Strong nonlinear optical processes with extraordinary polarization anisotropy in inversion-symmetry broken two-dimensional PdPSe.

Nonlinear optical activities, especially second harmonic generation (SHG), are key phenomena in inversion-symmetry-broken two-dimensional (2D) transition metal dichalcogenides (TMDCs). On the other hand, anisotropic nonlinear optical processes are important for unique applications in nano-nonlinear photonic devices with polarization functions, having become one of focused research topics in the field of nonlinear photonics. However, the strong nonlinearity and strong optical anisotropy do not exist simultaneously in common 2D materials. Here, we demonstrate strong second-order and third-order susceptibilities of 64 pm/V and 6.2×10-19 m2/V2, respectively, in the even-layer PdPSe, which has not been discovered in other common TMDCs (e.g., MoS2). Strikingly, it also simultaneously exhibited strong SHG anisotropy with an anisotropic ratio of ~45, which is the largest reported among all 2D materials to date, to the best of our knowledge. In addition, the SHG anisotropy ratio can be harnessed from 0.12 to 45 (375 times) by varying the excitation wavelength due to the dispersion of χ ( 2 ) values. As an illustrative example, we further demonstrate polarized SHG imaging for potential applications in crystal orientation identification and polarization-dependent spatial encoding. These findings in 2D PdPSe are promising for nonlinear nanophotonic and optoelectronic applications.

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.

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.

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.

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.

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.

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).

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.

2D Ruddlesden-Popper perovskite sensitized SnP2S6 ultraviolet photodetector enabling high responsivity and fast speed.

As the newly developed wide-bandgap semiconductors, two-dimensional layered metal phosphorus chalcogenides (2D LMPCs) exhibit enormous potential applications in ultraviolet (UV) photodetection due to their superior optoelectronic performance. However, 2D LMPC-based UV photodetectors generally suffer from low responsivity and slow response speed, which hinder their practical applications. Here, we present an effective strategy of sensitizing 2D LMPC UV photodetectors with a 2D Ruddlesden-Popper (RP) perovskite to enable high responsivity and fast response speed. As a demonstration, a hybrid heterojunction composed of RP perovskite (PEA)2PbI4 and a 2D SnP2S6 flake is fabricated by spin-coating method. Benefitting from the strong optical absorption of (PEA)2PbI4 and the efficient interfacial charge transfer caused by the favorable type-II energy band alignment, the as-fabricated 2D SnP2S6/(PEA)2PbI4 hybrid heterojunction photodetectors show high responsivity (67.1 A W-1), large detectivity (2.8 × 1011 Jones), fast rise/delay time (30/120 µs) and excellent external quantum efficiency (22825%) at 365 nm. Under field-effect modulation, the responsivity of the heterojunction photodetector can reach up to 239.4 A W-1, which is attributed to the photogating mechanism and reduced Schottky barriers. Owing to the excellent photodetection performance, the heterojunction device further shows superior imaging capability. This work provides an effective strategy for designing high-performance UV photodetectors toward future applications.

On-chip mid-infrared photothermoelectric detectors for full-Stokes detection.

On-chip polarimeters are highly desirable for the next-generation ultra-compact optical and optoelectronic systems. Polarization-sensitive photodetectors relying on anisotropic absorption of natural/artificial materials have emerged as a promising candidate for on-chip polarimeters owing to their filterless configurations. However, these photodetectors can only be applied for detection of either linearly or circularly polarized light, not applicable for full-Stokes detection. Here, we propose and demonstrate three-ports polarimeters comprising on-chip chiral plasmonic metamaterial-mediated mid-infrared photodetectors for full-Stokes detection. By manipulating the spatial distribution of chiral metamaterials, we could convert polarization-resolved absorptions to corresponding polarization-resolved photovoltages of three ports through the photothermoelectric effect. We utilize the developed polarimeter in an imaging demonstration showing reliable ability for polarization reconstruction. Our work provides an alternative strategy for developing polarization-resolved photodetectors with a bandgap-independent operation range in the mid-infrared.

Switchable Unipolar-Barrier Van der Waals Heterostructures with Natural Anisotropy for Full Linear Polarimetry Detection.

Polarization-resolved photodetection in a compact footprint is of great interest for ultraminiaturized polarimeters to be used in a wide range of applications. However, probing the states of polarization (SOP) in materials with natural anisotropy are usually weak, limited by the material's natural dichroism or diattenuation. Here, a twisted unipolar-barrier van der Waals heterostructure (vdWH) to construct a bias-switchable polarization detection for retrieval of full SOP (from 0 to 180°) for linear polarized incident light is reported. As a demonstration example, this study realizes the concept in a b-AsP/WS2 /b-AsP vdWH relying on the natural anisotropic properties of the materials without using additional plasmonic/metasurface nanostructures to realize linear polarimetry in the mid-infrared range. Polarimetric imaging is further demonstrated with the developed linear polarimetry by directly displaying the Jones-vector-described SOP distribution of certain target object. This method, with the capabilities of detecting full linear SOP, is promising for the next-generation on-chip miniaturized polarimeters.

Spin Ordering Induced Broadband Photodetection Based on Two-Dimensional Magnetic Semiconductor α-MnSe.

Two-dimensional (2D) magnetic semiconductors are considered to have great application prospects in spintronic logic devices, memory devices, and photodetectors, due to their unique structures and outstanding physical properties in 2D confinement. Understanding the influence of magnetism on optical/optoelectronic properties of 2D magnetic semiconductors is a significant issue for constructing multifunctional electronic devices and implementing sophisticated functions. Herein, the influence of spin ordering and magnons on the optical/optoelectronic properties of 2D magnetic semiconductor α-MnSe synthesized by space-confined chemical vapor deposition (CVD) is explored systematically. The spin-ordering-induced magnetic phase transition triggers temperature-dependent photoluminescence spectra to produce a huge transition at Néel temperature (TN  ≈ 160 K). The magnons- and defects-induced emissions are the primary luminescence path below TN and direct internal 4 a T1g →6 A1g transition-induced emissions are the main luminescence path above TN . Additionally, the magnons and defect structures endow 2D α-MnSe with a broadband luminescence from 550 to 880 nm, and an ultraviolet-near-infrared photoresponse from 365 to 808 nm. Moreover, the device also demonstrates improved photodetection performance at 80 K, possibly influenced by spin ordering and trap states associated with defects. These above findings indicate that 2D magnetic semiconductor α-MnSe provides an excellent platform for magneto-optical and magneto-optoelectronic research.

Improved Polarization in the Sr6 Cd2 Sb6 O7 Se10 Oxyselenide through Design of Lateral Sublattices for Efficient Photoelectric Conversion.

Highly-polarizable materials are favorable for photoelectric conversion due to their efficient charge separation, while precise design of them is still a big challenge. Herein a novel polar oxyselenide, Sr6 Cd2 Sb6 O7 Se10 , is rationally designed. It contains lateral sublattices of polarizable [Sb2 OSe4 ]4- chains and highly-orientated [CdSe3 ]4- chains. The intense polarization was evaluated by significant second-harmonic generation (SHG) signal (maximum: 12.6×AgGaS2 ) in broad spectrum range. The polarization was found to mainly improve the carrier separation with a much longer recombination lifetime (76.5 µs) than that of the nonpolar compound Sr2 Sb2 O2 Se3 (18.0 µs), resulting in better photoelectric performance. The single-crystal photoelectric device exhibited excellent response covering broad spectrum in 500-1000 nm with stable reproducibility. This work provides some new insights into the structure design of highly-polarizable heteroanionic materials for photoelectric conversion.

Discovery of Robust Ferroelectricity in 2D Defective Semiconductor α-Ga2 Se3.

2D ferroelectrics with robust polar order in the atomic-scale thickness at room temperature are needed to miniaturize ferroelectric devices and tackle challenges imposed by traditional ferroelectrics. These materials usually have polar point group structure regarding as a prerequisite of ferroelectricity. Yet, to introduce polar structure into otherwise nonpolar 2D materials for producing ferroelectricity remains a challenge. Here, by combining first-principles calculations and experimental studies, it is reported that the native Ga vacancy-defects located in the asymmetrical sites in cubic defective semiconductor α-Ga2 Se3 can induce polar structure. Meanwhile, the induced polarization can be switched in a moderate energy barrier. The switched polarization is observed in 2D α-Ga2 Se3 nanoflakes of ≈4 nm with a high switching temperature up to 450 K. Such polarization switching could arise from the displacement of Ga vacancy between neighboring asymmetrical sites by applying an electric field. This work removes the point group limit for ferroelectricity, expanding the range of 2D ferroelectrics into the native defective semiconductors.

Van der Waals Epitaxy of Bi2 Te2 Se/Bi2 O2 Se Vertical Heterojunction for High Performance Photodetector.

Bismuth oxyselenide (Bi2 O2 Se) has emerged as a promising candidate for electronic and optoelectronic applications due to its outstanding electron mobility and ambient stability. However, high dark current and relatively slow photoresponse that originate from high charge carrier concentration as well as bolometric effect in Bi2 O2 Se inhibit further improvement of Bi2 O2 Se based photodetectors. Here, a one-step van der Waals (vdW) epitaxy synthesis of Bi2 Te2 Se/Bi2 O2 Se vertical heterojunction with type-II band alignment and high-quality interface is demonstrated. The crystal quality and uniformity of the heterojunction are supported by Raman, transmission electron microscopy and energy dispersive spectroscopy results. A photodetector based on Bi2 Te2 Se/Bi2 O2 Se heterojunction demonstrates steady photoresponse over a large wavelength range (532-1456 nm), with a high specific responsivity of 2.21 × 103 A W-1 at 532 nm and fast response speed of 50 ms. Moreover, field effect regulation allows for further improvement of the photoresponse performance of the heterojunction field effect transistor device, where the responsivity can be increased to 3.34 × 103 A W-1 with a 60 V gate voltage. Overall, the one-step vdW epitaxy process is a promising and convenient route towards constructing high quality Bi2 O2 Se based heterojunction for improving its photodetection performance.

Epitaxial Growth of 2D Ultrathin Metastable γ-Bi2 O3 Flakes for High Performance Ultraviolet Photodetection.

Ultraviolet detection is of great significance due to its wide applications in the missile tracking, flame detecting, pollution monitoring, and so on. The nonlayered semiconductor γ-Bi2 O3 is a promising candidate toward high-performance UV detection due to the wide bandgap, excellent light sensitivity, environmental stability, nontoxic and elemental abundance properties. However, controllable preparation of ultrathin 2D γ-Bi2 O3 flakes remains a challenge, owing to its nonlayered structure, metastable nature, and other competing phases. Moreover, the UV photodetectors based on 2D γ-Bi2 O3 flake have not been implemented yet. Here, ultrathin (down to 4.8 nm) 2D γ-Bi2 O3 flakes with high crystal quality are obtained via a van der Waals epitaxy method. The as-synthesized single-crystalline γ-Bi2 O3 flakes show a body-centered cubic structure and grown along (111) lattice plane as revealed by experimental observations. More importantly, photodetectors based on the as-synthesized 2D γ-Bi2 O3 flakes exhibit promising UV detection ability, including a responsivity of 64.5 A W-1 , a detectivity of 1.3 × 1013 Jones, and an ultrafast response speed (τrise  ≈ 290 µs and τdecay  ≈ 870 µs) at 365 nm, suggesting its great potential for various optoelectronic applications.