Two-dimensional Janus Polarization Functioned by Mechanical Force.

Two-dimensional (2D) polarization materials have emerged as promising candidates for meeting the demands of device miniaturization, attributed to their unique electronic configurations and transport characteristics. Although the existing inherent and sliding mechanisms have been increasingly investigated in recent years, strategies for inducing 2D polarization with innovative mechanisms remain rare. In this study, we introduce a novel 2D Janus state by modulating the puckered structure. Combining scanning probe microscopy, transmission electron microscopy, and density functional theory calculations, we realized force-triggered out-of-plane and in-plane dipoles with distorted smaller warping in GeSe. The Janus state is preserved after removing the external mechanical perturbation, which could be switched by modulating the sliding direction. Our work offers a versatile method to break the space inversion symmetry in a 2D system to trigger polarization in the atomic scale, which may open an innovative insight into configuring novel 2D polarization materials. This article is protected by copyright. All rights reserved.

Spectrometer-Less Remote Sensing Image Classification Based on Gate-Tunable van der Waals Heterostructures.

Remote sensing technology, which conventionally employs spectrometers to capture hyperspectral images, allowing for the classification and unmixing based on the reflectance spectrum, has been extensively applied in diverse fields, including environmental monitoring, land resource management, and agriculture. However, miniaturization of remote sensing systems remains a challenge due to the complicated and dispersive optical components of spectrometers. Here, m-phase GaTe0.5Se0.5 with wide-spectral photoresponses (250-1064 nm) and stack it with WSe2 are utilizes to construct a two-dimensional van der Waals heterojunction (2D-vdWH), enabling the design of a gate-tunable wide-spectral photodetector. By utilizing the multi-photoresponses under varying gate voltages, high accuracy recognition can be achieved aided by deep learning algorithms without the original hyperspectral reflectance data. The proof-of-concept device, featuring dozens of tunable gate voltages, achieves an average classification accuracy of 87.00% on 6 prevalent hyperspectral datasets, which is competitive with the accuracy of 250-1000 nm hyperspectral data (88.72%) and far superior to the accuracy of non-tunable photoresponse (71.17%). Artificially designed gate-tunable wide-spectral 2D-vdWHs GaTe0.5Se0.5/WSe2-based photodetector present a promising pathway for the development of miniaturized and cost-effective remote sensing classification technology.

Machine-learning-assisted and real-time-feedback-controlled growth of InAs/GaAs quantum dots.

The applications of self-assembled InAs/GaAs quantum dots (QDs) for lasers and single photon sources strongly rely on their density and quality. Establishing the process parameters in molecular beam epitaxy (MBE) for a specific density of QDs is a multidimensional optimization challenge, usually addressed through time-consuming and iterative trial-and-error. Here, we report a real-time feedback control method to realize the growth of QDs with arbitrary density, which is fully automated and intelligent. We develop a machine learning (ML) model named 3D ResNet 50 trained using reflection high-energy electron diffraction (RHEED) videos as input instead of static images and providing real-time feedback on surface morphologies for process control. As a result, we demonstrate that ML from previous growth could predict the post-growth density of QDs, by successfully tuning the QD densities in near-real time from 1.5 × 1010 cm-2 down to 3.8 × 108 cm-2 or up to 1.4 × 1011 cm-2. Compared to traditional methods, our approach can dramatically expedite the optimization process and improve the reproducibility of MBE. The concepts and methodologies proved feasible in this work are promising to be applied to a variety of material growth processes, which will revolutionize semiconductor manufacturing for optoelectronic and microelectronic industries.

Patterned growth of AgBiS2 nanostructures on arbitrary substrates for broadband and eco-friendly optoelectronic sensing.

The patterning of functional nanomaterials shows a promising path in the advanced fabrication of electronic and optoelectronic devices. Current micropatterning strategies are indispensable for post-etching/liftoff processes that contaminate/damage functional materials. Herein, we developed an innovative, low-temperature, post-liftoff-free, seed-confined fabricating strategy that can tackle this issue, thus achieving designated patterns of flower-shaped AgBiS2 nanostructures at either micro- or macro-scale on arbitrary substrates that are either rigid or flexible. Made of patterned AgBiS2 nanostructures, the photoconductor shows broadband (320 nm-2200 nm), sensitive (Rpeak = 1.56 A W-1), and fast (less than 100 µs) photoresponses. Furthermore, single-pixel raster-scanning and 28 × 12 focal plane array imaging were performed to demonstrate reliable and resolved electrical responses to optical patterns, showcasing the potential of the photoconductor in practical imaging applications. Notably, the patterning process enables strain-releasing micro-structures, which lead to the fabrication of a flexible photodetector with high durability upon over 1000 bending/recovering testing cycles. This study provides a simple, low-temperature, and eco-friendly strategy to address the current challenges in non-aggressive micro-fabrication and arbitrary patterning of semiconductors, which are promising to meet the development of further emerging technologies in scalable and wearable optoelectronic sensors.

Interlayer bond polarizability model for interlayer phonons in van der Waals heterostructures.

Raman scattering provides essential insights into phonons, electronic structures and electron-phonon coupling within solids through the intensity of Raman peaks, which cannot be easily quantified using the classical bond polarizability model. The interlayer bond polarizability model (IBPM) had been developed to understand the Raman intensity of layer-breathing modes (LBMs) in two-dimensional materials. However, the quantitative understanding of the LBM intensity of a van der Waals heterostructure (vdWH) remains challenging. Here, in polynary vdWHs comprising twisted multilayer graphene (tMLG), MoS2 and hBN, we observed a series of LBMs, whose intensity is markedly dependent on the excitation energy and twist angle of the tMLG constituent. An improved IBPM is proposed to quantitatively understand the Raman intensity of LBMs in the tMLG-based vdWHs, including the emergence or absence of a specific LBM when the excitation energy is resonant with the electronic states of tMLG or MoS2 constituents. This work underscores the significant potential of the improved IBPM in accurately understanding and predicting the intensity profile of LBM in polynary vdWHs, even for the case of Raman scattering with excitation energies selectively resonant with the electronic states of the corresponding specific constituents.

2D Ruddlesden-Popper Sn-Based Perovskite Weak Light Detector for Image Transmission and Reflection Imaging.

2D Ruddlesden-Popper Sn-based perovskite has excellent optoelectronic properties and weak halide ion migration characteristics, making it an ideal candidate for weak light detection, which has great potential in light communication, and medical applications. Although Sn-based perovskite photodetectors are developed, weak light detection is not demonstrated yet. Herein, a high-performance self-powered photodetector with the capability to detect ultra-weak light signals is designed based on vertical PEA2 SnI4 /Si nanowires heterojunction. Due to the low dark current and high light absorption efficiency, the devices present a remarkable responsivity of 42.4 mA W-1 , a high detectivity of 8 × 1011 Jones, and an ultralow noise current of 2.47 × 10-13 A Hz-1/2 . Especially, the device exhibits a high on-off current ratio of 18.6 at light signals as low as 4.60 nW cm-2 , revealing the capacity to detect ultra-weak light. The device is applied as a signal receiver and realized image transmission in light communication system. Moreover, high-resolution reflection imaging and multispectral imaging are obtained using the device as the sensor in the imaging system. These results reveal that 2D PEA2 SnI4 -based self-powered photodetectors with low-noise current possess enormous potential in future weak light detection.

Polarization- and Gate-Tunable Optoelectronic Reverse in 2D Semimetal/Semiconductor Photovoltaic Heterostructure.

Polarimetric photodetector can acquire higher resolution and more surface information of imaging targets in complex environments due to the identification of light polarization. To date, the existing technologies yet sustain the poor polarization sensitivity (<10), far from market application requirement. Here, the photovoltaic detectors with polarization- and gate-tunable optoelectronic reverse phenomenon are developed based on semimetal 1T'-MoTe2 and ambipolar WSe2 . The device exhibits gate-tunable reverse in rectifying and photovoltaic characters due to the directional inversion of energy band, yielding a wide range of current rectification ratio from 10-2 to 103 and a clear object imaging with 100 × 100 pixels. Acting as a polarimetric photodetector, the polarization ratio (PR) value can reach a steady state value of ≈30, which is compelling among the state-of-the-art 2D-based polarized detectors. The sign reversal of polarization-sensitive photocurrent by varying the light polarization angles is also observed, that can enable the PR value with a potential to cover possible numbers (1→+∞/-∞→-1). This work develops a photovoltaic detector with polarization- and gate-tunable optoelectronic reverse phenomenon, making a significant progress in polarimetric imaging and multifunction integration applications.

Polarization Reversal of Group IV-VI Semiconductors with Pucker-Like Structure: Mechanism Dissecting and Function Demonstration.

Polarization imaging presents advantages in capturing spatial, spectral, and polarization information across various spectral bands. It can improve the perceptual ability of image sensors and has garnered more applications. Despite its potential, challenges persist in identifying band information and implementing image enhancement using polarization imaging. These challenges often necessitate integrating spectrometers or other components, resulting in increased complexities within image processing systems and hindering device miniaturization trends. Here, the characteristics of anisotropic absorption reversal are systematically elucidated in pucker-like group IV-VI semiconductors MX (M = Ge, Sn; X = S, Se) through theoretical predictions and experimental validations. Additionally, the fundamental mechanisms behind anisotropy reversal in different bands are also explored. The photodetector is constructed by utilizing MX as a light-absorbing layer, harnessing polarization-sensitive photoresponse for virtual imaging. The results indicate that the utilization of polarization reversal photodetectors holds advantages in achieving further multifunctional integration within the device structure while simplifying its configuration, including band information identification and image enhancement. This study provides a comprehensive analysis of polarization reversal mechanisms and presents a promising and reliable approach for achieving dual-band image band identification and image enhancement without additional auxiliary components.

Giant enhancement of second-harmonic generation of indium selenide on planar Au.

Two-dimensional (2D) van der Waals layered γ-type indium selenide (γ-InSe) holds great promise for the development of ultrathin and low-energy-consumption nonlinear optical devices due to its broken inversion symmetry regardless of layer number. Nevertheless, the 2D InSe thin flakes still exhibit short light-matter interaction lengths, thus resulting in low efficiencies of nonlinear optical processes. In this work, we provide a facile 2D semiconductor-metal structure consisting of InSe thin flakes (thickness: 11-54 nm) on planar Au film, which exhibits great second-harmonic generation (SHG) enhancement by a factor of up to 1182. The SHG enhancement is attributed to the interference effect-induced strong electric field in highly absorbing InSe; meanwhile, the increase in reflectivity by Au film also plays an important role. Furthermore, the InSe thickness and excitation wavelength dependences of enhancement factors are revealed. This work provides a convenient approach to developing high-efficiency 2D nonlinear optical devices with ultrathin form.

Strong Exciton-Exciton Scattering of Exfoliated van der Waals InSe toward Efficient Continuous-Wave Near-Infrared P-Band Emission.

P-band emission is a superlinear low-coherence emission through exciton-exciton (X-X) scattering into photon-like states. It occurs without the prerequisites of population inversion or macroscopical coherence, rendering lower power consumption than the widely explored superlinear low-coherence emissions including superfluorescence, amplified spontaneous emission, and random lasing, and holds great potential for speckle-free imaging and interferometric sensing. However, competition processes including exciton dissociation and annihilation undermine its operation at room temperature and/or low excitation conditions. Here we report room-temperature P-band emission from InSe microflakes with excitation density of 1010 cm-2, offering 2-orders-of-magnitude lower operation density compared to the state-of-the-art superlinear low-coherence emissions. The efficient P-band emission is attributed to a large X-X scattering strength of 0.25 µeV µm2 due to enhanced spatial confinement along with intrinsic material metrics of 3D/2D exciton complex and asymmetric electron/hole mass. These findings open an avenue toward strong low-coherence near-infrared light sources based on van der Waals semiconductors.

Probing Anisotropic Deformation and Near-Infrared Emission Tuning in Thin-Layered InSe Crystal under High Pressure.

Indium selenide (InSe) exhibits high lattice compressibility and an extraordinary capability of tailoring the optical band gap under pressure beyond other 2D materials. Herein, by applying hydrostatic pressure via a diamond anvil cell, we revealed an anisotropic deformation dynamic and efficient manipulation of near-infrared light emission in thin-layered InSe strongly correlated to layer numbers (N = 5-30). As N > 20, the InSe lattice is compressed in all directions, and the intralayer compression leads to widening of the band gap, resulting in an emission blue shift (∼120 meV at 1.5 GPa). In contrast, as N ≤ 15, an efficient emission red shift is observed from band gap shrinkage (rate of 100 meV GPa-1), which is attributed to the predominant uniaxial interlayer compression because of the high strain resistance along the InSe-diamond interface. These findings advance the understanding of pressure-induced lattice deformation and optical transition evolution in InSe and could be applied to other 2D materials.

High-Sensitivity and Fast-Speed UV Photodetectors Based on Asymmetric Nanoporous-GaN/Graphene Vertical Junction.

GaN-based photodetectors are strongly desirable in many advanced fields, such as space communication, environmental monitoring, etc. However, the slow photo-response speed in currently reported high-sensitivity GaN-based photodetectors still hinders their applications. Here, we demonstrate a high-sensitivity and fast-speed UV photodetector based on asymmetric Au/nanoporous-GaN/graphene vertical junctions. The nanoporous GaN-based vertical photodetector shows an excellent rectification ratio up to ∼105 at +4 V/-4 V. The photo-responsivity and specific detectivity of the device is up to 1.01 × 104 A/W and 7.84 × 1014 Jones, respectively, more than three orders of magnitude higher than the control planar photodetector. With switching light on and off, the repeatable on/off current ratio of the nanoporous GaN-based vertical photodetector is ∼4.32 × 103, which is about 1.51 × 103 times to that of the control planar device. The measured rise/decay time is 12.2 µs/14.6 µs, which is the fastest value for the high-sensitivity GaN-based photodetectors to date. These results suggest that the asymmetric Au/nanoporous-GaN/graphene structure can improve the sensitivity and the photo-response speed of GaN-based PDs simultaneously.

Meta-Atom Coupling Induced Chiral Hotspot in Silicon Nitride Staggered Nanorods Meta-Surface.

Dielectric meta-surfaces have emerged as an effective way for fabricating chiral optical devices, and the chiral meta-surfaces are usually constituted by periodic chiral meta-atom structures. Here, we report a chiral meta-surface consisting of nonchiral silicon nitride rectangular nanorods. The chiral hotspots are generated between the staggered nanorods due to the coupling between the two nearest neighbor nanorod units. 14.6% macroscopic circular dichroism (CD) is achieved experimentally with larger area staggered nanorods. Meanwhile, we demonstrate that the wavelength tuning capability of this design from 696 to 820 nm by simply modulating the overlap length of nanorods. Our work highlights the mechanisms for CD hotspot generation without complex chiral units, which paves a novel way for future on-chip photon-spin selective devices.

Photonic sampled and quantized analog-to- digital converters on thin-film lithium niobate platform.

In this paper, an on-chip photonic sampled and quantized analog-to-digital converter (ADC) on thin-film lithium niobate platform is experimentally demonstrated. Using two phase modulators as a sampler and a 5×5 multimode interference (MMI) coupler as a quantizer, a 1 GHz sinusoidal analog input signal was successfully converted to a digitized output with a 20 GSample/s sampling rate. To evaluate the system performance, the quantization curves together with the transfer function of the ADC were measured. The experimental effective number of bits (ENOB) was 3.17. The demonstrated device is capable of operating at a high frequency over 67 GHz, making it a promising solution for on-chip ultra-high speed analog-to-digital conversion.

Low symmetric sub-wavelength array enhanced lensless polarization-sensitivity photodetector of germanium selenium.

Polarization-sensitive photodetectors, with the ability of identifying the texture-, stress-, and roughness-induced light polarization state variation, displace unique advantages in the fields of national security, medical diagnosis, and aerospace. The utilization of in-plane anisotropic two-dimensional (2D) materials has led the polarization photodetector into a polarizer-free regime, and facilitated the miniaturization of optoelectronic device integration. However, the insufficient polarization ratio (usually less than 10) restricts the detection resolution of polarized signals. Here, we designed a sub-wavelength array (SWA) structure of 2D germanium selenium (GeSe) to further improve its anisotropic sensitivity, which boosts the polarized photocurrent ratio from 1.6 to 18. This enhancement comes from the combination of nano-scale arrays with atomic-scale lattice arrangement at the low-symmetric direction, while the polarization-sensitive photoresponse along the high-symmetric direction is strongly suppressed due to the SWA-caused depolarization effect. Our mechanism study revealed that the SWA can improve the asymmetry of charge distribution, attenuate the matrix element in zigzag direction, and the localized surface plasma, which elevates the photo absorption and photoelectric transition probability along the armchair direction, therefore accounts for the enhanced polarization sensitivity. In addition, the photodetector based on GeSe SWA exhibited a broad power range of 40 dB at a near-infrared wavelength of 808 nm and the ability of weak-light detection under 0.1 LUX of white light (two orders of magnitude smaller than pristine 2D GeSe). This work provides a feasible guideline to improve the polarization sensitivity of 2D materials, and will greatly benefit the development of polarized imaging sensors.

General low-temperature growth of two-dimensional nanosheets from layered and nonlayered materials.

Most of the current methods for the synthesis of two-dimensional materials (2DMs) require temperatures not compatible with traditional back-end-of-line (BEOL) processes in semiconductor industry (450 °C). Here, we report a general BiOCl-assisted chemical vapor deposition (CVD) approach for the low-temperature synthesis of 27 ultrathin 2DMs. In particular, by mixing BiOCl with selected metal powders to produce volatile intermediates, we show that ultrathin 2DMs can be produced at 280-500 °C, which are ~200-300 °C lower than the temperatures required for salt-assisted CVD processes. In-depth characterizations and theoretical calculations reveal the low-temperature processes promoting 2D growth and the oxygen-inhibited synthetic mechanism ensuring the formation of ultrathin nonlayered 2DMs. We demonstrate that the resulting 2DMs exhibit electrical, magnetic and optoelectronic properties comparable to those of 2DMs grown at much higher temperatures. The general low-temperature preparation of ultrathin 2DMs defines a rich material platform for exploring exotic physics and facile BEOL integration in semiconductor industry.

Selectively Controlled Ferromagnets by Electric Fields in van der Waals Ferromagnetic Heterojunctions.

Charge transfer plays a key role at the interfaces of heterostructures, which can affect electronic structures and ultimately the physical properties of the materials. However, charge transfer is difficult to manipulate externally once the interface is formed. The recently discovered van der Waals ferromagnets with atomically sharp interfaces provided a perfect platform for the electrical control of interfacial charge transfer. Here, we report magnetoresistance experiments revealing electrically tunable charge transfer in Fe3GeTe2/Cr2Ge2Te6/Fe3GeTe2 all-magnetic van der Waals heterostructures, which can be exploited to selectively modify the switching fields of the top or bottom Fe3GeTe2 electrodes. The directional charge transfer from metallic Fe3GeTe2 to semiconducting Cr2Ge2Te6 is revealed by first-principles calculations, which remarkably modifies the magnetic anisotropy energy of Fe3GeTe2, leading to the dramatically suppressed coercivity. The electrically selective control of magnetism demonstrated in this study could stimulate the development of spintronic devices based on van der Waals magnets.

A Gate Programmable van der Waals Metal-Ferroelectric-Semiconductor Vertical Heterojunction Memory.

Ferroelectricity, one of the keys to realize non-volatile memories owing to the remanent electric polarization, is an emerging phenomenon in the 2D limit. Yet the demonstrations of van der Waals (vdW) memories using 2D ferroelectric materials as an ingredient are very limited. Especially, gate-tunable ferroelectric vdW memristive device, which holds promises in future multi-bit data storage applications, remains challenging. Here, a gate-programmable multi-state memory is shown by vertically assembling graphite, CuInP2 S6 , and MoS2 layers into a metal(M)-ferroelectric(FE)-semiconductor(S) architecture. The resulted devices seamlessly integrate the functionality of both FE-memristor (with ON-OFF ratios exceeding 105 and long-term retention) and metal-oxide-semiconductor field effect transistor (MOS-FET). Thus, it yields a prototype of gate tunable giant electroresistance with multi-levelled ON-states in the FE-memristor in the vertical vdW assembly. First-principles calculations further reveal that such behaviors originate from the specific band alignment between the FE-S interface. Our findings pave the way for the engineering of ferroelectricity-mediated memories in future implementations of 2D nanoelectronics.

Initializing film homogeneity to retard phase segregation for stable perovskite solar cells.

The mixtures of cations and anions used in hybrid halide perovskites for high-performance solar cells often undergo element and phase segregation, which limits device lifetime. We adapted Schelling's model of segregation to study individual cation migration and found that the initial film inhomogeneity accelerates materials degradation. We fabricated perovskite films (FA1-xCsxPbI3; where FA is formamidinium) through the addition of selenophene, which led to homogeneous cation distribution that retarded cation aggregation during materials processing and device operation. The resultant devices achieved enhanced efficiency and retained >91% of their initial efficiency after 3190 hours at the maximum power point under 1 sun illumination. We also observe prolonged operational lifetime in devices with initially homogeneous FACsPb(Br0.13I0.87)3 absorbers.