Twist angle-dependent valley polarization switching in heterostructures.

The twist engineering of moiré superlattice in van der Waals heterostructures of transition metal dichalcogenides can manipulate valley physics of interlayer excitons (IXs), paving the way for next-generation valleytronic devices. However, the twist angle-dependent control of excitonic potential on valley polarization is not investigated so far in electrically controlled heterostructures and the physical mechanism underneath needs to be explored. Here, we demonstrate the dependence of both polarization switching and degree of valley polarization on the moiré period. We also find the mechanisms to reveal the modulation of twist angle on the exciton potential and the electron-hole exchange interaction, which elucidate the experimentally observed twist angle-dependent valley polarization of IXs. Furthermore, we realize the valley-addressable devices based on polarization switch. Our work demonstrates the manipulation of the valley polarization of IXs by tunning twist angle in electrically controlled heterostructures, which opens an avenue for electrically controlling the valley degrees of freedom in twistronic devices.

A programmable topological photonic chip.

Controlling topological phases of light allows the observation of abundant topological phenomena and the development of robust photonic devices. The prospect of more sophisticated control with topological photonic devices for practical implementations requires high-level programmability. Here we demonstrate a fully programmable topological photonic chip with large-scale integration of silicon photonic nanocircuits and microresonators. Photonic artificial atoms and their interactions in our compound system can be individually addressed and controlled, allowing the arbitrary adjustment of structural parameters and geometrical configurations for the observation of dynamic topological phase transitions and diverse photonic topological insulators. Individual programming of artificial atoms on the generic chip enables the comprehensive statistical characterization of topological robustness against relatively weak disorders, and counterintuitive topological Anderson phase transitions induced by strong disorders. This generic topological photonic chip can be rapidly reprogrammed to implement multifunctionalities, providing a flexible and versatile platform for applications across fundamental science and topological technologies.

Layer-dependent ultrafast carrier dynamics of PdSe2 investigated by photoemission electron microscopy.

For atomically thin two-dimensional materials, variations in layer thickness can result in significant changes in the electronic energy band structure and physicochemical properties, thereby influencing the carrier dynamics and device performance. In this work, we employ time- and energy-resolved photoemission electron microscopy to reveal the ultrafast carrier dynamics of PdSe2 with different layer thicknesses. We find that for few-layer PdSe2 with a semiconductor phase, an ultrafast hot carrier cooling on a timescale of approximately 0.3 ps and an ultrafast defect trapping on a timescale of approximately 1.3 ps are unveiled, followed by a slower decay of approximately tens of picoseconds. However, for bulk PdSe2 with a semimetal phase, only an ultrafast hot carrier cooling and a slower decay of approximately tens of picoseconds are observed, while the contribution of defect trapping is suppressed with the increase of layer number. Theoretical calculations of the electronic energy band structure further confirm the transition from a semiconductor to a semimetal. Our work demonstrates that TR- and ER-PEEM with ultrahigh spatiotemporal resolution and wide-field imaging capability has great advantages in revealing the intricate details of ultrafast carrier dynamics of nanomaterials.

Controlling the Polarization of Nitrogen Ion Lasing.

Air lasing provides a promising technique to remotely produce coherent radiation in the atmosphere and has attracted continuous attention. However, the polarization properties of N2+ lasing with seeding have not been understood since it was discovered 10 years ago, in which the polarization behaviors appear disordered and confusing. Here, we performed an experimental and theoretical investigation of the polarization properties of N2+ lasing and successfully revealed its underlying physical mechanism. We found that the optical gain is anisotropic, owing to the permanent alignment of N2+ induced by the preferential ionization of the pump light. As a result, the polarization of the N2+ lasing tends to align with that of the pump light after amplification, which becomes more pronounced as the amplification factor increases. Based on the permanent alignment of N2+, we built a theoretical model that analytically interpreted and numerically reproduced the experimental observations, which points out the key factors for controlling the polarization of N2+ lasing.

Information-entropy enabled identifying topological photonic phase in real space.

The topological photonics plays an important role in the fields of fundamental physics and photonic devices. The traditional method of designing topological system is based on the momentum space, which is not a direct and convenient way to grasp the topological properties, especially for the perturbative structures or coupled systems. Here, we propose an interdisciplinary approach to study the topological systems in real space through combining the information entropy and topological photonics. As a proof of concept, the Kagome model has been analyzed with information entropy. We reveal that the bandgap closing does not correspond to the topological edge state disappearing. This method can be used to identify the topological phase conveniently and directly, even the systems with perturbations or couplings. As a promotional validation, Su-Schrieffer-Heeger model and the valley-Hall photonic crystal have also been studied based on the information entropy method. This work provides a method to study topological photonic phase based on information theory, and brings inspiration to analyze the physical properties by taking advantage of interdisciplinarity.

Demonstration of hypergraph-state quantum information processing.

Complex entangled states are the key resources for measurement-based quantum computations, which is realised by performing a sequence of measurements on initially entangled qubits. Executable quantum algorithms in the graph-state quantum computing model are determined by the entanglement structure and the connectivity of entangled qubits. By generalisation from graph-type entanglement in which only the nearest qubits interact to a new type of hypergraph entanglement in which any subset of qubits can be arbitrarily entangled via hyperedges, hypergraph states represent more general resource states that allow arbitrary quantum computation with Pauli universality. Here we report experimental preparation, certification and processing of complete categories of four-qubit hypergraph states under the principle of local unitary equivalence, on a fully reprogrammable silicon-photonic quantum chip. Genuine multipartite entanglement for hypergraph states is certificated by the characterisation of entanglement witness, and the observation of violations of Mermin inequalities without any closure of distance or detection loopholes. A basic measurement-based protocol and an efficient resource state verification by color-encoding stabilizers are implemented with local Pauli measurement to benchmark the building blocks for hypergraph-state quantum computation. Our work prototypes hypergraph entanglement as a general resource for quantum information processing.

Amphoteric Chelating Ultrasmall Colloids for FAPbI3 Nanodomains Enable Efficient Near-Infrared Light-Emitting Diodes.

Perovskite light-emitting diodes (PeLEDs) are the next promising display technologies because of their high color purity and wide color gamut, while two classical emitter forms, i.e., polycrystalline domains and quantum dots, are encountering bottlenecks. Weak carrier confinement of large polycrystalline domains leads to inadequate radiative recombination, and surface ligands on quantum dots are the main annihilation sites for injected carriers. Here, pinpointing these issues, we screened out an amphoteric agent, namely, 2-(2-aminobenzoyl)benzoic acid (2-BA), to precisely control the in situ growth of FAPbI3 (FA: formamidine) nanodomains with enhanced space confinement, preferred crystal orientation, and passivated trap states on the transport-layer substrate. The amphoteric 2-BA performs bidentate chelating functions on the formation of ultrasmall perovskite colloids (<1 nm) in the precursor, resulting in a smoother FAPbI3 emitting layer. Based on monodispersed and homogeneous nanodomain films, a near-infrared PeLED device with a champion efficiency of >22% plus enhanced T80 operational stability was achieved. The proposed perovskite nanodomain film tends to be a mainstream emitter toward the performance breakthrough of PeLED devices covering visible wavelengths beyond infrared.

Spin-controlled topological phase transition in non-Euclidean space.

Modulation of topological phase transition has been pursued by researchers in both condensed matter and optics research fields, and has been realized in Euclidean systems, such as topological photonic crystals, topological metamaterials, and coupled resonator arrays. However, the spin-controlled topological phase transition in non-Euclidean space has not yet been explored. Here, we propose a non-Euclidean configuration based on Möbius rings, and we demonstrate the spin-controlled transition between the topological edge state and the bulk state. The Möbius ring, which is designed to have an 8π period, has a square cross section at the twist beginning and the length/width evolves adiabatically along the loop, accompanied by conversion from transverse electric to transverse magnetic modes resulting from the spin-locked effect. The 8π period Möbius rings are used to construct Su-Schrieffer-Heeger configuration, and the configuration can support the topological edge states excited by circularly polarized light, and meanwhile a transition from the topological edge state to the bulk state can be realized by controlling circular polarization. In addition, the spin-controlled topological phase transition in non-Euclidean space is feasible for both Hermitian and non-Hermitian cases in 2D systems. This work provides a new degree of polarization to control topological photonic states based on the spin of Möbius rings and opens a way to tune the topological phase in non-Euclidean space.

Sub-Second Long Lifetime Triplet Exciton Reservoir for Highly Efficient and Stable Organic Light-Emitting Diode.

In organic light-emitting diode (OLED), achieving high efficiency requires effective triplet exciton confinement by carrier-transporting materials, which typically have higher triplet energy (ET) than the emitter, leading to poor stability. Here, an electron-transporting material (ETM), whose ET is 0.32 eV lower than that of the emitter is reported. In devices, it surprisingly exhibits strong confinement effect and generates excellent efficiency. Additionally, the device operational lifetime is 4.9 times longer than the device with a standard ETM, 1,3,5-tri(1-phenyl-1H-benzo[d]imidazol-2-yl) phenyl (whose ET 0.36 eV is higher than the emitter). This anomalous finding is ascribed to the exceptionally long triplet state lifetime (≈0.2 s) of the ETM. It is named as long-lifetime triplet exciton reservoir effect. The systematic analysis reveals that the long triplet lifetime of ETM can compensate the requirement for high ET with the help of endothermic energy transfer. Such combination of low ET and long lifetime provides equivalent exciton confinement effect and high molecular stability simultaneously. It offers a novel molecular design paradigm for breaking the dilemma between high efficiency and prolonged operational lifetime in OLEDs.

Direct Hot-Electron Transfer at the Au Nanoparticle/Monolayer Transition-Metal Dichalcogenide Interface Observed with Ultrahigh Spatiotemporal Resolution.

Plasmon-induced hot-electron transfer at the metallic nanoparticle/semiconductor interface is the basis of plasmon-enhanced photocatalysis and energy harvesting. However, limited by the nanoscale size of hot spots and femtosecond time scale of hot-electron transfer, direct observation is still challenging. Herein, by using spatiotemporal-resolved photoemission electron microscopy with a two-color pump-probe beamline, we directly observed such a process with a concise system, the Au nanoparticle/monolayer transition-metal dichalcogenide (TMD) interface. The ultrafast hot-electron transfer from Au nanoparticles to monolayer TMDs and the plasmon-enhanced transfer process were directly measured and verified through an in situ comparison with the Au film/TMD interface and free TMDs. The lifetime at the Au nanoparticle/MoSe2 interface decreased from 410 to 42 fs, while the photoemission intensities exhibited a 27-fold increase compared to free MoSe2. We also measured the evolution of hot electrons in the energy distributions, indicating the hot-electron injection and decay happened in an ultrafast time scale of ∼50 fs without observable electron cooling.

Multifunctional ytterbium oxide buffer for perovskite solar cells.

Perovskite solar cells (PSCs) comprise a solid perovskite absorber sandwiched between several layers of different charge-selective materials, ensuring unidirectional current flow and high voltage output of the devices1,2. A 'buffer material' between the electron-selective layer and the metal electrode in p-type/intrinsic/n-type (p-i-n) PSCs (also known as inverted PSCs) enables electrons to flow from the electron-selective layer to the electrode3-5. Furthermore, it acts as a barrier inhibiting the inter-diffusion of harmful species into or degradation products out of the perovskite absorber6-8. Thus far, evaporable organic molecules9,10 and atomic-layer-deposited metal oxides11,12 have been successful, but each has specific imperfections. Here we report a chemically stable and multifunctional buffer material, ytterbium oxide (YbOx), for p-i-n PSCs by scalable thermal evaporation deposition. We used this YbOx buffer in the p-i-n PSCs with a narrow-bandgap perovskite absorber, yielding a certified power conversion efficiency of more than 25%. We also demonstrate the broad applicability of YbOx in enabling highly efficient PSCs from various types of perovskite absorber layer, delivering state-of-the-art efficiencies of 20.1% for the wide-bandgap perovskite absorber and 22.1% for the mid-bandgap perovskite absorber, respectively. Moreover, when subjected to ISOS-L-3 accelerated ageing, encapsulated devices with YbOx exhibit markedly enhanced device stability.

Spatiotemporal imaging and shaping of electron wave functions using novel attoclock interferometry.

Electrons detached from atoms by photoionization carry valuable information about light-atom interactions. Characterizing and shaping the electron wave function on its natural timescale is of paramount importance for understanding and controlling ultrafast electron dynamics in atoms, molecules and condensed matter. Here we propose a novel attoclock interferometry to shape and image the electron wave function in atomic photoionization. Using a combination of a strong circularly polarized second harmonic and a weak linearly polarized fundamental field, we spatiotemporally modulate the atomic potential barrier and shape the electron wave functions, which are mapped into a temporal interferometry. By analyzing the two-color phase-resolved and angle-resolved photoelectron interference, we are able to reconstruct the spatiotemporal evolution of the shaping on the amplitude and phase of electron wave function in momentum space within the optical cycle, from which we identify the quantum nature of strong-field ionization and reveal the effect of the spatiotemporal properties of atomic potential on the departing electron. This study provides a new approach for spatiotemporal shaping and imaging of electron wave function in intense light-matter interactions and holds great potential for resolving ultrafast electronic dynamics in molecules, solids, and liquids.

Buried-Metal-Grid Electrodes for Efficient Parallel-Connected Perovskite Solar Cells.

The limited conductivity of existing transparent conducting oxide (TCO) greatly restricts the further performance improvement of perovskite solar cells (PSCs), especially for large-area devices. Herein, buried-metal-grid tin-doped indium oxide (BMG ITO) electrodes are developed to minimize the power loss caused by the undesirable high sheet resistance of TCOs. By burying 140-nm-thick metal grids into ITO using a photolithography technique, the sheet resistance of ITO is reduced from 15.0 to 2.7 Ω sq-1 . The metal step of BMG over ITO has a huge impact on the charge carrier transport in PSCs. The PSCs using BMG ITO with a low metal step deliver power conversion efficiencies (PCEs) significantly better than that of their counterparts with higher metal steps. Moreover, compared with the pristine ITO-based PSCs, the BMG ITO-based PSCs show a smaller PCE decrease when scaling up the active area of devices. The parallel-connected large-area PSCs with an active area of 102.8 mm2 reach a PCE of 22.5%. The BMG ITO electrodes are also compatible with the fabrication of inverted-structure PSCs and organic solar cells. The work demonstrates the great efficacy of improving the conductivity of TCO by BMG and opens up a promising avenue for constructing highly efficient large-area PSCs.

Fractal photonic anomalous Floquet topological insulators to generate multiple quantum chiral edge states.

Anomalous Floquet topological insulators with vanishing Chern numbers but supporting chiral edge modes are attracting more and more attention. Since the existing anomalous Floquet topological insulators usually support only one kind of chiral edge mode even at a large lattice size, they are unscalable and unapplicable for multistate topological quantum systems. Recently, fractal topological insulators with self-similarity have been explored to support more nontrivial modes. Here, we demonstrate the first experimental realization of fractal photonic anomalous Floquet topological insulators based on dual Sierpinski carpet consisting of directional couplers using the femtosecond laser direct writing. The fabricated lattices support much more kinds of chiral edge states with fewer waveguides and enable perfect hopping of quantum states with near unit transfer efficiency. Instead of zero-dimensional bound modes for quantum state transport in previous laser direct-written topological insulators, we generate multiple propagating single-photon chiral edge states in the fractal lattice and observe high-visibility quantum interferences. These suggest the successful realization of highly indistinguishable single-photon chiral edge states, which can be applied in various quantum operations. This work provides the potential for enhancing the multi-fold manipulation of quantum states, enlarging the encodable quantum information capacity in a single lattice via high-dimensional encoding and many other fractal applications.

A scheme for realizing nonreciprocal interlayer coupling in bilayer topological systems.

Nonreciprocal interlayer coupling is difficult to practically implement in bilayer non-Hermitian topological photonic systems. In this work, we identify a similarity transformation between the Hamiltonians of systems with nonreciprocal interlayer coupling and on-site gain/loss. The similarity transformation is widely applicable, and we show its application in one- and two-dimensional bilayer topological systems as examples. The bilayer non-Hermitian system with nonreciprocal interlayer coupling, whose topological number can be defined using the gauge-smoothed Wilson loop, is topologically equivalent to the bilayer system with on-site gain/loss. We also show that the topological number of bilayer non-Hermitian C6v-typed domain-induced topological interface states can be defined in the same way as in the case of the bilayer non-Hermitian Su-Schrieffer-Heeger model. Our results show the relations between two microscopic provenances of the non-Hermiticity and provide a universal and convenient scheme for constructing and studying nonreciprocal interlayer coupling in bilayer non-Hermitian topological systems. This scheme is useful for observation of non-Hermitian skin effect in three-dimensional systems.

Bright and Dark Quadrupolar Excitons in the WSe_{2}/MoSe_{2}/WSe_{2} Heterotrilayer.

Transition metal dichalcogenide heterostructures have been extensively studied as a platform for investigating exciton physics. While heterobilayers such as WSe_{2}/MoSe_{2} have received significant attention, there has been comparatively less research on heterotrilayers, which may offer new excitonic species and phases, as well as unique physical properties. In this Letter, we present theoretical and experimental investigations on the emission properties of quadrupolar excitons (QXs), a newly predicted type of exciton, in a WSe_{2}/MoSe_{2}/WSe_{2} heterotrilayer device. Our findings reveal that the optical brightness or darkness of QXs is determined by horizontal mirror symmetry and valley and spin selection rules. Additionally, the emission intensity and energy of both bright and dark QXs can be adjusted by applying an out-of-plane electric field, due to changes in hole distribution and the Stark effect. These results not only provide experimental evidence for the existence of QXs in heterotrilayers but also uncover their novel properties, which have the potential to drive the development of new exciton-based applications.

Reveal Ultrafast Electron Relaxation across Sub-bands of Tellurium by Time- and Energy-Resolved Photoemission Microscopy.

Exploring ultrafast carrier dynamics is crucial for the materials' fundamental properties and device design. In this work, we employ time- and energy-resolved photoemission electron microscopy with tunable pump wavelengths from visible to near-infrared to reveal the ultrafast carrier dynamics of the elemental semiconductor tellurium. We find that two discrete sub-bands around the Γ point of the conduction band are involved in excited-state electron ultrafast relaxation and reveal that hot electrons first go through ultrafast intra sub-band cooling on a time scale of about 0.3 ps and then transfer from the higher sub-band to the lower one on a time scale of approximately 1 ps. Additionally, theoretical calculations reveal that the lower one has flat-band characteristics, possessing a large density of states and a long electron lifetime. Our work demonstrates that TR- and ER-PEEM with broad tunable pump wavelengths are powerful techniques in revealing the details of ultrafast carrier dynamics in time and energy domains.

Amplification of light pulses with orbital angular momentum (OAM) in nitrogen ions lasing.

Nitrogen ions pumped by intense femtosecond laser pulses give rise to optical amplification in the ultraviolet range. Here, we demonstrated that a seed light pulse carrying orbital angular momentum (OAM) can be significantly amplified in nitrogen plasma excited by a Gaussian femtosecond laser pulse. With the topological charge of ℓ = ±1, we observed an energy amplification of the seed light pulse by two orders of magnitude, while the amplified pulse carries the same OAM as the incident seed pulse. Moreover, we show that a spatial misalignment of the plasma amplifier with the OAM seed beam leads to an amplified emission of Gaussian mode without OAM, due to the special spatial profile of the OAM seed pulse that presents a donut-shaped intensity distribution. Utilizing this misalignment, we can implement an optical switch that toggles the output signal between Gaussian mode and OAM mode. This work not only certifies the phase transfer from the seed light to the amplified signal, but also highlights the important role of spatial overlap of the donut-shaped seed beam with the gain region of the nitrogen plasma for the achievement of OAM beam amplification.

Magnetically-dressed CrSBr exciton-polaritons in ultrastrong coupling regime.

Over the past few decades, exciton-polaritons have attracted substantial research interest due to their half-light-half-matter bosonic nature. Coupling exciton-polaritons with magnetic orders grants access to rich many-body phenomena, but has been limited by the availability of material systems that exhibit simultaneous exciton resonances and magnetic ordering. Here we report magnetically-dressed microcavity exciton-polaritons in the van der Waals antiferromagnetic (AFM) semiconductor CrSBr coupled to a Tamm plasmon microcavity. Using angle-resolved spectroscopy, we reveal an exceptionally high exciton-photon coupling strength, up to 169 meV, demonstrating ultrastrong coupling that persists up to room temperature. By performing temperature-dependent spectroscopy, we show the magnetic nature of the exciton-polaritons in CrSBr microcavity as the magnetic order changes from AFM to paramagnetic. By applying an out-of-plane magnetic field, we achieve effective tuning of the polariton energy while maintaining the ultrastrong exciton-photon coupling strength. We attribute this to the spin canting process that modulates the interlayer exciton interaction.

Ultrafast Electronic Dynamics in Anisotropic Indirect Interlayer Excitonic States of Monolayer WSe2/ReS2 Heterojunctions.

Understanding ultrafast electronic dynamics of the interlayer excitonic states in atomically thin transition metal dichalcogenides is of importance in engineering valleytronics and developing excitonic integrated circuits. In this work, we experimentally explored the ultrafast dynamics of indirect interlayer excitonic states in monolayer type II WSe2/ReS2 heterojunctions using time-resolved photoemission electron microscopy, which reveals its anisotropic behavior. The ultrafast cooling and decay of excited-state electrons exhibit significant linear dichroism. The ab initio theoretical calculations provide unambiguous evidence that this linear dichroism result is primarily associated with the anisotropic nonradiative recombination of indirect interlayer excitonic states. Measuring time-resolved photoemission energy spectra, we have further revealed the ultrafast evolution of excited-state electrons in anisotropic indirect interlayer excitonic states. The findings have important implications for controlling the interlayer moiré excitonic effects and designing anisotropic optoelectronic devices.