We build and commission a time-of-flight photon spectrometer (TOFS) for scanning tunneling microscopy luminescence (STML). We obtain the spectrum by exploiting the wavelength dependent refractive index of a long dispersive optical fiber that converts photon arrival times into wavelength information; blue photons are delayed more than red photons. The setup uses a pulsed excitation source, either laser flashes or voltage pulses, to launch the photons from the junction into a single photon detector. The TOFS calibration can be performed and transferred to the STML setup from a separate benchtop experiment using pulsed light sources with known wavelength. We verify the TOFS during STML operation by simultaneously recording luminescence from the Ag-Ag(111) plasmon using a conventional grating spectrometer. Our experiments show that the TOFS is a straightforward and cost-effective addition to existing STML setups with good performance in the near-infrared range. The TOFS is compatible with a drop-in replacement of the single photon detector such as a superconducting nanowire single photon detector or even bolometers that may expand the useful spectral range beyond the abilities of current STML setups.

The removal or cancellation of noise has wide-spread applications in imaging and acoustics. In applications in everyday life, such as image restoration, denoising may even include generative aspects, which are unfaithful to the ground truth. For scientific use, however, denoising must reproduce the ground truth accurately. Denoising scientific data is further challenged by unknown noise profiles. In fact, such data will often include noise from multiple distinct sources, which substantially reduces the applicability of simulation-based approaches. Here we show how scientific data can be denoised by using a deep convolutional neural network such that weak signals appear with quantitative accuracy. In particular, we study X-ray diffraction and resonant X-ray scattering data recorded on crystalline materials. We demonstrate that weak signals stemming from charge ordering, insignificant in the noisy data, become visible and accurate in the denoised data. This success is enabled by supervised training of a deep neural network with pairs of measured low- and high-noise data. We additionally show that using artificial noise does not yield such quantitatively accurate results. Our approach thus illustrates a practical strategy for noise filtering that can be applied to challenging acquisition problems.

We increase the dynamical range of a scanning tunneling microscope (STM) by actively subtracting dominant current-harmonics generated by nonlinearities in the current-voltage characteristics that could saturate the current preamplifier at low junction impedances or high gains. The strict phase relationship between a cosinusoidal excitation voltage and the current-harmonics allows excellent cancellation using the displacement-current of a driven compensating capacitor placed at the input of the preamplifier. Removal of DC currents has no effect on, and removal of the first harmonic only leads to a rigid shift in differential conductance that can be numerically reversed by adding the known removal current. Our method requires no permanent change of the hardware but only two phase synchronized voltage sources and a multi-frequency lock-in amplifier to enable high dynamic range spectroscopy and imaging.• Active power filter• Dynamic range compression• High gain preamplifier

We demonstrate and verify the in-situ addition of a collecting lens for electroluminescence experiments to an existing scanning tunneling microscope. We fabricate a simple clip-on lens that we reversibly attach at the sample plate via regular sample transfer tools to collimate the light emitted from a plasmonic tunneling junction to the viewport ordinarily used for optical access. The proximity of the lens to the tunneling junction allows us achieve good collection efficiencies, demonstrating the quick turnaround of converting an existing setup with optical access into a practical scanning luminescence microscope. We verify the function of the clip-on lens by measuring the bias dependent plasmon of Au, Ag, and spatial luminescence maps. • Reversible clip-on lens. • In-situ transfer. • Luminescence.

Superconducting (SC) tips for scanning tunneling microscopy (STM) can enhance a wide range of surface science studies because they offer exquisite energy resolution, allow the study of Josephson tunneling, or provide spatial contrast based on the local interaction of the SC tip with the sample. The appeal of a SC tip is also practical. An SC gap can be used to characterize and optimize the noise of a low-temperature apparatus. Unlike typical samples, SC tips can be made with less ordered materials, such as from SC polycrystalline wires or by coating a normal metal tip with a superconductor. Those recipes either require additional laboratory infrastructure or are carried out in ambient conditions, leaving an oxidized tip behind. Here, we revisit the vacuum cleaving of an Nb wire to prepare fully gapped tips in an accessible one-step procedure. To show their utility, we measure the SC gap of Nb on Au(111) to determine the base temperature of our microscope and to optimize its RF filtering. The deliberate coating of the Nb tip with Au fully suppresses the SC gap and we show how sputtering with Ar+ ions can be used to gradually recover the gap, promising tunability for tailored SC gaps sizes.

The on-surface synthesis of nano-graphenes has led the charge in prototyping structures with perspectives beyond silicon-based technology. Following reports of open-shell systems in graphene-nanoribbons (GNRs), a flurry of research activity was directed at investigating their magnetic properties with a keen eye for spintronic applications. Although the synthesis of nano-graphenes is usually carried out on Au(111), the substrate is difficult to use for electronic decoupling and spin-polarized measurements. Using a binary alloy Cu3Au(111), we show possibilities for gold-like on-surface synthesis compatible with spin polarization and electronic decoupling known from copper. We prepare copper oxide layers, demonstrate the synthesis of GNRs, and grow thermally stable magnetic Co islands. We functionalize the tip of a scanning tunneling microscope with carbon-monoxide, nickelocene, or attach Co clusters for high-resolution imaging, magnetic sensing, or spin-polarized measurements. This versatile platform will be a valuable tool in the advanced study of magnetic nano-graphenes.

We demonstrate a straightforward approach to integrating a magnetic field into a low-temperature scanning tunneling microscope (STM) by adhering an NdFeB permanent magnet to a magnetizable sample plate. To render our magnet concept compatible with high-temperature sample cleaning procedures, we make the irreversible demagnetization of the magnet a central part of our preparation cycle. After sacrificing the magnet by heating it above its Curie temperature, we use a transfer tool to attach a new magnet in-situ prior to transferring the sample into the STM. We characterize the magnetic field created by the magnet using the Abrikosov vortex lattice of superconducting NbSe2. Excellent agreement between the distance dependent magnetic fields from experiments and simulations allows us to predict the magnitude and orientation of magnetic flux at any location with respect to the magnet and the sample plate. Our concept is an accessible solution for field-dependent surface science studies that require fields in the range of up to 400 mT and otherwise detrimental heating procedures.•Accessible magnetic field generation.•Selectable field strength and orientation.•Compatible with high-temperature sample preparation.

Quasiparticle interference imaging (QPI) offers insight into the band structure of quantum materials from the Fourier transform of local density of states (LDOS) maps. Their acquisition with a scanning tunneling microscope is traditionally tedious due to the large number of required measurements that may take several days to complete. The recent demonstration of sparse sampling for QPI imaging showed how the effective measurement time could be fundamentally reduced by only sampling a small and random subset of the total LDOS. However, the amount of required sub-sampling to faithfully recover the QPI image remained a recurring question. Here we introduce an adaptive sparse sampling (ASS) approach in which we gradually accumulate sparsely sampled LDOS measurements until a desired quality level is achieved via compressive sensing recovery. The iteratively measured random subset of the LDOS can be interleaved with regular topographic images that are used for image registry and drift correction. These reference topographies also allow to resume interrupted measurements to further improve the QPI quality. Our ASS approach is a convenient extension to quasiparticle interference imaging that should remove further hesitation in the implementation of sparse sampling mapping schemes. • Accumulative sampling for unknown degree of sparsity • Controllably interrupt and resume QPI measurements • Scattering wave conserving background subtractions.

The pathway toward the tailored synthesis of materials starts with precise characterization of the conformational properties and dynamics of individual molecules. Electron spin resonance (ESR)-based scanning tunneling microscopy can potentially address molecular structure with unprecedented resolution. Here, we determine the fine structure and geometry of an individual titanium-hydride molecule, utilizing a combination of a newly developed millikelvin ESR scanning tunneling microscope in a vector magnetic field and ab initio approaches. We demonstrate a strikingly large anisotropy of the $g$ tensor, unusual for a spin doublet ground state, resulting from a nontrivial orbital angular momentum stemming from the molecular ground state. We quantify the relationship between the resultant fine structure, hindered rotational modes, and orbital excitations. Our model system provides avenues to determine the structure and dynamics of individual molecules.

Spectroscopic mapping refers to the massive recording of spectra whilst varying an additional degree of freedom, such as: magnetic field, location, temperature, or charge carrier concentration. As this involves two serial tasks, spectroscopic mapping can become excruciatingly slow. We demonstrate exponentially faster mapping through our combination of sparse sampling and parallel spectroscopy. We exemplify our concept using quasiparticle interference imaging of Au(111) and Bi2Sr2CaCu2O8 (Bi2212), as two well-known model systems. Our method is accessible, straightforward to implement with existing scanning tunneling microscopes, and can be easily extended to enhance gate or field-mapping spectroscopy. In view of a possible four orders of magnitude speed advantage, it is setting the stage to fundamentally promote the discovery of novel quantum materials.

‘Magic’-angle twisted bilayer graphene has received a lot of interest due to its flat bands with potentially nontrivial topology that lead to intricate correlated phases. A spectrum with flat bands, however, does not require a twist between multiple sheets of van der Waals materials, but rather can be realized with the application of an appropriate periodic potential. Here, we propose the imposition of a tailored periodic potential onto a single graphene layer through local perturbations that could be created via lithography or adatom manipulation, which also results in an energy spectrum featuring flat bands. Our first-principle calculations for an appropriate decoration of graphene with adatoms indeed show the presence of flat bands in the spectrum. Furthermore, we reveal the topological nature of the flat bands through a symmetry-indicator analysis. This non-trivial topology manifests itself in corner-localized states with a filling anomaly as we show using a tight-binding model. Our proposal of a single decorated graphene sheet provides a new versatile route to study correlated phases in topologically non-trivial, flat band structures.

In the last decade, detecting spin dynamics at the atomic scale has been enabled by combining techniques such as electron spin resonance (ESR) or pump-probe spectroscopy with scanning tunneling microscopy (STM). Here, we demonstrate an ultra-high vacuum STM operational at milliKelvin (mK) temperatures and in a vector magnetic field capable of both ESR and pump-probe spectroscopy. By implementing GHz compatible cabling, we achieve appreciable RF amplitudes at the junction while maintaining the mK base temperature and high energy resolution. We demonstrate the successful operation of our setup by utilizing two experimental ESR modes (frequency sweep and magnetic field sweep) on an individual TiH molecule on MgO/Ag(100) and extract the effective g-factor. We trace the ESR transitions down to MHz into an unprecedented low frequency band enabled by the mK base temperature. We also implement an all-electrical pump-probe scheme based on waveform sequencing suited for studying dynamics down to the nanoseconds range. We benchmark our system by detecting the spin relaxation time T1 of individual Fe atoms on MgO/Ag(100) and note a field strength and orientation dependent relaxation time.

Scanning tunneling microscopy (STM) is a notoriously slow technique; data-recording is serial, which renders complex measurement tasks, such as quasiparticle interference (QPI) mapping, impractical. However, QPI could provide insight into band-structure details of quantum materials that can be inaccessible to angle-resolved photoemission spectroscopy. Here we use compressed sensing (CS) to fundamentally speed-up QPI mapping. We reliably recover the QPI information from a fraction of the usual local density of state measurements. The requirement of CS is naturally fulfilled for QPI, since CS relies on sparsity in a vector domain, here given by few nonzero coefficients in Fourier space. We exemplify CS on a simulated Cu(111) surface using random sampling of uniform and varying probability density. The latter improves QPI recovery and mitigates Fourier artifacts. We further simplify the motion of the STM tip through an open traveling salesman's problem for greater efficiency and use the tip-path for drift correction. We expect that the implications of our CS approach will be transformative for the exploration of two-dimensional quantum materials.

The three essential pillars of magnetic data storage devices are readability, writeability, and stability. However, these requirements compete as magnetic domain sizes reach the fundamental limit of single atoms and molecules. The proven magnetic bistability of individual holmium atoms on magnesium oxide appeared to operate within this magnetic trilemma, sacrificing writeability for unprecedented stability. Using the magnetic stray field created by the tip of a spin-polarized scanning tunneling microscope (SP-STM), we controllably move the Ho state into the quantum regime, allowing us to write its state via the quantum tunneling of magnetization (QTM). We find that the hyperfine interaction causes both the excellent magnetic bistability, even at zero applied magnetic field, and the avoided level crossings which we use to control the magnetic state via QTM. We explore how to use such a system to realize a high-fidelity single atom NOT gate (inverter). Our approach reveals the prospect of combining the best traits of the classical and quantum worlds for next generation data storage.

The three essential pillars of magnetic data storage devices are readability, writeability, and stability. However, these requirements compete as magnetic domain sizes reach the fundamental limit of single atoms and molecules. The proven magnetic bistability of individual holmium atoms on magnesium oxide appeared to operate within this magnetic trilemma, sacrificing writeability for unprecedented stability. Using the magnetic stray field created by the tip of a spin-polarized scanning tunneling microscope (SP-STM), we controllably move the Ho state into the quantum regime, allowing us to write its state via the quantum tunneling of magnetization (QTM). We find that the hyperfine interaction causes both the excellent magnetic bistability, even at zero applied magnetic field, and the avoided level crossings which we use to control the magnetic state via QTM. We explore how to use such a system to realize a high-fidelity single atom NOT gate (inverter). Our approach reveals the prospect of combining the best traits of the classical and quantum worlds for next generation data storage.

Electron spin resonance with a scanning tunneling microscope (ESR-STM) combines the high energy resolution of spin resonance spectroscopy with the atomic scale control and spatial resolution of STM. Here we describe the upgrade of a helium-3 STM with a 2D vector-field magnet (Bz = 8.0 T, Bx = 0.8 T) to an ESR-STM. The system is capable of delivering radio frequency (RF) power to the tunnel junction at frequencies up to 30 GHz. We demonstrate magnetic field-sweep ESR for the model system TiH/MgO/Ag(100) and find a magnetic moment of (1.004 ± 0.001) μB. Our upgrade enables to toggle between a DC mode, where the STM is operated with the regular control electronics, and an ultrafast-pulsed mode that uses an arbitrary waveform generator for pump-probe spectroscopy or reading of spin-states. Both modes allow for simultaneous radiofrequency excitation, which we add via a resistive pick-off tee to the bias voltage path. The RF cabling from room temperature to the 350 mK stage has an average attenuation of 18 dB between 5 and 25 GHz. The cable segment between the 350 mK stage and the STM tip presently attenuates an additional 34-3 +5 dB from 10 to 26 GHz and 38-2 +3 dB between 20 and 30 GHz. We discuss our transmission losses and indicate ways to reduce this attenuation. We finally demonstrate how to synchronize the arrival times of RF and DC pulses coming from different paths to the STM junction, a prerequisite for future pulsed ESR experiments.