arXiv subjects

Andreas J. Heinrich

Publications and source records attributed to Andreas J. Heinrich.

At least 19 recordsLinked to original sources

arXiv2026

All-electrical Coherent Control of a Single Rare-earth Spin Qubit

Electrical control of single spin qubits is a major frontier for nanoscale, high-speed, and scalable quantum devices. Yet, extending it to highly shielded rare-earth 4f electrons remains an experimental challenge across solid-state platforms. Here we demonstrate all-electrical coherent control of a single Er electron spin, which is exchange-coupled to a nearby Ti atom. Scanning tunneling microscopy-based electron spin resonance with three-dimensional magnetic-field control enables comprehensive mapping of the resonance and Rabi frequencies, revealing pronounced anisotropies in both the Er g-tensor and the Er-Ti exchange interaction. The electrical modulation of the anisotropic Er-Ti coupling results in an efficient drive of the Er spin, allowing us to achieve near-gigahertz Rabi frequencies - a ten-fold improvement over the present record for rare-earth spin qubits. By establishing anisotropic exchange as a general resource for electrically accessing shielded rare-earth spins, our results open a new route to ultrafast and local control of rare-earth spins in solid-state quantum devices.

cond-mat.mes-hall↗

arXiv2026

On the interpretation of Hahn echo measurements in electron spin resonance scanning tunneling microscopy

Electron spin resonance scanning tunneling microscopy (ESR-STM) has become a powerful tool for probing spin dynamics and coherence of individual atoms and molecules on surfaces. In this work, we perform Rabi oscillation and Hahn echo pulse protocols on individual iron phthalocyanine (FePc) molecules on MgO/Ag(001) using ESR-STM. While Hahn echo protocols are widely used to extract spin coherence times, we show that in ESR-STM they are particularly susceptible to misinterpretation due to tunneling electrons generated by the applied radio-frequency (RF) voltage. The RF voltage not only drives the spin, but simultaneously probes and relaxes it, which consequently leads to an exponential decay that reflects spin relaxation rather than intrinsic phase coherence. We moreover show that varying both delay times in the refocusing pulse sequence is a reliable way to ensure a coherent nature of the echo signal. The extracted decay for the latter protocol suggests that T2 is approximately 30 ns and is thus closer to the decoherence time observed in Rabi oscillation measurements. This is significantly shorter than values reported in previous echo measurements. Our findings underscore the need for caution in interpreting T2 times from Hahn echo and Carr-Purcell protocols in ESR-STM and provide practical criteria for distinguishing true spin echoes from tunneling-induced relaxometry signals.

cond-mat.mes-hall↗

arXiv2025

Controlling the Exchange Field of Surface Spin Impurities via DC Voltages

Recent advances in scanning tunneling microscopy have enabled quantum-coherent control of single surface spins via all-electric electron spin resonance (ESR). Such control requires magnetoelectric coupling, since spin resonance is a magnetic effect. We show that a magnetic tip induces a bias-dependent exchange field on a localized Anderson impurity via virtual particle exchange with the magnetic lead. This field differs from Heisenberg exchange and can be tuned, reversed, or suppressed by the bias voltage. Our model reproduces bias-controlled resonance shifts for S = 1/2 titanium atoms and Fe(II) phthalocyanine, enabling spin control via the exchange field and revealing the magnetoelectric mechanism behind all-electric ESR for spin-based quantum technologies.

cond-mat.mes-hall↗

arXiv2025

Spin-State Engineering of Single Titanium Adsorbates on Ultrathin Magnesium Oxide

Single atomic adsorbates on ultrathin insulating films provide a promising route toward bottom-up quantum architectures based on atomically identical yet individually addressable spin qubits on solid surfaces. A key challenge in engineering quantum-coherent spin nanostructures lies in understanding and controlling the spin state of individual adsorbates. In this work, we investigate single titanium (Ti) atoms adsorbed on MgO/Ag(100) surfaces using a combined scanning tunneling microscopy and electron spin resonance. Our measurements reveal two distinct spin states, $S = 1/2$ and $S = 1$, depending on the local adsorption site and the thickness of the MgO film. Density functional theory calculations suggest a Ti$^+$ configuration for the Ti adsorbates with approximately 3 electrons in the 4$s$ and 3$d$ valence shells. Using a multi-orbital atomic multiplet calculations the site dependence of the spin can be rationalized as a charge redistribution between spin-polarizing and depolarizing orbitals. These findings underscore the potential of surface-supported single atoms as spin qubits with tunable spin and charge states, enabling atom-by-atom control in the realization of a versatile quantum platform on surfaces.

cond-mat.mes-hall↗

arXiv2025

Microscopic Scattering Approach to In-Gap States: Cr Adatoms on Superconducting β-Bi2Pd

We develop a microscopic scattering formalism to describe Yu-Shiba-Rusinov (YSR) states due to a single Cr adatom on the Bi-terminated surface of $β-Bi_2Pd$, by combining ab initio Wannier functions with a real-space Green's function approach in the Bogoliubov-de Gennes formalism. Our framework reproduces key scanning tunneling spectroscopy features, including a single particle-hole asymmetric YSR peak and isotropic dIdV maps around the impurity. Decomposing the YSR states reveals contributions from four nearly degenerate C4v representations, with energy broadening masking their individual signatures. Spin-orbit coupling induces partial spin polarization, while the spatial asymmetry between particle and hole components arises from Cr d-Bi p hybridization. These results highlight the importance of realistic band structures and microscopic modeling for interpreting STM data and provide a foundation for studying impurity chains hosting topological excitations.

cond-mat.supr-con↗

arXiv2025

Electron spin resonance with scanning tunneling microscopy: a tool for an on-surface quantum platform of identical qubits

Integration of electron spin resonance (ESR) in a scanning tunneling microscope (STM) has enabled an all-electrical control of atomic and molecular spins on solid surfaces with atomic-scale precision and energy resolution beyond thermal limitations. Further, coherent manipulation and detection of individual spins in an ESR-STM establishes a powerful quantum platform, allowing for the implementation of fundamental quantum logic operations to on-surface identical qubits. In this review, we introduce recent advances of ESR-STM, focusing on its application to atomic-scale qubits and extension to molecular qubit systems. We discuss the principles underlying ESR-STM, followed by single-spin addressability, coherent control via Rabi oscillations, and quantum state readout through frequency-resolved detection. We further demonstrate multi-qubit control architectures enabled by atom manipulation and local magnetic field engineering, culminating in the realization of multi-qubit logic gates such as the Controlled-NOT and Toffoli gates. These implementations highlight the specialty of ESR-STM towards atomic-scale quantum circuits. Indeed, ESR-STM can be an excellent tool to perform and evaluate quantum operations in molecular qubits. The results reviewed in this collection establish ESR-STM as a versatile tool for advancing quantum coherent science at the atomic and molecular level in solid-state environments.

cond-mat.mes-hall↗

arXiv2024

All-electrical driving and probing of dressed states in a single spin

The sub-nanometer 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 radio-frequency (RF) voltage of 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-electrical by a weakly coupled probe spin. Our work highlights the strength of the atomic-scale geometry inherent to the STM that facilitates creation and control of dressed states, which are promising for a design of atomically well-defined single spin quantum devices on surfaces.

cond-mat.mes-hall↗

arXiv2023

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.

cond-mat.mes-hall↗

arXiv2023

Electrically Driven Spin Resonance of 4f Electrons in a Single Atom on a Surface

A pivotal challenge in quantum technologies lies in reconciling long coherence times with efficient manipulation of the quantum states of a system. Lanthanide atoms, with their well-localized 4f electrons, emerge as a promising solution to this dilemma if provided with a rational design for manipulation and detection. Here we construct tailored spin structures to perform electron spin resonance on a single lanthanide atom using a scanning tunneling microscope. A magnetically coupled structure made of an erbium and a titanium atom enables us to both drive the erbium's 4f electron spins and indirectly probe them through the titanium's 3d electrons. In this coupled configuration, the erbium spin states exhibit a five-fold increase in the spin relaxation time and a two-fold increase in the driving efficiency compared to the 3d electron counterparts. Our work provides a new approach to accessing highly protected spin states, enabling their coherent control in an all-electric fashion.

cond-mat.mes-hall↗

arXiv2023

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 we present a combined experimental and modeling study of the ESR of a single hydrogenated Ti atom that is exchange-coupled to a Fe adatom located in 0.6-0.8 nm away. Continuous wave and pulsed ESR of the Ti spin showed a Rabi rate with two contributions, one from the tip and the other from the Fe, whose spin interactions with Ti were modulated by the radio-frequency electric field. The Fe contribution is comparable to the tip, as revealed from its dominance when the tip was retracted, and tunable using a vector magnetic field. Our 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.

cond-mat.mes-hall↗

arXiv2022

Development of a Scanning Tunneling Microscope for Variable Temperature Electron Spin Resonance

Recent advances in increasing 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 home-built STM capable of ESR at temperatures ranging from 1 K to 10 K. The STM is incorporated with a home-built Joule-Thomson refrigerator and a 2-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 couplings 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 in the sub-fA range. Our new design of ESR-STM, 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.

cond-mat.mes-hall↗

arXiv2022

An electron-spin qubit platform assembled atom-by-atom on a surface

Creating a quantum-coherent architecture at the atomic scale has long been an ambition in quantum science and nanotechnology. This ultimate length scale requires the use of fundamental quantum properties of atoms, such as the spin of electrons, which naturally occurs in many solid-state environments and allows high-fidelity operations and readout by electromagnetic means. Despite decades of effort, however, it remains a formidable task to realize an atomic-scale quantum architecture where multiple electron spin qubits can be precisely assembled, controllably coupled, and coherently operated. Electron spin qubits created in dopants in semiconductors and color centers in insulators, for example, can be well controlled individually6-8 but are difficult to couple together into a circuit. On the other hand, multiple magnetic atoms and molecules on surfaces can be coupled to each other by building sophisticated atomic structures using a scanning tunneling microscope (STM), but coherent operation has so far been limited to a single qubit in the tunnel junction. Here we demonstrate an atomic-scale qubit platform by showing atom-by-atom construction, coherent operations, and readout of multiple electron-spin qubits on a surface. To enable the coherent control of remote qubits that are outside the tunnel junction, we complement each electron spin with a local magnetic field gradient from a nearby single-atom magnet. To enable readout of remote qubits, we employ a sensor qubit in the tunnel junction and implement pulsed double electron spin resonance. Using these methods, we demonstrate fast single-, two-, and three-qubit operations in an all-electrical fashion. Our work marks the creation of an Angstrom-scale qubit platform, where quantum functionalities using electron spin arrays, built atom-by-atom on a surface, are now within reach.

cond-mat.mes-hall↗

arXiv2022

Anisotropic hyperfine interaction of surface-adsorbed single atoms

Hyperfine interactions between electron and nuclear spins have been widely used in material science, organic chemistry, and structural biology as a sensitive probe to the local chemical environment through spatial identification of nuclear spins. With the nuclear spins identified, the isotropic and anisotropic components of the hyperfine interactions in turn offer unique insight into the electronic ground-state properties of the paramagnetic centers. 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-titanium (Ti) atoms on MgO/Ag(100) and thereby determine the isotropic and anisotropic hyperfine interactions at the single-atom level. By combining vector-field ESR spectroscopy with STM-based atom manipulation, we characterize the full hyperfine tensor of individual Ti-47 and Ti-49 atoms and identify significant spatial anisotropy of hyperfine interaction for both isotopes when they are adsorbed at low-symmetry binding sites. Density functional theory calculations reveal that the large hyperfine anisotropy arises from a highly anisotropic distribution of the ground-state electron spin density. Our work highlights the power of ESR-STM-enabled single-atom hyperfine spectroscopy as a powerful tool in revealing ground-state electronic structures and atomic-scale chemical environments with nano-electronvolt resolution.

cond-mat.mes-hall↗

arXiv2022

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 a 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 manuscript 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.

cond-mat.mes-hall↗

arXiv2021

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 (ESR), 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.

physics.app-ph↗

arXiv2021

Spin Resonance Amplitude and Frequency of a Single Atom on a Surface in a Vector Magnetic Field

We used electron spin resonance (ESR) combined with scanning tunneling microscopy (STM) to measure hydrogenated Ti (spin-1/2) atoms at low-symmetry binding sites on MgO in vector magnetic fields. We found strongly anisotropic g-values in all three spatial directions. Interestingly, the amplitude and lineshape of the ESR signals are also strongly dependent on the angle of the field. We conclude that the Ti spin is aligned along the magnetic field, while the tip spin follows its strong magnetic anisotropy. Our results show the interplay between the tip and surface spins in determining the ESR signals and highlight the precision of ESR-STM to identify the single atom's spin states.

cond-mat.mes-hall↗

arXiv2020

Orbital-resolved single atom magnetism measured with X-ray absorption spectroscopy

Lanthanide atoms and molecules are promising candidates for atomic data storage and quantum logic due to the long magnetic lifetime of their electron quantum states. Accessing these states through electrical transport requires the engineering of their electronic configuration down to the level of individual atomic orbitals. Here, we address the magnetism of surface-supported lanthanide atoms, clusters, and films with orbital selectivity using X-ray absorption spectroscopy and magnetic circular dichroism. We exploit the selection rules of electric dipole transitions to reveal the occupation and magnetism of the valence electrons of Gd and Ho deposited on MgO/Ag(100). Comparing our results with multiplet calculations and density functional theory, we identify a charge transfer mechanism that leaves the lanthanide species in an unconventional singly ionized configuration. Our approach allows determining the role of valence electrons on the quantum level structure of lanthanide-based nanostructures.

cond-mat.mes-hall↗

arXiv2020

Sensing the spin of an individual Ce adatom

The magnetic moment of rare earth elements originates from electrons in the partially filled 4f orbitals. Accessing this moment electrically by scanning tunneling spectroscopy is hampered by shielding of outer-lying orbitals. Here we show that we can detect the magnetic moment of an individual Ce atom adsorbed on a Cu2N ultrathin film on Cu(100) by using a sensor tip that has its apex functionalized with a Kondo screened spin system. We calibrate the sensor tip by deliberately coupling it to a well characterized Fe atom. Subsequently, we use the splitting of the tip's Kondo resonance when approaching a spectroscopically dark Ce atom to sense its magnetic moment.

cond-mat.mes-hall↗