Halide Perovskite Artificial Solids as a New Platform to Simulate Collective Phenomena in Doped Mott Insulators.

The development of quantum simulators, artificial platforms where the predictions of many-body theories of correlated quantum materials can be tested in a controllable and tunable way, is one of the main challenges of condensed matter physics. Here we introduce artificial lattices made of lead halide perovskite nanocubes as a new platform to simulate and investigate the physics of correlated quantum materials. We demonstrate that optical injection of quantum confined excitons in this system realizes the two main features that ubiquitously pervade the phase diagram of many quantum materials: collective phenomena, in which long-range orders emerge from incoherent fluctuations, and the excitonic Mott transition, which has one-to-one correspondence with the insulator-to-metal transition described by the repulsive Hubbard model in a magnetic field. Our results demonstrate that time-resolved experiments provide a quantum simulator that is able to span a parameter range relevant for a broad class of phenomena, such as superconductivity and charge-density waves.

Superradiant Electron Energy Loss Spectroscopy.

We analyze the interaction between a free electron and an ensemble of identical optical emitters. The mutual coherence and correlations between the emitters can enhance the interaction with each electron and become imprinted on its energy spectrum. We present schemes by which such collective interactions can be realized. As a possible application, we investigate free-electron interactions with superradiant systems, showing how electrons can probe the ultrafast population dynamics of superradiance.

Holographic Brain Theory: Super-Radiance, Memory Capacity and Control Theory.

We investigate Quantum Electrodynamics corresponding to the holographic brain theory introduced by Pribram to describe memory in the human brain. First, we derive a super-radiance solution in Quantum Electrodynamics with non-relativistic charged bosons (a model of molecular conformational states of water) for coherent light sources of holograms. Next, we estimate memory capacity of a brain neocortex, and adopt binary holograms to manipulate optical information. Finally, we introduce a control theory to manipulate holograms involving biological water's molecular conformational states. We show how a desired waveform in holography is achieved in a hierarchical model using numerical simulations.

Superradiance and Exciton Delocalization in Perovskite Quantum Dot Superlattices.

Achieving superradiance in solids is challenging due to fast dephasing processes from inherent disorder and thermal fluctuations. Perovskite quantum dots (QDs) are an exciting class of exciton emitters with large oscillator strength and high quantum efficiency, making them promising for solid-state superradiance. However, a thorough understanding of the competition between coherence and dephasing from phonon scattering and energetic disorder is currently unavailable. Here, we present an investigation of exciton coherence in perovskite QD solids using temperature-dependent photoluminescence line width and lifetime measurements. Our results demonstrate that excitons are coherently delocalized over 3 QDs at 11 K in superlattices leading to superradiant emission. Scattering from optical phonons leads to the loss of coherence and exciton localization to a single QD at temperatures above 100 K. At low temperatures, static disorder and defects limit exciton coherence. These results highlight the promise and challenge in achieving coherence in perovskite QD solids.

Random Lasers as Social Processes Simulators.

In this work, we suggest a quantum-like simulator concept to study social processes related to the solution of NP-hard problems. The simulator is based on the solaser model recently proposed by us in the framework of information cascade growth and echo chamber formation in social network communities. The simulator is connected with the random laser approach that we examine in the A and D-class (superradiant) laser limits. Novel network-enforced cooperativity parameters of decision-making agents, which may be measured as a result of the solaser simulation, are introduced and justified for social systems. The innovation diffusion in complex networks is discussed as one of the possible impacts of our proposal.

Superradiant Quantum Phase Transition for an Exactly Solvable Two-Qubit Spin-Boson Model.

A spin-boson-like model with two interacting qubits is analysed. The model turns out to be exactly solvable since it is characterized by the exchange symmetry between the two spins. The explicit expressions of eigenstates and eigenenergies make it possible to analytically unveil the occurrence of first-order quantum phase transitions. The latter are physically relevant since they are characterized by abrupt changes in the two-spin subsystem concurrence, in the net spin magnetization and in the mean photon number.

Thermal Decoherence of Superradiance in Lead Halide Perovskite Nanocrystal Superlattices.

Recent experiments by Rainò et al. ( Nature 2018, 563, 671-675) have documented cooperative emission from CsPbBr3 nanocrystal superlattices, exhibiting the hallmarks of low-temperature superradiance. In particular, the optical response is coherent and the radiative decay rate is increased by a factor of 3, relative to that of individual nanocrystals. However, the increase is 6 orders of magnitude smaller than what is theoretically expected from the superradiance of large assemblies, consisting of 106-108 interacting nanocrystals. Here, we develop a theoretical model of superradiance for such systems and show that thermal decoherence is largely responsible for the drastic reduction of the radiative decay rate in nanocrystal superlattices. Our theoretical approach explains the experimental results ( Nature 2018, 563, 671-675), provides insight into the design of small nanocrystal superlattices, and shows a 4 orders of magnitude enhancement in superradiant response. These quantitative predictions pave the path toward observing superradiance at higher temperatures.

Estimate of the superradiance spectrum in dispersive media.

In 2016, the Nottingham group detected the rotational superradiance effect. While this experiment demonstrated the robustness of the superradiance process, it still lacks a complete theoretical description due to the many effects at stage in the experiment. In this paper, we shine new light on this experiment by deriving an estimate of the reflection coefficient in the dispersive regime by means of a Wentzel-Kramers-Brillouin analysis. This estimate is used to evaluate the reflection coefficient spectrum of counter-rotating modes in the Nottingham experiment. Our finding suggests that the vortex flow in the superradiance experiment was not purely absorbing, contrary to the event horizon of a rotating black hole. While this result increases the gap between this experimental vortex flow and a rotating black hole, it is argued that it is in fact this gap that is the source of novel ideas. This article is part of a discussion meeting issue 'The next generation of analogue gravity experiments'.

Dynamics landscape for acoustic superradiance.

We analyse the behaviour of acoustic vortex beams interacting with rotating, fluid-saturated porous materials. Regions of the parameter space that exhibit distinct dynamical features are identified, with a focus on features that are relevant to the characterization of rotational superradiance. We discuss the similarities and differences between two recent proposals to observe acoustic superradiance with rotating, air-saturated sound absorbers. Finally, theoretical predictions for macroscopic acoustic scattering, obtained by averaging over interactions between the fluid and the porous material at the microscopic level, are compared with predictions of the first-Born approximation. This article is part of a discussion meeting issue 'The next generation of analogue gravity experiments'.

Energy Transfer and Interference by Collective Electromagnetic Coupling.

The physics of collective optical response of molecular assemblies, pioneered by Dicke in 1954, has long been at the center of theoretical and experimental scrutiny. The influence of the environment on such phenomena is also of great interest due to various important applications in, e.g., energy conversion devices. In this Letter, we demonstrate both experimentally and theoretically the spatial modulations of the collective decay rates of molecules placed in proximity to a metal interface. We show in a very simple framework how the cooperative optical response can be analyzed in terms of intermolecular correlations causing interference between the response of different molecules and the polarization induced on a nearby metallic boundary and predict similar collective interference phenomena in excitation energy transfer between molecular aggregates.

The SwissFEL soft X-ray free-electron laser beamline: Athos.

The SwissFEL soft X-ray free-electron laser (FEL) beamline Athos will be ready for user operation in 2021. Its design includes a novel layout of alternating magnetic chicanes and short undulator segments. Together with the APPLE X architecture of undulators, the Athos branch can be operated in different modes producing FEL beams with unique characteristics ranging from attosecond pulse length to high-power modes. Further space has been reserved for upgrades including modulators and an external seeding laser for better timing control. All of these schemes rely on state-of-the-art technologies described in this overview. The optical transport line distributing the FEL beam to the experimental stations was designed with the whole range of beam parameters in mind. Currently two experimental stations, one for condensed matter and quantum materials research and a second one for atomic, molecular and optical physics, chemical sciences and ultrafast single-particle imaging, are being laid out such that they can profit from the unique soft X-ray pulses produced in the Athos branch in an optimal way.

Optimization of photon storage fidelity in ordered atomic arrays.

A major application for atomic ensembles consists of a quantum memory for light, in which an optical state can be reversibly converted to a collective atomic excitation on demand. There exists a well-known fundamental bound on the storage error, when the ensemble is describable by a continuous medium governed by the Maxwell-Bloch equations. However, these equations are semi-phenomenological, as they treat emission of the atoms into other directions other than the mode of interest as being independent. On the other hand, in systems such as dense, ordered atomic arrays, atoms interact with each other strongly and spatial interference of the emitted light might be exploited to suppress emission into unwanted directions, thereby enabling improved error bounds. Here, we develop a general formalism that fully accounts for spatial interference, and which finds the maximum storage efficiency for a single photon with known spatial input mode into a collection of atoms with discrete, known positions. As an example, we apply this technique to study a finite two-dimensional square array of atoms. We show that such a system enables a storage error that scales with atom number N a like ∼ ( log N a ) 2 ∕ N a 2 , and that, remarkably, an array of just 4 × 4 atoms in principle allows for an error of less than 1%, which is comparable to a disordered ensemble with an optical depth of around 600.

Mechanochemical Activation of Superradiance in Paramagnetic Polymer Composites.

The review examines the effect of radio-frequency superradiance during pulsed mechanochemical activation of polymer composites under high pressure. Mechanochemical activation is implemented in three modes: (a) rheological explosion of polymer composite under rapid uniaxial compression, when an elastic wave pulse occurs in a polymer composite sample and implements the physico-chemical transformations leading to the occurrence of a superradiance pulse; (b) parametric mode, when an elastic wave pulse is introduced from the outside through a waveguide into a composite sample; (c) the mode of rapid pressure release, which also leads to the occurrence of a superradiance pulse. Paramagnetic polymer composites-namely polystyrene-binuclear clusters Co(QH)2-O-Co(QH)2 or Mn(QH)2-O-Mn(QH)2, where QH is a ligand based on QH2-3,6-di-tert-butylpyrocatechin)-are considered as objects implementing such processes. These binuclear clusters exhibit the Dzyaloshinskii-Moriya effect, and polymer composites based on them exhibit multiferroic properties. A composite of a molecular magnet in polystyrene matrix (Eu(III)(SQ)3·bipy complex with four unpaired electrons on Eu(III) and on SQ ligands; SQ is 3,6-di-tert-butylquinolate paramagnetic ligand) is also considered. The binuclear clusters and europium complexes form 2D nano-objects in the polymer matrix with a diameter of 50-100 nm and a thickness of ~ 1-2 nm. The review considers the formalisms of Dicke, Lorentz, Landau-Lifshitz-Blombergen and Havriliak-Negami equations, which make it possible to conduct a time-frequency analysis of these processes, to obtain data on the relaxation processes of spin and charge density in objects responsible for the process of radio-frequency superradiation. It is also shown that the analysis of electron spin resonance data allows us to provide a probable quantum chemical scheme for the implementation of the radio-frequency superradiance process. The phenomenon of superradiation has a great deal of potential in such areas as energy-saving technologies, wireless power transmission and storage devices. The technique of studying fast mechanochemical processes considered in the review allows us to investigate the mechanisms of interaction of magnetic and electrical subsystems in multiferroics and molecular magnets, which expands the scientific base for the creation of new functional materials and enables the solving of related problems of condensed matter physics.

Collective States in Molecular Monolayers on 2D Materials.

Collective excited states form in organic two-dimensional layers through Coulomb coupling of the molecular transition dipole moments. They manifest as characteristic strong and narrow peaks in the excitation and emission spectra that are shifted to lower energies compared with the monomer transition. We study experimentally and theoretically how robust the collective states are against homogeneous and inhomogeneous broadening, as well as spatial disorder that occurs in real molecular monolayers. Using a microscopic model for a two-dimensional dipole lattice in real space, we calculate the properties of collective states and their extinction spectra. We find that the collective states persist even for 1-10% random variation in the molecular position and in the transition frequency, with a peak position and integrated intensity similar to those for the perfectly ordered system. We measured the optical response of a monolayer of the perylene derivative MePTCDI on two-dimensional materials. On the wide-band-gap insulator hexagonal boron nitride, it shows strong emission from the collective state with a line width that is dominated by the inhomogeneous broadening of the molecular state. When the semimetal graphene is used as a substrate, however, the luminescence is completely quenched. By combining optical absorption, luminescence, and multiwavelength Raman scattering, we verify that the MePTCDI molecules form very similar collective monolayer states on hexagonal boron nitride and graphene substrates, but on graphene the line width is dominated by nonradiative excitation transfer from the molecules to the substrate. Our study highlights the transition from the localized molecular state of the monomer to a delocalized collective state in the two-dimensional molecular lattice that is entirely based on Coulomb coupling between optically active excitations of the electrons and molecular vibrations. The excellent properties of organic monolayers make them promising candidates for components of soft-matter optoelectronic devices.

Plasmonically Enhanced Superradiance of Broken-Symmetry Diamond Color Center Arrays Inside Core-Shell Nanoresonators.

Superradiance was demonstrated in broken-symmetry arrays of SiV diamond color centers embedded into concave plasmonic nanoresonators. The coupled configurations, including the diamond-silver (bare) and diamond-silver-diamond (coated) nanoresonators' geometry parameters as well as the emitters' azimuthal orientation and distance from the metal, were numerically optimized. An objective function consisting of the total fluorescence enhancement multiplied by the corrected emission quantum efficiency was used to design nanoresonators that promote superradiance. A larger total fluorescence enhancement was achieved via a larger number of emitters in both geometries, in coated spherical and in bare ellipsoidal nanoresonators. The superradiance performance was better in the case of a smaller number of emitters in bare spherical and coated ellipsoidal nanoresonators and in the case of a larger number of emitters in coated spherical and bare ellipsoidal nanoresonators. Ellipsoidal geometry is advantageous independent of composition and seeding. The configurations optimal for non-cooperative fluorescence enhancement and superradiance are coincidental. A radiative rate enhancement proportional to the number of emitters was found in wide spectral regions; therefore, superradiance implies N-fold enhancements coexist at excitation and emission. In ellipsoidal nanoresonators, the better superradiance achieved via a smaller quality-factor is accompanied by larger frequency pulling.

Action of Mechanical Forces on Polymerization and Polymers.

In this review, we summarize recent developments in the field of the mechanochemistry of polymers. The aim of the review is to consider the consequences of mechanical forces and actions on polymers and polymer synthesis. First, we review classical works on chemical reactions and polymerization processes under strong shear deformations. Then, we analyze two emerging directions of research in mechanochemistry-the role of mechanophores and, for the first time, new physical phenomena, accompanying external impulse mechanical actions on polymers. Mechanophores have been recently proposed as sensors of fatigue and cracks in polymers and composites. The effects of the high-pressure pulsed loading of polymers and composites include the Dzyaloshinskii-Moriya effect, emission of superradiation and the formation of metal nanoparticles. These effects provide deeper insight into the mechanism of chemical reactions under shear deformations and pave the way for further research in the interests of modern technologies.

Superradiant lasing in inhomogeneously broadened ensembles with spatially varying coupling.

Background: Theoretical studies of superradiant lasing on optical clock transitions predict a superb frequency accuracy and precision closely tied to the bare atomic linewidth. Such a superradiant laser is also robust against cavity fluctuations when the spectral width of the lasing mode is much larger than that of the atomic medium. Recent predictions suggest that this unique feature persists even for a hot and thus strongly broadened ensemble, provided the effective atom number is large enough. Methods: Here we use a second-order cumulant expansion approach to study the power, linewidth and lineshifts of such a superradiant laser as a function of the inhomogeneous width of the ensemble including variations of the spatial atom-field coupling within the resonator. Results: We present conditions on the atom numbers, the pump and coupling strengths required to reach the buildup of collective atomic coherence as well as scaling and limitations for the achievable laser linewidth. Conclusions: We show how sufficiently large numbers of atoms subject to strong optical pumping can induce synchronization of the atomic dipoles over a large bandwidth. This generates collective stimulated emission of light into the cavity mode leading to narrow-band laser emission at the average of the atomic frequency distribution. The linewidth is orders of magnitudes smaller than that of the cavity as well as the inhomogeneous gain broadening and exhibits reduced sensitivity to cavity frequency noise.

Analog black holes and energy extraction by super-radiance from Bose Einstein condensates (BEC) with constant density.

This paper investigates the acoustic superradiance of the density and phase fluctuations from the single vortex state of a Bose-Einstein condensate, by employing full time-domain and asymptotic frequency domain numerical calculations. The draining bathtub model of an incompressible barotropic fluid is adopted to describe the vortex. The propagation of the axisymmetric density and phase fluctuations in the condensate are governed by the massless scalar Klein-Gordon wave equation, which establishes the rotating black-hole analogy. Hence, the amplified scattering of these fluctuations from the vortex comprise the superradiance effect. A particular coordinate transformation is applied to reveal the event horizon and the ergosphere termwise in the metric and the respective asymptotic spectral solutions. A comparative analysis of the time domain and asymptotic frequency domain results are given for a range of rotational speed of the vortex and the frequency of the impinging fluctuations. The agreement at low rotational speeds of the vortex is shown to be very good, which starts to deteriorate at higher rotational speeds due to increasing constraint violations of the time-domain calculations. We further demonstrate an asymptotic upper bound for the superradiance as a function of vortex rotational speed, provided that the vortex remains stable.

Radiation Brightening from Virus-like Particles.

Concentration quenching is a well-known challenge in many fluorescence imaging applications. Here, we show that the optical emission from hundreds of chromophores confined onto the surface of a 28 nm diameter virus particle can be recovered under pulsed irradiation. We have found that as one increases the number of chromophores tightly bound to the virus surface, fluorescence quenching ensues at first, but when the number of chromophores per particle is nearing the maximum number of surface sites allowable, a sudden brightening of the emitted light and a shortening of the excited-state lifetime are observed. This radiation brightening occurs only under short pulse excitation; steady-state excitation is characterized by conventional concentration quenching for any number of chromophores per particle. The observed suppression of fluorescence quenching is consistent with efficient, collective relaxation at room temperature. Interestingly, radiation brightening disappears when the emitters' spatial and/or dynamic heterogeneity is increased, suggesting that the template structural properties may play a role that could be instrumental in developing virus-enabled imaging vectors that have optical properties qualitatively different than those of state-of-the-art biophotonic agents.

Photochemical Control of Exciton Superradiance in Light-Harvesting Nanotubes.

Photosynthetic antennae and organic electronic materials use topological, structural, and molecular control of delocalized excitons to enhance and direct energy transfer. Interactions between the transition dipoles of individual chromophore units allow for coherent delocalization across multiple molecular sites. This delocalization, for specific geometries, greatly enhances the transition dipole moment of the lowest energy excitonic state relative to the chromophore and increases its radiative rate, a phenomenon known as superradiance. In this study, we show that ordered, self-assembled light-harvesting nanotubes (LHNs) display excitation-induced photobrightening and photodarkening. These changes in quantum yield arise due to changes in energetic disorder, which in turn increases/decreases excitonic superradiance. Through a combination of experiment and modeling, we show that intense illumination induces different types of chemical change in LHNs that reproducibly alter absorption and fluorescence properties, indicating control over excitonic delocalization. We also show that changes in spectral width and shift can be sensitive measures of system dimensionality, illustrating the mixed 1-2D nature of LHN excitons. Our results demonstrate a path forward for mastery of energetic disorder in an excitonic antenna, with implications for fundamental studies of coherent energy transport.