Cooperative spontaneous recombination (superfluorescence) of electron-hole plasmas in semiconductors has been a challenge to observe due to ultrafast decoherence. We argue that superfluorescence can be achieved in quantum-confined semiconductor systems and present experimental evidence for superfluorescence from high-density photoexcited electronhole plasmas in magnetized quantum wells. At a critical magnetic field strength and excitation fluence, we observe a clear transition in the band-edge photoluminescence from omnidirectional output to a randomly directed but highly collimated beam. Changes in the linewidth, carrier density, and magnetic field scaling of the emission spectra correlate precisely with the onset of random directionality and are consistent with cooperative recombination.
Cooperative spontaneous recombination (superfluorescence) of electron-hole plasmas in semiconductors has been a challenge to observe due to ultrafast decoherence. We argue that superfluorescence can be achieved in quantum-confined semiconductor systems and present experimental evidence for superfluorescence from high-density photoexcited electronhole plasmas in magnetized quantum wells. At a critical magnetic field strength and excitation fluence, we observe a clear transition in the band-edge photoluminescence from omnidirectional output to a randomly directed but highly collimated beam. Changes in the linewidth, carrier density, and magnetic field scaling of the emission spectra correlate precisely with the onset of random directionality and are consistent with cooperative recombination.
Cooperative spontaneous recombination (superfluorescence) of electron-hole plasmas in semiconductors has been a challenge to observe due to ultrafast decoherence. We argue that superfluorescence can be achieved in quantum-confined semiconductor systems and present experimental evidence for superfluorescence from high-density photoexcited electron-hole plasmas in quantum wells under high magnetic fields (> 20 T). At a critical magnetic field strength and excitation fluence, we observe a clear transition in the band-edge photoluminescence from omnidirectional output to a randomly directed but highly collimated beam. Changes in the linewidth, carrier density, and magnetic field scaling of the emission spectra correlate precisely with the onset of random directionality and are consistent with cooperative recombination. We further investigate the effects of spot size, temperature, and excitation geometry on the emission properties.
We present results of detailed investigations of light emission from semiconductor multiple quantum wells at low temperatures and high magnetic fields excited by intense femtosecond laser pulses. The intensity and linewidth as well as the directional and statistical properties of photoemission strongly depended on the magnetic field strength and pump laser fluence. We also investigated the effects of spot size, temperature, excitation geometry, and excitation pulse width on the emission properties. The results suggest that the initially incoherent photoexcited electron-hole pairs spontaneously form a macroscopic coherent state upon relaxation into the low-lying magnetoexcitonic states, followed by the emission of a superfluorescent burst of radiation. We have developed a theoretical model for superfluorescent emission from semiconductor quantum wells, which successfully explained the observed characteristics.
Superfluorescence (SF) is a many-body process in which a macroscopic polarization spontaneously builds up from an initially incoherent ensemble of excited dipoles and then cooperatively decays, producing a delayed pulse of coherent radiation. SF arising from electron-hole recombination has recently been observed in In0.2Ga0.8As/GaAs quantum wells [G. T. Noe et al., Nature Phys. 8, 219 (2012) and J.-H. Kim et al., Sci. Rep. 3, 3283 (2013)], but its observability conditions have not been fully established. Here, by performing magnetic field (B), temperature (T), and pump power (P) dependent studies of SF intensity, linewidth, and delay time through time-integrated and time-resolved magnetophotoluminescence spectroscopy, we have mapped out the $B\ensuremath{-}T\ensuremath{-}P$ region in which SF is observable. In general, SF can be observed only at sufficiently low temperatures, sufficiently high magnetic fields, and sufficiently high laser powers with characteristic threshold behavior. We provide theoretical insights into these behaviors based primarily on considerations on how the growth rate of macroscopic coherence depends on these parameters. These results provide fundamental new insight into electron-hole SF, highlighting the importance of Coulomb interactions among photogenerated carriers as well as various scattering processes that are absent in SF phenomena in atomic and molecular systems.
Superfluorescence, a cooperative coherent spontaneous emission, is of great importance to the understanding of many-body correlation in optical processes. Even though superfluorescence has been demonstrated in many diverse systems, it is hard to observe in electron-hole plasma (EHP) due to its rapid dephasing and hence needs strong magnetic fields or complex microcavities. Herein, we report the first experimental observation of superfluorescence from EHP up to a moderate temperature of 175 K without external stimuli in a coupled metal halide perovskite quantum dots film. The EHP exhibits macroscopic quantum coherence through spontaneous synchronization. The coherence of the excited state decays by superfluorescence, which is redshifted 40 meV from the spontaneous emission with a ∼1700 times faster decay rate and exhibits quadratic fluence dependence. Notably, the excited state population's delayed growth and abrupt decay, which are strongly influenced by the pump fluence and the Burnham-Chiao ringing, are the characteristics of the superfluorescence. Our findings will open up a new frontier for cooperative emission and light beam-based technologies.
Abstract Quantum particles sometimes cooperate to develop a macroscopically ordered state with extraordinary properties. Superconductivity and Bose‐Einstein condensation are examples of such cooperative phenomena where macroscopic order appears spontaneously. Here, we demonstrate that such an ordered state can also be obtained in an optically excited semiconductor quantum well in a high magnetic field. When we create a dense electron‐hole plasma with an intense laser pulse, after a certain delay, an ultrashort burst of coherent radiation emerges. We interpret this striking phenomenon as a manifestation of superfluorescence (SF), in which a macroscopic polarization spontaneously builds up from an initially incoherent ensemble of excited quantum oscillators and then decays abruptly producing giant pulses of coherent radiation. SF has been observed in atomic gases, but the present work represents the first observation of SF in a solid‐state setting. While there is an analogy between the recombination of electron‐hole pairs and radiative transitions in atoms, there is no a priori reason for SF in semiconductors to be similar to atomic SF. This is a complex many‐body system with a variety of ultrafast interactions, where the decoherence rates are at least 1,000 times faster than the radiative decay rate, an unusual situation totally unexplored in previous atomic SF studies. We show, nonetheless, that collective many‐body coupling via a common radiation field does develop under certain conditions and leads to SF bursts. The solid‐state realization of SF resulted in an unprecedented degree of controllability in the generation of SF, opening up opportunities for both fundamental many‐body studies and device applications. We demonstrate that the intensity and delay time of SF bursts are fully tunable through an external magnetic field, temperature, and pump laser power.
Nonequilibrium can be a source of order. This rather counterintuitive statement has been proven to be true through a variety of fluctuation-driven, self-organization behaviors exhibited by out-of-equilibrium, many-body systems in nature (physical, chemical, and biological), resulting in the spontaneous appearance of macroscopic coherence. Here, we report on the observation of spontaneous bursts of coherent radiation from a quantum-degenerate gas of nonequilibrium electron-hole pairs in semiconductor quantum wells. Unlike typical spontaneous emission from semiconductors, which occurs at the band edge, the observed emission occurs at the quasi-Fermi edge of the carrier distribution. As the carriers are consumed by recombination, the quasi-Fermi energy goes down toward the band edge, and we observe a continuously red-shifting streak. We interpret this emission as cooperative spontaneous recombination of electron-hole pairs, or superfluorescence (SF), which is enhanced by Coulomb interactions near the Fermi edge. This novel many-body enhancement allows the magnitude of the spontaneously developed macroscopic polarization to exceed the maximum value for ordinary SF, making electron-hole SF even more "super" than atomic SF.