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arXiv:1711.10772 · Optics Express

Tailored Raman-resonant four-wave-mixing processes

C. Ohae, J. Zheng, K. Ito, M. Suzuki, Kaoru Minoshima, M. Katsuragawa

Published Jan 12, 2018• 12 citations
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Abstract

Nonlinear optical processes are strongly dominated by phase relationships among electromagnetic fields involved. In this paper, we theoretically and experimentally show that in a Raman-resonant four-wave-mixing process, the first anti-Stokes and Stokes generations can be tailored in a variety of ways by manipulating the phase relationships among the relevant electromagnetic fields.

DOI
10.1364/oe.26.001452

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Nonlinear optical processes are strongly dominated by phase relationships among electromagnetic fields involved. In this paper, we theoretically and experimentally show that in a Raman-resonant four-wave-mixing process, the first anti-Stokes and Stokes generations can be tailored in a variety of ways by manipulating the phase relationships among the relevant electromagnetic fields.
Abstract Nonlinear optical processes are intrinsically dominated by the phase relationships among the relevant electromagnetic fields, including the phase of nonlinear polarization produced in them. If one can arbitrarily manipulate these phase relationships at a variety of desired interaction lengths, direct and highly designable manipulations for the nonlinear optical phenomenon could be achieved. Here, we report a proof-of-principle experiment in which a high-order Raman-resonant four-wave-mixing process is used as a representative nonlinear optical process and is tailored to a variety of targets by implementing such arbitrary manipulations of the phase relationships in the nonlinear optical process. We show that the output energy is accumulated to a specific, intentionally selected Raman mode on demand; and at the opposite extreme, we can also distribute the output energy equally over broad high-order Raman modes in the form of a frequency comb. This concept in nonlinear optical processes enables an attractive optical technology: a single-frequency tunable laser broadly covering the vacuum ultraviolet region, which will pave the way to frontiers in atomic-molecular-optical physics in the vacuum ultraviolet region.
A common assumption that Raman-resonant four-wave mixing does not transfer energy between the light and the Raman medium is shown to be incorrect. The derivation of the correct energy-transfer picture is compared with those for stimulated Raman scattering and for nonresonant mixing. The physical mechanism for Raman-gain suppression due to Stokes/anti-Stokes coupling under phase-matched conditions is clarified by this understanding of the energy transfer. An experimental demonstration of the nature of the energy transfer is proposed.
The evolution of enhanced four-wave mixing based on Raman coherence as the probe intensity increases is observed experimentally in an 85 R b atomic vapor system. We propose that for a Doppler-broadened Λ -type level system, the generated anti-Stokes field from one-photon resonance will be suppressed by the dressed-states resonance and can be controlled by the probe intensity, which influences the effective transverse relaxation rate of Raman coherence. When the probe field is not so weak, the double resonance for dressed states will greatly suppress the anti-Stokes emission at the central frequency, and the signal peak will be split. We show that this phenomenon is a result of the destructive polarization interference between atoms with different velocities from the two types of resonance. Based on our model, we present a new, to the best of our knowledge, interpretation of four-wave mixing enhancement in the conventional Λ -type electromagnetically induced transparency system.