Electron Spin Resonance-Scanning Tunneling Microscopy (ESR-STM) of C60 radical ion on graphene is a first demonstration on radical ions. ESR-STM signal at g=2.00 was measured in accordance with macroscopic ESR of fullerene radical ion. The ESR-STM signal was bias voltage dependent, as it reflects the charge state of the molecule. The signal appears in the bias voltage which enables the ionization of the lowest unoccupied molecular orbital (LUMO) (creation of radical anion) and the highest occupied molecular orbital (HOMO (creation of a radical cation) of the C60 molecule when it deposited on graphene.
The linewidth provides information on the lifetime of the free radical. In several experiments, a 13C hyperfine splitting was observed, and a change in the phase of the ESR-STM peak as a function of the speed of the magnetic field sweep was changed. This might be used to provide information on the relaxation times of the molecules. In parallel, ESR-STM signal at g=1.6 was ascribed to Tungsten oxide (W5+) at the tip apex, which is not bias voltage dependent.
The ability of ESR-STM to explore non paramagnetic molecules, significantly broadens the scope of this technique.
Multi-tip scanning tunneling microscopy (STM) is a powerful method to perform charge transport measurements at the nanoscale. With four STM tips positioned on the surface of a sample, four-point resistance measurements can be performed in dedicated geometric configurations. Here, we present an alternative to the most often used scanning electron microscope (SEM) imaging to infer the corresponding tip positions. After initial coarse positioning monitored by an optical microscope, STM scanning itself is used to determine the inter-tip distances. A large STM overview scan serves as a reference ma…
Mixing of atoms at the interface was studied for Mn/Fe magnetic hetero-epitaxial layers on Cu(001) by scanning tunneling microscopy/spectroscopy. The formation of a surface alloy was observed when the Mn layer was thinner than 3 atomic layers. From the fourth layer, Fe segregation is suppressed, and a pure Mn surface appears. Accordingly, spectroscopic measurements revealed the electronic difference between the surface alloy and Mn layers. The surface electronic structure of the fourth Mn layer is slightly different from that of the fifth layers, which is attributed to the hybridization of the…
We present a design for a tunneling-current-assisted scanning near-field microwave microscope. For stable operation at cryogenic temperatures, making a small and rigid microwave probe is important. Our coaxial resonator probe has a length of approxomately 30 mm and can fit inside the 2-inch bore of a superconducting magnet. The probe design includes an insulating joint, which separates DC and microwave signals without degrading the quality factor. By applying the SMM to the imaging of an electrically inhomogeneous superconductor, we obtain the spatial distribution of the microwave response wit…
The detection of fluorescence with submolecular resolution enables the exploration of spatially varying photon yields and vibronic properties at the single-molecule level. By placing individual polycyclic aromatic hydrocarbon molecules into the plasmon cavity formed by the tip of a scanning tunneling microscope and a NaCl-covered Ag(111) surface, molecular light emission spectra are obtained that unravel vibrational progression. In addition, light spectra unveil a signature of the molecule even when the tunneling current is injected well separated from the molecular emitter. This signature exh…
Recent advances in scanning probe techniques rely on the chemical functionalization of the probe-tip termination by a single molecule. The success of this approach opens the tantalizing prospect of introducing spin sensitivity through the functionalization by a magnetic molecule. Here, we use a nickelocene-terminated tip (Nc-tip), which offers the possibility of producing spin excitations on the tip apex of a scanning tunneling microscope (STM). We show that when the Nc-tip is a hundred pm away from point contact with a surface-supported object, magnetic effects may be probed through changes i…
The quantitative characterization of the degree of randomness and aggregation of surface micro and nanostructures is critical to evaluate their effects on targeted functionalities. To this end, the methods of Point Pattern Analysis (PPA), largely used in ecology and medical imaging, seem to provide a powerful toolset. However, the application of these techniques requires the extraction of the point pattern of nanostructures from their microscope images. In this work, we address the issue of the impact that Scanning Electron Microscope (SEM) image processing may have on the fundamental metric o…
The Majorana fermion can be described by a real wave function with only two phases (0 and π) which provide a controllable degree of freedom. We propose a strategy to regulate the phase of the chiral Majorana state by coupling with a scanning tunneling microscope tip in a system consisting of quantum anomalous Hall insulator coupled with a superconductor. With the change of the chemical potential, the chiral Majorana state can be tuned alternately between 0 and π, in which, correspondingly, the perfect normal tunneling and perfect crossed Andreev reflection appear. The perfect crossed Andreev r…
Inelastic electron tunneling in a scanning tunneling microscope (STM) is used to generate excitons in monolayer tungsten disulfide (WS$_2$). Excitonic electroluminescence is measured both at positive and negative sample bias. Using optical spectroscopy and Fourier-space optical microscopy, we show that the bias polarity of the tunnel junction determines the spectral and angular distribution of the emitted light. At positive sample bias, only emission from excitonic species featuring an in-plane transition dipole moment is detected. Based on the spectral distribution of the emitted light, we in…
The scanning-tunneling-microscope-induced luminescence emerges recently as an incisive tool to measure the molecular properties down to the single-molecule level. The rapid experimental progress is far ahead of the theoretical effort to understand the observed phenomena. Such incompetence leads to a significant difficulty in quantitatively assigning the observed feature of the fluorescence spectrum to the structure and dynamics of a single molecule. This letter is devoted to reveal the microscopic origin of the molecular excitation via inelastic scattering of the tunneling electrons in scannin…
We report a scanning superconducting quantum interference device (SQUID) microscope in a cryogen-free dilution refrigerator with a base temperature at the sample stage of at least 30 mK. The microscope is rigidly mounted to the mixing chamber plate to optimize thermal anchoring of the sample. The microscope housing fits into the bore of a superconducting vector magnet, and our design accommodates a large number of wires connecting the sample and sensor. Through a combination of vibration isolation in the cryostat and a rigid microscope housing, we achieve relative vibrations between the SQUID …
Quantum sensors based on solid-state spins provide tremendous opportunities in a wide range of fields from basic physics and chemistry to biomedical imaging. However, integrating them into a scanning probe microscope to enable practical, nanoscale quantum imaging is a highly challenging task. Recently, the use of single spins in diamond in conjunction with atomic force microscopy techniques has allowed significant progress towards this goal, but generalisation of this approach has so far been impeded by long acquisition times or by the absence of simultaneous topographic information. Here we r…
Scanning tunneling microscopes (STM) are used extensively for studying and manipulating matter at the atomic scale. In spite of the critical role of the STM tip, the control of the atomic-scale shape of STM tips remains a poorly solved problem. Here, we present a method for preparing tips {\it in-situ} and for ensuring the crystalline structure and reproducibly preparing tip structure up to the second atomic layer. We demonstrate a controlled evolution of such tips starting from undefined tip shapes.
In scanning tunneling microscopy induced luminescence (STML), the photon counting is measured to reflect the single-molecule properties, e.g., the first molecular excited state. The energy of the first excited state is typically determined by a rising position of the photon counting as a function of the bias voltage between the tip and the substrate. It remains a challenge to determine the precise rise position of the current due to the possible experimental noise. In this work, we propose an alternating current version of STML to resolve the fine structures in the photon counting measurement.…
The molecular dark state participates in many important photon-induced processes, yet is typically beyond the optical-spectroscopic measurement due to the forbidden transition dictated by the selection rule. In this work, we propose to use the scanning tunneling microscope (STM) as an incisive tool to directly profile the dark-state transition density of a single molecule, taking advantage of the localized static electronic field near the metal tip. The detection of dark state is achieved by measuring the fluorescence from a higher bright state to the ground state with assistant optical pumpin…
We describe the design, construction, and performance of an ultra-high vacuum (UHV) scanning tunneling microscope (STM) capable of imaging at dilution-refrigerator temperatures and equipped with a vector magnet. The primary objective of our design is to achieve a high level of modularity by partitioning the STM system into a set of easily separable, interchangeable components. This naturally segregates the UHV needs of STM instrumentation from the typically non-UHV construction of a dilution refrigerator, facilitating the usage of non-UHV materials while maintaining a fully bakeable UHV chambe…
We present a Scanning Hall Probe Microscope operating in ambient conditions. One of the unique features of this microscope is the use of the same stepper motors for both sample positioning as well as scanning, which makes it possible to have a large scan range (few mm) in x and y directions, with a scan resolution of 0.1 $μ$m. Protocols have been implemented to enable scanning at different heights from the sample surface. The z range is 35 mm. Microstructured Hall probes of size 1-5 $μ$m have been developed. A minimum probe-sample distance \textless{} 2 $μ$m has been obtained by the combinatio…
The Scanning Quantum Cryogenic Atom Microscope (SQCRAMscope) is a quantum sensor in which a quasi-1D quantum gas images electromagnetic fields emitted from a nearby sample. We report improvements to the microscope. Cryogen usage is reduced by replacing the liquid cryostat with a closed-cycle system and modified cold finger, and cryogenic cooling is enhanced by adding a radiation shield. The minimum accessible sample temperature is reduced from 35 K to 5.8 K while maintaining low sample vibrations. A new sample mount is easier to exchange, and quantum gas preparation is streamlined.
The coupling between molecular exciton and gap plasmons plays a key role in single molecular electroluminescence induced by a scanning tunneling microscope (STM). But it has been difficult to clarify the complex experimental phenomena. By employing the nonequilibrium Green's function method, we propose a general theoretical model to understand the light emission spectrum from single molecule and gap plasmons from an energy transport point of view. The coherent interaction between gap plasmons and molecular exciton leads to a prominent Fano resonance in the emission spectrum. We analyze the dep…
Silicon can be isotopically enriched, allowing for the fabrication of highly coherent semiconductor spin qubits. However, the conduction band of bulk Si exhibits a six-fold valley degeneracy, which may adversely impact the performance of silicon quantum devices. To date, the spatial characterization of valley states in Si remains limited. Moreover, techniques for probing valley states in functional electronic devices are needed. We describe here a cryogen-free scanning gate microscope for the characterization of Si/Si$_{0.7}$Ge$_{0.3}$ quantum devices at mK temperatures. The microscope is base…
We present the design and performance of a cryogenic scanning tunneling microscope (STM) which operates inside a water-cooled Bitter magnet, which can attain a magnetic field of up to 38 T. Due to the high vibration environment generated by the magnet cooling water, a uniquely designed STM and vibration damping system are required. The STM scan head is designed to be as compact and rigid as possible, to minimize the effect of vibrational noise as well as fit the size constraints of the Bitter magnet. The STM uses a differential screw mechanism for coarse tip - sample approach, and operates in …
We describe the design and performance of a scanning tunneling microscope (STM) which operates at a base temperature of 30 mK in a vector magnetic field. The cryogenics is based on an ultra-high vacuum (UHV) top-loading wet dilution refrigerator that contains a vector magnet allowing for fields up to 9 T perpendicular and 4 T parallel to the sample. The STM is placed in a multi-chamber UHV system, which allows in-situ preparation and exchange of samples and tips. The entire system rests on a 150-ton concrete block suspended by pneumatic isolators, which is housed in an acoustically isolated an…
We present a scanning probe microscopy technique for spatially resolving transport in cold atomic gases, in close analogy with scanning gate microscopy in semiconductor physics. The conductance of a quantum point contact connected to two atomic reservoirs is measured in the presence of a tightly focused laser beam acting as a local perturbation that can be precisely positioned in space. By scanning its position and recording the subsequent variations of conductance, we retrieve a high-resolution map of transport through a quantum point contact. We demonstrate a spatial resolution comparable to…
We describe the development and performance of an ultra-high vacuum scanning tunneling microscope working under combined extreme conditions of ultra-low temperatures and high magnetic fields. We combined a top-loading dilution refrigerator and a standard bucket dewar with a bottom-loading superconducting magnet to achieve 4.5 days operating time, which is long enough to perform various spectroscopic-imaging measurements. To bring the effective electron temperature closer to the mixing-chamber temperature, we paid particular attention to filtering out the radio-frequency noise, as well as enhan…
