Silicon-Nanomembrane-Based Broadband Synaptic Phototransistors for Neuromorphic Vision.

Neuromorphic vision has been attracting much attention due to its advantages over conventional machine vision (e.g., lower data redundancy and lower power consumption). Here we develop synaptic phototransistors based on the silicon nanomembrane (Si NM), which are coupled with lead sulfide quantum dots (PbS QDs) and poly(3-hexylthiophene) (P3HT) to form a heterostructure with distinct photogating. Synaptic phototransistors with optical stimulation have outstanding synaptic functionalities ranging from ultraviolet (UV) to near-infrared (NIR). The broadband synaptic functionalities enable an array of synaptic phototransistors to achieve the perception of brightness and color. In addition, an array of synaptic phototransistors is capable of simultaneous sensing, processing, and memory, which well mimics human vision.

Molecular beam epitaxy growth and scanning tunneling microscopy study of 2D layered materials on epitaxial graphene/silicon carbide.

Since the advent of atomically flat graphene, two-dimensional (2D) layered materials have gained extensive interest due to their unique properties. The 2D layered materials prepared on epitaxial graphene/silicon carbide (EG/SiC) surface by molecular beam epitaxy (MBE) have high quality, which can be directly applied without further transfer to other substrates. Scanning tunneling microscopy and spectroscopy (STM/STS) with high spatial resolution and high-energy resolution are often used to study the morphologies and electronic structures of 2D layered materials. In this review, recent progress in the preparation of various 2D layered materials that are either monoelemental or transition metal dichalcogenides on EG/SiC surface by MBE and their STM/STS investigations are introduced.

Recent Progress on the Scanning Tunneling Microscopy and Spectroscopy Study of Semiconductor Heterojunctions.

The band alignment, interface states, interface coupling, and carrier transport of semiconductor heterojunctions (SHs) need to be well understood for the design and fabrication of various important semiconductor structures and devices. Scanning tunneling microscopy (STM) with high spatial resolution and scanning tunneling spectroscopy (STS) with high energy resolution are significantly contributing to the understanding on the important properties of SHs. In this work, the recent progress on the use of STM and STS to study lateral, vertical and bulk SHs is reviewed. The spatial structures of SHs with atomically flat surface have been examined with STM. The electronic band structures (e. g., the band offset, interface state, and space charge region) of SHs are measured with STS. Combined with the spatial structures and the tunneling spectra features, the mechanism for the carrier transport in the SH may be proposed.

Low-temperature processed tantalum/niobium co-doped TiO2electron transport layer for high-performance planar perovskite solar cells.

A low-temperature preparation process is significantly important for scalable and flexible devices. However, the serious interface defects between the normally used titanium dioxide (TiO2) electron transport layer (ETL) obtained via a low-temperature method and perovskite suppress the further improvement of perovskite solar cells (PSCs). Here, we develop a facile low-temperature chemical bath method to prepare a TiO2ETL with tantalum (Ta) and niobium (Nb) co-doping. Systematic investigations indicate that Ta/Nb co-doping could increase the conduction band level of TiO2and could decrease the trap-state density, boosting electron injection efficiency and reducing the charge recombination between the perovskite/ETL interface. A superior power conversion efficiency of 19.44% can be achieved by a planar PSC with a Ta/Nb co-doped TiO2ETL, which is much higher than that of pristine TiO2(17.60%). Our achievements in this work provide new insights on low-temperature fabrication of low-cost and highly efficient PSCs.

Optically Stimulated Synaptic Devices Based on the Hybrid Structure of Silicon Nanomembrane and Perovskite.

Optoelectronic synaptic devices have been attracting increasing attention due to their critical role in the development of neuromorphic computing based on optoelectronic integration. Here we start with silicon nanomembrane (Si NM) to fabricate optoelectronic synaptic devices. Organolead halide perovskite (MAPbI3) is exploited to form a hybrid structure with Si NM. We demonstrate that synaptic transistors based on the hybrid structure are very sensitive to optical stimulation with low energy consumption. Synaptic functionalities such as excitatory post-synaptic current (EPSC), paired-pulse facilitation, and transition from short-term memory to long-term memory (LTM) are all successfully mimicked by using these optically stimulated synaptic transistors. The backgate-enabled tunability of the EPSC of these devices further leads to the LTM-based mimicking of visual learning and memory processes under different mood states. This work contributes to the development of Si-based optoelectronic synaptic devices for neuromorphic computing.

Cera alba-assisted ultraclean graphene transfer for high-performance PbI2 UV photodetectors.

Large polymer residues introduced by the graphene transfer process is still a major obstacle limiting the integration of chemical vapor deposition (CVD)-grown graphene into next-generation electronic and photoelectronic devices. Here we use cera alba, a natural and environmental-friendly material that derives from honeycomb, as the supporting layer for ultraclean graphene transfer. The transferred graphene has a low surface roughness with a surface height fluctuation within 5 nm and an only 80.08% average sheet resistance of the polymethyl methacrylate (PMMA)-transferred graphene. Further, the ultraclean graphene is used as electrodes for the PbI2-based UV photodetector and enables a 135% improvement on responsivity. The cera alba assisted transfer method reported here could achieve clean and damage-free graphene transfer, promoting the application of CVD-grown two-dimensional (2D) materials in large-area thin-film electronic and optoelectronic devices.

A review of theoretical study of graphene chemical vapor deposition synthesis on metals: nucleation, growth, and the role of hydrogen and oxygen.

Graphene has attracted intense research interest due to its extraordinary properties and great application potential. Various methods have been proposed for the synthesis of graphene, among which chemical vapor deposition has drawn a great deal of attention for synthesizing large-area and high-quality graphene. Theoretical understanding of the synthesis mechanism is crucial for optimizing the experimental design for desired graphene production. In this review, we discuss the three fundamental steps of graphene synthesis in details, i.e. (1) decomposition of carbon feedstocks and formation of various active carbon species, (2) nucleation, and (3) attachment and extension. We provide a complete scenario of graphene synthesis on metal surfaces at atomistic level by means of density functional theory, molecular dynamics (MD), Monte Carlo (MC) and their combination and interface with other simulation methods such as quantum mechanical molecular dynamics, density functional tight binding molecular dynamics, and combination of MD and MC. We also address the latest investigation of the influences of the hydrogen and oxygen on the synthesis and the quality of the synthesized graphene.

Perovskite/Organic Bulk-Heterojunction Integrated Ultrasensitive Broadband Photodetectors with High Near-Infrared External Quantum Efficiency over 70.

Ultraviolet-visible-near infrared (UV-Vis-NIR) broadband detection is important for image sensing, communication, and environmental monitoring, yet remains as a challenge in achieving high external quantum efficiency (EQE) in the broad spectrum range. Herein, sensitive broadband integrated photodetectors (PDs) with high EQE levels are reported. The organic bulk-heterojunction (OBHJ) layer, based on a NIR sensitive organic acceptor, is employed to extend the response spectrum of the perovskite PDs. A key strategy of introducing dual electron transport materials respectively for Vis and NIR regions into the active layer of integrated PDs is applied. Further combined with the proper energy level alignment and reasonable distribution of PC61 BM in the active layer, the extraction and transport of photo induced charges in between perovskite and OBHJ is promoted efficiently. The integrated PD with the optimized structure exhibits an EQE mostly beyond 70% in the Vis-NIR region, which is the highest value among the ever reported solution-processable broadband PDs. The highest responsivity is 0.444 and 0.518 A W-1 in the Vis and NIR region, respectively. The specific detectivity is beyond 1010 Jones in the range from 340 to 940 nm, enabling the device to detect weak signals in the UV to NIR broad region.

Electronic and thermoelectric properties of atomically thin C3Si3/C and C3Ge3/C superlattices.

The nanostructuring of graphene into superlattices offers the possibility of tuning both the electronic and thermal properties of graphene. Using classical and quantum mechanical calculations, we have investigated the electronic and thermoelectric properties of the atomically thin superlattice of C3Si3/C (C3Ge3/C) formed by the incorporation of Si (Ge) atoms into graphene. The bandgap and phonon thermal conductivity of C3Si3/C (C3Ge3/C) are 0.54 (0.51) eV and 15.48 (12.64) W m-1 K-1, respectively, while the carrier mobility of C3Si3/C (C3Ge3/C) is 1.285 × 105 (1.311 × 105) cm2 V-1 s-1 at 300 K. The thermoelectric figure of merit for C3Si3/C (C3Ge3/C) can be optimized via the tuning of carrier concentration to obtain the prominent ZT value of 1.95 (2.72).

Density functional theory study on boron- and phosphorus-doped hydrogen-passivated silicene.

When silicene is passivated by hydrogen, a bandgap occurs so that it becomes a semiconductor. Analogous to all the other semiconductors, doping is highly desired to realize the potential of hydrogen-passivated silicene (H-silicene). In the framework of density functional theory (DFT), we have studied the doping of H-silicene with boron (B) and phosphorus (P). The concentration of B or P ranges from 1.4% to 12.5%. It is found that the doping of B or P enables the indirect-bandgap H-silicene to be a semiconductor with a direct bandgap. With the increase of the concentration of B or P, both the valence band and the conduction band shift to lower energies, while the bandgap decreases. Both B- and P-doping lead to the decrease of the effective mass of holes and electrons in H-silicene. For both B- and P-doped H-silicene a subband absorption peak may appear, which blueshifts with the increase of the dopant concentration.

All-silicon multidimensionally-encoded optical physical unclonable functions for integrated circuit anti-counterfeiting.

Integrated circuit anti-counterfeiting based on optical physical unclonable functions (PUFs) plays a crucial role in guaranteeing secure identification and authentication for Internet of Things (IoT) devices. While considerable efforts have been devoted to exploring optical PUFs, two critical challenges remain: incompatibility with the complementary metal-oxide-semiconductor (CMOS) technology and limited information entropy. Here, we demonstrate all-silicon multidimensionally-encoded optical PUFs fabricated by integrating silicon (Si) metasurface and erbium-doped Si quantum dots (Er-Si QDs) with a CMOS-compatible procedure. Five in-situ optical responses have been manifested within a single pixel, rendering an ultrahigh information entropy of 2.32 bits/pixel. The position-dependent optical responses originate from the position-dependent radiation field and Purcell effect. Our evaluation highlights their potential in IoT security through advanced metrics like bit uniformity, similarity, intra- and inter-Hamming distance, false-acceptance and rejection rates, and encoding capacity. We finally demonstrate the implementation of efficient lightweight mutual authentication protocols for IoT applications by using the all-Si multidimensionally-encoded optical PUFs.

Tight-binding calculations of the optical response of optimally P-doped Si nanocrystals: a model for localized surface plasmon resonance.

We present tight-binding calculations in the random-phase approximation of the optical response of Silicon nanocrystals (Si NCs) ideally doped with large concentrations of phosphorus (P) atoms. A collective response of P-induced electrons is demonstrated, leading to localized surface plasmon resonance (LSPR) when a Si NC contains more than ≈10 P atoms. The LSPR energy varies not only with doping concentration but also with NC size due to size-dependent screening by valence electrons. The simple Drude-like behavior is recovered for NC size above 4 nm. Si NCs containing a large number of deep defects in place of hydrogenic impurities do not give rise to LSPR.

Surface modification of chlorine-passivated silicon nanocrystals.

Theoretical understanding of the surface modification of Cl-passivated silicon nanocrystals (Si NCs) is rather limited, in stark contrast to that for H-passivated Si NCs. We now investigate four surface-modification schemes (silanization, alkylation, alkoxylation and aminization) that have been experimentally adopted for Cl-passivated Si NCs in the framework of density functional theory. It is found that aminization most significantly affects the electronic structures of Si NCs by raising the highest occupied molecular orbital (HOMO). The effect of aminization depends on the substituents of amines, rather than the coverage of amine-derived ligands at the NC surface. The lowest unoccupied molecular orbital (LUMO) is more sensitive to the NC size than the HOMO. Only the HOMO is sensitive to surface modification. All the aminization leads to the decrease of the HOMO-LUMO gap despite that the dominant role of quantum confinement effect is maintained in most cases. The current results contribute to the understanding of the optical behavior of Si NCs derived from the surface modification of Cl-passivated ones.

Optical properties of free-standing gelatin-Si nanoparticle composite films and gelatin-Si-Au nanoparticle composite films.

A free-standing fluorescent gelatin-Si nanoparticle composite thin film is facilely prepared by means of a filtration technique assisted by porous copper hydroxide nanostrands as a sacrificial layer. The as-prepared gelatin-Si nanoparticle composite film is greatly portable, flexible, transparent and free-standing. The most important advantage is its robust storage stability stored in ambient air, which make it promising for various applications. Meanwhile, a gelatin-Si-Au nanoparticle composite film is also successfully prepared by the formation of Au NPs in a gelatin-Si nanoparticle composite film through the in situ reduction of HAuCl4 at room temperature. The photoluminescence (PL) quenching and blue shift in the peak of the emission spectra occur due to the energy transfer from Si NPs to Au NPs. By varying the amount and size of Au NPs incorporated into the gelatin-Si nanoparticle composite film, the energy transfer efficiency can be controlled. This is a general method to prepare metal-semiconductor hybrid fluorescent nanomaterials, which offers the possibility of tuning the luminescence intensity and wavelength of the emitted light.

Highly Efficient Energy Transfer from Silicon to Erbium in Erbium-Hyperdoped Silicon Quantum Dots.

Erbium-doped silicon (Er-doped Si) materials hold great potential for advancing Si photonic devices. For Er-doped Si, the efficiency of energy transfer (ηET) from Si to Er3+ is crucial. In order to achieve high ηET, we used nonthermal plasma to synthesize Si quantum dots (QDs) hyperdoped with Er at the concentration of ~1% (i.e., ~5 × 1020 cm-3). The QD surface was subsequently modified by hydrosilylation using 1-dodecene. The Er-hyperdoped Si QDs emitted near-infrared (NIR) light at wavelengths of ~830 and ~1540 nm. An ultrahigh ηET (~93%) was obtained owing to the effective energy transfer from Si QDs to Er3+, which led to the weakening of the NIR emission at ~830 nm and the enhancement of the NIR emission at ~1540 nm. The coupling constant (γ) between Si QDs and Er3+ was comparable to or greater than 1.8 × 10-12 cm3·s-1. The temperature-dependent photoluminescence and excitation rate of Er-hyperdoped Si QDs indicate that strong coupling between Si QDs and Er3+ allows Er3+ to be efficiently excited.

Anti-reflection effect of high refractive index polyurethane with different light trapping structures on solar cells.

The textured surfaces to reduce light reflectivity by using acid-alkali chemical etching and SiNx films are generally necessary for commercial crystalline silicon solar cells. However, this etching process requires a large amount of environmentally harmful acid-alkali solution and has limited options for texture and size. To overcome these disadvantages, a new anti-reflection strategy is proposed in this study, which is using soft nanoimprint lithography to prepare the textured structures on the outside of the SiNx films. The polyurethane with a high refractive index of 1.64 is selected as the texture material, and different templates are selected to prepare it into different light trapping structures, including positive-inverted pyramids, inverted lace cones, and positive-inverted moth-eye nanostructures allowing for easy customization of the textured structures. The finite element simulation and experiments demonstrate that these light trapping structures have a wide spectrum anti-reflection performance in visible and near-infrared bands. With the back surface of the commercial passivated emitter rear contact (PERC) bi-facial solar cells as the imprint substrates, some light trapping structures can reduce the surface weighted average light reflectivity (Rw) at the band of 300-1200 nm from 18.31% to less than 10% and the optimal structures can reduce Rw to 8.71%. This anti-reflection strategy can also be applied to thin-film solar cells and crystalline silicon solar cells of other structures, such as HIT, Topcon, Perovskite/c-Si tandem, and so forth, which shows great development potential.

Interface-Enhanced SiOx/Ru Heterocatalysts for Efficient Electrochemical Water Splitting.

Developing a bifunctional electrocatalyst with remarkable performance viable for overall water splitting is increasingly essential for industrial-scale renewable energy conversion. However, the current electrocatalyst still requires a large cell voltage to drive water splitting due to the unsuitable adsorption/desorption capacity of reaction intermediates, which seriously hinders the practical application of water splitting. Herein, a unique SiOx/Ru nanosheet (NS) material was proposed as a high-performance electrocatalyst for overall water splitting. The SiOx/Ru NSs show superior performance in the hydrogen evolution reaction with a low overpotential of 23 mV (@ 10 mA cm-2) and excellent stability for nearly 200 h (@ 10 mA cm-2) in 1 M KOH. By means of the introduction of SiOx, it is beneficial for balancing the local charge density of the surrounding Ru sites. The suitable electronic coupling between the d-band electrons of Ru and the adsorbed species effectively balances the adsorption and desorption of reaction intermediates on the surface. As a result, the catalyst also exhibits overall water splitting activity with a cell voltage of only 1.496 V to reach the current density of 10 mA cm-2. The present work opens up a new strategy for designing high-performance electrocatalysts for water splitting.

Optogenetics-Inspired Fluorescent Synaptic Devices with Nonvolatility.

Given the synergy of optogenetics and bioimaging in neuroscience, it is possible for light to simultaneously modulate and visualize synaptic events of optoelectronic synaptic devices, which are building blocks of a neuromorphic computing system with optoelectronic integration. Here we demonstrate the realization of the simultaneous modulation and visualization of synaptic events by using optically stimulated synaptic devices based on the heterostructure of fluorescent silicon quantum dots (Si QDs) and monolayer molybdenum disulfide (MoS2). The charge-transfer-enabled photogating effect of the Si QDs/MoS2 heterostructure leads to the nonvolatility of the synaptic devices, which exhibit important synaptic functionalities and synchronous fluorescence upon optical stimulation. An array of the Si QDs/MoS2 optoelectronic synaptic devices is well-employed to mimic robust neural population coding. Defective devices in this array may be pinpointed by the absence of their fluorescence. This work has an important implication for the development of synaptic devices facilitating the system-level diagnosis and device-level positioning of a neuromorphic computing system.

Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current.

Solution growth of single-crystal ferroelectric oxide films has long been pursued for the low-cost development of high-performance electronic and optoelectronic devices. However, the established principles of vapor-phase epitaxy cannot be directly applied to solution epitaxy, as the interactions between the substrates and the grown materials in solution are quite different. Here, we report the successful epitaxy of single-domain ferroelectric oxide films on Nb-doped SrTiO3 single-crystal substrates by solution reaction at a low temperature of ~200 oC. The epitaxy is mainly driven by an electronic polarization screening effect at the interface between the substrates and the as-grown ferroelectric oxide films, which is realized by the electrons from the doped substrates. Atomic-level characterization reveals a nontrivial polarization gradient throughout the films in a long range up to ~500 nm because of a possible structural transition from the monoclinic phase to the tetragonal phase. This polarization gradient generates an extremely high photovoltaic short-circuit current density of ~2.153 mA/cm2 and open-circuit voltage of ~1.15 V under 375 nm light illumination with power intensity of 500 mW/cm2, corresponding to the highest photoresponsivity of ~4.306×10-3 A/W among all known ferroelectrics. Our results establish a general low-temperature solution route to produce single-crystal gradient films of ferroelectric oxides and thus open the avenue for their broad applications in self-powered photo-detectors, photovoltaic and optoelectronic devices.

Recent progress of heterostructures based on two dimensional materials and wide bandgap semiconductors.

Recent progress in the synthesis and assembly of two-dimensional (2D) materials has laid the foundation for various applications of atomically thin layer films. These 2D materials possess rich and diverse properties such as layer-dependent band gaps, interesting spin degrees of freedom, and variable crystal structures. They exhibit broad application prospects in micro-nano devices. In the meantime, the wide bandgap semiconductors (WBS) with an elevated breakdown voltage, high mobility, and high thermal conductivity have shown important applications in high-frequency microwave devices, high-temperature and high-power electronic devices. Beyond the study on single 2D materials or WBS materials, the multi-functional 2D/WBS heterostructures can promote the carrier transport at the interface, potentially providing novel physical phenomena and applications, and improving the performance of electronic and optoelectronic devices. In this review, we overview the advantages of the heterostructures of 2D materials and WBS materials, and introduce the construction methods of 2D/WBS heterostructures. Then, we present the diversity and recent progress in the applications of 2D/WBS heterostructures, including photodetectors, photocatalysis, sensors, and energy related devices. Finally, we put forward the current challenges of 2D/WBS heterostructures and propose the promising research directions in the future.