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Annual Meeting Optical Society of America

Phase-resolved resonance scattering and emission in iodine vapor

P. Mitra, Azriel Z. Genack

Published Jan 1, 1985• 0 citations
Publisher

Abstract

We address the distinction between resonance Raman scattering and fluorescence as the excitation source is continuously tuned through resonance. The experiments are performed in iodine vapor using a cw laser, whose intensity is electrooptically modulated in the 0.1-50-MHz frequency range. A lock-in amplifier is used to detect both the in-phase and out-of-phase response of the emission. The modulated signal is found to be the sum of two components. One component varies with angular modulation frequency ω, as (1 + ω2τ2)-1/2, where τ is the lifetime of the excited state. The other is found to be flat within the range of modulation frequency used in the experiment. Since the results of the modulation experiment are the Fourier transform of the response to pulsed excitation, the first component corresponds to exponential decay with the fluorescence lifetime and the second corresponds to a prompt response. A density matrix calculation shows that the prompt response would be absent if the absorption were independent of laser frequency. It exists as a result of the finite inhomogeneous linewidth and the laser detuning from the center of the transition. The amplitude of the delayed and prompt components is a function of laser frequency. This gives a full description of the dynamical response to the emission to linear excitation as the laser is tuned continuously through resonance. The response of the sample to nonlinear excitation is also discussed.

DOI
10.1364/oam.1985.ft3

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We address the distinction between resonance Raman scattering and fluorescence as the excitation source is continuously tuned through resonance. The experiments are performed in iodine vapor using a cw laser, whose intensity is electrooptically modulated in the 0.1-50-MHz frequency range. A lock-in amplifier is used to detect both the in-phase and out-of-phase response of the emission. The modulated signal is found to be the sum of two components. One component varies with angular modulation frequency ω, as (1 + ω2τ2)-1/2, where τ is the lifetime of the excited state. The other is found to be flat within the range of modulation frequency used in the experiment. Since the results of the modulation experiment are the Fourier transform of the response to pulsed excitation, the first component corresponds to exponential decay with the fluorescence lifetime and the second corresponds to a prompt response. A density matrix calculation shows that the prompt response would be absent if the absorption were independent of laser frequency. It exists as a result of the finite inhomogeneous linewidth and the laser detuning from the center of the transition. The amplitude of the delayed and prompt components is a function of laser frequency. This gives a full description of the dynamical response to the emission to linear excitation as the laser is tuned continuously through resonance. The response of the sample to nonlinear excitation is also discussed.
The response of emission in I2 vapor to intensity modulated light at radial frequency ω is measured and described in terms of the lifetime of the excited state, T1, the rate of phase interrupting collisions γ, and the inhomogeneously broadened absorption line. When the laser is tuned to resonance, the variation of amplitude of the modulated emission with ω corresponds to a single exponential decay with lifetime T1. Off resonance, the modulation is described as the sum of the above ‘‘delayed’’ component and a ‘‘prompt’’ in‐phase component which is independent of modulation frequency. The ratio of the delayed to prompt component for off resonant excitation is shown to be 2γT1. This relation is used to determine the rate of phase interrupting collisions in I2 vapor.
The phase relaxation of the resonance fluorescence from sodium vapor was studied by measuring the contrast of interference between the delayed fluorescence pulses. It is shown that the phase relaxation time can be measured by a conventional cw mode-locked pico-second pulsed laser without any sophisticated apparatus to actively lock the phases of exciting laser pulses. Using a modified Michelson type interferometer, and a homemade software based on FFT algorithm, we obtained a phase correlation time as 300 ps with good S/N ratio. A local minimum observed in the decay curve is attributed to the ground state hyperfine splitting and the temperature dependence of the phase relaxation time is explained by the change in the spread of atomic velocity distribution with temperature (Doppler broadening mechanism). Analytical calculation indicates that when the laser bandwidth is much broader than the linewidth of the fluorescence, as in the present case, the envelope of the interfering fluorescence signal can be represented by Fourier transform of the absorption spectra. The analysis based on this approximation are in good agreement with the results obtained in the experiment.
We report a significantly shortened scattering lifetime in molecular iodine when the frequency of a single-mode 5145-\AA{}A incident laser is tuned away from resonance with a discrete transition. This observation of a shortened scattering time is indicative of what has been conventionally called a Raman process. Off-resonance lifetime measurements, as reported here, may provide a means of determining the relative contribution to the absorption linewidth of homogeneous and inhomogeneous broadening.
In this work we investigate the transmission in an optical cell containing an atomic vapor, when a laser is tuned to the wings of the Doppler line, presenting inhomogeneous broadening. The experiment is designed to detect the transmission of a laser beam through a an atomic cesium vapor within a quartz cell. Due to the high atomic density in the 1 mm cell, the laser beam is totally absorbed at resonance. On the other hand, when the detuning by few GHz from the center of the line an oscillatory signal is observed as a function of the laser frequency. The amplitude of the transmission signal varies linearly with the laser intensity. These oscillations exhibit diferent behavior as we change some parameters of the system, and the rate of the oscillations vary with laser detuning and on the atomic density. The phase of the transmited field is also sensitive to the angle of incidence of the laser beam in the cell, which allows to vary the lineshape of the signal without changing the parameters of the laser (intensity, frequency, ...) or atomic vapor. Out of resonance with the atomic vapor, the parallel windows of commercial optical cell cavity works as a low finesse Fabry-Pérot with a free spectral range of 150 GHz. However, in resonance, the optical path of the cavity changes varies with frequency due to the dispersive response of the atomic vapor. This study experimentally characterized the transmission signal through a cavity containing resonant vapor as a function of intensity and frequency of the laser, as well as its dependence on the angle of incidence of the beam. A numerical model that allows to determine the collisional broadening of the atomic vapor adjusting the spectral curves of the transmission signal was developed. As an application, exploring the oscillations in the wings of the resonance, we can lock the laser frequency at a few GHz off the center of the atomic resonance. The lock was performed in the frequency range between 0,8 GHz and 2,4 GHz from the center of the D2 line of cesium. To characterize the locking stability we measure the optical beat signal between two similar experiments, using the same locking technique.
The effects of the finite correlation time of the external modulation on the secondary-emission spectra are clarified emphasizing the deviation from the motional narrowing limit or the impact approximation in the case of large off-resonance excitation. The dependences of the excitation spectrum of the secondary emission on the modulation parameters and on the inhomogeneous broadening are studied systematically. It is found that the excitation spectrum of the luminescence shows a faster decrease than that of the Raman scattering as the off-resonance frequency increases. The present theory is relevant for explaining the recent experiment by Watanabe, Kinoshita, and Kushida [Chem. Phys. Lett. 126, 197 (1986)] on the \ensuremath{\beta}-carotene in solutions. A general theory of the time-resolved spectra of the secondary emission is formulated to incorporate the effect of the finite correlation time. The luminescence component shows a slow temporal decay with the longitudinal relaxation rate. It is found for the first time that the difference is unexpectedly large between the transient behavior of the luminescence intensity and that of the intermediate-state population for the slow-modulation regime and that the difference indicates the effect of finite correlation time of the frequency modulation. On the other hand, the transient behavior of the Raman scattering contains a fast component that follows the envelope of the excitation-pulse intensity and the same slow component as the luminescence. The ratio of the slow component to the total intensity depends sensitively on the modulation parameters and the off-resonance frequency. The modulation parameters of the system in question can be estimated from these dependences in combination with the spectral characteristics of the emission under stationary excitation.
Abstract A practical approach to understanding light scattering processes in the condensed phase is presented. First a theoretical discussion of the various parameters in resonance light scattering is given and there is a special emphasis on our simplified approach to this question. As with other approaches the two level density matrix in association with a quantum regression theorem leads to two types of emission from an ensemble of molecules at finite temperature (T2 ≠ 2T1). We have called one of these fluorescence and the other sharper emission Raman scattering because it results directly from the presence of a coherent polarization in the medium. A brief discussion of time dependent scattering is also given. An experiment that reproduces the main features of the theory is described for resonance scattering from azulene in naphthalene at 30 K. For all values of the laser frequency (near resonance) both a sharp (Raman) and diffuse (fluorescent) component occurs in the emission spectrum. These spectra when interpreted by the simplified theory yield a value of T2 = 0.7 ps from fluorescence linewidth, and T2 = 0.8 ps from the incoherent to coherent scattering ratio, for the 0–0 two level system of azulene in naphthalene. A discussion of practical aspects of the influence of inhomogeneous line broadening is also presented.