The limits of the well-established single-atom model for describing photon-pair generation via four-wave mixing in a diamond configuration in atomic ensembles are experimentally tested. Using a cold-atom source, biphotons are generated and detected through polarization analyzers that resolve the emitted light into horizontal and vertical components in the laboratory frame. The pump lasers driving the first and second excitation transitions are horizontally and vertically polarized, respectively. To predict single-photon counts and coincidence rates in all polarization channels, the first- and second-order correlation functions are calculated directly using a comprehensive model that accounts for all Zeeman sublevels of the relevant hyperfine states. Furthermore, the population dynamics with and without the re-pump laser of the magneto-optical trap are compared, revealing substantial differences in the populations of the Zeeman sublevels. This motivates the inclusion of two additional hyperfine levels and their corresponding Zeeman sublevels in the final model. The resulting density matrix is used to calculate expectation values of the far-field electric-field operators and compare them with experimental measurements over a range of pump-laser powers. Excellent agreement with the measured photon counts is obtained over most of this range. For the coincidence measurements, good agreement is found when the polarization of the photon generated by the first (second) decay is parallel to that of the first (second) pump beam. In contrast, the model consistently underestimates the experimental coincidence rates for the opposite polarization configuration. These findings indicate that effects beyond the internal level dynamics of individual atoms, most notably collective phenomena, are required to fully account for photon coincidences generated by four-wave mixing in atomic ensembles.
The limits of the well-established single-atom model for describing photon-pair generation via four-wave mixing in a diamond configuration in atomic ensembles are experimentally tested. Using a cold-atom source, biphotons are generated and detected through polarization analyzers that resolve the emitted light into horizontal and vertical components in the laboratory frame. The pump lasers driving the first and second excitation transitions are horizontally and vertically polarized, respectively. To predict single-photon counts and coincidence rates in all polarization channels, the first- and second-order correlation functions are calculated directly using a comprehensive model that accounts for all Zeeman sublevels of the relevant hyperfine states. Furthermore, the population dynamics with and without the re-pump laser of the magneto-optical trap are compared, revealing substantial differences in the populations of the Zeeman sublevels. This motivates the inclusion of two additional hyperfine levels and their corresponding Zeeman sublevels in the final model. The resulting density matrix is used to calculate expectation values of the far-field electric-field operators and compare them with experimental measurements over a range of pump-laser powers. Excellent agreement with the measured photon counts is obtained over most of this range. For the coincidence measurements, good agreement is found when the polarization of the photon generated by the first (second) decay is parallel to that of the first (second) pump beam. In contrast, the model consistently underestimates the experimental coincidence rates for the opposite polarization configuration. These findings indicate that effects beyond the internal level dynamics of individual atoms, most notably collective phenomena, are required to fully account for photon coincidences generated by four-wave mixing in atomic ensembles.
We report an investigation to establish the physical mechanisms responsible for decoherence in the generation of photon pairs from atomic ensembles, via the protocol of Duan et al. for long-distance quantum communication [Nature (London) 414, 413 (2001)] and present the experimental techniques necessary to properly control the process. We develop a theory to model in detail the decoherence process in experiments with magneto-optical traps. The inhomogeneous broadening of the ground state by the trap magnetic field is identified as the principal mechanism for decoherence. The theory includes the Zeeman structure of the atomic hyperfine levels used in the experiment, and the polarization of both excitation fields and detected photons. In conjunction with our theoretical analysis, we report a series of measurements to characterize and control the coherence time in our experimental setup. We use copropagating stimulated Raman spectroscopy to access directly the ground-state energy distribution of the ensemble. These spectroscopic measurements allow us to switch off the trap magnetic field in a controlled way, optimizing the repetition rate for single-photon measurements. With the magnetic field off, we then measure nonclassical correlations for pairs of photons generated by the ensemble as a function of the storage time of the single collective atomic excitation. We report coherence times longer than $10\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$, corresponding to an increase of two orders of magnitude compared to previous results in cold ensembles. The coherence time is now two orders of magnitude longer than the duration of the excitation pulses. The comparison between these experimental results and the theory shows good agreement. Finally, we employ our theory to devise ways to improve the experiment by optical pumping to specific initial states.
This thesis discusses four-wave mixing (4WM) in a warm ensemble of rubidium using the diamond configuration level structure. Both classical 4WM and non- classical photon-pair production are investigated. Quantum information science has spawned a great amount of experimental work on the interaction of light with collective modes of excitation in atomic ensem- bles. Plans to build quantum networks and quantum repeaters with atom ensembles take advantage of nonlinear interactions to produce and store non-classical states of light. These technologies will require photon sources that not only generate non- classical light, but also resonant, narrow band light. Here we investigate a system which could be used as such a source. We take advantage of the 4WM interaction in a warm ensemble of Rubidium atoms. Our scheme utilizes the diamond energy level configuration which, in ru- bidium, allows for correlated pairs at telecommunications wavelengths. We start by examining the properties of classical 4WM in the system. We measure the reso- nance structure and see that it can be understood in terms of velocity class selective resonant enhancement and power splitting effects. The efficiency of the process is low and limited by linear absorption of the pumps. Our observations agree with a semi-classical Maxwell-Bloch theoretical treatment. Next we observe pair generation by spontaneous 4WM from the warm ensem- ble. The temporal profile of the cross-correlation function (CCF) for the photons depends on pump-laser power and detuning. This allows us to produce biphotons with controllable spectra. A simple quantum optical theoretical treatment based on linear filtering gives qualitative agreement with the data. We show that the photon pairs are polarization entangled, clearly violating Bell's Inequality. A perturbative quantum optical treatment predicts the polariza- tion state of the pairs and agrees with our measurements. We analyze the photon statistics of the source and find the largest violation of the two beam Cauchy-Schwarz inequality from a warm atomic source yet. We cast the system as a heralded sin- gle photon source at telecommunications wavelengths and see that it is competitive with other systems in terms of spectral brightness.
In this work, we present a set of experiments involving four-wave mixing processes in rubidium atoms. We employ several experimental configurations exploring two- and three-level systems in cascade or Λ configurations, all of which are in a copropagating geometry, to investigate different physical phenomena present in each scenario. In the first experiment, we combine a cw diode laser and a 1 GHz femtosecond pulse train to generate coherent blue light through the four-wave mixing process in hot rubidium vapor. The generated coherent signal is analyzed by scanning either the diode frequency or the repetition rate of the frequency comb. In both cases, the cw laser induces an Autler- Townes splitting with a wide separation in the doublet structure due to the configuration of copropagating fields. To model these results, we employ the density matrix formalism to write the Bloch equations and solve them numerically. The solutions allow us to explore other cases beyond those involving our experimental setup, comparing the response of the upper-level population and the generated signal coherence for homogeneously and non-homogeneously broadened systems. Moreover, in this same experiment, we also observed an unexpected interference effect between excitation routes of the four-wave mixing process when the repetition rate of the pulse train is scanned. The theoretical model demonstrates that the interfering effect appears only when the repetition rate is carefully chosen to produce a pair of modes of the frequency comb resonant with both one- and two-photon transitions for the same atomic velocity group. In the second experiment, still with a hot rubidium vapor, we explore two symmetrical degenerate four- wave mixing signals induced by two almost copropagating laser beams, with~ka and~kb wave-vectors, and detected simultaneously in the 2~ka −~kb and 2~kb −~ka directions. Each spectrum has a single peak with a short frequency separation between them, which our model indicates is due to the nonlinear behavior of the refractive indexes, a consequence of the high intensity of both input fields. Finally, we use the same experimental setup for the two symmetrical signals to study the field intensity fluctuations of the degenerate four-wave mixing signals and the transmission signals. In this case, the sample is an ensemble of cold rubidium atoms in a magneto-optical trap. There is an intensity- intensity cross-correlation between the signals due to the resonant phase-noise to amplitude-noise conversion. In this type of cold system, we can neglect the Doppler- broadening, allowing a straightforward study of the dependency of the correlations on the laser detuning. In these measurements, we observe a type of oscillation in the correlation curves that the theoretical model indicates to be connected with Rabi oscillations, revealed by the fluctuations long after the transient period.
In this paper we report on the study of two and multi-level atoms interacting with multiple laser beams. The semi-classical approach is used to describe the system in which the atoms are treated quantum mechanically via the density matrix operator, while the laser beams are treated classically using Maxwells equations. We present results of a two level atom interacting with single and multiple laser beams and demonstrate Rabi oscillations between the levels. The effects of laser modulation on the dynamics of the atom (atomic populations and coherences) are examined by solving the optical Bloch equations. Plots of the density matrix elements as a function of time are presented for various parameters such as laser intensity, detuning, modulation etc. In addition, phase-space plots and Fourier analysis of the density matrix elements are provided. The atomic polarization, estimated from the coherence terms of the density matrix elements, is used in the numerical solution of Maxwells equations to determine the behaviour of the laser beams as they propagate through the atomic ensemble. The effects of saturation and hole-burning are demonstrated in the case of two counter propagating beams with one being a strong beam and the other being very weak. The above work is extended to include four-wave mixing in four level atoms in a diamond configuration. Two co-propagating beams of different wavelengths drive the atoms from a ground state |1〉 to an excited state |3〉 via an intermediate state |2〉. The atoms then move back to the ground state via another intermediate state |4〉, resulting in the generation of two additional correlated photon beams. The characteristics of these additional photons are studied.
The physics of the degenerate four-wave mixing process for resonant transitions between two degenerate energy levels is investigated by direct numerical integration of the time-dependent density matrix equations. The Zeeman structure of the upper and lower energy levels is included in a multistate formulation of the density matrix equations. The inclusion of the Zeeman structure enables the investigation of the degenerate four-wave mixing process for different polarization configurations of the forward pump, backward pump, and probe beams. Saturation curves and lineshapes are calculated for different polarization configurations and for numerous low-J transitions. At low laser intensity, the results of our calculations are in excellent agreement with perturbation theory in terms of the relative intensities of the degenerate four-wave mixing signal for linear polarization configurations. As the laser intensity increases and the resonance starts to saturate, we find in general that the relative degenerate four-wave mixing reflectivity increases for the crossed polarization configurations compared to the parallel polarization configuration because the saturation intensity is higher. However, for some resonance transitions, some of the crossed polarization configurations saturate at lower laser intensities than the parallel polarization configuration, even though the reflectivity for these crossed polarization configurations is much lower than for the parallel polarization configuration in the perturbative intensity limit. This result is explained in terms of the coupling of the various Zeeman states during the degenerate four-wave mixing interaction for specific polarization configurations. The effect of saturation on the resonance line shapes for the different polarization configurations is also investigated. Finally, a limited number of calculations are performed for resonances that are Doppler broadened as well as collision broadened. The effect of saturation on the reflectivity of the crossed polarization configurations compared to the parallel polarization configuration is even more significant for resonances with comparable Doppler and collisional broadening.
Microscopic models based on multilevel atoms are central to optimizing nonlinear optical responses and the coherent control of light. These models are traditionally based on single-atom effects that are parametrically extrapolated to include collective effects, such as an enhanced response or propagation within atomic media. In this work, we present a systematic analysis of the cooperative effects arising in driven systems composed of multilevel atoms coupled via a common electromagnetic environment. The analysis is based on an interplay between dressed states induced by the driving field and photon exchanges, and collective decay channels. This theory is applied to the case of four-wave mixing induced by a pair of lasers acting on an atomic pair with internal levels in the diamond configuration. The effect of interatomic correlations and collective decay over the photons created in this nonlinear process is then explored. We identify three regions of operation: (i) laser-dominated, (ii) intermediate, and (iii) dipole-dominated. The dependence of single- and two-photon correlations is studied in detail for each region by varying atomic orientations and laser parameters consistent with current experiments involving atomic gases. Photonic correlation functions are shown to exhibit a transition from a Lorentz-like dependence on the two-photon detuning—with general features that can be obtained in an isolated atom scheme—to a two-peaked distribution when the dipole-dipole interactions become relevant. For weak Rabi frequencies whose value is smaller than the highest collective decay rate, the atoms are trapped inside their ground state as they approach each other. It is found that the anisotropy of the dipole-dipole interaction and its wave nature are essential to understand the behavior of the photon correlations. Signatures of these processes are identified for existing experimental realizations. The intuition obtained from this connection helps to uncover relevant parameters that could be exploited for quantum control protocols based on dispersive and dissipative cooperative effects in multilevel systems.