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DOE OSTI2026

Many-body entanglement in solid-state emitters

The preparation and control of quantum states lie at the heart of quantum information science. Recent advances in solid-state quantum emitters (QEs) and nanophotonics have transformed the landscape of quantum photonic technologies, enabling scalable generation of quantum states of light and matter. A new frontier in solid-state quantum photonics is the engineering of many-body interactions between QEs and photons to achieve robust coherence and controllable many-body entanglement. These entangled states, including photonic graph and cluster states, superradiant emission and emergent quantum phases, are promising for quantum computation, sensing and simulation. However, intrinsic inhomogeneities and decoherence in solid-state platforms pose considerable challenges in realizing such complex entangled states. This Review provides an overview of fundamental many-body interactions and dynamics at the light–matter interfaces of solid-state QEs and discusses recent advances in mitigating decoherence and harnessing robust many-body coherence.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Hydrogen density mapping in biomolecular crystals through dynamic nuclear polarization

Many fundamental biological processes, including those in photosynthetic reaction centers and enzyme active sites, involve charge and energy transfer, bond cleavage, protonation and hydrogen bonding. Because H atoms play such central roles in these reactions, accurately determining their positions is essential. Yet, conventional X-ray crystallography primarily resolves the heavy atoms in biological structures and provides limited insight into hydrogen, even at atomic resolution. Neutron macromolecular crystallography (NMC) overcomes this limitation by offering exceptional sensitivity to hydrogen and deuterium. Here, we present a theoretical framework for the development of dynamic nuclear polarization NMC (DNP-NMC) techniques, which exploit the alignment of neutron and proton nuclear spins to enhance and tune the hydrogen signal contribution. The DNP-NMC approach advances the resolution of H atoms within biomolecular crystals, whether bound to protein residues or present in solvent. The method establishes key relationships for the coherent structure factor of polarized neutron scattering from hydrogenous matter. It theoretically achieves full accuracy in phase reconstruction and offers a path to improve neutron structure determination, achieving accuracies exceeding ≳80% by incorporating titration states. Using a variant of the hybrid input/output phase-retrieval algorithm, it allows recovery of the hydrogen density with ≳90% phase accuracy. In conclusion, we further discuss sources of experimental uncertainty for the upcoming DNP-enabled, quasi-Laue IMAGINE-X experiment at Oak Ridge National Laboratory's High Flux Isotope Reactor.

dynamic nuclear polarization↗

DOE OSTI2025

Revealing rotational symmetry breaking charge density wave order in the kagome superconductor (Rb, K)⁢V 3 ⁢Sb 5 by ultrafast pump-probe experiments

The recently discovered Kagome superconductor 𝐴⁢V 3 ⁢Sb 5 (where 𝐴 refers to K, Rb, Cs) has stimulated widespread research interest due to its interplay of nontrivial topology and unconventional correlated physics including charge-density waves (CDW) and superconductivity. The essential prerequisite to understanding the microscopic mechanisms of this complex electronic landscape is to unveil the configuration and symmetry of the charge-density wave order. As to now, little consensus has been made on what symmetry is broken. Herein, we clarify the microscopic structure and symmetry breaking of the CDW phase in RbV 3 ⁢Sb 5 and KV 3 ⁢Sb 5 by ultrafast time-resolved reflectivity. Our approach is based on extracting coherent phonon spectra induced by three-dimensional CDW and comparing them to calculated phonon frequencies via density-functional theory. The combination of these experimental results and calculations provides compelling evidence that the CDW structure of both compounds prevailing up to 𝑇 CDW is the 2 × 2 × 2 staggered inverse Star-of-David pattern with interlayer 𝜋 phase shift, in which the sixfold rotational symmetry is broken. Finally, these observations thus corroborate sixfold rotational symmetry breaking throughout the CDW phase of RbV 3 ⁢Sb 5 and KV 3⁢ Sb 5 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

ZTF SN Ia DR2: Improved SN Ia colors through expanded dimensionality with SALT3+

Context. Type Ia supernovae (SNe Ia) are a key probe in modern cosmology, as they can be used to measure luminosity distances at gigaparsec scales. Models of their light curves are used to project heterogeneous observed data onto a common basis for analysis. Aims. The SALT model currently used for SN Ia cosmology describes SNe as having two sources of variability, accounted for by a color parameter c , and a “stretch” parameter x 1 . We extend the model to include an additional parameter we label x 2 , to investigate the cosmological impact of currently unaddressed light-curve variability. Methods. We constructed a new SALT model, that we dub “SALT3+”. This model was trained by an improved version of the SALTshaker code, using training data combining a selection of the second data release of cosmological SNe Ia from the Zwicky Transient Facility and the existing SALT3 training compilation. Results. We find additional, coherent variability in supernova light curves beyond SALT3. Most of this variation can be described as phase-dependent variation in g − r and r − i color curves, correlated with a boost in the height of the secondary maximum in i -band. These behaviors correlate with spectral differences, particularly in line velocity. We find that fits with the existing SALT3 model tend to address this excess variation with the color parameter, leading to less informative measurements of supernova color. We find that neglecting the new parameter in light-curve fits leads to a trend in Hubble residuals with x 2 of 0.039 ± 0.005 mag, representing a potential systematic uncertainty. However, we find no evidence of a bias in current cosmological measurements. Conclusions. We conclude that extended SN Ia light-curve models promise mild improvement in the accuracy of color measurements, and corresponding cosmological precision. However, models with more parameters are unlikely to substantially affect current cosmological results.

Kenworthy, W. D. (ORCID:0000000251535983)↗

DOE OSTI2025

Stretched exponential magnetic relaxation dynamics in artificial square ice revealed through x-ray photon correlation spectroscopy

X-ray photon correlation scattering measurements are undertaken on a thermally active artificial spin ice based on the square lattice, referred to as artificial square ice, to probe the fluctuation timescales as a function of temperature as the system passes through the paramagnetic-antiferromagnetic phase transition, which belongs to the two-dimensional Ising universality class. In the paramagnetic regime, a single exponential timescale is seen, whereas at and below the critical temperature, a stretched exponential decorrelation is observed, with the stretching exponent decreasing from unity down to below one-half as the temperature reduces. This trend is confirmed by kinetic Monte Carlo simulations of a simplified point-dipolar square ice system, and is in agreement with past theoretical work on the kinetic Ising model where stretched exponential relaxation due to equilibrium domain wall dynamics below the critical temperature was found.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Quantification of Native Lignin Structural Features with Gel–Phase 2D–HSQC 0 Reveals Lignin Structural Changes During Extraction

Our ability to study and valorize the lignin fraction of biomass is hampered by the fundamental and still unmet challenge of precisely quantifying native lignin's structural features. Here, we developed a rapid elevated-temperature 1 H– 13 C Heteronuclear Single-Quantum Coherence Zero (HSQC 0 ) NMR method that enables this precise quantification of native lignin structural characteristics even with whole plant cell wall (WPCW) NMR spectroscopy, overcoming fast spin relaxation in the gel phase. We also formulated a Gaussian fitting algorithm to perform automatic and reliable spectral integration. By combining HSQC 0 measurements with yield measurements following depolymerisation, we can confirm the combinatorial nature of radical coupling reactions during biosynthesis leading to a random sequential organization of linkages within a largely linear lignin chain. Such analyses illustrate how this analytical method can greatly facilitate the study of native lignin structure, which can then be used for fundamental studies or to understand lignin depolymerization methods like reductive catalytic fractionation or aldehyde-assisted fractionation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Quantification of Native Lignin Structural Features with Gel–Phase 2D–HSQC 0 Reveals Lignin Structural Changes During Extraction

09 BIOMASS FUELS↗

DOE OSTI2026

Observation of room-temperature charge density wave correlations via coherent phonon spectroscopy in the Sn-doped kagome superconductor CsV 3 ⁢Sb 5

In this study, we perform ultrafast time-resolved reflectivity measurements to track the evolution of charge density wave (CDW) correlations in Sn-doped Kagome superconductor CsV 3⁢ Sb 5−𝑥 ⁢Sn 𝑥 . By extracting the coherent phonon spectrum, we evidence robust signatures of CDW correlations at temperature and doping ranges far beyond the phase boundary of long-range CDW order. Remarkably, we show that short-range CDW correlations survive up to room temperature in 𝑥 = 0.32 Sn-doped CsV 3 ⁢Sb 5 , supported by synchrotron x-ray diffraction measurements. We point out that the introduction of quenched disorder by Sn doping can pin the CDW and form static short-range CDW, which can explain the observed persistent CDW signatures. Our results thus corroborate the ubiquity and robustness of CDW correlations in Sn-doped CsV 3⁢ Sb 5 and provide new insights on the role of disorders on the CDW correlations in AV 3 ⁢Sb 5 family.

Charge density waves↗

DOE OSTI2025

Demonstration of controlled spatial incoherence for beam smoothing

A concept for beam smoothing of high-energy laser systems is demonstrated. Multiple coherent beams are multiplexed so that their incoherent mix decreases the far-field nonuniformity after random spatial phase modulation introduced by a phase plate. Modeling shows that the incoherent mix effectively leads to the expected scaling in terms of the number of uncorrelated beams, and that spatial multiplexing can be combined with smoothing by spectral dispersion. The results of an experimental demonstration of this concept with up to six beams, leading to more than 40 modes with polarization multiplexing and angular dispersion, are consistent with expectations. The potential practical advantages of this smoothing scheme and future developments are discussed.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Prolonging All-Optical Molecular Electron Spin Coherence in the Tissue Transparency Window

Coherent electron spin states within paramagnetic molecules hold significant potential for microscopic quantum sensing. However, all-optical coherence measurements amenable to high spatial and temporal resolution under ambient conditions remain a significant challenge. Here we conduct room-temperature, picosecond time-resolved Faraday ellipticity/rotation (TRFE/R) measurements of the electron spin decoherence time T 2 * in [IrBr 6 ] 2- . Decoherence is strongly sensitive to solution phase viscosity, pointing to molecular tumbling as an important decoherence mechanism. Accordingly, immobilization of [IrBr 6 ] 2- molecules in thin polymer films results in an order-of-magnitude increase in coherence lifetime and significantly greater magnetic field sensitivity. Here, by tuning energies of ligand-to-metal charge transfer (LMCT) states, TRFE/R enables spin initialization and readout in the tissue transparency window, paving the way toward all-optical, ultrafast molecular electron spin coherence imaging in biological systems.

Electron paramagnetic resonance spectroscopy↗

DOE OSTI2024

Diagnostics of Mixed-State Topological Order and Breakdown of Quantum Memory

Topological quantum memory can protect information against local errors up to finite error thresholds. Such thresholds are usually determined based on the success of decoding algorithms rather than the intrinsic properties of the mixed states describing corrupted memories. Here we provide an intrinsic characterization of the breakdown of topological quantum memory, which both gives a bound on the performance of decoding algorithms and provides examples of topologically distinct mixed states. We employ three information-theoretical quantities that can be regarded as generalizations of the diagnostics of ground-state topological order, and serve as a definition for topological order in error-corrupted mixed states. We consider the topological contribution to entanglement negativity and two other metrics based on quantum relative entropy and coherent information. In the concrete example of the two-dimensional (2D) Toric code with local bit-flip and phase errors, we map three quantities to observables in 2D classical spin models and analytically show they all undergo a transition at the same error threshold. This threshold is an upper bound on that achieved in any decoding algorithm and is indeed saturated by that in the optimal decoding algorithm for the Toric code. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Large-𝑁 SU(4) Schwinger boson theory for coupled-dimer antiferromagnets

Here, we develop a systematic large-𝑁 expansion based on the Schwinger boson representation of SU(4) coherent states of dimers for the paradigmatic spin-1/2 bilayer square lattice Heisenberg antiferromagnet. This system exhibits a quantum phase transition between a quantum paramagnetic state and a Néel order state, driven by the coupling constant 𝑔 = 𝐽′/𝐽, which is defined as the ratio between the interdimer 𝐽′ and intradimer 𝐽 exchange interactions. We demonstrate that this approach accurately describes static and dynamic properties on both sides of the quantum phase transition. The critical coupling constant 𝑔 𝑐 ≈ 0.42 and the dynamic spin structure factor reproduce quantum Monte Carlo results with high precision. Notably, the 1/𝑁 corrections reveal the longitudinal mode of the magnetically ordered phase along with the overdamping caused by its decay into the two-magnon continuum. The present large-𝑁 SU(4) Schwinger boson theory can be extended to more general cases of quantum paramagnets that undergo a quantum phase transition into magnetically ordered states.

Schwinger boson method↗

DOE OSTI2026

Exact Fock-State Preparation with $n^{1/4}$ Circuit Depth

Efficient, deterministic, and high-fidelity preparation of large Fock states is essential for scaling bosonic quantum technologies and exploring quantum phenomena at large excitation energies. We introduce a deterministic one-parameter (D1p) protocol that maps Fock-state preparation in an infinite-dimensional Hilbert space onto two-dimensional amplitude amplification. Starting from a coherent state with $|α|\simeq\sqrt{n}$, the initial target-state population scales as $n^{-1/2}$, yielding an iteration count and circuit depth of $\mathcal{O}(n^{1/4})$. Phase matching guarantees unit fidelity in the ideal model; remarkably, preparing $|{10^6}\rangle$ requires only 39 iterations. The protocol uses only displacements and number-selective phase operations, requires no numerical optimization, and further extends to state transfer, general superpositions, finite-dimensional systems, and multipartite entangled states. In the large-amplitude regime, its multi-target form prepares $L$-legged cat states with an iteration count determined only by $L$; cats with up to ten legs require only two iterations, independent of the coherent-state amplitude. This framework provides a broadly applicable route to highly excited bosonic states on platforms supporting these elementary controls.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗

DOE OSTI2025

The importance of shear on the collective charge transport in CDWs revealed by an XFEL source

Charge transport in materials has an impact on a wide range of devices based on semiconductor, battery, or superconductor technology. Charge transport in sliding charge density waves (CDW) differs from all others in that the atomic lattice is directly involved in the transport process. To obtain an overall picture of the structural changes associated to the collective transport, the large coherent x-ray beam generated by an x-ray free-electron laser (XFEL) source was used. The CDW phase can be retrieved over the entire sample from diffracted intensities using a genetic algorithm. For currents below threshold, increasing shear deformation is observed in the central part of the sample while longitudinal deformation appears above threshold when shear relaxes. Shear thus precedes longitudinal deformation, with relaxation of one leading to the appearance of the other. Moreover, strain accumulates on surface steps in the sliding regime, demonstrating the strong pinning character of these surface discontinuities. The sliding process of nanometric CDW involves macroscopic sample dimensions.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Coupling magnons to an opto-electronic parametric oscillator

Hybrid magnonic systems have emerged as versatile modular components for quantum signal transduction and sensing applications owing to their capability of connecting distinct quantum platforms. To date, the majority of the magnonic systems have been explored in a local, near-field scheme, due to the close proximity required for realizing a strong coupling between magnons and other excitations. This constraint greatly limits the applicability of magnons in developing remotely coupled, distributed quantum network systems. On the contrary, opto-electronic architectures hosting self-sustained oscillations have been a unique platform for long-haul signal transmission and processing. Here, we integrated an opto-electronic oscillator with a magnonic oscillator consisting of a microwave waveguide and a Y 3 Fe 5 O 12 (YIG) sphere, and demonstrated strong and coherent coupling between YIG’s magnon modes and the opto-electronic oscillator’s characteristic photon modes—revealing the hallmark anti-crossing gap in the measured spectrum. In particular, the photon mode is produced on-demand via a nonlinear, parametric process as stipulated by an external seed pump. Both the internal cavity phase and the external pump phase can be precisely tuned to stabilize either degenerate or nondegenerate auto-oscillations. Our result lays out a new, hybrid platform for investigating the long-distance coupling and nonlinearity in coherent magnonic phenomena, which may be found useful in constructing the future “distributed hybrid magnonic systems.”

36 MATERIALS SCIENCE↗

DOE OSTI2024

Quantum Spin Dynamics Due to Strong Kitaev Interactions in the Triangular-Lattice Antiferromagnet CsCeSe 2

The extraordinary properties of the Kitaev model have motivated an intense search for new physics in materials that combine geometrical and bond frustration. In this Letter, we employ inelastic neutron scattering, spin wave theory, and exact diagonalization to study the spin dynamics in the perfect triangular-lattice antiferromagnet (TLAF) CsCeSe 2 . This material orders into a stripe phase, which is demonstrated to arise as a consequence of the off-diagonal bond-dependent terms in the spin Hamiltonian. By studying the spin dynamics at intermediate fields, we identify an interaction between the single-magnon state and the two-magnon continuum that causes decay of coherent magnon excitations, level repulsion, and transfer of spectral weight to the continuum that are controlled by the strength of the magnetic field. Our results provide a microscopic mechanism for the stabilization of the stripe phase in TLAF and show how complex many-body physics can be present in the spin dynamics in a magnet with strong Kitaev coupling even in an ordered ground state. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

A topological superconductor tuned by electronic correlations

A topological superconductor, characterized by either a chiral order parameter or a topological surface state in proximity to bulk superconductivity, is foundational to topological quantum computing. A key open challenge is whether electron-electron interactions can tune such topological superconducting phases. Here, we provide experimental signatures of a unique topological superconducting phase in competition with electronic correlations in 10-unit-cell thick FeTe x Se 1-x films grown on SrTiO 3 substrates. When the Te content x exceeds 0.7, we observe a topological transition marked by the emergence of a superconducting surface state. Near the FeTe limit, the system undergoes another transition where the surface state disappears, and superconductivity is suppressed. Theory suggests that electron-electron interactions in the odd-parity xy− band drives this second topological transition. The flattening and eventual decoherence of d xy -derived bands track the superconducting dome, linking correlation effects directly to superconducting coherent transport. Our work establishes many-body electronic correlations as a sensitive knob for tuning topology and superconductivity, offering a pathway to engineer new topological phases in correlated materials.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Topology and spectral entanglement in cavity-mediated photon scattering

Here, we develop a microscopic diagrammatic theory for cavity-mediated photon scattering in a topological one-dimensional insulator described by the Su–Schrieffer–Heeger model. Within the velocity-gauge formulation, we derive the photon self-energy and vertex corrections arising from virtual electron–hole excitations coupled to a quantized cavity mode, and we evaluate the resulting polariton dispersion and two-photon correlation spectra. Our analysis shows that vacuum fluctuations of the cavity field induce a momentum-resolved self-energy that mixes conduction and valence bands through virtual photon exchange, producing interband hybridization and avoided crossings in the electronic dispersion. This “cavity dressing” is symmetry-dependent, vanishing at the Brillouin-zone edge where the dipole matrix element is zero, and its strength is controlled by the spatial coherence range ζ ≈ (l c /a) 2 of virtual excitations. We further examine how the cavity modifies nonlinear optical observables, including the Kerr nonlinearity and biphoton spectral entanglement, and identify the regimes where these effects become sensitive to the underlying topological phase. The theoretical framework established here provides a unified description of light–matter coupling in topological and polaritonic systems, bridging solid-state cavity QED with the emerging field of cavity-modified quantum materials. Our results suggest that engineered photonic environments can coherently reshape the electronic landscape of topological insulators, offering new routes to control collective electronic and optical phenomena through vacuum-field fluctuations.

74 ATOMIC AND MOLECULAR PHYSICS↗