During the last half century, quantum coherence has been of great interest due to its own right and also due to its broad range of applications in many areas of physics. The reason for that is the technological progress made last century, specially, the invention of coherent light sources and their commercialization. Indeed, coherent laser sources allow us to coherently excite atoms and molecules, as a consequence, to study variety of coherent and collective phenomena in atomic physics, for instance, coherent optical spectroscopy, superradiance, superflourescence, lasing without inversion and so forth. Interestingly, recent studies in biological systems also seem to exhibit coherent processes, in particular, photosynthetic transport and avian compass.\n\nIn this dissertation, we present some of the theory and applications of the quantum coherence. This study considers (i) application of quantum coherence to enhance output signals of coherent anti-Stokes Raman spectroscopy of optically active media (chiral molecules), (ii) a way to find general formulas of single- and double-excited subradiant Dicke states using symmetry group theory, (iii) an impact of Fano-Agarwal coupling and other virtual processes arising from non-rotating wave approximation on the decay of super and subradiant timed Dicke states, and finally (iv) quantum coherence and collective phenomena of relativistically and uniformly accelerating atoms.\n\nApplications of the results presented in the dissertation may be a new method for resolving chirality of molecules using coherent anti-Stokes Raman spectroscopy - Raman optical activity, and a sidewise excitation method for single- and double-excited subradiant states. The obtained results also advance our theoretical understanding of quantum coherence specially theory of super and subradiance.
During the last half century, quantum coherence has been of great interest due to its own right and also due to its broad range of applications in many areas of physics. The reason for that is the technological progress made last century, specially, the invention of coherent light sources and their commercialization. Indeed, coherent laser sources allow us to coherently excite atoms and molecules, as a consequence, to study variety of coherent and collective phenomena in atomic physics, for instance, coherent optical spectroscopy, superradiance, superflourescence, lasing without inversion and so forth. Interestingly, recent studies in biological systems also seem to exhibit coherent processes, in particular, photosynthetic transport and avian compass.\n\nIn this dissertation, we present some of the theory and applications of the quantum coherence. This study considers (i) application of quantum coherence to enhance output signals of coherent anti-Stokes Raman spectroscopy of optically active media (chiral molecules), (ii) a way to find general formulas of single- and double-excited subradiant Dicke states using symmetry group theory, (iii) an impact of Fano-Agarwal coupling and other virtual processes arising from non-rotating wave approximation on the decay of super and subradiant timed Dicke states, and finally (iv) quantum coherence and collective phenomena of relativistically and uniformly accelerating atoms.\n\nApplications of the results presented in the dissertation may be a new method for resolving chirality of molecules using coherent anti-Stokes Raman spectroscopy - Raman optical activity, and a sidewise excitation method for single- and double-excited subradiant states. The obtained results also advance our theoretical understanding of quantum coherence specially theory of super and subradiance.
It is well known that the optical properties of multi-level atomic and molecular system can be controlled and manipulated efficiently using quantum coherence and interference, which has led to many new effects in quantum optics for e.g. lasing action without population inversion, ultraslow light, high resolution nonlinear spectroscopy etc. Recent experimental and theoretical studies have also provided support for the hypothesis that biological systems uses quantum coherence. Nearly perfect excitation energy transfer in photosynthesis is an excellent example of this.\n\nIn this dissertation we studied quantum coherence and interference effects in the transient and the continuous-wave regimes. This study led to (i) the first experimental demonstration of carrier-envelope phase effects on bound-bound atomic excitation in multi-cycle regime (~15 cycles), (ii) a unique possibility for standoff detection of trace gases using their rotational and vibrational spectroscopic signals and from herein called Coherent Raman Umklappscattering, (iii) several possibilities for frequency up-conversion and generation of short-wavelength radiation using quantum coherence (iv) the measurement of spontaneous emission noise intensity in Yoked-superfluorescence scheme.\n\nApplications of the obtained results are development of XUV (X-Ray) lasers, con- trolled superfluorescent (superradiant) emission, carrier-envelope phase effects, coherent Raman scattering in the backward direction, enhancement of efficiency for generating radiation in XUV and X-Ray regime using quantum coherence with and without population inversion and to extend XUV and X-Ray lasing to ~4.023 nm in Helium-like carbon.
Optical response of an active medium can substantially be modified when coherent superpositions of states are excited, that is, when systems display quantum coherence and interference. This has led to fascinating applications in atomic and molecular systems. Examples include coherent population trapping, lasing without inversion, electromagnetically induced transparency, cooperative spontaneous emission, and quantum entanglement. \n \nWe study quantum coherence effects in several quantum optical systems and find interesting applications. We show that quantum coherence can lead to transient Raman lasing and lasing without inversion in short wavelength spectral regions--extreme ultraviolet and x-ray--without the requirement of incoherent pumping. For example, we demonstrate transient Raman lasing at 58.4 nm in Helium atom and transient lasing without inversion at 6.1 nm in Helium-like Boron (triply-ionized Boron). We also investigate dynamical properties of a collective superradiant state prepared by absorption of a single photon when the size of the sample is larger than the radiation wavelength. We show that for large number of atoms such a state, to a good approximation, decays exponentially with a rate proportional to the number of atoms. We also find that the collective frequency shift resulting from repeated emission and reabsorption of short-lived virtual photons is proportional to the number of species in the sample. Furthermore, we examine how a position-dependent excitation phase affects the evolution of entanglement between two dipole-coupled qubits. It turns out that the coherence induced by position-dependent excitation phase slows down the otherwise fast decay of the two-qubit entanglement. We also show that it is possible to entangle two spatially separated and uncoupled qubits via interaction with correlated photons in a cavity quantum electrodynamics setup. Finally, we analyze how quantum coherence can be used to generate continuous-variable entanglement in quantum-beat lasers in steady state and propose possible implementation in quantum lithography.
Technological progress in commercializing ultrafast lasers and detectors has allowed realization of cooperative processes on an ultrashort time scale, which demand a re-evaluation of the conventional cooperative phenomena with a new insight. Ultrafast cooperative phenomena in coherently prepared media and various applications of superfluorescence and coherent Raman scattering are studied in this dissertation. In particular, a simple theoretical testimony on analogy between a cooperative emission and coherent Raman scattering is presented by offering an opportunity to perform parallel research on these two processes from a unified point of view.\n\nOn one hand, the superfluorescent pulse with a time duration of a few tens of picoseconds (ps) from alkali metal vapor is observed for the first time, even though cooperative phenomena in atomic vapor have been extensively studied for more than five decades. A dense rubidium vapor pumped by ultrashort (100 femtosecond, fs) pulses allows a realization of the ultrafast superfluorescence while a time-resolved study of superfluorescence is accomplished by using a streak camera with 2 ps time resolution. Experimental research on quantum nature of cooperative emissions has been “frozen” over the years (three decades) possibly because of the technical difficulties. Quantum fluctuations of superfluorescence development are explored experimentally by taking advantage of the ultra fast streak camera. Presumable applications of the superfluorescent pulse in e.g., a remote sensing, and an ultraviolet upconversion of the input infrared laser pulse are presented. The quantum interference due to different excitation pathways is revealed by the temporal coherent control technique while observing interferometric signals from alkali metal vapors. \n\nOn the other hand, a new spectroscopic technique based on ultrafast coherent Raman scattering is developed. The key advantage of the presented technique is to suppress the non-resonant background noise which usually obscures possible applications of the other conventional coherent Raman techniques in practice. A reduction of the background noise is achieved by shaping and delaying the third pulse which probes the coherence of the medium (i.e., an enhancement of specific vibrations of the target molecules in unison) firstly prepared by two broadband pulses. We demonstrate a robustness and superiority of signal-to-noise ratio of the developed technique by identifying as few as 10000 bacterial spores at a single laser shot level.\n\nFinally, several comparative studies between cooperative and uncooperative processes are presented. A picosecond cooperative phenomenon in a three-photon resonant medium induced by a single as well as two-color ultrashort pulses is investigated. A time-resolved study shows that a picosecond cooperative effect is crucial in the well-established fields of resonant-enhanced multiphoton ionizations and harmonic generations. We also present a quantitative analysis for spontaneous versus broadband coherent Raman scattering on pyridine molecules. The spontaneous Raman signal is enhanced by 5 orders as a result of cooperative phenomena.
In this dissertation we focused on two topics: 1. atomic cooperative effect, including superradiance, subradiance and collective Lamb shift in an atomic ensemble; 2. novel topological effect in quantum optics system, such as Haldane model, synthetic magnetic field in superradiance lattice and synthetic spin-orbit interaction in Fock-state lattices. \n\nIn the first part, we start from the Dicke state, an N-particle atomic ensemble excited by a single photon. Due to the interaction of the atoms with a continuum of vacuum modes, the Dicke state has a larger decay rate compared with an isolated atom, termed the single photon superradiance. In the “opposite” case, the single-photon subradiance state does not decay because of the destructive interference of the atomic transitions. We study the protection of subradiant states by the symmetry of the atomic distributions in the Dicke limit, in which collective Lamb shifts cannot be neglected. We find that antisymmetric states are subradiant states for distributions with reflection symmetry. Continuous symmetry can also be used to achieve subradiance in an extended ensemble. This study is relevant to the problem of robust quantum memory with long storage time and fast readout.\n\nIn the second part, we start from introducing the concepts, methods, and models from quantum optics or condensed matter physics. They include the timed-Dicke states, electromagnetically induced transparency, coupled wave equations, tight-binding model, band theory, Floquet theory, superradiance lattice, integer quantum Hall effect, Haldane model, etc.. Based upon these tools, we study three topological quantum optics systems: (i) a Haldane model with in situ tunable topological properties in a two-dimensional momentumspace superradiance lattice composed of timed Dicke states in electromagnetically induced transparency; (ii) a spin-orbit coupled Fock-state lattice, which introduce a novel quantum operation to generate mesoscopic superposition states, e.g., the NOON states and cat states; (iii) a synthetic magnetic field created in a quasi one dimensional superradiance lattice, which is predicted to be observed in thermal vapours of alkali atoms instead of only in cold atoms (as in previous experiments). This study aims to provide a novel, highly tunable platform simulating exotic phenomena in condensed matter physics and offers a basis of topological quantum optics and novel photonic devices.
This work is focused on quantum coherence and superradiant emission in a dense pencil-like multi-level medium where many novel effects appear such as transient lasing without inversion, coherence-brightened sky laser, and quantum amplification by superradiant emission of radiation. \n\nWe start from an interesting cascade model where quantum coherence effects can lead to surprising phenomena, gain without population inversion and gain suppression, under different parameters. We further show superradiant emission inside helium plasma. The population evolution shows the decay is significantly faster than collisional decoherence and spontaneous decay rates. This indicates superradiant coherent behavior of the atomic system inside the plasma.\n\nBased on these results, we demonstrate lasing without inversion on a time scale shorter than the decoherence time. The possibility of transient lasing without inversion holds promise for lasing in the extreme-ultraviolet/x-ray regime. We propose experiments to demonstrate this in helium or helium-like ions plasma. \n\nWe also study coherent emission from ambient air and demonstrate efficient generation of laser-like beams directed both forward and backward with respect to a nanosecond ultraviolet pumping laser beam. The emission process exhibits nonadiabatic quantum coherence, which is similar in nature to Dicke superradiance. This coherence-brightened backward light source in air provides possibility for atmospheric remote sensing through a phase-matched coherent Raman scattering process.\n\nFinally, we present a new kind of quantum amplifier, the QASER (quantum amplification by superradiant emission of radiation), based on collective superradiant emission which does not require initial population in the excited state. We show that parametric resonance between the driving field and collective superradiant oscillations of the atomic polarization can yield light amplification at high frequencies. The resulting superradiant amplifier is many orders of magnitude more efficient than nonlinear multiphoton excitation and holds promise as a new way to generate high-frequency coherent radiation.
Quantum coherence effects in atomic media such as electromagnetically-induced transparency and absorption, lasing without inversion, super-radiance and gain-assisted superluminality have become well-known in atomic physics. But these effects are not unique to atoms, nor are they uniquely quantum in nature, but rather are fundamental to systems of coherently coupled oscillators. In this talk I will review a variety of analogous photonic coherence phenomena that can occur in passive and active coupled optical resonators. Specifically, I will examine the evolution of the response that can occur upon the addition of a second resonator, to a single resonator that is side-coupled to a waveguide, as the coupling is increased, and discuss the conditions for slow and fast light propagation, coupled-resonator-induced transparency and absorption, lasing without gain, and gain-assisted superluminal pulse propagation. Finally, I will discuss the application of these systems to laser stabilization and gyroscopy.