Quantum interference in atomic media has elicited interest for a very wide range of investigations and applications. As well as being a fascinating effect in itself, it also found applications in spectroscopy, nonlinear optics and has recently been drawing attention in the field of quantum optics for the realisation of sources of entangled photons, optical switching, and quantum information storage. The work presented in this thesis consists of two main projects centred around the theme of quantum interference in atomic processes. As cooled atomic vapours provide favourable conditions for the investigation of coherent phenomena, a magneto-optical trap was built for the future study of quantum interference in four-level link- ages. The number of trapped atoms is estimated to be ≈ 8 × 10^8, and the density to be ≈ 10^9 atoms per cubic centimetre. This represents the first stage of an ongoing study of quantum interference in four-level linkages. However, coherent effects can also be observed in hot vapours. A spontaneous, highly efficient, frequency up-conversion arising from four-wave mixing can indeed be observed in Rubidium. This complex phenomenon was investigated experimentally and theoretically so as to improve the conversion efficiency, and understand the underlying physics. The optimum conditions found in this study yield 1 mW of converted light for 40 mW of pumping light. As part of the study of the phase coherence of the process, the conversion of spatial modes in the four-wave mixing process was also examined. The observation of the transfer of orbital angular momentum in the process is reported, and a preliminary theoretical interpretation is presented.
Quantum interference in atomic media has elicited interest for a very wide range of investigations and applications. As well as being a fascinating effect in itself, it also found applications in spectroscopy, nonlinear optics and has recently been drawing attention in the field of quantum optics for the realisation of sources of entangled photons, optical switching, and quantum information storage. The work presented in this thesis consists of two main projects centred around the theme of quantum interference in atomic processes. As cooled atomic vapours provide favourable conditions for the investigation of coherent phenomena, a magneto-optical trap was built for the future study of quantum interference in four-level link- ages. The number of trapped atoms is estimated to be ≈ 8 × 10^8, and the density to be ≈ 10^9 atoms per cubic centimetre. This represents the first stage of an ongoing study of quantum interference in four-level linkages. However, coherent effects can also be observed in hot vapours. A spontaneous, highly efficient, frequency up-conversion arising from four-wave mixing can indeed be observed in Rubidium. This complex phenomenon was investigated experimentally and theoretically so as to improve the conversion efficiency, and understand the underlying physics. The optimum conditions found in this study yield 1 mW of converted light for 40 mW of pumping light. As part of the study of the phase coherence of the process, the conversion of spatial modes in the four-wave mixing process was also examined. The observation of the transfer of orbital angular momentum in the process is reported, and a preliminary theoretical interpretation is presented.
The fields of quantum and nonlinear optics have given rise to a variety of nonclassical states of light that have been proven to surpass certain limitations set by classical physics. Namely, certain squeezed and entangled states have been shown to beat the shot-noise limit when making precision phase measurements in interferometry, as well as write lithographic patterns that are smaller than classically allowed by the Rayleigh diffraction limit. Additionally, single-photon sources and entangled photon pairs have given rise to provably secure quantum key distribution for cryptography. Producing these quantum states of light has proven a difficult task. Nonlinear crystals, when pumped by a laser, produce pairs of single photons via the process of spontaneous parametric down conversion (SPDC). This process is mediated by the second order nonlinear susceptibility of the material. When pumped in a high gain regime, these crystals give rise to optical parametric amplification, which is a viable source of squeezed light. The vast majority of research in this area has focused on crystals that are seeded by vacuum in their two modes. This dissertation concerns the field of quantum nonlinear optics. It is an investigation into the processes that occur when nonlinear materials interact with the electromagnetic field on the single photon level. I have focused on seeding nonlinear crystals with quantum states of light, including single photons and entangled states. This process results in various states directly applicable to interferometry, imaging, and cryptography. Another application investigated is an absolute radiance measurement via stimulated parametric down conversion resulting from non-vacuum seeding of a nonlinear crystal. Additionally, other nonlinear processes, including four-wave mixing, nonlinear magneto-optical effects and coherent population trapping in warm atomic vapor involving quantum states of light are investigated. The process of seeding third-order nonlinear interactions, such as in atomic vapors, gives rise to a variety of interesting, nonclassical phenomena such as entangled image transfer and nonlocal imaging. Strong analogies between SPDC and four-wave mixing are drawn. I also experimentally show an all optical pi-only phase shift of one light beam via another in warm Cesium vapor.
Quantum interference and coherence lead to many interesting phenomenon and applications in quantum optics. In this dissertation, we study the quantum coherent properties in the following systems and aspects. We first investigate the optical bistability in a combined cavity-cold atoms system. In such a system the atom-photon interaction provides an optical lattice to the atoms and affects the mechanical motion of the atoms while atoms induce a position dependent phase shift on the cavity field. This highly nonlinearity induces optical bistability of intra-cavity photon number with respect to the pumping light added along the cavity axis. We show that the presence of this bistability can be controlled by a second pumping field added perpendicular to the cavity axis. It is also found that the critical input intensity of switching from one branch of bistability to the other depends on the the way of the field being added. This behavior is similar to the anomalous switching of the dispersive optical bistability of atomic media in the cavity. We also study the effect of counter-rotating terms in the control of spontaneous emission. We make use of a unitary transformation method and investigate the effect of dynamic energy shifts on the spontaneous emission modification via quantum interference in a four-level atomic system. We show that the counter-rotating terms, which are normally neglected in the usual investigation of atomic systems, do produce a significant influence on the evolution of the atomic amplitudes and the emission spectrum. This effect of counter-rotating terms can be observed in the time scale of the decay rate even when the dipole moments of the two upper levels are orthogonal to each other. The effect of counter-rotating terms on the spontaneous emission in a 3-D anisotropic photonic crystal is also discussed. It is shown that the behavior of the emission is similar to the case making rotating wave approximation, i.e., the localized and propagating fields are also separated by two characteristic atomic transition frequencies. However, the two characteristic frequencies are shifted due to the full Lamb shift which is obtained with counter-rotating terms being included in the Hamiltonian. We also utilize the unitary transformation method to show how the Lamb shift in a multi-level atom can be controlled by a driving field. Finally, we propose a subwavelength atom localization scheme for an atom located in a standing-wave field. The strategy is based on the observation that the photon statistics of resonance fluorescence depends on the position-dependent Rabi frequency.
Multi-photon nonlinear processes in atoms have served as important tools for quantum metrology, quantum communications, and quantum sensing. In this thesis, we experimentally address the interplay of various multi-photon Raman processes in hot Rb vapor, with the four-wave mixing (FWM) process being a central theme. FWM is the nonlinear response of a medium to a strong optical pump field inelastically scattering off atomic resonances and resulting in the generation of additional photons in different modes. FWM is a detrimental, but inherent part of electromagnetically induced transparency (EIT) and Raman based quantum memories. However, we were able to weaken the four-photon resonance by utilizing two-photon absorption to remove the additional photons without interfering with the signal beam. We also demonstrate the ability to tailor FWM to generate new photons in a controlled fashion for mode conversion. With this, we showed the conversion of 795 nm light to 420 nm light. While FWM is a source of noise in quantum memories, it can also be used for the generation squeezed twin-beams. Such beams have relative intensity noise reduced below the classical shot noise limit and share mode dependence based on the phase-matching conditions. Using this, we demonstrated that twin-beams can be generated with largely different spatial structure (optical angular momentum) and still share strong correlations, so long as the phase-matching conditions are satisfied. We then constructed and demonstrated the operation of a polarization-based quantum interferometer using squeezed twin-beams and showed that our beams were entangled under the inseparability condition. Using this interferometer, we were also able to achieve squeezing at low detection frequencies, which is necessary for things like quantum imaging and gravitational wave detection. We also demonstrated that squeezed twin-beams can be utilized to enhance the sensitivity of two-photon absorption spectroscopy. This research has touched on many different subjects related to quantum information science and improved upon some of the tools needed for the implementation of such technologies.
This PhD thesis treats applications of nonlinear optical effects for quantum information processing. The two main applications are four-wave mixing in the form of Bragg scattering (BS) for quantum-state-preserving frequency conversion, and sum-frequency generation (SFG) in second-order nonlinear materials for heralded entanglement. BS is shown to be separable in the input and output modes in the low-conversion regime, the regime of small pump powers or short interaction times. The selective frequency conversion of a signal is found to only depend on one of the pumps, while the temporal output of the converted idler depends on the other pump. This allows for temporal-mode-multiplexing. When the effects of nonlinear phase modulation (NPM) are included, the phases of the natural input and output modes are changed, reducing the separability. These effects are to some degree mediated by pre-chirping the pumps. In the high-conversion regime without the effects of NPM, exact Green functions for BS are derived. In this limit, separability is possible for conversion efficiencies up to 60 %. However, the system still allows for selective frequency conversion as well as re-shaping of the output. One way to obtain a 100 % conversion efficiency is to use multiple stages of frequency conversion, but this setup suffers from the combined effects of NPM. This problem is circumvented by using asymmetrically pumped BS, where one pump is continuous wave. For this setup, NPM is found to only lead to linear phase shifts of the input and output modes, corresponding to shifts of the central frequencies of the fields. The trade-off is that one is only able to select which signals are converted, or change the shape of the output idler. Finally, entanglement swapping using SFG was investigated. Considering two pairs of entangled photons, the process of up-converting one photon from each pair leads to heralded entangled pairs by successful detection of the up-converted photon. It was seen that this was indeed possible in the case of anti-correlated phasematching in the up-conversion crystal. Possible ways of increasing the probability of an up-conversion event were investigated briefly.
In this thesis, atomic coherence is used to enhance nonlinear optical processes in multi-level atoms. The multi-photon transitions are driven resonantly, and at the same time without absorptive losses, by using electromagnetically induced transparency (EIT), thereby allowing the study of χ(3) and χ(5) nonlinearities using weak driving fields. The coherently modified probe beam(s) and the atom-radiated signal fields arising from four- and six- wave- mixing (FWM and SWM) processes are measured in the spectral, temporal and spatial domains. In a three-level ladder-type atomic system, multiple peaks having spectral asymmetries are observed in the EIT window as well as in the FWM signal waveforms due to the diverse multiplicities of the participating atomic states. Using phase control tailored in the frequency domain, we demonstrate all-optical methods to control these spectral waveforms and discuss applications involving waveform-shaping and metrology. For the EIT study we demonstrate a switching of multiple dark peaks into bright peaks via phase-control of interferences in the underlying dark-states. In the FWM study we demonstrate all-optical spectral line shape symmetrization, linewidth narrowing and bandwidth switching. In a four-level inverted-Y-type atomic system, we drive and measure coexisting and phase-matched FWM and SWM signals. By using precision control of the relative phase and amplitude between these two processes of different nonlinear orders, we demonstrate phase coherence between them. First, a single-phase measurement is performed in the temporal and spatial domains, and the interferogram is used to measure the resonant frequency of the 5D5/2-5P3/2 atomic transition in 85Rb. Second, the method is extended to realize a capacity for two-phase measurement. In this case, the spectral bandwidth of the signal is modified in order to measure the phase-shift occurring in one Mach-Zehnder interferometer, while the intensity of the total signal waveform measures the phase-shift occurring in a second interferometer. Finally, we demonstrate phase-dependent spatial fusion between two ultra-weak optical fields by using a strong coupling field to first convert the weak fields into bosonic dark-state polaritons, which are then steered into a common all-optical waveguide mode arising due to the coupling field's intensity distribution and the resulting cross-Kerr refractive index gradient.
This dissertation reports experimental studies of nonlinear optical effects manifested by electromagnetically induced transparency (EIT) in cold Rb atoms. The cold Rb atoms are confined in a magneto-optic trap (MOT) obtained with the standard laser cooling and trapping technique. Because of the near zero Doppler shift and a high phase density, the cold Rb sample is well suited for studies of atomic coherence and interference and related applications, and the experiments can be compared quantitatively with theoretical calculations. It is shown that with EIT induced in the multi-level Rb system by laser fields, the linear absorption is suppressed and the nonlinear susceptibility is enhanced, which enables studies of nonlinear optics in the cold atoms with slow photons and at low light intensities. Three independent experiments are described and the experimental results are presented. First, an experimental method that can produce simultaneously co-propagating slow and fast light pulses is discussed and the experimental demonstration is reported. Second, it is shown that in a three-level Rb system coupled by multi-color laser fields, the multi-channel two-photon Raman transitions can be manipulated by the relative phase and frequency of a control laser field. Third, a scheme for all-optical switching near single photon levels is developed. The scheme is based on the phase-dependent multi-photon interference in a coherently coupled four-level system. The phase dependent multi-photon interference is observed and switching of a single light pulse by a control pulse containing ∼20 photons is demonstrated. These experimental studies reveal new phenomena manifested by quantum coherence and interference in cold atoms, contribute to the advancement of fundamental quantum optics and nonlinear optics at ultra-low light intensities, and may lead to the development of new techniques to control quantum states of atoms and photons, which will be useful for applications in quantum measurements and quantum photonic devices.