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Physical Review A

Atoms as nonlinear mixers for detection of quantum correlations at ultrahigh frequencies

N. Ph. Georgiades, Eugene Simon Polzik, Harry J. Kimble

Published Mar 1, 1997• 56 citations
Publisher

Abstract

Measurements of quantum correlations are reported for a frequency difference of 25 THz between the signal and idler output fields generated by a subthreshold nondegenerate optical parametric oscillator. By simultaneously exciting a two-photon transition in atomic Cs by a combination of signal, idler, and ``references oscillator'' fields, we record modulation of the excited-state population due to quantum interference between two alternative excitation pathways. The observed phase-sensitive modulation is proportional to the correlation function 〈E-|${\mathrm{Ax}}_{\mathrm{s}}$E-|${\mathrm{Ax}}_{\mathrm{i}}$〉 for the quantized signal and idler fields.

DOI
10.1103/physreva.55.r1605

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Measurements of quantum correlations are reported for a frequency difference of 25 THz between the signal and idler output fields generated by a subthreshold nondegenerate optical parametric oscillator. By simultaneously exciting a two-photon transition in atomic Cs by a combination of signal, idler, and ``references oscillator'' fields, we record modulation of the excited-state population due to quantum interference between two alternative excitation pathways. The observed phase-sensitive modulation is proportional to the correlation function 〈E-|Axs{\mathrm{Ax}}_{\mathrm{s}}Axs​E-|Axi{\mathrm{Ax}}_{\mathrm{i}}Axi​〉 for the quantized signal and idler fields.
Two-photon excitation of a three-level atom in a ladder configuration $(\stackrel{\ensuremath{\rightarrow}}{1}\stackrel{\ensuremath{\rightarrow}}{2}3)$ by simultaneous illumination with fields in squeezed vacuum and coherent states results in quantum interference for the excitation process. The particular configuration considered here is one for which the signal and idler output fields of a subthreshold nondegenerate optical parametric oscillator are in resonance with the two-stepwise dipole atomic transitions $(\stackrel{\ensuremath{\rightarrow}}{1}2,\stackrel{\ensuremath{\rightarrow}}{2}3),$ while a ``reference oscillator'' field is in two-photon resonance with the quadrupole transition $(\stackrel{\ensuremath{\rightarrow}}{1}3).$ In an extension of the work of Ficek and Drummond [Phys. Rev. A 43, 6247 (1991)], a theoretical formulation based on the full quantum master equation for the problem is presented. The combined effects of quantum interference and the nonclassical character of the squeezed state are investigated, and offer the potential for a new detection strategy for quantum fluctuations of the electromagnetic field with ultrahigh frequencies (10's--100's THz). Based on the theory developed, we analyze quantum interference in excitation in several special cases relevant to experimental realizations, including the effects of a small focusing angle of the squeezing onto the atoms, and unusual population inversions. Special emphasis is given to identifying intrinsically quantum optical field effects versus classical field effects. Procedures that could distinguish between the two (i.e., classical and nonclassical) are suggested.
Non-classical properties and quantum interference (QI) in two-photon excitation of a three level atom (|1〉), |2〉, |3〉) in a ladder configuration, illuminated by multiple fields in non-classical (squeezed) and/or classical (coherent) states, is studied. Fundamentally new effects associated with quantum correlations in the squeezed fields and QI due to multiple excitation pathways have been observed. Theoretical studies and extrapolations of these findings have revealed possible applications which are far beyond any current capabilities, including ultrafast nonlinear mixing, ultrafast homodyne detection and frequency metrology. The atom used throughout the experiments was Cesium, which was magneto-optically trapped in a vapor cell to produce a Doppler-free sample. For the first part of the work the |1〉 → |2〉 → |3〉 transition (corresponding to the 6S1/2F = 4 → 6P3/2F' = 5 → 6D5/2F = 6 transition) was excited by using the quantum-correlated signal (Ɛs) and idler (Ɛi) output fields of a subthreshold non-degenerate optical parametric oscillator, which was tuned so that the signal and idler fields were resonant with the |1〉 → |2〉 and |2〉 → |3〉 transitions, respectively. In contrast to excitation with classical fields for which the excitation rate as a function of intensity has always an exponent greater than or equal to two, excitation with squeezed-fields has been theoretically predicted to have an exponent that approaches unity for small enough intensities. This was verified experimentally by probing the exponent down to a slope of 1.3, demonstrating for the first time a purely non-classical effect associated with the interaction of squeezed fields and atoms. In the second part excitation of the two-photon transition by three phase coherent fields Ɛ1 , Ɛ2 and Ɛ0, resonant with the dipole |1〉 → |2〉 and |2〉 → |3〉 and quadrupole |1〉 → |3〉 transitions, respectively, is studied. QI in the excited state population is observed due to two alternative excitation pathways. This is equivalent to nonlinear mixing of the three excitation fields by the atom. Realizing that in the experiment the three fields are spaced in frequency over a range of 25 THz, and extending this scheme to other energy triplets and atoms, leads to the discovery that ranges up to 100's of THz can be bridged in a single mixing step. Motivated by these results, a master equation model has been developed for the system and its properties have been extensively studied.
For measurements describable by a discrete set of possibilities, numerous demonstrations of the violation of Bell's inequalities have been reported in optical physics based on observations of polarization correlations for photon pairs. By contrast for observables with a continuous spectrum, there appears to be no general inequalities corresponding to those of Bell and no experimental realization of the original Einstein-Podolsky-Rosen paradox. Following Reid and Drummond,1 we are attempting to demonstrate the EPR paradox in the context of the measurement of continuous quantum variables with a subthreshold optical parametric oscillator operated in a frequency degenerate but polarization nondegenerate mode. In this case, the EPR paradox is formulated in terms of two sets of quadrature phase amplitudes for the spatially separated signal and idler fields. As the parametric gain is increased toward threshold, the quadrature amplitudes of the signal and idler beams become increasingly faithful quantum copies of one another. Our measurements of quadrature amplitudes are carried out using independent balanced homodyne detectors at two sites. When operated for the detection of squeezing at one site, noise reductions of 4 dB relative to the vacuum state limit are observed, which is most encouraging since noise reductions >3 dB in the difference photocurrent from the two sites are sufficient for inference at a distance of a signal observable from a measurement of the corresponding idler variable.
We have carried out a linearized quantum analysis of the steady-state operation of an optical parametric oscillator (OPO) without cavity detunings; our analysis emphasizes the effects of pump quantum noise and pump excess noise. We show that pump excess noise reduces the observable signal/idler intensity correlation at low frequencies only in the presence of a cavity-loss mismatch between these subharmonic waves. This effect is so strong that the combination of pump excess noise and cavity-loss mismatch explains the rapid low-frequency noise increase well above the shot-noise level that has been seen in recent signal/idler correlation measurements. Moreover, the critical dependence of intensity correlation on cavity-loss mismatch opens a new possibility for ultrasensitive intracavity absorption spectroscopy. Specifically, sinusoidal amplitude modulation of the OPO pump beam with lock-in amplification of the signal/idler photocurrent affords a sensitive probe of subharmonic cavity-loss mismatch. Although this robust measurement capability exploits the strong intracavity correlation between the signal and idler waves, it does not require that nonclassical correlation be externally observable, nor is it limited to near-threshold OPO operation.
SUMMARY Parametric processes in the interaction of electromagnetic field with a medium in an optical cavity are well known to produce states of light with nonclassical properties. The quantum correlations between these states can be employed for a realization of an EinsteinPodolsky-Rosen (EPR) paradox [l], in the original formulation using continuous variables, as proposed [2] and experimentally demonstrated [3] in the case of Nondegenerate Parametric Amplification below threshold. In this paper we study EPR-like behaviour between the signal and idler fields emitted by a degenerate optical parametric oscillator (OPO) above threshold; these fields, generated by conversion of a pump photon of frequency 2w0 in two photons of frequency w. , are spatially separated in the far field, showing non-local quantum correlations. The system is described by the full Hamiltonian for the operators associated with the pump and signal fields; the optical cavity introduces proper damping constants and corresponding vacuum field operators [4,5]. Above the threshold for the generation of the signal field, we consider the fluctuations in the intensity difference and in the phase sum of the signal beams, which are related to their degree of mutual correlation. By linearizing around the stationary state, we calculate the spectral variances of these quantities (i.e. the Fourier transform of the two time correlation functions). The Heisenberg uncertainty principle sets a lower limit to the product of the spectral variances for the fluctuations in the intensity and in the phase of each individual signal field; by using the idler beam to infer results of measurements on the correlated signal beam, we have an EPR paradox if the product of the spectral variances for the fluctuations in the intensity difference and phase sum of the fields, is below the uncertainty limit. This feature is apparent for a wide interval around zero frequency in the far field of the active OPO system, depending on the parameter space; in particular there is maximum correlation between signal beams, and therefore maximum breaking of the uncertainty limit, if the damping constant of the signal field is larger than that of the pump field.