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Physical Review A

Theoretical analysis of the coherence-brightened laser in air

Luqi Yuan, Brett H. Hokr, Andrew J. Traverso, Dmitri V. Voronine, Yuri V. Rostovtsev, Alexei V. Sokolov, Marlan O. Scully

Published Feb 20, 2013• 37 citations
Publisher

Abstract

We present a detailed theoretical study of a recent experiment [A. J. Traverso et al., Proc. Natl. Acad. Sci. USA 109, 15185 (2012)] in which a laserlike source is created in air by pumping with a nanosecond pulse. The source generates radiation in the forward and backward directions. The temporal behavior of the emitted pulses is investigated for different pump shapes and durations. Our analysis indicates that the spiky emission is due to quantum coherence via cooperation between atoms of an ensemble, which leads to strong-oscillatory superfluorescence. We show that these cooperative nonadiabatic coherence effects cannot be described by rate equations and instead a full set of the Maxwell-Bloch equations must be used. We consider a range of parameters and study transitions between various regimes. Understanding these coherence-brightened processes in air should lead to improvements in environmental, atmospheric remote sensing and other applications.

DOI
10.1103/physreva.87.023826

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Optics and Spectroscopy•Nov 1, 2004•0 citations
We present a detailed theoretical study of a recent experiment [A. J. Traverso et al., Proc. Natl. Acad. Sci. USA 109, 15185 (2012)] in which a laserlike source is created in air by pumping with a nanosecond pulse. The source generates radiation in the forward and backward directions. The temporal behavior of the emitted pulses is investigated for different pump shapes and durations. Our analysis indicates that the spiky emission is due to quantum coherence via cooperation between atoms of an ensemble, which leads to strong-oscillatory superfluorescence. We show that these cooperative nonadiabatic coherence effects cannot be described by rate equations and instead a full set of the Maxwell-Bloch equations must be used. We consider a range of parameters and study transitions between various regimes. Understanding these coherence-brightened processes in air should lead to improvements in environmental, atmospheric remote sensing and other applications.
We have studied coherent emission from ambient air and demonstrated efficient generation of laser-like beams directed both forward and backward with respect to a nanosecond ultraviolet pumping laser beam. The generated optical gain is a result of two-photon photolysis of atmospheric O(2), followed by two-photon excitation of atomic oxygen. We have analyzed the temporal shapes of the emitted pulses and have observed very short duration intensity spikes as well as a large Rabi frequency that corresponds to the emitted field. Our results suggest that the emission process exhibits nonadiabatic atomic coherence, which is similar in nature to Dicke superradiance where atomic coherence is large and can be contrasted with ordinary lasing where atomic coherence is negligible. This atomic coherence in oxygen adds insight to the optical emission physics and holds promise for remote sensing techniques employing nonlinear spectroscopy.
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.
Abstract There has been an experimental report (Traverso et al 2012 Proc. Natl Acad. Sci. USA 109 15185) that oxygen lasing in ambient air exhibits a spiky feature. We theoretically explore a ladder-type three-level atomic system driven by a two-photon resonant pump pulse in a lossy medium, which corresponds to that oxygen experiment. We study the Maxwell–Bloch equations both numerically and analytically and discover that a long pump field brings competition between two mechanisms of coherent pumping and coherent emission, leading to the spiky emission, which cannot be produced using a short pump. The results indicate that atomic coherence occurs in the experiment. Our study provides a clear understanding of the oxygen experiment using a nanosecond pump laser and could lead to the potential application of this oxygen lasing in future experiments.
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.
The dynamics of the pulse shape and spectra of superfluorescence, stimulated superradiance, and coherent amplification of ultrashort light pulses is studied for a system of four-level atoms under incoherent cw pumping taking into account homogeneous and inhomogeneous broadening of the luminescence lines. It is found that incoherent pumping at a high level of excitation may significantly change the shape of the emission pulse in cooperative coherent processes. Also, it is found that, depending on the ratio of parameters of the pump, nonradiative transitions, and relaxation, different regimes of superfluorescence and stimulated superradiance may be realized.