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New Journal of Physics

Broadband generation in a Raman crystal driven by a pair of time-delayed linearly chirped pulses

Miaochan Zhi, Alexei V. Sokolov

Published Feb 29, 2008• 43 citations
Publisher

Abstract

A pair of time-delayed linearly chirped pulses with sub-picosecond duration is used to selectively excite Raman transitions in a lead tungstate crystal. Significant molecular coherence leads to generation of up to 40 anti-Stokes and 5 Stokes sidebands. High conversion efficiency (from the two pump beams to the sidebands) is measured. The broadband generation with chirped pulses whose duration is comparable to the Raman coherence lifetime is considerably more efficient, when compared to the case of excitation by two-color femtosecond pulses. In the future, mutual coherence among the generated sidebands may allow ultrashort pulse synthesis.

DOI
10.1088/1367-2630/10/2/025032

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A pair of time-delayed linearly chirped pulses with sub-picosecond duration is used to selectively excite Raman transitions in a lead tungstate crystal. Significant molecular coherence leads to generation of up to 40 anti-Stokes and 5 Stokes sidebands. High conversion efficiency (from the two pump beams to the sidebands) is measured. The broadband generation with chirped pulses whose duration is comparable to the Raman coherence lifetime is considerably more efficient, when compared to the case of excitation by two-color femtosecond pulses. In the future, mutual coherence among the generated sidebands may allow ultrashort pulse synthesis.
We demonstrate broadband light generation in diamond pumped by two-color femtosecond laser pulses. We find that phase matching plays a critical role in the output angle and frequency of the generated sidebands. When a third femtosecond probe pulse is applied to the crystal in the boxed Coherent anti-Stokes Raman Scattering geometry, a two-dimensional array of multi-color beams is generated through the Raman, four-wave mixing, and six-wave-mixing processes. We test the mutual coherence between the generated sidebands. Such coherence, maintained over the broad spectrum, opens possibilities for synthesis of subfemtosecond light waveforms.
Subfemtosecond pulses can be generated in a Raman generator by using electromagnetically induced transparency if ultrabroad Raman sidebands are generated and then propagate in such a way that the generated sidebands at higher frequencies are temporally advanced with regard to those at lower frequencies. However, it was recently demonstrated by experiments [1] that above-resonance Raman excitations ensured the establishment of anti-phased Raman coherence for pulse compression but only very limited number of Raman sidebands could be generated due to Raman self-defocusing [2], while broadband sidebands could be generated under below-resonance Raman excitations, which supported no pulse compression in the same Raman media. In order to establish anti-phased Raman coherence and simultaneously overcome Raman self-defocusing to benefit efficient generation of broadband sidebands, we suggest in this report a new technique to generate sub-fs pulse train in a Raman generator driven by three sufficiently intense single-mode laser beams whose carrier frequencies are tuned off the Raman resonance with two different two-photon detunings. The Raman interaction establishes a molecular modulation through nonadibatic processes. The simulation on the basis of the fundamental rotational Raman transitions in H2 shows that sub-fs pulse can be generated by above-resonance or below-resonance Raman excitations, or even Raman excitations with opposite detunings, as is shown in Fig.1. This opens a new way for experiments to observe enhanced generation of broadband Raman sidebands, together with compression of the phase-locked Raman sidebands into sub-fs pulse trains in the same Raman media
We have investigated the behavior of high-order stimulated Raman scattering in a highly-transient regime. We demonstrate efficient collinear generation of vibrational sidebands in molecular hydrogen and methane using two-color pumping with pulses of duration $\ensuremath{\tau}\ensuremath{\sim}100\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ tuned to a vibrational Raman transition. A Raman spectrum with a large bandwidth was observed, ranging from the IR to the UV. Under some conditions strong pump depletion was observed and up to five anti-Stokes sidebands were observed to have energies exceeding 10% of the transmitted pump pulse energies. A numerical simulation reproduces qualitatively and quantitatively the experimental results and allows us to explain key experimental features. The simulation also confirms that the molecular coherence in the medium is substantially increased by the two-color pumping and allows us to deduce values for the degree of material excitation. The use of this technique looks promising for efficient subfemtosecond pulse generation.
We have demonstrated that coherent molecular modulation can result in the collinear generation of mutually-coherent spectral sidebands that extend in frequency from the infrared to the far ultraviolet. Our technique is based on adiabatic preparation of a highly coherent molecular superposition-state, which is achieved by using narrow-linewidth lasers slightly detuned from a Raman resonance. The phases of the resultant Stokes and anti-Stokes sidebands are adjusted in order to synthesize desired single-cycle pulse trains at the target. In this article we review recent improvements and developments in this area, including: techniques for increasing the number of generated sidebands; synchronization of the pulse trains with the molecular motion in the given molecular system; laser self-focusing and spatial soliton formation due to the coherent interaction of light with oscillating molecules. In the future, this Raman source may produce sub-cycle optical pulses, and allow synthesis of waveforms where the electric field is a predetermined function of time, not limited to a quasi-sinusoidal oscillation.
High order Raman generation has received considerable attention as a possible method for generating ultrashort pulses. A large number of Raman orders can be generated when the Raman-active medium is pumped by two laser pulses that have a frequency separation equal to the Raman transition frequency. High order Raman generation has been studied in the different temporal regimes, namely: adiabatic, where the pump pulses are much longer than the coherence time of the transition; transient, where the pulse duration is comparable to the coherence time; and impulsive, where the bandwidth of the ultrashort pulse is wider than the transition frequency. To date, almost all of the work has been concerned with generating as broad a spectrum as possible, but we are interested in studying the spectra of the individual orders when pumped in the transient regime. We concentrate on looking at extra peaks that are generated when the Raman medium is pumped with linearly chirped pulses. The extra peaks are generated on the low frequency side of the Raman orders. We discuss how linear Raman scattering from two-photon dressed states can lead to the generation of these extra peaks.