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Physical Review A

Quantum features of resonance fluorescence as probes of two-atom dynamical correlations

Gershon Kurizki

Published Mar 1, 1991• 11 citations
Publisher

Abstract

A system of two colliding neutral or ionized atoms with excited states that exhibit fine-structure splitting is shown to emit resonance fluorescence, the quantum features of which can reveal the collisional dynamical correlations between the atoms. Time-resolved measurements of quantum noise (squeezing properties) of the emitted field are shown to yield detailed information on the dynamical correlations. Notably, they disclose the phase between the dynamically correlated two-atom adiabatic states, which is not available from conventional spectroscopy. Such phase information can be a sensitive probe of collision dynamics. It is also important for the achievement of enhanced selectivity in laser-induced reactive collisions or dissociation, based on controllable coherent superpositions of adiabatic states.

DOI
10.1103/physreva.43.2599

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Journal of Physics B Atomic and Molecular Physics•Jan 28, 1980•102 citations
A system of two colliding neutral or ionized atoms with excited states that exhibit fine-structure splitting is shown to emit resonance fluorescence, the quantum features of which can reveal the collisional dynamical correlations between the atoms. Time-resolved measurements of quantum noise (squeezing properties) of the emitted field are shown to yield detailed information on the dynamical correlations. Notably, they disclose the phase between the dynamically correlated two-atom adiabatic states, which is not available from conventional spectroscopy. Such phase information can be a sensitive probe of collision dynamics. It is also important for the achievement of enhanced selectivity in laser-induced reactive collisions or dissociation, based on controllable coherent superpositions of adiabatic states.
The phenomenon of resonance fluorescence provides an interesting manifestation of the quantum theory of light and is a “real world” application of the material of the Chapters 8 and 9. In this process, a two-level atom is typically driven by a resonant continuous-wave laser field and the spectral and quantum statistical properties of the fluorescent light emitted by the atom are measured. Experimentally this can be achieved by scattering a laser off a collimated atomic beam such that the directions of the laser beam, atomic beam, and detector axis are mutually perpendicular as shown in Fig. 10.1. If the driving field is monochromatic, then at low excitation intensity the atom absorbs a photon at the excitation frequency and reemits it at the same frequency as a consequence of conservation of energy. The spectral width of the fluorescent light is therefore very narrow. The situation, however, is considerably more complicated when the excitation intensity increases and the Rabi frequency associated with the driving field becomes comparable to, or larger than, the atomic linewidth. At such intensity levels, the Rabi oscillations show up as a modulation of the quantum dipole moment and sidebands start emerging in the spectrum of the emitted radiation. This so-called dynamic Stark splitting is an interesting feature of the atom–field interaction. In addition to that, the fluorescent light exhibits certain nonclassical properties including photon antibunching and squeezing. In this chapter, we develop a theory of resonance fluorescence to explain these phenomena.
We discuss the phase-sensitive noise properties of fluorescence emitted by three-level atoms coherently excited by two laser fields, using both undressed and dressed uncoupled-state representations. The occurrence of steady-state squeezing is found to be highly sensitive to relaxation processes between the two-photon resonant levels. For purely radiative decay from the upper level, and no lower-state relaxation, the population is susceptible to coherent population trapping. Near two-photon resonance, the atom is optically pumped into a nonabsorbing (trapped) superposition state, which, although it reduces upper-level population, also leads to an interference cancellation of dipole moments and to suppression of squeezing. Lower-level relaxation unbalances this interference and restores the squeezing to some extent. Transient squeezing is also predicted in the time-dependent fluorescence.
Phase-sensitive detection of resonance fluorescence, i.e., allowing the light emitted from an atom which is undergoing Rabi oscillations in free space to interfere with a coherent local oscillator (LO) beam, has drawn considerable attention throughout the history of quantum optics. Recently, phase-sensitive squeezing spectra for single-atom resonance fluorescence were observed for the first time using strongly-driven long-lived atoms. A measurement of phase-sensitive intensity correlations for this system will be presented. Using physical arguments I will construct the phase-sensitive two-time intensity autocorrelation function, and elucidate the role played by quantum fluctuations in phase-dependent resonance fluorescence.
Phase-sensitive squeezing in the resonance fluorescence of two-level atoms, that are coherently driven by a near-resonant laser field in free space, was observed recently (Lu et al 1998 Phys. Rev .L ett. 81 3635). This was accomplished via homodyne detection at a phase near ±45 ◦ relative to the driving field for strong off-resonant excitation of ‘long-lived’ atoms (where th ea tomic lifetime far exceeded the laser–atom interaction time, meaning that relaxation effects could be ignored). On the other hand, traditional theoretical predictions of phase-sensitive squeezing in the resonance fluorescence from two-level atoms have emphasized in- and out-of-phase (i.e., 0 ◦ and 90 ◦ ) quadratures, and weak, on-resonant excitation of ‘short-lived’ atoms (where the observation time for laser–atom interaction fa re xceeded the natural atomic lifetime, meaning that relaxation effects dominate). Here, we calculate the probability of a delayed-coincidence detection in the interference field of a fluorescing dipole with a local oscillator (LO). We show that, despite the strikingly different conditions in which squeezing occurs in short- and long-lived atoms, squeezing in both cases can be shown to arise from a joint detection of two photons which are related by a quantum jump in the following way: the first photodetection precipitates a quantum jump of the atom to the ground state, and the second measures the mean amplitude of the fluorescent field subsequent to the quantum jump.
The resonance fluorescence of a two-level atom interacting with a laser pulse is studied, following the short-pulse approximation. The authors demonstrate that an explicit expression of the energy spectrum in terms of atomic-state amplitudes holds also for an off-resonance excitation. Some analytically solvable cases are studied in detail, showing that the main spectral properties of the fluorescence emitted under adiabatic and non-adiabatic pulsed excitation can be easily described. For the first time the continuous dependence of the fluorescence spectrum on laser detuning is reported for a smooth pulse.
Attention is focused on the dynamic evolution of the emission spectrum following abrupt excitation of a near-resonant two-level absorber by a strong laser field. The multiphoton character of the absorption-emission process is evident in the AC Stark splitting of the spectrum, which begins approximately half an atomic lifetime after excitation, if the laser field is strong enough. Analytic expressions for the spectra are given of arbitrary laser field strength, atomic lifetime, laser-atom detuning, and the bandwidth of the spectrometer used to analyse the spectrum. Selected graphs are included to illustrate various time-dependent features of the spectrum. The influence on the transient spectrum of three different states of atomic excitation prior to laser irradiation and the effect on the spectrum of irradiation by a phase-noisy laser are also considered. Comparison of the transient spectra from atoms initially prepared in ' pi /2' and '3 pi /2' states show clearly that phase relationships between the irradiating field and the emitting dipole are important even in fluorescence.