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.
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 T30 μK to T3 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.
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.
The objective of this thesis is to expand our understanding of collective light-scattering phenomena, which manifest themselves in the strong suppression of radiation from the scattering medium. In particular, we are interested in subradiance, a collective effect in spontaneous emission which, as a result of the dissipative coupling of atoms through common electromagnetic modes, creates long-lived excitation modes in an ensemble of cold atoms, with lifetimes much longer than those of individual, isolated atoms. Previously, subradiance had been well-characterized for dilute cold-atom scattering media and the low-intensity limit of the driving laser (linear-optics regime). In this thesis, we study this collective phenomenon beyond the linear-optics and dilute regimes.To study experimentally subradiance beyond the linear-optics regime, we varied the saturation parameter of the excitation laser up to relatively large values and we have observed the increase of the subradiant population with increasing saturation parameter. More importantly, we have identified the super-linear scaling of the subradiant population beyond the linear-optics regime, due to a process similar to optical pumping via multi-excitation superradiant states. This study showed that the increase in the intensity of the driving laser beyond the linear-optics regime can overcome the weak coupling of subradiant modes with the external world.Moreover, we have numerically studied subradiance using the vectorial coupled-dipole model, with a focus on understanding the effect of the near-field dipole-dipole interaction. For that, we extensively compared the vectorial and scalar (which does not contain near-field interaction terms) models and studied the subradiant lifetime as a function of the density and optical thickness of the cold-atom cloud. We observed that the near-field terms are detrimental for subradiance, which was seen in the reduction of the subradiant lifetimes with increasing density. This detrimental character of near-field terms can be interpreted as being due to an effective inhomogeneous broadening induced by the near-field interaction, which reduces the subradiant lifetimes as the density increases.The detrimental character of near-field interaction has also been previously numerically identified for Anderson localization of light waves (Anderson localization is a coherent multiple-scattering wave phenomenon in a strongly scattering medium that results in a cessation of a diffusive wave transport; it also yields long-lived modes): the scalar coupled-dipole model predicts Anderson localization of light waves, but not the vectorial one. However, adding a strong magnetic field allows one to recover localized modes for vectorial light. In this context, we numerically studied a possible signature of Anderson localization of light in cold atoms, based on the measurement of intensity fluctuations of the scattered light. We have shown that at the transition to the localized regime, the fluctuations are enhanced. In particular, for vectorial light, we have demonstrated the absence and recovery of enhanced intensity fluctuations without and with the applied magnetic field, which further corroborates that the intensity fluctuations could serve as an experimental way to probe the localized states.
Coupling between quantum emitters and modes of light is foundational to studies of quantum systems. Coherent interactions between matter and light have greatly advanced the development of quantum technologies. When an ensemble of atoms interacts with light that is confined within a cavity---a resonator for photons---light also mediates atom-atom interactions, leading to collective phenomena that cannot be extrapolated from microscopic behaviors. Understanding how interactions among quantum particles lead to macroscopic phenomena, such as phase transitions and breaking of symmetries, remains a challenge in modern physics. In this dissertation, I present results addressing this challenge in the context of mesoscopic arrays of optical-tweezer-trapped atoms interfaced with a high-finesse optical cavity. In particular, the physics we investigate arises from the collective scattering of light. Utilizing the ability to place atoms with nanometer-scale precision, we engineer superradiant and subradiant states, where control over interference of the emission from multiple atoms leads to collectively enhanced or suppressed amounts of scattered light. Building on this work, we investigate the emergence of optomechanical self-organization, mediated by superradiance in the cavity electromagnetic field. By coupling atoms to the same cavity mode, the atoms exert forces on one another through the exchange of photons, leading them to autonomously order themselves spatially. We characterize mesoscopic fluctuations and their effect on symmetry-breaking dynamics associated with self-organization. Finally, we extend this framework to theoretically investigate how the phase of the atom-cavity coupling can be altered to generate higher symmetries. Our analysis reveals first-order phase transitions and instabilities induced by non-reciprocal forces. Altogether, this work establishes a path towards realizing mesoscopic systems of complex phases of matter in cavity quantum electrodynamics with unprecedented programmability.
Summary form only given. Spontaneous optical pattern formation occurs in a variety of nonlinear systems [1], including hot atomic vapors [2]. On the other hand, the spatial self-organization of atomic ensembles due to opto-mechanical coupling has received a lot of interest in recent years [3].We report on the observation of transverse self-organization of a cold atomic cloud (issued from a magnetooptical trap) under the action of a single pump laser beam. Two symmetries (translation and rotation) in the plane orthogonal to the beam propagation direction are spontaneously broken. We use a simple optical feedback scheme [4], where the transmitted pump beam is retro-reflected to the atoms by a high-reflectivity mirror located at a distance d behind the cloud. This feedback loop transforms phase fluctuations of the transmitted wave into intensity fluctuations, which then react on the atomic medium. If the feedback is positive, a transverse instability can develop leading to the spontaneous apparition of patterns in the transmitted pump intensity profile, as shown in the figure below (left).Using a weak probe beam sent a few tens of μs after the e,tinction of the pump, we demonstrate that the instability also results in a transverse spatial ordering of the atomic medium as shown in the right image. The cold atoms thus e,perience strong spatial bunching due to the dipole force associated to the inhomogeneous intensity distribution. We identified two different instability regimes. For short pump durations (- 1 μs), high pump intensity and cloud optical density, the instability relies on the Kerr effect (electronic nonlinearity). For longer pump durations (- 100 μs), the instability is driven by the opto-mechanical effect, resulting in lower intensity and optical density thresholds than for the electronic nonlinearity. These observations are well reproduced by a theoretical model including the coupled dynamics of the light field and the atomic e,ternal degrees of freedom.