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DOE OSTI2025

Spin-filter tunneling detection of antiferromagnetic resonance with electrically tunable damping

Antiferromagnetic spintronics offers the potential for higher-frequency operations and improved insensitivity to magnetic fields compared to ferromagnetic spintronics. However, previous electrical techniques to detect antiferromagnetic dynamics have utilized large, millimeter-scale bulk crystals. In this work, we demonstrate direct electrical detection of antiferromagnetic resonance in structures on the few-micrometer scale using spin-filter tunneling in platinum ditelluride (PtTe 2 )/bilayer chromium sulfide bromide (CrSBr)/graphite junctions in which the tunnel barrier is the van der Waals antiferromagnet CrSBr. This sample geometry allows not only efficient detection but also electrical control of the antiferromagnetic resonance through spin-orbit torque from the PtTe 2 electrode. The ability to efficiently detect and control antiferromagnetic resonance enables detailed studies of the physics governing these high-frequency dynamics.

Cham, Thow Min Jerald [Cornell University, Ithaca,↗

DOE OSTI2024

Extraordinary phase transition revealed in a van der Waals antiferromagnet

While the surface-bulk correspondence has been ubiquitously shown in topological phases, the relationship between surface and bulk in Landau-like phases is much less explored. Theoretical investigations since 1970s for semi-infinite systems have predicted the possibility of the surface order emerging at a higher temperature than the bulk, clearly illustrating a counterintuitive situation and greatly enriching phase transitions. But experimental realizations of this prediction remain missing. Here, we demonstrate the higher-temperature surface and lower-temperature bulk phase transitions in CrSBr, a van der Waals (vdW) layered antiferromagnet. We leverage the surface sensitivity of electric dipole second harmonic generation (SHG) to resolve surface magnetism, the bulk nature of electric quadrupole SHG to probe bulk spin correlations, and their interference to capture the two magnetic domain states. Our density functional theory calculations show the suppression of ferromagnetic-antiferromagnetic competition at the surface is responsible for this enhanced surface magnetism. Our results not only show counterintuitive, richer phase transitions in vdW magnets, but also provide viable ways to enhance magnetism in their 2D form.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Magnon-mediated exciton–exciton interaction in a van der Waals antiferromagnet

Excitons are fundamental excitations that govern the optical properties of semiconductors. Interactions between excitons can lead to various emergent phases of matter and large nonlinear optical responses. In most semiconductors, excitons interact via exchange interactions or phase-space filling. Correlated materials that host excitons coupled to other degrees of freedom could offer pathways for controlling these interactions. Here, in this study, we demonstrate magnon-mediated interactions between excitons in CrSBr, an antiferromagnetic semiconductor. These interactions manifest as the dependence of the exciton energy on the exciton density via a magnonic adjustment of the spin canting angle. Our study demonstrates the emergence of quasiparticle-mediated interactions in correlated quantum materials, leading to large nonlinear optical responses and potential device concepts such as magnon-mediated quantum transducers.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Field-resolved observation of exciton coherence in a van der Waals magnet

The emergence of coherence among electronic quasiparticles underlies collective quantum phenomena from superconductivity to superradiance. In semiconductors, exciton coherence is generally thought to decay rapidly due to scattering and dephasing, limiting its persistence on ultrafast timescales. Here, in this work, we demonstrate a light-field-driven mechanism that creates and stabilizes exciton coherence in the layered antiferromagnet CrSBr. We directly record the coherent optical field emitted by excitons and track in real time how a deterministic phase, imprinted by the excitation laser, drives incoherent excitons to synchronize into a collective state. This ensemble remains phase coherent for more than 2 ps, whereas its resonance energy undergoes an ultrafast modulation mediated by spin and lattice interactions. The time-resolved field evolution indicates that the multiple peaks seen in conventional spectra originate from a single excitonic resonance subject to dynamic energy modulation. Our findings establish optical phase imprinting as a mechanism to control and sustain collective order in semiconducting magnets, bridging light-driven dynamics with excitonic and magnetic correlations in layered quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Tunable interaction between excitons and hybridized magnons in a layered semiconductor

The interaction between distinct excitations in solids is of both fundamental interest and technological importance. One example of such interactions is coupling between an exciton, a Coulomb bound electron-hole pair, and a magnon, a collective spin excitation. The recent emergence of van der Waals magnetic semiconductors1 provides a powerful platform for exploring these exciton-magnon interactions and their fundamental properties, such as strong correlation2, as well as their photo-spintronic and quantum transduction3 applications. Here we demonstrate precise control of coherent exciton-magnon interactions in the layered magnetic semiconductor CrSBr. We show that by controlling the direction of applied magnetic fields relative to the crystal axes, and thus the rotational symmetry of the magnetic system4, we can tune not only the exciton coupling to the bright magnon, but also to an optically dark mode via magnon hybridization. The exciton-magnon coupling and associated magnon dispersion curves can be further modulated by applying a uniaxial strain. At the critical strain, a dispersionless dark magnon band emerges. Our results demonstrate unprecedented control of the opto-mechanical-magnonic coupling, and a step towards the predictable and controllable implementation of hybrid quantum magnonics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2025

Exciton dressing by extreme nonlinear magnons in a layered semiconductor

Collective excitations presenting nonlinear dynamics are fundamental phenomena with broad applications. A prime example is nonlinear optics, where diverse frequency mixing processes are central to communication, sensing, wavelength conversion, and attosecond physics. Leveraging recent progress in van der Waals magnetic semiconductors, we demonstrate nonlinear opto-magnonic coupling by presenting exciton states dressed by up to 20 harmonics of magnons, resulting from their nonlinearities, in the layered antiferromagnetic semiconductor CrSBr. We also create tunable optical side bands from sum- and difference-frequency generation between two optically bright magnon modes under symmetry breaking magnetic fields. Moreover, the observed difference-frequency generation mode can be continuously tuned into resonance with one of the fundamental magnons, resulting in parametric amplification of magnons. These findings realize the modulation of the optical frequency exciton with the extreme nonlinearity of magnons at microwave frequencies, which could find applications in magnonics and hybrid quantum systems, and provide new avenues for implementing opto-magnonic devices.

Diederich, Geoffrey M.↗

DOE OSTI2026

Mesoscale atomic engineering in a crystal lattice

Controlling individual atoms using lasers, ion traps and scanning probe tips has transformed our understanding of matter and enabled breakthroughs in quantum science. Extending this control into three-dimensional (3D) solids and across mesoscopic scales, however, remains a foundational challenge. Electron irradiation in electron microscopes is known to induce atomic displacements, and atomic manipulation has been proposed and demonstrated. Yet repeated and deterministic control has remained elusive. Here, in this study, we demonstrate deterministic atomic engineering in a 3D crystal, creating ordered arrangements of more than 40,000 user-defined defects within minutes across a 150 nm × 100 nm × 13 nm volume. By steering individual Cr atoms in the magnetic semiconductor CrSBr into selected interstitial sites using an electron beam directed with sub-20-pm-scale accuracy, we create vacancy–interstitial complexes. The resulting impurity array forms a mesoscale crystal embedded within the host lattice, a new form of engineered artificial matter that remains stable at room temperature and outside the microscope. By tracking Cr atom displacements, we identify conditions under which the defect structures are predictable. Our calculations suggest that these defects form correlated impurity states with intra-defect optical transitions and inter-defect kinetic and Coulomb interactions. This establishes a generalizable platform for atomic defect engineering at mesoscopic, and potentially macroscopic, scales, opening opportunities for scalable quantum technologies, including deterministic colour-centre placement, quantum simulation of many-body lattice models and atomic-scale manufacturing.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2026

Creation of depth-confined, shallow nitrogen-vacancy centers in diamond with tunable density

Engineering shallow nitrogen-vacancy (NV) centers in diamond holds the key to unlocking new advances in nanoscale quantum sensing. We find that the creation of near-surface NVs through delta doping during diamond growth allows for tunable control over both NV depth confinement (with a twofold improvement relative to low-energy ion implantation) and NV density, ultimately resulting in highly sensitive single defects and ensembles with coherence limited by NV–NV interactions. Additionally, we demonstrate the utility of our shallow delta-doped NVs by imaging magnetism in few-layer CrSBr, a two-dimensional magnet. Here, we anticipate that the control afforded by near-surface delta doping will enable new developments in NV quantum sensing from nanoscale nuclear magnetic resonance to entanglement-enhanced metrology.

Chemical vapor deposition↗

DOE OSTI2022

Spin injection by spin–charge coupling in proximity induced magnetic graphene

Abstract Within the field of spintronics major efforts are directed towards developing applications for spin-based transport devices made fully out of two-dimensional materials. In this work we present an experimental realization of a spin-valve device where the generation of the spin signal is exclusively attributed to the spin-dependent conductivity of the magnetic graphene resulting from the proximity of an interlayer antiferromagnet, chromium sulfide bromide (CrSBr). We clearly demonstrate that the usage of the conventional air-sensitive 3D magnetic contacts can be fully avoided when graphene/CrSBr heterostructures are employed. Moreover, apart from providing exceptionally long spin relaxation length, the usage of graphene for both generation and transport of the spin allows to automatically avoid the conductivity mismatch between the source and the channel circuits that has to be considered when using conventional low-resistive contacts. Our results address a necessary step in the engineering of spintronic circuitry out of layered materials and precede further developments in the area of complex spin-logic devices. Moreover, we introduce a fabrication procedure where we designed and implemented a recipe for the preparation of electrodes via a damage-free technique that offers an immediate advantage in the fields of air-sensitive and delicate organic materials.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Electron Beam-Induced Phase Transformations in Different Crystal Orientations of a 2D van der Waals Magnet

To control materials properties at the nanoscale, the well-focused electron beam of the scanning transmission electron microscope (STEM) can be used as a tool to engineer structure with atomic precision. For 2D magnets, especially the highly anisotropic materials AgCrP2S6 and CrSBr, we find here that the STEM serves as a powerful tool for sculpting the arrangement of atoms, with the potential to modulate local magnetic properties.

Park, Eugene [Massachusetts Inst. of Technology (M↗

DOE OSTI2026

Space-Charge-Limited van der Waals Spin Transistor

Integrating semiconducting and magnetic materials could combine transistorlike operation with nonvolatility and enable architectures such as logic in memory. Here, in this work, we employ correlated electrical transport and scanning nitrogen-vacancy center magnetic imaging to elucidate a spin transistor concept that amalgamates vertical and lateral hopping transport inside a 2D antiferromagnetic semiconductor, mechanistically distinct from vertical tunneling devices. Our device, based on a monolayer-bilayer junction in CrSBr, displays giant, gate-tunable magnetoresistance driven by the dual action of electrostatic doping on space-charge-limited lateral conduction and interlayer exchange coupling. Moreover, we visualize a field-trainable, layer-sharing effect that selects between coherent or domain-wall reversal at the spin-flip transition, enabling multilevel, memristive conductance states. Our layer-dependent space charge mechanism for convergent electrical and magnetic control opens opportunities to address limitations in contemporary computing.

2-dimensional systems↗

DOE OSTI2025

Twist Engineering of Anisotropic Excitonic and Optical Properties of a Two-Dimensional Magnetic Semiconductor

Two-dimensional (2D) van der Waals (vdW) magnetic semiconductors are a new class of quantum materials for studying the emergent physics of excitons and spins in the 2D limit. Twist engineering provides a powerful tool to manipulate the fundamental properties of 2D vdW materials. Here, in this work, we show that twist engineering of the anisotropic ferromagnetic monolayer semiconductor CrSBr leads to bilayer magnetic semiconductors with continuously tunable magnetic moment, dielectric anisotropy, exciton energy, and linear dichroism. We furthermore provide a model for exciton energy in the media with tunable anisotropy. These results advance fundamental studies of 2D vdW materials and open doors to applications to nano-optics, twistronics, and spintronics.

36 MATERIALS SCIENCE↗