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Lee C. Bassett

Publications and source records attributed to Lee C. Bassett.

At least 19 recordsLinked to original sources

High-Performance Near-Infrared Quantum Emission from Color Centers in hBN

Color centers hosted in hexagonal boron nitride have emerged as a highly promising platform for single-photon emission and spin-photon technologies relevant to quantum communication and quantum networking. As a wide-bandgap van der Waals material, hBN can host optically active quantum defects across a broad spectral range. Here, we demonstrate a simple and scalable oxygen-plasma process that reproducibly creates single quantum emitters in hBN with blinking-free zero-phonon lines spanning the near-infrared from 700 up to 971 nm. These emitters combine MHz-level brightness, single-photon purity up to 99.9\%, and ultranarrow cryogenic linewidths down to 2.7~GHz under quasi-resonant excitation, placing them in a particularly attractive regime for quantum photonics. Photostability measurements further reveal resistance to photobleaching, sub-nm spectral stability over long timescales, and near-shot-noise-limited intensity fluctuations. Analysis of the phonon sidebands shows weak vibronic coupling and ZPL-dominated emission, with Debye--Waller factors approaching 50\%. Control experiments together with EDS elemental mapping support oxygen incorporation as a necessary ingredient in activating the NIR emitter population, while first-principles calculations identify O$_N$V$_N$ and O$_N$V$_N$H as the leading defect candidates. These results establish a high-performance NIR quantum-emitter platform in hBN for free-space quantum networking and future integrated quantum-photonic architectures.

quant-ph↗

Single-gate, multipartite entanglement on a room-temperature quantum register

Multipartite entanglement is an essential aspect of quantum systems, needed to execute quantum algorithms, implement error correction, and achieve quantum-enhanced sensing. In solid-state quantum registers such nitrogen-vacancy (NV) centers in diamond, entangled states are typically created using sequential, pairwise gates between the central electron and individual nuclear qubits. This sequential approach is slow and suffers from crosstalk errors. Here, we demonstrate a parallelized multi-qubit entangling gate to generate a four-qubit GHZ state using a room-temperature NV center in only 14.8 $μ$s $-$ 10 times faster than using sequences of two-qubit gates and close to the fundamental limit set by the hyperfine coupling frequencies. Parallel three-qubit gates are also realized with all nuclear-qubit subsets. The entangled states are verified by measuring multiple quantum coherences. The four-qubit parallel gate has a fidelity of 0.92(4), whereas the sequential four-qubit gate fidelity is only 0.69(3). The approach is generalizable to other solid-state platforms, and it lays the foundation for scalable generation and control of entanglement in practical devices.

quant-ph↗

Site-selective enhancement of Eu emission in delta-doped GaN

Europium-doped gallium nitride (GaN:Eu) is a promising platform for classical and quantum optoelectronic applications. When grown using organometallic vapor-phase epitaxy, the dominant red emission from Eu exhibits an inhomogeneous photoluminescence (PL) spectrum due to contributions from several non-equivalent incorporation sites that can be distinguished with combined excitation emission spectroscopy. Energy transfer from the GaN bandgap to the majority site is inefficient, limiting the performance of GaN:Eu LEDs and resulting in an inhomogeneous emission spectrum dominated by disproportionate contributions from minority sites. In this work, we use site-selective spectroscopy to characterize the photoluminescence properties of delta-doped structures with alternating doped and undoped layers of varying thicknesses and demonstrate that they selectively enhance emission from the majority site when compared to uniformly-doped samples. Samples with 2-nm and 10-nm doped layers show much greater PL intensity per Eu concentration as well as more efficient energy transfer to the majority site, which are both highly desirable for creating power-efficient LEDs. Meanwhile, a sample with 1-nm doped layers shows emission only from the majority site, resulting in a narrow, homogeneous emission spectrum that is desirable for quantum technologies. This utilization of delta-doping has the potential to be broadly applicable for engineering desirable defect properties in rare-earth doped semiconductors.

cond-mat.mtrl-sci↗

Room-temperature quantum emission from $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects in ZnS:Cu colloidal nanocrystals

We report room-temperature observations of $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ quantum emitters in individual ZnS:Cu nanocrystals (NCs). Using time-gated imaging, we isolate the distinct, $\sim$3-$μ$s-long, red photoluminescence (PL) emission of $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects, enabling their precise identification and statistical characterization. The emitters exhibit distinct blinking and photon antibunching, consistent with individual NCs containing two to four $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects. The quantum emitters' PL spectra show a pronounced blue shift compared to NC dispersions, likely due to photochemical and charging effects. Emission polarization measurements of quantum emitters are consistent with a $σ$-character optical dipole transition and the symmetry of the $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defect. These observations motivate further investigation of $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects in ZnS NCs for use in quantum technologies.

cond-mat.mes-hall↗

Excitation and inhibition imbalance affects dynamical complexity through symmetries

From the perfect radial symmetries of radiolarian mineral skeletons to the broken symmetry of homochirality, the logic of Nature's regularities has fascinated scientists for centuries. Some of Nature's symmetries are clearly visible in morphology and physical structure, whereas others are hidden in the network of interactions among system components. Just as visible symmetries and asymmetries contribute to the system's beauty, might hidden symmetries contribute to the system's functional harmony? And if so, how? Here we demonstrate that the interaction networks of biological systems from cell signaling to cancer display a form of dynamical reflection symmetry that serves to expand their dynamical complexity. The expansion proceeds according to precise rules regarding the lengths of dynamical cycles, made possible by a peculiar imbalance between excitation and inhibition. To probe the conditions under which this reflection symmetry evolves, we use a multi-objective genetic algorithm to produce networks with long dynamical cycles. We find that local structural motifs that break the reflection symmetry are deleted in the evolutionary process, providing evidence for symmetry's causal role in dynamical complexity. Finally, we identify symmetries in real continuous-valued scRNA-seq data of gene expression in drug-resistant cancer cells. Broadly, our work reveals a class of hidden symmetries in biology, present in the network of interactions among system components, and it underscores their functional importance. Mathematically simple and computational inexpensive, our approach is applicable to the types of biological data commonly acquired in modern experiments.

physics.bio-ph↗

Mechanical prions: Self-assembling microstructures

Prions are misfolded proteins that transmit their structural arrangement to neighboring proteins. In biological systems, prion dynamics can produce a variety of complex functional outcomes. Yet, an understanding of prionic causes has been hampered by the fact that few computational models exist that allow for experimental design, hypothesis testing, and control. Here, we identify essential prionic properties and present a biologically inspired model of prions using simple mechanical structures capable of undergoing complex conformational change. We demonstrate the utility of our approach by designing a prototypical mechanical prion and validating its properties experimentally. Our work provides a design framework for harnessing and manipulating prionic properties in natural and artificial systems.

cond-mat.soft↗

Quadrupolar resonance spectroscopy of individual nuclei using a room-temperature quantum sensor

Nuclear quadrupolar resonance (NQR) spectroscopy reveals chemical bonding patterns in materials and molecules through the unique coupling between nuclear spins and local fields. However, traditional NQR techniques require macroscopic ensembles of nuclei to yield a detectable signal, which precludes the study of individual molecules and obscures molecule-to-molecule variations due to local perturbations or deformations. Optically active electronic spin qubits, such as the nitrogen-vacancy (NV) center in diamond, facilitate the detection and control of individual nuclei through their local magnetic couplings. Here, we use NV centers to perform NQR spectroscopy on their associated nitrogen-14 ($^{14}$N) nuclei at room temperature. In mapping the nuclear quadrupolar Hamiltonian, we resolve minute variations between individual nuclei. The measurements further reveal correlations between the parameters in the NV center's electronic spin Hamiltonian and the $^{14}$N quadropolar Hamiltonian, as well as a previously unreported Hamiltonian term that results from symmetry breaking. We further design pulse sequences to initialize, readout, and control the quantum evolution of the $^{14}$N nuclear state using the nuclear quadrupolar Hamiltonian.

cond-mat.mes-hall↗

Electronic Noise Considerations for Designing Integrated Solid-State Quantum Memories

As quantum networks expand and are deployed outside research laboratories, a need arises to design and integrate compact control electronics for each memory node. It is essential to understand the performance requirements for such systems, especially concerning tolerable levels of noise, since these specifications dramatically affect a system's design complexity and cost. Here, using an approach that can be easily generalized across quantum-hardware platforms, we present a case study based on nitrogen-vacancy (NV) centers in diamond. We model and experimentally verify the effects of phase noise and timing jitter in the control system in conjunction with the spin qubit's environmental noise. We further consider the impact of different phase noise characteristics on the fidelity of dynamical decoupling sequences. The results demonstrate a procedure to specify design requirements for integrated quantum control signal generators for solid-state spin qubits, depending on their coherence time, intrinsic noise spectrum, and required fidelity.

quant-ph↗

Correlated Structural and Optical Characterization of Hexagonal Boron Nitride

Hexagonal boron nitride (hBN) plays a central role in nanoelectronics and nanophotonics. Moreover, hBN hosts room-temperature quantum emitters and optically addressable spins, making it promising for quantum sensing and quantum photonics. Despite many investigations of their optical properties, however, the emitters' chemical structure remains unclear, as does the role of contamination at surfaces and interfaces in forming the emitters or modifying their properties. We prepare hBN samples that are compatible with confocal photoluminescence (PL) microscopy, transmission electron microscopy (TEM), and atomic-force microscopy (AFM), and we use those techniques to quantitatively investigate correlations between fluorescent emission, flake morphology, and surface residue. We find that the microscopy techniques themselves induce changes in hBN's optical activity and residue morphology: PL measurements induce photobleaching, whereas TEM measurements alter surface residue and emission characteristics. We also study the effects of common treatments $\unicode{x2014}$ annealing and oxygen plasma cleaning $\unicode{x2014}$ on the structure and optical activity of hBN. The methods can be broadly applied to study two-dimensional materials, and the results illustrate the importance of correlative studies to elucidate structural factors that influence hBN's functionality as a host for quantum emitters and spin defects.

cond-mat.mtrl-sci↗

Designing metasurface optical interfaces for solid-state qubits using many-body adjoint shape optimization

We present a general strategy for the inverse design of metasurfaces composed of elementary shapes. We use it to design a structure that collects and collimates light from nitrogen-vacancy centers in diamond. Such metasurfaces constitute scalable optical interfaces for solid-state qubits, enabling efficient photon coupling into optical fibers and eliminating free-space collection optics. The many-body shape optimization strategy is a practical alternative to topology optimization that explicitly enforces material and fabrication constraints throughout the optimization, while still achieving high performance. The metasurface is easily adaptable to other solid-state qubits, and the optimization method is broadly applicable to fabrication-constrained photonic design problems.

physics.optics↗

Nanodiamond emulsions for enhanced quantum sensing and click-chemistry conjugation

Nanodiamonds containing nitrogen-vacancy (NV) centers can serve as colloidal quantum sensors of local fields in biological and chemical environments. However, nanodiamond surfaces are challenging to modify without degrading their colloidal stability or the NV center's optical and spin properties. Here, we report a simple and general method to coat nanodiamonds with a thin emulsion layer that preserves their quantum features, enhances their colloidal stability, and provides functional groups for subsequent crosslinking and click-chemistry conjugation reactions. To demonstrate this technique, we decorate the nanodiamonds with combinations of carboxyl- and azide-terminated amphiphiles that enable conjugation using two different strategies. We study the effect of the emulsion layer on the NV center's spin lifetime, and we quantify the nanodiamonds' chemical sensitivity to paramagnetic ions using $T_1$ relaxometry. This general approach to nanodiamond surface functionalization will enable advances in quantum nanomedicine and biological sensing.

cond-mat.mes-hall↗

Room Temperature Dynamics of an Optically Addressable Single Spin in Hexagonal Boron Nitride

Hexagonal boron nitride (h-BN) hosts pure single-photon emitters that have shown evidence of optically detected electronic spin dynamics. However, the electrical and chemical structure of these optically addressable spins is unknown, and the nature of their spin-optical interactions remains mysterious. Here, we use time-domain optical and microwave experiments to characterize a single emitter in h-BN exhibiting room temperature optically detected magnetic resonance. Using dynamical simulations, we constrain and quantify transition rates in the model, and we design optical control protocols that optimize the signal-to-noise ratio for spin readout. This constitutes a necessary step towards quantum control of spin states in h-BN.

cond-mat.mes-hall↗

Red Emission from Copper-Vacancy Color Centers in Zinc Sulfide Colloidal Nanocrystals

Copper-doped zinc sulfide (ZnS:Cu) exhibits down-conversion luminescence in the UV, visible, and IR regions of the electromagnetic spectrum; the visible red, green, and blue emission is referred to as R-Cu, G-Cu, and B-Cu, respectively. The sub-bandgap emission arises from optical transitions between localized electronic states created by point defects, making ZnS:Cu a prolific phosphor material and an intriguing candidate material for quantum information science, where point defects excel as single-photon sources and spin qubits. Colloidal nanocrystals (NCs) of ZnS:Cu are particularly interesting as hosts for the creation, isolation, and measurement of quantum defects, since their size, composition, and surface chemistry can be precisely tailored for bio-sensing and opto-electronic applications. Here, we present a method for synthesizing colloidal ZnS:Cu NCs that emit primarily R-Cu, which has been proposed to arise from the Cu$_{Zn}$-V$_S$ complex, an impurity-vacancy point defect structure analogous to well-known quantum defects in other materials that produce favorable optical and spin dynamics. First principles calculations confirm the thermodynamic stability and electronic structure of Cu$_{Zn}$-V$_S$. Temperature- and time-dependent optical properties of ZnS:Cu NCs show blueshifting luminescence and an anomalous plateau in the intensity dependence as temperature is increased from 19 K to 290 K, for which we propose an empirical dynamical model based on thermally-activated coupling between two manifolds of states inside the ZnS bandgap. Understanding of R-Cu emission dynamics, combined with a controlled synthesis method for obtaining R-Cu centers in colloidal NC hosts, will greatly facilitate the development of Cu$_{Zn}$-V$_S$ and related complexes as quantum point defects in ZnS.

cond-mat.mtrl-sci↗

Photon emission correlation spectroscopy as an analytical tool for quantum defects

Photon emission correlation spectroscopy is an indispensable tool for the study of atoms, molecules, and, more recently, solid-state quantum defects. In solid-state systems, its most common use is as an indicator of single-photon emission, a key property for quantum technology. Beyond an emitter's single-photon purity, however, photon correlation measurements can provide a wealth of information that can reveal details about its electronic structure and optical dynamics that are hidden by other spectroscopy techniques. This tutorial presents a standardized framework for using photon emission correlation spectroscopy to study quantum emitters, including discussion of theoretical background, considerations for data acquisition and statistical analysis, and interpretation. We highlight important nuances and best practices regarding the commonly-used $g^{(2)}(τ=0)<0.5$ test for single-photon emission. Finally, we illustrate how this experimental technique can be paired with optical dynamics simulations to formulate an electronic model for unknown quantum emitters, enabling the design of quantum control protocols and assessment of their suitability for quantum information science applications.

quant-ph↗

Probing the Optical Dynamics of Quantum Emitters in Hexagonal Boron Nitride

Hexagonal boron nitride is a van der Waals material that hosts visible-wavelength quantum emitters at room temperature. However, experimental identification of the quantum emitters' electronic structure is lacking, and key details of their charge and spin properties remain unknown. Here, we probe the optical dynamics of quantum emitters in hexagonal boron nitride using photon emission correlation spectroscopy. Several quantum emitters exhibit ideal single-photon emission with noise-limited photon antibunching, $g^{(2)}(0)=0$. The photoluminescence emission lineshapes are consistent with individual vibronic transitions. However, polarization-resolved excitation and emission suggests the role of multiple optical transitions, and photon emission correlation spectroscopy reveals complicated optical dynamics associated with excitation and relaxation through multiple electronic excited states. We compare the experimental results to quantitative optical dynamics simulations, develop electronic structure models that are consistent with the observations, and discuss the results in the context of ab initio theoretical calculations.

cond-mat.mes-hall↗

Citation inequity and gendered citation practices in contemporary physics

The historical and contemporary under-attribution of women's contributions to scientific scholarship is well-known and well-studied, with effects that are felt today in myriad ways by women scientists. One measure of this under-attribution is the so-called citation gap between men and women: the under-citation of papers authored by women relative to expected rates coupled with a corresponding over-citation of papers authored by men relative to expected rates. We explore the citation gap in contemporary physics, analyzing over one million articles published over the last 25 years in 35 physics journals that span a wide range of subfields. Using a model that predicts papers' expected citation rates according to a set of characteristics separate from author gender, we find a global bias wherein papers authored by women are significantly under-cited, and papers authored by men are significantly over-cited. Moreover, we find that citation behavior varies along several dimensions, such that imbalances differ according to who is citing, where they are citing, and how they are citing. Specifically, citation imbalance in favor of man-authored papers is highest for papers authored by men, papers published in general physics journals, and papers likely to be less familiar to citing authors. Our results suggest that, although deciding which papers to cite is an individual choice, the cumulative effects of these choices needlessly harm a subset of scholars. We discuss several strategies for the mitigation of these effects, including conscious behavioral changes at the individual, journal, and community levels.

physics.soc-ph↗

Efficient Analysis of Photoluminescence Images for the Classification of Single-Photon Emitters

Solid-state single-photon emitters (SPE) are a basis for emerging technologies such as quantum communication and quantum sensing. SPE based on fluorescent point defects are ubiquitous in semiconductors and insulators, and new systems with desirable properties for quantum information science may exist amongst the vast number of unexplored defects. However, the characterization of new SPE typically relies on time-consuming techniques for identifying point source emitters by eye in photoluminescence (PL) images. This manual strategy is a bottleneck for discovering new SPE, motivating a more efficient method for characterizing emitters in PL images. Here we present a quantitative method using image analysis and regression fitting to automatically identify Gaussian emitters in PL images and classify them according to their stability, shape, and intensity relative to the background. We demonstrate efficient emitter classification for SPEs in nanodiamond arrays and hexagonal boron nitride flakes. Adaptive criteria detect SPE in both samples despite variation in emitter intensity, stability, and background features. The detection criteria can be tuned for specific material systems and experimental setups to accommodate the diverse properties of SPE.

cond-mat.mes-hall↗

Template-Assisted Self Assembly of Fluorescent Nanodiamonds for Scalable Quantum Technologies

Milled nanodiamonds containing nitrogen-vacancy (NV) centers provide an excellent platform for sensing applications as they are optically robust, have nanoscale quantum sensitivity, and form colloidal dispersions which enable bottom-up assembly techniques for device integration. However, variations in their size, shape, and surface chemistry limit the ability to position individual nanodiamonds and statistically study properties that affect their optical and quantum characteristics. Here, we present a scalable strategy to form ordered arrays of nanodiamonds using capillary-driven, template-assisted self assembly. This method enables the precise spatial arrangement of isolated nanodiamonds with diameters below 50 nm across millimeter-scale areas. Measurements of over 200 assembled nanodiamonds yield a statistical understanding of their structural, optical, and quantum properties. The NV centers' spin and charge properties are uncorrelated with nanodiamond size, but rather are consistent with heterogeneity in their nanoscale environment. This flexible assembly method, together with improved understanding of the material, will enable the integration of nanodiamonds into future quantum photonic and electronic devices.

cond-mat.mes-hall↗