arXiv subjects

Soo-hyon Phark

Publications and source records attributed to Soo-hyon Phark.

12 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

Efficient driving of a spin-qubit using single-atom magnets

The realization of electron-spin resonance at the single-atom level using scanning tunneling microscopy has opened new avenues for coherent quantum sensing and quantum state manipulation at the ultimate size limit. This allows to build many-body Hamiltonians and the study of their complex physical behavior. Recently, a novel qubit platform has emerged from this field, raising questions about the driving mechanism from single-atom magnets. In this work, we demonstrate how single-atom magnets can be used to drive a nearby single spin qubit efficiently. We show that the modulation of exchange coupling is the primary driving force, which successfully reproduces Rabi rates in the tens of MHz range, consistent with experimental data, while also addressing critical aspects related to the optimization of experimental parameters.

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

Tailoring the Electronic Configurations of YPc$_2$ on Cu(111): Decoupling Strategies for Molecular Spin Qubits Platforms

Among the potential spin qubit candidates, yttrium phthalocyanine double-decker (YPc$_2$) features a diamagnetic metal ion core that stabilizes the molecular structure, while its magnetic properties arise primarily from an unpaired electron (S=1/2) delocalized over the two phthalocyanine (Pc) ligands. Understanding its properties in the proximity of metal electrodes is crucial to assess its potential use in molecular spin qubits architectures. Here, we investigated the morphology and electronic structure of this molecule adsorbed on Cu(111) surface using scanning tunneling microscopy (STM). On Cu(111), YPc$_2$ adsorbs flat, with isolated molecules showing a preferred orientation along the <111> crystal axes. Moreover, we observed two different types of self-assembly molecular packing when growing molecular patches. For YPc$_2$ in direct contact with Cu(111), STM revealed a widely separated highest occupied and lowest unoccupied molecular orbitals (HOMO/LUMO), suggesting the quenching of the unpaired spin. Conversely, when YPc$_2$ is separated from the metal substrate by a few-layer thick diamagnetic zinc phthalocyanine (ZnPc) layer, we found the HOMO to split into singly occupied and singly unoccupied molecular orbitals (SOMO/SUMO). We observed that more than 2 layers of ZnPc are needed to avoid intermixing between the two molecules and spin quenching in YPc2. Density functional theory (DFT) reveals the spin quenching is due to the hybridization between YPc$_2$ and Cu(111) states, confirming the importance of using suitable decoupling layers to preserve the unpaired molecular spin. Our results suggest the potential of YPc$_2$/ZnPc heterostructures as a stable and effective molecular spin qubit platform and validate the possibility of integrating this molecular spin qubit candidate in future quantum logic devices.

cond-mat.mes-hall↗

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

Automated classification of individual atoms on surfaces using machine learning

Leveraging scanning tunneling microscopy (STM) for atomic-scale fabrication has led to many advancements such as the creation of atomic electron-spin qubit structures on surfaces. However, the time-consuming and tedious nature of this process calls for improvements, and this study explores the use of machine learning (ML) to automate certain steps, notably identifying appropriate atomic candidates for the structures. We classify titanium and iron atoms on a magnesium oxide (MgO) surface, which are prototypical on-surface spin qubit candidates, showing distinct topographic and spectroscopic features depending on the bonding sites of the MgO surface. Employing a semi-automated computer vision process, we train a convolutional neural network with STM topographic images and scanning tunneling spectroscopy (STS) curves of several hundred atoms. After training, the topography model achieves an 86% validation accuracy in classifying 200 new images, and the STS model, a 100% accuracy for a sample size of 100 atoms. This method extends its applicability to various nanoscopic measurements, including atomically resolved imaging and local probing of electronic properties, offering a promising approach for classifying atoms and molecules on surfaces.

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↗

arXiv2024

Protocol for certifying entanglement in surface spin systems using a scanning tunneling microscope

Certifying quantum entanglement is a critical step towards realizing quantum-coherent applications of surface spin systems. In this work, we show that entanglement can be unambiguously shown in a scanning tunneling microscope (STM) with electron spin resonance by exploiting the fact that entangled states undergo a free time evolution with a distinct characteristic time constant that clearly distinguishes it from any other time evolution in the system. By implementing a suitable phase control scheme, the phase of this time evolution can be mapped back onto the population of one entangled spin in a pair, which can then be read out reliably using a weakly coupled sensor spin in the junction of the scanning tunneling microscope. We demonstrate through open quantum system simulations with realistic spin systems, which are currently available with spin coherence times of $T_2\approx$ 300 ns, that a signal directly correlated with the degree of entanglement can be measured at a temperature range of 100$-$400 mK accessible in sub-Kelvin cryogenic STM systems.

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↗

arXiv2013

Superparamagnetic response of Fe-coated W tips in spin-polarized scanning tunneling microscopy

We performed spin-polarized scanning tunneling spectroscopy on biatomic-layer-high Co nanoislands grown on Cu(111) in magnetic fields oriented normal to the sample surface, with Fe-coated W tips. Increasing the temperature from 10 to 30 K, we observe a reduced slope of the differential conductance around zero field. A quantitative analysis of the field- and temperature-dependent differential conductance data in the framework of superparamagnetism as described by a Langevin function gives an excellent description of the experimental results. The analysis suggests that a Fe nano-apex at the W tip, which is composed of 220-300 Fe atoms, determines the magnetic response of the tip.

cond-mat.mes-hall↗

arXiv2011

Selective growth of perovskite oxides on SrTiO3 (001) by control of surface reconstructions

We report surface reconstruction (RC)-dependent growths of SrTiO3 and SrVO3 on a SrTiO3 (001) surface with two different coexisting surface RCs, namely (2x1) and c(6x2). Up to the coverage of several layers, epitaxial growth was forbidden on the c(6x2) RC under the growth conditions that permitted layer-by-layer epitaxial growth on the (2x1) RC. Scanning tunneling microscopy examination of the lattice structure of the c(6x2) RC revealed that this RC-selective growth mainly originated from the significant structural/stoichiometric dissimilarity between the c(6x2) RC and the cubic perovskite films. As a result, the formation of SrTiO3 islands was forbidden from the nucleation stage.

cond-mat.mtrl-sci↗