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Frequency-time and time-space mappings with broadband and supercontinuum chirped pulses in coherent wave mixing and pump-probe

Lomonosov Moscow

Published Jan 1, 2003• 0 citations
OpenAlex

Abstract

Broadband and supercontinuum pulses with a lin- ear chirp define a linear transform, mapping the difference between the instantaneous frequencies of pump pulses onto the delay time between these pulses. This delay between the pump pulses can be then mapped onto the spatial coordinate with the use of a broad-beam wave-mixing or pump-probe geometry. The new possibilities offered by these mappings for four-wave-mixing techniques are discussed. The spectral and temporal resolution of chirped-pulse wave-mixing and pump- probe techniques are examined. Single-shot multidimensional wave-mixing techniques using broadband and supercontinuum chirped pulses are discussed.

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Broadband and supercontinuum pulses with a lin- ear chirp define a linear transform, mapping the difference between the instantaneous frequencies of pump pulses onto the delay time between these pulses. This delay between the pump pulses can be then mapped onto the spatial coordinate with the use of a broad-beam wave-mixing or pump-probe geometry. The new possibilities offered by these mappings for four-wave-mixing techniques are discussed. The spectral and temporal resolution of chirped-pulse wave-mixing and pump- probe techniques are examined. Single-shot multidimensional wave-mixing techniques using broadband and supercontinuum chirped pulses are discussed.
It is nowadays possible to generate, in different spectral ranges, ultrabroadband light pulses with transform-limited (TL) duration corresponding to a few optical cycles. Whenever broadband pulses are employed, the dispersion experienced by the pulses causes a frequency chirp which may severely lengthen their duration and influence time-resolved measurements. While it is well known that the relative weight of ground-state versus excited-state oscillations can be controlled by the chirp in the pump pulse, the effects of probe pulse chirp have not been fully investigated. In this paper we show, both theoretically and experimentally, that a pump-probe experiment using strongly-chirped probe pulses can preserve the temporal resolution of the TL pulses.
A novel technique for programming broadband true-time delays that uses two frequency-offset temporally overlapped linear frequency-chirped pulses to produce periodic spectral gratings in an inhomogeneously broadened absorber is presented. Advantages of this technique include its ability to use chirped pulses that are longer than the coherence time of the crystal, less stringent laser frequency-stability requirements for grating accumulation, lower power requirements, a simplified system design, and the ability to tune broadband (multigigahertz) delays over a wide dynamic range (picoseconds to microseconds).
Summary form only given. Nonlinear techniques using broadband light have been developed and applied for studying dephasing processes, population and orientational dynamics of molecules. These techniques are based on the fact that in wave-mixing processes one may have the time resolution determined by the laser coherence time instead of the laser pulse duration. One limiting factor of the measurement sensitivity is a constant signal (pedestal), which is present even when the delay time between the exciting broadband beams is substantially longer than their coherence time and relaxation time under study. A technique has been developed, which uses not "white" detection, but spectral filtering in field-correlated four-wave mixing, the so called interferometric four-wave mixing (IFWM), which gives a signal that reveals oscillatory modulation, enabling us to discriminate it more easily from the pedestal. The technique allows to determine rather precisely the frequency of a molecular vibration and its dephasing time, as well as to study damped molecular rotations in liquids. We report the first measurements of population relaxation rates affected by stimulated emission in the presence of the pump field applying the IFWM technique.
A technique is proposed and experimentally demonstrated that achieves simultaneous optical pattern waveform storage and programmable time delay for continuous real-time signal processing by use of optical coherent transient technology. We achieve variable-time-delay and broadband signal processing by frequency shifting of two chirped programming pulses, the chirp rate of one being twice that of the other, without using brief reference pulses and without changing the timing of the programming sequence. We demonstrate the technique experimentally in Tm(3+): YAG at 5 K for 40-MHz chirps by performing temporal signal convolution with true-time delays that vary over a 250-ns range.