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Physical Review Letters

Fluctuation Spectroscopy by Tunable Energy Compensation: Application to Radiator Reorientation Kernels

J. M. Liang, L. A. Spinelli, R. W. Quinn, Ramachandra Rao Dasari, Michael S. Feld, J. E. Thomas

Published Dec 9, 1985• 14 citations
Publisher

Abstract

A new method for investigating fluctuations in macroscopic coherences is suggested and demonstrated by measurement of radiator reorientation kernels in Stark-tunable infrared transitions of $^{13}\mathrm{C}$${\mathrm{H}}_{3}$F. The dominant ($\ensuremath{\Delta}M=1$) kernel is obtained by a scale transformation from the shape of a curve of two-pulse photon-echo intensity versus Stark voltage, at fixed large echo time delay.

DOI
10.1103/physrevlett.55.2684

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Experiments exploiting similarities for coherence collisional evolution in velocity space and in M space are reported. Generally, there is a total outgoing rate from any state and incoming rates (kernels) from neighboring states. Collision-induced velocity changes, ΔV, are studied with lasers by measuring the Doppler frequency Δ V/λ (λ = optical wavelength). To obtain information about coherence M transfer, it is only necessary to associate a frequency with each ΔM. This idea is demonstrated by measuring two-pulse photon echo intensity Ie for 13CH3F in a small dc Stark field. Acoustooptic modulation of infrared cw laser radiation, polarized parallel to the Stark field, is used to excite a number of uncoupled M → M transitions on the R(4,3) line. Each transition has a resonance frequency, vo + M· vs (vs is M = 1 Stark shift, Hz). A most remarkable result is obtained for large echo delays T with ΔVT/λ >> 1, all ΔV. The shape of the curve ln[ Ie(o)/ Ie(V)] vs Stark voltage V tends to that of the dominant coherence ΔM transfer kernel itself. Physically this arises because, for large T, the macroscopic coherence is preserved only for collisions where the frequency changing due to M transfer compensates the Doppler shift due to the ΔV, i.e., Δ V/λ + ΔM-·vs = 0. Generalizations are discussed.

Annual Meeting Optical Society of America•Jan 1, 1985•0 citations
A new method for investigating fluctuations in macroscopic coherences is suggested and demonstrated by measurement of radiator reorientation kernels in Stark-tunable infrared transitions of ^{13}\mathrm{C}$${\mathrm{H}}_{3}F. The dominant (\ensuremathΔM=1\ensuremath{\Delta}M=1\ensuremathΔM=1) kernel is obtained by a scale transformation from the shape of a curve of two-pulse photon-echo intensity versus Stark voltage, at fixed large echo time delay.
Radiator reorientation kernels are measured in Stark-tunable infrared transitions of 13CH3F. The dominant (ΔM = 1) kernel is obtained by a scale transformation from the shape of a two-pulse photon-echo intensity versus Stark voltage curve, at fixed large echo time delay. The quantum-mechanical transport equation in the presence of coherence M transfer and a dc electric field is reviewed, and the applications of photon echoes in a tunable Stark field to measure reorientation collision kernels are discussed.
We describe a new Stark sublevel photon echo technique for measuring fluctuations in macroscopic coherences. This idea is applied to the Stark tunable infrared (λ = 9 μm) R(4, 3, V3 = 0 → 1) transition of 13CH3F to measure, for the first time, the radiator reorientation velocity changing kernels WΔ M (Δv) which describe the rates (per unit velocity) at which the radiator orientation M changes by an amount ΔM accompanied by a velocity change Δv.1 In the experiments, two pulse photon echoes are obtained using a laser field polarized along an applied weak de Stark field ( z ^ direction) which shifts each M transition by Mvs (Hz).
Experiments exploiting similarities for coherence collisional evolution in velocity space and in M space are reported. Generally, there is a total outgoing rate from any state and incoming rates (kernels) from neighboring states. Collision-induced velocity changes, ΔV, are studied with lasers by measuring the Doppler frequency Δ V/λ (λ = optical wavelength). To obtain information about coherence M transfer, it is only necessary to associate a frequency with each ΔM. This idea is demonstrated by measuring two-pulse photon echo intensity Ie for 13CH3F in a small dc Stark field. Acoustooptic modulation of infrared cw laser radiation, polarized parallel to the Stark field, is used to excite a number of uncoupled M → M transitions on the R(4,3) line. Each transition has a resonance frequency, vo + M· vs (vs is M = 1 Stark shift, Hz). A most remarkable result is obtained for large echo delays T with ΔVT/λ >> 1, all ΔV. The shape of the curve ln[ Ie(o)/ Ie(V)] vs Stark voltage V tends to that of the dominant coherence ΔM transfer kernel itself. Physically this arises because, for large T, the macroscopic coherence is preserved only for collisions where the frequency changing due to M transfer compensates the Doppler shift due to the ΔV, i.e., Δ V/λ + ΔM-·vs = 0. Generalizations are discussed.