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Journal of Physics B Atomic and Molecular Physics

Photon correlation in resonance scattering-a new approach to the investigation of the excited states of atoms and molecules

Pavel A Apanasevich, S. Ya. Kilin, A F Fedorov

Published Feb 14, 1985• 2 citations
Publisher

Abstract

It is shown that analysis of the spectral time correlations of resonantly scattered photons is a new Doppler-free method for the investigating excited states of atoms and molecules. By using this method for investigation of the photon correlation, the times of transitions between excited states can be measured. Unlike the usual method of the delayed fluorescence the measurement can be accomplished with a continuous excitation of upper levels.

DOI
10.1088/0022-3700/18/3/005

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It is shown that analysis of the spectral time correlations of resonantly scattered photons is a new Doppler-free method for the investigating excited states of atoms and molecules. By using this method for investigation of the photon correlation, the times of transitions between excited states can be measured. Unlike the usual method of the delayed fluorescence the measurement can be accomplished with a continuous excitation of upper levels.
We describe a method to probe the spectral fluctuations of a transition over broad ranges of frequencies and timescales with the high spectral resolution of Fourier spectroscopy, and a temporal resolution as high as the excited state lifetime, even in the limit of very low photocounting rates. The method derives from a simple relation between the fluorescence spectral dynamics of a single radi-ating dipole and its fluorescence intensity correlations at the outputs of a continuously scanning Michelson interferometer. These findings define an approach to investigate the fast fluorescence spectral dynamics of single molecules and other faint light sources beyond the time-resolution capabilities of standard spectroscopy experiments.
Fluorescence photons emitted by a single molecule trapped in a solid at low temperature are correlated in time. A simple theory of the correlation pattern is presented, including in the same formalism photon antibunching from coherent Rabi oscillations and photon bunching due to incoherent quantum transitions between electronic levels. The correlation method is applied to single pentacene molecules in a para-terphenyl crystal. A clear photon bunching allows us to determine the ISC rates for each molecule. We attribute the scatter of our results for the transition rate between excited singlet and triplet states, and the difference with the average value taken from the literature, to molecular distortions induced by crystal defects in our small sample. We conclude that the correlation method associated to single molecule spectroscopy has a great potential to study dynamical processes on intermediate time scales in condensed matter.
Abstract Resonance scattering techniques are very useful for high-resolution atomic spectroscopy. The applicability of these techniques has been much extended, particularly through the rapid development of tunable-laser technology. The use of a narrow-band tunable laser, acting on a collimated atomic beam, gives a direct method enabling, for example, hyperfine structure and isotope shift studies. The intensity of lasers allows stepwise excitations to be performed, and with the two-photon absorption technique, Doppler-free measurements on thermal gases are also possible. By using pulsed lasers, time-resolved measurements yielding radiative life-times and structural information can be performed. The basic resonance scattering methods can be combined with radiofrequency and coherence techniques to yield a resolution, limited only by the uncertainty relation. Optical double resonance and level-crossing techniques, not requiring a narrow-band light source, have been extensively used. Several examples of the application of resonance scattering methods are given.
We consider a special kind of correlation measurements in single-atom resonance fluorescence, which includes detection of a spectrally filtered photon followed by detection of an unfiltered photon. We relate the stationary normalized intensity correlation function measured in such a scheme to the reduced atomic state following detection of the filtered photon. In the limit of well separated spectral lines of the resonance fluorescence spectrum, we obtain the analytic expression for the reduced atomic state. We show that at resonance excitation, this state is inverted when the filter is tuned in between the central line and any of the sidebands. This effect is interpreted as a result of quantum interference between the complementary atomic radiative transitions giving rise to the detected photon. We propose to observe this effect in measuring the equal-time field correlation function of the filtered and unfiltered photons as a function of the filter resonance frequency.
Two-time correlations in the emissions of photons by a single atom of sodium in the presence of a coherent exciting field near resonance have been investigated. In the experiment sodium atoms in an atomic beam are excited by a perpendicular light beam from a tunable dye laser, and they are prepared by optical pumping to behave as two-level quantum systems. The fluorescent light is collected by a microscope objective in a direction that is approximately orthogonal to both beams and imaged on two photomultipliers. Photoelectric pulse correlations are measured in the presence of exciting fields of various strengths and for various detunings from the atomic resonance, and are found to exhibit significant nonclassical features. The results show clearly that the emitted photons exhibit antibunching, in good quantitative agreement with the predictions of quantum electrodynamics.