Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3.

Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. The van der Waals magnet chromium triiodide (CrI3) has been shown to be a layered antiferromagnetic insulator in its few-layer form1, opening up opportunities for various functionalities2-7 in electronic and optical devices. Here we report an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI3. The observed second-harmonic generation (SHG; a nonlinear optical process that converts two photons of the same frequency into one photon of twice the fundamental frequency) is several orders of magnitude larger than known magnetization-induced SHG8-11 and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far12,13 (for example, molybdenum disulfide). We show that although the parent lattice of bilayer CrI3 is centrosymmetric, and thus does not contribute to the SHG signal, the observed giant nonreciprocal SHG originates only from the layered antiferromagnetic order, which breaks both the spatial-inversion symmetry and the time-reversal symmetry. Furthermore, polarization-resolved measurements reveal underlying C2h crystallographic symmetry-and thus monoclinic stacking order-in bilayer CrI3, providing key structural information for the microscopic origin of layered antiferromagnetism14-18. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.

Femtosecond Dynamics of a Polariton Bosonic Cascade at Room Temperature.

Whispering gallery modes in a microwire are characterized by a nearly equidistant energy spectrum. In the strong exciton-photon coupling regime, this system represents a bosonic cascade: a ladder of discrete energy levels that sustains stimulated transitions between neighboring steps. Here, by using a femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of polaritons in a bosonic cascade based on a one-dimensional ZnO whispering gallery microcavity are explicitly visualized. Clear ladder-form build-up processes from higher to lower energy branches of the polariton condensates are observed, which are well reproduced by modeling using rate equations. Remarkably, a pronounced superbunching feature, which could serve as solid evidence for bosonic cascades, is demonstrated by the measured second-order time correlation factor. In addition, the nonlinear polariton parametric scattering dynamics on a time scale of hundreds of femtoseconds are revealed. Our understandings pave the way toward ultrafast coherent control of polaritons at room temperature.

Perovskite semiconductors for room-temperature exciton-polaritonics.

Lead-halide perovskites are generally excellent light emitters and can have larger exciton binding energies than thermal energy at room temperature, exhibiting great promise for room-temperature exciton-polaritonics. Rapid progress has been made recently, although challenges and mysteries remain in lead-halide perovskite semiconductors to push polaritons to room-temperature operation. In this Perspective, we discuss fundamental aspects of perovskite semiconductors for exciton-polaritons and review the recent rapid experimental advances using lead-halide perovskites for room-temperature polaritonics, including the experimental realization of strong light-matter interaction using various types of microcavities as well as reaching the polariton condensation regime in planar microcavities and lattices.

Optically Controlled Femtosecond Polariton Switch at Room Temperature.

Exciton polaritons have shown great potential for applications such as low-threshold lasing, quantum simulation, and dissipation-free circuits. In this paper, we realize a room temperature ultrafast polaritonic switch where the Bose-Einstein condensate population can be depleted at the hundred femtosecond timescale with high extinction ratios. This is achieved by applying an ultrashort optical control pulse, inducing parametric scattering within the photon part of the polariton condensate via a four-wave mixing process. Using a femtosecond angle-resolved spectroscopic imaging technique, the erasure and revival of the polariton condensates can be visualized. The condensate depletion and revival are well modeled by an open-dissipative Gross-Pitaevskii equation including parametric scattering process. This pushes the speed frontier of all-optical controlled polaritonic switches at room temperature towards the THz regime.

Probing the Chiral Domains and Excitonic States in Individual WS2 Tubes by Second-Harmonic Generation.

Distinct from carbon nanotubes, transition-metal dichalcogenide (TMD) nanotubes are noncentrosymmetric and polar and can exhibit some intriguing phenomena such as nonreciprocal superconductivity, chiral shift current, bulk photovoltaic effect, and exciton-polaritons. However, basic characterizations of individual TMD nanotubes are still quite limited, and much remains unclear about their structural chirality and electronic properties. Here we report an optical second-harmonic generation (SHG) study on multiwalled WS2 nanotubes on a single-tube level. As it is highly sensitive to the crystallographic symmetry, SHG microscopy unveiled multiple structural domains within a single WS2 nanotube, which are otherwise hidden under conventional white-light optical microscopy. Moreover, the polarization-resolved SHG anisotropy patterns revealed that different domains on the same tube can be of different chirality. In addition, we observed the excitonic states of individual WS2 nanotubes via SHG excitation spectroscopy, which were otherwise difficult to acquire due to the indirect band gap of the material.

Room-Temperature Macroscopic Coherence of Two Electron-Hole Plasmas in a Microcavity.

Macroscopic coherence of Bose condensates is a fundamental and practical phenomenon in many-body systems, such as the long-range correlation of exciton-polariton condensates with a dipole density typically below the exciton Mott-transition limit. Here we extend the macroscopic coherence of electron-hole-photon interacting systems to a new region in the phase diagram-the high-density plasma region, where long-range correlation is generally assumed to be broken due to the rapid dephasing. Nonetheless, a cooperative state of electron-hole plasma does emerge through the sharing of the superfluorescence field in an optical microcavity. In addition to the in situ coherence of e-h plasma, a long-range correlation is formed between two 8-µm-spaced plasma ensembles even at room temperature. Quantized and self-modulated correlation modes are generated for e-h ensembles in the plasma region. By controlling the distance between the two ensembles, multiple coupling regimes are revealed, from strong correlation to perturbative phase correlation and finally to an incoherent classical case, which has potential implications for tunable and high-temperature-compatible quantum devices.

Weak lasing in one-dimensional polariton superlattices.

Bosons with finite lifetime exhibit condensation and lasing when their influx exceeds the lasing threshold determined by the dissipative losses. In general, different one-particle states decay differently, and the bosons are usually assumed to condense in the state with the longest lifetime. Interaction between the bosons partially neglected by such an assumption can smear the lasing threshold into a threshold domain--a stable lasing many-body state exists within certain intervals of the bosonic influxes. This recently described weak lasing regime is formed by the spontaneously symmetry breaking and phase-locking self-organization of bosonic modes, which results in an essentially many-body state with a stable balance between gains and losses. Here we report, to our knowledge, the first observation of the weak lasing phase in a one-dimensional condensate of exciton-polaritons subject to a periodic potential. Real and reciprocal space photoluminescence images demonstrate that the spatial period of the condensate is twice as large as the period of the underlying periodic potential. These experiments are realized at room temperature in a ZnO microwire deposited on a silicon grating. The period doubling takes place at a critical pumping power, whereas at a lower power polariton emission images have the same periodicity as the grating.

Room-Temperature Polariton Lasing in All-Inorganic Perovskite Nanoplatelets.

Polariton lasing is the coherent emission arising from a macroscopic polariton condensate first proposed in 1996. Over the past two decades, polariton lasing has been demonstrated in a few inorganic and organic semiconductors in both low and room temperatures. Polariton lasing in inorganic materials significantly relies on sophisticated epitaxial growth of crystalline gain medium layers sandwiched by two distributed Bragg reflectors in which combating the built-in strain and mismatched thermal properties is nontrivial. On the other hand, organic active media usually suffer from large threshold density and weak nonlinearity due to the Frenkel exciton nature. Further development of polariton lasing toward technologically significant applications demand more accessible materials, ease of device fabrication, and broadly tunable emission at room temperature. Herein, we report the experimental realization of room-temperature polariton lasing based on an epitaxy-free all-inorganic cesium lead chloride perovskite nanoplatelet microcavity. Polariton lasing is unambiguously evidenced by a superlinear power dependence, macroscopic ground-state occupation, blueshift of the ground-state emission, narrowing of the line width and the buildup of long-range spatial coherence. Our work suggests considerable promise of lead halide perovskites toward large-area, low-cost, high-performance room-temperature polariton devices and coherent light sources extending from the ultraviolet to near-infrared range.

Exciton-polariton light-emitting diode based on a ZnO microwire.

Room temperature electrically pumped exciton-polariton light-emitting diode (LED) based on the n-ZnO microwire/MgO/p-GaN heterojunction was fabricated. With the injection current of 1.5 mA, the ultraviolet electroluminescence centered at wavelength of 400 nm is obtained. The whispering gallery cavity model combined with the coupling oscillator model is used to describe the emission intensity modulation, from which the strong coupling regime of the system is proved to be surviving at room temperature.

Exciton-Polariton Fano Resonance Driven by Second Harmonic Generation.

Angle-resolved second harmonic generation (SHG) spectra of ZnO microwires show characteristic Fano resonances in the spectral vicinity of exciton-polariton modes. We observe a resonant peak followed by a strong dip in SHG originating from the constructive and destructive interference of the nonresonant SHG and the resonant contribution of the polariton mode. It is demonstrated that the Fano line shape, and thus the Fano asymmetry parameter q, can be tuned by the phase shift of the two channels. We develop a model to calculate the phase-dependent q as a function of the radial angle in the microwire and achieve a good agreement with the experimental results. The deduced phase-to-q relation unveils the crucial information about the dynamics of the system and offers a tool for control on the line shape of the SHG spectra in the vicinity of exciton-polariton modes.

Enhancing Perovskite Solar Cell Performance by Interface Engineering Using CH3NH3PbBr0.9I2.1 Quantum Dots.

To improve the interfacial charge transfer that is crucial to the performance of perovskite solar cells, the interface engineering in a device should be rationally designed. Here we have developed an interface engineering method to tune the photovoltaic performance of planar-heterojunction perovskite solar cells by incorporating MAPbBr3-xIx (MA = CH3NH3) quantum dots (QDs) between the MAPbI3 perovskite film and the hole-transporting material (HTM) layer. By adjustment of the Br:I ratio, the as-synthesized MAPbBr3-xIx QDs show tunable fluorescence and band edge positions. When the valence band (VB) edge of MAPbBr3-xIx QDs is located below that of the MAPbI3 perovskite, the hole transfer from the MAPbI3 perovskite film to the HTM layer is hindered, and hence, the power conversion efficiency decreases. In contrast, when the VB edge of MAPbBr3-xIx QDs is located between the VB edge of the MAPbI3 perovskite film and the highest occupied molecular orbital of the HTM layer, the hole transfer from the MAPbI3 perovskite film to the HTM layer is well-facilitated, resulting in significant improvements in the fill factor, short-circuit photocurrent, and power conversion efficiency.

Three-dimensional confinement of polaritons in ZnO microcylinder.

High quality ZnO microcylinders (MCDs), which naturally form three-dimensional (3D) optical microcavities, were synthesized by a simple vapor transportation deposition method. The exciton-polariton effects in these 3D microcavities were investigated through the angle-resolved micro-photoluminescence (µ-PL) mappings. By using the coupled oscillator model, the 3D confinement effect of polaritons, i.e., two-dimensional (2D) whispering gallery (WG) type confinement in the cross section of the ZnO MCD, overlapping with the one-dimensional (1D) Fabry-Pérot (F-P) type confinement along the c-axis, was well interpreted.

Strong bound exciton-photon coupling in ZnO whispering gallery microcavity.

We report the cathodoluminescence (CL) study of bound-exciton-polaritons in ZnO whispering gallery (WG) microcavity. Thanks to the very high spatial resolution (: 100 nm) of CL technique, a scanning CL mapping along the tapered ZnO nanowire is achieved. We observe a clear anticrossing behavior which demonstrates the strong coupling between cavity mode and bound-excitons. Coupled oscillator model including both bound excitons and free excitons fits well with the experimental results. The energy splitting of bound-exciton-polaritons:2.6 meV is obtained.

Spin-resolved Purcell effect in a quantum dot microcavity system.

We demonstrate the spin selective coupling of the exciton state with cavity mode in a single quantum dot (QD)-micropillar cavity system. By tuning an external magnetic field, each spin polarized exciton state can be selectively coupled with the cavity mode due to the Zeeman effect. A significant enhancement of spontaneous emission rate of each spin state is achieved, giving rise to a tunable circular polarization degree from -90% to 93%. A four-level rate equation model is developed, and it agrees well with our experimental data. In addition, the coupling between photon mode and each exciton spin state is also achieved by varying temperature, demonstrating the full manipulation over the spin states in the QD-cavity system. Our results pave the way for the realization of future quantum light sources and the quantum information processing applications.

Room-temperature polariton parametric scattering driven by a one-dimensional polariton condensate.

We demonstrate a novel way to realize room-temperature polariton parametric scattering in a one-dimensional ZnO microcavity. The polariton parametric scattering is driven by a polariton condensate, with a balanced polariton pair generated at the adjacent polariton mode. This parametric scattering is experimentally investigated by the angle-resolved photoluminescence spectroscopy technique under different pump powers and it is well described by the rate equation of interacting bosons. The direct relation between the intensity of the scattered polariton signal and that of the polariton reservoir is acquired under nonresonant excitation, exhibiting the explicit nonlinear characteristic of this room-temperature polariton parametric process.

Excitation-polarization-dependent dynamics of polariton condensates in the ZnO microwire at room temperature.

Based on ZnO microcavities with high quality factors, where the gain medium exhibits confinement of wave packets due to the intrinsically formed whispering gallery microcavity, strong coupling between excitons and cavity photons can be obtained at room temperature resulting in hybrid quasiparticles, e.g. exciton polaritons. In this work, polariton condensation is induced under the non-resonant excitation by linearly polarized femtosecond laser pulses with different polarization directions. The dynamical angle-resolvedk-space spectra of the photoluminescence emission of polariton condensates are measured with sub-picosecond resolution by the self-developed femtosecond angle-resolved spectroscopic imaging technique. Our results show that the ultrafast dynamics of polariton condensation is sensitive to the polarization direction of the excitation pulses which can be explained qualitatively by the combined effect of selective excitation of distinct exciton modes in the sample and the effective coupling strength of the excitation pulses in the ZnO microcavity for various polarization directions. This work strengthened the understanding of the condensation process for cavity exciton polaritons at room temperature.

Localized-surface-plasmon enhanced emission from porous silicon by gold nanoparticles.

The porous silicon (PS) samples, decorated by Au nanoparticles (NPs) possessing localized-surface-plasmon (LSP) resonance, are prepared by the conventional anodization method. Photoluminescence (PL) is studied systematically, in particular, its dependence on the excitation power. It is found that undecorated PS samples exhibit a saturation behavior in PL intensity with increasing the pumping laser power, while the luminescence of Au-decorated PS hybrid samples have a purely linear dependence on the excitation power. In the linear response region of PS samples, addition of metal NPs layer moderately suppresses the emission while, in the saturation region, the net emission is enhanced by approximately up to 4-fold. Several possible mechanisms are discussed. We believe that the observed PL enhancement in saturation region is dominantly due to the resonant coupling between the LSP of Au NPs and the electronic excitation of PS, which inhibits the nonradiative Auger recombination process at high excitation power. These results indicate that the plasmon effect could be useful for designing even more efficient optoelectronic devices such as super bright light emitting devices and solar cells with high efficiencies. Despite many challenges, Au NPs can potentially be applied to introduce LSP resonance for the future silicon-based optoelectronics or photonics.

Ultrafast dynamics of exciton-polariton in optically tailored potential landscapes at room temperature.

In this work, by using femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of confined exciton-polaritons in an optical induced potential well based on a ZnO whispering-gallery microcavity is explicitly visualized. The sub-picosecond transition between succeeding quantum harmonic oscillator states can be experimentally distinguished. The landscape of the potential well can be modified by the pump power, the spatial distance and the time delay of the two input laser pulses. Clarifying the underlying mechanism of the polariton harmonic oscillator is interesting for the applications of polariton-based optoelectronic devices and quantum information processing.

Quasi-whispering gallery modes of exciton-polaritons in a ZnO microrod.

We report the photoluminescence (PL) investigations of quasi-whispering gallery mode (quasi-WGM) polaritons in a ZnO microrod at room temperature. By using the confocal micro-PL spectroscopic technique, we observe the clear optical quasi-WGMs. These quasi-WGMs appeared in the ultraviolet (UV) emission region where the cavity modes strongly couple with excitons and form polaritons. The quasi-WGMs polaritons can be well described by the plane wave interference and the coupling oscillator model.

Magnetic field control of the quantum chaotic dynamics of hydrogen analogs in an anisotropic crystal field.

We report magnetic field control of the quantum chaotic dynamics of hydrogen analogues in an anisotropic solid state environment. The chaoticity of the system dynamics was quantified by means of energy level statistics. We analyzed the magnetic field dependence of the statistical distribution of the impurity energy levels and found a smooth transition between the Poisson limit and the Wigner limit, i.e., transition between regular Poisson and fully chaotic Wigner dynamics. The effect of the crystal field anisotropy on the quantum chaotic dynamics, which manifests itself in characteristic transitions between regularity and chaos for different field orientations, was demonstrated.