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Superfluorescence Dynamics in Er:YLF

Bortoli Saygashev, Alexey Vladimirovic

Published Sep 17, 2019• 0 citations
OpenAlex

Abstract

Spontaneous decay is a phenomenon that has been described for the first time by Dirac, Wigner and Weisskopf, at the early ages of the development of quantum electrodynamics. The theory is applicable to a multi-body system only when atoms don’t interact during their decay. Dicke introduces in his seminal paper the case where this assumption doesn’t hold. The results he obtains not only tell that the system emits pulses, but the pulse duration now depends on 1/N, where N is the number of participating atoms to the process. The pulses temporal profile is described by a squared hyperbolic secant function. The resulting emission intensity scales as N^2. The atomic system radiates more intensively than the ordinary fluorescent emission, this is the reason why the process is called superradiance, or by a generalization to extended systems, superfluorescence. The superradiant emission has preferential escape directions, depending on the atomic sample shape. Superradiance is a collective process and it takes place when the group of excited atoms is left unper- turbed during the formation of of the macroscopic dipole. A fundamental difference compared to the spontaneous and stimulated emission processes is that all atoms act together as a single entity and it isn’t possible to identify single atoms involved. This remarkable behaviour is manifest when the atomic coherence of the system, while influenced by environmental interactions that cause dephasing in atoms, persists for a sufficient interval of time. Typical dephasing mechanisms, such as collisions in gases or lattice phonon interactions in crystals, make its experimental observation difficult. A possible solution to this problem is the use of optical crystals doped with rare-earths that are characterized by long and narrow levels lifetimes.

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Spontaneous decay is a phenomenon that has been described for the first time by Dirac, Wigner
and Weisskopf, at the early ages of the development of quantum electrodynamics. The theory is
applicable to a multi-body system only when atoms don’t interact during their decay. Dicke introduces
in his seminal paper the case where this assumption doesn’t hold.
The results he obtains not only tell that the system emits pulses, but the pulse duration now depends
on 1/N, where N is the number of participating atoms to the process. The pulses temporal profile
is described by a squared hyperbolic secant function. The resulting emission intensity scales as N^2.
The atomic system radiates more intensively than the ordinary fluorescent emission, this is the reason
why the process is called superradiance, or by a generalization to extended systems, superfluorescence.
The superradiant emission has preferential escape directions, depending on the atomic sample shape.
Superradiance is a collective process and it takes place when the group of excited atoms is left unper-
turbed during the formation of of the macroscopic dipole. A fundamental difference compared to the
spontaneous and stimulated emission processes is that all atoms act together as a single entity and it
isn’t possible to identify single atoms involved.
This remarkable behaviour is manifest when the atomic coherence of the system, while influenced by
environmental interactions that cause dephasing in atoms, persists for a sufficient interval of time.
Typical dephasing mechanisms, such as collisions in gases or lattice phonon interactions in crystals,
make its experimental observation difficult. A possible solution to this problem is the use of optical
crystals doped with rare-earths that are characterized by long and narrow levels lifetimes.
Recent advances in optical studies of condensed matter systems have led to the emergence of a variety of phenomena that have conventionally been studied in the realm of quantum optics. These studies have not only deepened our understanding of light–matter interactions but have also introduced aspects of many-body correlations inherent in optical processes in condensed matter systems. This paper is concerned with the phenomenon of superradiance (SR), a profound quantum optical process originally predicted by Dicke in 1954. The basic concept of SR applies to a general N body system, where constituent oscillating dipoles couple together through interaction with a common light field and accelerate the radiative decay of the whole system. Hence, the term SR ubiquitously appears in order to describe radiative coupling of an arbitrary number of oscillators in many situations in modern science of both classical and quantum description. In the most fascinating manifestation of SR, known as superfluorescence (SF), an incoherently prepared system of N inverted atoms spontaneously develops macroscopic coherence from vacuum fluctuations and produces a delayed pulse of coherent light whose peak intensity ∝N2. Such SF pulses have been observed in atomic and molecular gases, and their intriguing quantum nature has been unambiguously demonstrated. In this review, we focus on the rapidly developing field of research on SR phenomena in solids, where not only photon-mediated coupling (as in atoms) but also strong Coulomb interactions and ultrafast scattering processes exist. We describe SR and SF in molecular centers in solids, molecular aggregates and crystals, quantum dots, and quantum wells. In particular, we will summarize a series of studies we have recently performed on semiconductor quantum wells in the presence of a strong magnetic field. In one type of experiment, electron-hole pairs were incoherently prepared, but a macroscopic polarization spontaneously emerged and cooperatively decayed, emitting an intense SF burst. In another type of experiment, we observed the SR decay of coherent cyclotron resonance of ultrahigh-mobility 2D electron gases, leading to a decay rate that is proportional to the electron density. These results show that cooperative effects in solid-state systems are not merely small corrections that require exotic conditions to be observed; rather, they can dominate the nonequilibrium dynamics and light emission processes of the entire system of interacting electrons.
Fully-excited two-level atoms separated by less than the transition wavelength cooperatively emit light in a short burst, a phenomenon called superradiance by R. Dicke in 1954. The burst is characterized by a maximum intensity scaling with the square of the number of atoms NNN and a temporal width reduced by NNN compared to the single atom spontaneous decay time. Both effects are usually attributed to a synchronization of the electric dipole moments of the atoms occurring during the process of light emission. Contrary to this explanation, it was recently shown by use of a quantum path description that the peak intensity results from the quantum correlations among the atoms when occupying symmetric Dicke states. Here we investigate from this perspective the temporal evolution of the ensemble, starting in the small sample limit, i.e., when the atoms have mutual separations much smaller than the transition wavelength λλλ and pass down the ladder of symmetric Dicke states. In addition, we explore the temporal evolution for the case of non-interacting atoms with mutual separations much larger than λλλ. We show that in this case a similar superradiant burst of the emitted radiation is observed if the quantum correlations of the atoms are generated by conditional photon measurements retaining the atomic ensemble within or close to the symmetric subspace.
Fully excited two-level atoms separated by less than the transition wavelength cooperatively emit light in a short burst, a phenomenon called superradiance by R. Dicke in 1954 [Phys. Rev. 93, 99 (1954)]. The burst is characterized by a maximum intensity scaling with the square of the number of atoms NNN and a temporal width reduced by NNN compared to the single atom spontaneous decay time. Both effects are usually attributed to a synchronization of the electric dipole moments of the atoms occurring during the process of light emission. Contrary to this explanation, it was recently shown by use of a quantum path description that the peak intensity results from the quantum correlations among the atoms when occupying symmetric Dicke states. Here we investigate from this perspective the temporal evolution of the ensemble, starting in the small sample limit, i.e., when the atoms have mutual separations much smaller than the transition wavelength $\ensuremath{\lambda}$ and pass down the ladder of symmetric Dicke states. In addition, we explore the temporal evolution for the case of distant noninteracting atoms with mutual separations much larger than $\ensuremath{\lambda}$. We show that in this case a similar superradiant burst of the emitted radiation is observed if the quantum correlations of the atoms are generated by conditional photon measurements retaining the atomic ensemble within or close to the symmetric subspace.
Superradiance is an extensive cooperative spontaneous emission phenomenon, exhibited by some atomic collective-spin states. However, distinct initial states differ in their decay dynamics. Dicke states ∣j,m⟩|j,m\rangle∣j,m⟩ with distinct numbers of excitations n=m+jn=m+jn=m+j, driven by vacuum fluctuations, have their peak emission intensity shifted in time. Rotating Dicke states relative to the decay axis introduces an interesting parity structure that affects the pulse profile and photon correlations. Squeezed-bath prepared states undergo a squeezing-controlled crossover to the rotated Dicke states, making the emission character dependent on the amount of squeezing transferred from light to the atomic state. For semiclassical states with a macroscopic dipole moment, like the atomic coherent state, the emission intensity depends on their polarization. We present detailed results on the superradiant dynamics of a representative selection of states expanded in Dicke states to highlight the initial state as an independent dynamical control parameter. For large-NNN, we are able to predict fairly accurately the pulse profile in each case using the mean-field approximation, an approach based on the Fokker--Planck equation. We also present comparative results on the intensity correlation function, quantify the coherent and incoherent contributions of the emission, and contrast between small and large ensembles.
Irradiation of a medium by short intense pulses from x-ray (XUV) free-electron lasers can result in saturated photoionization of inner electronic shells. As a result an inversion of populations between core levels appears. The resulting fluorescent radiation can be amplified during its propagation through the inverted medium and results in intense, quasi-transform-limited radiation bursts. While the optical counterpart of this phenomena, known as superfluorescence, was intensively investigated, a generalized treatment is needed in the x-ray (XUV) domain, where the dynamics of pumping and evolution due to fast decay processes play a crucial role. To provide a general theoretical approach, we start from the fundamental, quantized minimal coupling Hamiltonian of light-matter interaction and after a series of approximations arrive at a closed system of equations for the two-point correlation function of atomic coherences and the two-time correlation function of the emitted field. The obtained formalism enables us to investigate collective spontaneous emission in various regimes. It is extended consistently to include incoherent processes that are relevant in the x-ray (XUV) domain. These processes are introduced into the formalism by corresponding Lindblad superoperators. The connection to other approaches is discussed and numerical examples related to recent experiments are presented.
We have observed and characterized 501.6 nm collective spontaneous emission (superfluorescence) following 1s(2) → 1s3p excitation of helium atoms by 53.7 nm free-electron laser radiation. Emitted pulse energies of up to 100 nJ are observed, corresponding to a photon number conversion efficiency of up to 10%. We observe the peak intensity to scale as ρ(2) and the emitted pulse width and delay to scale as ρ(-1), where ρ is the atom number density. Emitted pulses as short as 1 ps are observed, which corresponds to a rate around 75,000 times faster than the spontaneous 1s3p → 1s2s decay rate. To our knowledge, this is the first observation of superfluorescence following pumping in the extreme ultraviolet wavelength region, and extension of the technique to the generation of extreme ultraviolet and x-ray superfluorescence pulses should be straightforward by using suitable atomic systems and pump wavelengths.