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Tunable biphoton quantum entanglement generated from nonlinear processes is highly desirable for cutting-edge quantum technologies, yet its tunability is substantially constrained by the symmetry of material nonlinear tensors. Here, we overcome this constraint by introducing symmetry-breaking in nonlinear polarization to generate optically tunable biphoton entanglement at picosecond speeds. Asymmetric optical responses have made breakthroughs in classical applications like non-reciprocal light transmission. We now experimentally demonstrate the nonlinear asymmetry response for biphoton entanglement using a semiconductor metasurface incorporating [110] InGaP nano-resonators with structural asymmetry. We realize continuous tuning of polarization entanglement from near-unentangled states to a Bell state. This tunability can also extend to produce tailored hyperentanglement. Furthermore, our nanoscale entanglement source features an ultra-high coincidence-to-accidental ratio of $\approx7\times10^4$, outperforming existing semiconductor flat optics by two orders of magnitude. Introducing asymmetric nonlinear response in quantum metasurfaces opens new directions for tailoring on-demand quantum states and beyond., Comment: 27 pages, 4 figures

Active wavelength-scale optoelectronic components are widely used in photonic integrated circuitry, however coherent sources of light -- namely optical lasers -- remain the most challenging component to integrate. Semiconductor nanowire lasers represent a flexible class of light source where each nanowire is both gain material and cavity; however, strong coupling between these properties and the performance leads to inhomogeneity across the population. While this has been studied and optimized for individual material systems, no architecture-wide insight is available. Here, nine nanowire laser material systems are studied and compared using 55,516 nanowire lasers to provide statistically robust insight into performance. These results demonstrate that, while it may be important to optimise internal quantum efficiency for certain materials, cavity effects are always critical. Our study provides a roadmap to optimize the performance of nanowire lasers made from any material: this can be achieved by ensuring a narrow spread of lengths and end-facet reflectivities.

Diabetic ketoacidosis (DKA) is a life-threatening acute complication of diabetes in which ketone bodies accumulate in the blood. Breath acetone (a ketone) directly correlates with blood ketones, such that breath acetone monitoring could be used to improve safety in diabetes care. In this work, we report the design and fabrication of a chitosan/Pt/InP nanowire array based chemiresistive acetone sensor. By implementing chitosan as a surface functionalization layer and a Pt Schottky contact for efficient charge transfer processes and photovoltaic effect, self-powered, highly selective acetone sensing has been achieved. This sensor has an ultra-wide detection range from sub-ppb to >100,000 ppm levels at room temperature, incorporating the range from healthy individuals (300-800 ppb) to those at high-risk of DKA (> 75 ppm). The nanowire sensor has been further integrated into a handheld breath testing prototype, the Ketowhistle, which can successfully detect different ranges of acetone concentrations in simulated breath. The Ketowhistle demonstrates immediate potential for non-invasive ketone testing and monitoring for persons living with diabetes, in particular for DKA prevention.

Single-photon detector (SPD), an essential building block of the quantum communication system, plays a fundamental role in developing next-generation quantum technologies. In this work, we propose an efficient modeling workflow of nanowire SPDs utilizing avalanche breakdown at reverse-biased conditions. The proposed workflow is explored to maximize computational efficiency and balance time-consuming drift-diffusion simulation with fast script-based post-processing. Without excessive computational effort, we could predict a suite of key device performance metrics, including breakdown voltage, dark/light avalanche built-up time, photon detection efficiency, dark count rate, and the deterministic part of timing jitter due to device structures. Implementing the proposed workflow onto a single InP nanowire and comparing it to the extensively studied planar devices and superconducting nanowire SPDs, we showed the great potential of nanowire avalanche SPD to outperform their planar counterparts and obtain as superior performance as superconducting nanowires, i.e., achieve a high photon detection efficiency of 70% with a dark count rate less than 20 Hz at non-cryogenic temperature. The proposed workflow is not limited to single-nanowire or nanowire-based device modeling and can be readily extended to more complicated two-/three dimensional structures.

Nanowire devices have long been proposed as an efficient alternative to their planar counterparts for different optoelectronic applications. Unfortunately, challenges related to the growth and characterization of doping and p-n junction formation in nanowire devices (along axial or radial axis) have significantly impeded their development. The problems are further amplified if a p-n junction has to be implemented radially. Therefore, even though radial junction devices are expected to be on par with their axial junction counterparts, there are minimal reports on high-performance radial junction nanowire optoelectronic devices. This paper summarizes our recent results on the simulation and fabrication of radial junction nanowire solar cells and photodetectors, which have shown unprecedented performance and clearly demonstrate the importance of radial junction for optoelectronic applications. Our simulation results show that the proposed radial junction device is both optically and electrically optimal for solar cell and photodetector applications, especially if the absorber quality is extremely low. The radial junction nanowire solar cells could achieve a 17.2% efficiency, whereas the unbiased radial junction photodetector could show sensitivity down to a single photon level using an absorber with a lifetime of less than 50 ps. In comparison, the axial junction planar device made using same substrate as absorber showed less than 1% solar cell efficiency and almost no photodetection at 0 V. This study is conclusive experimental proof of the superiority of radial junction nanowire devices over their thin film or axial junction counterparts, especially when absorber lifetime is extremely low. The proposed device holds huge promise for III-V based photovoltaics and photodetectors.

We demonstrate a non-monotonic evolution of thermal conductivity of large-area hexagonal boron nitride films with thickness. Wrinkles and defects/impurities are present in these films. Raman spectroscopy, an optothermal non-contact technique, is employed to probe the temperature and laser power dependence property of the Raman active E2ghigh phonon mode, which in turn is used to estimate the rise in the temperature of the films under different laser powers. As the conventional Fourier law of heat diffusion cannot be directly employed analytically to evaluate the thermal conductivity of these films with defects and wrinkles, finite element modeling is used instead. In the model, average heat resistance is used to incorporate an overall defect structure, and Voronoi cells with contact resistance at the cell boundaries are constructed to mimic the wrinkled domains. The effective thermal conductivity is estimated to be 87, 55, and 117 W/m.K for the 2, 10, and 30 nm-thick films, respectively. We also present a quantitative estimation of the thermal resistance by defects and wrinkles individually to the heat flow. Our study reveals that the defects/impurities render a much higher resistance to heat transfer in the films than wrinkles., Comment: 24 pages, 8 figures, minor changes

Highly sensitive photodetectors with single photon level detection is one of the key components to a range of emerging technologies, in particular the ever-growing field of optical communication, remote sensing, and quantum computing. Currently, most of the single-photon detection technologies require external biasing at high voltages and/or cooling to low temperatures, posing great limitations for wider applications. Here, we demonstrate InP nanowire array photodetectors that can achieve single-photon level light detection at room temperature without an external bias. We use top-down etched, heavily doped p-type InP nanowires and n-type AZO/ZnO carrier selective contact to form a radial p-n junction with a built-in electric field exceeding 3x10^5 V/cm at 0 V. The device exhibits broadband light sensitivity and can distinguish a single photon per pulse from the dark noise at 0 V, enabled by its design to realize near-ideal broadband absorption, extremely low dark current, and highly efficient charge carrier separation. Meanwhile, the bandwidth of the device reaches above 600 MHz with a timing jitter of 538 ps. The proposed device design provides a new pathway towards low-cost, high-sensitivity, self-powered photodetectors for numerous future applications.

We present single-mode nanowire (NW) lasers with ultralow threshold in the near-infrared spectral range. To ensure the single-mode operation, the NW diameter and length are reduced specifically to minimize the longitudinal and transverse modes of the NW cavity. Increased optical losses and reduced gain volume by the dimension reduction are compensated by excellent NW morphology and InGaAs/GaAs multi-quantum disks. At 5 K, a threshold low as 1.6 {\mu}J/cm2 per pulse is achieved with a resulting quality factor exceeding 6400. By further passivating the NW with an AlGaAs shell to suppress surface non-radiative recombination, single-mode lasing operation is obtained with a threshold of only 48 {\mu}J/cm2 per pulse at room temperature with a high characteristic temperature of 223 K and power output of ~ 0.9 {\mu}W. These single-mode, ultralow threshold, high power output NW lasers are promising for the development of near-infrared nanoscale coherent light sources for integrated photonic circuits, sensing, and spectroscopy.

Both axial and radial junction nanowire solar cells have their challenges and advantages. However, so far, there is no review that explicitly provides a detailed comparative analysis of both axial and radial junction solar cells. This article reviews some of the recent results on axial and radial junction nanowire solar cells with an attempt to perform a comparative study between the optical and device behavior of these cells. In particular, we start by reviewing different results on how the absorption can be tuned in axial and radial junction solar cells. We also discuss results on some of the critical device concepts that are required to achieve high efficiency in axial and radial junction solar cells. We include a section on new device concepts that can be realized in nanowire structures. Finally, we conclude this review by discussing a few of the standing challenges of nanowire solar cells., Comment: It is a comparative review on axial vs. radial junction solar cell

Infrared imaging is a crucial technique in a multitude of applications, including night vision, autonomous vehicles navigation, optical tomography, and food quality control. Conventional infrared imaging technologies, however, require the use of materials like narrow-band gap semiconductors which are sensitive to thermal noise and often require cryogenic cooling. Here, we demonstrate a compact all-optical alternative to perform infrared imaging in a metasurface composed of GaAs semiconductor nanoantennas, using a nonlinear wave-mixing process. We experimentally show the up-conversion of short-wave infrared wavelengths via the coherent parametric process of sum-frequency generation. In this process, an infrared image of a target is mixed inside the metasurface with a strong pump beam, translating the image from infrared to the visible in a nanoscale ultra-thin imaging device. Our results open up new opportunities for the development of compact infrared imaging devices with applications in infrared vision and life sciences., Comment: 32 pages, 13 figures

Single photon emitters (SPEs) in hexagonal boron nitride (hBN) have garnered significant attention over the last few years due to their superior optical properties. However, despite the vast range of experimental results and theoretical calculations, the defect structure responsible for the observed emission has remained elusive. Here, by controlling the incorporation of impurities into hBN and by comparing various synthesis methods, we provide direct evidence that the visible SPEs are carbon related. Room temperature optically detected magnetic resonance (ODMR) is demonstrated on ensembles of these defects. We also perform ion implantation experiments and confirm that only carbon implantation creates SPEs in the visible spectral range. Computational analysis of hundreds of potential carbon-based defect transitions suggest that the emission results from the negatively charged VBCN- defect, which experiences long-range out-of-plane deformations and is environmentally sensitive. Our results resolve a long-standing debate about the origin of single emitters at the visible range in hBN and will be key to deterministic engineering of these defects for quantum photonic devices.

Semiconductor nanowire (NW) lasers are a promising technology for the realisation of coherent optical sources with extremely small footprint. To fully realize their potential as building blocks in on-chip photonic systems, scalable methods are required for dealing with large populations of inhomogeneous devices that are typically randomly distributed on host substrates. In this work two complementary, high-throughput techniques are combined: the characterisation of nanowire laser populations using automated optical microscopy, and a high accuracy transfer printing process with automatic device spatial registration and transfer. In this work a population of NW lasers is characterised, binned by threshold energy density and subsequently printed in arrays onto a secondary substrate. Statistical analysis of the transferred and control devices show that the transfer process does not incur measurable laser damage and the threshold binning can be maintained. Analysis is provided on the threshold and mode spectra of the device populations to investigate the potential for using NW lasers for integrated systems fabrication., Comment: 18 pages, 7 figures

We use polarized photocurrent spectroscopy in a nanowire device to investigate the band structure of hexagonal Wurtzite InAs. Signatures of optical transitions between four valence bands and two conduction bands are observed which are consistent with the symmetries expected from group theory. The ground state transition energy identified from photocurrent spectra is seen to be consistent with photoluminescence emitted from a cluster of nanowires from the same growth substrate. From the energies of the observed bands we determine the spin orbit and crystal field energies in Wurtzite InAs. This information is essential to the development of crystal phase engineering of this important III-V semiconductor., Comment: 25 pages, 5 figures

We use Transient Rayleigh Scattering to study the thermalization of hot photoexcited carriers in single GaAsSb/InP nanowire heterostructures. By comparing the energy loss rate in single bare GaAsSb nanowires which do not show substantial hot carrier effects with the core-shell nanowires, we show that the presence of an InP shell substantially suppresses the LO phonon emission rate at low temperatures leading to strong hot carrier effects., Comment: 17 pages, 5 figures

Two-dimensional hexagonal boron nitride (h-BN) single crystals with various shapes have been synthesized by chemical vapor deposition over the past several years. Here we report the formation of three-leaf dart (3LD)-shaped single crystals of h-BN on Cu foil by atmospheric-pressure chemical vapor deposition. The leaves of the 3LD-shaped h-BN are as long as 18 {\mu}m and their edges are smooth armchair on one side and stepped armchair on the other. Careful analysis revealed that surface oxygen plays an important role in the formation of the 3LD shape. Oxygen suppressed h-BN nucleation by passivating Cu surface active sites and lowered the edge attachment energy, which caused the growth kinetics to change to a diffusion-controlled mode., Comment: 7 pages,6 figures

Eutectic related reaction is a special chemical/physical reaction involving multiple phases, solid and liquid. Visualization of phase reaction of composite nanomaterials with high spatial and temporal resolution provides a key understanding of alloy growth with important industrial applications. However, it has been a rather challenging task. Here we report the direct imaging and control of the phase reaction dynamics of a single, as-grown free-standing gallium arsenide nanowire encapped with a gold nanoparticle, free from environmental confinement or disturbance, using four-dimensional electron microscopy. The non-destructive preparation of as-grown free-standing nanowires without supporting films allows us to study their anisotropic properties in their native environment with better statistical character. A laser heating pulse initiates the eutectic related reaction at a temperature much lower than the melting points of the composite materials, followed by a precisely time-delayed electron pulse to visualize the irreversible transient states of nucleation, growth and solidification of the complex. Combined with theoretical modeling, useful thermodynamic parameters of the newly formed alloy phases and their crystal structures could be determined. This technique of dynamical control and 4D imaging of phase reaction processes on the nanometer-ultrafast time scale open new venues for engineering various reactions in a wide variety of other systems.

We investigate the dynamics of high aspect ratio nanowires trapped axially in a single gradient force optical tweezers. A power spectrum analysis of the Brownian dynamics reveals a broad spectral resonance of the order of a kHz with peak properties that are strongly dependent on the input trapping power. Modelling of the dynamical equations of motion of the trapped nanowire that incorporate non-conservative effects through asymmetric coupling between translational and rotational degrees of freedom provides excellent agreement with the experimental observations. An associated observation of persistent cyclical motion around the equilibrium trapping position using winding analysis provides further evidence for the influence of non-conservative forces.

Two-dimensional (2D) materials have emerged as promising candidates for miniaturized optoelectronic devices, due to their strong inelastic interactions with light. On the other hand, a miniaturized optical system also requires strong elastic light-matter interactions to control the flow of light. Here, we report giant optical path length (OPL) from a single-layer molybdenum disulfide (MoS2), which is around one order of magnitude larger than that from a single-layer graphene. Using such giant OPL to engineer the phase front of optical beams, we demonstrated, to the best of our knowledge, the world's thinnest optical lens consisting of a few layers of MoS2 less than 6.3 nm thick. Moreover, we show that MoS2 has much better dielectric response than good conductor (like gold) and other dielectric materials (like Si, SiO2 or graphene). By taking advantage of the giant elastic scattering efficiency in ultra-thin high-index 2D materials, we demonstrated high-efficiency gratings based on a single- or few-layers of MoS2. The capability of manipulating the flow of light in 2D materials opens an exciting avenue towards unprecedented miniaturization of optical components and the integration of advanced optical functionalities.

Using transient Rayleigh scattering (TRS) measurements, we obtain photoexcited carrier thermalization dynamics for both zincblende (ZB) and wurtzite (WZ) InP single nanowires (NW) with picosecond resolution. A phenomenological fitting model based on direct band to band transition theory is developed to extract the electron-hole-plasma density and temperature as a function of time from TRS measurements of single nanowires which have complex valence band structures. We find that the thermalization dynamics of hot carriers depends strongly on material (GaAs NW vs. InP NW) and less strongly on crystal structure (ZB vs. WZ). The thermalization dynamics of ZB and WZ InP NWs are similar. But a comparison of the thermalization dynamics in ZB and WZ InP NWs with ZB GaAs NW reveals more than an order of magnitude slower relaxation for the InP NWs. We interpret these results as reflecting their distinctive phonon band structures which lead to different hot phonon effects. Knowledge of hot carrier thermalization dynamics is an essential component for effective incorporation of nanowire materials into electronic devices.