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International Conference on Optoelectronic Science and Engineering '90

Optical heterodyne detection via four wave mixing process in iodine and sodium molecules

Long-Sheng Ma

Published Jul 1, 1990• 0 citations
Publisher

Abstract

As a high sensitivity and high resolution spectroscopy, opti.cal heterodyne detection via nearly- degenerate four-wave mixing has been investigated since 1980 . The technique has been used for stabilizing lasers and precision spectroscopy measurement. Using optical heterodyne technique, we performed experiments to detect four-wave mixing process in iodine and sodium molecules.

DOI
10.1117/12.2294726

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As a high sensitivity and high resolution spectroscopy, opti.cal heterodyne detection via nearly- degenerate four-wave mixing has been investigated since 1980 . The technique has been used for stabilizing lasers and precision spectroscopy measurement. Using optical heterodyne technique, we performed experiments to detect four-wave mixing process in iodine and sodium molecules.
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.
The spectral behavior of the third order nonlinear optical response of atomic sodium was studied. As a result, new kinds of frequency domain spectroscopy techniques were developed: nearly degenerate four-wave mixing, polarization nearly degenerate four-wave mixing, frequency domain three-state spectroscopy, and nonlinear Hanle effect in degenerate four-wave mixing. These techniques have provided new information on several areas of collision physics including: dephasing collisions (spectral broadening and frequency shift), velocity changing collisions, state changing collisions, and spin-flip collisions. (Author)
Cavity ring-down spectroscopy and degenerate four-wave mixing have been applied for spectroscopic studies, temperature determination, and measurement of relative dipole transition moments of photochemically produced sodium hydride. In our experiment, NaH was formed within a heat-pipe oven after 3p excitation of sodium in a hydrogen atmosphere with a second dye laser. The reaction product NaH was probed in the near ultraviolet part of the spectrum at 382 nm with 1-4-/spl mu/s delay to the excitation pulse using both a linear and nonlinear spectroscopic technique with a pulsed dye laser source (pulsewidth 15-ns full-width half-maximum). The strengths and limitations of these two spectroscopic techniques are discussed. Since the two processes depend on different parameters and the image-forming beams have different properties, it is difficult to define a single criterion for comparison. But our measurements indicate that cavity ring-down spectroscopy is a powerful tool with a sensitivity better than 10/sup 9/ particles per cm/sup 3/ and quantum state which is comparable to degenerate four-wave mixing in our case.