Evolution of the Fermi Surface of 1T-VSe2 across a Structural Phase Transition.

Periodic lattice distortion, known as the charge density wave, is generally attributed to electron-phonon coupling. This correlation is expected to induce a pseudogap at the Fermi level in order to gain the required energy for stable lattice distortion. The transition metal dichalcogenide 1T-VSe2 also undergoes such a transition at 110 K. Here, we present detailed angle-resolved photoemission spectroscopy experiments to investigate the electronic structure in 1T-VSe2 across the structural transition. Previously reported warping of the electronic structure and the energy shift of a secondary peak near the Fermi level as the origin of the charge density wave phase are shown to be temperature independent and hence cannot be attributed to the structural transition. Our work reveals new states that were not resolved in previous studies. Earlier results can be explained by the different dispersion natures of these states and temperature-induced broadening. Only the overall size of the Fermi surface is found to change across the structural transition. These observations, quite different from the charge density wave scenario commonly considered for 1T-VSe2 and other transition metal dichalcogenides, bring fresh perspectives toward correctly describing structural transitions. Therefore, these new results can be applied to material families in which the origin of the structural transition has not been resolved.

Reactivity of Ultrathin Kagome Metal FeSn toward Oxygen and Water.

The kagome metal FeSn consists of alternating layers of kagome-lattice Fe3Sn and honeycomb Sn2 and exhibits great potential for applications in future low-energy electronics and spintronics because of an ideal combination of topological phases and high-temperature magnetic ordering. Robust synthesis methods for ultrathin FeSn films, as well as an understanding of their air stability, are crucial for its development and long-term operation in future devices. In this work, we realize large-area, <10 nm thick, epitaxial FeSn thin films and explore the oxidation process via synchrotron-based photoelectron spectroscopy using in situ oxygen and water dosing, as well as ex situ air exposure. Upon exposure to the atmosphere, the FeSn films are shown to be highly reactive, with a stable ∼3 nm thick oxide layer forming at the surface within 10 min. Notably, the surface Fe remains largely unoxidized when compared with Sn, which undergoes near-complete oxidation. Additionally, the band structure remains metallic under oxygen exposure. These are further confirmed with controlled in situ dosing of O2 and H2O, where only the Sn2 (stanene) interlayers within the FeSn lattice oxidize, suggesting the Fe3Sn kagome layers remain almost pristine. These results are in excellent agreement with first-principles calculations, which show that Fe-O bonds to the Fe3Sn layer are energetically unfavorable and a large formation energy preference of 1.37 eV for Sn-O bonds in the stanene Sn2 layer over Sn-O bonds in the kagome Fe3Sn layer. The demonstration that oxidation only occurs within the stanene layers and the preservation of the Dirac bands may provide additional avenues in how to engineer, handle, and prepare future kagome metal devices.

Observation of Spin Splitting in Room-Temperature Metallic Antiferromagnet CrSb.

Recently, unconventional antiferromagnets that enable the spin splitting (SS) of electronic states have been theoretically proposed and experimentally realized, where the magnetic sublattices containing moments pointing at different directions are connected by a novel set of symmetries. Such SS is substantial, k-dependent, and independent of the spin-orbit coupling (SOC) strength, making these magnets promising materials for antiferromagnetic spintronics. Here, combined with angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, a systematic study on CrSb, a metallic spin-split antiferromagnet candidate with Néel temperature TN = 703 K, is conducted. The data reveal the electronic structure of CrSb along both out-of-plane and in-plane momentum directions, rendering an anisotropic k-dependent SS that agrees well with the calculational results. The magnitude of such SS reaches up to at least 0.8 eV at non-high-symmetry momentum points, which is significantly higher than the largest known SOC-induced SS. This compound expands the choice of materials in the field of antiferromagnetic spintronics and is likely to stimulate subsequent investigations of high-efficiency spintronic devices that are functional at room temperature.

Coincidence detection probability of(γ,2e)photoemission measurement.

In the study of strongly correlated electrons, one of the challenging core tasks is to develop the potential techniques for direct detection of the many-body correlations of strongly correlated electrons. The(γ,2e)photoemission technique has been developed to investigate the two-body correlations of the target correlated electrons. In this article, we will focus on this technique for the correlated electrons near the Fermi energy in condensed matter. The coincidence detection probability of the two emitted electrons in the(γ,2e)photoemission measurement is shown to be relevant to a two-body Bethe-Salpeter wave function, which describes the dynamical two-body correlations of the target correlated electrons near the Fermi energy. As the coincidence detection probability involves an electron-electron interaction matrix element, the arbitrary momentum and/or energy transfer due to this electron-electron interaction makes the(γ,2e)photoemission technique fail to reveal the inner-pair structures of the two-body Bethe-Salpeter wave function. However, the center-of-mass momentum and energy of the two-body Bethe-Salpeter wave function can be distinctly resolved. Thus, the(γ,2e)photoemission technique can provide the center-of-mass physics of the two-body correlations of the target correlated electrons. It will be one potential technique to study the center-of-mass physics of the Cooper pairs in superconductor.

Magnetotransport and angle-resolved photoemission spectroscopy of MnSb12Te19: a new member of MnSb2nTe3n+1family.

The quest for intrinsically ferromagnetic topological materials is a focal point in the study of topological phases of matter, as intrinsic ferromagnetism plays a vital role in realizing exotic properties such as the anomalous Hall effect (AHE) in quasi-two-dimensional materials, and this stands out as one of the most pressing concerns within the field. Here, we investigate a novel higher order member of the MnSb2nTe3n+1family, MnSb12Te19, for the first time combining magnetotransport and angle-resolved photoemission spectroscopy (ARPES) measurements. Our magnetic susceptibility experiments identify ferromagnetic transitions at temperatureTc= 18.7 K, consistent with our heat capacity measurements (T= 18.8 K). The AHE is observed for the field along thec-axis belowTc. Our study of Shubinikov-de-Haas oscillations provides evidence for Dirac fermions withπBerry phase. Our comprehensive investigation reveals that MnSb12Te19exhibits a FM ground state along with AHE, and hole-dominated transport properties consistent with ARPES measurements.

Coupling Between Electrons and Charge Density Wave Fluctuation and its Possible Role in Superconductivity.

In most charge density wave (CDW) systems of different material classes, ranging from traditional correlated systems in low-dimension to recent topological systems with Kagome lattice, superconductivity emerges when the system is driven toward the quantum critical point (QCP) of CDW via external parameters of doping and pressure. Despite this rather universal trend, the essential hinge between CDW and superconductivity has not been established yet. Here, the evidence of coupling between electron and CDW fluctuation is reported, based on a temperature- and intercalation-dependent kink in the angle-resolved photoemission spectra of 2H-PdxTaSe2. Kinks are observed only when the system is in the CDW phase, regardless of whether a long- or short-range order is established. Notably, the coupling strength is enhanced upon long-range CDW suppression, albeit the coupling energy scale is reduced. Interestingly, the estimation of the superconducting critical temperature by incorporating the observed coupling characteristics into McMillan's equation yields results closely resembling the known values of the superconducting dome. The results thus highlight a compelling possibility that this new coupling mediates Cooper pairs, which provides new insights into the competing relationship not only for CDW but also for other competing orders.

Quantum-Confined Lifshitz Transition on Weyl Semimetal Td-MoTe2.

Adsorption of alkali atoms onto material surfaces is widely utilized for controlling electronic properties and is particularly effective for two-dimensional materials. While tuning the chemical potential and band gap and creating quantum-confined states are well established for alkali adsorption on semiconductors, the effects on semimetallic systems remain largely elusive. Here, utilizing angle-resolved photoemission spectroscopy measurements and density functional theory calculations, we disclose the creation of two-dimensional electron gas and the quantum-confined Lifshitz transition at the surface of a Weyl semimetal Td-MoTe2 by potassium adsorption. Electrons from potassium adatoms are shown to be transferred mainly to the lowest unoccupied band within the gapped part of the Brillouin zone, which, in turn, induces strong surface band bending and quantum confinement in the topmost layer. The quantum-confined topmost layer evolves from a semimetal to a strong metal with a Lifshitz transition departing substantially from the bulk band. The present finding and its underlying mechanism can be exploited for the creation of electronic heterojunctions in van der Waals semimetals.

Graphene Intermediate Layer for Robust and Spectrum-Extended Cu Photocathode Activated with Cs and O.

Developing an effective method to stably enhance the quantum efficiency (QE) and extend the photoemission threshold of Cu photocathodes beyond the ultraviolet region could benefit the photoinjector for ultrafast electron source applications. The implementation of a 2D material protective layer is considered a promising approach to extending the operating lifetime of photocathodes. We propose that graphene can serve as an intermediate layer at the interface between photocathode material and low-work-function coating. The role of oxygen in the Cs/O activation process on the Cu surface is altered by the graphene interlayer. Besides, the few-layer graphene (FLG) surface could be more likely to induce the formation of Cs2O. Thus, the graphene-Cu composite photocathode can achieve an ultralow surface work function of down to 0.878 eV through Cs/O activation. The photoemission performance of the composite cathode with a FLG interlayer is significantly enhanced. The photocathode has an extended spectral response to the near-infrared region and a higher QE. At 350 nm, its QE is more than twice that of the cesiated bare Cu, reaching 0.247%. After degradation, the graphene-Cu cathode can be fully restored by reactivation, with remarkably enhanced stability. In addition, the composite cathode can be operated reliably under a poor vacuum pressure of over 4 × 10-6 Pa. This study validates a new method for incorporating 2D materials into photocathodes, offering novel approaches to explore robust and spectrum-extended photocathodes.

Versatile Method for Preparing Two-Dimensional Metal Dihalides.

Ever since the ground-breaking isolation of graphene, numerous two-dimensional (2D) materials have emerged with 2D metal dihalides gaining significant attention due to their intriguing electrical and magnetic properties. In this study, we introduce an innovative approach via anhydrous solvent-induced recrystallization of bulk powders to obtain crystals of metal dihalides (MX2, with M = Cu, Ni, Co and X = Br, Cl, I), which can be exfoliated to 2D flakes. We demonstrate the effectiveness of our method using CuBr2 as an example, which forms large layered crystals. We investigate the structural properties of both the bulk and 2D CuBr2 using X-ray diffraction, along with Raman scattering and optical spectroscopy, revealing its quasi-1D chain structure, which translates to distinct emission and scattering characteristics. Furthermore, microultraviolet photoemission spectroscopy and electronic transport reveal the electronic properties of CuBr2 flakes, including their valence band structure. We extend our methodology to other metal halides and assess the stability of the metal halide flakes in controlled environments. We show that optical contrast can be used to characterize the flake thicknesses for these materials. Our findings demonstrate the versatility and potential applications of the proposed methodology for preparing and studying 2D metal halide flakes.

Realization of Two-Dimensional Intrinsic Polar Metal in a Buckled Honeycomb Binary Lattice.

Structural topology and symmetry of a two-dimensional (2D) network play pivotal roles in defining its electrical properties and functionalities. Here, a binary buckled honeycomb lattice with C3v symmetry, which naturally hosts topological Dirac fermions and out-of-plane polarity, is proposed. It is successfully achieved in a group IV-V compound, namely monolayer SiP epitaxially grown on Ag(111) surface. Combining first-principles calculations with angle-resolved photoemission spectroscopy, the degeneration of the Dirac nodal lines to points due to the broken horizonal mirror symmetry is elucidated. More interesting, the SiP monolayer manifests metallic nature, which is mutually exclusive with polarity in conventional materials. It is further found that the out-of-plane polarity is strongly suppressed by the metallic substrate. This study not only represents a breakthrough of realizing intrinsic polarity in 2D metallic material via ingenious design but also provides a comprehensive understanding of the intricate interplay of many exotic low-dimensional quantum phenomena.

Light-induced insulator-metal transition in Sr2IrO4 reveals the nature of the insulating ground state.

Sr2IrO4 has attracted considerable attention due to its structural and electronic similarities to La2CuO4, the parent compound of high-Tc superconducting cuprates. It was proposed as a strong spin-orbit-coupled Jeff = 1/2 Mott insulator, but the Mott nature of its insulating ground state has not been conclusively established. Here, we use ultrafast laser pulses to realize an insulator-metal transition in Sr2IrO4 and probe the resulting dynamics using time- and angle-resolved photoemission spectroscopy. We observe a gap closure and the formation of weakly renormalized electronic bands in the gap region. Comparing these observations to the expected temperature and doping evolution of Mott gaps and Hubbard bands provides clear evidence that the insulating state does not originate from Mott correlations. We instead propose a correlated band insulator picture, where antiferromagnetic correlations play a key role in the gap opening. More broadly, our results demonstrate that energy-momentum-resolved nonequilibrium dynamics can be used to clarify the nature of equilibrium states in correlated materials.

Near-infrared detection based on the excitation of hot electrons in Au/Si microcone array.

Although the photoresponse cut-off wavelength of Si is about 1100 nm due to the Si bandgap energy, the internal photoemission effect (IPE) of the Au/Si junction in Schottky detector can extend the absorption wavelength, which makes it a promising candidate for the Si-based infrared detector. However, due to low light absorption, low photon-electron interaction, and poor electron injection efficiency, the near-infrared light detection efficiency of the Schottky detector is still insufficient. The synergistic effect of Si nano/microstructures with a strong light trapping effect and nanoscale Au films with surface plasmon enhanced absorption may provide an effective solution for improving the detection efficiency. In this paper, a large-area periodic Si microcone array covered by an Au film has successfully been fabricated by one-time dry etching based on the mature polystyrene microspheres lithography technique and vacuum thermal deposition, and its properties for hot electron-based near infrared photodetection are investigated. Optical measurements show that the 20 nm-thick Au covered Si microcone array exhibits a low reflectance and a strong absorption (about 85%) in wide wavelength range (900-2500 nm), and the detection responsivity can reach a value as high as 17.1 and 7.0 mA W-1at 1200 and 1310 nm under the front illumination, and 35.9 mA W-1at 1310 nm under the back illumination respectively. Three-dimensional finite difference time domain (3D-FDTD) simulation results show that the enhanced local electric field in the Au layer distributes near the air/Au interface under the front illumination and close to the Au/Si interface under the back illumination. The back illumination favors the injection of photo-generated hot electrons in Au layer into Si, which can explain the higher responsivity under the back illumination. Our research is expected to promote the practical application of Schottky photodetectors to Si-compatible near infrared photodetectors.

Dependence of Ultrafast Electron Emission Characteristics of Graphene Cold Cathode on Femtosecond Photoexcitation Polarization Angle.

Ultrafast electron pulses, generated through femtosecond photoexcitation in nanocathode materials, introduce high-frequency characteristics and ultrahigh temporal-spatial resolution to vacuum micro-nano electronic devices. To advance the development of ultrafast electron sources sensitive to polarized light, we propose an ultrafast pulsed electron source based on a vertical few-layer graphene cold cathode. This source exhibits selective electron emission properties for varying polarization angles, with high switching ratios of 277 (at 0°) and 235 (at 90°). The electron emission of the graphene evolves from cosine to sine as the polarization angle increases from 0° to 90°. The variation of electron emission current with polarization angle is intrinsically related to light absorption, local field enhancement, and photothermal conversion efficiency. A physical mechanism model and semiempirical expression were presented to reveal the MPP and PTE mechanisms at different polarization angles. This tunable conversion between mechanisms indicates potential applications in tunable ultrafast optoelectronic devices.

Inferior Interfacial Superconductivity in 1 UC FeSe/SrVO3/SrTiO3 with Screened Interfacial Electron-Phonon Coupling.

Single-unit cell (1 UC) FeSe interfaced with TiOx or FeOx exhibits significantly enhanced superconductivity compared to that of bulk FeSe, with interfacial electron-phonon coupling (EPC) playing a crucial role. However, the reduced dimensionality in 1 UC FeSe, which may drive superconducting fluctuations, complicates our understanding of the enhancement mechanisms. We construct a new superconducting interface, 1 UC FeSe/SrVO3/SrTiO3. Here, the itinerant electrons of highly metallic SrVO3 films can screen all high-energy Fuchs-Kliewer phonons, including those of SrTiO3, making it the first FeSe/oxide system with screened interfacial EPC while maintaining the 1 UC FeSe thickness. Despite comparable doping levels, the heavily electron-doped 1 UC FeSe/SrVO3 exhibits a pairing temperature (Tg ∼ 48 K) lower than those of FeSe/SrTiO3 and FeSe/LaFeO3. Our findings disentangle the contributions of interfacial EPC from dimensionality in terms of enhancing Tg in FeSe/oxide interfaces, underscoring the critical importance of interfacial EPC. This FeSe/VOx interface also provides a platform for studying interfacial superconductivity.

Realization of Honeycomb Tellurene with Topological Edge States.

The two-dimensional (2D) honeycomb lattice has attracted intensive research interest due to the appearance of Dirac-type band structures as the consequence of two sublattices in the honeycomb structure. Introducing strong spin-orbit coupling (SOC) leads to a gap opening at the Dirac point, transforming the honeycomb lattice into a 2D topological insulator as a platform for the quantum spin Hall effect (QSHE). In this work, we realize a 2D honeycomb-structured film with tellurium, the heaviest nonradioactive element in Group VI, namely, tellurene, via molecular beam epitaxy. We revealed the gap opening of 160 meV at the Dirac point due to the strong SOC in the honeycomb-structured tellurene by angle-resolved photoemission spectroscopy. The topological edge states of tellurene are detected via scanning tunneling microscopy/spectroscopy. These results demonstrate that tellurene is a novel 2D honeycomb lattice with strong SOC, and they unambiguously prove that tellurene is a promising candidate for a room-temperature QSHE system.

Antimony-Platinum Modulated Contact Enabling Majority Carrier Polarity Selection on a Monolayer Tungsten Diselenide Channel.

We develop a novel metal contact approach using an antimony (Sb)-platinum (Pt) bilayer to mitigate Fermi-level pinning in 2D transition metal dichalcogenide channels. This strategy allows for control over the transport polarity in monolayer WSe2 devices. By adjustment of the Sb interfacial layer thickness from 10 to 30 nm, the effective work function of the contact/WSe2 interface can be tuned from 4.42 eV (p-type) to 4.19 eV (n-type), enabling selectable n-/p-FET operation in enhancement mode. The shift in effective work function is linked to Sb-Se bond formation and an emerging n-doping effect. This work demonstrates high-performance n- and p-FETs with a single WSe2 channel through Sb-Pt contact modulation. After oxide encapsulation, the maximum current density at |VD| = 1 V reaches 170 µA/µm for p-FET and 165 µA/µm for n-FET. This approach shows promise for cost-effective CMOS transistor applications using a single channel material and metal contact scheme.

Enhanced Photoemission Performance of InGaN Inclined Nanowire Array.

We propose to improve the solar energy utilization by using InGaN inclined nanowire array photocathodes. We first study vertical nanowire array. On the basis of vertical nanowire array, we study inclined nanowires by changing the inclination angle of nanowires. The inclined nanowires exhibit higher quantum efficiency at larger period and larger inclination angle. However, the infinite expansion of period will cause its performance to degrade. The quantum efficiency of inclined nanowires with a period of 175 nm and an inclination angle of 5.35° is as high as 80.2% when the incident light angle is irradiated at 5°. In addition, applying an electric field can improve the collection efficiency of inclined nanowires and help them maintain a high collection efficiency over a longer wavelength range. The design principles proposed in this work will provide a theoretical reference for the performance improvement of InGaN photocathodes.

Quasi-Homoepitaxial Growth of Highly Strained Alkali-Metal Ultrathin Films on Kagome Superconductors.

Applying lattice strain to thin films, a critical factor to tailor their properties such as stabilizing a structural phase unstable at ambient pressure, generally necessitates heteroepitaxial growth to control the lattice mismatch with substrate. Therefore, while homoepitaxy, the growth of thin film on a substrate made of the same material, is a useful method to fabricate high-quality thin films, its application to studying strain-induced structural phases is limited. Contrary to this general belief, here the quasi-homoepitaxial growth of Cs and Rb thin films is reported with substantial in-plane compressive strain. This is achieved by utilizing the alkali-metal layer existing in bulk crystal of kagome metals AV3Sb5 (A = Cs and Rb) as a structural template. The angle-resolved photoemission spectroscopy measurements reveal the formation of metallic quantum well states and notable thickness-dependent quasiparticle lifetime. Comparison with density functional theory calculations suggests that the obtained thin films crystalize in the face-centered cubic structure, which is typically stable only under high pressure in bulk crystals. These findings provide a useful approach for synthesizing highly strained thin films by quasi-homoepitaxy, and pave the way for investigating many-body interactions in Fermi liquids with tunable dimensionality.

Emergence of two distinct phase transitions in monolayer CoSe2 on graphene.

Dimensional modifications play a crucial role in various applications, especially in the context of device miniaturization, giving rise to novel quantum phenomena. The many-body dynamics induced by dimensional modifications, including electron-electron, electron-phonon, electron-magnon and electron-plasmon coupling, are known to significantly affect the atomic and electronic properties of the materials. By reducing the dimensionality of orthorhombic CoSe2 and forming heterostructure with bilayer graphene using molecular beam epitaxy, we unveil the emergence of two types of phase transitions through angle-resolved photoemission spectroscopy and scanning tunneling microscopy measurements. We disclose that the 2 × 1 superstructure is associated with charge density wave induced by Fermi surface nesting, characterized by a transition temperature of 340 K. Additionally, another phase transition at temperature of 160 K based on temperature dependent gap evolution are observed with renormalized electronic structure induced by electron-boson coupling. These discoveries of the electronic and atomic modifications, influenced by electron-electron and electron-boson interactions, underscore that many-body physics play significant roles in understanding low-dimensional properties of non-van der Waals Co-chalcogenides and related heterostructures.

Electron Imaging of Nanoscale Charge Distributions Induced by Femtosecond Light Pulses.

Surface charging is ubiquitously observable during in situ transmission electron microscopy of nonconducting specimens as a result of electron beam/sample interactions or optical stimuli and often limits the achievable image stability and spatial or spectral resolution. Here, we report on the electron-optical imaging of surface charging on a nanostructured surface following femtosecond multiphoton photoemission. By quantitatively extracting the light-induced electrostatic potential and studying the charging dynamics on relevant time scales, we gain insights into the details of the multiphoton photoemission process in the presence of an electrostatic background field. We study the interaction of the charge distribution with the high-energy electron beam and secondary electrons and propose a simple model to describe the interplay of electron- and light-induced processes. In addition, we demonstrate how to mitigate sample charging by simultaneously optically illuminating the sample.