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SnSe, an environmental-friendly group-IV monochalcogenide semiconductor, demonstrates outstanding performance in various applications ranging from thermoelectric devices to solar energy harvesting. Its ultrathin films show promise in the fabrication of ferroelectric nonvolatile devices. However, the microscopic identification and manipulation of point defects in ultrathin SnSe single crystalline films, which significantly impact their electronic structure, have been inadequately studied. This study presents a comprehensive investigation of point defects in monolayer SnSe films grown via molecular beam epitaxy. By combining scanning tunneling microscopy (STM) characterization with first-principles calculations, we identified four types of atomic/molecular vacancies, four types of atomic substitutions, and three types of extrinsic defects. Notably, we have demonstrated the ability to convert a substitutional defect into a vacancy and to reposition an adsorbate by manipulating a single atom or molecule using an STM tip. We have also analyzed the local atomic displacement induced by the vacancies. This work provides a solid foundation for engineering the electronic structure of future SnSe-based nanodevices.

Colloidal quantum dots display remarkable optical and electrical characteristics with the potential for extensive applications in contemporary nanotechnology. As an ideal instrument for examining surface topography and local density of states (LDOS) at an atomic scale, scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) has become indispensable approaches to gain better understanding of their physical properties. This article presents a comprehensive review of the research advancements in measuring the electronic orbits and corresponding energy levels of colloidal quantum dots in various systems using STM and STS. The first three sections introduce the basic principles of colloidal quantum dots synthesis and the fundamental methodology of STM research on quantum dots. The fourth section explores the latest progress in the application of STM for colloidal quantum dot studies. Finally, a summary and prospective is presented., (© 2023 The Chemical Society of Japan & Wiley-VCH GmbH.)

Recent advances in inverse-design approaches for discovering optical structures based on desired functional characteristics have reshaped the landscape of nanophotonic structures, where most studies have focused on how light interacts with nanophotonic structures only. When quantum emitters (QEs), such as atoms, molecules, and quantum dots, are introduced to couple to the nanophotonic structures, the light-matter interactions become much more complicated, forming a rapidly developing field - quantum nanophotonics. Typical quantum functional characteristics depend on the intrinsic properties of the QE and its electromagnetic environment created by the nanophotonic structures, commonly represented by a scalar quantity, local-density-of-states (LDOS). In this work, we introduce a generalized inverse-design framework in quantum nanophotonics by taking LDOS as the bridge to connect the nanophotonic structures and the quantum functional characteristics. We take a simple system consisting of QEs sitting on a single multilayer shell-metal-nanoparticle (SMNP) as an example, apply fully-connected neural networks to model the LDOS of SMNP, inversely design and optimize the geometry of the SMNP based on LDOS, and realize desirable quantum characteristics in two quantum nanophotonic problems: spontaneous emission and entanglement. Our work introduces deep learning to the quantum optics domain for advancing quantum device designs; and provides a new platform for practicing deep learning to design nanophotonic structures for complex problems without a direct link between structures and functional characteristics., (© 2023 the author(s), published by De Gruyter, Berlin/Boston.)

The electronic properties of the surface of β -FeSi 2 have been debated for a long. We studied the surface states of β -FeSi 2 films grown on Si(001) substrates using scanning tunnelling microscopy (STM) and spectroscopy (STS), with the aid of density functional theory calculations. STM simulations using the surface model proposed by Romanyuk et al (2014 Phys. Rev. B 90 155305) reproduce the detailed features of experimental STM images. The result of STS showed metallic surface states in accordance with theoretical predictions. The Fermi level was pinned by a surface state that appeared in the bulk band gap of the β -FeSi 2 film, irrespective of the polarity of the substrate. We also observed negative differential conductance at ∼0.45 eV above the Fermi level in STS measurements performed at 4.5 K, reflecting the presence of an energy gap in the unoccupied surface states of β -FeSi 2 ., (© 2023 IOP Publishing Ltd.)

The electromagnetic local density of states (LDOS) is crucial to many aspects of photonics engineering, from enhancing emission of photon sources to radiative heat transfer and photovoltaics. We present a framework for evaluating upper bounds on the LDOS in structured media that can handle arbitrary bandwidths and accounts for critical wave scattering effects. The bounds are solely determined by the bandwidth, material susceptibility, and device footprint, with no assumptions on geometry. We derive an analytical expression for the maximum LDOS consistent with the conservation of energy across the entire design domain, which upon benchmarking with topology-optimized structures is shown to be nearly tight for large devices. Novel scaling laws for maximum LDOS enhancement are found: the bounds saturate to a finite value with increasing susceptibility and scale as the quartic root of the bandwidth for semi-infinite structures made of lossy materials, with direct implications on material selection and design applications., (© 2022 the author(s), published by De Gruyter, Berlin/Boston.)

Mismatch between adjacent atomic layers in low-dimensional materials, generating moiré patterns, has recently emerged as a suitable method to tune electronic properties by inducing strong electron correlations and generating novel phenomena. Beyond graphene, van der Waals structures such as three-dimensional (3D) topological insulators (TIs) appear as ideal candidates for the study of these phenomena due to the weak coupling between layers. Here we discover and investigate the origin of 1D moiré stripes on the surface of Bi 2 Se 3 TI thin films and nanobelts. Scanning tunneling microscopy and high-resolution transmission electron microscopy reveal a unidirectional strained top layer, in the range 14-25%, with respect to the relaxed bulk structure, which cannot be ascribed to the mismatch with the substrate lattice but rather to strain induced by a specific growth mechanism. The 1D stripes are characterized by a spatial modulation of the local density of states, which is strongly enhanced compared to the bulk system. Density functional theory calculations confirm the experimental findings, showing that the TI surface Dirac cone is preserved in the 1D moiré stripes, as expected from the topology, though with a heavily renormalized Fermi velocity that also changes between the top and valley of the stripes. The strongly enhanced density of surface states in the TI 1D moiré superstructure can be instrumental in promoting strong correlations in the topological surface states, which can be responsible for surface magnetism and topological superconductivity.

Dissipation, often associated with plasmons, leads to decoherence and is generally considered fatal for quantum nonlinearities and entanglement. Counterintuitively, by introducing a dissipative plasmonic nanoantenna into a typical cavity quantum electrodynamics (QED) system, we unveil the wide existence of the atom-photon quasi-bound state (qBS), a kind of exotic eigenstate with anomalously small decay, in the hybrid plasmonic-photonic cavity. To derive the analytical condition of atom-photon qBS, we formulate a quantized two-mode model of the local density of states by connecting the interacting uncoupled cavity modes to the macroscopic QED. With resonant plasmon-photon coupling, we showcase the single-atom qBS that improves the efficiency of single-photon generation over one order of magnitude; and the two-atom qBS that significantly enhances spontaneous entanglement generation compared with a bare photonic cavity. Notably, such single-atom and multi-atom qBS can be simultaneously accessed in realistic plasmonic-photonic cavities, providing a versatile platform for advanced quantum technologies, such as quantum light sources, quantum computation, and quantum information., (© 2022 Yu-Wei Lu et al., published by De Gruyter, Berlin/Boston.)

Probing light-matter interaction at the nanometer scale is one of the most fascinating topics of modern optics. Its importance is underlined by the large span of fields in which such accurate knowledge of light-matter interaction is needed, namely nanophotonics, quantum electrodynamics, atomic physics, biosensing, quantum computing and many more. Increasing innovations in the field of microscopy in the last decade have pushed the ability of observing such phenomena across multiple length scales, from micrometers to nanometers. In bioimaging, the advent of super-resolution single-molecule localization microscopy (SMLM) has opened a completely new perspective for the study and understanding of molecular mechanisms, with unprecedented resolution, which take place inside the cell. Since then, the field of SMLM has been continuously improving, shifting from an initial drive for pushing technological limitations to the acquisition of new knowledge. Interestingly, such developments have become also of great interest for the study of light-matter interaction in nanostructured materials, either dielectric, metallic, or hybrid metallic-dielectric. The purpose of this review is to summarize the recent advances in the field of nanophotonics that have leveraged SMLM, and conversely to show how some concepts commonly used in nanophotonics can benefit the development of new microscopy techniques for biophysics. To this aim, we will first introduce the basic concepts of SMLM and the observables that can be measured. Then, we will link them with their corresponding physical quantities of interest in biophysics and nanophotonics and we will describe state-of-the-art experiments that apply SMLM to nanophotonics. The problem of localization artifacts due to the interaction of the fluorescent emitter with a resonant medium and possible solutions will be also discussed. Then, we will show how the interaction of fluorescent emitters with plasmonic structures can be successfully employed in biology for cell profiling and membrane organization studies. We present an outlook on emerging research directions enabled by the synergy of localization microscopy and nanophotonics., (© 2021 A. Femius Koenderink et al., published by De Gruyter, Berlin/Boston.)

Optical nanoantennas are well-known for the confinement of light into nanoscale hot spots, suitable for emission enhancement and sensing applications. Here, we show how control of the antenna dimensions allows tuning the local optical phase, hence turning a hot spot into a cold spot. We manipulate the local intensity exploiting the interference between driving and scattered field. Using single molecules as local detectors, we experimentally show the creation of subwavelength pockets with full suppression of the driving field. Remarkably, together with the cold excitation spots, we observe inhibition of emission by the phase-tuned nanoantenna. The fluorescence lifetime of a molecule scanned in such volumes becomes longer, showing slow down of spontaneous decay. In conclusion, the spatial phase of a nanoantenna is a powerful knob to tune between enhancement and inhibition in a 3-dimensional subwavelength volume.

Plasmonic nanostructures dramatically alter the radiative and nonradiative properties of single molecules in their vicinity. This coupling-induced change in decay channels selectively enhances specific vibronic transitions, which can enable plasmonic control of molecular reactivity. Here, we report coupling-dependent spectral emission shaping of single Rhodamine 800 molecules in the vicinity of plasmonic gold nanorods. We show that the relative vibronic transition rates of the first two vibronic transitions of the spontaneous emission spectrum can be tuned in the weak coupling regime, by approximately 25-fold, on the single molecule level.

The use of immobilization methods to treat radioactive nuclear waste liquid is one of the most effective ways for preventing radioactive contamination. Understanding the solidification matrix for the immobilization behavior of radioactive ions is ​​an important issue. In this work, ab initio calculation was used to study the solidification mechanism of Cs + in K-struvite crystal in the aqueous solution. Corresponding experiments were carried out and analyzed by XRF 1 , XPS 2 , AAS 3 , FI-IR 4 , SEM 5 , EDS 6 and XRD 7 . This work proposed a calculation method for the ΔE aq 8 . By analyzing ΔE aq , the tendency of Cs + to occupy the K site in K-struvite crystal is remarkable. Furthermore, in-depth first-principles calculations show that this immobilization behavior is related to the electronic structures of K-struvite and Cs-struvite 9 , and they together with the interaction of cation and aqueous solution determine the energy change of the process. This work provides a basic perspective for the study of magnesium phosphate potassium cement solidified nuclides, which is convenient for judging the solidification of other nuclide ions, thereby designing K-struvite cement for solidified nuclide. This method is also readily extended to other studies of the chemical immobilization of any crystal in the solution to any other ions., (Copyright © 2019. Published by Elsevier B.V.)

The desire to improve human lives has led to striking development in biosensing technologies. While the ongoing research efforts are mostly dedicated to enhancing speed and sensitivity of the sensor, a third consideration that has become increasingly important is compactness, which is strongly desired in emergency situations and personal health management. Surface plasmon resonance imaging (SPRi) is one of the few techniques that can potentially fulfill all the three goals, considering its multiplexed assay capability. However, miniaturizing SPRi biosensors remains elusive as it entails complicated optical gears. Here, we significantly slim the architecture of SPRi devices by visualizing the varied local density of states around analytes. The unusual detection scheme is realized by building a gain-assisted SPRi with InGaN quantum wells (QWs), where the QW-plasmon coupling efficiency hinges on localized refractive index variation. This new modality abolishes the prism, the polarizer, and the beam-tracking components in the most used Kretschmann configuration without compromising the performances.

Many applications in (quantum) nanophotonics rely on controlling light-matter interaction through strong, nanoscale modification of the local density of states (LDOS). All-optical techniques probing emission dynamics in active media are commonly used to measure the LDOS and benchmark experimental performance against theoretical predictions. However, metal coatings needed to obtain strong LDOS modifications in, for instance, nanocavities, are incompatible with all-optical characterization. So far, no reliable method exists to validate theoretical predictions. Here, we use subnanosecond pulses of focused electrons to penetrate the metal and excite a buried active medium at precisely defined locations inside subwavelength resonant nanocavities. We reveal the spatial layout of the spontaneous-emission decay dynamics inside the cavities with deep-subwavelength detail, directly mapping the LDOS. We show that emission enhancement converts to inhibition despite an increased number of modes, emphasizing the critical role of optimal emitter location. Our approach yields fundamental insight in dynamics at deep-subwavelength scales for a wide range of nano-optical systems.

The controlled fabrication of nanostructures has often used a substrate template to mediate and control the growth kinetics. Electronic substrate-mediated interactions have been demonstrated to guide the assembly of organic molecules or the nucleation of metal atoms but usually at cryogenic temperatures, where the diffusion has been limited. Combining STM, STS, and DFT studies, we report that the strong electronic interaction between transition metals and oxides could indeed govern the growth of low-dimensional oxide nanostructures. As a demonstration, a series of FeO triangles, which are of the same structure and electronic properties but with different sizes (side length >3 nm), are synthesized on Pt(111). The strong interfacial interaction confines the growth of FeO nanostructures, leading to a discrete size distribution and a uniform step structure. Given the same interfacial configuration, as-grown FeO nanostructures not only expose identical edge/surface structure but also exhibit the same electronic properties, as manifested by the local density of states and local work functions. We expect the interfacial confinement effect can be generally applied to control the growth of oxide nanostructures on transition metal surfaces. These oxide nanostructures of the same structure and electronic properties are excellent models for studies of nanoscale effects and applications.