The study of processes concerning adsorption, diffusion and reaction of atoms and molecules on surfaces is one of the core areas of surface science research. Resolving these dynamic processes with atomic resolution in real space and at real time is of great significance for the understanding of catalytic reaction mechanism and the development of new materials. A scanning tunneling microscope with fast imaging function, a so-called “high-speed scanning tunneling microscope” combining both high temporal and high spatial resolution, is an ideal instrument to characterize processes within this area. This review aims to highlight some recent developments of high-speed scanning tunneling microscope technique and its application to study the structural dynamics on surfaces. Firstly, factors that limit the time resolution of scanning tunneling microscope are analyzed from the aspects of both hardware and software. Secondly, strategies and instrument designs enabling imaging rate up to 100 frames per second are introduced. Then, recent breakthroughs on resolving surface structural dynamics, such as atom diffusion, on-surface synthesis of low-dimensional materials and chemical reaction, by high-speed scanning tunneling microscope are highlighted. Finally, the challenges and opportunities of high-speed scanning tunneling microscope technique are outlined and a perspective is provided.

Many fundamental processes in nature occur on ultrashort time scales within picoseconds to attoseconds, and on intrinsic length scales from nanometers to picometers. The structure of crystalline solids is dictated by long range order and the periodic arrangement of atoms, but the elementary excitations that define its interaction with the environment may vary locally at the atomic scale. Multiple domains and phases can coexist on length scales down to a few nanometer, and impurities and defects can influence the collective many-body response of solids at the single-atom level. Ultrafast pump–probe techniques provide valuable information about fundamental many-body interactions in solids and at surfaces, but spatially average over macroscopic spot sizes such that the influence of local order or disorder at angstrom scales is not directly accessible. Therefore, real-space observation of ultrafast dynamics with atomic spatial resolution is highly desirable, and motivates the development of time-resolved ultrafast scanning tunneling microscopy (USTM) since the early 1990’s. Tremendous progress has been made in this field in the past decade, and a number of breakthrough achievements have significantly advanced our possibilities to add ultrafast time resolution to the angstrom spatial resolution of STM. This article reviews new technical approaches and developments in the field of USTM. A particular focus will be the classification of light-matter interaction in tunnel junctions, based on the criteria for adiabatic tunneling from Keldysh's theory of strong-field ionization and a tunneling time as defined by Büttiker and Landauer, and on Tucker's definition of quantum detection in a tunnel junction mixer. Moreover, various mechanisms to generate an ultrafast tunneling current in USTM are discussed and are to some extent related to those from other techniques such as optical spectroscopy or photoemission spectroscopy. The resulting new possibilities for imaging the ultrafast dynamics of electronic and vibrational excitations at surfaces with USTM will be highlighted. Finally, the article outlines possible future directions of USTM for studying ultrafast processes and light-induced phenomena at surfaces and in quantum materials.

Plasmons are self-sustained collective excitations of electron liquid, which have received increasing attention since its proposal by David Pines at 1960s. For the great potential in applications, the researches on plasmons make great advances all the way from semiconductors, metals, semimetals, to monolayer graphene. With the fast development of the field of topological materials, the research of plasmons has been extended into topological insulators, generating many exciting discoveries related to the topologically protected surface states. Topological semimetals, exhibiting various fantastic properties different from topological insulators, have become another research focus in condensed matter. Recently the plasmons in topological semimetals, providing a new perspective to further understand and utilize the topological states, have been attracting more and more attention. In this article, we review the recent theoretical and experimental investigations on the plasmons of topological semimetals, including the Dirac, Weyl and nodal line semimetals. In theoretical aspects, main different behaviors between the plasmons of topological semimetals and traditional metals are reviewed, such as the quantum nature, unusual dependence on temperature and charge carrier density, and the properties related to the chiral anomaly and Fermi arcs. The experimental studies are less reported, and the review is mainly focused on the measurements of optical conductivity and electron energy loss spectra in several typical real materials. Finally, the prospects of the future of the plasmons in topological semimetals in theories and experiments are outlooked.

With the development of laser and magneto-optical technology and the discovery of a broad range of magnetic quantum materials exhibiting exotic properties and new physics, ultrafast magnetization dynamics has become increasingly appealing to advanced magnetic information technology. Furthermore, manipulating magnetization via light provides insights into interactions among multiple degrees of freedom in condensed matters and has revealed a wide range of nonequilibrium phenomena. In this minireview, we first present the theoretical considerations of ultrafast magnetization dynamics from both classical and ab initio points of view. We then discuss several aspects of state-of-the-art experimental studies on light-induced magnetization dynamics in various materials, including ultrafast demagnetization and magnetization reversal, as well as coherent-phonon-driven magnetization precession and phase transitions. In particular, we highlight the role of light-induced phonons from some recent work in the latter two aspects, providing a completely new perspective as well as an alternative approach for optical control of magnetization dynamics. As a powerful means of dynamical control and thanks to the progress and advances of experimental techniques, all-optical quantum manipulation of emergent materials is becoming one of the most far-reaching frontier research areas of ultrafast sciences.

Light at optical frequencies interacting with a metal surface can excite interband quantum transitions, or intraband currents at frequencies approaching the PHz range. Momentum conservation enables the interband excitation to occur in first order as a dipole transition, while intraband excitations involve second-order momentum scattering processes. The free electron response to optical fields can also be collective, causing the optical field to be screened by the multipole plasmon response. We describe the exitation of single crystal silver surfaces in the region where the dielectric response transits from negative to positive passing through the epsilon near zero (ENZ) condition. There, electrons can no longer screen the optical field, so that it penetrates as a collective charge density wave of the free electron plasma, in other words, as a bulk transverse or longitudinal plasmon field. We examine two-photon photoemission (2PP) signals from Ag(111), (100) and (110) surfaces through the ENZ region under conditions where intraband, and interband single particle, and bulk plasmon collective responses dominate. We are specifically interested in the bulk plasmon decay into plasmonic photoemission. Plasmonic decay into excitation of electrons from the Fermi level, which we observe as a nonlinear 2PP process, has been established for the free electron and noble metals, but its significance to transduction of optical-to-electronic energy has not penetrated the plasmonics community. 2PP spectra show evidence for intraband hot electron generation, interband surface and bulk band excitation, and nonlinear bulk plasmon driven plasmonic single particle excitation. Because the intraband and plasmonic decay into hot electron distributions have been extensively considered in the literature, without reference to explicit experimental measurements, we discuss such processes in light of the directional anisotropy of the electronic structure of single crystalline silver. We note that projected band gaps in silver exclude large regions of the unoccupied state density from hot electron generation, such that it predominantly occurs in the (110) direction. Moreover, the excited hot electron distributions do not follow expectations from the joint density of the occupied and unoccupied states of a free electron metal, as assumed in majority of research on hot electron processes. We describe the strongly anisotropic hot electron distributions recorded by 2PP spectroscopy of Ag surfaces, and the plasmonic photoemission process that occurs on all surfaces irrespective of the momentum-dependent single particle band structure of silver. Plasmonic photoemission, or its linear analog that excites hot electrons at energies below the work function of Ag, is an important process for harvesting hot electron energy in photocatalytic and electronic device applications because the plasmon energy is not distributed between an electron and hole. This plasmonic decay channel is robust, but many aspects raise further questions. The accompanying publication by Gumhalter and Novko discusses the plasmonic photoemission from a theoretical point of view and its extension to Floquet engineering, as an exploration of novel plasmonic excitation processes in metals.

Recent high resolution multiphoton photoemission studies of low index Ag surfaces have revealed spectral features whose energetics was controlled by multiple quanta of plasmon energy rather than the photon energies appearing in the standard Einstein’s one-electron energy scaling in photoeffect. To elucidate these peculiar features we introduce and elaborate the mechanism of bulk- and surface plasmon-induced electron emission from metal surfaces, conveniently termed plasmoemission. Our point of departure is the cloud of hot plasmons generated in the primary interactions of external electromagnetic (EM) field(s) with the system. Such hot plasmon distributions acquire the form of a coherent state plasmonic bath which may serve as a source of energy and momentum required for electron emission from the system. These plasmoemission channels are complementary to the standard photoemission channels driven directly by the primary EM fields. Adopting this paradigm we analyze the plasmonically induced electron yield by using perturbative and nonperturbative approaches in the length and velocity gauge representations of the electron–plasmon interaction. Pursuing the perturbative approach to one- and two bulk plasmon-induced electron emission from Ag(110) surface we have investigated the effects of underlying band structure on the electron yield and proposed as how to discern them in the measured spectra. This also enables putting the perturbative descriptions of plasmoemission into the general context of pump–probe spectroscopy. The more demanding nonperturbative approach has been implemented by invoking the Volkov ansatz type of electron wavefunction in the velocity gauge and applied to surface plasmon-induced electron emission from quasi-two-dimensional surface bands on Ag(111). In this formulation the electrons emanate from the surface Floquet bands generated from the parent surface state band by the action of prepumped plasmonic coherent state field. A quantitative assessment of the multiplasmoemission yield is presented in terms of the plasmonic coherent state parameters controlled by the external pumping fields. The opposite limit of plasmonically induced electron tunneling regime is recovered in the quasistatic strong field limit. The pump–probe concept can be established also in the nonperturbative picture albeit in a more complex form.

The copper (Cu) source-drain electrodes based on copper–calcium (CuCa) diffusion barrier were fabricated without annealing process and in one wet etching step in order to develop the applications of Cu in hydrogenated amorphous silicon thin film transistor (α-Si:H TFT). The results show that oxygen flux and substrate temperature in depositing CuCa buffer layer affect greatly the adhesion of source-drain electrodes, and a perfect adhesion was obtained by an increasing oxygen flux to 4 sccm or an increasing substrate temperature to 150 °C, despite no annealing process. The specific resistance of source-drain electrodes has a slight increase with the increasing oxygen flux or substrate temperature or CuCa thickness. Auger electron spectroscopy (AES) show that the CuCa alloy barrier layer has perfect anti-diffusion between Cu film and α-Si:H. A much-desired taper angle of 43.4° and a little critical dimension (CD) bias of 0.91 μm for the Cu/CuCa electrodes were obtained in one wet etching step. The α-Si:H TFT with the Cu/CuCa source-drain electrodes demonstrated the field-effect mobility of 0.73 cm2/Vs, the subthreshold slope of 0.73 V/dec, the threshold voltage of 0.45 V, and the Ion/Ioff ratio of 106 due to the superior performances of the source-drain electrodes with the desired adhesion, specific resistance and taper angle despite no annealing process.

Electronic states in quantum materials can be engineered by light irradiation, which is greatly advanced by ab-initio computational predictions in realistic light-matter coupled systems. Here we review the most recent progresses from first principles computation in the light-driven Floquet steady states and transient dynamical states with topological electronic bands in real crystals. We first introduce the first-principles modeling approach, dubbed time-dependent Wannier scheme, for simulating real quantum materials under light irradiation. Then, we present a few examples of theoretically-predicted Floquet-Bloch electronic bands engineered by time-periodic light fields, which include the three types of Floquet-Dirac fermions in graphene and black phosphorus, the Floquet-Chern flat bands with an unprecedented high flatness ratio of band width over band gap in a Kagome material, and the Floquet conversion between bright and dark valley excitons in monolayer transition-metal dichalcogenides. Next, we show the ultrafast dynamical evolution of Weyl nodal points in orthorhombic WTe2 driven by a time-aperiodic short light pulse, and discuss the connection between the Floquet and transient states engineered by light. After that, we introduce three prominent experiments, inspired by theoretical predictions, on the light-induced topological Floquet electronic bands in quantum crystalline materials. Finally, we make a brief summary and perspective on the engineering of topological electronic states through light-matter interactions.

Borophene, a two-dimensional (2D) planar boron sheet, has attracted dramatic attention for its unique physical properties that are theoretically predicted to be different from those of bulk boron, such as polymorphism, superconductivity, Dirac fermions, mechanical flexibility and anisotropic metallicity. Nevertheless, it has long been difficult to obtain borophene experimentally due to its susceptibility to oxidation and the strong covalent bonds in bulk forms. With the development of growth technology in ultra-high vacuum (UHV), borophene has been successfully synthesized by molecular beam epitaxy (MBE) supported by substrates in recent years. Due to the intrinsic polymorphism of borophene, the choice of substrates in the synthesis of borophene is pivotal to the atomic structure of borophene. The different interactions and commensuration of borophene on various substrates can induce various allotropes of borophene with distinct atomic structures, which suggests a potential approach to explore and manipulate the structure of borophene and benefits the realization of novel physical and chemical properties in borophene due to the structure–property correspondence. In this review, we summarize the recent research progress in the synthesis of monolayer (ML) borophene on various substrates, including Ag(111), Ag(110), Ag(100), Cu(111), Cu(100), Au(111), Al(111) and Ir(111), in which the polymorphism of borophene is present. Moreover, we introduce the realization of bilayer (BL) borophene on Ag(111), Cu(111) and Ru(0001) surfaces, which possess richer electronic properties, including better thermal stability and oxidation resistance. Then, the stabilization mechanism of polymorphic borophene on their substrates is discussed. In addition, experimental investigations on the unique physical properties of borophene are also introduced, including metallicity, topology, superconductivity, optical and mechanical properties. Finally, we present an outlook on the challenges and prospects for the synthesis and potential applications of borophene.

Quantum coherent physics and chemistry concern the creation and manipulation of an excited-state manifold that contains the superposition and entanglement of multiple quantum levels. Electromagnetic waves such as light and microwave can be used to generate and probe different quantum coherent phenomena. The recent advances in scanning tunneling microscopy (STM) techniques including ultrafast laser coupled STM and electron spin resonance STM combine electromagnetic excitation with tunneling electron detection, bringing the investigation of quantum coherence down to the atomic and molecular level. Here, we survey the latest STM studies of different quantum coherent phenomena covering molecular vibration, electron transfer, surface plasmon resonance, phonon, spin oscillation, and electronic transition, and discuss the state and promise of characterizing and manipulating quantum coherence at the atomic or molecular scale.