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IEEE Journal of Selected Topics in Quantum Electronics

Toward Single-Cycle Pulse Generation in Raman-Active Crystals

Miaochan Zhi, Alexei V. Sokolov

Published Jun 21, 2011• 15 citations
Publisher

Abstract

We study broadband sideband generation in Raman-active crystals. The sidebands come out at different angles and cover infrared, visible, and ultraviolet spectral regions. We combine the sidebands into a collinear beam by using a prism. We use a pulse shaper to control the relative phases of the sidebands aiming to produce single-cycle pulses.

DOI
10.1109/jstqe.2011.2159780

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We study broadband sideband generation in Raman-active crystals. The sidebands come out at different angles and cover infrared, visible, and ultraviolet spectral regions. We combine the sidebands into a collinear beam by using a prism. We use a pulse shaper to control the relative phases of the sidebands aiming to produce single-cycle pulses.
We report pulse-shaper-assisted phase control of a broad spectrum, aiming to synthesize nonsinusoidal waveforms. We first generate multiple-order coherent Raman sidebands by focusing two laser beams into a piece of diamond. Then we combine five sidebands into a single beam by using a prism. Our setup allows for both coarse, manual phase adjustments and fine tuning of the spectral phases. A flat spectral phase across these five frequency-separated sub-bands is achieved, which implies generation of two to three optical-cycle pulses.
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 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.
We show that two Raman generators which have different Raman transition frequencies and are used in series result in a multiplicative increase in the total number of generated sidebands. When phase-corrected, these sidebands synthesize to a train of randomly timed single-cycle pulses. For series generators on the rotational transitions of molecular D2{\mathrm{D}}_{2}D2​ $(J=\stackrel{\ensuremath{\rightarrow}}{0}2)$ and H2{\mathrm{H}}_{2}H2​ $(J=\stackrel{\ensuremath{\rightarrow}}{1}3),$ each with 40 modes, the average peak power enhancement is 1600 and the average duration between random pulses is 1.74 ps.
We use molecular deuterium and two driving lasers to demonstrate collinear generation of mutually coherent equidistant sidebands, covering $50000{\mathrm{cm}}^{\ensuremath{-}1}$ of spectral bandwidth and ranging from $2.94\ensuremath{\mu}\mathrm{m}$ to 195 nm in wavelength. The essential idea is the adiabatic preparation of a single, highly coherent ( $|{\ensuremath{\rho}}_{\mathrm{ab}}|\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0.33$) molecular eigenstate.