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Dehui Li

Publications and source records attributed to Dehui Li.

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Self-Trapping Enabled Highly Bright Momentum-Indirect Interlayer Excitons

Interlayer excitons in two dimensional material heterostructures exhibit large exciton binding energies and long lifetimes, making them ideal platforms for studying excitonic devices and many body quantum phenomena. However, the spatially separated electron and hole nature of IXs reduces their oscillator strength by two orders of magnitude compared to intralayer excitons. Achieving high efficiency IX emission remains challenging and requires optimal material selection with appropriate momentum matching and meticulous device fabrication. Here we demonstrate a highly bright momentum indirect IX emission within heterostructures formed between 2D perovskites and monolayer transition metal dichalcogenides. The quantum yield of IX emission reaches 35.2% on average, over 50 times higher than that of the corresponding constituent TMD monolayer, with the highest value exceeding 60%. Notably, the radiative recombination efficiency of this momentum indirect IX exceeds that of momentum direct IXs in monolayer TMD-based heterostructures by two orders of magnitude. We suggest that the remarkably bright IX emission in our heterostructure originates from IX self trapping, induced by strong exciton phonon coupling arising from the soft lattice nature of the 2D perovskite. Our findings provide new insights into achieving high IX emission efficiency and open new avenues for exploring long lifetime excitonic devices.

cond-mat.mes-hall

Agent-Native Immune System: Architecture, Taxonomy, and Engineering

The transition from static chat bots to autonomous agents--equipped with persistent memory, tool-use protocols, and multi-agent collaboration--has fundamentally expanded the AI threat landscape. Current defense mechanisms, such as perimeter security and training-time alignment, remain external to the agent's active reasoning loop. Consequently, they fall short: a fully aligned agent remains highly vulnerable to runtime hijacking via memory poisoning, tool-chain manipulation, or multi-agent protocol attacks. To address this critical gap, we introduce the Agent-Native Immune System (ANIS), the first biologically inspired, endogenous defense architecture embedded directly within the agent's cognitive loop. Our framework presents four primary contributions. First, we design a six-layer Immune Tower (L0-L5), distinctly incorporating Barrier Immunity (L1) as a non-cognitive, physical-and-logical isolation layer. Second, we establish a unified taxonomy of Agent Viruses and Agent Vaccines, formalizing the critical distinction between superficial non-parametric defenses and robust parametric vaccines. Third, we conceptualize the Harness Triad--Meta, Self, and Auto--a self-monitoring, meta-cognitive automation backbone that drives Continual Immune Learning (CIL), enabling vaccines to dynamically adapt to novel threats. Finally, we establish a rigorous theoretical demarcation between model alignment and agent immunity: while alignment provides a static "constitutional" value foundation during training, ANIS serves as the dynamic "law enforcement" mechanism during runtime. We conclude by framing open challenges for the field, including immune protocol standardization, novel evaluation metrics such as the Autoimmunity Rate (false-positive intervention rate), and the co-evolutionary dynamics between pathogens and vaccines within collective intelligence ecosystems.

cs.AI

Forster energy transfer boosts indirect anisotropic interlayer excitons in 2L-MoSe2/perovskite heterostructures

Interlayer excitons (IXs) in two-dimensional (2D) van der Waals heterostructures have attracted considerable attention due to their unique optical and electronic properties. Owing to the spatially indirect nature, the radiative emission efficiency highly sensitive to interlayer twist angles. Further considering that their uniformly oriented out-of-plane dipole moments limit directional emission, strategies to simultaneously improve emission efficiency and induce optical anisotropy warrant in-depth investigation. In this work, we report significant photoluminescence (PL) enhancement and optical anisotropy of IXs in 2L-MoSe2/perovskite heterostructures mediated by energy transfer from ReS2. We attribute this enhancement to Forster resonance energy transfer (FRET), which increases the 2L-MoSe2 emission by approximately eight-fold at room temperature, and nearly doubles the emission intensity of momentum-indirect IXs in 2L-MoSe2/perovskite heterostructures at 78 K. Importantly, the optical anisotropy of ReS2 can be effectively imprinted onto 2L-MoSe2 and associated indirect IXs during the energy transfer process, yielding a linear dichroism of approximately 1.1 for both intralayer excitons and IXs with identical polarization directions. These findings expand the scope of IX study beyond direct bandgap materials with strong intrinsic emission to include systems with indirect bandgaps, offering new avenues for realizing high-performance polarization-sensitive optoelectronic devices.

cond-mat.mtrl-sci

Out-of-plane orientated self-trapped excitons enabled polarized light guiding in 2D perovskites

Active optical waveguides combine light source and waveguides together in an individual component, which are essential for the integrated photonic chips. Although 1D luminescent materials based optical waveguides were extensively investigated, 2D waveguides allow photons to flow within a plane and serve as an ideal component for the ultracompact photonic circuits. Nevertheless, light guiding in 2D planar structures normally relies on the precise control of molecular orientation, which is complicated and low yield. Here, we report a strategy to guide polarized light in 2D microflakes by making use of the out-of-plane (OP) orientation of self-trapped excitons in as-synthesized 2D perovskite microplates. A space confined crystallization method is developed to synthesize 2D perovskite microflakes with dominated broad self-trapped excitons emission at room temperature, which are highly OP orientated with a percentage of the OP component over 85%. Taking advantages of the negligible absorption coefficient and improved coupling efficiency of OP orientated self-trapped exciton emission to the planar waveguide mode of the as-synthesized perovskite microflakes, we have achieved a broadband polarized light guiding with a full width at half maximum over 120 nm. Our findings provide a promising platform for the development of ultracompact photonic circuits.

physics.optics

Efficient electrical switching of exciton states for valley contrast manipulation in two-dimensional perovskite/monolayer WS2 heterostructures

The coupled spin-valley physics in transition metal dichalcogenides (TMDs) endows exciton states with valley degrees of freedom, making them promising for valleytronic applications in TMDs monolayers and/or their heterostructures. Although the valley dynamics of intralayer and interlayer excitons (IXs) have been studied, efficient manipulation of valley pseudospins by switching exciton states remains elusive. Therefore, it is of great importance to effectively tune the exciton states to obtain practical valley polarization switches for valley encoding. Here, we demonstrate the electrical switching of exciton emission with highly variable valley polarization mediated by charged IXs (CIXs) in the heterostructure of monolayer WS2 and two-dimensional (2D) perovskite, irrespective of lattice constants, the rotational and translational alignment. The formation of IXs is identified by photoluminescence excitation (PLE) and photoluminescence (PL) studies, which can be further electrically tuned from positively charged to negatively charged depending on the electrostatic doping level of monolayer WS2. Importantly, we demonstrate an electrical switching from type two to type one band alignment, manifesting as a change in the PL profile from CIX to charged intralayer exciton emission. Such transition induces a large contrast in valley polarization between the two exciton states, enabling the reversible electrically regulated valley polarization switch with a maximum ON/OFF ratio of 15.8. Our study provides an alternative mechanism to achieve valley polarization switching with great simplicity for valleytronics and the electrical control of exciton species and associated valley-contrasting physics would further facilitate the development of optoelectronic and valleytronic devices

physics.app-ph

Self-powered Filterless On-chip Full-Stokes Polarimeter

The detection of polarization states of light is essential in photonic and optoelectronic devices. Currently, the polarimeters are usually constructed with the help of waveplates or a comprehensive metasurface, which will inevitably increase the fabrication complexity and unnecessary energy loss. Here, we have successfully demonstrated a self-powered filterless on-chip full-Stokes polarimeter based on a single-layer MoS2/few-layer MoS2 homojunction. Combining the built-in electric field enhanced circular photogalvanic effect with the intrinsic optical anisotropy of MoS2 between in-plane and out-of-plane direction, the device is able to conveniently sense four Stokes parameters of incident light at zero bias without requiring an extra filtering layer, and can function in the wavelength range of 650-690 nm with acceptable average errors. Besides, this homojunction device is easy to integrate with silicon-based chips and could have much smaller sizes than metasurface based polarimeters. Our study thus provides an excellent paradigm for high-performance on-chip filterless polarimeters.

physics.optics

Interlayer-Exciton Based Nonvolatile Valleytronic Memory

Analogous to conventional charge-based electronics, valleytronics aims at encoding data via the valley degree of freedom, enabling new routes for information processing. Long-lived interlayer excitons (IXs) in van der Waals heterostructures (HSs) stacked by transition metal dichalcogenides (TMDs) carry valley-polarized information and thus could find promising applications in valleytronic devices. Although great progress of studies on valleytronic devices has been achieved, nonvolatile valleytronic memory, an indispensable device in valleytronics, is still lacking up to date. Here, we demonstrate an IX-based nonvolatile valleytronic memory in a WS2/WSe2 HS. In this device, the emission characteristics of IXs exhibit a large excitonic/valleytronic hysteresis upon cyclic-voltage sweeping, which is ascribed to the chemical-doping of O2/H2O redox couple trapped between the TMDs and substrate. Taking advantage of the large hysteresis, the first nonvolatile valleytronic memory has been successfully made, which shows a good performance with retention time exceeding 60 minutes. These findings open up an avenue for nonvolatile valleytronic memory and could stimulate more investigations on valleytronic devices.

physics.app-ph

PCNN: Pattern-based Fine-Grained Regular Pruning towards Optimizing CNN Accelerators

Weight pruning is a powerful technique to realize model compression. We propose PCNN, a fine-grained regular 1D pruning method. A novel index format called Sparsity Pattern Mask (SPM) is presented to encode the sparsity in PCNN. Leveraging SPM with limited pruning patterns and non-zero sequences with equal length, PCNN can be efficiently employed in hardware. Evaluated on VGG-16 and ResNet-18, our PCNN achieves the compression rate up to 8.4X with only 0.2% accuracy loss. We also implement a pattern-aware architecture in 55nm process, achieving up to 9.0X speedup and 28.39 TOPS/W efficiency with only 3.1% on-chip memory overhead of indices.

cs.LG

Controllable growth of centimeter-size 2D perovskite heterostructural single crystals for highly narrow dual-band photodetectors

Two-dimensional (2D) organic-inorganic perovskites have recently attracted increasing attention due to their great environmental stability, remarkable quantum confinement effect and layered characteristic. Heterostructures consisting of 2D layered perovskites are expected to exhibit new physical phenomena inaccessible to the single 2D perovskites and can greatly extend their functionalities for novel electronic and optoelectronic applications. Herein, we develop a novel solution method to synthesize 2D perovskite single-crystals with the centimeter size, high phase purity, controllable junction depth, high crystalline quality and great stability for highly narrow dual-band photodetectors. On the basis of the different lattice constant, solubility and growth rate between different n number, the newly designed synthesis method allows to first grow n=1 perovskite guided by the self-assembled layer of the organic cations at the water-air interface and subsequently n=2 layer is formed via diffusion process. Such growth process provides an efficient away for us to readily obtain 2D perovskite heterostructural single-crystals with various thickness and junction depth by controlling the concentration, reaction temperature and time. Photodetectors based on such heterostructural single crystal plates exhibit extremely low dark current, high on-off current ratio, and highly narrow dual-band spectral response with a full-width at half-maximum of 20 nm at 540 nm and 34 nm at 610 nm. In particular, the synthetic strategy is general for other 2D perovskites and the narrow dual-band spectral response with all full-width at half-maximum below 40 nm can be continuously tuned from red to blue by properly changing the halide compositions.

physics.app-ph

Gate-induced insulator to band-like transport transition in organolead halide perovskite

Understanding the intrinsic charge transport in organolead halide perovskites is essential for the development of high-efficiency photovoltaics and other optoelectronic devices. Despite the rapid advancement of the organolead halide perovskite in photovoltaic and optoelectronic applications, the intrinsic charge carrier transport in these materials remains elusive partly due to the difficulty of fabricating electrical devices and obtaining good electrical contact. Here, we report the fabrication of organolead halide perovskite microplates with monolayer graphene as low barrier electrical contact. A systematic charge transport studies reveal an insulator to band-like transport transition. Our studies indicate that the insulator to band-like transport transition depends on the orthorhombic-to-tetragonal phase transition temperature and defect densities of the organolead halide perovskite microplates. Our findings are not only important for the fundamental understanding of charge transport behavior but also offer valuable practical implications for photovoltaics and optoelectronic applications based on the organolead halide perovskite.

cond-mat.mtrl-sci

Electric field induced strong enhancement of electroluminescence in multi-Layer MoS2

The layered transition metal dichalcogenides (TMDs) have attracted considerable interest due to their unique electronic and optical properties. Here we report electric field induced strong electroluminescence in multi-layer MoS2 and WSe2. We show that GaN-Al2O3-MoS2 and GaN-Al2O3-MoS2-Al2O3-graphene vertical heterojunctions can be created with excellent rectification behaviour. Electroluminescence studies demonstrate prominent direct bandgap excitonic emission in multi-layer MoS2 over the entire vertical junction area. Importantly, the electroluminescence efficiency observed in multi-layer MoS2 is comparable to or even higher than that in monolayers, corresponding to a relative electroluminescence enhancement factor of >1000 in multi-layer MoS2 when compared to its photoluminescence. This striking enhancement of electroluminescence can be attributed to the high electric field induced carrier redistribution from low energy points (indirect bandgap) to high energy points (direct bandgap) of k-space, arising from the unique band structure of MoS2 with a much higher density of states at high energy points. The electric field induced electroluminescence is general for other TMDs including WSe2, and can provide a fundamental platform to probe the carrier injection, population and recombination in multi-layer TMDs and open up a new pathway toward TMD based optoelectronic devices.

cond-mat.mes-hall

Wafer-scale growth of large arrays of perovskite microplate crystals for functional electronics and optoelectronics

Methylammonium lead iodide perovskite has attracted intensive interest for its diverse optoelectronic applications. However, most studies to date have been limited to bulk thin films that are difficult to implement for integrated device arrays because of their incompatibility with typical lithography processes. We report the first patterned growth of regular arrays of perovskite microplate crystals for functional electronics and optoelectronics. We show that large arrays of lead iodide microplates can be grown from an aqueous solution through a seeded growth process and can be further intercalated with methylammonium iodide to produce perovskite crystals. Structural and optical characterizations demonstrate that the resulting materials display excellent crystalline quality and optical properties. We further show that perovskite crystals can be selectively grown on prepatterned electrode arrays to create independently addressable photodetector arrays and functional field effect transistors. The ability to grow perovskite microplates and to precisely place them at specific locations offers a new material platform for the fundamental investigation of the electronic and optical properties of perovskite materials and opens a pathway for integrated electronic and optoelectronic systems.

cond-mat.mtrl-sci

Van der Waals heterojunction devices based on organohalide perovskites and two-dimensional materials

The recently emerged organohalide perovskites (e.g., CH3NH3PbI3) have drawn intense attention for high efficiency solar cells. However, with a considerable solubility in many solvents, these perovskites are not typically compatible with conventional lithography processes for more complicated device fabrications that are important for both fundamental studies and technological applications. Here we report the creation of novel heterojunction devices based on perovskites and two-dimensional (2D) crystals by taking advantage of the layered characteristic of lead iodide (PbI2) and vapor phase intercalation. We show a graphene/perovskite/graphene vertical stack can deliver a highest photoresponsivity of ~950 A/W and photoconductive gain of ~2200, and a graphene/WSe2/perovskite/graphene heterojunction can display a high on/off ratio (~10^6) transistor behavior with distinct gate-tunable diode characteristics and open-circuit voltages. Such unique perovskite-2D heterostructures have significant potential for future optoelectronic research and can enable broad possibilities with compositional tunability of organohalide perovskites and the versatility offered by diverse 2D materials.

cond-mat.mtrl-sci

Towards barrier free contact to MoS2 using graphene electrodes

The two-dimensional (2D) layered semiconductors such as MoS2 have attracted tremendous interest as a new class of electronic materials. However, there is considerable challenge in making reliable contacts to these atomically thin materials. Here we present a new strategy by using graphene as back electrodes to achieve Ohmic contact to MoS2. With a finite density of states, the Fermi level of graphene can be readily modified by gate potential to ensure a nearly perfect band alignment with MoS2. We demonstrate, for the first time, a transparent contact can be made to MoS2 with essentially zero contact barrier and linear output behaviour at cryogenic temperatures (down to 1.9 K) for both monolayer and multilayer MoS2. Benefiting from the barrier-free transparent contacts, we show that a metal-insulator-transition (MIT) can be observed in a two-terminal MoS2 device, a phenomenon that could be easily masked by Schottky barrier and only seen in four-terminal devices in conventional metal-contacted MoS2 system. With further passivation y born nitride encapsulation, we demonstrate a record high extrinsic (two-terminal) field effect mobility over 1300 cm2/Vs in MoS2.

cond-mat.mtrl-sci

Electroluminescence and photocurrent generation from atomically sharp WSe2/MoS2 heterojunction p-n diodes

The p-n diodes represent the most fundamental device building block for diverse optoelectronic functions, but are difficult to achieve in atomically thin transition metal dichalcogenides (TMDs) due to the inability to selectively dope them into p- or n-type semiconductors. Here we report the first demonstration of an atomically thin and atomically sharp heterojunction p-n diode by vertically stacking p-type monolayer tungsten diselenide (WSe2) and n-type few-layer molybdenum disulfide (MoS2). Electrical measurement demonstrates excellent diode characteristics with well-defined current rectification behaviour and an ideality factor of 1.2. Photocurrent mapping shows fast photoresponse over the entire overlapping region with a highest external quantum efficiency up to 12 %. Electroluminescence studies show prominent band edge excitonic emission and strikingly enhanced hot electron luminescence. A systematic investigation shows distinct layer-number dependent emission characteristics and reveals important insight about the origin of hot-electron luminescence and the nature of electron-orbital interaction in TMDs. We believe that these atomically thin heterojunction p-n diodes represent an interesting system for probing the fundamental electro-optical properties in TMDs, and can open up a new pathway to novel optoelectronic devices such as atomically thin photodetectors, photovoltaics, as well as spin-/valley-polarized light emitting diodes and on-chip lasers.

cond-mat.mes-hall