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Acta Optica Sinica

Theoretical mode of Ufetime measurement by phase shift method

Li S

Published Jan 1, 1988• 0 citations
OpenAlex

Abstract

The lifetime of atoms and molecules can be measured by using modulated resonant single-mode laser field. A theoretical mode for this method is presented. It is shown that the laser induced fluorescence, a resonance flourescence is modulated at the same frequency, but phase shift from the exciting laser. The phase shift is mainly due to three processes (1) coherent excitation process characterized by transverse relaxation rate and line width of the laser, (2) population damping process characterized by the decay time of excited levels and other populated levels, (3) collision process characterized by the relaxation time by which the system to be in equilibrium state. The effect of these processes on measurement result is discussed. The Doppler broading is considered also.

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AC Stark effect and fluorescence using modulated laser beams. I. Effect of laser fluctuations and arbitrary relaxation parameters

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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.

AIP conference proceedings•Jan 1, 1986•0 citations

Effect of Radiative Relaxation of Excitation Anisotropy on the Measurement of Atomic Lifetime. Demonstration on Argon 2p4Level

Takashi Fujimoto, Chiaki Goto, Yasunori Uetani +1 more

We have measured the atomic lifetime of the argon 2 p 4 level by the laser-induced-fluorescence spectroscopy to be 30.5 ns. This contradicts the recent measurement using the high-frequency plused electron-beam excitation. We conjecture that, in their experiment, the radiation trapping not only affects the decay of the upper-level population but also relaxes the alignment initially produced by the electron-collision excitation in the upper-level population. Thus, the directly observed decay of the emission-line intensity is different from the decay of the upper-level population. We have observed the radiative relaxation of alignment on the neon 2 p 2 level which is a complementary effect to coherence narrowing.

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The Effect of Collisions on the Resonance Fluorescence Spectrum of Three-Level Atoms with a V-Configuration of Levels

А. И. Пархоменко, Anatolii M. Shalagin

The effect of collisions on the resonance fluorescence spectrum of three-level atoms with a V-configuration of levels when excited by two monochromatic resonance fields has been theoretically investigated. The analysis has been carried out for the systems with a small Doppler broadening compared to the collision frequency (high buffer gas pressures) and for the general case of an arbitrary change (from complete failure to complete preservation) of the phase memory at any of the three transitions in the V-system. It has been shown that in the three-level V-type atoms excited by two monochromatic fields, the resonant fluorescence spectrum (the number of spectral lines and their widths) at one of the transitions strongly depends on the presence of resonant radiation at the adjacent transition. Under certain conditions, the line widths will be completely determined by the relaxation characteristics of the adjacent transition and, in particular, can be repeatedly narrowed with an increase in the radiation intensity at the adjacent transition. It has been shown that despite the homogeneous nature of the broadening of the absorption lines, the resonance fluorescence spectrum has a pronounced anisotropy with respect to the mutual orientation of the wave vectors of spontaneous and exciting radiation. It has been established that the line widths in the resonance fluorescence spectrum are proportional to the diffusion coefficient of the atoms interacting with radiation under certain conditions. This fact can serve as the basis for a spectroscopic method for measuring the transport frequencies of the collisions of the radiation-absorbing particles with the buffer ones. It has been shown that the effects of phase memory in the collisions lead to a strong qualitative and quantitative modification of the resonance fluorescence spectrum.

Optics and Spectroscopy•Dec 1, 2021•1 citation
The lifetime of atoms and molecules can be measured by using modulated resonant single-mode laser field. A theoretical mode for this method is presented. It is shown that the laser induced fluorescence, a resonance flourescence is modulated at the same frequency, but phase shift from the exciting laser. The phase shift is mainly due to three processes (1) coherent excitation process characterized by transverse relaxation rate and line width of the laser, (2) population damping process characterized by the decay time of excited levels and other populated levels, (3) collision process characterized by the relaxation time by which the system to be in equilibrium state. The effect of these processes on measurement result is discussed. The Doppler broading is considered also.
The influence of relaxation parameters, as well as temporal fluctuations in the laser field on the modulation rate and phaseshift of the fluorescence from a two-level atom excited by a weakly modulated source is studied in detail. It is shown that, for intense resonant laser fields, the resonance in the modulation rate occurs at the modulation frequency Omega =2 due to the dynamical Stark splitting and has a width equal to 1 / 2 (T 1 -1 +T 2 -1 ). When temporal fluctuations of the exciting laser field are taken into account, the phaseshift of the scattered light is found to be strongly dependent on the bandwidth of the exciting source, as well as the frequency of modulation; hence experimental results on the determination of the lifetime by the phaseshift method have to be interpreted carefully. Numerical results for the modulation rates and phaseshift at different field strengths and various values of T 1 -1 , T 2 -1 , Delta laser bandwidth and Doppler broadening are presented.
This paper describes a new class of techniques, called time-delayed laser saturation spectroscopy, which combine frequency- and time-domain methods of laser spectroscopy to provide a way of studying a molecular system as it evolves from an initially prepared stationary state to a second, final state. The specific example analyzed here is three-level free induction decay, in which the time-dependent gain of a Doppler-broadened molecular transition is probed after the sudden termination of an intense field resonating with a coupled transition. The theoretical calculation is based on the coupled density-matrix equations of motion in the slowly-varying envelope approximation. The time-delayed line shapes, which may be studied in either transmission or side fluorescence, exhibit linewidth asymmetries, line-shape deformations, Ramsey-type fringes, power broadening and dephasing, and dynamic Stark splittings and oscillatory decays. The technique provides a unique way of distinguishing the influence of Raman-type processes from that of population saturation and a means to separately measure the associated decay rates. The relationship of the present work to other studies is also discussed.
It is shown that, if one uses an essentially monochromatic but weakly modulated light source to excite atoms or molecules in a resonant way, the phase shift of the scattered light is strongly dependent on the strength of the excitation. However, for low values of the excitation strength, this dependence disappears but a result which differs by a factor of two from the result obtained for broad-band light excitation is found. In addition, the strength of the modulated component of the scattered light displays a resonant behaviour in the modulation frequency, this response being directly related to the well-known Autler-Townes effect.
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.
We have measured the atomic lifetime of the argon 2 p 4 level by the laser-induced-fluorescence spectroscopy to be 30.5 ns. This contradicts the recent measurement using the high-frequency plused electron-beam excitation. We conjecture that, in their experiment, the radiation trapping not only affects the decay of the upper-level population but also relaxes the alignment initially produced by the electron-collision excitation in the upper-level population. Thus, the directly observed decay of the emission-line intensity is different from the decay of the upper-level population. We have observed the radiative relaxation of alignment on the neon 2 p 2 level which is a complementary effect to coherence narrowing.
The effect of collisions on the resonance fluorescence spectrum of three-level atoms with a V-configuration of levels when excited by two monochromatic resonance fields has been theoretically investigated. The analysis has been carried out for the systems with a small Doppler broadening compared to the collision frequency (high buffer gas pressures) and for the general case of an arbitrary change (from complete failure to complete preservation) of the phase memory at any of the three transitions in the V-system. It has been shown that in the three-level V-type atoms excited by two monochromatic fields, the resonant fluorescence spectrum (the number of spectral lines and their widths) at one of the transitions strongly depends on the presence of resonant radiation at the adjacent transition. Under certain conditions, the line widths will be completely determined by the relaxation characteristics of the adjacent transition and, in particular, can be repeatedly narrowed with an increase in the radiation intensity at the adjacent transition. It has been shown that despite the homogeneous nature of the broadening of the absorption lines, the resonance fluorescence spectrum has a pronounced anisotropy with respect to the mutual orientation of the wave vectors of spontaneous and exciting radiation. It has been established that the line widths in the resonance fluorescence spectrum are proportional to the diffusion coefficient of the atoms interacting with radiation under certain conditions. This fact can serve as the basis for a spectroscopic method for measuring the transport frequencies of the collisions of the radiation-absorbing particles with the buffer ones. It has been shown that the effects of phase memory in the collisions lead to a strong qualitative and quantitative modification of the resonance fluorescence spectrum.