Inherent symmetries of a system lead to multiple degeneracies of its energy spectra. Introducing individual atomic impurities can locally break these symmetries, which is expected to lift the degenerate degrees of freedom around the impurities. Although central to our understanding of the fundamental properties of solids, the broken-symmetry states induced by individual atomic impurities have so far eluded observation. Here, we report nanoscale probing of the broken-symmetry states in graphene induced by two types of individual atomic impurities, i.e., isolated nitrogen dopants and isolated hydrogen atoms chemisorbed on graphene. Our experiments demonstrate that both types of atomic impurities can locally break sublattice symmetry of graphene and generate valley-polarized states, which extends several nanometers around the impurities. For the isolated hydrogen atom chemisorbed on graphene, the enhanced spin-orbit coupling, which arises from the sp3 distortion of graphene due to the hydrogen chemisorption, further lifts the spin degeneracy, resulting in a fully spin and valley polarized states within about 1 nm around the hydrogen atom. Our result paves the way to control various broken-symmetry states at the nanoscale by various atomic impurities.
A universal challenge facing the development of electrochemical materials is our lack of understanding of physical and chemical processes at local length scales in 10-100 nm regime, and acquiring this understanding requires a new generation of imaging techniques. In this article, we introduce the scanning thermo-ionic microscopy (STIM) for probing local electrochemistry at the nanoscale, using for imaging the Vegard strain induced via thermal stress excitations. Since ionic oscillation is driven by the stress instead of voltage, the responses are insensitive to the electromechanical, electrost…
Quantum dots exhibit reproducible conductance fluctuations at low temperatures due to electron quantum interference. The sensitivity of these fluctuations to the underlying disorder potential has only recently been fully realized. We exploit this sensitivity to obtain a novel tool for better understanding the role that background impurities play in the electrical properties of high-mobility AlGaAs/GaAs heterostructures and nanoscale devices. In particular, we report the remarkable ability to first alter the disorder potential in an undoped AlGaAs/GaAs heterostructure by optical illumination an…
We use confocal Raman microscopy and modified vector analysis methods to investigate the nanoscale origin of strain and carrier concentration in exfoliated graphene-hexagonal boron nitride (hBN) heterostructures on silicon dioxide (SiO2). Two types of heterostructures are studied: graphene on SiO2 partially coved by hBN, and graphene fully encapsulated between two hBN flakes. We extend the vector analysis methods to produce spatial maps of the strain and doping variation across the heterostructures. This allows us to visualise and directly quantify the much-speculated effect of the environment…
A precise definition for a quantum electron thermometer is given, as an electron reservoir coupled locally (e.g., by tunneling) to a sample, and brought into electrical and thermal equilibrium with it. A realistic model of a scanning thermal microscope with atomic resolution is then developed, where the resolution is limited in ultrahigh vacuum by thermal coupling to the electromagnetic environment. We show that the temperatures of individual atomic orbitals or bonds in a conjugated molecule with a temperature gradient across it exhibit quantum oscillations, whose origin can be traced to a rea…
Phosphorene is an anisotropic puckered two-dimensional ($2$D) hexagonal lattice of phosphorus atoms. The edge modes in a zigzag phosphorene nanoribbon (ZPNR) are quasi-flat in nature and fully isolated from the bulk states, which are unique in comparison to the other hexagonal lattices like graphene, silicene etc. We theoretically investigate the Ruderman-Kittel-Kasuya-Yosida (RKKY) exchange interaction between two magnetic impurities placed on the nanoribbon, and extract the signatures of the flat edge states via the behavior of it. Due to the complete separation of the edge states from the b…
Surface phonon polaritons hold much potential for subwavelength control and manipulation of light at the infrared to terahertz wavelengths. Here, aided by monochromatic scanning transmission electron microscopy - electron energy loss spectroscopy technique, we study the excitation of optical phonon modes in SiC nanorods. Surface phonon polaritons are modulated by the geometry and size of SiC nanorods. In particular, we study the dispersion relation, spatial dependence and geometry and size effects of surface phonon polaritons. These experimental results are in agreement with dielectric respons…
We propose a method to probe and control the interactions between an ensemble of magnetic impurities in a superconductor via microwave radiation. Our method relies upon the presence of sub-gap Yu-Shiba-Rusinov (YSR) states associated with the impurities. Depending on the sign of the detuning, radiation generates either a ferro- or antiferromagnetic contribution to the exchange interaction. This contribution can bias the statistics of the random exchange constants stemming from the RKKY interaction. Moreover, by measuring the microwave response at the YSR resonance, one gains information about …
We show how impurity atoms can measure moments of ultracold atomic gas densities, using the example of bosons in a one-dimensional lattice. This builds on a body of work regarding the probing of systems by measuring the dephasing of an immersed qubit. We show this dephasing is captured by a function resembling characteristic functions of probability theory, of which the derivatives at short times reveal moments of the system operator to which the qubit couples. For a qubit formed by an impurity atom, in a system of ultracold atoms, this operator can be the density of the system at the location…
The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction (U-CBED) with a nanoscale probe beam for the quantitative retrieval of the time-dependent local distortion tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformation…
Nanoscale devices are being extensively studied for their tunable electronic and optical properties, but the influence of impurities and defects is amplified at these length scales and can lead to poorly understood variations in characteristics of semiconducting materials. By performing a large ensemble of photoconductivity measurements in nanogaps bridged by core-shell CdSe/ZnS semiconductor nanocrystals, we discover optoelectronic methods for affecting solid-state charge trap populations. We introduce a model that unifies previous work and transforms the problem of irreproducibility in nanoc…
Nuclear spin-lattice relaxation times are measured on copper using magnetic resonance force microscopy performed at temperatures down to 42 mK. The low temperature is verified by comparison with the Korringa relation. Measuring spin-lattice relaxation times locally at very low temperatures opens up the possibility to measure the magnetic properties of inhomogeneous electron systems realized in oxide interfaces, topological insulators and other strongly correlated electron systems such as high-Tc superconductors.
Understanding the dynamics of molecules adsorbed to surfaces or confined to small volumes is a matter of increasing scientific and technological importance. Here, we demonstrate a pulse protocol using individual paramagnetic nitrogen vacancy (NV) centers in diamond to observe the time evolution of 1H spins from organic molecules located a few nanometers from the diamond surface. The protocol records temporal correlations among the interacting 1H spins, and thus is sensitive to the local system dynamics via its impact on the nuclear spin relaxation and interaction with the NV. We are able to ga…
Using the density functional theory, we perform a full atomic relaxation of the bulk ferrite with 12.5%-concentration of monoatomic interstitial Cr periodically located at the edges of the bcc Fe$_α$ cell. We show that structural relaxation in such artificially engineered alloys leads to significant atomic displacements and results in the formation of novel highly stable configurations with parallel chains of octahedrically arranged Fe. The enhanced magnetic polarization in the low-symmetry metallic state of this type of alloys can be externally controlled by additional inclusion of nonmagneti…
Manipulating materials at the nanometer scale is challenging, particularly if alignment with nanoscale electrodes is desired. Here we describe a lithography-free, self-aligned nanotrench ablation (SANTA) technique to create nanoscale trenches in a polymer like poly(methyl) methacrylate (PMMA). The nanotrenches are self-aligned with carbon nanotube (CNT) and graphene ribbon electrodes through a simple Joule heating process. Using simulations and experiments we investigate how the Joule power, ambient temperature, PMMA thickness, and substrate properties can improve the spatial resolution of thi…
Thermal properties have an outsized impact on efficiency and sensitivity of devices with nanoscale structures, such as in integrated electronic circuits. A number of thermal conductivity measurements for semiconductor nanostructures exist, but are hindered by the diffraction limit of light, the need for transducer layers, the slow-scan rate of probes, ultra-thin sample requirements, or extensive fabrication. Here, we overcome these limitations by extracting temperature from measurements of bandgap cathodoluminescence in GaN nanowires with spatial resolution limited by the electron cascade, and…
While imaging individual atoms can routinely be achieved in high resolution transmission electron microscopy, visualizing the potential distribution of individually charged adsorbates leading to a phase shift of the probing electron wave is still a challenging task. Low-energy electrons (30 - 250 eV) are sensitive to localized potential gradients. We employed low-energy electron holography to acquire in-line holograms of individual charged impurities on free-standing graphene. By applying an iterative phase retrieval reconstruction routine we recover the potential distribution of the localized…
We have measured in gold wires the energy exchange rate between quasiparticles, the phase coherence time of quasiparticles and the resistance vs. temperature, in order to probe the interaction processes which are relevant at low temperatures. We find that the energy exchange rate is higher than expected from the theory of electron-electron interactions, and that it has a different energy dependence. The dephasing time is constant at temperatures between 8 K and 0.5 K, and it increases below 0.5 K. The magnetoresistance is negative at large field scales, and the resistance decreases logarithmic…
The recent discovery of ferromagnetism in 2D van der Waals (vdw) crystals has generated widespread interest, owing to their potential for fundamental and applied research. Advancing the understanding and applications of vdw magnets requires methods to quantitatively probe their magnetic properties on the nanoscale. Here, we report the study of atomically thin crystals of the vdw magnet CrI$_3$ down to individual monolayers using scanning single-spin magnetometry, and demonstrate quantitative, nanoscale imaging of magnetisation, localised defects and magnetic domains. We determine the magnetisa…
Sensitive nanoscale magnetic resonance imaging (MRI) of target spins using nitrogen-vacancy (NV) centers in diamond will require a quantitative understanding of dominant noise at the surface. We probe this noise by applying dynamical decoupling to shallow NVs at calibrated depths. Results support a model of NV dephasing by a surface bath of electronic spins having a correlation rate of 200 kHz, much faster than that of the bulk N spin bath. Our method of combining nitrogen delta-doping growth and nanoscale depth imaging paves a way for studying spin noise present in diverse material surfaces.
Graphene with high carrier mobility μ is required both for graphene-based electronic devices and for the investigation of the fundamental properties of graphene's Dirac fermions. It is largely accepted that the mobility-limiting factor in graphene is the Coulomb scattering off of charged impurities that reside either on graphene or in the underlying substrate. This is true both for traditional graphene devices on SiO2 substrates and possibly for the recently reported high-mobility suspended and supported devices. An attractive approach to reduce such scattering is to place graphene in an envir…
A novel mechanical approach is developed to explore by means of atom-scale simulation the concept of line tension at a solid-liquid-vapor contact line as well as its dependence on temperature, confinement, and solid/fluid interactions. More precisely, by estimating the stresses exerted along and normal to a straight contact line formed within a partially wet pore, the line tension can be estimated while avoiding the pitfalls inherent to the geometrical scaling methodology based on hemispherical drops. The line tension for Lennard-Jones fluids is found to follow a generic behavior with temperat…
We investigate electron transport across a complex oxide heterointerface of La$_{0.67}$Sr$_{0.33}$MnO$_3$ (LSMO) on Nb:SrTiO$_3$ (Nb:STO) at different temperatures. For this, we employ the conventional current-voltage method as well as the technique of Ballistic Electron Emission Microscopy (BEEM), which can probe lateral inhomogeneities in transport at the nanometer scale. From current-voltage measurements, we find that the Schottky Barrier height (SBH) at the LSMO/Nb:STO interface decreases at low temperatures accompanied by a larger than unity ideality factor. This is ascribed to the tunnel…
Understanding the coordination of cell division timing is one of the outstanding questions in the field of developmental biology. One active control parameter of the cell cycle duration is temperature, as it can accelerate or decelerate the rate of biochemical reactions. However, controlled experiments at the cellular-scale are challenging due to the limited availability of biocompatible temperature sensors as well as the lack of practical methods to systematically control local temperatures and cellular dynamics. Here, we demonstrate a method to probe and control the cell division timing in C…
Probing two-dimensional single-layer quantum magnets remains a significant challenge. In this letter, we propose exploiting tunneling spectroscopy in the presence of magnetic impurities to obtain information about the magnon dispersion relations in analogy to quasiparticle interference in non-magnetic materials. We show this technique can be used to establish the dispersion relations even for frustrated magnets, where the presence of an impurity generally leads to a nontrivial spin texture. Finally, we consider the problem of establishing Chern magnon bands in 2D magnets showing how tuneable i…
Quantum spin Hall (QSH) insulators have unique electronic properties, comprising a band gap in their two-dimensional interior and one-dimensional spin-polarized edge states in which current flows ballistically. In scanning tunneling microscopy (STM), the edge states manifest themselves as a localized density of states. However, there is a significant research gap between the observation of edge states in nanoscale spectroscopy, and the detection of ballistic transport in edge channels which typically relies on transport experiments with microscale lithographic contacts. Here, we study few-laye…
Obtaining conductance spectra for a concentration of disordered impurities distributed over a nanoscale device with sensing capabilities is a well-defined problem. However, to do this inversely, i.e., extracting information about the scatters from the conductance spectrum alone, is not an easy task. In the presence of impurities, even advanced techniques of inversion can become particularly challenging. This article extends the applicability of a methodology we proposed capable of extracting composition information about a nanoscale sensing device using the conductance spectrum. The inversion …
We investigate single Fe and Co atoms buried below a Cu(100) surface using low temperature scanning tunneling spectroscopy. By mapping the local density of states of the itinerant electrons at the surface, the Kondo resonance near the Fermi energy is analyzed. Probing bulk impurities in this well-defined scattering geometry allows separating the physics of the Kondo system and the measuring process. The line shape of the Kondo signature shows an oscillatory behavior as a function of depth of the impurity as well as a function of lateral distance. The oscillation period along the different dire…
The plasmon modes of pristine and impurity doped graphene are calculated, using a real-space theory which determines the non-local dielectric response within the random phase approximation. A full diagonalization of the polarization operator is performed, allowing the extraction of all its poles. It is demonstrated how impurities induce the formation of localized modes which are absent in pristine graphene. The dependence of the spatial modulations over few lattice sites and frequencies of the localized plasmons on the electronic filling and impurity strength is discussed. Furthermore, it is s…
We consider non-interacting multi-qubit systems as controllable probes of an environment of defects/impurities modelled as a composite spin-boson environment. The spin-boson environment consists of a small number of quantum-coherent two-level fluctuators (TLFs) damped by independent bosonic baths. A master equation of the Lindblad form is derived for the probe-plus-TLF system. We discuss how correlation measurements in the probe system encode information about the environment structure and could be exploited to efficiently discriminate between different experimental preparation techniques, wit…
Probing the wave-vector gap in nanoscale magnonics
CEITEC BUT, Brno University of Technology（布尔诺理工大学 CEITEC）；Department of Materials Science and Engineering, Massachusetts Institute of Technology（麻省理工学院材料科学与工程系）；Institute of Photonics and Quantum Sciences, SUPA, Heriot-Watt University（赫瑞-瓦特大学光子与量子科学研究所）；Department of Quantum Nanoscience, Kavli Institute of Nanoscience, Delft University of Technology（代尔夫特理工大学量子纳米科学系卡弗里纳米科学研究所）；Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy（马克斯·玻恩非线性光学和短脉冲光谱研究所）；Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；Department of Chemistry, Massachusetts Institute of Technology（麻省理工学院化学系）
Nanoscale materials usually can trap light and strongly interact with it leading to many photonic device applications. The light-matter interactions are commonly probed by optical spectroscopy, which, however, have some limitations such as diffraction-limited spatial resolution, tiny momentum transfer and non-continuous excitation/detection. In this work, using scanning transmission electron microscopy-electron energy loss spectroscopy (STEM-EELS) with ultra-wide energy and momentum match and sub-nanometer spatial resolution, we study the optical microcavity resonant spectroscopy in a single S…
Due to the large surface-to-volume ratio, surface trap states play a dominant role in the optoelectronic properties of nanoscale devices(1-6). Understanding the surface trap states allows us to properly engineer the device surfaces for better performance. But characterization of surface trap states at nanoscale has been a formidable challenge using the traditional capacitive techniques based on metal-insulator-semiconductor (MIS) structures(7) and deep level transient spectroscopy (DLTS)(8-11). Here, we demonstrate a simple but powerful optoelectronic method to probe the density of nanowire su…
Localized magnetic moments have been predicted to develop in graphene samples with vacancies or adsorbates. The interplay between such magnetic impurities and graphene's Dirac quasiparticles leads to remarkable many-body phenomena, which have so far proved elusive to experimental efforts. In this article, we study the thermodynamic, spectral and transport signatures of quantum criticality and Kondo physics of a dilute ensemble of atomic impurities in graphene. We consider vacancies and adatoms that either break or preserve graphene's $C_{3v}$ and inversion symmetries. In a neutral graphene sam…
Plasmonics, the science and technology of the interaction of light with metallic objects, is fundamentally changing the way we can detect, generate and manipulate light. Although the field is progressing swiftly, thanks to the availability of nanoscale manufacturing and analysis methods, fundamental properties such as the plasmonic excitations' symmetries cannot be accessed directly, leading to a partial, sometimes incorrect, understanding of their properties. Here we overcome this limitation by deliberately shaping the wave function of an electron beam to match a plasmonic excitations' symmet…
We investigate the effect of vacancy defects on the electronic and magnetic properties of zigzag graphene nanoribbons (zGNRs) by making use of the Green's function formalism in combination with the tight-binding Hamiltonian. The evolution of the indirect exchange coupling, known as Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction, including single, double, and multiple 5-8-5 divacancy defects is explained. Our numerical calculations show that the changes in the electronic structure and the exchange coupling of zGNRs depend significantly on the location of the divacancy defects with respect to …
The recent discovery of two-dimensional magnetic insulators has generated a great deal of excitement over their potential for nanoscale manipulation of spin or magnetism. One intriguing use for these materials is to put them in contact with graphene, with the goal of making graphene magnetic while maintaining its unique electronic properties. Such a system could prove useful in applications such as magnetic memories, or could serve as a host for exotic states of matter. Proximity to a magnetic insulator will alter the spin transport properties of graphene, and the strength of this interaction …
The coherent transport of charge and spin is one key requirement of future devices for quantum computing and communication. Scattering at defects or impurities may seriously reduce the coherence of quantum-mechanical states, thereby affecting device functionality. While numerous methods exist to experimentally assess charge transport, the real-space detection of a material's spin transport properties with nanometer resolution remains a challenge. Here we report on a novel approach which utilizes a combination of spin-polarized scanning tunneling microscopy (SP-STM) and the recently introduced …
We theoretically investigate the quantum reflection of different atoms by two-dimensional (2D) materials of the graphene family (silicene, germanene, and stanene), subjected to an external electric field and circularly polarized light. By using Lifshitz theory to compute the Casimir-Polder potential, which ensures that our predictions apply to all regimes of atom-2D surface distances, we demonstrate that the quantum reflection probability exhibits distinctive, unambiguous signatures of topological phase transitions that occur in 2D materials. We also show that the quantum reflection probabilit…
Ballistic atomic transport in narrow carbon nanotubes
Università degli Studi di Padova（帕多瓦大学）；Griffith University（格里菲斯大学）；Istituto Nazionale di Ottica del Consiglio Nazionale delle Ricerche（意大利国家光学研究所）；Istituto Nazionale di Fisica Nucleare, Sezione di Padova（意大利国家核物理研究所帕多瓦分部）
The ability to confine light into tiny spatial dimensions is important for applications such as microscopy, sensing and nanoscale lasers. While plasmons offer an appealing avenue to confine light, Landau damping in metals imposes a trade-off between optical field confinement and losses. We show that a graphene-insulator-metal heterostructure can overcome that trade-off, and demonstrate plasmon confinement down to the ultimate limit of the lengthscale of one atom. This is achieved by far-field excitation of plasmon modes squeezed into an atomically thin hexagonal boron nitride dielectric h-BN s…
