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Optics Express

Prospects for continuous-wave molecular modulation in Raman-active microresonators

J. T. Karpel, David C. Gold, Deniz D. Yavuz

Published Nov 7, 2019• 4 citations
Publisher

Abstract

We propose the extension of existing molecular modulation techniques for continuous-wave optical modulation to Raman-active microresonators. Intense pump and Stokes modes inside a microresonator prepare a high coherence of the Raman transition between two ro-vibrational states. With the coherence prepared, any laser in the optical region can be coupled to the microresonator and be modulated. We perform numerical simulations which predict that these "microresonator-based molecular modulators" could have modulation efficiencies on the order of 1% at 10 THz-scale frequencies for any optical wavelength.

DOI
10.1364/oe.27.034154

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We propose the extension of existing molecular modulation techniques for continuous-wave optical modulation to Raman-active microresonators. Intense pump and Stokes modes inside a microresonator prepare a high coherence of the Raman transition between two ro-vibrational states. With the coherence prepared, any laser in the optical region can be coupled to the microresonator and be modulated. We perform numerical simulations which predict that these "microresonator-based molecular modulators" could have modulation efficiencies on the order of 1% at 10 THz-scale frequencies for any optical wavelength.
We suggest a technique where a molecular Raman transition is prepared near a maximally coherent state with continuous-wave (CW) laser beams. The key idea is to put the molecules inside a high-finesse cavity and to drive the molecular transition with two lasers whose frequency difference is slightly detuned from the Raman resonance. In this regime, the molecules become very efficient CW modulators with a modulation frequency that can be as high as 100THz100\phantom{\rule{0.3em}{0ex}}\mathrm{THz}100THz.
We demonstrate an optical modulator at a frequency of 90 THz that has the capability to modulate any laser beam in the optical region of the spectrum. The modulator is constructed by placing deuterium molecules inside a high-finesse cavity and driving a vibrational transition with two continuous-wave laser beams. The two beams, the pump and the Stokes, are resonant with the cavity. The high intra-cavity intensities that build up drive the molecules to a coherent state. This molecular coherence can then be used to modulate an independent laser beam, to produce frequency up-shifted and down-shifted sidebands. The beam to be modulated is not resonant with the cavity and thus the sidebands are produced in a single pass.
Modulation features in the frequency domain can be transferred from an amplitude-modulated laser field to a nonmodulated one by a strong Raman coupling, which is based on refractive index control with a strong Raman coherence established with two sufficiently intense laser fields slightly off the two-photon Raman resonance of a selected Raman mode. Numerical simulations show that modulation transfers between the driving lasers, such as transfers from ultraviolet to extreme ultraviolet and from infrared to middle infrared lasers, can be realized in gaseous Raman media. This provides an efficient way to extend the optical modulation range beyond the transparent ranges of commercial modulators. Modulation features can also be transferred from a low-intensity driving laser to a high-intensity one, which ensures a direct application to modulate lasers with high intensities beyond the damage thresholds of standard modulators.
A THz optical modulator for a continuous-wave laser using a hollow-core photonic crystal fiber (HC-PCF) was proposed and theoretically analyzed. Lightwaves traveling through the HC-PCF is modulated by interactions with coherently driven Raman-active molecules in the core. The coherent molecular motion is excited by a pulse train having an interval between successive pulses shorter than the molecular dephasing time. In principle, a rotational transition of molecular hydrogen (S 0 (1)) at a pressure of 1 atm has a long enough dephasing time to maintain molecular coherence during a 1 GHz commercially available mode-locked pulse train. Optimization of the waveguide dispersion would enable phase-matching between the probe beam and generated sidebands during optical modulation. The proposed scheme would be achievable with a reasonable pump beam power and HC-PCF length, and with a feasible pressure of molecules in the core.
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.