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At least 397 records · Page 22

Electron Sextets as Optically Addressable Molecular Qubits: Triplet Carbenes

There is a growing demand in quantum information science and sensing for electron spin purification and readout via a spin-optical interface. This technique, known as optically detected magnetic resonance (ODMR), has been applied to diamond-NV centers and transition-metal complexes. Metal-free counterparts of these optically addressable spin qubits promise to be cheaper, more sustainable color centers with prolonged polarization lifetimes. However, progress has been hindered by the low ODMR signals of carbon-based π-diradicals, partly due to the lack of a ground singlet-to-triplet intersystem crossing (ISC). In this work, we propose exploring organic systems that are even more electron-deficient: electron sextets. Using triplet carbenes as an example, we illustrate how the ground singlet-triplet gap can be widened beyond thermal energy with the associated singlet-to-triplet ISC made available by vibronic effects. Through careful molecular engineering, this ISC can occur at a rate similar to and with an opposite spin selectivity from the excited-state ISC well-established in π-diradicals, unlocking a new ODMR pathway with potential signal gains. Persistent triplet carbenes are a renascent field, with multiple stable molecules being isolated in the past five years. To motivate further development of its emissive properties, we illustrate our design in three realistic carbene candidates that incorporate existing strategies for carbene stabilization. Furthermore, we believe that a new realm of quantum materials can be uncovered by expanding our scope toward stable electron sextets.

Carbene compounds↗

Detecting Spin-Bath Polarization with Quantum Quench Phase Shifts of Single Spins in Diamond

Single-qubit sensing protocols can be used to measure qubit-bath coupling parameters. However, for sufficiently large coupling, the sensing protocol itself perturbs the bath, which is predicted to result in a characteristic response in the sensing measurements. Here, we observe this bath perturbation, also known as a quantum quench, by preparing the nuclear spin bath of a nitrogen-vacancy (NV) center in polarized initial states and performing phase-resolved spin-echo measurements on the NV electron spin. These measurements reveal a time-dependent phase determined by the initial state of the bath. We derive the relationship between the sensor phase and the Gaussian spin-bath polarization and apply it to reconstruct both the axial and transverse polarization components. Using this insight, we optimize the transfer efficiency of our dynamic nuclear polarization sequence. This technique for directly measuring bath polarization may assist in preparing high-fidelity quantum memory states, improving nanoscale NMR methods, and investigating non-Gaussian quantum baths.

36 MATERIALS SCIENCE↗

Cybersecurity Considerations for Emerging Energy Technologies

AI, cloud computing, post-quantum cryptography, zero-trust architectures, microgrids, and virtual power plants. What do these things have in common? They are all emerging technologies in the clean energy space that will be a critical part of grid modernization efforts. As we work towards clean energy and decarbonization targets, these technologies, developed to solve real-world problems, will help us reach goals and achieve new efficiencies as the paradigm of grid operation shifts. However, there are growing concerns about the cybersecurity risks associated with these trending topics as they are used in critical infrastructure applications. This talk will cover gaps, challenges, and opportunities for the secure implementation of grid modernization solutions and novel energy applications of state-of-the-art networking and communications. Proactive risk mitigation strategies, including the application of cyber-informed engineering, will be discussed. Practical applications of these techniques will help provide countermeasures to the impact of cyberattacks on critical infrastructure technologies in a new, digitized grid landscape.

14 SOLAR ENERGY↗

Substitutional doping of 2D transition metal dichalcogenides for device applications: Current status, challenges and prospects

Two-dimensional (2D) transition metal dichalcogenides (TMDs) have emerged as a class of materials with exceptional electronic, optical, and mechanical properties, making them highly tunable for diverse applications in nanoelectronics, optoelectronics, and catalysis. Here, this review focuses on substitutional doping of TMDs, a key strategy to tailor their properties and enhance device performance, with a focus on its applications over the past five years (2019–2024). We delve into both theoretical and experimental doping approaches, including established methods like chemical vapor transport (CVT) and chemical vapor deposition (CVD) alongside liquid phase exfoliation (LPE) and post-synthesis treatments. Advanced growth techniques are also explored. Challenges like dopant uniformity, concentration control, and stability are addressed. The influence of various dopants on the electronic band structure, carrier concentration, and defect engineering is analyzed in detail. We further explore recent advancements in utilizing doped TMDs for field-effect transistors (FETs), photodetectors, sensors, photovoltaics, optoelectronic devices, energy storage and conversion, and even quantum computers. By examining both the potential and limitations of substitutional doping, this review aims to propel future research and technological advancements in this exciting field.

36 MATERIALS SCIENCE↗

Gauss Sum Strong Simulation v.0.1

Universal quantum circuits can be formulated in the Pauli measurement-based formalism as input T gate magic states, Clifford gates, and then multi-Pauli measurements. This code simulates single-Pauli measurements to show some theoretical bounds on the cost of full multi-Pauli measurements. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. SAND2020-14080 O

SciDAC↗

Gauge-fixing quantum density operators at scale

We provide a theory, algorithms, and simulations of nonequilibrium quantum systems using a one-dimensional (1D) completely positive (CP), matrix-product (MP) density-operator (𝜌) representation. By generalizing the matrix product state's orthogonality center, to additionally store positive classical mixture correlations, the MP⁢𝜌 factorization naturally emerges. In this setting, we analytically and numerically examine the virtual gauge freedoms associated with the representation of quantum density operators. Based on this perspective, we simplify algorithms in certain limits to speed up the integration of the canonical-form master-equation dynamics. This enables us to quickly evolve under the dynamics of two-body quantum channels without resorting to optimization-based methods. In addition to this technical advance, we also scale up numerical examples and discuss implications for accurately modeling hardware architectures and predicting their performance in the near term. This includes an example of the quantum to classical transition of informationally leaky, i.e., decohering, qubits. In this setting, because of loss from environmental interactions, nonlocal complex coherence correlations are converted into global incoherent classical statistical mixture correlations. Lastly, the representation of both global and local correlations is discussed. We expect this work to have applications in additional nonequilibrium settings, beyond qubit engineering.

Gangapuram, Amit Jamadagni [Oak Ridge National Lab↗

Low energy backgrounds and excess noise in a two-channel low-threshold calorimeter

Here, we describe observations of low energy excess (LEE) events, background events observed in all light dark matter direct detection calorimeters, and noise in a transition edge sensor based two-channel silicon athermal phonon detector with 375 meV baseline energy resolution. We measure two distinct LEE populations: “shared” multichannel events with a pulse shape consistent with substrate athermal phonon events and sub-eV events that couple nearly exclusively to a single channel with a significantly faster pulse shape. These “singles” are consistent with events occurring within the aluminum athermal phonon collection fins. Similarly, our measured detector noise is higher than the theoretical expectation. Measured noise can be split into an uncorrelated component, consistent with shot noise from small energy depositions within the athermal phonon sensor itself, and a correlated component, consistent with shot noise from energy depositions within the silicon substrate's phonon system.

47 OTHER INSTRUMENTATION↗

Flexoelectricity and New Phenomena

It is easy to miss the scientific implications of our recent work on Triboelectricity. Everyone knows that rubbing and contact can produce static electricity; less appreciated is that the thermodynamic driver has been an open question since static electricity was first observed by Thales of Miletus around 585 BC. People think they understand it, for instance one common explanation that can still be found in the current literature is that differences in the work function drives charge transfer, often called the Volta-Helmholtz hypothesis. As summarized in 1967 by Harper, this fails to explain many experimental observations, for instance that charging can occur when two pieces of the same material are rubbed against each other. We are the first to place triboelectricity on a solid foundation rooted in quantum mechanics – the flexoelectric effect. We were able to explain a significant number of previously unexplained phenomena: 1) Bipolar tribocurrents associated with stick-slip, due to the change in sign of the strain gradients. 2) A one-third power scaling of tribocurrents with indentation force. 3) Tribocharging when two identical materials are used, these being due to local variations in the asperities so there are usually local potential differences. 4) Inhomogeneous charging of insulators, related to the statistical nature of asperities. 5) An experimentally observed reversal in the sign of charge transfer for negative and positive curvature, which is related to a change in the sign of the strain gradient. Exploiting our DOE prior funded work on flexoelectricity, we obtained semi-quantitative matching to existing experimental measurements of the surface charge in triboelectric experiments. The work has been well received in the literature. The work has been the focus of a number of popular science press articles, and also formed the basis for a Podcast for children 6-10 “The Rise and Fall of Static Man” posted in December 2019 by NPR as part of their “Wow in the World” series. I was also briefly interviewed by the Chicago PBS station in January 2020. This work are significant for a wide range of energy applications; to quote from an independent source: "Triboelectric power has plenty of potential, says Wenzhuo Wu, an assistant professor of engineering at Purdue. If the basics of static electricity are better understood, we could maximize the efficiency of wind or wave power generators, Wu says. The body's own movement could be used to power internal medical devices. Imagine being able to create a roof shaped to harness the power of a raindrop — the friction of the rain passing over the surface — to generate triboelectricity, powering the building below it." This is the start of new science, some of which we already partially understand such as the role of band bending in charge transfer. We need to understand charge transfer combining elasticity, quantum mechanics, band bending and defect states. These directly involve several of the DOE Grand Challenges: "How do we control material processes at the level of electrons? How do remarkable properties of matter emerge from complex correlations of the atomic or electronic constituents and how can we control these properties? How do we characterize and control matter away—especially very far away— from equilibrium?" I will argue that this work truly falls into the class of disruptive science; it is not just a simple extension, linear science. Not everyone will accept the approach. Since we explain far more about triboelectricity than anyone before, the preponderance of evidence supports the model. The feedback I have received is that many agree with the work, to quote: "The model makes sense, says Michael McAlpine, a professor of engineering at the University of Minnesota. "It's such a simple explanation, I was surprised I didn't put my finger on that," McAlpine says." The proposal received strong reviews. It was also publicized on the Department of Energy Web Site.

16 TIDAL AND WAVE POWER↗

On closures for reduced order models - A spectrum of first-principle to machine-learned avenues

For over a century, reduced order models (ROMs) have been a fundamental discipline of theoretical fluid mechanics. Early examples include Galerkin models inspired by the Orr–Sommerfeld stability equation and numerous vortex models, of which the von Karman vortex street is one of the most prominent. Subsequent ROMs typically relied on first principles, like mathematical Galerkin models, weakly nonlinear stability theory, and two- and three-dimensional vortex models pioneered the data-driven proper orthogonal decomposition (POD) modeling. In early POD modeling, available data were used to build an optimal basis, which was then utilized in a classical Galerkin procedure to construct the ROM, but data have made a profound impact on ROMs beyond the Galerkin expansion. In this paper, we take a modest step and illustrate the impact of data-driven modeling on one significant ROM area. Specifically, we focus on ROM closures, which are correction terms that are added to the classical ROMs in order to model the effect of the discarded ROM modes in under-resolved simulations. Through simple examples, we illustrate the main modeling principles used to construct the classical ROMs, motivate and introduce modern ROM closures, and show how data-driven modeling, artificial intelligence, and machine learning have changed the standard ROM methodology over the last two decades. Finally, we outline our vision on how the state-of-the-art data-driven modeling can continue to reshape the field of reduced order modeling.

42 ENGINEERING↗

Deterministic nanoscale quantum spin-defect implantation and diffraction strain imaging

Abstract Local crystallographic features negatively affect quantum spin defects by changing the local electrostatic environment, often resulting in degraded or varied qubit optical and coherence properties. Few tools exist that enable the deterministic synthesis and study of such intricate systems on the nano-scale, making defect-to-defect strain environment quantification difficult. In this paper, we highlight state-of-the-art capabilities from the U.S. Department of Energy’s Nanoscale Science Research Centers that directly address these shortcomings. Specifically, we demonstrate how complementary capabilities of nano-implantation and nano-diffraction can be used to demonstrate the quantum relevant, spatially deterministic creation of neutral divacancy centers in 4H silicon carbide, while investigating and characterizing these systems on the ≤ 25 nm scale with strain sensitivities on the order of 1 × 10 − 6 , relevant to defect formation dynamics. This work lays the foundation for ongoing studies into the dynamics and deterministic formation of low strain homogeneous quantum relevant spin defects in the solid state.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Overcoming the fundamental limit of quantum transduction via intraband entanglement

A quantum transducer converts an input signal to an output probe at a distant frequency band while maintaining the quantum information with high fidelity, which is crucial for quantum networking and distributed quantum sensing and computing. In terms of microwave–optical quantum transduction, the state-of-the-art quantum transducers suffer low transduction efficiency from weak nonlinear coupling, wherein increasing pump power to enhance efficiency inevitably leads to thermal noise from heating. Moreover, we reveal that the efficiency-bandwidth product of a cavity electro-optical or electro-optomechanical transducer is fundamentally limited by pump power and nonlinear coupling coefficient, irrespective of cavity engineering efforts. To overcome this fundamental limit, we propose to noiselessly boost the transduction efficiency by consuming intraband entanglement (e.g., microwave–microwave or optical–optical entanglement in the case of microwave–optical transduction). Via a squeezer–coupler–antisqueezer sandwich structure, the protocol enhances the transduction efficiency to unity in the ideal lossless case, given an arbitrarily weak pump and nonlinear coupling. In practical cavity systems, our entanglement-assisted protocol surpasses the non-assisted fundamental limit of the efficiency-bandwidth product and reduces the threshold cooperativity for positive quantum capacity by a factor proportional to two-mode squeezing gain. Given a fixed cooperativity, our approach increases the broadband quantum capacity by orders of magnitude. The entanglement-assisted advantage is robust to ancilla loss and cavity detuning.

Shi, Haowei [Southern California U.] (ORCID:000000↗

Microstructural Topology as a Prescriptor for Quantum Coherence: Towards A Unified Framework for Decoherence in Superconducting Qubits

In superconducting quantum circuits, decoherence improvements are frequently obtained through process interventions that simultaneously modify surface chemistry, microstructural topology, and device geometry, leaving mechanistic attribution structurally underdetermined. Predictive materials engineering requires measurable structural statistics to be separated from geometry-dependent coupling coefficients into independently testable factors. We introduce the concept of classical and quantum microstructure. In that context, we formulate a channel-wise separable framework for decoherence in superconducting transmon qubits in which each loss channel is described by a reduced prescriptor. Here, a channel-specific microstructural state variable is determined independently of device geometry, and a geometry-dependent coupling functional is computable from field solutions without reference to surface chemistry. We derive this product form from a spatially resolved kernel representation and establish a perturbative separability criterion that defines the regime where independent variation of the variables is valid. The framework specifies five prescriptor classes for dominant loss pathways in transmon-class devices. Falsifiability is operationalized through a pre-committed 2x2 experimental protocol in which the variables must satisfy independent ratio checks within propagated uncertainty. A Minimum-Dataset Specification standardizes reporting for cross-laboratory inference. Part I establishes the conceptual and mathematical architecture; coordinated experimental validation is reserved for Part II.

Dravid, Vinayak P. [Northwestern U.]↗

Characterization of Cs 3 Sb photocathodes at cryogenic temperatures

Here, we report measurements of quantum efficiency (QE) and mean transverse energy (MTE) from Cs 3 Sb photocathodes in a wide range of photon energies at both room and cryogenic temperatures. Our measurements show a strong temperature dependence of MTE even at photon energies well above threshold, indicating the presence of strong inelastic scattering of excited electrons during transport before emission into vacuum. We also demonstrate a cathode cooling method that largely preserves the QE while reducing MTE, allowing us to achieve MTEs as low as 58 meV with 3% QE in green light from Cs 3 Sb photocathodes. Our results are crucial for producing brighter electron beams for various photoinjector applications like ultrafast electron diffraction and microscopy, x-ray free-electron lasers, and particle colliders.

36 MATERIALS SCIENCE↗

Optimal coupling of Ho W 10 molecular magnets to superconducting circuits near spin clock transitions

A central goal in quantum technologies is to maximize GT 2 , where G stands for the coupling of a qubit to control and readout signals and T 2 is the qubit’s coherence time. Furthermore, this is challenging, as increasing G (e.g., by coupling the qubit more strongly to external stimuli) often leads to deleterious effects on T 2 . Here, we study the coupling of pure and magnetically diluted crystals of Ho W 10 magnetic clusters to microwave superconducting coplanar waveguides. Absorption lines give a broadband picture of the magnetic energy level scheme and, in particular, confirm the existence of level anticrossings at equidistant magnetic fields determined by the combination of crystal field and hyperfine interactions. Such “spin clock transitions” are known to shield the electronic spins against magnetic field fluctuations. The analysis of the microwave transmission shows that the spin-photon coupling also becomes maximum at these transitions. The results show that engineering spin-clock states of molecular systems offers a promising strategy to combine sizable spin-photon interactions with a sufficient isolation from unwanted magnetic noise sources.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Experimental realization of an extended Fermi-Hubbard model using a 2D lattice of dopant-based quantum dots

The Hubbard model is an essential tool for understanding many-body physics in condensed matter systems. Artificial lattices of dopants in silicon are a promising method for the analog quantum simulation of extended Fermi-Hubbard Hamiltonians in the strong interaction regime. However, complex atom-based device fabrication requirements have meant emulating a tunable two-dimensional Fermi-Hubbard Hamiltonian in silicon has not been achieved. Here, we fabricate 3 × 3 arrays of single/few-dopant quantum dots with finite disorder and demonstrate tuning of the electron ensemble using gates and probe the many-body states using quantum transport measurements. By controlling the lattice constants, we tune the hopping amplitude and long-range interactions and observe the finite-size analogue of a transition from metallic to Mott insulating behavior. We simulate thermally activated hopping and Hubbard band formation using increased temperatures. As atomically precise fabrication continues to improve, these results enable a new class of engineered artificial lattices to simulate interactive fermionic models.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum Enhanced Fiber Sensing for Oil and Gas Applications (Final Technical Report)

The major goal of the project was to develop a quantum sensing approach compatible with current infrastructure in the oil and gas industry that could provide a quantum enhancement, with a focus towards pipeline leak detection. The proposed approach to achieving this goal consisted of the use of quantum states of light to enhance the sensitivity of fiber optic sensors beyond the classical limit. To address the limitations of existing commercial leak detection, the project focused on the study of two technologies: distributed acoustic sensors (DAS) and fiber Bragg grating (FBG)-based sensors. The initial phase of the project centered around the identification and mitigation of dominant sources of classical noise to enable operation at the classical shot noise limit (SNL). The second phase focused on the use of quantum resources to obtain sensitivities beyond the classical SNL. The final phase sought to combine quantum noise reduction techniques with advanced dynamical classical noise cancelation approaches.

02 PETROLEUM↗

Adjoint-optimized nanoscale light extractor for nitrogen-vacancy centers in diamond

Abstract We designed a nanoscale light extractor (NLE) for the efficient outcoupling and beaming of broadband light emitted by shallow, negatively charged nitrogen-vacancy (NV) centers in bulk diamond. The NLE consists of a patterned silicon layer on diamond and requires no etching of the diamond surface. Our design process is based on adjoint optimization using broadband time-domain simulations and yields structures that are inherently robust to positioning and fabrication errors. Our NLE functions like a transmission antenna for the NV center, enhancing the optical power extracted from an NV center positioned 10 nm below the diamond surface by a factor of more than 35, and beaming the light into a ±30° cone in the far field. This approach to light extraction can be readily adapted to other solid-state color centers.

42 ENGINEERING↗

Photoinduced Dirac semimetal in ZrTe5

Abstract Novel phases of matter with unique properties that emerge from quantum and topological protection present an important thrust of modern research. Of particular interest is to engineer these phases on demand using ultrafast external stimuli, such as photoexcitation, which offers prospects of their integration into future devices compatible with optical communication and information technology. Here, we use MeV Ultrafast Electron Diffraction (UED) to show how a transient three-dimensional (3D) Dirac semimetal state can be induced by a femtosecond laser pulse in a topological insulator ZrTe 5 . We observe marked changes in Bragg diffraction, which are characteristic of bond distortions in the photoinduced state. Using the atomic positions refined from the UED, we perform density functional theory (DFT) analysis of the electronic band structure. Our results reveal that the equilibrium state of ZrTe 5 is a topological insulator with a small band gap of ~ 25 meV, consistent with angle-resolved photoemission (ARPES) experiments. However, the gap is closed in the presence of strong spin-orbit coupling (SOC) in the photoinduced transient state, where massless Dirac fermions emerge in the chiral band structure. The time scale of the relaxation dynamics to the transient Dirac semimetal state is remarkably long, τ ~ 160 ps, which is two orders of magnitude longer than the conventional phonon-driven structural relaxation. The long relaxation is consistent with the vanishing density of states in Dirac spectrum and slow spin-repolarization of the SOC-controlled band structure accompanying the emergence of Dirac fermions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗