There is a broad interest in enhancing the strength of light-atom interactions to the point where injecting a single photon induces a nonlinear material response. Here we show theoretically that sub-Doppler-cooled two-level atoms that are spatially organized by weak optical fields give rise to a nonlinear material response that is greatly enhanced beyond that attainable in a homogeneous gas. Specifically, in the regime where the intensity of the applied optical fields is much less than the off-resonance saturation intensity, we show that the third-order nonlinear susceptibility scales inversely with atomic temperature and, due to this scaling, can be two orders of magnitude larger than that of a homogeneous gas for typical experimental parameters. As a result, we predict that spatially bunched two-level atoms can exhibit single-photon nonlinearities. Our model is valid for all regimes of atomic bunching and simultaneously accounts for the backaction of the atoms on the optical fields. Our results agree with previous theoretical and experimental results for light-atom interactions that have considered only limited regimes of atomic bunching. For lattice beams tuned to the low-frequency side of the atomic transition, we find that the nonlinearity transitions from a self-focusing type to a self-defocusing type at a critical intensity. We also show that higher than third-order nonlinear optical susceptibilities are significant in the regime where the dipole potential energy is on the order of the atomic thermal energy. We therefore find that it is crucial to retain high-order nonlinearities to accurately predict interactions of laser fields with spatially organized ultracold atoms. The model presented here is a foundation for modeling low-light-level nonlinear optical processes for ultracold atoms in optical lattices.
There is a broad interest in enhancing the strength of light-atom interactions to the point where injecting a single photon induces a nonlinear material response. Here we show theoretically that sub-Doppler-cooled two-level atoms that are spatially organized by weak optical fields give rise to a nonlinear material response that is greatly enhanced beyond that attainable in a homogeneous gas. Specifically, in the regime where the intensity of the applied optical fields is much less than the off-resonance saturation intensity, we show that the third-order nonlinear susceptibility scales inversely with atomic temperature and, due to this scaling, can be two orders of magnitude larger than that of a homogeneous gas for typical experimental parameters. As a result, we predict that spatially bunched two-level atoms can exhibit single-photon nonlinearities. Our model is valid for all regimes of atomic bunching and simultaneously accounts for the backaction of the atoms on the optical fields. Our results agree with previous theoretical and experimental results for light-atom interactions that have considered only limited regimes of atomic bunching. For lattice beams tuned to the low-frequency side of the atomic transition, we find that the nonlinearity transitions from a self-focusing type to a self-defocusing type at a critical intensity. We also show that higher than third-order nonlinear optical susceptibilities are significant in the regime where the dipole potential energy is on the order of the atomic thermal energy. We therefore find that it is crucial to retain high-order nonlinearities to accurately predict interactions of laser fields with spatially organized ultracold atoms. The model presented here is a foundation for modeling low-light-level nonlinear optical processes for ultracold atoms in optical lattices.
Collective behavior in many-body systems, where the dynamics of an individual element depend on the state of the entire ensemble, play an important role in both basic science research and applied technologies. Over the last twenty years, studies of such effects in cold atomic vapors have lead to breakthroughs in areas such as quantum information science and atomic and condensed matter physics. Nevertheless, in order to generate photon-mediated atom-atom coupling strengths that are large enough to produce collective behavior, these studies employ techniques that intrinsically limit their applicability. In this thesis, I describe a novel nonlinear optical process that enables me to overcome these limitations and realize a new regime of collective light-matter interaction. My experiment involves an anisotropic cloud of cold rubidium atoms illuminated by a pair of counterpropagating optical (pump) fields propagating at an angle to the trap's long axis. When the pump beam intensities exceed a threshold value, a collective instability occurs in which new beams of light are generated spontaneously and counterpropagate along the trap's long axis. In order to understand the physical mechanism responsible for this behavior, I study first the system's nonlinear optical response when driven below the instability threshold. I find that the incident optical fields produce an optical lattice that causes the atoms to become spatially organized on the sub-wavelength length scale. This organization corresponds to the formation of an atomic density grating, which effectively couples the involved fields to one another and enables the transfer of energy between them. The loading of atoms into this grating is enhanced by my choice of field polarizations, which simultaneously results in cooling of the atoms from T~30 μK to T~3 μK via the Sisyphus effect. As a result, I observe a fifth-order nonlinear susceptibility χ^{(5)}=1.9x10^-12 (m/V)^4 that is 7 orders of magnitude larger than previously observed. In addition, because of the unique scaling of the resulting nonlinear response with material parameters, the magnitude of the nonlinearity can be large for small pump intensities (\\ie, below the resonant electronic saturation intensity 1.6 mW/cm^2) while simultaneously suffering little linear absorption. I confirm my interpretation of the nonlinearity by developing a theoretical model that agrees quantitatively with my experimental observations with no free parameters. The collective instability therefore corresponds to the situation where the cold vapor transitions spontaneously from a spatially-homogeneous state to an ordered one. This emergent organization leads to the simultaneous emission of new optical fields in a process that one can interpret either in terms of mirrorless parametric self-oscillation or superradiance. By mapping out the phase diagram for this transition, I find that the instability can occur for pump intensities as low as 1 mW/cm^2, which is approximately 50 times smaller than previous observations of similar phenomena. The intensity of the emitted light can be up to 20% of the pump beam intensity and depends superlinearly on the number of atoms, which is a clear signature of collective behavior. In addition, the generated light demonstrates temporal correlations between the counterpropagating modes of up to 0.987 and is nearly coherent over several hundred μs. The most significant attributes of the light, though, are that it consists of multiple transverse spatial modes and persists in steady-state. This result represents the first observation of such dynamics, which have been shown theoretically to lead to a rich array of new phenomena and possible applications.
We report a new nonlinear optical process that occurs in a cloud of cold atoms at low-light-levels when the incident optical fields simultaneously polarize, cool, and spatially-organize the atoms. We observe an extremely large effective fifth-order nonlinear susceptibility of χ(⁵) = 7.6 × 10⁻¹⁵ (m/V)⁴, which results in efficient Bragg scattering via six-wave mixing, slow group velocities (∼ c/10⁵), and enhanced atomic coherence times (> 100 μs). In addition, this process is particularly sensitive to the atomic temperatures, and provides a new tool for in-situ monitoring of the atomic momentum distribution in an optical lattice. For sufficiently large light-matter couplings, we observe an optical instability for intensities as low as ∼ 1 mW/cm² in which new, intense beams of light are generated and result in the formation of controllable transverse optical patterns.
The nonlinear interaction between light and atoms is an extensive field of study with a broad range of applications in quantum information science and condensed matter physics. Nonlinear optical phenomena occurring in cold atoms are particularly interesting because such slowly moving atoms can spatially organize into density gratings, which allows for studies involving optical interactions with structured materials. In this thesis, I describe a novel nonlinear optical effect that arises when cold atoms spatially bunch in an optical lattice. I show that employing this spatial atomic bunching provides access to a unique physical regime with reduced thresholds for nonlinear optical processes and enhanced material properties. Using this method, I observe the nonlinear optical phenomenon of transverse optical pattern formation at record-low powers. These transverse optical patterns are generated by a wave- mixing process that is mediated by the cold atomic vapor. The optical patterns are highly multimode and induce rich non-equilibrium atomic dynamics. In particular, I find that there exists a synergistic interplay between the generated optical pat- terns and the atoms, wherein the scattered fields help the atoms to self-organize into new, multimode structures that are not externally imposed on the atomic sample. These self-organized structures in turn enhance the power in the optical patterns. I provide the first detailed investigation of the motional dynamics of atoms that have self-organized in a multimode geometry. I also show that the transverse optical patterns induce Sisyphus cooling in all three spatial dimensions, which is the first observation of spontaneous three-dimensional cooling. My experiment represents a unique means by which to study nonlinear optics and non-equilibrium dynamics at ultra-low required powers.
This thesis summarizes the research work we did in the past years, which focuses on the theoretical study of quantum effects of ordered atomic structures interacting with the quantum electric field of an optical resonator. Within this work we investigated the quantum properties of the light at the cavity output, emitted by this kind of system, and the quantum state of the atoms confined by the light fields of the cavity mode. Following one possible partition, we have organized the thesis in two parts. The first part of the thesis is devoted to the quantum properties of the light at the output of optical cavities, in which atoms are confined. After a brief introduction on the basics of atom-photon interactions, we show theoretically, that two atomic dipoles in a resonator can behave as a quantum non-linear medium, whose response can be controlled through the interactomic distance of the atoms inside the resonator. We identify the parameter regime, for which the system operates as a parametric amplifier, based on the atoms' collective dipole cascade emission. Moreover we also determine the corresponding field squeezing spectrum at the cavity output. These dynamics could be observed as a result of self-organization processes of laser-cooled atoms in resonators. The second part of the thesis studies the quantum ground state of an ultracold atomic gas trapped inside an optical resonator by the mechanical effects of atom-photon interactions. Due to the strong coupling regime, the ultracold atomic gas feels a quantum potential, where the fluctuations at the single photon level may be relevant in determining the trapping conditions. This potential depends on the atomic distribution, which at the same time determines the intracavity field amplitude. Here, after a brief introduction on ultracold atoms in optical lattices, we study the low temperature physics of an ultracold atomic gas in the quantum potential formed inside a pumped cavity, by mapping the dynamics to an effective Bose-Hubbard model. We predict the existence of non-compressible states of the atomic gas, and determine a phase diagram as a function of the cavity parameters. Novel effects are encountered, such as the existence of overlapping stability regions corresponding to competing insulator-like states when the laser pumps the cavity, to provide one example out of many. At the end of the thesis a concluding chapter presents some general outlooks to this thesis work.
We predict and experimentally demonstrate a type of collective (cooperative) coupling effect where a disordered atomic ensemble absorbs light with a rise time longer (i.e., at a rate slower) than what is dictated by single-atom physics. This effect, which we name subabsorption, can be viewed as the absorptive analog of subradiance. The experiment is performed using a dilute ensemble of ultracold 87Rb atoms with a low optical depth, and time resolving the absorption of a weak (tens of photons per pulse) resonant laser beam. In this dilute regime, the collective interaction relies on establishing dipole-dipole correlations over many atoms; i.e., the interaction is not dominated by the nearest neighbors. As a result, subabsorption is highly susceptible to motional dephasing: even a temperature increase of $60\phantom{\rule{0.28em}{0ex}}\textmu{}\mathrm{K}$ is enough to completely extinguish the subabsorption signal. We also present a theoretical model whose results are in reasonable agreement with the experimental observations. The model uses the density-dependent dephasing rate of the long-range dipole-dipole correlations as a single adjustable parameter. Experiment-theory comparison indicates a dephasing coefficient of $\ensuremath{\beta}/2\ensuremath{\pi}=4.9\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}5}\phantom{\rule{0.28em}{0ex}}\mathrm{Hz}\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{3}$, which is more than two orders of magnitude larger than the known dipole-dipole line broadening coefficient in 87Rb.
The study of transverse optical pattern formation has been studied extensively in nonlinear optics, with a recent experimental interest in studying the phenomenon using cold atoms, which can undergo real-space self-organization. Here, we describe our experimental observation of pattern formation in cold atoms, which occurs using less than 1 μW of applied power. We show that the optical patterns and the self-organized atomic structures undergo continuous symmetry breaking, which is characteristic of nonequilibrium phenomena in a multimode system. To theoretically describe pattern formation in cold atoms, we present a self-consistent model that allows for tight atomic bunching in the applied optical lattice. We derive the nonlinear refractive index of a gas of multilevel atoms in an optical lattice, and we derive the threshold conditions under which pattern formation occurs. We show that by using small detunings and sub-Doppler temperatures, one achieves intensity thresholds for pattern formation that are reduced by two orders of magnitude compared to warm atoms.