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Xuehao Wu

Publications and source records attributed to Xuehao Wu.

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Molecular spin qubits in a van der Waals bottle

Advancing quantum information technologies requires qubits whose coherence can be precisely engineered. Among the qubit platforms in development, molecular spin qubits (MSQs) stand out for their atomic scale tunability and chemical specificity, making them powerful candidates for sensing, simulation, and information processing. However, integrating MSQs into solid-state architectures without degrading their coherence remains a central challenge. Here, we introduce van der Waals (vdW) confinement within two-dimensional materials as a strategy for stabilizing quantum states in MSQs by engineering their local electronic, vibrational, and symmetry environments. Using cobaltocene as a model system, we show that confinement within vdW SnS2 and CdPS3 single crystals reorganizes the single-ion energy landscape and slows spin-lattice relaxation by over two orders of magnitude relative to unconfined cobaltocene. The confined MSQs adopt deterministic orientations and self-assemble into ordered, atomically precise superlattices, establishing vdW confinement as a pathway for integrating MSQs into functional quantum devices.

cond-mat.mtrl-sci

Fully compensated ferrimagnetic triferroics and multistate transport in hidden-phase wurtzite MnSe monolayer

Fully compensated ferrimagnets (fFIMs) have attracted interest due to their compensated moments and nonrelativistic spin splitting across the Brillouin zone. Known fFIMs, however, are mostly restricted to complex three-dimensional (3D) systems or require external fields in two-dimensional (2D) heterostructures, leaving intrinsic fFIM monolayers unexplored. We identify a hidden-phase MnSe monolayer, derived from the (001) planes of wurtzite, as an intrinsic fFIM featuring inequivalent sublattices not linked by any symmetry. It is a unipolar magnetic semiconductor (UMS) with perpendicular magnetic anisotropy (528.60 * 10^-3 eV per unit cell) and simultaneously exhibits ferroelectricity (polarization 4.63 * 10^-10 C/m) and ferroelasticity (signal 61%), with barriers of 7.6 * 10^-3 and 0.10 eV/f.u., respectively, establishing a single-phase triferroic system. The ground fFIM UMS characteristics are robust against strain up to 3%. The In2Se3/MnSe heterostructure enables nonvolatile electrical control between semiconducting and metallic states. Constructed tunnel junctions exhibit giant tunneling magnetoresistance (2.98 * 10^5%), electroresistance (6.97 * 10^14%), elastoresistance (7.95 * 10^4%), and near-perfect spin filtering (~100%). Collectively, this spontaneous 2D fFIM with coexisting triferroic orders provides a promising platform for ultrahigh-density, low-power, and miniaturized memory devices.

physics.app-ph

Programmable, Spontaneous Superlattice Memory in a Monolayer Topological Insulator

Memory is a foundational concept across disciplines, from neurobiology and electronics to artificial intelligence and quantum gravity. In materials, memory effects typically arise from ferroic orders, such as ferroelectricity and ferromagnetism, where information is stored in charge or spin degrees of freedom. Here, we report a surprising discovery of a nonvolatile superlattice memory effect in monolayer TaIrTe4, a dual quantum spin Hall insulator, where information is encoded through sharply contrasting lattice periodicities. In particular, in a pristine monolayer, we observe the spontaneous emergence of a long-period superlattice that can be programmed ON and OFF in a nonvolatile manner by electrostatic tuning of low-energy electronic states. This switching toggles the system between two structural configurations with unit cell areas differing by nearly two orders of magnitude. Mechanistically, our results reveal two independent and distinct instabilities, one in the lattice and the other in the QSH electrons, which are coupled, leading to electrostatic control of lattice configurations with nonvolatile memory. This finding is enabled by combining linear and nonlinear transport measurements, Raman spectroscopy, and scanning tunneling microscopy, which probe complementary aspects of the underlying orders. Remarkably, this nonvolatile memory effect stabilizes a spontaneous superlattice with a periodicity on the few-nanometer scale that remains robust across a wide doping range, persists over days, and survives above 70 K. Combined with the QSH topology, this stability offers a promising route to nonvolatile memory control of topological flat bands and their filling enabled quantum states. Our preliminary data indeed show the emergence of new insulating states at fractional superlattice fillings, which can be clearly switched ON and OFF together with the superlattice.

cond-mat.mes-hall

All-Altermagnetic Tunnel Junction of RuO2/NiF2/RuO2

Emerging altermagnets with zero net magnetic moment and moment-dependent spin splitting offer a promising avenue for antiferromagnetic spintronic devices, yet their integration into magnetic tunnel junctions has been hindered by reliance on ferromagnetic electrodes (introducing stray fields) or by limited functionality (non-tunable magnetoresistance without spin filtering). Here, we propose an all-altermagnetic tunnel junction (AAMTJ) paradigm composed exclusively of altermagnets, exemplified by experimentally feasible RuO2/NiF2/RuO2. By introducing an altermagnetic NiF2 barrier, the achieved tunneling magnetoresistances of 11,704%, 2,496% and 1,892% for RuO2/NiF2/RuO2 are much higher than that of 221% for RuO2/TiO2/RuO2 with a nonmagnetic TiO2 barrier. High spin filtering efficiencies of ~90% are also obtained. This architecture unlocks multistate high magnetoresistance and spin filtering via magnetization control of the electrodes and barrier, stemming from their synergistic and antagonistic alignments of momentum-dependent altermagnetic spin-splitting. Importantly, high tunneling magnetoresistances are still achieved in the AAMTJ with TiO2 spacer of RuO2/TiO2/NiF2/TiO2/RuO2. Our AAMTJ inherently exhibits low consumption and zero stray field, with nonrelativistic spin splitting and vanishing magnetic moment, combining the advantages of both ferromagnetic and antiferromagnetic tunnel junctions. This AAMTJ paradigm opens an interesting avenue within the area of high-performance altermagnet-based tunnel junctions.

cond-mat.mtrl-sci

Sliding Disassembly of van der Waals Heterostructures

Many recent advances in our understanding of two-dimensional (2D) electron systems stem from van der Waals (vdW) heterostructures. The assembly process relies on the weak bonding across interfaces between layered vdW compounds, making it possible to construct exceptionally clean heterostructures from chemically and structurally distinct materials - a challenging task for traditional thin-film growth techniques. Here we demonstrate an additional, dynamic degree of freedom afforded by vdW interfaces, wherein we use microstructured polymer stamps to disassemble and reconfigure vdW heterostructures by sliding. We apply this technique to alter the dielectric environment of monolayer graphene, perform scanning tunneling microscopy on semiconducting and air-sensitive monolayers, and manipulate strain-sensitive moiré materials. Together these demonstrations suggest a new paradigm for assembling and dynamically modifying van der Waals heterostructures, with the potential to reveal new insights into 2D electron systems.

cond-mat.mes-hall

Optical Band Engineering of Monolayer WSe2 in a Scanning Tunneling Microscope

Intense electromagnetic fields can result in dramatic changes in the electronic properties of solids. These changes are commonly studied using optical probes of the modified electronic structure. Here we use optical-scanning tunneling microscopy (optical-STM) equipped with near-field continuous wave (CW) laser excitation to directly measure the electronic structure of light-dressed states in a monolayer transition metal dichalcogenide (TMD) semiconductor, WSe2. We find that the effective tunneling gap and tunneling density of states are strongly influenced by the intensity of the electromagnetic field when the applied field is resonant with the bandgap of the semiconductor. Our findings indicate that CW laser excitation can be used to generate light-dressed electronic states of quantum materials when confined strongly to the nanoscale.

cond-mat.mtrl-sci

Highly tunable room-temperature plexcitons in monolayer WSe2 /gap-plasmon nanocavities

The advancement of quantum photonic technologies relies on the ability to precisely control the degrees of freedom of optically active states. Here, we realize real-time, room-temperature tunable strong plasmon-exciton coupling in 2D semiconductor monolayers enabled by a general approach that combines strain engineering plus force- and voltage-adjustable plasmonic nanocavities. We show that the exciton energy and nanocavity plasmon resonance can be controllably toggled in concert by applying pressure with a plasmonic nanoprobe, allowing in operando control of detuning and coupling strength, with observed Rabi splittings >100 meV. Leveraging correlated force spectroscopy, nano-photoluminescence (nano-PL) and nano-Raman measurements, augmented with electromagnetic simulations, we identify distinct polariton bands and dark polariton states, and map their evolution as a function of nanogap and strain tuning. Uniquely, the system allows for manipulation of coupling strength over a range of cavity parameters without dramatically altering the detuning. Further, we establish that the tunable strong coupling is robust under multiple pressing cycles and repeated experiments over multiple nanobubbles. Finally, we show that the nanogap size can be directly modulated via an applied DC voltage between the substrate and plasmonic tip, highlighting the inherent nature of the concept as a plexcitonic nano-electro-mechanical system (NEMS). Our work demonstrates the potential to precisely control and tailor plexciton states localized in monolayer (1L) transition metal dichalcogenides (TMDs), paving the way for on-chip polariton-based nanophotonic applications spanning quantum information processing to photochemistry.

physics.optics

Visualizing delocalized correlated electronic states in twisted double bilayer graphene

The discovery of interaction-driven insulating and superconducting phases in moiré van der Waals heterostructures has sparked considerable interest in understanding the novel correlated physics of these systems. While a significant number of studies have focused on twisted bilayer graphene, correlated insulating states and a superconductivity-like transition up to 12 K have been reported in recent transport measurements of twisted double bilayer graphene. Here we present a scanning tunneling microscopy and spectroscopy study of gate-tunable twisted double bilayer graphene devices. We observe splitting of the van Hove singularity peak by ~20 meV at half-filling of the conduction flat band, with a corresponding reduction of the local density of states at the Fermi level. By mapping the tunneling differential conductance we show that this correlated system exhibits energetically split states that are spatially delocalized throughout the different regions in the moiré unit cell, inconsistent with order originating solely from onsite Coulomb repulsion within strongly-localized orbitals. We have performed self-consistent Hartree-Fock calculations that suggest exchange-driven spontaneous symmetry breaking in the degenerate conduction flat band is the origin of the observed correlated state. Our results provide new insight into the nature of electron-electron interactions in twisted double bilayer graphene and related moiré systems.

cond-mat.str-el