Development of spontaneous coherence is one of the hallmarks of bosonic condensation in a variety of physical systems, such as cold atoms, confined photons, and hybrid light-matter quasiparticles like exciton polaritons in semiconductors. While spatial coherence is well understood once a steady-state condensate has been established, its temporal evolution as the condensate forms is largely unexplored. Here, we explore the dynamical formation of a non-equilibrium, driven-dissipative exciton-polariton condensate through both time-resolved experiments and numerical modeling. Our study reveals that the spatial coherence is established through two distinct stages. The early-time stage is interaction-driven and features transient oscillations in spatial coherence. This stage is followed by a steady-state regime characterized by a spatially-uniform high degree of coherence that extends over the entire size of the system and persists over time. These stages of spatial coherence development occur in both free flowing and confined exciton-polariton systems that undergo a quench - rapid growth of the condensate starting from two different initial settings. Our study offers a deep insight into the process by which long-range spatial coherence is established in a non-equilibrium bosonic condensate.

The emergence of spatial coherence in a confined two-dimensional Bose gas of exciton polaritons with tuneable interactions offers a unique opportunity to explore the role of interactions in a phase transition in a driven-dissipative quantum system, where both the phase transition and thermalisation are mediated by interactions. We investigate, experimentally and numerically, the spatial coherence and steady-state properties of the gas over a wide range of interaction strengths by varying the photonic/excitonic fraction of the polaritons and their density. We find that the first order spatial correlation function exhibits algebraic decay consistent with the Berezinskii-Kosterlitz-Thouless (BKT) phase transition. The exponent of the algebraic decay is inversely proportional to the coherent fraction of polaritons, in analogy to superfluid fraction of equilibrium quantum gases above the BKT transition, but with a different proportionality constant. Our work paves the way for future investigations of the phenomenon of phase transitions and superfluidity in a driven-dissipative setting.

We present a careful calibration of the exciton fraction of polaritons in high-Q (∼ 300,000), long-lifetime (∼ 300 ps), GaAs/AlGaAs microcavities.This is a crucial parameter for many-body theories which include the polariton-polariton interactions.It is much harder to establish this number in high-Q structures compared to low-Q structures, because the upper polariton is nearly invisible in high-Q cavities.We present a combination of photoluminescence, photoluminescence excitation, and reflectivity measurements to highly constrain the fit model, and compare the results of this model to the results from low-Q structures.We present a fitted curve of exciton fraction as a function of the lower polariton energy for multiple samples which have been used in prior experiments.

Exciton-polariton laser is a promising source of coherent light for low-energy applications due to its low-threshold operation. However, a detailed experimental study of its spectral purity, which directly affects its coherence properties is still missing. Here}, we present a high-resolution spectroscopic investigation of the energy and linewidth of an exciton-polariton laser in the single-mode regime, which derives its coherent emission from an optically pumped and confined exciton-polariton condensate. We report an ultra-narrow linewidth of 56~MHz or 0.24~$\mu$eV, corresponding to a coherence time of 5.7~ns. The narrow linewidth is consistently achieved by using an exciton-polariton condensate with a high photonic content confined in an optically induced trap. Contrary to previous studies, we show that the excitonic reservoir created by the pump and responsible for creating the trap does not strongly affect the emission linewidth as long as the condensate is trapped and the pump power is well above the condensation (lasing) threshold. \red{The long coherence time of the exciton-polariton system uncovered here opens up opportunities for manipulating its macroscopic quantum state, which is essential for applications in classical and quantum computing.

Manifesting chemical differences in individual rare earth (RE) element complexes is challenging due to the similar sizes of the tripositive cations and the corelike 4f shell. We disclose a new strategy for differentiating between similarly sized Dy3+ and Y3+ ions through a tailored photochemical reaction of their isostructural complexes in which the f-electron states of Dy3+ act as an energy sink. Complexes RE(hfac)3(NMMO)2 (RE = Dy (2-Dy) and Y (2-Y), hfac = hexafluoroacetylacetonate, and NMMO = N-methylmorpholine-N-oxide) showed variable rates of oxygen atom transfer (OAT) to triphenylphosphine under ultraviolet (UV) irradiation, as monitored by 1H and 19F NMR spectroscopies. Ultrafast transient absorption spectroscopy (TAS) identified the excited state(s) responsible for the photochemical OAT reaction or lack thereof. Competing sensitization pathways leading to excited-state deactivation in 2-Dy through energy transfer to the 4f electron manifold ultimately slows the OAT reaction at this metal cation. The measured rate differences between the open-shell Dy3+ and closed-shell Y3+ complexes demonstrate that using established principles of 4f ion sensitization may deliver new, selective modalities for differentiating the RE elements that do not depend on cation size.

The polariton-polariton interaction strength is an important parameter for all kinds of applications using the nonlinear properties of polaritons, such as optical switching and single-photon blockade devices. In this paper, we review and compare the results of a series of experiments on polariton-polariton interactions in GaAs/Al_xGa_-1xAs microcavity polariton structures, and present new theoretical analysis of these experiments. We show that not just the energy shift of the spectral lines, but also the results of measurements sensitive to the polariton scattering rate are important for the calibration of the interaction parameter at low excitation density. We find that when adjustments are made to correct for new understanding of the experiments, the value of the interaction parameter at low density is lower than previous reported, but still significantly higher than theoretically predicted.

Using the reciprocal space, two types of structures are simple to identify: simple periodic (photonic crystals), which have high diffractive efficiencies but sparse resonances (narrow-band), and random structures, with a continuous reciprocal space (broadband) but suffering from low diffraction efficiencies. A third type, quasirandom structures, lies in between; these provide high diffractive efficiency over a target wavelength range, which is broader than simple photonic crystals but narrower than a random structure. These structures are promising for ultrathin solar cells due to their broader nature. We present our numerical work towards evolving simple photonic crystals in quasirandom structures, and our fabrication approach based on polymer-blend lithography, with initial results on solar cells.

Ultrathin solar cells reduce material usage and allow the use of lower-quality materials thanks to their one order of magnitude smaller thickness than their conventional counterparts. However, efficient photonic light-trapping is required to harvest the incident light efficiently for an otherwise insufficient absorber thickness. Quasi-random photonic crystals are predicted to have high efficient light-trapping while being more robust under angle and thickness variations than simple photonic crystals. Here we experimentally demonstrate a light-trapping solution based on quasi-random photonic crystals fabricated by polymer blend lithography. We control the average lattice parameter by modifying the spin-coating speed. We demonstrate an ultrathin GaAs cell of 260 nm with a rear quasi-random pattern with submicron features, and a Jsc = 26.4 mA/cm2 and an efficiency of 22.35% under the global solar spectrum.

Solid-state dispersions of isolated single-walled carbon nanotubes (SWCNTs) in polymer matrices or networks of electronically coupled SWCNTs are gaining interest for a broad variety of optoelectronic applications. However, little is known about either the stability or degradation mechanisms of these systems. We show dramatic sp2-to-sp3 defect transformations of the SWCNT sidewall when either the S11 or S22 exciton transitions are optically pumped in ambient conditions, leading to the rapid decay of absorption and emission properties in less than 24 h for conditions similar to exposure to solar illumination. Importantly, we demonstrate that either (i) encapsulation to block reactive O2 from SWCNT excited states or (ii) exciton quenching via donor-to-acceptor electron transfer is an effective route for "kinetic stabilization" against photodegradation, with <8% loss in absorbance after 1200 h of illumination. We find that SWCNT:polymer loading does not impact degradation. Our study suggests that the sp3 defects are associated with the formation of oxygenic groups on the SWCNT sidewall. While such defect populations can detrimentally evolve over time in films where SWCNTs are environmentally exposed in the presence of light, we offer multiple pathways to arrest this degradation and enable their robust application as advanced optical materials in optical and electronic devices.

Equilibrium Bose-Einstein condensation of exciton-polaritons, demonstrated with a long-lifetime microcavity [Phys. Rev. Lett. 118, 016602 (2017)], has proven that driven-dissipative systems can undergo thermodynamic phase transitions in the limit where the quasiparticle lifetime exceeds the thermalization time. Here, we identify the role of dimensionality and polariton interactions in determining the degree of thermalization in optically generated traps. To distinguish the effect of trapping from interactions and lifetimes, we measured the polariton distribution under four nonresonant Gaussian pumps in a square geometry and compared it with polariton distributions measured with each pump individually. We found that significant redistribution of polaritons arises by trapping and modification of the density of states. Surprisingly efficient polariton-polariton scattering below the condensation threshold is evidenced by the depletion of the inflection-point polaritons. Our work provides a deeper understanding of polariton distributions and their interactions under various geometries of optically generated potentials.

Exploiting the extraordinary transport and optical properties of 3D topological semimetals for device applications requires epitaxial integration with semiconductors to carefully control carrier transport, yet no studies have established heteroepitaxy on top of any topological semimetals to date. Here, a novel approach toward fabricating heterostructures is demonstrated by epitaxially incorporating the Dirac semimetal Cd 3 As 2 between Zn x Cd 1‐x Te and CdTe layers via molecular beam epitaxy on GaAs (001) substrates. The approach utilizes the higher energy (001) surface of Cd 3 As 2 to stabilize 2D epitaxy of zinc blende semiconductors. To demonstrate the impact heterostructure formation offers to device performance, an all‐epitaxial, barrier‐type vertical photodetector is fabricated that accesses a different carrier separation mechanism than previously reported non‐epitaxial junctions and consequently exhibits significantly reduced dark currents. The results highlight the important role that epitaxial integration can play in accessing advanced architectures for topological semimetal‐based devices.

The classic Bogoliubov theory of weakly interacting Bose gases rests upon the assumption that nearly all the bosons condense into the lowest quantum state at sufficiently low temperatures. Here we develop a generalized version of Bogoliubov theory for the case of a driven-dissipative exciton-polariton condensate with a large incoherent uncondensed component, or excitonic reservoir. We argue that such a reservoir can consist of both excitonic high-momentum polaritons and optically dark superpositions of excitons across different optically active layers, such as multiple quantum wells in a microcavity. In particular, we predict interconversion between the dark and bright (light-coupled) excitonic states that can lead to a dynamical equilibrium between the condensate and reservoir populations. We show that the presence of the reservoir fundamentally modifies both the energy and the amplitudes of the Bogoliubov quasiparticle excitations due to the non-Galilean-invariant nature of polaritons. Our theoretical findings are supported by our experiment, where we directly detect the Bogoliubov excitation branches of an optically trapped polariton condensate in the high-density regime. By analyzing the measured occupations of the excitation branches, we extract the Bogoliubov amplitudes across a range of momenta and show that they agree with our generalized theory.

Topological insulators are a class of electronic materials exhibiting robust edge states immune to perturbations and disorder. This concept has been successfully adapted in photonics, where topologically nontrivial waveguides and topological lasers were developed. However, the exploration of topological properties in a given photonic system is limited to a fabricated sample, without the flexibility to reconfigure the structure in situ. Here, we demonstrate an all-optical realization of the orbital Su–Schrieffer–Heeger model in a microcavity exciton-polariton system, whereby a cavity photon is hybridized with an exciton in a GaAs quantum well. We induce a zigzag potential for exciton polaritons all-optically by shaping the nonresonant laser excitation, and measure directly the eigenspectrum and topological edge states of a polariton lattice in a nonlinear regime of bosonic condensation. Furthermore, taking advantage of the tunability of the optically induced lattice, we modify the intersite tunneling to realize a topological phase transition to a trivial state. Our results open the way to study topological phase transitions on-demand in fully reconfigurable hybrid photonic systems that do not require sophisticated sample engineering.

Collective (elementary) excitations of quantum bosonic condensates, including condensates of exciton polaritons in semiconductor microcavities, are a sensitive probe of interparticle interactions. In anisotropic microcavities with momentum-dependent transverse-electric-transverse-magnetic splitting of the optical modes, the excitations' dispersions are predicted to be strongly anisotropic, which is a consequence of the synthetic magnetic gauge field of the cavity, as well as the interplay between different interaction strengths for polaritons in the singlet and triplet spin configurations. Here, by directly measuring the dispersion of the collective excitations in a high-density optically trapped exciton-polariton condensate, we observe excellent agreement with the theoretical predictions for spinor polariton excitations. We extract the interaction constants for polaritons of the same and opposite spin and map out the characteristic spin textures in an interacting spinor condensate of exciton polaritons.

We report the observation of low-energy, low-momenta collective oscillations of an excitonpolariton condensate in a round "box" trap. The oscillations are dominated by the dipole and breathing modes, and the ratio of the frequencies of the two modes is consistent with that of a weakly interacting two-dimensional trapped Bose gas. The speed of sound extracted from the dipole oscillation frequency is smaller than the Bogoliubov sound, which can be partly explained by the influence of the incoherent reservoir. These results pave the way for understanding the effects of reservoir, dissipation, energy relaxation, and finite temperature on the superfluid properties of exciton-polariton condensates and other two-dimensional open-dissipative quantum fluids.

We have observed the effect of pseudomagnetic field originating from the polaritonic analog of spin-orbit coupling [transverse electric and transverse magnetic (TE-TM) splitting] on a polariton condensate in a ring-shaped microcavity. The effect gives rise to a stable four-leaf pattern around the ring as seen from the linear polarization measurements of the condensate photoluminescence. This pattern is found to originate from the interplay of the cavity potential, energy relaxation, and TE-TM splitting in the ring. Our observations are compared to the dissipative one-dimensional spinor Gross-Pitaevskii equation with the TE-TM splitting energy, which shows good qualitative agreement.

The Higgs amplitude mode is a collective excitation studied and observed in a broad class of matter, including superconductors, charge density waves, antiferromagnets, He-3 p-wave superfluid, and ultracold atomic condensates. In all the observations reported thus far, the amplitude mode was excited by perturbing the condensate out of equilibrium. Studying an exciton-polariton condensate, here, we report the observation of this amplitude mode purely driven by intrinsic quantum fluctuations without such perturbations. By using an ultrahigh quality microcavity and a Raman spectrometer to maximally reject photoluminescence (PL) from the condensate, we observe weak but distinct PL at energies below the condensate emission. We identify this as the so-called ghost branches of the amplitude mode arising from quantum depletion of the condensate into this mode. These energies, as well as the overall structure of the PL spectra, are in good agreement with our theoretical analysis.

Two-dimensional metal-halide perovskites (MHPs) are versatile solution-processed organic/inorganic quantum wells where the structural anisotropy creates profound anisotropy in their electronic and excitonic properties and associated optical constants. We here employ a wholistic framework, based on semiempirical modeling (k·p/effective mass theory calculations) informed by hybrid density functional theory (DFT) and multimodal spectroscopic ellipsometry on (C6H5(CH2)2NH3)2PbI4 films and crystals, that allows us to link the observed optical properties and anisotropy precisely to the underlying physical parameters that shape the electronic structure of a layered MHP. We find substantial frequency-dependent anisotropy in the optical constants and close correspondence between experiment and theory, demonstrating a high degree of in-plane alignment of the two-dimensional planes in both spin-coated thin films and cleaved single crystals made in this study. Hybrid DFT results elucidate the degree to which organic and inorganic frontier orbitals contribute to optical transitions polarized along a particular axis. The combined experimental and theoretical approach enables us to estimate the fundamental electronic bandgap of 2.65-2.68 eV in this prototypical 2D perovskite and to determine the spin-orbit coupling (ΔSO = 1.20 eV) and effective crystal field (δ = -1.36 eV) which break the degeneracy of the frontier conduction band states and determine the exciton fine structure. The methods and results described here afford a better understanding of the connection between structure and induced optical anisotropy in quantum-confined MHPs, an important structure-property relationship for optoelectronic applications and devices.

Traditional metallic contacts on solar cells can cover a substantial portion of the device area, resulting in shadowing of light that diminishes the amount of current collected. In this paper, we developed trapezoidal electron-beam evaporated Ti/Al front grid fingers on GaAs single-junction solar cells to decrease the optical shadowing and increase the photogenerated current. We observe a high fill factor of 87% at 1-Sun light intensity and we observe no degradation on the open-circuit voltage. The short-circuit current density is found to increase by 0.4 mA/cm2 when compared to previously demonstrated electroplated Ni/Au front grid fingers, resulting in an efficiency improvement of ~0.8% absolute.