulse creates nonstationarity and coherence in the medium. The amplification (absorption) of the probe pulse in the nonstationary coherent medium belongs to phase-dependent Raman amplification (absorption). In this inversionless mechanism of amplification the phase is determined by the delay time between the pump and the probe pulses.
In ultrashort (femtosecond) pump-probe spectroscopy, the pump pulse creates a nonstationary medium while the probe pulse propagates in such a medium. The analysis of this situation is performed in the framework of linear nonstationary optics. Constitutive equations and electrodynamics of the nonstationary media are analyzed. The propagation of the probe-pulse energy is characterized by the coarse-grained susceptibility introduced in the previous works of the authors [S. H. Lin and B. Fain, Chem. Phys. Lett. 157, 233 (1989); B. Fain, S. H. Lin, and N. Hamer, J. Chem. Phys. 91, 4485 (1989); B. Fain and S. H. Lin, Chem. Phys. 161, 515 (1992)]. The main objective of the paper is the derivation and analysis of the delay-time-dependent absorption and dispersion line shapes of the probe pulse. This line shape has a very specific form corresponding to phase-dependent Raman absorption (emission). The latter phenomenon is introduced and described in the present paper.
Recent progress has been made in the theoretical and experimental study of the amplification of optical signals without population inversion (AWI) of the participating electronic levels. Induced coherence among appropriate levels in the active medium is the necessary condition for obtaining AWI. Similarly, the generation of wave packet states in atoms and molecules also relies on the coherent superposition of several states. It is feasible, therefore, that AWI is possible in a system which has been excited into a wave packet state. We have thus demonstrated experimentally such amplification in an extended sample of sodium dimers and we term this process wave packet amplification (WPA). An important characteristic of WPA is that the gain is doubly phase-sensitive—it is modulated at both the wave packet oscillation period and the optical period. The former time-dependence is a result of the periodic revivals of the pump-induced electronic polarization and the latter optical phase-sensitivity is a manifestation of the coherent nature of the molecular wave packet. The experiments to be described use a time-resolved upconversion method to detect the change in energy of a 50 fs probe pulse after it passes through a sodium heat pipe that has been pumped with another 50 fs pulse. The maximum saturated energy gain in this system is four and corresponds to all of the available energy being transferred from the wave packet to the probe pulse.