arXiv subjects

Wantong Huang

Publications and source records attributed to Wantong Huang.

13 recordsLinked to original sources

arXiv2026

Electrical Spin Pumping in Exchange-coupled Molecules

Electron spins in single molecules are a promising platform for quantum information processing. However, their practical implementation as qubits requires reliable control at the single-entity level, including an efficient state initialization. Here, we demonstrate the remote, all-electrical initialization of the electron spin in single molecules: Using electron spin resonance scanning tunneling microscopy, we investigate coupled pairs of S=1/2 molecules (Fe-FePc), where one molecule serves as a readout and pumping unit for the neighboring one. We show that the exchange interaction between them enables angular momentum transfer, which allows for the control of the remote spin state via the direction and magnitude of the spin-polarized tunneling current and the exchange coupling strength. These results establish a general, all-electrical approach for remote spin initialization that is readily transferable to a wide range of spin-based quantum architectures.

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↗

arXiv2026

Atomic-Scale Quantum Control of Single Spin Defects in a Two-Dimensional Semiconductor

Individual spin defects in solids are promising building blocks for quantum technologies, but their deterministic creation, individual addressability, and operation near surfaces remain major challenges. Two-dimensional materials provide an attractive alternative, as their single-layer thickness enables direct atomic-scale access to defect states. Here, we demonstrate single-spin control of solid-state defects in a two-dimensional semiconductor by a combination of scanning tunneling microscopy and electron spin resonance. We create and manipulate individual sulfur vacancies and carbon substitution defects in monolayer molybdenum disulfide and characterize their spin dynamics, including coherent control, at the single-defect level. Using atomic manipulation, we further engineer and probe spin-spin interactions between defect pairs. Our results demonstrate deterministic creation, addressability, coherent manipulation, and controlled coupling of individual spin defects within a single experimental platform. This establishes atomically engineered spin defects in two-dimensional semiconductors as a versatile class of controllable solid-state quantum systems and opens a route towards tailored quantum sensing experiments.

cond-mat.mes-hall↗

arXiv2025

Spin-Electric Control of Individual Molecules on Surfaces

Individual magnetic molecules are promising building blocks for quantum technologies because of their chemical tunability, nanoscale dimensions, and ability to self-assemble into ordered arrays. However, harnessing their properties in quantum information processing requires precise local control of their spin properties. In this work, we present spin-electric coupling (SEC) for two molecular spin systems, iron phthalocyanine (FePc) and Fe-FePc complexes, adsorbed on a surface. We use electron spin resonance combined with scanning tunnelling microscopy (ESR-STM) to locally address them with the STM tip and electrically tune them using the applied bias voltage. These measurements reveal a pronounced nonlinear voltage dependence of the resonance frequency, linked to the energic onset of other molecular orbitals. We attribute this effect to a transport-mediated exchange field from the magnetic tip, providing a large, highly localized, and broadly applicable SEC mechanism. Finally, we demonstrate that the SEC enables all-electrical coherent spin control: In Rabi oscillation measurements of both single and coupled Fe-FePc complexes we show that the spin dynamics can be tuned, demonstrating a pathway towards electrically controlled quantum operation.

cond-mat.mes-hall↗

arXiv2025

An electrically controlled single molecule spin switch

Precise control of spin states and spin-spin interactions in atomic-scale magnetic structures is crucial for spin-based quantum technologies. A promising architecture is molecular spin systems, which offer chemical tunability and scalability for larger structures. An essential component, in addition to the qubits themselves, is switchable qubit-qubit interactions that can be individually addressed. In this study, we present an electrically controlled single-molecule spin switch based on a bistable complex adsorbed on an insulating magnesium oxide film. The complex, which consists of an Fe adatom coupled to an iron phthalocyanine (FePc) molecule, can be reversibly switched between two stable states using voltage pulses locally via the tip of a scanning tunnelling microscope (STM). Inelastic electron tunnelling spectroscopy (IETS) measurements and density functional theory (DFT) calculations reveal a distinct change between a paramagnetic and a non-magnetic spin configuration. Lastly, we demonstrate the functionality of this molecular spin switch by using it to modify the electron spin resonance (ESR) frequency of a nearby target FePc spin within a spin-spin coupled structure. Thus, we showcase how individual molecular machines can be utilized to create scalable and tunable quantum devices.

cond-mat.mes-hall↗

arXiv2025

Probing Magnetism in Self-Assembled Organometallic Complexes using Kondo Spectroscopy

Control of individual spins at the atomic level holds great promise for miniaturized spintronics, quantum sensing, and quantum information processing. Both single atomic and molecular spin centers are prime candidates for these applications and are often individually addressed and manipulated using scanning tunneling microscopy (STM). In this work, we present a hybrid approach and demonstrate a robust method for self-assembly of magnetic organometallic complexes consisting of individual iron (Fe) atoms and molecules on a silver substrate using STM. We employ two types of molecules, bis(dibenzoylmethane) copper(II) [Cu(dbm)2] and iron phthalocyanine (FePc). We show that in both cases the Fe atoms preferentially attach underneath the benzene ring ligand of the molecules, effectively forming an organometallic half-sandwich arene complex, Fe(C6H6), that is akin to the properties of metallocenes. In both situations, a molecule can be combined with up to two Fe atoms. In addition, we observe a change in the magnetic properties of the attached Fe atoms in scanning tunneling spectroscopy, revealing a distinct Kondo signature at the Fe sites. We explain the latter using density functional theory calculations, and find that the bond formation between the Fe 3d-orbitals and the benzene {\pi}-molecular orbitals creates a favorable situation for Kondo screening of the d_xz- and d_yz-like orbitals. Thus, this work establishes a reliable design principle for forming hybrid organometallic complexes and simultaneous tuning of their atomic spin states.

cond-mat.mes-hall↗

arXiv2024

Experimental discovery of Sarma state in atomically thick superconducting FeSe films under high magnetic fields

Many-body ground states of imbalanced Fermi gas have been studied both theoretically and experimentally for several decades because of their fundamental significance in condensed matter physics, cold atom physics and nuclear physics. The Sarma state, a gapless spin-polarized superfluid, is one of those long sought-after exotic ground states of spin imbalanced Fermi gas. Yet, an unambiguous experimental evidence of Sarma superfluid state has not been found. Here, we report the experimental discovery of the Sarma state in atomically thick FeSe films by a dilution-refrigerator scanning tunneling microscope under high magnetic fields. In the bilayer or trilayer FeSe films, we directly observe the key evidence of the entrance of the Sarma state: the inner Zeeman splitting coherence peaks cross the Fermi level under high in-plane magnetic fields. The angle dependent critical in-plane magnetic field of coherence peak crossing shows a two-fold symmetry due to the anisotropy of the in-plane g-factor of FeSe films. Moreover, in a superconducting FeSe monolayer of a lateral size of several hundred nanometers, the Sarma state can also be induced by strong out-of-plane magnetic fields. Our findings pave the way to explore the unusual physical properties and potential applications in superconducting spintronics of the spin-polarized Sarma superfluid state.

cond-mat.supr-con↗

arXiv2024

Landau-Level Quantization and Band Splitting of FeSe Monolayers Revealed by Scanning Tunneling Spectroscopy

Two-dimensional (2D) superconductors that reside on substrates must be influenced by Rashba spin-orbit coupling (SOC). The intriguing effect of Rashba-type SOCs on iron-based superconductors (IBSs) has remained largely a mystery. In this work, we unveil modified Landau-level spectroscopy and the intricate band splitting of FeSe monolayers through the precision of scanning tunneling spectroscopy, which unequivocally demonstrates the presence of Rashba SOC. The discovery sheds light on a nonparabolic electron band at the X/Y point, displaying a distinctive Landau quantization behavior characterized by $E_n\propto(nB)^{4/3}$. The theoretical model aligns with our experimental insights, positing that the k$^4$-term of the electron band becomes predominant and profoundly reshapes the band structure. Our research underscores the pivotal role of the Rashba SOC effect on 2D superconductors and sets the stage to probe new quantum states in systems with remarkably low carrier concentrations.

cond-mat.supr-con↗

arXiv2024

Quantum Spin-Engineering in On-Surface Molecular Ferrimagnets

The design and control of atomic-scale spin structures constitute major challenges for spin-based quantum technology platforms, including quantum dots, color centers, and molecular spins. Here, we showcase a strategy for designing the quantum properties of molecular spin qubits by combining tip-assisted on-surface assembly with electron spin resonance scanning tunneling microscopy (ESR-STM): We fabricate magnetic dimer complexes that consist of an iron phthalocyanine (FePc) molecule and an organometallic half-sandwich complex formed by the FePc ligand and an attached iron atom, Fe(C6H6). The total complex forms a mixed-spin (1/2,1) quantum ferrimagnet with a well-separated correlated ground state doublet, which we utilize for coherent control. As a result of the correlation, the quantum ferrimagnet shows an improved spin lifetime (>1.5 ${\mu}$s) as it is partially protected against inelastic electron scattering. Lastly, the ferrimagnet units also enable intermolecular coupling, that can be used to realize both ferromagnetic or antiferromagnetic structures. Thus, quantum ferrimagnets provide a versatile platform to improve coherent control in general and to study complex magnetic interactions.

cond-mat.mes-hall↗

arXiv2022

Real-space BCS-BEC crossover in FeSe monolayer

The quantum many body states in the BCS-BEC crossover regime are of long-lasting interest. Here we report direct spectroscopic evidence of BCS-BEC crossover in real-space in a FeSe monolayer thin film by using spatially resolved scanning tunneling spectra. The crossover is driven by the shift of band structure relative to the Fermi level. The theoretical calculation based on a two-band model qualitatively reproduces the measured spectra in the whole crossover range. In addition, the Zeeman splitting of the quasi-particle states is found to be consistent with the characteristics of a condensate. Our work paves the way to study the exotic states of BCS-BEC crossover in a two-dimensional crystalline material at the atomic scale.

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arXiv2021

Superconducting FeSe monolayer with milli-electron volt Fermi energy

Iron selenide (FeSe) is an iron-based superconductor which shows unique properties, including strongly anisotropic superconducting gap, paramagnetism in undoped compound and extremely small Fermi pocket size. In this work, we demonstrate that the sizes of electron and hole pockets in FeSe monolayer become much smaller than those in bulk. The Fermi energy is in the order of a few meV and can be fine-tuned by the thickness of graphene layers underneath. Despite the low carrier density, the FeSe monolayers grown on trilayer or multi-layer graphene are superconducting. The superconducting gap size is sensitive to the Fermi energy of the hole band. Remarkably, the FeSe monolayer provides the opportunity to study the physics in the crossover regime where the Fermi energy and superconducting gap are comparable to each other.

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arXiv2019

Disorder induced multifractal superconductivity in monolayer niobium dichalcogenides

The interplay between disorder and superconductivity is a subtle and fascinating phenomenon in quantum many body physics. The conventional superconductors are insensitive to dilute nonmagnetic impurities, known as the Anderson's theorem. Destruction of superconductivity and even superconductor-insulator transitions occur in the regime of strong disorder. Hence disorder-enhanced superconductivity is rare and has only been observed in some alloys or granular states. Because of the entanglement of various effects, the mechanism of enhancement is still under debate. Here we report well-controlled disorder effect in the recently discovered monolayer NbSe$_2$ superconductor. The superconducting transition temperatures of NbSe$_2$ monolayers are substantially increased by disorder. Realistic theoretical modeling shows that the unusual enhancement possibly arises from the multifractality of electron wave functions. This work provides the first experimental evidence of the multifractal superconducting state.

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arXiv2017

Molecular Beam Epitaxy Growth of Tetragonal FeS Film on SrTiO3(001) Substrate

We report the successful growth of tetragonal FeS film with one or two unit-cell (UC) thickness on SrTiO3(001) substrate by molecular beam epitaxy. Large lattice constant mismatch with the substrate leads to high density of defects in single UC FeS, while it has been significantly reduced in double UC thick film due to the lattice relaxation. The scanning tunneling spectra on the surface of FeS thin film reveal the electronic doping effect of single UC FeS from the substrate. In addition, at the Fermi level, the energy gaps of approximate 1.5 meV are observed in films of both thicknesses at 4.6 K and below. The absence of coherence peaks of gap spectra may be related to the preformed Cooper-pairs without phase coherence.

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