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

Spectral repers and slow-molecule detection using the photon echo technique and its modifications

L. S. Vasilenko, Н. Н. Рубцова, Хворостов Евгений Борисович

Published Oct 21, 1998• 0 citations
Publisher

Abstract

The contrast and steepness of spectral repers, detected by two nonlinear Doppler free techniques -- photon echo in standing waves (PESW) and saturated absorption spectroscopy (SAS) -- are investigated at 0 yields 1 (nu) 3 P(33) A1/2 SF6 transition for identical experimental conditions versus intensity of CO2 laser radiation. S/N advantage of PESW technique as compared to SAS method is demonstrated. The increasing role of slow molecules in generation of photon echo response at elevated time delays between exciting pulses manifests itself experimentally in slowing down the photon echo decay rate.

DOI
10.1117/12.328224

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The contrast and steepness of spectral repers, detected by two nonlinear Doppler free techniques -- photon echo in standing waves (PESW) and saturated absorption spectroscopy (SAS) -- are investigated at 0 yields 1 (nu) 3 P(33) A1/2 SF6 transition for identical experimental conditions versus intensity of CO2 laser radiation. S/N advantage of PESW technique as compared to SAS method is demonstrated. The increasing role of slow molecules in generation of photon echo response at elevated time delays between exciting pulses manifests itself experimentally in slowing down the photon echo decay rate.
The contrast and steepness of spectral repers, detected by two nonlinear Doppler free techniques -- photon echo in standing waves (PESW) and saturated absorption spectroscopy (SAS) -- are investigated at 0 yields 1 (nu) 3 P(33) A21 SF6 transition for identical experimental conditions (over gas pressure and exciting beams geometry) versus intensity of CO2 laser radiation. S/N advantage of PESW technique as compared to SAS method is demonstrated. The increasing role of slow molecules in generation of photon echo response at elevated time delays between exciting pulses manifests itself experimentally in slowing down the photon echo decay rate.
A review of theoretical and experimental works on the polarization photon-echo spectroscopy (PPE spectroscopy) is carded out. The main attention is payed to the following advantages of the PPE spectroscopy. First, the PPE spectroscopy, free of the influence of the inhomogeneous spectral line broadening, allows to make the high precision measurements within the envelope of a inhomogeneously broadened spectral line. Second, the high resolution ability of the PPE spectroscopy, directly in the temporal field, unables to accomplish the investigations of the fast relaxation processes, when ultrashort nano- and picosecond exciting pulse are used. Third, in the PPE spectroscopy the investigated relaxation processes are not subjected to the perturbing action of the intensive laser radiation. Farther, it is necessary to note the flexibility of the PPE spectroscopy consisting in the existence of a great number of various methods used for receiving different spectroscopic information. Finally, as far as the signal intensifies of the photon echo and of its variants are proportional to the squared number of the resonant atoms (molecules), it secures the definite advantages for the PPE spectroscopy as compared to the spectroscopk methods based on the non-coherent phenomena (especially for low pressure a gas considered). The possibilities of new experiments on photon echo and its variants aimed for obtaining a detailed new spectroscopic information are discussed.
Up to now, Doppler-free nonlinear spectroscopy has been applied to atoms inside a gas medium (volume spectroscopy). We have extended these methods to atoms in the vicinity of a surface. The basic principle consists of monitoring reflectivity changes produced when a laser beam, incident on a glass–vapor interface, is brought into resonance with an atomic transition. For Doppler-free spectroscopy, two counterpropagating beams are used to operate velocity selection. If these two beams are under normal incidence in the glass—velocity selection perpendicular to the surface—one observes saturated dispersion (selective reflection sensitive to the real index). For incidence angles in the glass (prism) larger than the critical angle (total internal reflection), a standing evanescent wave is produced in the gas (velocity selection along the surface), and saturated absorption is detected. Experimental demonstration was performed on the Na resonance line; high sensitivity (10−4 relative reflectivity change) and spectral resolution as good as 20 MHz were obtained. The main limitation to better resolution comes from the short atomic transit time in the evanescent wave (typical extension ~λ). Relevant applications of these techniques should also concern the diagnostics of optically thick media, as analysis of interaction between gas-phase atoms and the surface, notably atom–wall collisions, and modification of the spontaneous emission characteristics.
A general conceptual problem of time-dependent single molecule spectra is discussed theoretically in the framework of recently developed intensity-time-frequency correlation spectroscopy. It is shown that the new method is closely related to a ``gedanken'' three-pulse photon echo experiment done on an ensemble of identical molecules interacting with statistically identical microscopic environments. The correlation function is an integral transform (under certain conditions a Fourier transform) of the echo amplitude as a function of the delay between the first and the second pulses.
Free polarization decay and photon echo were studied experimentally in polar gas 13CH3F at the transition R(4,3) of vibrational mode 0 yields 1 (nu) 3 by Stark switching of molecular levels under irradiation by CW CO2 laser at 9P(32) line. Application of 4.5 mcs pulse to the Stark electrodes inside the gas cell allows to detect the free polarization decay signal, combined with the optical nutation. The sign of the signal corresponds to the increase of absorption in the limit of low intensity (not over 0.01 W/cm2) saturating radiation. Exciting intensity growth till the level of 6.0 W/cm2 implies decrease of signal absolute value, till the change of its sign, while the oscillation of the free polarization decay signal reveals remarkable frequency shift. Such behavior is attributed to the combined action of the dynamic Stark effect of CW radiation field and the levels splitting by the Stark voltage. Two shorter (of about 0.1 and 0.2 mcs) Stark pulses, applied to the gas, generate the photon echo signals detected by the same heterodyne technique. The study of the variations of photon echo parameters versus exciting radiation intensity is in progress.
In this paper, we describe two complementary nonlinear spectroscopy methods which both allow one to achieve Doppler-free spectra of atomic gases. First, saturated absorption spectroscopy is used to investigate the structure of the 5S 1/2 → 5P 3/2 transition in rubidium. Using a slightly modified experimental setup, Doppler-free two-photon absorption spectroscopy is then performed on the 5S 1/2 → 5D 5/2 transition in rubidium, leading to accurate measurements of the hyperfine structure of the 5D 5/2 energy level. In addition, electric dipole selection rules of the two-photon transition are investigated, first by modifying the polarization of the excitation laser, and then by measuring two-photon absorption spectra when a magnetic field is applied close to the rubidium vapour. All experiments are performed with the same grating-feedback laser diode, providing an opportunity to compare different high-resolution spectroscopy methods using a single experimental setup. Such experiments may acquaint students with quantum mechanics selection rules, atomic spectra and Zeeman effect.