Spectrum-Dependent Image Convolutional Processing via a Two-Dimensional Polarization-Sensitive Photodetector.

Currently, the improvement in the processing capacity of traditional processors considerably lags behind the demands of real-time image processing caused by the advancement of photodetectors and the widespread deployment of high-definition image sensors. Therefore, achieving real-time image processing at the sensor level has become a prominent research domain in the field of photodetector technology. This goal underscores the need for photodetectors with enhanced multifunctional integration capabilities than can perform real-time computations using optical or electrical signals. In this study, we employ an innovative p-type semiconductor GaTe0.5Se0.5 to construct a polarization-sensitive wide-spectral photodetector. Leveraging the wide-spectral photoresponse, we realize three-band imaging within a wavelength range of 390-810 nm. Furthermore, real-time image convolutional processing is enabled by configuring appropriate convolution kernels based on the polarization-sensitive photocurrents. The innovative design of the polarization-sensitive wide-spectral GaTe0.5Se0.5-based photodetector represents a notable contribution to the domain of real-time image perception and processing.

Spatiotemporal-Dependent Confinement Effect of Bubble Swarms Enables a Fractal Hierarchical Assembly with Promoted Chirality.

The submarine-confined bubble swarm is considered an important constraining environment for the early evolution of living matter due to the abundant gas/water interfaces it provides. Similarly, the spatiotemporal characteristics of the confinement effect in this particular scenario may also impact the origin, transfer, and amplification of chirality in organisms. Here, we explore the confinement effect on the chiral hierarchical assembly of the amphiphiles in the confined bubble array stabilized by the micropillar templates. Compared with the other confinement conditions, the assembly in the bubble scenario yields a fractal morphology and exhibits a unique level of the chiral degree, ordering, and orientation consistency, which can be attributed to the characteristic interfacial effects of the rapidly formed gas/water interfaces. Thus, molecules with a balanced amphiphilicity can be more favorable for the promotion. Not limited to the pure enantiomers, chiral amplification of the enantiomer-mixed assembly is observed only in the bubble scenario. Beyond the interfacial mechanism, the fast formation kinetics of the confined liquid bridges in the bubble scenario endows the assembly with the tunable hierarchical morphology when regulating the amphiphilicity, aggregates, and confined spaces. Furthermore, the chiral-induced spin selectivity (CISS) effect of the fractal hierarchical assembly was systematically investigated, and a strategy based on photoisomerization was developed to efficiently modulate the CISS effect. This work provides insights into the robustness of confined bubble swarms in promoting a chiral hierarchical assembly and the potential applications of the resulting chiral hierarchical patterns in solid-state spintronic and optical devices.

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.

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.

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.

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.

Engineering Near-Infrared Light Emission in Mechanically Exfoliated InSe Platelets through Hydrostatic Pressure for Multicolor Microlasing.

γ-indium selenide (InSe) is a van der Waals semiconductor and holds great potentials for low-energy-consumption electronic and optoelectronic devices. Herein, we investigated the hydrostatic pressure engineered near-infrared (NIR) light emission of mechanically exfoliated γ-InSe crystals using the diamond anvil cell (DAC) technique. A record-wide spectral tuning range of 185 nm and a large linear pressure coefficient of 40 nm GPa-1 were achieved for spontaneous emissions, leading to ultrabroadband microlasing spectrally ranging from 1022 to 911 nm. This high emission tunability can be attributed to the compression of the soft intralayer In-Se bonds under high pressure, which suppressed the band gap shrinkage by increasing the interlayer interaction. Furthermore, two band gap crossovers of valence (direct-to-indirect) and conduction bands were resolved at approximately 4.0 and 7.0 GPa, respectively, resulting in pressure-sensitive emission lifetime and intensity. These findings pave the pathways for pressure-sensitive InSe-based NIR light sources, sensors and so on.

Van der Waals epitaxial growth of air-stable CrSe2 nanosheets with thickness-tunable magnetic order.

The discovery of intrinsic ferromagnetism in ultrathin two-dimensional van der Waals crystals opens up exciting prospects for exploring magnetism in the ultimate two-dimensional limit. Here, we show that environmentally stable CrSe2 nanosheets can be readily grown on a dangling-bond-free WSe2 substrate with systematically tunable thickness down to the monolayer limit. These CrSe2/WSe2 heterostructures display high-quality van der Waals interfaces with well-resolved moiré superlattices and ferromagnetic behaviour. We find no apparent change in surface roughness or magnetic properties after months of exposure in air. Our calculations suggest that charge transfer from the WSe2 substrate and interlayer coupling within CrSe2 play a critical role in the magnetic order in few-layer CrSe2 nanosheets. The highly controllable growth of environmentally stable CrSe2 nanosheets with tunable thickness defines a robust two-dimensional magnet for fundamental studies and potential applications in magnetoelectronic and spintronic devices.

Recombination Time Mismatch and Spin Dependent Photocurrent at a Ferromagnetic-Metal-Semiconductor Tunnel Junction.

We report on carrier dynamics in a spin photodiode based on a ferromagnetic-metal-GaAs tunnel junction. We show that the helicity-dependent current is determined not only by the electron spin polarization and spin asymmetry of the tunneling but in great part by a dynamical factor resulting from the competition between tunneling and recombination in the semiconductor, as well as by a specific quantity: the charge polarization of the photocurrent. The two latter factors can be efficiently controlled through an electrical bias. Under longitudinal magnetic field, we observe a strong increase of the signal arising from inverted Hanle effect, which is a fingerprint of its spin origin. Our approach represents a radical shift in the physical description of this family of emerging spin devices.

Birefringence and Dichroism in Quasi-1D Transition Metal Trichalcogenides: Direct Experimental Investigation.

Birefringence and dichroism are very important properties in optical anisotropy. Understanding the intrinsic birefringence and dichroism of a material can provide great help to utilize its optical anisotropy. But the direct experimental investigation of birefringence in nanoscale materials is rarely reported. As typical anisotropic transition metals trichalcogenides (TMTCs) materials with quasi-1D structure, TiS3 and ZrS3 have attracted extensive attention due to their special crystal structure and optical anisotropy characteristics. Here, the optical anisotropy properties such as birefringence and dichroism of two kinds of quasi-1D TMTCs, TiS3 and ZrS3 , are theoretically and experimentally studied. In experimental results, the anisotropic refraction and anisotropic reflection of TiS3 and ZrS3 are studied by polarization-resolved optical microscopy and azimuth-dependent reflectance difference microscopy, respectively. In addition, the birefringence and dichroism of ZrS3 nanoribbon in experiment are directly measured by spectrometric ellipsometry measurements, and a reasonable result is obtained. This work provides the basic optical anisotropy information of TiS3 and ZrS3 . It lays a foundation for the further study of the optical anisotropy of these two materials and provides a feasible method for the study of birefringence and dichroism of other nanomaterials in the future.

Extrinsic Photoconduction Induced Short-Wavelength Infrared Photodetectors Based on Ge-Based Chalcogenides.

2D layered photodetectors have been widely researched for intriguing optoelectronic properties but their application fields are limited by the bandgap. Extending the detection waveband can significantly enrich functionalities and applications of photodetectors. For example, after breaking through bandgap limitation, extrinsic Si photodetectors are used for short-wavelength infrared or even long-wavelength infrared detection. Utilizing extrinsic photoconduction to extend the detection waveband of 2D layered photodetectors is attractive and desirable. However, extrinsic photoconduction has yet not been observed in 2D layered materials. Here, extrinsic photoconduction-induced short-wavelength infrared photodetectors based on Ge-based chalcogenides are reported for the first time and the effectiveness of intrinsic point defects are demonstrated. The detection waveband of room-temperature extrinsic GeSe photodetectors with the assistance of Ge vacancies is broadened to 1.6 µm. Extrinsic GeSe photodetectors have an excellent external quantum efficiency (0.5%) at the communication band of 1.31 µm and polarization-resolved capability to subwaveband radiation. Moreover, room-temperature extrinsic GeS photodetectors with a detection waveband to the communication band of 1.55 µm further verify the versatility of intrinsic point defects. This approach provides design strategies to enrich the functionalities of 2D layered photodetectors.

Strain-engineering on GeSe: Raman spectroscopy study.

Among the IV-VI compounds, GeSe has wide applications in nanoelectronics due to its unique photoelectric properties and adjustable band gap. Even though modulation of its physical characteristics, including the band gap, by an external field will be useful for designing novel devices, experimental work is still rare. Here, we report a detailed anisotropic Raman response of GeSe flakes under uniaxial tension strain. Based on theoretical analysis, the anisotropy of the phonon response is attributed to a change in anisotropic bond length and bond angle under in-plane uniaxial strain. An enhancement in anisotropy and band gap is found due to strain along the ZZ or AC directions. This study shows that strain-engineering is an effective method for controlling the GeSe lattice, and paves the way for modulating the anisotropic electric and optical properties of GeSe.

Symmetry-Reduction Enhanced Polarization-Sensitive Photodetection in Core-Shell SbI3 /Sb2 O3 van der Waals Heterostructure.

Structural symmetry is a simple way to quantify the anisotropic properties of materials toward unique device applications including anisotropic transportation and polarization-sensitive photodetection. The enhancement of anisotropy can be achieved by artificial symmetry-reduction design. A core-shell SbI3 /Sb2 O3 nanowire, a heterostructure bonded by van der Waals forces, is introduced as an example of enhancing the performance of polarization-sensitive photodetectors via symmetry reduction. The structural, vibrational, and optical anisotropies of such core-shell nanostructures are systematically investigated. It is found that the anisotropic absorbance of a core-shell nanowire is obviously higher than that of two single compounds from both theoretical and experimental investigations. Anisotropic photocurrents of the polarization-sensitive photodetectors based on these core-shell SbI3 /Sb2 O3 van der Waals nanowires are measured ranging from ultraviolet (UV) to visible light (360-532 nm). Compared with other van der Waals 1D materials, low anisotropy ratio (Imax /Imin ) is measured based on SbI3 but a device based on this core-shell nanowire possesses a relatively high anisotropy ratio of ≈3.14 under 450 nm polarized light. This work shows that the low-symmetrical core-shell van der Waals heterostructure has large potential to be applied in wide range polarization-sensitive photodetectors.

Temperature dependence of charge transport in solid-state molecular junctions based on oligo(phenylene ethynylene)s.

The ultimate goal of molecular electronics is to achieve practical applications. For approaching the target, we have successfully fabricated solid-state junctions based on oligo(phenylene ethynylene)s (OPEs) and cruciform OPEs with extended tetrathiafulvalene (TTF) (OPE3 and OPE3-TTF) self-assembled monolayers (SAMs) with a diamine anchoring group. SAMs were confined in micropores with gold substrates to ensure well-defined device surface areas. The transport properties were conducted on a double-junction layout, which the rGO films used for top contacts and interconnects between adjacent SAMs. The solid-state devices based on OPE3-TTF SAMs showed the expected higher conductance under ambient conditions because of the incorporation of a TTF moiety. The two devices displayed varying degrees of temperature dependence with decreasing temperature, which resulted from the cross-conjugated OPE3-TTF molecule exhibiting quantum interference while the linear-conjugated OPE3 molecule did not. This study shows the temperature dependence of the electrical properties of molecular devices based on cruciform OPEs, further enriching the research results of functional molecular devices.

Growth of two-dimensional materials on hexagonal boron nitride (h-BN).

With its atomically smooth surface yet no dangling bond, chemical inertness and high temperature sustainability, the insulating hexagonal boron nitride (h-BN) can be an ideal substrate for two-dimensional (2D) material growth and device measurement. In this review, research progress on the chemical growth of 2D materials on h-BN has been summarized, such as chemical vapor deposition and molecular beam epitaxy of graphene and various transition metal dichalcogenides. Further, stacking of the as-grown 2D materials relative to h-BN, thermal expansion matching between the deposited materials and h-BN, electrical property of 2D materials on h-BN have been discussed in detail.

Type-I Transition Metal Dichalcogenides Lateral Homojunctions: Layer Thickness and External Electric Field Effects.

Transition metal dichalcogenide (TMD) heterostructures have been widely explored due to the formation of type-II band alignment and interlayer exciton. However, the studies of type-I TMD heterostructures are still lacking, which limit their applications in luminescence devices. Here, the 1L/nL MX2 (n = 2, 3, 4; M = Mo, W; X = S, Se) lateral homojunction based on the layer-dependent band gaps of TMD nanosheets is theoretically simulated. The studies show that the TMD homojunction presents with high thermal stability and type-I band alignment. The band offset and quantum confinement of carriers can be easily tuned by controlling the thickness of the multilayer region. Moreover, the electric field can decrease the band gaps of 1L/3L and 1L/4L homojunctions linearly. Interestingly, for the 1L/2L MX2 homojunction, the gap value is robust to the weak electric field, while it drops sharply under a strong electric field. This study sheds light on the physical pictures in the TMD lateral homojunction, and provides a practicable and general approach to engineer a type-I homojunction based 2D semiconductor materials.

Highly polarization sensitive photodetectors based on quasi-1D titanium trisulfide (TiS3).

Photodetectors with high polarization sensitivity are in great demand in advanced optical communication. Here, we demonstrate that photodetectors based on titanium trisulfide (TiS3) are extremely sensitive to polarized light (from visible to the infrared), due to its reduced in-plane structural symmetry. By density functional theory calculation, TiS3 has a direct bandgap of 1.13 eV. The highest photoresponsivity reaches 2500 A W-1. What is more, in-plane optical selection caused by strong anisotropy leads to the photoresponsivity ratio for different directions of polarization that can reach 4:1. The angle-dependent photocurrents of TiS3 clearly display strong linear dichroism. Moreover, the Raman peak at 370 cm-1 is also very sensitive to the polarization direction. The theoretical optical absorption of TiS3 is calculated by using the HSE06 hybrid functional method, in qualitative agreement with the observed experimental photoresponsivity.

Dry Chemistry of Ferrate(VI): A Solvent-Free Mechanochemical Way for Versatile Green Oxidation.

The +6 oxidation state of iron generally exists in the form of ferrate(VI) with high redox potential and environmentally friendly nature. Although ferrate(VI) has been known for over a century, its chemistry is still limited to the solvent-based reactions that suffers from the insolubility/instability of this oxidant and the environmental issues caused by hazardous solvents. Herein, we explore the solvent-free reactivity of ferrate(VI) under mechanical milling, revealing that its strong oxidizing power is accessible in the "dry" solid state towards a broad variety of substrates, for example, aromatic alcohols/aldehydes and carbon nanotubes. More significantly, solvent-free mechanochemistry also reshapes the oxidizing ability of ferrate(VI) due to the underlying solvent-free effect and the promotive mechanical actions. This study opens up a new chemistry of ferrate(VI) with promising application in green oxidative transformation of both organic and inorganic substrates.

Short-Wave Near-Infrared Linear Dichroism of Two-Dimensional Germanium Selenide.

Polarized detection has been brought into operation for optics applications in the visible band. Meanwhile, an advanced requirement in short-wave near-infrared (SW-NIR) (700-1100 nm) is proposed. Typical IV-VI chalcogenides-2D GeSe with anisotropic layered orthorhombic structure and narrow 1.1-1.2 eV band gap-potentially meets the demand. Here we report the unusual angle dependences of Raman spectra on high-quality GeSe crystals. The polarization-resolved absorption spectra (400-950 nm) and polarization-sensitive photodetectors (532, 638, and 808 nm) both exhibited well-reproducible cycles, distinct anisotropic features, and typical absorption ratios αy/αx ≈ 1.09 at 532 nm, 1.26 at 638 nm, and 3.02 at 808 nm (the dichroic ratio Ipy/Ipx ≈ 1.09 at 532 nm, 1.44 at 638 nm, 2.16 at 808 nm). Obviously, the polarized measurement for GeSe showed superior anisotropic response at around 808 nm within the SW-NIR band. Besides, the two testing methods have demonstrated the superior reliability for each other. For the layer dependence of linear dichroism, the GeSe samples with different thicknesses measured under both 638 and 808 nm lasers identify that the best results can be achieved at a moderate thickness about 8-16 nm. Overall, few-layer GeSe has capacity with the integrated SW-NIR optical applications for polarization detection.

Band engineering of the MoS2/stanene heterostructure: strain and electrostatic gating.

In a fast developing field, it has been found that van der Waals heterostructures can overcome the weakness of single two-dimensional layered materials and extend their electronic and optoelectronic applications. Through first-principles methods, the studied MoS2/stanene heterostructure preserves high-speed carrier characteristics and opens the direct band gap. Simultaneously, the band alignment shows that the electrons transfer from stanene to MoS2, which forms an internal electric field. As an effective strategy, the out-of-plane strain remarkably changes the band gaps of the heterostructure and enhances its carrier concentration. In addition, the combined effects of the internal and external electric fields can further open the band gaps and induce a direct-to-indirect gap transition in the heterostructure. More interestingly, when the external electric field is equal to the reverse internal one, the heterostructure regains a Dirac cone. Our results show that the MoS2/stanene heterostructure has potential applications in high-speed optoelectronic devices.