Exciton polaritons, with extremely low effective mass1, are regarded as promising candidates to realize Bose–Einstein condensation in lattices for quantum simulations2 towards room-temperature ...operations3–8. Along with the condensation, an efficient exciton polariton quantum simulator9 would require a strong lattice with robust polariton trapping as well as strong intersite coupling to allow coherent quantum motion of polaritons within the lattice. A strong lattice can be characterized with a larger forbidden bandgap opening and a larger lattice bandwidth compared with the linewidth. However, exciton polaritons in such strong lattices have only been shown to condense at cryogenic temperatures3–8. Here, we report the observation of non-equilibrium exciton polariton condensation in a one-dimensional strong lead halide perovskite lattice at room temperature. Modulated by deep periodic potentials, the strong lead halide perovskite lattice exhibits a large forbidden bandgap opening up to 13.3 meV and a lattice band up to 8.5 meV wide, which are at least 10 times larger than previous systems. Above a critical density, we observe polariton condensation into py orbital states with long-range spatial coherence at room temperature. Our result opens the route to the implementation of polariton condensates in quantum simulators at room temperature.Non-equilibrium Bose–Einstein condensation of exciton polaritons in chains of lead halide perovskite pillars can occur at room temperature. These condensates have long spatial coherence.
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.An outlook on the potential of lead-halide perovskites as a playground for exciton-polariton studies and for the development of polaritonic devices operating at room temperature is provided.
Abstract
Metallic tungsten disulfide (WS
2
) monolayers have been demonstrated as promising electrocatalysts for hydrogen evolution reaction (HER) induced by the high intrinsic conductivity, however, ...the key challenges to maximize the catalytic activity are achieving the metallic WS
2
with high concentration and increasing the density of the active sites. In this work, single-atom-V catalysts (V SACs) substitutions in 1T-WS
2
monolayers (91% phase purity) are fabricated to significantly enhance the HER performance via a one-step chemical vapor deposition strategy. Atomic-resolution scanning transmission electron microscopy (STEM) imaging together with Raman spectroscopy confirm the atomic dispersion of V species on the 1T-WS
2
monolayers instead of energetically favorable 2H-WS
2
monolayers. The growth mechanism of V SACs@1T-WS
2
monolayers is experimentally and theoretically demonstrated. Density functional theory (DFT) calculations demonstrate that the activated V-atom sites play vital important role in enhancing the HER activity. In this work, it opens a novel path to directly synthesize atomically dispersed single-metal catalysts on metastable materials as efficient and robust electrocatalysts.
Semiconductor micro/nano‐cavities with high quality factor (Q) and small modal volume provide critical platforms for exploring strong light‐matter interactions and quantum optics, enabling further ...development of coherent and quantum photonic devices. Constrained by exciton binding energy and thermal fluctuation, only a handful of wide‐band semiconductors such as ZnO and GaN have stable excitons at room temperature. Metal halide perovskite with cubic lattice and well‐controlled exciton may provide solutions. In this work, high‐quality single‐crystalline cesium lead halide CsPbX3 (X = Cl, Br, I) whispering‐gallery‐mode (WGM) microcavities are synthesized by vapor‐phase van der Waals epitaxy method. The as‐grown perovskites show strong emission and stable exciton at room temperature over the whole visible spectra range. By varying the halide composition, multi‐color (400–700 nm).WGM excitonic lasing is achieved at room temperature with low threshold (~ 2.0 μJ cm−2) and high spectra coherence (~0.14–0.15 nm). The results advocate the promise of inorganic perovskites towards development of optoelectronic devices and strong light‐matter coupling in quantum optics.
High‐quality cesium lead halide nanoplatelets functioning as whispering‐gallery‐mode microcavities are synthesized by vapor‐phase van der Waals epitaxy method. Multicolor, low‐threshold excitonic lasing action with a high spectra coherence of 0.14–0.15 nm is realized at room temperature. The findings are not only important for developing on‐chip small lasers and high‐speed exciton devices but also promising for fundamental studies in cavity quantum electrodynamics.
Optical irradiation accompanied by spontaneous anti-Stokes emission can lead to cooling of matter, in a phenomenon known as laser cooling, or optical refrigeration, which was proposed by Pringsheim ...in 1929. In gaseous matter, an extremely low temperature can be obtained in diluted atomic gases by Doppler cooling, and laser cooling of ultradense gas has been demonstrated by collisional redistribution of radiation. In solid-state materials, laser cooling is achieved by the annihilation of phonons, which are quanta of lattice vibrations, during anti-Stokes luminescence. Since the first experimental demonstration in glasses doped with rare-earth metals, considerable progress has been made, particularly in ytterbium-doped glasses or crystals: recently a record was set of cooling to about 110 kelvin from the ambient temperature, surpassing the thermoelectric Peltier cooler. It would be interesting to realize laser cooling in semiconductors, in which excitonic resonances dominate, rather than in systems doped with rare-earth metals, where atomic resonances dominate. However, so far no net cooling in semiconductors has been achieved despite much experimental and theoretical work, mainly on group-III-V gallium arsenide quantum wells. Here we report a net cooling by about 40 kelvin in a semiconductor using group-II-VI cadmium sulphide nanoribbons, or nanobelts, starting from 290 kelvin. We use a pump laser with a wavelength of 514 nanometres, and obtain an estimated cooling efficiency of about 1.3 per cent and an estimated cooling power of 180 microwatts. At 100 kelvin, 532-nm pumping leads to a net cooling of about 15 kelvin with a cooling efficiency of about 2.0 per cent. We attribute the net laser cooling in cadmium sulphide nanobelts to strong coupling between excitons and longitudinal optical phonons (LOPs), which allows the resonant annihilation of multiple LOPs in luminescence up-conversion processes, high external quantum efficiency and negligible background absorption. Our findings suggest that, alternatively, group-II-VI semiconductors with strong exciton-LOP coupling could be harnessed to achieve laser cooling and open the way to optical refrigeration based on semiconductors.
Celotno besedilo
Dostopno za:
DOBA, IJS, IZUM, KILJ, KISLJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Near-infrared (NIR) solid-state micro/nanolasers are important building blocks for true integration of optoelectronic circuitry. Although significant progress has been made in III–V nanowire lasers ...with achieving NIR lasing at room temperature, − challenges remain including low quantum efficiencies and high Auger losses. Importantly, the obstacles toward integrating one-dimensional nanowires on the planar ubiquitous Si platform need to be effectively tackled. Here we demonstrate a new family of planar room-temperature NIR nanolasers based on organic–inorganic perovskite CH3NH3PbI3-aXa (X = I, Br, Cl) nanoplatelets. Their large exciton binding energies, long diffusion lengths, and naturally formed high-quality planar whispering-gallery mode cavities ensure adequate gain and efficient optical feedback for low-threshold optically pumped in-plane lasing. We show that these remarkable wavelength tunable whispering-gallery nanolasers can be easily integrated onto conductive platforms (Si, Au, indium tin oxide, and so forth). Our findings open up a new class of wavelength tunable planar nanomaterials potentially suitable for on-chip integration.
Optical irradiation with suitable energy can cool solids, a phenomenon known as optical refrigeration, first proposed in 1929 and experimentally achieved in ytterbium-doped glasses in 1995. Since ...then, considerable progress has been made in various rare earth element-doped materials, with a recent record of cooling to 91 K directly from ambient temperatures. For practical use and to suit future applications of optical refrigeration, the discovery of materials with facile and scalable synthesis and high cooling power density will be required. Herein we present the realization of a net cooling of 23.0 K in micrometre-thick 3D CH3 NH3 PbI3 (MAPbI3 ) and 58.7 K in exfoliated 2D (C6 H5 C2 H4 NH3 )2 PbI4 (PhEPbI4 ) perovskite crystals directly from room temperature. We found that the perovskite crystals exhibit strong photoluminescence upconversion and near unity external quantum efficiency, properties that are responsible for the realization of net laser cooling. Our findings indicate that solution-processed perovskite thin films may be a highly suitable candidate for constructing integrated optical cooler devices.
Photoacoustic (PA) imaging holds great promise for preclinical research and clinical practice. However, most studies rely on the laser wavelength in the first near-infrared (NIR) window (NIR-I, ...650–950 nm), while few studies have been exploited in the second NIR window (NIR-II, 1000–1700 nm), mainly due to the lack of NIR-II absorbing contrast agents. We herein report the synthesis of a broadband absorbing PA contrast agent based on semiconducting polymer nanoparticles (SPN-II) and apply it for PA imaging in NIR-II window. SPN-II can absorb in both NIR-I and NIR-II regions, providing the feasibility to directly compare PA imaging at 750 nm with that at 1064 nm. Because of the weaker background PA signals from biological tissues in NIR-II window, the signal-to-noise ratio (SNR) of SPN-II resulted PA images at 1064 nm can be 1.4-times higher than that at 750 nm when comparing at the imaging depth of 3 cm. The proof-of-concept application of NIR-II PA imaging is demonstrated in in vivo imaging of brain vasculature in living rats, which showed 1.5-times higher SNR as compared with NIR-I PA imaging. Our study not only introduces the first broadband absorbing organic contrast agent that is applicable for PA imaging in both NIR-I and NIR-II windows but also reveals the advantages of NIR-II over NIR-I in PA imaging.
Heterostructures consisting of 2D layered perovskites are expected to exhibit interesting physical phenomena inaccessible to the single 2D perovskites and can greatly extend their functionalities for ...electronic and optoelectronic applications. Herein, we develop a solution method to synthesize (C4H9NH3)2PbI4/(C4H9NH3)2(CH3NH3)Pb2I7 heterostructures with centimeter size, high phase purity, controllable thickness and junction depth, high crystalline quality, and great stability for highly narrow dual-band photodetectors. On the basis of the different lattice constant, solubility, and growth rate between (C4H9NH3)2PbI4 and (C4H9NH3)2(CH3NH3)Pb2I7, the designed synthetic method allows to first grow the (C4H9NH3)2PbI4 at the water–air interface and subsequently the (C4H9NH3)2(CH3NH3)Pb2I7 layer is formed via a diffusion process. Such a growth process provides an efficient way for us to readily obtain heterostructures with various thickness and junction depth by controlling the concentration, reaction temperature, and time. The formation of heterostructures has been verified by X-ray diffraction, cross-section photoluminescence, and reflection spectroscopy with the estimated junction width below 100 nm. Photodetectors based on such heterostructures exhibit low dark current (∼10–12 A), high on–off current ratio (∼103), and highly narrow dual-band spectral response with a full-width at half-maximum (fwhm) of 20 nm at 540 nm and 34 nm at 610 nm. The high performance can be attributed to the high crystalline quality of the heterostructures and the extremely large resistance in the out-of-plane direction. The synthetic strategy is versatile for other 2D perovskites, and the narrow dual-band spectral response with all fwhm < 40 nm can be continuously tuned from red to blue by properly changing the halide compositions.
NiFe‐based layered double hydroxides (LDHs) are among the most efficient oxygen evolution reaction (OER) catalysts in alkaline medium, but their long‐term OER stabilities are questionable. In this ...work, it is demonstrated that the layered structure makes bulk NiFe LDH intrinsically not stable in OER and the deactivation mechanism of NiFe LDH in OER is further revealed. Both operando electrochemical and structural characterizations show that the interlayer basal plane in bulk NiFe LDH contributes to the OER activity, and the slow diffusion of proton acceptors (e.g., OH−) within the NiFe LDH interlayers during OER causes dissolution of NiFe LDH and therefore decrease in OER activity with time. To improve diffusion of proton acceptors, it is proposed to delaminate NiFe LDH into atomically thin nanosheets, which is able to effectively improve OER stability of NiFe LDH especially at industrial operating conditions such as elevated operating temperatures (e.g., at 80 °C) and large current densities (e.g., at 500 mA cm−2).
The interlayer basal plane in bulk NiFe layered double hydroxide (LDH) contributes to the oxygen evolution reaction (OER) activity. Restricted diffusion of proton acceptors within the interlayers of bulk NiFe LDH causes catalyst dissolution. Exfoliating multilayered NiFe LDH into single‐layered nanosheets greatly improves the catalytic stability of NiFe LDH in alkaline OER.
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