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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Single nuclear spin detection and control in a van der Waals material

Optically active spin defects in solids are leading candidates for quantum sensing and quantum networking. Recently, single spin defects were discovered in hexagonal boron nitride (hBN), a layered van der Waals (vdW) material. Owing to its two-dimensional structure, hBN allows spin defects to be positioned closer to target samples than in three-dimensional crystals, making it ideal for atomic-scale quantum sensing, including nuclear magnetic resonance (NMR) of single molecules. However, the chemical structures of these defects remain unknown and detecting a single nuclear spin with a hBN spin defect has been elusive. Here we report the creation of single spin defects in hBN using 13 C ion implantation and the identification of three distinct defect types based on hyperfine interactions. We observed both S = 1/2 and S = 1 spin states within a single hBN spin defect. We demonstrated atomic-scale NMR and coherent control of individual nuclear spins in a vdW material, with a π-gate fidelity up to 99.75% at room temperature. By comparing experimental results with density functional theory (DFT) calculations, we propose chemical structures for these spin defects. Our work advances the understanding of single spin defects in hBN and provides a pathway to enhance quantum sensing using hBN spin defects with nuclear spins as quantum memories.

Quantum metrology↗
DOE OSTI2023

Selective Detection in Impulsive Low-Frequency Raman Imaging Using Shaped Probe Pulses

Impulsive stimulated Raman scattering (ISRS) using a single short femtosecond pump pulse to excite molecular vibrations offers an elegant pump-probe approach to perform vibrational imaging below 200 cm –1 . One shortcoming of ISRS is its inability to offer vibrational selectivity as all the vibrational bonds whose frequencies lie within the short pump-pulse bandwidth are excited. To date, several coherent control techniques have been explored to address this issue and selectively excite a specific molecular vibration by shaping the pump pulse. There has not been any systematic work that reports an analogous shaping of the probe pulse to implement preferential detection. In this work, we focus on vibrational imaging and report vibrational selective detection by shaping the probe pulse in time. Here, we demonstrate numerically and experimentally two pulse-shaping strategies with one functioning as a vibrational notch filter and the other functioning as a vibrational low-pass filter. This enables fast (25 μs/pixel) and selective hyperspectral imaging in the low-frequency regime (< 200 cm –1 ).

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Observation of polarization density waves in SrTiO 3

The nature of the incipient ferroelectric transition in SrTiO 3 has been a long-standing puzzle in condensed matter physics. One explanation involves the competition between ferroelectricity and an instability characterized by the mesoscopic modulation of the polarization. These polarization density waves, which should intensify near the quantum critical point, break local inversion symmetry and are difficult to characterize with conventional X-ray scattering methods. Here, in this study, we probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization at the nanometre scale in SrTiO3 by combining a femtosecond X-ray free-electron laser with terahertz coherent control methods. We found polar-acoustic collective modes that are soft, particularly at the tens of nanometre scale. These precursor collective excitations provide evidence for the conjectured mesoscopic-modulated phase in SrTiO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Quantum Simulation of Polarized Light-Induced Electron Transfer with a Trapped-Ion Qutrit System

Electron transfer within and between molecules is crucial in chemistry, biochemistry, and energy science. Here this study describes a quantum simulation method that explores the influence of light polarization on electron transfer between two molecules. By implementing precise and coherent control among the quantum states of trapped atomic ions, we can induce quantum dynamics that mimic the electron-transfer dynamics in molecules. We use three-level systems (qutrits), rather than traditional two-level systems (qubits), to enhance the simulation efficiency and realize high-fidelity simulations of electron-transfer dynamics. We treat the quantum interference between the electron coupling pathways from a donor with two degenerate excited states to an acceptor and analyze the transfer efficiency. We also examine the potential error sources that enter the quantum simulations. The trapped-ion systems have favorable scalings with system size compared to those of classical computers, promising access to richer electron-transfer simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Trigonal Bipyramidal V 3+ Complex as an Optically Addressable Molecular Qubit Candidate

Synthetic chemistry enables a bottom-up approach to quantum information science, where atoms can be deterministically positioned in a quantum bit or qubit. Two key requirements to realize quantum technologies are qubit initialization and read-out. By imbuing molecular spins with optical initialization and readout mechanisms, analogous to solid-state defects, molecules could be integrated into existing quantum infrastructure. To mimic the electronic structure of optically addressable defect sites, we designed the spin-triplet, V 3+ complex, (C 6 F 5 ) 3 trenVCN t Bu (1).We measured the static spin properties as well as the spin coherence time of1demonstrating coherent control of this spin qubit with a 240 GHz electron paramagnetic resonance spectrometer powered by a free electron laser. We found that1exhibited narrow, near-infrared photoluminescence (PL) from a spin-singlet excited state. Using variable magnetic field PL spectroscopy, we resolved emission into each of the ground-state spin sublevels, a crucial component for spin-selective optical initialization and readout. This work demonstrates that trigonally symmetric, heteroleptic V 3+ complexes are candidates for optical spin addressability.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2019

Coupling a single electron on superfluid helium to a superconducting resonator

Abstract Electrons on helium form a unique two-dimensional system on the interface of liquid helium and vacuum. A small number of trapped electrons on helium exhibits strong interactions in the absence of disorder, and can be used as a qubit. Trapped electrons typically have orbital frequencies in the microwave regime and can therefore be integrated with circuit quantum electrodynamics (cQED), which studies light–matter interactions using microwave photons. Here, we experimentally realize a cQED platform with the orbitals of single electrons on helium. We deterministically trap one to four electrons in a dot integrated with a microwave resonator, allowing us to study the electrons’ response to microwaves. Furthermore, we find a single-electron-photon coupling strength of $$g/2\pi =4.8\pm 0.3$$ g ∕ 2 π = 4.8 ± 0.3 MHz, greatly exceeding the resonator linewidth $$\kappa /2\pi =0.5$$ κ ∕ 2 π = 0.5 MHz. These results pave the way towards microwave studies of Wigner molecules and coherent control of the orbital and spin state of a single electron on helium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Magnetically brightened dark electron-phonon bound states in a van der Waals antiferromagnet

In van der Waals (vdW) materials, strong coupling between different degrees of freedom can hybridize elementary excitations into bound states with mixed character. Correctly identifying the nature and composition of these bound states is key to understanding their ground state properties and excitation spectra. Here, we use ultrafast spectroscopy to reveal bound states of d-orbitals and phonons in 2D vdW antiferromagnet NiPS 3 . These bound states manifest themselves through equally spaced phonon replicas in frequency domain. These states are optically dark above the Néel temperature and become accessible with magnetic order. By launching this phonon and spectrally tracking its amplitude, we establish the electronic origin of bound states as localized d–d excitations. Our data directly yield electron-phonon coupling strength which exceeds the highest known value in 2D systems. These results demonstrate NiPS 3 as a platform to study strong interactions between spins, orbitals and lattice, and open pathways to coherent control of 2D magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Isotope engineering for spin defects in van der Waals materials

Abstract Spin defects in van der Waals materials offer a promising platform for advancing quantum technologies. Here, we propose and demonstrate a powerful technique based on isotope engineering of host materials to significantly enhance the coherence properties of embedded spin defects. Focusing on the recently-discovered negatively charged boron vacancy center ($${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − ) in hexagonal boron nitride (hBN), we grow isotopically purified h 10 B 15 N crystals. Compared to$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − in hBN with the natural distribution of isotopes, we observe substantially narrower and less crowded$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − spin transitions as well as extended coherence timeT 2 and relaxation timeT 1 . For quantum sensing,$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − centers in our h 10 B 15 N samples exhibit a factor of 4 (2) enhancement in DC (AC) magnetic field sensitivity. For additional quantum resources, the individual addressability of the$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − hyperfine levels enables the dynamical polarization and coherent control of the three nearest-neighbor 15 N nuclear spins. Our results demonstrate the power of isotope engineering for enhancing the properties of quantum spin defects in hBN, and can be readily extended to improving spin qubits in a broad family of van der Waals materials.

Science & Technology - Other Topics↗
DOE OSTI2025

Resolving the phase of Fano resonance wave packets with photoelectron frequency-resolved optical gating

The creation of structured electronic wave packets (EWPs) energetically close to Fano resonances has been achieved with ultrafast extreme ultraviolet coherent light sources. However, direct real-time observations of EWP evolution and full reconstructions of the quantum properties of EWPs, including both amplitude and phase, are lacking. Here we introduce and demonstrate a comprehensive approach for the direct measurement and complete characterization of structured EWPs created within a prototypical Fano resonance. Because of its analogy with frequency-resolved optical gating (FROG), we named the method photoelectron FROG. The correlated EWP is initiated by a carefully engineered extreme UV pump pulse. A weak near-infrared laser field, serving as a probe pulse, samples the evolution of the EWPs in the time domain, as well as in the frequency domain. The amplitude and phase of the EWPs are obtained via a time-dependent reconstruction algorithm based on a short-time Fourier transformation. Given the excellent agreement between our experimental results and time-dependent reconstructions, we expect this method to be broadly applicable to the study of ultrafast processes, especially electronic ones, in complex systems, as well as the coherent control of such systems on their fundamental timescales.

quantum optics↗
DOE OSTI2023

High-fidelity parallel entangling gates on a neutral-atom quantum computer

The ability to perform entangling quantum operations with low error rates in a scalable fashion is a central element of useful quantum information processing. Neutral-atom arrays have recently emerged as a promising quantum computing platform, featuring coherent control over hundreds of qubits and any-to-any gate connectivity in a flexible, dynamically reconfigurable architecture. The main outstanding challenge has been to reduce errors in entangling operations mediated through Rydberg interactions. Here we report the realization of two-qubit entangling gates with 99.5% fidelity on up to 60 atoms in parallel, surpassing the surface-code threshold for error correction. Our method uses fast, single-pulse gates based on optimal control, atomic dark states to reduce scattering and improvements to Rydberg excitation and atom cooling. We benchmark fidelity using several methods based on repeated gate applications, characterize the physical error sources and outline future improvements. Finally, we generalize our method to design entangling gates involving a higher number of qubits, which we demonstrate by realizing low-error three-qubit gates. By enabling high-fidelity operation in a scalable, highly connected system, these advances lay the groundwork for large-scale implementation of quantum algorithms, error-corrected circuits and digital simulations.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2021

Crystal phases of charged interlayer excitons in van der Waals heterostructures

Throughout the years, strongly correlated coherent states of excitons have been the subject of intense theoretical and experimental studies. This topic has recently boomed due to new emerging quantum materials such as van der Waals (vdW) bound atomically thin layers of transition metal dichalcogenides (TMDs). We analyze the collective properties of charged interlayer excitons observed recently in bilayer TMD heterostructures. We predict strongly correlated phases—crystal and Wigner crystal—that can be selectively realized with TMD bilayers of properly chosen electron-hole effective masses by just varying their interlayer separation distance. Our results can be used for nonlinear coherent control, charge transport and spinoptronics application development with quantum vdW heterostuctures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe 2

In this report 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 coupling resulting in a vibronic bound state. Complex, mesoscale interplay between phonon modes and CEF modes is observed in real space. Additionally, an unexpected resonant Raman excitation condition is satisfied, yielding up to third-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.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Engineering local strain for single-atom nuclear acoustic resonance in silicon

Mechanical strain plays a key role in the physics and operation of nanoscale semiconductor systems, including quantum dots and single-dopant devices. In this report we describe the design of a nanoelectronic device, where a single nuclear spin is coherently controlled via nuclear acoustic resonance (NAR) through the local application of dynamical strain. The strain drives spin transitions by modulating the nuclear quadrupole interaction. We adopt an AlN piezoelectric actuator compatible with standard silicon metal–oxide–semiconductor processing and optimize the device layout to maximize the NAR drive. We predict NAR Rabi frequencies of order 200 Hz for a single 123Sb nucleus in a wide region of the device. Spin transitions driven directly by electric fields are suppressed in the center of the device, allowing the observation of pure NAR. Using electric field gradient-elastic tensors calculated by the density-functional theory, we extend our predictions to other high-spin group-V donors in silicon and to the isoelectronic 73Ge atom.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Electron choreography at the attosecond time scale

Abstract In this work, we report on coherent control of electron dynamics in atoms via attosecond pulse-shaping. We show that the photoelectron emission from argon gas produced by absorption of an attosecond pulse train (APT) made of odd and even harmonics can be manipulated along the direction of polarization of the light by tuning the spectral components (amplitude and phase) of the pulse. In addition, we show that APTs produced with a two-color (400- plus 800 nm) femtosecond driving field exhibit high temporal tunability, which is optimized for an intensity ratio between the two colors in the range of 0.1 to 5%.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Topological quantum interference in a pumped Su-Schrieffer-Heeger lattice

Topological quantum interference emerges from the interplay between quantum mechanics and topology. We present evidence for two types of such interference phenomenon that can result from the quantum dynamics of initial topological states. We realize both types of topological quantum interference in a pumped non-Hermitian Su-Schrieffer-Heeger lattice that can be implemented by creation and coherent control of excitonic states of trapped neutral atoms. On quenching the system from the topological to the gapless phases and then back again, we find that interference patterns develop in the gapless phase and also after switching back to the topological phase. These patterns occur both as many-excitation interferences generated in the presence of pumping the atoms at the end sites, and as one- and two-excitation interferences seen in the absence of pumping when starting with edge excitations. Investigation of the excitation dynamics shows that these interference patterns originate from the topological nature of the initial states and are very different from quantum interferences originating from nontopological states of the lattice. Our results also reveal that unlike well-known situations where topological states are protected against local perturbations, in the non-Hermitian SSH systems resulting from driving the excited-state populations, a local dissipation at each lattice site can suppress both the topological interference and the total population of the lattice.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Dynamical properties of a driven dissipative dimerized $S$ =1/2 chain

We consider the dynamical properties of a gapped quantum spin system coupled to the electric field of a laser, which drives the resonant excitation of specific phonon modes that modulate the magnetic interactions. Here, we deduce the quantum master equations governing the time-evolution of both the lattice and spin sectors, by developing a Lindblad formalism with bath operators providing an explicit description of their respective phonon-mediated damping terms. We investigate the nonequilibrium steady states (NESS) of the spin system established by a continuous driving, delineating parameter regimes in driving frequency, damping, and spin-phonon coupling for the establishment of physically meaningful NESS and their related nontrivial properties. Focusing on the regime of generic weak spin-phonon coupling, we characterize the NESS by their frequency and wave-vector content, explore their transient and relaxation behavior, and discuss the energy flow, the system temperature, and the critical role of the type of bath adopted. Our study lays a foundation for the quantitative modeling of experiments currently being designed to control coherent many-body spin states in quantum magnetic materials.

1-dimensional spin chains↗
DOE OSTI2020

Coherent Transfer of Spin Angular Momentum by Evanescent Spin Waves within Antiferromagnetic NiO

Insulating antiferromagnets are efficient and robust conductors of spin current. To realise the full potential of these materials within spintronics, the outstanding challenges are to demonstrate scalability down to nanometric lengthscales and the transmission of coherent spin currents. Here, we report the coherent transfer of spin angular momentum by excitation of evanescent spin waves of GHz frequency within antiferromagnetic NiO at room temperature. Using element-specific and phase-resolved x-ray ferromagnetic resonance, we probe the injection and transmission of ac spin current, and demonstrate that insertion of a few nanometre thick epitaxial NiO(001) layer between a ferromagnet and non-magnet can even enhance the flow of spin current. Our results pave the way towards coherent control of the phase and amplitude of spin currents at the nanoscale, and enable the realization of spin-logic devices and spin current amplifiers that operate at GHz and THz frequencies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Controlling $T_c$ through Band Structure and Correlation Engineering in Collapsed and Uncollapsed Phases of Iron Arsenides

Recent observations of selective emergence (suppression) of superconductivity in the uncollapsed (collapsed) tetragonal phase of LaFe 2 As 2 has rekindled interest in understanding what features of the band structure control the superconducting $T_c$. In this work, we show that the proximity of the narrow Fe-$d_{xy}$ state to the Fermi energy emerges as the primary factor. In the uncollapsed phase this state is at the Fermi energy, and is most strongly correlated and a source of enhanced scattering in both single and two particle channels. The resulting intense and broad low energy spin fluctuations suppress magnetic ordering and simultaneously provide glue for Cooper pair formation. In the collapsed tetragonal phase, the $d_{xy}$ state is driven far below the Fermi energy, which suppresses the low-energy scattering and blocks superconductivity. A similar source of broad spin excitation appears in uncollapsed and collapsed phases of CaFe 2 As 2 . This suggests controlling coherence provides a way to engineer $T_c$ in unconventional superconductors primarily mediated through spin fluctuations.

36 MATERIALS SCIENCE↗