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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Spectrum of Na 2 by optical heterodyne techniques

Liangen Ding, Ziyi Bi, Long-Sheng Ma

Published Oct 28, 1992• 0 citations
Publisher

Abstract

Optical heterodyne spectroscopy is one of the ultrasensitive and high resolution laser spectroscopies. During past years, it has extended from saturation absorption to two-photon transitions in a three level quantum system of atoms and ions. The particularly interesting case is the modulation transfer spectroscopy, where the optical heterodyne detection is performed via nearly degenerate four-wave mixing (NDFWM) in the nonlinear medium. In this report, the modulation transfer spectroscopy is used to observe the optical heterodyne saturation absorption and two-photon transition spectra simultaneously in Na2 without Doppler background. The line shapes of optical heterodyne signal are discussed in detail.

DOI
10.1117/12.130465

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Optical heterodyne spectroscopy is one of the ultrasensitive and high resolution laser spectroscopies. During past years, it has extended from saturation absorption to two-photon transitions in a three level quantum system of atoms and ions. The particularly interesting case is the modulation transfer spectroscopy, where the optical heterodyne detection is performed via nearly degenerate four-wave mixing (NDFWM) in the nonlinear medium. In this report, the modulation transfer spectroscopy is used to observe the optical heterodyne saturation absorption and two-photon transition spectra simultaneously in Na2 without Doppler background. The line shapes of optical heterodyne signal are discussed in detail.
Abstract This tutorial provides a joint theoretical and experimental overview of heterodyne wave mixing spectroscopy, focusing mainly on four-wave mixing (FWM). This powerful and versatile time-resolved nonlinear optical spectroscopy technique enables the investigation of individual localized single photon emitters, as well as microscopy of extended samples, e.g. two-dimensional transition metal dichalcogenides. Starting with the fundamental theory of optically driven two-level systems, we motivate the utility of wave mixing spectroscopy via a discussion on homogeneous and inhomogeneous linewidths which can be independently measured using FWM. We then provide a detailed overview of the heterodyne wave mixing setup operated by one of the authors (JK) at Institut Néel in Grenoble, supported by theoretical modeling of the signal detection process. Throughout the paper we elaborate on important benefits of heterodyne wave mixing spectroscopy, e.g. background-free detection, measurement of the full signal field including amplitude and phase, and investigation of coupling mechanisms in few-level systems. Within the context of the latter point we discuss the significance of two-dimensional FWM spectra. This tutorial is dedicated to students, young researchers, as well as experts in the field of nonlinear spectroscopy in general and FWM in particular. It explains the fundamental concepts and building blocks required to operate a heterodyne wave mixing experiment both from the experimental and theoretical side. This joint approach is helpful for theoreticians who want to accurately and quantitatively model wave mixing signals, as well as for experimentalists who aim to interpret their recorded data.
We present a theoretical analysis of high-frequency optical heterodyne saturation spectroscopy in Doppler-broadened coupled three-level systems. The saturating beam, which is assumed to be amplitude modulated at frequency δ (double-sideband suppressed carrier amplitude modulation) is resonant for one of the transitions. Through non-degenerate four-wave mixing processes, this modulation is transferred to a probe beam, resonant for the coupled transition. Saturating and probe fields may be either co-propagating or counter-propagating. The lineshape of the probe modulation is analysed via a third-order perturbation expansion of the atomic density matrix with respect to the incident field amplitudes. The resulting signal is integrated over velocities, in the Doppler limit approximation. Both population saturation effects and coherent (Raman-type, or two-photon) processes contribute to the signal. The various contributions appear as Lorentzian-type resonance doublets. We show that, in the absence of relaxation processes (collisional dephasing, or radiative cascades), destructive interferences between population saturation and coherent two-photon processes are responsible for the disappearance of one resonance doublet. Phase-interrupting collisions are thus predicted to lead to the existence of a « pressure-induced extra-resonance » (PIER) doublet, which could yield information on collisional processes in the impact regime. The properties of the predicted PIER doublets are analysed in relation with other types of PIER signals studied in four-wave mixing, and in time-resolved saturation spectroscopy.
Heterodyne Doppler-free spectroscopy, previously demonstrated on single-photon resonances (heterodyne saturation spectroscopy), has been extended to two-photon transitions in rubidium (5S-5D and 5S-7S). It provides a simple method of observing the two-photon dispersion lineshape directly. The noticeable sensitivity of this absorption technique, which has been used for an optical measurement of the hyperfine structure of the 5D level, is discussed in comparison with that currently obtained in two-photon-induced fluorescence.
We study modulation spectroscopy of the potassium D 2 transitions at 766.7 nm. The vapour pressure, controlled by heating a commercial reference cell, is first optimized using conventional saturated absorption spectroscopy. Heterodyne detection then yields sub-Doppler frequency discriminants suitable for stabilizing lasers in experiments with cold atoms. Comparisons are made between spectra obtained by direct modulation of the probe beam and those using modulation transfer from the pump via nonlinear mixing. Finally, suggestions are made for further optimization of the signals.