Efficient Carrier Multiplication in Self-Powered Near-Ultraviolet γ-InSe/Graphene Heterostructure Photodetector with External Quantum Efficiency Exceeding 161.

Carrier multiplication (CM) in semiconductors, the process of absorbing a single high-energy photon to form two or more electron-hole pairs, offers great potential for the high-response detection of high-energy photons in the ultraviolet spectrum. However, compared to two-dimensional semiconductors, conventional bulk semiconductors not only face integration and flexibility bottlenecks but also exhibit inferior CM performance. To attain efficient CM for ultraviolet detection, we designed a two-terminal photodetector featuring a unilateral Schottky junction based on a two-dimensional γ-InSe/graphene heterostructure. Benefiting from a strong built-in electric field, the photogenerated high-energy electrons in γ-InSe, an ideal ultraviolet light-absorbing layer, can efficiently transfer to graphene without cooling. It results in efficient CM within the graphene, yielding an ultrahigh responsivity of 468 mA/W and a record-high external quantum efficiency of 161.2% when it is exposed to 360 nm light at zero bias. This work provides valuable insights into developing next-generation ultraviolet photodetectors with high performance and low-power consumption.

Giant Tunability of Intersubband Transitions and Quantum Hall Quartets in Few-Layer InSe Quantum Wells.

A two-dimensional (2D) quantum electron system is characterized by quantized energy levels, or subbands, in the out-of-plane direction. Populating higher subbands and controlling the intersubband transitions have wide technological applications such as optical modulators and quantum cascade lasers. In conventional materials, however, the tunability of intersubband spacing is limited. Here we demonstrate electrostatic population and characterization of the second subband in few-layer InSe quantum wells, with giant tunability of its energy, population, and spin-orbit coupling strength, via the control of not only layer thickness but also the out-of-plane displacement field. A modulation of as much as 350% or over 250 meV is achievable, underscoring the promise of InSe for tunable infrared and THz sources, detectors, and modulators.

Synergy Between Surface Confinement and Heterointerfacial Regulations with Fast Electron/Ion Migration in InSe-PPy for Sodium-Ion Storage.

Layered indium selenide (InSe) is a new 2D semiconductor material with high carrier mobility, widely adjustable bandgap, and high ductility. However, its ion storage behavior and related electrochemical reaction mechanism are rarely reported. In this study, InSe nanoflakes encapsulated in conductive polypyrrole (InSe@PPy) are designed in consideration of restraining the severe volume change in the electrochemical reaction and increasing conductivity via in situ chemical oxidation polymerization. Density functional theory calculations demonstrate that the construction of heterostructure can generate an internal electric field to accelerate electron transfer via additional driving forces, offering synergistically enhanced structural stability, electrical conductivity, and Na+ diffusion process. The resulting InSe@PPy composite shows outstanding electrochemical performance in the sodium ion batteries system, achieving a high reversible capacity of 336.4 mA h g-1 after 500 cycles at 1 A g-1 and a long-term cyclic stability with capacity of 274.4 mA h g-1 after 2800 cycles at 5 A g-1 . In particular, the investigation of capacity fluctuation within the first cycling reveals the alternating significance of intercalation and conversion reactions and evanescent alloying reaction. The combined reaction mechanism of insertion, conversion, and alloying of InSe@PPy is revealed by in situ X-ray diffraction, ex situ electrochemical impedance spectroscopy, and transmission electron microscopy.

Giant Out-of-Plane Exciton Emission Enhancement in Two-Dimensional Indium Selenide via a Plasmonic Nanocavity.

Out-of-plane (OP) exciton-based emitters in two-dimensional semiconductor materials are attractive candidates for novel photonic applications, such as radially polarized sources, integrated photonic chips, and quantum communications. However, their low quantum efficiency resulting from forbidden transitions limits their practicality. In this work, we achieve a giant enhancement of up to 34000 for OP exciton emission in indium selenide (InSe) via a designed Ag nanocube-over-Au film plasmonic nanocavity. The large photoluminescence enhancement factor (PLEF) is attributed to the induced OP local electric field (Ez) within the nanocavity, which facilitates effective OP exciton-plasmon interaction and subsequent tremendous enhancement. Moreover, the nanoantenna effect resulting from the effective interaction improves the directivity of spontaneous radiation. Our results not only reveal an effective photoluminescence enhancement approach for OP excitons but also present an avenue for designing on-chip photonic devices with an OP dipole orientation.

Photoelectric performance of InSe vdW semi-floating gate p-n junction transistor.

Semi-floating gate transistors based on vdW materials are often used in memory and programmable logic applications. In this paper, we propose a semi-floating gate photoelectric p-n junction transistor structure which is stacked by InSe/h-BN/Gr. By modulating gate voltage, InSe can be presented as N-type and P-type respectively on different substrates, and then combined into p-n junction. Moreover, InSe/h-BN/Gr device can be switched freely between N-type resistance and p-n junction. The resistance value of InSe resistor and the photoelectric properties of the p-n junction are also sensitively modulated by laser. Under dark conditions, the rectification ratio of p-n junction can be as high as 107. After laser modulation, the device has a response up to 1.154 × 104A W-1, a detection rate up to 5.238 × 1012Jones, an external quantum efficiency of 5.435 × 106%, and a noise equivalent power as low as 1.262 × 10-16W/Hz1/2. It lays a foundation for the development of high sensitivity and fast response rate tunable photoelectric p-n junction transistor.

Phase Modulation of Self-Gating in Ionic Liquid-Functionalized InSe Field-Effect Transistors.

Understanding the Coulomb interactions between two-dimensional (2D) materials and adjacent ions/impurities is essential to realizing 2D material-based hybrid devices. Electrostatic gating via ionic liquids (ILs) has been employed to study the properties of 2D materials. However, the intrinsic interactions between 2D materials and ILs are rarely addressed. This work studies the intersystem Coulomb interactions in IL-functionalized InSe field-effect transistors by displacement current measurements. We uncover a strong self-gating effect that yields a 50-fold enhancement in interfacial capacitance, reaching 550 nF/cm2 in the maximum. Moreover, we reveal the IL-phase-dependent transport characteristics, including the channel current, carrier mobility, and density, substantiating the self-gating at the InSe/IL interface. The dominance of self-gating in the rubber phase is attributed to the correlation between the intra- and intersystem Coulomb interactions, further confirmed by Raman spectroscopy. This study provides insights into the capacitive coupling at the InSe/IL interface, paving the way to developing liquid/2D material hybrid devices.

Electronic Transport Properties in GaAs/AlGaAs and InSe/InP Finite Superlattices under the Effect of a Non-Resonant Intense Laser Field and Considering Geometric Modifications.

In this work, a finite periodic superlattice is studied, analyzing the probability of electronic transmission for two types of semiconductor heterostructures, GaAs/AlGaAs and InSe/InP. The changes in the maxima of the quasistationary states for both materials are discussed, making variations in the number of periods of the superlattice and its shape by means of geometric parameters. The effect of a non-resonant intense laser field has been included in the system to analyze the changes in the electronic transport properties by means of the Landauer formalism. It is found that the highest tunneling current is given for the GaAs-based compared to the InSe-based system and that the intense laser field improves the current-voltage characteristics generating higher current peaks, maintaining a negative differential resistance (NDR) effect, both with and without laser field for both materials and this fact allows to tune the magnitude of the current peak with the external field and therefore extend the range of operation for multiple applications. Finally, the power of the system is discussed for different bias voltages as a function of the chemical potential.

Out-of-plane and in-plane ferroelectricity of atom-thick two-dimensional InSe.

Two-dimensional (2D) ferroelectric materials are promising substitutes of three-dimensional perovskite based ferroelectric ceramic materials. Yet most studies have been focused on the construction of non-centrosymmetric 2D van der Waals materials and only a few are constructed experimentally. Herein, we experimentally demonstrate the co-existence of voltage-tunable out-of-plane (OOP) and in-plane (IP) ferroelectricity in few-layer InSe prepared by a solution-processable method and fabricate ferroelectric semiconductor channel transistors. The reversible polarization can initiate instant switch of resistance with high ON/OFF ratios and a comparable subthreshold swing of 160 mV/dec under gate modulation. The origins of such unique OOP and IP ferroelectricity of the centrosymmetric structure are theoretically analyzed.

Ferroelectric-Gated InSe Photodetectors with High On/Off Ratios and Photoresponsivity.

Indium selenide (InSe) has a high electron mobility and tunable direct band gap, enabling its potential applications to electronic and optoelectronic devices. Here, we report the fabrication of InSe photodetectors with high on/off ratios and ultrahigh photoresponsivity, using ferroelectric poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) copolymer films as the top-gate dielectric. Benefiting from the successful suppression of the dark current down to ∼10-14A in the InSe channel by tuning the three different polarization states in ferroelectric P(VDF-TrFE) and improved interface properties using h-BN as a substrate, the ferroelectric-gated InSe photodetectors show a high on/off ratio of over 108, a high photoresponsivity up to 14 250 AW-1, a high detectivity up to 1.63 × 1013 Jones, and a fast response time of 600 µs even at zero-gate voltage. The present results highlight the role of ferroelectric P(VDF-TrFE) in tuning the carrier transport of InSe and may provide an avenue for the development of InSe-based photodetectors.

How Universal Is the Wetting Aging in 2D Materials.

Previous studies indicate that 2D materials such as graphene, WS2, and MoS2 deposited on oxidized silicon substrate are susceptible to aging due to the adsorption of airborne contamination. As a result, their surfaces become more hydrophobic. However, it is not clear how ubiquitous such a hydrophobization is, and the interplay between the specific adsorbed species and resultant wetting aging remains elusive. Here, we report a pronounced and general hydrophilic-to-hydrophobic wetting aging on 2D InSe films, which is independent of the substrates to synthesize these films (silicon, glass, nickel, copper, aluminum oxide), though the extent of wetting aging is sensitive to the layer of films. Our findings are ascribed to the occurrence and enrichment of airborne contamination that contains alkyl chains. Our results also suggest that the wetting aging effect might be universal to a wide range of 2D materials.

Probing Effective Out-of-Plane Piezoelectricity in van der Waals Layered Materials Induced by Flexoelectricity.

Many van der Waals layered 2D materials, such as h-BN, transition metal dichalcogenides (TMDs), and group-III monochalcogenides, have been predicted to possess piezoelectric and mechanically flexible natures, which greatly motivates potential applications in piezotronic devices and nanogenerators. However, only intrinsic in-plane piezoelectricity exists in these 2D materials and the piezoelectric effect is confined in odd-layers of TMDs. The present work is intent on combining the free-standing design and piezoresponse force microscopy techniques to obtain and directly quantify the effective out-of-plane electromechanical coupling induced by strain gradient on atomically thin MoS2 and InSe flakes. Conspicuous piezoresponse and the measured piezoelectric coefficient with respect to the number of layers or thickness are systematically illustrated for both MoS2 and InSe flakes. Note that the promising effective piezoelectric coefficient (deff 33 ) of about 21.9 pm V-1 is observed on few-layered InSe. The out-of-plane piezoresponse arises from the net dipole moment along the normal direction of the curvature membrane induced by strain gradient. This work not only provides a feasible and flexible method to acquire and quantify the out-of-plane electromechanical coupling on van der Waals layered materials, but also paves the way to understand and tune the flexoelectric effect of 2D systems.

Experimental Identification of Critical Condition for Drastically Enhancing Thermoelectric Power Factor of Two-Dimensional Layered Materials.

Nanostructuring is an extremely promising path to high-performance thermoelectrics. Favorable improvements in thermal conductivity are attainable in many material systems, and theoretical work points to large improvements in electronic properties. However, realization of the electronic benefits in practical materials has been elusive experimentally. A key challenge is that experimental identification of the quantum confinement length, below which the thermoelectric power factor is significantly enhanced, remains elusive due to lack of simultaneous control of size and carrier density. Here we investigate gate-tunable and temperature-dependent thermoelectric transport in γ-phase indium selenide (γ-InSe, n-type semiconductor) samples with thickness varying from 7 to 29 nm. This allows us to properly map out dimension and doping space. Combining theoretical and experimental studies, we reveal that the sharper pre-edge of the conduction-band density of states arising from quantum confinement gives rise to an enhancement of the Seebeck coefficient and the power factor in the thinner InSe samples. Most importantly, we experimentally identify the role of the competition between quantum confinement length and thermal de Broglie wavelength in the enhancement of power factor. Our results provide an important and general experimental guideline for optimizing the power factor and improving the thermoelectric performance of two-dimensional layered semiconductors.

An Atomically Layered InSe Avalanche Photodetector.

Atomically thin photodetectors based on 2D materials have attracted great interest due to their potential as highly energy-efficient integrated devices. However, photoinduced carrier generation in these media is relatively poor due to low optical absorption, limiting device performance. Current methods for overcoming this problem, such as reducing contact resistances or back gating, tend to increase dark current and suffer slow response times. Here, we realize the avalanche effect in a 2D material-based photodetector and show that avalanche multiplication can greatly enhance the device response of an ultrathin InSe-based photodetector. This is achieved by exploiting the large Schottky barrier formed between InSe and Al electrodes, enabling the application of a large bias voltage. Plasmonic enhancement of the photosensitivity, achieved by patterning arrays of Al nanodisks onto the InSe layer, further improves device efficiency. With an external quantum efficiency approaching 866%, a dark current in the picoamp range, and a fast response time of 87 µs, this atomic layer device exhibits multiple significant advances in overall performance for this class of devices.

Intrinsic Electron Mobility Exceeding 10³ cm²/(V s) in Multilayer InSe FETs.

Graphene-like two-dimensional (2D) materials not only are interesting for their exotic electronic structure and fundamental electronic transport or optical properties but also hold promises for device miniaturization down to atomic thickness. As one material belonging to this category, InSe, a III-VI semiconductor, not only is a promising candidate for optoelectronic devices but also has potential for ultrathin field effect transistor (FET) with high mobility transport. In this work, various substrates such as PMMA, bare silicon oxide, passivated silicon oxide, and silicon nitride were used to fabricate multilayer InSe FET devices. Through back gating and Hall measurement in four-probe configuration, the device's field effect mobility and intrinsic Hall mobility were extracted at various temperatures to study the material's intrinsic transport behavior and the effect of dielectric substrate. The sample's field effect and Hall mobilities over the range of 20-300 K fall in the range of 0.1-2.0 × 10(3) cm(2)/(V s), which are comparable or better than the state of the art FETs made of widely studied 2D transition metal dichalcogenides.

Optoelectronic memory using two-dimensional materials.

An atomically thin optoelectronic memory array for image sensing is demonstrated with layered CuIn7Se11 and extended to InSe and MoS2 atomic layers. Photogenerated charge carriers are trapped and subsequently retrieved from the potential well formed by gating a 2D material with Schottky barriers. The atomically thin layered optoelectronic memory can accumulate photon-generated charges during light exposure, and the charges can be read out later for data processing and permanent storage. An array of atomically thin image memory pixels was built to illustrate the potential of fabricating large-scale 2D material-based image sensors for image capture and storage.

Electric-field-controlled electronic structures and quantum transport in monolayer InSe nanoribbons.

Electronic structures and quantum transport properties of the monolayer InSe nanoribbons are studied by adopting the tight-binding model in combination with the lattice Green function method. Besides the normal bulk and edge electronic states, a unique electronic state dubbed as edge-surface is found in the InSe nanoribbon with zigzag edge type. In contrast to the zigzag InSe nanoribbon, a singular electronic state termed as bulk-surface is observed along with the normal bulk and edge electronic states in the armchair InSe nanoribbons. Moreover, the band gap, the transversal electron probability distributions in the two sublayers, and the electronic state of the topmost valence subband can be manipulated by adding a perpendicular electric field to the InSe nanoribbon. Further study shows that the charge conductance of the two-terminal monolayer InSe nanoribbons can be switched on or off by varying the electric field strength. In addition, the transport of the bulk electronic state is delicate to even a weak disorder strength, however, that of the edge and edge-surface electronic states shows a strong robustness against to the disorders. These findings may be helpful to understand the electronic characteristics of the InSe nanostructures and broaden their potential applications in two-dimensional nanoelectronic devices as well.

Carrier and phonon transport in 2D InSe and its Janus structures.

Recently, two-dimensional (2D) Indium Selenide (InSe) has been receiving much attention in the scientific community due to its reduced size, extraordinary physical properties, and potential applications in various fields. In this review, we discussed the recent research advancement in the carrier and phonon transport properties of 2D InSe and its related Janus structures. We first introduced the progress in the synthesis of 2D InSe. We summarized the recent experimental and theoretical works on the carrier mobility, thermal conductivity, and thermoelectric characteristics of 2D InSe. Based on the Boltzmann transport equation (BTE), the mechanisms underlying carrier or phonon scattering of 2D InSe were discussed in detail. Moreover, the structural and transport properties of Janus structures based on InSe were also presented, with an emphasis on the theoretical simulations. At last, we discussed the prospects for continued research of 2D InSe.

Uniaxial Strain Dependence on Angle-Resolved Optical Second Harmonic Generation from a Few Layers of Indium Selenide.

Indium selenide (InSe) is an emerging van der Waals material, which exhibits the potential to serve in excellent electronic and optoelectronic devices. One of the advantages of layered materials is their application to flexible devices. How strain alters the electronic and optical properties is, thus, an important issue. In this work, we experimentally measured the strain dependence on the angle-resolved second harmonic generation (SHG) pattern of a few layers of InSe. We used the exfoliation method to fabricate InSe flakes and measured the SHG images of the flakes with different azimuthal angles. We found the SHG intensity of InSe decreased, while the compressive strain increased. Through first-principles electronic structure calculations, we investigated the strain dependence on SHG susceptibilities and the corresponding angle-resolved SHG pattern. The experimental data could be fitted well by the calculated results using only a fitting parameter. The demonstrated method based on first-principles in this work can be used to quantitatively model the strain-induced angle-resolved SHG patterns in 2D materials. Our obtained results are very useful for the exploration of the physical properties of flexible devices based on 2D materials.

Highly Stable InSe-FET Biosensor for Ultra-Sensitive Detection of Breast Cancer Biomarker CA125.

Two-dimensional materials-based field-effect transistors (FETs) are promising biosensors because of their outstanding electrical properties, tunable band gap, high specific surface area, label-free detection, and potential miniaturization for portable diagnostic products. However, it is crucial for FET biosensors to have a high electrical performance and stability degradation in liquid environments for their practical application. Here, a high-performance InSe-FET biosensor is developed and demonstrated for the detection of the CA125 biomarker in clinical samples. The InSe-FET is integrated with a homemade microfluidic channel, exhibiting good electrical stability during the liquid channel process because of the passivation effect on the InSe channel. The InSe-FET biosensor is capable of the quantitative detection of the CA125 biomarker in breast cancer in the range of 0.01-1000 U/mL, with a detection time of 20 min. This work provides a universal detection tool for protein biomarker sensing. The detection results of the clinical samples demonstrate its promising application in early screenings of major diseases.

Tunable electronic and optical properties of MoTe2/InSe heterostructure via external electric field and strain engineering.

Based on first-principles calculation under density functional theory, the geometry, electronic and optical properties of the MoTe2/InSe heterojunction have been investigated. The results reveal that the MoTe2/InSe heterojunction has a typical type-Ⅱ band alignment and exhibits an indirect bandgap of 0.99 eV. In addition, the Z-scheme electron transport mechanism is capable of efficiently separating photogenerated carriers. The bandgap of the heterostructure changes regularly under applied electric field and exhibits a significant Giant Stark effect. Under an applied electric field of 0.5 V Å-1, the band alignment of the heterojunction shifts from type-Ⅱ to type-I. The application of strain produced comparable changes in the heterojunction. More importantly, the transition from semiconductor to metal is completed in the heterostructure under the applied electric field and strain. Furthermore, the MoTe2/InSe heterojunction retains the optical properties of two monolayers and produces greater light absorption on this basis, especially for UV light. The above results offer a theoretical basis for the application of MoTe2/InSe heterostructure in the next generation of photodetectors.