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.
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.
Enhancing optical signal is a subject of long term interest with many applications, such as trace chemical detection in the lab and standoff detection in the atmosphere. It is well known that optical properties of multi-level atomic and molecular system can be controlled and manipulated efficiently using quantum coherence and interference resulting an enhancement in optical signals. In this dissertation we investigate methods both with/without utilizing coherence of atomic and molecular systems to enhance optical signals. We use resonant Raman scattering and surface-enhanced Raman scattering which do not rely on molecular coherence to boost Raman signal from molecules, several orders of magnitude enhancement has been achieved. When coherence is introduced into atomic systems, cooperative emission is produced as a result of coherence. The emission is named Superfluorescence (SF) or superradiance (SR) depending on the initial coherence of the prepared systems. We study the properties of SF, yoked SF (YSF) and SR, the transition from YSF to SR and quantum beat exhibits in YSF/SR signal. More than thirty folds of pulse energy is obtained from SR compare to that of YSF. Possible applications of these results are also discussed.
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.
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.
Quantum coherence and correlations in atomic and radiation physics have led to many interesting and unexpected consequences. For example, an atomic ensemble prepared in a coherent superposition of states yields the Hanle effect, quantum beats, photon echo, self-induced transparency, and coherent Raman beats. In fact, in Section 1.4, we saw that the quantum beat effect provides one of the most compelling reasons for quantizing the radiation field. A further interesting consequence of preparing an atomic system in a coherent superposition of states is that, under certain conditions, it is possible for atomic coherence to cancel absorption. Such atomic states are called trapping states †. The observation of nonabsorbing resonances via atomic coherence and interference impacts on the concepts of lasing without inversion (LWI),‡ enhancement of the index of refraction accompanied by vanishing absorption, and electromagnetically induced transparency. In lasing without inversion, the essential idea is the absorption cancellation by atomic coherence and interference. This phenomenon is also the essence of electromagnetically induced transparency. Usually this is accomplished in three-level atomic systems in which there are two coherent routes for absorption that can destructively interfere, thus leading to the cancellation of absorption. A small population in the excited state can thus lead to net gain. A related phenomenon is that of resonantly enhanced refractive index without absorption in an ensemble of phase-coherent atoms ( phaseonium ). In a phaseonium gas with no population in the excited level, the absorption cancellation always coincides with vanishing refractivity.