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Frontiers in Optics

Subfemtosecond pulse generation by three correlated Raman generators

Jian Wu, Heping Zeng

Published Jan 1, 2003• 0 citations
Publisher

Abstract

It has been proposed that single-cycle pulses with an average spacing between two random pulses as large as 1.74 ps can be generated when two cascaded Raman medium are used [1]. In this report, we propose a new technique to generate of subfemtosecond (sub-fs) pulse train with large pulse spacing, on the basis of three correlated Raman generators within three involved molecular levels in a Raman medium. Each Raman generator comes from the corresponding Raman transition between two of the three involved molecular levels, which are coupled by two of three single-mode laser beams of sufficient intensities in such a way that correlation between the Raman generators are established. A large enough pulse spacing can be possibly achieved if proper Raman transitions are selected so that the frequency difference between two adjacent Raman sidebands is small enough.

DOI
10.1364/fio.2003.mt20

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It has been proposed that single-cycle pulses with an average spacing between two random pulses as large as 1.74 ps can be generated when two cascaded Raman medium are used [1]. In this report, we propose a new technique to generate of subfemtosecond (sub-fs) pulse train with large pulse spacing, on the basis of three correlated Raman generators within three involved molecular levels in a Raman medium. Each Raman generator comes from the corresponding Raman transition between two of the three involved molecular levels, which are coupled by two of three single-mode laser beams of sufficient intensities in such a way that correlation between the Raman generators are established. A large enough pulse spacing can be possibly achieved if proper Raman transitions are selected so that the frequency difference between two adjacent Raman sidebands is small enough.
We show that subfemtosecond pulse train with large pulse spacing can be generated by using three correlated Raman generators between three Raman levels with strong molecular modulation to control the generation and propagation of the cascade stimulated Raman sidebands. For three Raman generators based on the fundamental rotational and vibrational Raman transitions $(v=0,J=0\ensuremath{\leftrightarrow}v=0,J=2\ensuremath{\leftrightarrow}v=1,J=0\ensuremath{\leftrightarrow}v=0,J=0)$ in molecular hydrogen, a train of subfemtosecond pulses with a pulse spacing of 379.9 fs and pulse width down to 0.26 fs can be generated.
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 suggest a technique to generate subfemtosecond 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 a nonadiabatic process. The simulation based on the first fundamental vibrational Raman transition of solid hydrogen indicates that subfemtosecond pulse train can be generated when the signs of the two-photon detunings are opposite. This opens an experimentally feasible way to observe enhanced generation of broadband Raman sidebands as well as compression of the phase-locked Raman sidebands into subfemtosecond pulse trains in the same Raman media with above- and below-resonance Raman excitations.
Subfemtosecond (sub-fs) pulses can be generated by cascade-stimulated Raman scattering in a Raman medium with modulated Raman excitations, driven by two sufficiently intense laser beams, one of which is amplitude modulated. The nonadiabatic Raman interaction establishes a strong modulated Raman coherence, which supports compression of the generated broadband Raman sidebands to a train of sub-fs pulses regardless of whether the carrier frequencies of the driving lasers are tuned above, below or on two-photon Raman resonance.
A technique is proposed to increase multiplicatively the pulse spacing of a periodic subfemtosecond-pulse train based on molecular modulation, with more pairs of driving lasers to control the higher-order stimulated Raman scattering. We demonstrate that the pulse spacing can be readily doubled, tripled, or even quadrupled by using pairs of off-resonant two-photon Raman transitions driven by laser beams of sufficient intensities and relatively shifted carrier frequencies. A periodic subfemtosecond-pulse train with a pulse width down to 0.53 fs and pulse spacing up to 376 fs can be generated with appropriate molecular coherence control of the fundamental rotational transition in molecular hydrogen.
We suggest that subfemtosecond pulses can be generated by using high-order stimulated Raman scattering when a Raman transition is driven by three intense single-mode laser beams with two different modulation frequencies. An oscillatory strong Raman coherence is established by the modulated molecular modulation. Numeric simulations based on the first fundamental vibrational Raman transition of gaseous and solid deuterium indicate that subfemtosecond pulses can be generated by Raman excitations with above, below, or opposite Raman detunings.