Extraordinary Enhancement of Nonlinear Optical Interaction in NbOBr2 Microcavities.

2D materials are burgeoning as promising candidates for investigating nonlinear optical effects due to high nonlinear susceptibilities, broadband optical response, and tunable nonlinearity. However, most 2D materials suffer from poor nonlinear conversion efficiencies, resulting from reduced light-matter interactions and lack of phase matching at atomic thicknesses. Herein, a new 2D nonlinear material, niobium oxide dibromide (NbOBr2) is reported, featuring strong and anisotropic optical nonlinearities with scalable nonlinear intensity. Furthermore, Fabry-Pérot (F-P) microcavities are constructed by coupling NbOBr2 with air holes in silicon. Remarkable enhancement factors of ≈630 times in second harmonic generation (SHG) and 210 times in third harmonic generation (THG) are achieved on cavity at the resonance wavelength of 1500 nm. Notably, the cavity enhancement effect exhibits strong anisotropic feature tunable with pump wavelength, owing to the robust optical birefringence of NbOBr2. The ratio of the enhancement factor along the b- and c-axis of NbOBr2 reaches 2.43 and 5.27 for SHG and THG at 1500 nm pump, respectively, which leads to an extraordinarily high SHG anisotropic ratio of 17.82 and a 10° rotation of THG polarization. The research presents a feasible and practical strategy for developing high-efficiency and low-power-pumped on-chip nonlinear optical devices with tunable anisotropy.

Ultrastrong exciton-plasmon couplings in WS2 multilayers synthesized with a random multi-singular metasurface at room temperature.

Van der Waals semiconductors exemplified by two-dimensional transition-metal dichalcogenides have promised next-generation atomically thin optoelectronics. Boosting their interaction with light is vital for practical applications, especially in the quantum regime where ultrastrong coupling is highly demanded but not yet realized. Here we report ultrastrong exciton-plasmon coupling at room temperature in tungsten disulfide (WS2) layers loaded with a random multi-singular plasmonic metasurface deposited on a flexible polymer substrate. Different from seeking perfect metals or high-quality resonators, we create a unique type of metasurface with a dense array of singularities that can support nanometre-sized plasmonic hotspots to which several WS2 excitons coherently interact. The associated normalized coupling strength is 0.12 for monolayer WS2 and can be up to 0.164 for quadrilayers, showcasing the ultrastrong exciton-plasmon coupling that is important for practical optoelectronic devices based on low-dimensional semiconductors.

Multidimensional detection enabled by twisted black arsenic-phosphorus homojunctions.

A light field carrying multidimensional optical information, including but not limited to polarization, intensity and wavelength, is essential for numerous applications such as environmental monitoring, thermal imaging, medical diagnosis and free-space communications. Simultaneous acquisition of this multidimensional information could provide comprehensive insights for understanding complex environments but remains a challenge. Here we demonstrate a multidimensional optical information detection device based on zero-bias double twisted black arsenic-phosphorus homojunctions, where the photoresponse is dominated by the photothermoelectric effect. By using a bipolar and phase-offset polarization photoresponse, the device operated in the mid-infrared range can simultaneously detect both the polarization angle and incident intensity information through direct measurement of the photocurrents in the double twisted black arsenic-phosphorus homojunctions. The device's responsivity makes it possible to retrieve wavelength information, typically perceived as difficult to obtain. Moreover, the device exhibits an electrically tunable polarization photoresponse, enabling precise distinction of polarization angles under low-intensity light exposure. These demonstrations offer a promising approach for simultaneous detection of multidimensional optical information, indicating potential for diverse photonic applications.

Modal Phase-Matched Bound States in the Continuum for Enhancing Third Harmonic Generation of Deep Ultraviolet Emission.

Coherent deep ultraviolet (DUV) light sources are crucial for various applications such as nanolithography, biomedical imaging, and spectroscopy. DUV light sources can be generated by using conventional nonlinear optical crystals (NLOs). However, NLOs are limited by their bulky size, inadequate transparency at the DUV regime, and stringent phase-matching requirements for harmonic generation. Recently, dielectric metasurfaces support high Q-factor resonances and offer a promising approach for efficient harmonic generation at short wavelengths. In this study, we demonstrated a crystalline silicon (c-Si) metasurface simultaneously exciting modal phase-matched bound states in the continuum (BIC) resonance at the fundamental wavelength of 840 nm with a higher degree of freedom for precise control of the BIC resonance and a plasmonic resonance at the wavelength of 280 nm in the DUV to enhance third harmonic generation (THG). We experimentally achieved a Q-factor of ∼180 owing to the relatively large refractive index of the c-Si and the geometric symmetry breaking of the structure. We realized THG at a wavelength of 280 nm with a power of 14.5 nW by using a peak power density of 15 GW/cm2 excitation. The measured THG power is 14 times higher than the state-of-the-art THG dielectric metasurfaces using the same peak power density in the DUV regime, and the maximum obtained THG power enhancement factor is up to 48. This approach relies on the significant third-order nonlinear susceptibility of c-Si, the interband plasmonic nature of the c-Si in the DUV, and the strong field confinement of BIC resonance to boost overall nonlinear conversion efficiency to 5.2 × 10-6% in the DUV regime. Our work shows the potential of c-Si BIC metasurfaces for developing efficient and ultracompact DUV light sources using high-efficacy nonlinear optical devices.

Highly efficient octave-spanning long-wavelength infrared generation with a 74% quantum efficiency in a χ(2) waveguide.

The realization of compact and efficient broadband mid-infrared (MIR) lasers has enormous impacts in promoting MIR spectroscopy for various important applications. A number of well-designed waveguide platforms have been demonstrated for MIR supercontinuum and frequency comb generations based on cubic nonlinearities, but unfortunately third-order nonlinear response is inherently weak. Here, we propose and demonstrate for the first time a χ(2) micrometer waveguide platform based on birefringence phase matching for long-wavelength infrared (LWIR) laser generation with a high quantum efficiency. In a ZnGeP2-based waveguide platform, an octave-spanning spectrum covering 5-11 µm is generated through optical parametric generation (OPG). A quantum conversion efficiency of 74% as a new record in LWIR single-pass parametric processes is achieved. The threshold energy is measured as ~616 pJ, reduced by more than 1-order of magnitude as compared to those of MIR OPGs in bulk media. Our prototype micro-waveguide platform could be extended to other χ(2) birefringence crystals and trigger new frontiers of MIR integrated nonlinear photonics.

Impact of Cavity Geometry on Microlaser Dynamics.

We experimentally investigate spatiotemporal lasing dynamics in semiconductor microcavities with various geometries, featuring integrable or chaotic ray dynamics. The classical ray dynamics directly impacts the lasing dynamics, which is primarily determined by the local directionality of long-lived ray trajectories. The directionality of optical propagation dictates the characteristic length scales of intensity variations, which play a pivotal role in nonlinear light-matter interactions. While wavelength-scale intensity variations tend to stabilize lasing dynamics, modulation on much longer scales causes spatial filamentation and irregular pulsation. Our results will pave the way to control the lasing dynamics by engineering the cavity geometry and ray dynamical properties.

Mid-Infrared Bipolar and Unipolar Linear Polarization Detections in Nb2 GeTe4 /MoS2 Heterostructures.

Detecting and distinguishing light polarization states, one of the most basic elements of optical fields, have significant importance in both scientific studies and industry applications. Artificially fabricated structures, e.g., metasurfaces with anisotropic absorptions, have shown the capabilities of detecting polarization light and controlling. However, their operations mainly rely on resonant absorptions based on structural designs that are usually narrow bands. Here, a mid-infrared (MIR) broadband polarization photodetector with high PRs and wavelength-dependent polarities using a 2D anisotropic/isotropic Nb2 GeTe4 /MoS2 van der Waals (vdWs) heterostructure is demonstrated. It is shown that the photodetector exhibits high PRs of 48 and 34 at 4.6  and 11.0 µm wavelengths, respectively, and even a negative PR of -3.38 for 3.7 µm under the zero bias condition at room temperature. Such interesting results can be attributed to the superimposed effects of a photovoltaic (PV) mechanism in the Nb2 GeTe4 /MoS2 hetero-junction region and a bolometric mechanism in the MoS2 layer. Furthermore, the photodetector demonstrates its effectiveness in bipolar and unipolar polarization encoding communications and polarization imaging enabled by its unique and high PRs.

Long wavelength mid-infrared multi-gases spectroscopy using tunable single-mode slot waveguide quantum cascade laser.

Single-mode tunable quantum cascade lasers (QCLs) are promising for high-resolution and highly sensitive trace gases sensing across the mid-infrared (MIR) region. We report on the development of a tunable single-mode slot waveguide QCL array in the long wavelength part of the MIR regime (>12 µm). This laser array exhibits a tuning range of around 12 cm-1, from 735.3 to 747.3 cm-1. Using this developed single-mode tunable QCL, we demonstrate individual gas sensing, yielding the detection limit of 940 ppb and 470 ppb for acetylene and o-xylene, respectively. To verify the potential of the developed QCL array in multi-species gas detection, laser absorption measurements of two mixed gases of acetylene and o-xylene were conducted, showing the absorption features of the corresponding gases agree well with the theoretical predictions.

Long-wave infrared photothermoelectric detectors with ultrahigh polarization sensitivity.

Filter-free miniaturized polarization-sensitive photodetectors have important applications in the next-generation on-chip polarimeters. However, their polarization sensitivity is thus far limited by the intrinsic low diattenuation and inefficient photon-to-electron conversion. Here, we implement experimentally a miniaturized detector based on one-dimensional tellurium nanoribbon, which can significantly improve the photothermoelectric responses by translating the polarization-sensitive absorption into a large temperature gradient together with the finite-size effect of a perfect plasmonic absorber. Our devices exhibit a zero-bias responsivity of 410 V/W and an ultrahigh polarization ratio (2.5 × 104), as well as a peak polarization angle sensitivity of 7.10 V/W•degree, which is one order of magnitude higher than those reported in the literature. Full linear polarimetry detection is also achieved with the proposed device in a simple geometrical configuration. Polarization-coded communication and optical strain measurement are demonstrated showing the great potential of the proposed devices. Our work presents a feasible solution for miniaturized room-temperature infrared photodetectors with ultrahigh polarization sensitivity.

Extreme Polarization Anisotropy in Resonant Third-Harmonic Generation from Aligned Carbon Nanotube Films.

Carbon nanotubes (CNTs) possess extremely anisotropic electronic, thermal, and optical properties owing to their 1D character. While their linear optical properties have been extensively studied, nonlinear optical processes, such as harmonic generation for frequency conversion, remain largely unexplored in CNTs, particularly in macroscopic CNT assemblies. In this work, macroscopic films of aligned and type-separated (semiconducting and metallic) CNTs are synthesized and polarization-dependent third-harmonic generation (THG) from the films with fundamental wavelengths ranging from 1.5 to 2.5 µm is studied. Both films exhibited strongly wavelength-dependent, intense THG signals, enhanced through exciton resonances, and third-order nonlinear optical susceptibilities of 2.50 × 10-19  m2  V-2 (semiconducting CNTs) and 1.23 × 10-19  m2  V-2 (metallic CNTs), respectively are found, for 1.8 µm excitation. Further, through systematic polarization-dependent THG measurements, the values of all elements of the susceptibility tensor are determined, verifying the macroscopically 1D nature of the films. Finally, polarized THG imaging is performed to demonstrate the nonlinear anisotropy in the large-size CNT film with good alignment. These findings promise applications of aligned CNT films in mid-infrared frequency conversion, nonlinear optical switching, polarized pulsed lasers, polarized long-wave detection, and high-performance anisotropic nonlinear photonic devices.

Electrically-pumped compact topological bulk lasers driven by band-inverted bound states in the continuum.

One of the most exciting breakthroughs in physics is the concept of topology that was recently introduced to photonics, achieving robust functionalities, as manifested in the recently demonstrated topological lasers. However, so far almost all attention was focused on lasing from topological edge states. Bulk bands that reflect the topological bulk-edge correspondence have been largely missed. Here, we demonstrate an electrically pumped topological bulk quantum cascade laser (QCL) operating in the terahertz (THz) frequency range. In addition to the band-inversion induced in-plane reflection due to topological nontrivial cavity surrounded by a trivial domain, we further illustrate the band edges of such topological bulk lasers are recognized as the bound states in the continuum (BICs) due to their nonradiative characteristics and robust topological polarization charges in the momentum space. Therefore, the lasing modes show both in-plane and out-of-plane tight confinements in a compact laser cavity (lateral size ~3λlaser). Experimentally, we realize a miniaturized THz QCL that shows single-mode lasing with a side-mode suppression ratio (SMSR) around 20 dB. We also observe a cylindrical vector beam for the far-field emission, which is evidence for topological bulk BIC lasers. Our demonstration on miniaturization of single-mode beam-engineered THz lasers is promising for many applications including imaging, sensing, and communications.

Strong second-harmonic generation by sublattice polarization in non-uniformly strained monolayer graphene.

Despite the potential of graphene for building a variety of quantum photonic devices, its centrosymmetric nature forbids the observation of second harmonic generation (SHG) for developing second-order nonlinear devices. To activate SHG in graphene, extensive research efforts have been directed towards disrupting graphene's inversion symmetry using external stimuli like electric fields. However, these methods fail to engineer graphene's lattice symmetry, which is the root cause of the forbidden SHG. Here, we harness strain engineering to directly manipulate graphene's lattice arrangement and induce sublattice polarization to activate SHG. Surprisingly, the SHG signal is boosted 50-fold at low temperatures, which can be explained by resonant transitions between strain-induced pseudo-Landau levels. The second-order susceptibility of strained graphene is found to be larger than that of hexagonal boron nitride with intrinsic broken inversion symmetry. Our demonstration of strong SHG in strained graphene offers promising possibilities for developing high-efficiency nonlinear devices for integrated quantum circuits.

A two-dimensional mid-infrared optoelectronic retina enabling simultaneous perception and encoding.

Infrared machine vision system for object perception and recognition is becoming increasingly important in the Internet of Things era. However, the current system suffers from bulkiness and inefficiency as compared to the human retina with the intelligent and compact neural architecture. Here, we present a retina-inspired mid-infrared (MIR) optoelectronic device based on a two-dimensional (2D) heterostructure for simultaneous data perception and encoding. A single device can perceive the illumination intensity of a MIR stimulus signal, while encoding the intensity into a spike train based on a rate encoding algorithm for subsequent neuromorphic computing with the assistance of an all-optical excitation mechanism, a stochastic near-infrared (NIR) sampling terminal. The device features wide dynamic working range, high encoding precision, and flexible adaption ability to the MIR intensity. Moreover, an inference accuracy more than 96% to MIR MNIST data set encoded by the device is achieved using a trained spiking neural network (SNN).

Photonic Majorana quantum cascade laser with polarization-winding emission.

Topological cavities, whose modes are protected against perturbations, are promising candidates for novel semiconductor laser devices. To date, there have been several demonstrations of topological lasers (TLs) exhibiting robust lasing modes. The possibility of achieving nontrivial beam profiles in TLs has recently been explored in the form of vortex wavefront emissions enabled by a structured optical pump or strong magnetic field, which are inconvenient for device applications. Electrically pumped TLs, by contrast, have attracted attention for their compact footprint and easy on-chip integration with photonic circuits. Here, we experimentally demonstrate an electrically pumped TL based on photonic analogue of a Majorana zero mode (MZM), implemented monolithically on a quantum cascade chip. We show that the MZM emits a cylindrical vector (CV) beam, with a topologically nontrivial polarization profile from a terahertz (THz) semiconductor laser.

Higher-Order Topological States in Thermal Diffusion.

Unlike conventional topological materials that carry topological states at their boundaries, higher-order topological materials are able to support topological states at boundaries of boundaries, such as corners and hinges. While band topology has been recently extended into thermal diffusion for thermal metamaterials, its realization is limited to a 1D thermal lattice, lacking access to the higher-order topology. In this work, the experimental realization is reported of a higher-order thermal topological insulator in a generalized 2D diffusion lattice. The topological corner states for thermal diffusion are observed in the bandgap of diffusion rate of the bulk, as a consequence of the anti-Hermitian nature of the diffusion Hamiltonian. The topological protection of these thermal corner states is demonstrated with the stability of their diffusion profile in the presence of amorphous deformation. This work constitutes the first realization of higher-order topology in purely diffusive systems and opens the door for future thermal management with topological protection beyond 1D geometries.

Ultrastrong Optical Harmonic Generations in Layered Platinum Disulfide in the Mid-Infrared.

Nonlinear optical activities (e.g., harmonic generations) in two-dimensional (2D) layered materials have attracted much attention due to the great promise in diverse optoelectronic applications such as nonlinear optical modulators, nonreciprocal optical device, and nonlinear optical imaging. Exploration of nonlinear optical response (e.g., frequency conversion) in the infrared, especially the mid-infrared (MIR) region, is highly desirable for ultrafast MIR laser applications ranging from tunable MIR coherent sources, MIR supercontinuum generation, and MIR frequency-comb-based spectroscopy to high harmonic generation. However, nonlinear optical effects in 2D layered materials under MIR pump are rarely reported, mainly due to the lack of suitable 2D layered materials. Van der Waals layered platinum disulfide (PtS2) with a sizable bandgap from the visible to the infrared region is a promising candidate for realizing MIR nonlinear optical devices. In this work, we investigate the nonlinear optical properties including third-and fifth-harmonic generation (THG and FHG) in thin layered PtS2 under infrared pump (1550-2510 nm). Strikingly, the ultrastrong third-order nonlinear susceptibility χ(3)(-3ω;ω,ω,ω) of thin layered PtS2 in the MIR region was estimated to be over 10-18 m2/V2, which is about one order of that in traditional transition metal chalcogenides. Such excellent performance makes air-stable PtS2 a potential candidate for developing next-generation MIR nonlinear photonic devices.

High-harmonic generation in polycrystalline CdTe nano-films via macroscopic investigations.

Bright high harmonics generation (HHG) in CMOS-compatible nano-films can provide new opportunities for integrated coherent ultra-violet sources and attosecond photonic devices. Up to now, most HHG studies have been limited to single crystals. Polycrystalline materials, which consist of many grains separated by grain boundaries and normally have random crystallographic orientations, have rarely been explored for HHG. Understanding and predicting the HHG properties in polycrystalline nano-films are important owing to its merits of low cost and diversified properties, but challenging due to their complicated electronic structures. Here, we for the first time experimentally discover the correspondence between HHG in polycrystalline matters and macroscopic material parameters, to the best of our knowledge. Pumped by a mid-infrared femtosecond laser centered at 7.1 µm wavelength, bright and long-term stable harmonics extending to 25th orders (284 nm) are demonstrated in polycrystalline cadmium telluride (CdTe) nano-films. It is found that the HHG strengths in the transmission and the reflection behave differently as a function of the material thickness in the range from 6 nm to 4 µm, which is highly correlated to the measured macroscopic conductivity. The experimental findings agree well with the recent theoretical prediction [Phys. Rev. B103(15), 155426 (2021)10.1103/PhysRevB.103.155426]. This work provides a simple gauge to study and predict HHG in complicated polycrystalline and amorphous nano-systems, and paves the way for novel strong-field nanophotonics based on polycrystalline nano-films.

A Review of Machine Learning for Near-Infrared Spectroscopy.

The analysis of infrared spectroscopy of substances is a non-invasive measurement technique that can be used in analytics. Although the main objective of this study is to provide a review of machine learning (ML) algorithms that have been reported for analyzing near-infrared (NIR) spectroscopy from traditional machine learning methods to deep network architectures, we also provide different NIR measurement modes, instruments, signal preprocessing methods, etc. Firstly, four different measurement modes available in NIR are reviewed, different types of NIR instruments are compared, and a summary of NIR data analysis methods is provided. Secondly, the public NIR spectroscopy datasets are briefly discussed, with links provided. Thirdly, the widely used data preprocessing and feature selection algorithms that have been reported for NIR spectroscopy are presented. Then, the majority of the traditional machine learning methods and deep network architectures that are commonly employed are covered. Finally, we conclude that developing the integration of a variety of machine learning algorithms in an efficient and lightweight manner is a significant future research direction.

Efficient Avalanche Photodiodes with a WSe2/MoS2 Heterostructure via Two-Photon Absorption.

Two-dimensional (2D) materials-based photodetectors in the infrared range hold the key to enabling a wide range of optoelectronics applications including infrared imaging and optical communications. While there exist 2D materials with a narrow bandgap sensitive to infrared photons, a two-photon absorption (TPA) process can also enable infrared photodetection in well-established 2D materials with large bandgaps such as WSe2 and MoS2. However, most of the TPA photodetectors suffer from low responsivity, preventing this method from being widely adopted for infrared photodetection. Herein, we experimentally demonstrate 2D materials-based TPA avalanche photodiodes achieving an ultrahigh responsivity. The WSe2/MoS2 heterostructure absorbs infrared photons with an energy smaller than the material bandgaps via a low-efficiency TPA process. The significant avalanche effect with a gain of ∼1300 improves the responsivity, resulting in the record-high responsivity of 88 µA/W. We believe that this work paves the way toward building practical and high-efficiency 2D materials-based infrared photodetectors.