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Ultrafast Cooperative Phenomena in Coherently Prepared Media: From Superfluorescence to Coherent Raman Scattering and Applications

Ariunbold Gombojav

Published Jan 1, 2011• 4 citations
OpenAlex

Abstract

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.

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We study the superfluorescence (SF) from a gas of rubidium atoms. The atoms of a dense vapor are excited to the $5D$ state from the $5S$ state by a two-photon process driven by 100-fs laser pulses. The atoms decay to the $6P$ state and then to the $5S$ state. The SF emission at 420 nm on the $6P$--$5S$ transition is recorded by a streak camera with picosecond time resolution. The time duration of the generated SF is tens of picoseconds, which is much shorter than the time scale of the usual relaxation processes, including spontaneous emission and atomic coherence dephasing. The dependence of the time delay between the reference input pulse and SF is measured as a function of laser power. The experimental data are described quantitatively by a simulation based on the semiclassical atom-field interaction theory. The observed change in scaling laws for the peak intensity and delay time can be elucidated by an SF theory in which the sample length is larger than the cooperation length.

Physical Review A•Oct 20, 2010•52 citations
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.
We report the observation of coherent UV light pulses by the coherent scattering of IR pulses from atomic rubidium vapor. Rubidium atoms were first excited by a 100 fs pulse from the 5S ground state to the 5D state via a two-photon transition. The atoms were then pumped by an IR pulse resonant to the 5D–12P transition. The presence of the IR pulse triggered the instantaneous emission of a UV light pulse on the 12P–5S transition. The pulse had a time duration of tens of picoseconds, which was measured by a picosecond-resolution streak camera. The temporal shape of the generated light is explained by a simplified atom–field interaction theory.
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.
Abstract : This project was initiated to identify conditions in dense upconversion media under which ultrashort pulses could lead to new applications. Four main results were obtained. First, a new channel for the generation of ultraviolet upconversion emission in Erbium-doped compounds was discovered. Second, an extremely promising imaging technique which relies on time-gated, ultrafast upconversion was demonstrated. Third, induced nonlinear response in dense upconversion materials was shown to be primarily dispersive in nature, even for resonant interactions, and we were able to explain how this apparently contradictory behavior arises. This revealed for the first time that cooperative nonlinearities could be useful in lossless, ultrafast applications. Fourth, a local mode of Yb in CsCdBr3 crystals was identified with properties which should permit coherent control of upconversion by ultrashort pulses.
The conventional method to measure atomic interference is usually based on incoherent processes which can be scaled by nano or microseconds. However, atomic interference may be studied in association with coherent process such as superfluorescence. Producing superfluorescent picosecond pulses in 87Rb vapor pumped by ~100 fs laser pulses, we report an observation of quantum beat due to D-lines. The relative delay of the superfluorescent pulses is measured by the streak camera with picosecond time resolution, as a function of time interval between input pulses, which also enables us to study atomic interference.
The short-pulse conversion efficiency of stimulated Raman scattering in Pb vapor is increased from 15% to 35% by using a novel technique that employs a closely spaced pair of pump pulses. The second pulse scatters off the coherent excitation induced in the medium by the first pulse, with a resultant enhancement in efficiency. To our knowledge these results give the first observation of such long-lived cooperative phenomena in stimulated Raman scattering. We have also observed this phenomenon in H(2) and show that this technique is readily applicable to other Raman-active media.
We study the superfluorescence (SF) from a gas of rubidium atoms. The atoms of a dense vapor are excited to the 5D5D5D state from the 5S5S5S state by a two-photon process driven by 100-fs laser pulses. The atoms decay to the 6P6P6P state and then to the 5S5S5S state. The SF emission at 420 nm on the 6P6P6P--5S5S5S transition is recorded by a streak camera with picosecond time resolution. The time duration of the generated SF is tens of picoseconds, which is much shorter than the time scale of the usual relaxation processes, including spontaneous emission and atomic coherence dephasing. The dependence of the time delay between the reference input pulse and SF is measured as a function of laser power. The experimental data are described quantitatively by a simulation based on the semiclassical atom-field interaction theory. The observed change in scaling laws for the peak intensity and delay time can be elucidated by an SF theory in which the sample length is larger than the cooperation length.