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At least 163 records · Page 9

Diffeomorphism invariance and quantum mechanical paradoxes

Paradoxes in gravitational physics, such as grandfather paradoxes with closed timelike curves or the AMPS paradox, are often constructed in a weak gravity regime but upon further examination engender strong gravitational responses such as unstable Cauchy horizons or firewalls. In contrast, some proposed paradoxes in nonrelativistic quantum mechanics ignore gravity completely. Such nonrelativistic proposed paradoxes are often not gauge invariant — they use local operators which should be forbidden by diffeomorphism-invariant quantum gravity. Ignoring this complication is reasonable if there is a consistent weak gravity regime where the paradox can be formulated with gauge invariant observables up to some order in Newton’s constant. Here, we show that this approach remains inconsistent due to a lack of analyticity of the necessary solutions. As a consequence, there is no consistent weak gravity, diffeomorphism invariant embedding of such paradoxes—just as in other gravitational paradoxes they generate a strong gravitational response and are in principle sensitive to quantum gravity.

quantum gravity↗

Perspective on Many-Body Methods for Molecular Polaritonic Systems

Recent advances in strong light–matter interactions have revealed a wealth of new physical phenomena in molecules embedded in optical cavities, including modified chemical reactivity, altered excitation spectra, and novel quantum correlations. To describe these effects from first-principles, the field of ab initio quantum electrodynamics (QED) has emerged as a compelling extension of quantum chemistry that treats electronic and photonic degrees of freedom on equal footing. In this Perspective, we review the growing landscape of many-body QED methods, including Hartree–Fock, density functional theory (QEDFT), time-dependent DFT (QED-TDDFT), configuration interaction (QED-CI), complete active space (QED-CASSCF), coupled cluster (QED-CC), quantum Monte Carlo (QED-QMC), and density matrix renormalization group (QED-DMRG), highlighting recent developments and implementations. We further explore real-time methods, gradient and Hessian formalisms, and the integration of nonadiabatic nuclear dynamics. Applications range from benchmark simulations of polaritonic chemistry to quantum simulations on emerging quantum hardware. We conclude by outlining future directions for theory development and interdisciplinary efforts at the interface of quantum chemistry, condensed matter, and quantum optics.

36 MATERIALS SCIENCE↗

Universal construction of black hole microstates

We refine and extend a recent construction of sets of black hole microstates with semiclassical interiors that span a Hilbert space of dimension e S , where S is the black hole entropy. We elaborate on the definition and properties of microstates in statistical and black hole mechanics. The gravitational description of microstates employs matter shells in the interior of the black hole, and we argue that in the limit where the shells are very heavy, the construction acquires universal validity. To this end, we show it for very wide classes of black holes; we first extend the construction to rotating and charged black holes, including extremal and near-extremal solutions, with or without supersymmetry, and we sketch how the construction of microstates can be embedded in string theory. We then describe how the approach can include general quantum corrections, near or far from extremality. For supersymmetric black holes, the microstates we construct differ from other recent constructions in that the interior excitations are not confined within the near-extremal throat. Published by the American Physical Society 2024

Astronomy & Astrophysics↗

Detecting rare earth elements via optically detected magnetic resonance (ODMR) and spin-relaxometry using nitrogen vacancy centers in nanodiamonds

Nanodiamonds embedded with nitrogen-vacancy (NV) centers are emerging as powerful tools in quantum sensing due to their remarkable sensitivity to local variations in electromagnetic fields, temperature, and pressure. These point defects in the diamond lattice can be probed using optically detected magnetic resonance (ODMR) and spin relaxometry techniques, allowing for the detection and characterization of magnetic nanoparticles and ions. The sensing mechanism relies on laser-induced excitation of the NV center's non-degenerate triplet ground state, which promotes electrons to an excited state. Subsequent photoluminescence (PL) emission, which is spin-state dependent, is then measured. These spin states are highly responsive to magnetic perturbations in the surrounding environment. By analyzing changes in the ODMR spectra and spin relaxation times, we can effectively monitor how magnetic species influence the NV center's spin dynamics, thus enabling sensitive and selective characterization of nanoscale magnetic materials. These techniques have been applied for the characterization of transition metals and rare earth elements which shows natural ferromagnetic properties.

magnetic nanopartgicles and ions↗

State-Chart Autocoder

A computer program translates Unified Modeling Language (UML) representations of state charts into source code in the C, C++, and Python computing languages. ( State charts signifies graphical descriptions of states and state transitions of a spacecraft or other complex system.) The UML representations constituting the input to this program are generated by using a UML-compliant graphical design program to draw the state charts. The generated source code is consistent with the "quantum programming" approach, which is so named because it involves discrete states and state transitions that have features in common with states and state transitions in quantum mechanics. Quantum programming enables efficient implementation of state charts, suitable for real-time embedded flight software. In addition to source code, the autocoder program generates a graphical-user-interface (GUI) program that, in turn, generates a display of state transitions in response to events triggered by the user. The GUI program is wrapped around, and can be used to exercise the state-chart behavior of, the generated source code. Once the expected state-chart behavior is confirmed, the generated source code can be augmented with a software interface to the rest of the software with which the source code is required to interact.

Clark, Kenneth↗

Kondo screening in a Majorana metal

Kondo impurities provide a nontrivial probe to unravel the character of the excitations of a quantum spin liquid. In the S = 1/2 Kitaev model on the honeycomb lattice, Kondo impurities embedded in the spin-liquid host can be screened by itinerant Majorana fermions via gauge-flux binding. Here, we report experimental signatures of metallic-like Kondo screening at intermediate temperatures in the Kitaev honeycomb material α-RuCl 3 with dilute Cr 3+ (S = 3/2) impurities. The static magnetic susceptibility, the muon Knight shift, and the muon spin-relaxation rate all feature logarithmic divergences, a hallmark of a metallic Kondo effect. Concurrently, the linear coefficient of the magnetic specific heat is large in the same temperature regime, indicating the presence of a host Majorana metal. This observation opens new avenues for exploring uncharted Kondo physics in insulating quantum magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Optically Active Spin Defects in Few-Layer Thick Hexagonal Boron Nitride

Optically active spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of two-dimensional quantum sensing units offering optimal proximity to the sample being probed. In this Letter, we first demonstrate that the electron spin resonance frequencies of boron vacancy centers ($V$$^{–}_{B}$) can be detected optically in the limit of few-atomic-layer thick hBN flakes despite the nanoscale proximity of the crystal surface that often leads to a degradation of the stability of solid-state spin defects. We then analyze the variations of the electronic spin properties of $V$$^{–}_{B}$ centers with the hBN thickness with a focus on (i) the zero-field splitting parameters, (ii) the optically induced spin polarization rate and (iii) the longitudinal spin relaxation time. Furthermore, this Letter provides important insights into the properties of $V$$^{–}_{B}$ centers embedded in ultrathin hBN flakes, which are valuable for future developments of foil-based quantum sensing technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Topological terms with qubit regularization and relativistic quantum circuits

Qubit regularization provides a rich framework to explore quantum field theories. The freedom to choose how the important symmetries of the theory are embedded in the qubit regularization scheme allows us to construct new lattice models with rich phase diagrams. Some of the phases can contain topological terms which lead to critical phases. In this work we introduce and study the SU(3)-F qubit regularization scheme to embed the SO(3) spin-symmetry. We argue that qubit models in this regularization scheme contain several phases including a critical phase which describes the k = 1 Wess-Zumino-Witten (WZW) conformal field theory (CFT) at long distances, and two massive phases one of which is trvially gapped and the other which breaks the lattice translation symmetry. We construct a simple space-time Euclidean lattice model with a single coupling U and study it using the Monte Carlo method. We show the model has a critical phase at small U and a trivially massive phase at large U with a first order transition separating the two. Another feature of our model is that it is symmetric under space-time rotations, which means the temporal and spatial lattice spacing are connected to each other. The unitary time evolution operator obtained by a Wick rotation of the transfer matrix of our model can help us compute the physics of the k = 1 WZW CFT in real time without the need for tuning the temporal lattice spacing to zero. We use this idea to introduce the concept of a relativistic quantum circuit on a discrete space-time lattice.

Bhattacharya, Tanmoy↗

Enhanced dilepton emission from a phase transition in dense matter

It is demonstrated that the presence of a phase transition in heavy-ion collisions, at beam energies that probe dense quantum chromodynamics (QCD) matter, leads to a significant enhancement of the dilepton yield at low invariant mass and requires the embedding of low beam energies per produced pion due to the extended emission time. In addition, the temperature of low-mass dileptons shows a modest decrease due to the mixed phase. The emission of dileptons in the SIS18–SIS100 beam energy range is studied by augmenting the ultra-relativistic quantum molecular dynamics (UrQMD) transport model with a realistic density-dependent equation of state, as well as two different phase transitions. This is achieved by extending the molecular dynamics interaction part of the UrQMD model to a density-dependent interaction potential with a high-density minimum, leading to a phase transition and metastable coexisting high-density states. Together with a high-precision measurement, these simulations will be able to constrain the existence of a phase transition in QCD up to densities of several times nuclear saturation density.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Benchmarking an Embedded Adaptive Sampling Configuration Interaction Method for Surface Reactions: H 2 Desorption from and CH 4 Dissociation on Cu(111)

Embedded (emb-) correlated wavefunction (CW) theory enables accurate assessments of both ground- and excited-state reaction mechanisms involved in heterogeneous catalysis. Embedded multireference second-order perturbation theory (emb-MRPT2) based on reference wavefunctions generated via embedded complete active space self-consistent field (emb-CASSCF) theory is currently state-of-the-art. However, the factorial scaling of CASSCF limits the size of active space and the complexity of systems that can be studied. In this work, we assess the efficacy of an alternative CW method, adaptive sampling configuration interaction (ASCI)–which enables large active spaces to be used–for studying surface reactions. We couple ASCI with density functional embedding theory (DFET) and benchmark its performance for two reactions: H 2 desorption from and CH 4 dissociation on the Cu(111) surface. Unlike embedded complete active space second-order perturbation theory (emb-CASPT2) that accurately reproduces a measured H 2 desorption barrier, embedded ASCI, using a very large active space (though one that still comprises a small portion of the full set of orbitals) fails to do so. Adding an extra correlation term from embedded Møller–Plesset second-order perturbation theory (emb-MP2) improves the desorption barrier and endothermicity predictions. Thus, the inaccuracy of embedded ASCI comes from the missing dynamic correlation from the many other electrons and orbitals not included in the active space. For CH 4 dissociation, again embedded ASCI overestimates the dissociation barrier compared to emb-CASPT2 predictions. Adding dynamic correlation from emb-MP2 helps correct the barrier. However, this composite approach suffers from double counting of correlation within embedded ASCI followed by emb-MP2 calculations. We therefore conclude that the state-of-the-art emb-MRPT2 based on reference wavefunctions generated via emb-CASSCF remains the method of choice for studying surface reactions. emb-ASCI is useful when large active spaces beyond the limit of emb-CASSCF are essential, such as to study complex surface reactions with significant multiconfigurational character (static correlation) but weak dynamic correlation.

08 HYDROGEN↗

Electronic Spin Qubit Candidates Arrayed within Layered Two-Dimensional Polymers

Molecular electronic spin qubits are promising candidates for quantum information science applications because they can be reliably produced and engineered via chemical design. Embedding electronic spin qubits within two-dimensional polymers (2DPs) offers the possibility to systematically engineer inter-qubit interactions while maintaining long coherence times, both of which are prerequisites to their technological utility. Here, we introduce electronic spin qubits into a diamagnetic 2DP by n-doping naphthalene diimide subunits with varying amounts of CoCp 2 and analyze their spin densities by quantitative electronic paramagnetic resonance spectroscopy. Low spin densities (e.g., 6.0 × 10 12 spins mm –3 ) enable lengthy spin–lattice (T 1 ) and spin–spin relaxation (T 2 ) times across a range of temperatures, ranging from T 1 values of 164 ms at 10 K to 30.2 μs at 296 K and T 2 values of 2.36 μs at 10 K to 0.49 μs at 296 K for the lowest spin density sample examined. Higher spin densities and temperatures were both found to diminish T 1 times, which we attribute to detrimental cross-relaxation from spin–spin dipolar interactions and spin–phonon coupling, respectively. Higher spin densities decreased T 2 times and modulated the T 2 temperature dependence. Here, we attribute these differences to the competition between hyperfine and dipolar interactions for electron spin decoherence, with the dominant interaction transitioning from the former to the latter as spin density and temperature increase. Overall, this investigation demonstrates that dispersing electronic spin qubits within layered 2DPs enables chemical control of their inter-qubit interactions and spin decoherence times.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A graphene edge-mediated quantum gate

We propose a quantum gate architecture that allows for the systematic control of the effective exchange interactions between magnetic impurities embedded in nanoscale graphene flakes connected by a gated bridge. The entanglement between the magnetic moment and the edge states of the fragments is used to electrostatically tune the exchange interaction from ferro to antiferromagnetic by merely changing the bridge's carrier density. By characterizing the effects of size and coupling parameters, we explore different operation regimes of this device by means of exact calculations with the density matrix renormalization group. We analyze the results utilizing a simplified model that accounts for the main many-body mechanisms. Finally, we discuss how to use arrays of these devices to build quantum simulators for quantum many-body Hamiltonians.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Protein3D: Enabling analysis and extraction of metal‐containing sites from the Protein Data Bank with molSimplify

Abstract Metalloenzymes catalyze a wide range of chemical transformations, with the active site residues playing a key role in modulating chemical reactivity and selectivity. Unlike smaller synthetic catalysts, a metalloenzyme active site is embedded in a larger protein, which makes interrogation of electronic properties and geometric features with quantum mechanical calculations challenging. Here we implement the ability to fetch crystallographic structures from the Protein Data Bank and analyze the metal binding sites in the program molSimplify. We show the usefulness of the newly created protein3D class to extract the local environment around non‐heme iron enzymes containing a two histidine motif and prepare 372 structures for quantum mechanical calculations. Our implementation of protein3D serves to expand the range of systems molSimplify can be used to analyze and will enable high‐throughput study of metal‐containing active sites in proteins.

Edholm, Freya↗

Photosynthetic biohybrid systems for solar fuels catalysis

Photosynthetic reaction center (RC) proteins are finely tuned molecular systems optimized for solar energy conversion. RCs effectively capture and convert sunlight with near unity quantum efficiency utilizing light-induced directional electron transfer through a series of molecular cofactors embedded within the protein core to generate a long-lived charge separated state with a useable electrochemical potential. Of current interest are new strategies that couple RC chemistry to the direct synthesis of energy-rich compounds. This Feature Article highlights recent work from our lab on RC and RC-inspired hybrid systems that capture the Sun's energy and convert it to chemical energy in the form of H2, a carbon-neutral energy source derived from water. Further, biohybrids made from the Photosystem I (PSI) RC are among the best photocatalytic H2-producing protein hybrids to date. Targeted self-assembly strategies that couple abiotic catalysts to PSI translate to catalyst incorporation at intrinsic PSI sites within thylakoid membranes to achieve complete solar water-splitting systems. RC-inspired biohybrids interface synthetic photosensitizers and molecular catalysts with small proteins to create photocatalytic systems and enable the spectroscopic discernment of the structural features and electron transfer processes that underpin solar-driven proton reduction. In total, these studies showcase the incredible scientific opportunities photosynthetic biohybrid research provides for harnessing the optimal qualities of both artificial and natural photosynthetic systems and developing materials that capture, convert, and store solar energy as a fuel.

14 SOLAR ENERGY↗

Artificial Intelligence-Enhanced, Multi-Level, Modular System Design

As Moore’s Law and Dennard Scaling come to an end, it is becoming increasingly important to develop non-von Neumann computing architectures that can perform low-power computing in the domains of scientific computing, artificial intelligence, embedded systems, and edge computing. Next-generation computing technologies, such as neuromorphic computing and quantum computing, have the potential to revolutionize computing. However, in order to make progress in these fields, it is necessary to fundamentally change the current computing paradigm by codesigning systems across all system level, from materials to software. Because skilled labor is limited in the field of next-generation computing, we are developing artificial intelligence-enhanced tools to automate the codesign and co-discovery of next-generation computers. Here, we develop a method called Modular and Multi-level MAchine Learning (MAMMAL) which is able to perform analog codesign and co-discovery across multiple system levels, spanning devices to circuits. We prototype MAMMAL by using it to design simple passive analog low-pass filters. We also explore methods to incorporate uncertainty quantification into MAMMAL and to accelerate MAMMAL by using emerging technologies, such as crossbar arrays. Ultimately, we believe that MAMMAL will enable rapid progress in developing next-generation computers by automating the codesign and co-discovery of electronic systems.

97 MATHEMATICS AND COMPUTING↗

Squeezed states of electrons and transitions of the density of states

Electron systems which have low dimensional properties have been constructed by squeezing the motion in zero, one, or two-directions. An isolated quantum dot is modeled by a potential box with delta-profiled, penetrable potential walls embedded in a large outer box with infinitely high potential walls which represent the world function with respect to vacuum. We show the smooth crossover of the density of states from the three-dimensional to the quasi-zero dimensional electron gas.

Lee, Seung Joo↗

Er-doped anatase TiO 2 thin films on LaAlO 3 (001) for quantum interconnects (QuICs)

Rare-earth ions (REIs) doped into solid-state crystal hosts offer an attractive platform for realizing quantum interconnects that can function as quantum memories and quantum repeaters. The 4f valence electrons of REIs are shielded by 5s and 5p electrons and undergo highly coherent transitions even when embedded in host crystals. In particular, Er 3+ has an optical transition in the telecom band that is suitable for low-loss communication. Recently, REIs in thin film systems have gained interest due to potential advantages in providing a flexible host crystal environment, enabling scalable on-chip integration with other quantum devices. Here, we investigate the structural and optical properties of Er-doped anatase TiO 2 thin films on LaAlO 3 (001) substrates. By choosing a system with minimal lattice mismatch and adjusting Er-dopant concentration, we achieve optical inhomogeneous linewidths of 5 GHz at 4.5 K. Furthermore, we show that 9 nm-thick buffer and capping layers can reduce the linewidth by more than 40%, suggesting a pathway to further narrowing linewidths in this system. We also identify that Er 3+ ions mainly incorporate into substitutional Ti 4+ sites with non-polar D 2d symmetry, which makes Er dopants insensitive to the first order to local electric fields from impurities and is desirable for coherence properties of Er 3+ spins.

42 ENGINEERING↗

Assessing Ground State Energy of Molecules and Energy Profile of the NH3 Capturing CO2 System Using the Quantum Computing Algorithms

Molecule size correlates with the number of electrons on electronic energies and strength of anharmonicity on vibrational properties, however, it is challenging to address using classical computing. In this study, variational quantum eigensolver (VQE) algorithm was implemented on a quantum simulator to quantify electronic and vibrational energies and reaction pathways of CO2 + NH3 = NH2COOH. The VQE-based Hartree-Fock-Embedding algorithm was adopted to benchmark electronic energies for a series of molecules (doi.org/10.1063/5.0188249) and quantify the reaction energy profile of the CO2 capture reaction (doi.org/10.1116/5.0137750). The generated reaction profile is in good agreement with the classical high-level Coupled-Cluster-Singles-and-Doubles (CCSD) results. The quantum computing algorithm also helps enhance the calculation of vibrational ground-state energies by considering the many-body coupling using the Vibrational Self-Consistent Field method, providing results for CO2 and NH3 molecules with accuracy comparable to the direct diagonalization method. Our approach indicates quantum computing can be applied to solve practical problems.

Lee, Yueh-Lin↗