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CRC Press eBooks

Experimental Apparatus and Technique for Optical Coherent Spectroscopy of Gases

Igor V. Yevseyev, Valery M. Yermachenko, Самарцев Виталий Владимирович

Published Feb 24, 2004• 0 citations
Publisher

Abstract

This chapter is devoted to the description of the main methods employed in the investigation of optical transient processes in gas media and the apparatus used in these studies. Recently, a new direction of laser spectroscopy has appeared. This direction is based on several methods of extracting the information concerning a resonant medium, including: a ) analysis of decay curves for the intensities of optical coherent responses within certain time intervals; b) analysis of temperature lowering, i.e., the dependencies of the intensities of coherent responses on the temperature of a gas medium under study; c) investigation of the modulated structures of optical coherent responses related to the hyperfine coupling of unpaired electrons with nuclei of molecules or atoms in the gas (modulation coherent spectroscopy), including the regime of double resonances; d) polarization coherent spectroscopy associated with the identification of the type of the energy transition being studied and the determination of characteristics of this transition from the polarization properties of optical coherent responses; e) the method of optical “coherent averaging,” which is closely related to a multipulse excitation of gas particles and the regime of double resonances; and ƒ) the method of angular spectroscopy, which is based on the spatial features of the generation of optical coherent responses and superradiance.

DOI
10.1201/9780203642696-3

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This chapter is devoted to the description of the main methods employed in the investigation of optical transient processes in gas media and the apparatus used in these studies. Recently, a new direction of laser spectroscopy has appeared. This direction is based on several methods of extracting the information concerning a resonant medium, including: a ) analysis of decay curves for the intensities of optical coherent responses within certain time intervals; b) analysis of temperature lowering, i.e., the dependencies of the intensities of coherent responses on the temperature of a gas medium under study; c) investigation of the modulated structures of optical coherent responses related to the hyperfine coupling of unpaired electrons with nuclei of molecules or atoms in the gas (modulation coherent spectroscopy), including the regime of double resonances; d) polarization coherent spectroscopy associated with the identification of the type of the energy transition being studied and the determination of characteristics of this transition from the polarization properties of optical coherent responses; e) the method of optical “coherent averaging,” which is closely related to a multipulse excitation of gas particles and the regime of double resonances; and ƒ) the method of angular spectroscopy, which is based on the spatial features of the generation of optical coherent responses and superradiance.
A new technique is presented for measuring the incoherent resonance decay (IRD) and the coherent optical ringing of selectively (5 MHz) prepared electronic states. The method utilizes electro-optic switching of a single laser mode that is on or off resonance with respect to the homogeneous molecular packets in the excited ensemble. The technique was applied to a variety of systems (gases at low pressures, gases at relatively high pressures, and solids at low temperatures) to give information about their phase memory (optical T2 processes), radiative and radiationless decay (optical T1 processes), and to measure directly their optical transition moment between the ground state and the prepared electronic state. The theory of coherent and incoherent states is also given.
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Each of three basic coherent transient phenomena (optical nutation, free polarization decay photon echo) can be generated by sufficiently abrupt modulation of the interaction between the matter and radiation. This can be performed by rapid commutation of either radiation parameters, or the parameters of the matter. I present here comparative analysis of these two approaches (the first one, using electro-optical switching of the resonant laser power to create the pulses for the gas excitation and the second one, based on the Stark switching of vibro-rotational levels in a gas, excited by CW laser radiation), used in our experiments in molecular gases, from the point of view of both their capability to generate various coherent transients and their sensitivity to the intensity of laser radiation.
A novel spectroscopic tool is presented for measuring the incoherent resonance decay (IRD) of selectively (6 MHz) prepared electronic states. The method utilizes electro-optic switching of a single laser mode that is on or off resonance with respect to the homogeneous molecular packets in the excited ensemble. The technique is applied to a variety of systems: gases at low and high pressures, molecular beams, and solids at low temperatures. The coherent transient of solids observed in the forward direction of the laser gives the phase memory (optical T2 processes) while the IRD measures directly the radiative and radiationless decay (optical T1 processes), and the optical transition moment between the ground state and the prepared electronic state. The theory of coherent and incoherent states is also given, and related to the different aspects of time-resolved spectroscopy of molecular beams and solids.
Coherent transient phenomena can be generated by the abrupt changes of parameters either of the electromagnetic field or of the matter. Comparative analysis of these two approaches, made on the base of experimental research in molecular gases SF6, 15NH3, HFCO and 13CH3F, excited by the radiation of CW CO2 and 13CO2 lasers, is presented. The first approach of photon echo (and its modifications) generation, based on electro-optic pulses formation from the resonant CW exciting radiation, has proven to be successful for intense infrared molecular transitions. The coherent responses are sufficiently powerful to be applied in high resolution spectroscopy, the spectral markers creation ,and molecular collisions investigations. However, this technique is not very effective for the free polarization decay investigations. Another approach based on the Stark switching molecular levels of polar gas, irradiated by CW laser, was demonstrated for free polarization decay and photon echo generation in 13CH3F. Free polarization decay has shown the pronounced frequency shift because of dynamic Stark effect in the CW radiation field. This specific feature of coherent transients, created by Stark switching, limits the high resolution spectroscopy by the low intensity range of exciting radiation. From other viewpoint, it gives unique possibility to investigate coherent transients generated at the dressed molecular levels.
Our recent studies of methods for obtaining ultrashort light pulses and analysis of the impact of ultrashort optical pulses on classical and quantum micro-objects with the identification of the determining role of the degree of unipolarity of pulses (maximum for strictly unipolar pulses) in the efficiency of direct laser acceleration of charged particles and excitation of atoms and molecules have been reviewed. Special attention has been paid to the coherent mode locking regime in lasers, which is implemented when the laser pulse duration is less than the relaxation time of the working transition in media with resonance amplification and absorption (laser analog of the phenomenon of self-induced transparency). Experimental data on coherent mode locking in a titanium-sapphire laser with a cell with rubidium vapor at self-induced transparency in rubidium have been presented. The interaction of ultrashort pulses in resonant media has also been analyzed.