Roadmap on nanoscale magnetic resonance imaging.

The field of nanoscale magnetic resonance imaging (NanoMRI) was started 30 years ago. It was motivated by the desire to image single molecules and molecular assemblies, such as proteins and virus particles, with near-atomic spatial resolution and on a length scale of 100 nm. Over the years, the NanoMRI field has also expanded to include the goal of useful high-resolution nuclear magnetic resonance (NMR) spectroscopy of molecules under ambient conditions, including samples up to the micron-scale. The realization of these goals requires the development of spin detection techniques that are many orders of magnitude more sensitive than conventional NMR and MRI, capable of detecting and controlling nanoscale ensembles of spins. Over the years, a number of different technical approaches to NanoMRI have emerged, each possessing a distinct set of capabilities for basic and applied areas of science. The goal of this roadmap article is to report the current state of the art in NanoMRI technologies, outline the areas where they are poised to have impact, identify the challenges that lie ahead, and propose methods to meet these challenges. This roadmap also shows how developments in NanoMRI techniques can lead to breakthroughs in emerging quantum science and technology applications. .

All-Electrical Driving and Probing of Dressed States in a Single Spin.

The subnanometer distance between tip and sample in a scanning tunneling microscope (STM) enables the application of very large electric fields with a strength as high as ∼1 GV/m. This has allowed for efficient electrical driving of Rabi oscillations of a single spin on a surface at a moderate radiofrequency (RF) voltage on the order of tens of millivolts. Here, we demonstrate the creation of dressed states of a single electron spin localized in the STM tunnel junction by using resonant RF driving voltages. The read-out of these dressed states was achieved all electrically by a weakly coupled probe spin. Our work highlights the strength of the atomic-scale geometry inherent to the STM that facilitates the creation and control of dressed states, which are promising for the design of atomic scale quantum devices using individual spins on surfaces.

Standardization of a CT Protocol for Imaging Patients with Suspected COVID-19-A RACOON Project.

CT protocols that diagnose COVID-19 vary in regard to the associated radiation exposure and the desired image quality (IQ). This study aims to evaluate CT protocols of hospitals participating in the RACOON (Radiological Cooperative Network) project, consolidating CT protocols to provide recommendations and strategies for future pandemics. In this retrospective study, CT acquisitions of COVID-19 patients scanned between March 2020 and October 2020 (RACOON phase 1) were included, and all non-contrast protocols were evaluated. For this purpose, CT protocol parameters, IQ ratings, radiation exposure (CTDIvol), and central patient diameters were sampled. Eventually, the data from 14 sites and 534 CT acquisitions were analyzed. IQ was rated good for 81% of the evaluated examinations. Motion, beam-hardening artefacts, or image noise were reasons for a suboptimal IQ. The tube potential ranged between 80 and 140 kVp, with the majority between 100 and 120 kVp. CTDIvol was 3.7 ± 3.4 mGy. Most healthcare facilities included did not have a specific non-contrast CT protocol. Furthermore, CT protocols for chest imaging varied in their settings and radiation exposure. In future, it will be necessary to make recommendations regarding the required IQ and protocol parameters for the majority of CT scanners to enable comparable IQ as well as radiation exposure for different sites but identical diagnostic questions.

Accelerating computer vision-based human identification through the integration of deep learning-based age estimation from 2 to 89 years.

Computer Vision (CV)-based human identification using orthopantomograms (OPGs) has the potential to identify unknown deceased individuals by comparing postmortem OPGs with a comprehensive antemortem CV database. However, the growing size of the CV database leads to longer processing times. This study aims to develop a standardized and reliable Convolutional Neural Network (CNN) for age estimation using OPGs and integrate it into the CV-based human identification process. The CNN was trained on 50,000 OPGs, each labeled with ages ranging from 2 to 89 years. Testing included three postmortem OPGs, 10,779 antemortem OPGs, and an additional set of 70 OPGs within the context of CV-based human identification. Integrating the CNN for age estimation into CV-based human identification process resulted in a substantial reduction of up to 96% in processing time for a CV database containing 105,251 entries. Age estimation accuracy varied between postmortem and antemortem OPGs, with a mean absolute error (MAE) of 2.76 ± 2.67 years and 3.26 ± 3.06 years across all ages, as well as 3.69 ± 3.14 years for an additional 70 OPGs. In conclusion, the incorporation of a CNN for age estimation in the CV-based human identification process significantly reduces processing time while delivering reliable results.

An atomic-scale multi-qubit platform.

Individual electron spins in solids are promising candidates for quantum science and technology, where bottom-up assembly of a quantum device with atomically precise couplings has long been envisioned. Here, we realized atom-by-atom construction, coherent operations, and readout of coupled electron-spin qubits using a scanning tunneling microscope. To enable the coherent control of "remote" qubits that are outside of the tunnel junction, we complemented each electron spin with a local magnetic field gradient from a nearby single-atom magnet. Readout was achieved by using a sensor qubit in the tunnel junction and implementing pulsed double electron spin resonance. Fast single-, two-, and three-qubit operations were thereby demonstrated in an all-electrical fashion. Our angstrom-scale qubit platform may enable quantum functionalities using electron spin arrays built atom by atom on a surface.

Investigation of Inkjet-Printed Masks for Fast and Easy Photolithographic NIL Masters Manufacturing.

Modern optical systems often require small, optically effective structures that have to be manufactured both precisely and cost-effectively. One option to do this is using nanoimprint lithography (NIL), in which the optical structures are replicated as masters using a stamping process. It would also be advantageous to manufacture the master structures quickly and easily. A master manufacturing process based on a photolithographic image of an inkjet-printed mask is presented and investigated in this paper. An essential element is that a deliberate blurring of the printed structure edge of the mask is used in the photolithographic process. Combined with the use of a non-linear photoresist, this allows for improved edge geometries of the master structure. We discuss the inkjet-printed photomask, the custom photolithography system to prevent imaging of the printing dot roughness and the manufacturing processes of NIL polymer masks as well as their subsequent stamp imprinting. Finally, it was shown that stamp geometries with a width of 1.7 µm could be realised using inkjet-printed photomasks in the master manufacturing process. This methodology opens up the potential of fast and simple master manufacturing for the development and manufacturing of optical elements.

Influence of the Magnetic Tip on Heterodimers in Electron Spin Resonance Combined with Scanning Tunneling Microscopy.

Investigating the quantum properties of individual spins adsorbed on surfaces by electron spin resonance combined with scanning tunneling microscopy (ESR-STM) has shown great potential for the development of quantum information technology on the atomic scale. A magnetic tip exhibiting high spin polarization is critical for performing an ESR-STM experiment. While the tip has been conventionally treated as providing a static magnetic field in ESR-STM, it was found that the tip can exhibit bistability, influencing ESR spectra. Ideally, the ESR splitting caused by the magnetic interaction between two spins on a surface should be independent of the tip. However, we found that the measured ESR splitting of a metal atom-molecule heterodimer can be tip-dependent. Detailed theoretical analysis reveals that this tip-dependent ESR splitting is caused by a different interaction energy between the tip and each spin of the heterodimer. Our work provides a comprehensive reference for characterizing tip features in ESR-STM experiments and highlights the importance of employing a proper physical model when describing the ESR tip, in particular, for heterospin systems.

Electric-Field-Driven Spin Resonance by On-Surface Exchange Coupling to a Single-Atom Magnet.

Coherent control of individual atomic and molecular spins on surfaces has recently been demonstrated by using electron spin resonance (ESR) in a scanning tunneling microscope (STM). Here, a combined experimental and modeling study of the ESR of a single hydrogenated Ti atom that is exchange-coupled to a Fe adatom positioned 0.6-0.8 nm away by means of atom manipulation is presented. Continuous wave and pulsed ESR of the Ti spin show a Rabi rate with two contributions, one from the tip and the other from the Fe, whose spin interactions with Ti are modulated by the radio-frequency electric field. The Fe contribution is comparable to the tip, as revealed by its dominance when the tip is retracted, and tunable using a vector magnetic field. The new ESR scheme allows on-surface individual spins to be addressed and coherently controlled without the need for magnetic interaction with a tip. This study establishes a feasible implementation of spin-based multi-qubit systems on surfaces.

Double-Resonance Spectroscopy of Coupled Electron Spins on a Surface.

Scanning-tunneling microscopy (STM) combined with electron spin resonance (ESR) has enabled single-spin spectroscopy with nanoelectronvolt energy resolution and angstrom-scale spatial resolution, which allows quantum sensing and magnetic resonance imaging at the atomic scale. Extending this spectroscopic tool to a study of multiple spins, however, is nontrivial due to the extreme locality of the STM tunnel junction. Here we demonstrate double electron-electron spin resonance spectroscopy in an STM for two coupled atomic spins by simultaneously and independently driving them using two continuous-wave radio frequency voltages. We show the ability to drive and detect the resonance of a spin that is remote from the tunnel junction while read-out is achieved via the spin in the tunnel junction. Open quantum system simulations for two coupled spins reproduce all double-resonance spectra and further reveal a relaxation time of the remote spin that is longer by an order of magnitude than that of the local spin in the tunnel junction. Our technique can be applied to quantum-coherent multi-spin sensing, simulation, and manipulation in engineered spin structures on surfaces.

Template-directed 2D nanopatterning of S = 1/2 molecular spins.

Molecular spins are emerging platforms for quantum information processing. By chemically tuning their molecular structure, it is possible to prepare a robust environment for electron spins and drive the assembly of a large number of qubits in atomically precise spin-architectures. The main challenges in the integration of molecular qubits into solid-state devices are (i) minimizing the interaction with the supporting substrate to suppress quantum decoherence and (ii) controlling the spatial distribution of the spins at the nanometer scale to tailor the coupling among qubits. Herein, we provide a nanofabrication method for the realization of a 2D patterned array of individually addressable Vanadyl Phthalocyanine (VOPc) spin qubits. The molecular nanoarchitecture is crafted on top of a diamagnetic monolayer of Titanyl Phthalocyanine (TiOPc) that electronically decouples the electronic spin of VOPc from the underlying Ag(100) substrate. The isostructural TiOPc interlayer also serves as a template to regulate the spacing between VOPc spin qubits on a scale of a few nanometers, as demonstrated using scanning tunneling microscopy, X-ray circular dichroism, and density functional theory. The long-range molecular ordering is due to a combination of charge transfer from the metallic substrate and strain in the TiOPc interlayer, which is attained without altering the pristine VOPc spin characteristics. Our results pave a viable route towards the future integration of molecular spin qubits into solid-state devices.

Harnessing the Quantum Behavior of Spins on Surfaces.

The desire to control and measure individual quantum systems such as atoms and ions in a vacuum has led to significant scientific and engineering developments in the past decades that form the basis of today's quantum information science. Single atoms and molecules on surfaces, on the other hand, are heavily investigated by physicists, chemists, and material scientists in search of novel electronic and magnetic functionalities. These two paths crossed in 2015 when it was first clearly demonstrated that individual spins on a surface can be coherently controlled and read out in an all-electrical fashion. The enabling technique is a combination of scanning tunneling microscopy (STM) and electron spin resonance, which offers unprecedented coherent controllability at the Angstrom length scale. This review aims to illustrate the essential ingredients that allow the quantum operations of single spins on surfaces. Three domains of applications of surface spins, namely quantum sensing, quantum control, and quantum simulation, are discussed with physical principles explained and examples presented. Enabled by the atomically-precise fabrication capability of STM, single spins on surfaces might one day lead to the realization of quantum nanodevices and artificial quantum materials at the atomic scale.

Quality measures for fully automatic CT histogram-based fat estimation on a corpse sample.

In a previous article a new algorithm for fully automatic 'CT histogram based Fat Estimation and quasi-Segmentation' (CFES) was validated on synthetic data, on a special CT phantom, and tested on one corpse. Usage of said data in FE-modelling for temperature-based death time estimation is the investigation's number one long-term goal. The article presents CFES's results on a human corpse sample of size R = 32, evaluating three different performance measures: the τ-value, measuring the ability to differentiate fat from muscle, the anatomical fat-muscle misclassification rate D, and the weighted distance S between the empirical and the theoretical grey-scale value histogram. CFES-performance on the sample was: D = 3.6% for weight exponent α = 1, slightly higher for α ≥ 2 and much higher for α ≤ 0. Investigating τ, S and D on the sample revealed some unexpected results: While large values of τ imply small D-values, rising S implies falling D and there is a positive linear relationship between τ and S. The latter two findings seem to be counter-intuitive. Our Monte Carlo analysis detected a general umbrella type relation between τ and S, which seems to stem from a pivotal problem in fitting Normal mixture distributions.

Anisotropic Hyperfine Interaction of Surface-Adsorbed Single Atoms.

Hyperfine interactions have been widely used in material science, organic chemistry, and structural biology as a sensitive probe to local chemical environments. However, traditional ensemble measurements of hyperfine interactions average over a macroscopic number of spins with different geometrical locations and nuclear isotopes. Here, we use a scanning tunneling microscope (STM) combined with electron spin resonance (ESR) to measure hyperfine spectra of hydrogenated-Ti on MgO/Ag(100) at low-symmetry binding sites and thereby determine the isotropic and anisotropic hyperfine interactions at the single-atom level. Combining vector-field ESR spectroscopy with STM-based atom manipulation, we characterize the full hyperfine tensors of 47Ti and 49Ti and identify significant spatial anisotropy of the hyperfine interactions for both isotopes. Density functional theory calculations reveal that the large hyperfine anisotropy arises from highly anisotropic distributions of the ground-state electron spin density. Our work highlights the power of ESR-STM-enabled single-atom hyperfine spectroscopy in revealing electronic ground states and atomic-scale chemical environments.

Development of a scanning tunneling microscope for variable temperature electron spin resonance.

Recent advances in improving the spectroscopic energy resolution in scanning tunneling microscopy (STM) have been achieved by integrating electron spin resonance (ESR) with STM. Here, we demonstrate the design and performance of a homebuilt STM capable of ESR at temperatures ranging from 1 to 10 K. The STM is incorporated with a homebuilt Joule-Thomson refrigerator and a two-axis vector magnet. Our STM design allows for the deposition of atoms and molecules directly into the cold STM, eliminating the need to extract the sample for deposition. In addition, we adopt two methods to apply radio-frequency (RF) voltages to the tunnel junction: the early design of wiring to the STM tip directly and a more recent idea to use an RF antenna. Direct comparisons of ESR results measured using the two methods and simulations of electric field distribution around the tunnel junction show that, despite their different designs and capacitive coupling to the tunnel junction, there is no discernible difference in the driving and detection of ESR. Furthermore, at a magnetic field of ∼1.6 T, we observe ESR signals (near 40 GHz) sustained up to 10 K, which is the highest temperature for ESR-STM measurement reported to date, to the best of our knowledge. Although the ESR intensity exponentially decreases with increasing temperature, our ESR-STM system with low noise at the tunnel junction allows us to measure weak ESR signals with intensities of a few fA. Our new design of an ESR-STM system, which is operational in a large frequency and temperature range, can broaden the use of ESR spectroscopy in STM and enable the simple modification of existing STM systems, which will hopefully accelerate a generalized use of ESR-STM.

Drug loss from Paclitaxel-Coated Balloons During Preparation, Insertion and Inflation for Angioplasty: A Laboratory Investigation.

PURPOSE: To investigate drug contamination of the working environment with paclitaxel drug-coated balloon (DCB) angioplasty due to loss of paclitaxel containing particles from the coating during DCB preparation, insertion, and inflation. MATERIAL AND METHODS: In an experimetal laboratory setting, drug loss during removal of the protective cover and insertion of the DCB through the hemostatic valve of the introducer sheath and after inflation was examined. In seven DCB types of different manufacturers, semi-quantitative image analysis was performed during five standardized tests cycles. Additionally, every DCB type passed one cycle of a wipe test and one cycle of air sampling. RESULTS: By removing the protective cover, the paclitaxel-covered balloon surface was significantly reduced in 3 out of 7 products (P = 0.043). Overall, extend of decline ranged from 0.4 to 12%. In 6 of 7 products, powdered paclitaxel clusters dropped down upon removal of the protective cover (0.099 ng/cm2 up to approx. 22 ng/cm2). Contamination of the air was detected in none of the DCB types. When pushed through the vascular sheath, none of the investigated DCB types showed a significant loss of paclitaxel from the coated balloon surface. After balloon inflation, the paclitaxel-coated surface area varied between manufacturers ranging from 25.9 to 97.8%. CONCLUSION: In some DCB types, the removal of the protective cover already leads to a significant loss of paclitaxel and paclitaxel-coated surfaces. As a result, there will be a contamination of the workplace and a reduction in the therapeutic dose. LEVEL OF EVIDENCE: No level of evidence.

CT-based thermometry with virtual monoenergetic images by dual-energy of fat, muscle and bone using FBP, iterative and deep learning-based reconstruction.

OBJECTIVES: The aim of this study was to evaluate the sensitivity of CT-based thermometry for clinical applications regarding a three-component tissue phantom of fat, muscle and bone. Virtual monoenergetic images (VMI) by dual-energy measurements and conventional polychromatic 120-kVp images with modern reconstruction algorithms adaptive statistical iterative reconstruction-Volume (ASIR-V) and deep learning image reconstruction (DLIR) were compared. METHODS: A temperature-regulating water circuit system was developed for the systematic evaluation of the correlation between temperature and Hounsfield units (HU). The measurements were performed on a Revolution CT with gemstone spectral imaging technology (GSI). Complementary measurements were performed without GSI (voltage 120 kVp, current 130-545 mA). The measured object was a tissue equivalent phantom in a temperature range of 18 to 50°C. The evaluation was carried out for VMI at 40 to 140 keV and polychromatic 120-kVp images. RESULTS: The regression analysis showed a significant inverse linear dependency between temperature and average HU regardless of ASIR-V and DLIR. VMI show a higher temperature sensitivity compared to polychromatic images. The temperature sensitivities were 1.25 HU/°C (120 kVp) and 1.35 HU/°C (VMI at 140 keV) for fat, 0.38 HU/°C (120 kVp) and 0.47 HU/°C (VMI at 40 keV) for muscle and 1.15 HU/°C (120 kVp) and 3.58 HU/°C (VMI at 50 keV) for bone. CONCLUSIONS: Dual-energy with VMI enables a higher temperature sensitivity for fat, muscle and bone. The reconstruction with ASIR-V and DLIR has no significant influence on CT-based thermometry, which opens up the potential of drastic dose reductions. KEY POINTS: • Virtual monoenergetic images (VMI) enable a higher temperature sensitivity for fat (8%), muscle (24%) and bone (211%) compared to conventional polychromatic 120-kVp images. • With VMI, there are parameters, e.g. monoenergy and reconstruction kernel, to modulate the temperature sensitivity. In contrast, there are no parameters to influence the temperature sensitivity for conventional polychromatic 120-kVp images. • The application of adaptive statistical iterative reconstruction-Volume (ASIR-V) and deep learning-based image reconstruction (DLIR) has no effect on CT-based thermometry, opening up the potential of drastic dose reductions in clinical applications.

Electron spin resonance of single iron phthalocyanine molecules and role of their non-localized spins in magnetic interactions.

Electron spin resonance (ESR) spectroscopy is a crucial tool, through spin labelling, in investigations of the chemical structure of materials and of the electronic structure of materials associated with unpaired spins. ESR spectra measured in molecular systems, however, are established on large ensembles of spins and usually require a complicated structural analysis. Recently, the combination of scanning tunnelling microscopy with ESR has proved to be a powerful tool to image and coherently control individual atomic spins on surfaces. Here we extend this technique to single coordination complexes-iron phthalocyanines (FePc)-and investigate the magnetic interactions between their molecular spin with either another molecular spin (in FePc-FePc dimers) or an atomic spin (in FePc-Ti pairs). We show that the molecular spin density of FePc is both localized at the central Fe atom and also distributed to the ligands (Pc), which yields a strongly molecular-geometry-dependent exchange coupling.

Quantum-coherent nanoscience.

For the past three decades nanoscience has widely affected many areas in physics, chemistry and engineering, and has led to numerous fundamental discoveries, as well as applications and products. Concurrently, quantum science and technology has developed into a cross-disciplinary research endeavour connecting these same areas and holds burgeoning commercial promise. Although quantum physics dictates the behaviour of nanoscale objects, quantum coherence, which is central to quantum information, communication and sensing, has not played an explicit role in much of nanoscience. This Review describes fundamental principles and practical applications of quantum coherence in nanoscale systems, a research area we call quantum-coherent nanoscience. We structure this Review according to specific degrees of freedom that can be quantum-coherently controlled in a given nanoscale system, such as charge, spin, mechanical motion and photons. We review the current state of the art and focus on outstanding challenges and opportunities unlocked by the merging of nanoscience and coherent quantum operations.

Spin-Selective Hole-Exciton Coupling in a V-Doped WSe2 Ferromagnetic Semiconductor at Room Temperature.

While valley polarization with strong Zeeman splitting is the most prominent characteristic of two-dimensional (2D) transition metal dichalcogenide (TMD) semiconductors under magnetic fields, enhancement of the Zeeman splitting has been demonstrated by incorporating magnetic dopants into the host materials. Unlike Fe, Mn, and Co, V is a distinctive dopant for ferromagnetic semiconducting properties at room temperature with large Zeeman shifting of band edges. Nevertheless, little known is the excitons interacting with spin-polarized carriers in V-doped TMDs. Here, we report anomalous circularly polarized photoluminescence (CPL) in a V-doped WSe2 monolayer at room temperature. Excitons couple to V-induced spin-polarized holes to generate spin-selective positive trions, leading to differences in the populations of neutral excitons and trions between left and right CPL. Using transient absorption spectroscopy, we elucidate the origin of excitons and trions that are inherently distinct for defect-mediated and impurity-mediated trions. Ferromagnetic characteristics are further confirmed by the significant Zeeman splitting of nanodiamonds deposited on the V-doped WSe2 monolayer.