We find that intense short pulses of XUV radiation can be produced by cooperative spontaneous emission from visible or IR laser pulses driving atoms or ions. The process depends on the generation and utilization of atomic coherence as is the case in lasing without inversion. However, the radiation process is not stimulated emission, but is rather cooperative spontaneous emission in the sense of Dicke. More precisely, the many atom mathematics of superradiance has much in common with coherent anti-Stokes Raman scattering. The generation of Raman coherence is considered from the perspectives of multi-photon excitation and breaking of adiabaticity. In particular, we find that the advent of an ultrashort (e.g. single cycle) pulse rewards rethinking of conventional (nanosecond) nonlinear optics with new insights.
We find that intense short pulses of XUV radiation can be produced by cooperative spontaneous emission from visible or IR laser pulses driving atoms or ions. The process depends on the generation and utilization of atomic coherence as is the case in lasing without inversion. However, the radiation process is not stimulated emission, but is rather cooperative spontaneous emission in the sense of Dicke. More precisely, the many atom mathematics of superradiance has much in common with coherent anti-Stokes Raman scattering. The generation of Raman coherence is considered from the perspectives of multi-photon excitation and breaking of adiabaticity. In particular, we find that the advent of an ultrashort (e.g. single cycle) pulse rewards rethinking of conventional (nanosecond) nonlinear optics with new insights.
We suggest a highly efficient method of ultrashort pulse formation from resonant XUV radiation due to sub-laser-cycle modulation of the excited state of non-hydrogen-like atoms by a nonionizing IR laser field. This modulation results in formation of the Raman-Stokes and anti-Stokes sidebands in coherently forward-scattered radiation, which, in turn, leads to formation of short pulses, when the phases of the sidebands are matched. This method is a generalization of a recently suggested technique [V. A. Antonov et al., Phys. Rev. A 88, 053849 (2013)] for a non-hydrogen-like medium. The possibility to form 2-fs XUV pulses in the gas of helium atoms and 990-as XUV pulses in the plasma of Li+ ions with efficiencies over 80% is shown.
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.
New approaches for generating coherent light are of keen interest to the scientific community due to the increasing demand for unique sources tailored to specific applications. In fields like microscopy, remote sensing, and soft X-ray/XUV lasers this interest is especially pronounced as novel techniques would have a profound impact. Here, we present new methods for generating coherent light by inducing collective coherence in the gain medium. In particular, we demonstrate coherent emission produced through four-wave mixing on a dressed state, stimulated Raman by inducing coherence between two vibrational levels via 2-photon coupling, and finally, a remote atmospheric coherent source via strong-oscillatory superfluorescence in atomic oxygen. Four-wave mixing on a dressed state could be used to generate XUV coherent radiation or remote atmospheric sensing, as it produces both a forward and backward propagating field. We observe this in Rb vapor with emission occurring at detunings of up to 30 nm from the transition. Similarly, 2-photon enhanced stimulated Raman could be implemented for XUV generation as well, due to the asymmetric gain observed on the anti-Stokes emission relative to the Stokes in Methane. It is also a great platform for microscopy as it is background-free unlike other conventional methods like CARS and CSRS. Atmospheric lasing via oxygen is a prime candidate for nextgeneration remote sensing techniques, and here we study its emission mechanisms in depth demonstrating that superfluorescence serves as the main driving process for the observed 845 nm generation. This intense strong-oscillatory emission lends itself for use in coherent Raman techniques. Furthermore, a dual Raman-Brillouin microscope is also presented and demonstrated, which could prove to be a powerful new tool in biomedical and material characterizations applications.
It was shown some time ago that when the excitation of an ensemble of two-level atoms is swept in the direction of lasing, so that atoms are prepared in the excited state just as the radiation from previously excited atoms reaches them, the resulting laser amplifier is “highly anomalous” and yields superradiant emission without population inversion. We here show that transient gain in a three-level system has common features with Dicke superradiance and can yield strong extreme ultraviolet lasing in, for example, He atoms (at 58 nm) or He-like ions such asB3+(at 6.1 nm).
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.
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.