arXiv subjects

Benjamin J. Lawrie

Publications and source records attributed to Benjamin J. Lawrie.

At least 19 recordsLinked to original sources

arXiv2026

Probing Boron Vacancy Defects in hBN via Single Spin Relaxometry

Spin defects in solids offer promising platforms for quantum sensing and memory due to their long coherence times and optical addressability. Here, we integrate a single nitrogen-vacancy (NV) center in diamond with scanning probe microscopy to discover, read out, and spatially map arbitrary spin-based quantum sensors at the nanoscale. Using the boron vacancy ($\mathrm{V}_\mathrm{B}^-$) center in hexagonal boron nitride$\unicode{x2013}$an emerging two-dimensional spin system$\unicode{x2013}$as a model, we detect its electron spin resonance indirectly via changes in the spin relaxation time ($T_1$) of a nearby NV center, eliminating the need for optical excitation or fluorescence detection of the $\mathrm{V}_\mathrm{B}^-$. Cross-relaxation between NV and $\mathrm{V}_\mathrm{B}^-$ ensembles significantly reduces NV $T_1$, enabling quantitative nanoscale mapping of defect densities beyond the optical diffraction limit and clear resolution of hyperfine splitting in isotopically enriched h$^{10}$B$^{15}$N. Our method demonstrates interactions between 3D and 2D spin sensors, establishing NV centers as versatile probes for characterizing otherwise inaccessible spin defects.

cond-mat.mtrl-sci↗

arXiv2026

Photonic Links for Spin-Based Quantum Sensors

A growing variety of optically accessible spin qubits have emerged in recent years as key components for quantum sensors, qubits, and quantum memories. However, the scalability of conventional spin-based quantum architectures remains limited by direct microwave delivery, which introduces thermal noise, electromagnetic cross-talk, and design constraints for cryogenic, high-field, and distributed systems. In this work, we present a unified framework for RF-over-fiber (RFoF) control of optically accessible spins through RFoF optically detected magnetic resonance (ODMR) spectroscopy of nitrogen-vacancy (NV) centers in diamond. The RFoF platform relies on an electro-optically modulated telecom-band laser that transmits microwave signals over fiber and a high-speed photodiode that recovers the RF waveform to drive NV center spin transitions. We obtain an RFoF efficiency of 1.81\% at 2.90~GHz, corresponding to $P_{\mathrm{RF,out}}=-0.7$~dBm. The RFoF architecture provides a path toward low-noise, thermally isolated, and cryo-compatible ODMR systems bridging conventional spin-based quantum sensing protocols with emerging distributed quantum technologies.

quant-ph↗

arXiv2025

Real-space visualization of orbital-selective superconductivity in FeSe

We investigate the orbitally resolved superconducting properties of bulk FeSe using scanning tunneling microscopy (STM). We find that the spectral weights of both the large $Δ_1$ and small $Δ_2$ superconducting gaps remain nearly unchanged at the top Se sites as the STM tip approaches atomic contact. In contrast, the spectral weight of $Δ_2$ increases significantly at the Fe and bottom Se sites. These results suggest that the gap $Δ_2$ is localized in the xy-plane and likely associated with the dxy orbital band. Furthermore, we observe a long-range suppression of the large gap $Δ_1$ near one-dimensional (1D) defects such as twin boundaries, wrinkles, and step edges, whereas $Δ_2$ remains robust. This indicates that the two superconducting gaps respond differently to such 1D defects. High-resolution measurement using a Pb-coated tip reveals localized in-gap states near 1D defects, indicating possible defect-induced magnetism. Our findings highlight the contrasting behaviors of gap $Δ_1$ and gap $Δ_2$ in response to local electronic and magnetic environments and provide real-space evidence for orbital-selective superconductivity.

cond-mat.supr-con↗

arXiv2024

Non-perturbative cathodoluminescence microscopy of beam-sensitive materials

Cathodoluminescence microscopy is now a well-established and powerful tool for probing the photonic properties of nanoscale materials, but in many cases, nanophotonic materials are easily damaged by the electron-beam doses necessary to achieve reasonable cathodoluminescence signal-to-noise ratios. Two-dimensional materials have proven particularly susceptible to beam-induced modifications, yielding both obstacles to high spatial-resolution measurement and opportunities for beam-induced patterning of quantum photonic systems. Here pan-sharpening techniques are applied to cathodoluminescence microscopy in order to address these challenges and experimentally demonstrate the promise of pan-sharpening for minimally-perturbative high-spatial-resolution spectrum imaging of beam-sensitive materials.

physics.optics↗

arXiv2024

Nanoscale control over single vortex motion in an unconventional superconductor

To realize braiding of vortex lines and understand the basic properties of the energy landscape for vortex motion, precise manipulation of superconducting vortices on the nanoscale is required. Here, we reveal that a localized trapping potential powerful enough to pull in the vortex line can be created with nanoscale precision on the surface of an FeSe superconductor using the tip of a scanning tunneling microscope. The mechanism of tip-induced force is traced to local modification of electronic properties and reduction of the superconducting gap, most likely due to tip-induced strain. Intriguingly, the tip-induced trapping potential is much less pronounced along the twin boundaries, dramatically reducing the vortice's degree of motion relative to the surrounding lattice. By enabling nanoscale manipulation of single vortices in Fe-based superconductors, and likely similar materials with strong strain-susceptibility of the superconducting gap, our findings provide an important step toward further development of vortex-based quantum information processing.

cond-mat.supr-con↗

arXiv2024

Nanoscale magnetic ordering dynamics in a high Curie temperature ferromagnet

Thermally driven transitions between ferromagnetic and paramagnetic phases are characterized by critical behavior with divergent susceptibilities, long-range correlations, and spin dynamics that can span kHz to GHz scales as the material approaches the critical temperature $\mathrm{T_c}$, but it has proven technically challenging to probe the relevant length and time scales with most conventional measurement techniques. In this study, we employ scanning nitrogen-vacancy center based magnetometry and relaxometry to reveal the critical behavior of a high-$\mathrm{T_c}$ ferromagnetic oxide near its Curie temperature. Cluster analysis of the measured temperature-dependent nanoscale magnetic textures points to a 3D universality class with a correlation length that diverges near $\mathrm{T_c}$. Meanwhile, the temperature-dependent spin dynamics, measured through all optical relaxometry suggest that the phase transition is in the XY universality class. Our results capture both static and dynamic aspects of critical behavior, providing insights into universal properties that govern phase transitions in magnetic materials.

cond-mat.mtrl-sci↗

arXiv2023

Parallel Quantum-Enhanced Sensing

Quantum metrology takes advantage of quantum correlations to enhance the sensitivity of sensors and measurement techniques beyond their fundamental classical limit given by the shot noise limit. The use of both temporal and spatial correlations present in quantum states of light can extend quantum-enhanced sensing to a parallel configuration that can simultaneously probe an array of sensors or independently measure multiple parameters. To this end, we use multi-spatial mode twin beams of light, which are characterized by independent quantum-correlated spatial subregions in addition to quantum temporal correlations, to probe a four-sensor quadrant plasmonic array. We show that it is possible to independently and simultaneously measure local changes in refractive index for all four sensors with a quantum enhancement in sensitivity in the range of $22\%$ to $24\%$ over the corresponding classical configuration. These results provide a first step towards highly parallel spatially resolved quantum-enhanced sensing techniques and pave the way toward more complex quantum sensing and quantum imaging platforms.

quant-ph↗

arXiv2023

Emergent magnetism with continuous control in the ultrahigh conductivity layered oxide PdCoO2

The current challenge to realizing continuously tunable magnetism lies in our inability to systematically change properties such as valence, spin, and orbital degrees of freedom as well as crystallographic geometry. Here, we demonstrate that ferromagnetism can be externally turned on with the application of low-energy helium implantation and subsequently erased and returned to the pristine state via annealing. This high level of continuous control is made possible by targeting magnetic metastability in the ultra-high conductivity, non-magnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce emergence of a net moment on the surrounding transition metal octahedral sites. These highly-localized moments communicate through the itinerant metal states which triggers the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultra-high conductivity film and will be critical to applications across spintronics.

cond-mat.mtrl-sci↗

arXiv2023

Quantum Enhanced Probes of Magnetic Circular Dichroism

Magneto-optical microscopies, including optical measurements of magnetic circular dichroism, are increasingly ubiquitous tools for probing spin-orbit coupling, charge-carrier g-factors, and chiral excitations in matter, but the minimum detectable signal in classical magnetic circular dichroism measurements is fundamentally limited by the shot-noise limit of the optical readout field. Here, we use a two-mode squeezed light source to improve the minimum detectable signal in magnetic circular dichroism measurements by 3 dB compared with state-of-the-art classical measurements, even with relatively lossy samples like terbium gallium garnet. We also identify additional opportunities for improvement in quantum-enhanced magneto-optical microscopies, and we demonstrate the importance of these approaches for environmentally sensitive materials and for low temperature measurements where increased optical power can introduce unacceptable thermal perturbations.

quant-ph↗

arXiv2023

Photophysics of Intrinsic Single-Photon Emitters in Silicon Nitride at Low Temperatures

A robust process for fabricating intrinsic single-photon emitters in silicon nitride has been recently established. These emitters show promise for quantum applications due to room-temperature operation and monolithic integration with the technologically mature silicon nitride photonics platform. Here, the fundamental photophysical properties of these emitters are probed through measurements of optical transition wavelengths, linewidths, and photon antibunching as a function of temperature from 4.2K to 300K. Important insight into the potential for lifetime-limited linewidths is provided through measurements of inhomogeneous and temperature-dependent homogeneous broadening of the zero-phonon lines. At 4.2K, spectral diffusion was found to be the main broadening mechanism, while time-resolved spectroscopy measurements revealed homogeneously broadened zero-phonon lines with instrument-limited linewidths.

quant-ph↗

arXiv2022

Disentangling electronic transport and hysteresis at individual grain boundaries in hybrid perovskites via automated scanning probe microscopy

Underlying the rapidly increasing photovoltaic efficiency and stability of metal halide perovskites (MHPs) is the advance in the understanding of the microstructure of polycrystalline MHP thin film. Over the past decade, intense efforts have aimed to understand the effect of microstructure on MHP properties, including chemical heterogeneity, strain disorder, phase impurity, etc. It has been found that grain and grain boundary (GB) are tightly related to lots of microscale and nanoscale behavior in MHP thin film. Atomic force microscopy (AFM) is widely used to observe grain and boundary structures in topography and subsequently to study the correlative surface potential and conductivity of these structures. For now, most AFM measurements have been performed in imaging mode to study the static behavior, in contrast, AFM spectroscopy mode allows us to investigate the dynamic behavior of materials, e.g. conductivity under sweeping voltage. However, a major limitation of AFM spectroscopy measurements is that it requests manual operation by human operators, as such only limited data can be obtained, hindering systematic investigations of these microstructures. In this work, we designed a workflow combining the conductive AFM measurement with a machine learning (ML) algorithm to systematically investigate grain boundaries in MHPs. The trained ML model can extract GBs locations from the topography image, and the workflow drives the AFM probe to each GB location to perform a current-voltage (IV) curve automatically. Then, we are able to IV curves at all GB locations, allowing us to systematically understand the property of GBs. Using this method, we discover that the GB junction points are more photoactive, while most previous works only focused on the difference between GB and grains.

cond-mat.mtrl-sci↗

arXiv2022

Surface-Driven Evolution of the Anomalous Hall Effect in Magnetic Topological Insulator MnBi2Te4 Thin Films

Understanding the effects of interfacial modification to the functional properties of magnetic topological insulator thin films is crucial for developing novel technological applications from spintronics to quantum computing. Here, we report that a large electronic and magnetic response is induced in the intrinsic magnetic topological insulator MnBi2Te4 by controlling the propagation of surface oxidation. We show that the formation of the surface oxide layer is confined to the top 1-2 unit cells but drives large changes in the overall magnetic response. Specifically, we observe a dramatic reversal of the sign of the anomalous Hall effect driven by finite thickness magnetism, which indicates that the film splits into distinct magnetic layers each with a unique electronic signature. These data reveal a delicate dependence of the overall magnetic and electronic response of MnBi2Te4 on the stoichiometry of the top layers. Our study suggests that perturbations resulting from surface oxidation may play a non-trivial role in the stabilization of the quantum anomalous Hall effect in this system and that understanding targeted modifications to the surface may open new routes for engineering novel topological and magnetic responses in this fascinating material.

cond-mat.mtrl-sci↗

arXiv2022

Phonon Chirality Induced by Vibronic-Orbital Coupling

The notion that phonons can carry pseudo-angular momentum has become popular in the last decade, with recent research efforts highlighting phonon chirality, Berry curvature of phonon band structure, and the phonon Hall effect. When a phonon is resonantly coupled to a crystal electric field excitation, a so-called vibronic bound state forms. Here, we observe angular momentum transfer of $δ$Jz = $\pm$1$\hbar$ between phonons and an orbital state in a vibronic bound state of a candidate quantum spin liquid. This observation has profound implications for the engineering of phonon band structure topology through chiral quasiparticle interactions.

cond-mat.mes-hall↗

arXiv2022

Angle-Resolved Cathodoluminescence Polarimetry of Hybrid Perovskites

Coupling between light and matter strongly depends on the polarization of the electromagnetic field and the nature of the excitations in the material. As hybrid perovskites emerge as a promising class of materials for light-based technologies like LEDs, lasers, and photodetectors, understanding the microscopic details of how photons couple to matter is critical. While most optical studies have focused on the spectral content and quantum efficiency of emitted photons in various hybrid perovskite thin-film and nanoscale structures, few studies have explored other properties of the emitted photons such as polarization and emission angle. Here, we use angle-resolved cathodoluminescence microscopy to access the full polarization state of photons emitted from large-grain hybrid perovskite films with spatial resolution well below the optical diffraction limit. Mapping the Stokes parameters as a function of the emission angle in a thin film, we reveal the effect of a grain boundary on the degree of polarization and angle at which the photons are emitted. This exploration of angle- and polarization-resolved emission near grain boundaries provides an improved understanding of the emission properties of hybrid perovskites in thin film geometries -- a necessary investigation for subsequent engineering of subwavelength nanophotonic structures using the hybrid perovskite class of materials.

cond-mat.mes-hall↗

arXiv2022

Hyperspectral nanoscale mapping of hybrid perovskite photophysics at the single grain level

Hybrid organic-inorganic perovskites have drawn significant interest for applications in optoelectronics over the last few years. Despite rapid progress in understanding the photophysics of perovskite, there remains a need for improved understanding of the effect of microstructure on perovskite photophysical processes. Here, we combine unsupervised machine learning and cathodoluminescence microscopy of a prototypical hybrid perovskite film to decode photophysical processes that are otherwise lost with conventional Gaussian image processing. Hyperspectral maps are decoded with non-negative matrix factorization, revealing components relating to primary band-edge emission, photon recycling, and defect emission. A blind-spectral non-negative matrix factorization procedure provides additional understanding of changes in an intermediate perovskite phase under electron beam exposure and illustrates how traditional Gaussian techniques may hide relevant emission features that are critical to the development of environmentally robust perovskite devices

cond-mat.mes-hall↗

arXiv2021

Advanced Architectures for High-Performance Quantum Networking

As practical quantum networks prepare to serve an ever-expanding number of nodes, there has grown a need for advanced auxiliary classical systems that support the quantum protocols and maintain compatibility with the existing fiber-optic infrastructure. We propose and demonstrate a quantum local area network design that addresses current deployment limitations in timing and security in a scalable fashion using commercial off-the-shelf components. We employ White Rabbit switches to synchronize three remote nodes with ultra-low timing jitter, significantly increasing the fidelities of the distributed entangled states over previous work with Global Positioning System clocks. Second, using a parallel quantum key distribution channel, we secure the classical communications needed for instrument control and data management. In this way, the conventional network which manages our entanglement network is secured using keys generated via an underlying quantum key distribution layer, preserving the integrity of the supporting systems and the relevant data in a future-proof fashion.

quant-ph↗

arXiv2021

Nearly-Resonant Crystalline-Phononic Coupling in Quantum Spin Liquid Candidate CsYbSe$_2$

CsYbSe$_2$, a recently identified quantum spin liquid (QSL) candidate, exhibits strong crystal electric field (CEF) excitations. Here, we identify phonon and CEF modes with Raman spectroscopy and observe strong CEF-phonon mixing resulting in a vibronic bound state. Complex, mesoscale interplay between phonon modes and CEF modes is observed in real space, and an unexpected nearly resonant condition is satisfied, yielding up to fifth-order combination modes, with a total of 17 modes identified in the spectra. This study paves the way to coherent control of possible QSL ground states with optically accessible CEF-phonon manifolds and mesoscale engineering of CEF-phonon interactions.

cond-mat.str-el↗

arXiv2021

Self-regulated growth of candidate topological superconducting parkerite by molecular beam epitaxy

Ternary chalcogenides such as the parkerites and shandites are a broad class of materials exhibiting rich diversity of transport and magnetic behavior as well as an array of topological phases including Weyl and Dirac nodes. However, they remain largely unexplored as high-quality epitaxial thin films. Here, we report the self-regulated growth of thin films of the strong spin-orbit coupled superconductor Pd3Bi2Se2 on SrTiO3 by molecular beam epitaxy. Films are found to grow in a self-regulated fashion, where, in excess Se, the temperature and relative flux ratio of Pd to Bi controls the formation of Pd3Bi2Se2 due to the combined volatility of Bi, Se, and Bi-Se bonded phases. The resulting films are shown to be of high structural quality, the stoichiometry is independent of the Pd:Bi and Se flux ratio and exhibit a superconducting transition temperature of 800 mK and critical field of 17.7 +/- 0.5 mT, as probed by transport as well as magnetometry. Understanding and navigating the growth of the chemically and structurally diverse classes of ternary chalcogenides opens a vast space for discovering new phenomena as well as enabling new applications.

cond-mat.mtrl-sci↗