Showing 1–50 of 83 results for author: Miller, R

Demonstration of a scalable all-solid-state refrigerator exploiting diffusion geometries and limiting interfacial conductances at temperatures below 1 kelvin

Authors: Northrop Grumman Microelectronics Design, Applications Team, :, Robert M. Young, Zachary Stegen, John X. Przybysz, Edward R. Engbrecht, Aaron A. Hathaway, Justin C. Hackley, Kirby B. Myers, Christian C. Thorpe, Aurelius L. Graninger, Robert Miller, Diego A. Morales, Roberto D. Carcamo, Glen Walters, Jeric P. Sarad, Nicholas F. Pleim, Seth Whitsitt, Joshua T. Shipman, Anil Erol, Melissa G. Loving, Evan Donohue, Corey A. Kegerreis, Benjamin Dalfort , et al. (13 additional authors not shown)

Abstract: Solid-state refrigerators using Normal-metal/Insulator/Superconductor (NIS) junctions have previously demonstrated excellent electron cooling but limited ability to cool phonons. The energy gap of the superconductor is used as an energy filter to allow higher than average energy electrons to preferentially tunnel from the normal-metal through the insulator into the superconductor where they travel… ▽ More Solid-state refrigerators using Normal-metal/Insulator/Superconductor (NIS) junctions have previously demonstrated excellent electron cooling but limited ability to cool phonons. The energy gap of the superconductor is used as an energy filter to allow higher than average energy electrons to preferentially tunnel from the normal-metal through the insulator into the superconductor where they travel as quasi-particles. Typically, the heat is moved and work is done to deposit hot quasi-particles into a normal-metal quasi-particle trap for rejection to the next refrigeration stage. Realizing that (1) the quasi-particles flow diffusively, driven by a concentration gradient in the electric field-free superconductor, and (2) that the undesirable backwards leaking of heat from the hot-side trap can be reduced by engineering the geometry and materials at the superconductor-to-trap interface, enhanced cooling can be achieved. Fabrication of the refrigerator was accomplished using a tungsten and titanium-tungsten alloy as the cold-side normal-metal, aluminum oxide as the insulator, aluminum as the superconductor, and gold as the trap, with the cold-side NIS portion being attached to the hot-side gold trap by bump bonding. The refrigerator consisted of 1121 junction pairs, each pair being an SINIS unit, all electrically connected in series. Using this we have measured the effective phonon temperature of a 3.9 mm x 3.9 mm x 0.65 mm silicon chip driven down to 70 mK from a bath temperature of 120 mK, and down to 174 mK from a 271 mK rejection temperature (a cooling of -97 mK). This is the first demonstration of the sub 1 K cooling of an entire silicon chip using NIS junctions. △ Less

Submitted 20 August, 2026; v1 submitted 17 August, 2026; originally announced August 2026.

Detection of scintillation light in noble gases with wavelength-shifting optical fibers

Authors: S. R. Soleti, S. Torelli, G. Martínez-Lema, H. Almazán, A. Beck, A. Castillo, M. del Barrio-Torregrosa, P. Dietz, C. Echeverria, L. Gurriana, Y. Ifergan, I. Israelashvili, F. Lopez, F. Monrabal, E. Oblak, J. Pelegrin, J. G. M. Saraiva, M. Seemann, L. Arazi, J. J. Gómez-Cadenas, V. Álvarez, I. J. Arnquist, F. Auria-Luna, S. Ayet, Y. Ayyad , et al. (88 additional authors not shown)

Abstract: Wavelength-shifting (WLS) techniques enable particle detectors based on noble gases, whose scintillation light is predominantly emitted in the vacuum-ultraviolet. We investigate WLS fibers coated with tetraphenyl butadiene (TPB) for scintillation light detection in gaseous xenon and argon at pressures up to 8.5 bar, motivated by future high-pressure xenon time-projection chambers of the NEXT progr… ▽ More Wavelength-shifting (WLS) techniques enable particle detectors based on noble gases, whose scintillation light is predominantly emitted in the vacuum-ultraviolet. We investigate WLS fibers coated with tetraphenyl butadiene (TPB) for scintillation light detection in gaseous xenon and argon at pressures up to 8.5 bar, motivated by future high-pressure xenon time-projection chambers of the NEXT program. Two detector configurations are studied: an elongated high-pressure vessel with four PTFE panels equipped with WLS fibers read by temperature-stabilized SiPMs, and a compact box-shaped detector operated at 1 bar Xe with WLS fibers read out by PMTs. Both operate with continuous gas purification. The detector response is characterized using cosmic muons and alpha particles from a $^{241}$Am source. With the SiPM setup, we measure a light collection efficiency (LCE) of ${1.18 \pm 0.01~\mathrm{(sta.)}~^{+0.07}_{-0.09}~\mathrm{(sys.)}~\%}$ for xenon and ${1.07 \pm 0.01~\mathrm{(sta.)}~^{+0.06}_{-0.08}~\mathrm{(sys.)}~\%}$ for argon. With PMT readout, we measure a LCE of ${0.45 \pm 0.01~\mathrm{(sta.)} \pm 0.05~\mathrm{(sys.)}~\%}$ in xenon, in agreement with the SiPM result once photon detection efficiency is accounted for. Average scintillation waveforms in xenon and argon are studied to assess the time structure of the emitted light. Cosmic-muon measurements yield a mean energy required to produce a scintillation photon $45\pm7~\mathrm{(sta.)}~^{+4}_{-5}~\mathrm{(sys.)}~\mathrm{eV}$ at 1.5 bar, in agreement with the literature. The results demonstrate that TPB-coated WLS fiber systems can reliably detect scintillation light in high-pressure gaseous noble detectors, with a LCE representing an upper limit for realistic large-scale TPCs, where additional photon losses from materials and fiber attenuation are expected. △ Less

Submitted 6 July, 2026; originally announced July 2026.

Comments: 19 pages, 15 figures

Conical Intersections Enable Ultrafast Molecular Spin Control in a Chromium Complex

Authors: Zihui Liu, Junhua Zhou, Tianrui Chen, Michael Penny, Sara Mosca, Mengyuan Cui, Vandana Tiwari, R. J. Dwayne Miller, Fulu Zheng, Ajay Jha, Hong-Guang Duan

Abstract: Molecular spintronics seeks to control spin states in single molecules for ultrafast switching and efficient information processing. Transition metal complexes are promising candidates for such applications due to their modular ligand fields, diverse spin configurations, and potential for spin-vibronic coupling that facilitates rapid spin dynamics. Chromium(III) complexes, in particular, offer lon… ▽ More Molecular spintronics seeks to control spin states in single molecules for ultrafast switching and efficient information processing. Transition metal complexes are promising candidates for such applications due to their modular ligand fields, diverse spin configurations, and potential for spin-vibronic coupling that facilitates rapid spin dynamics. Chromium(III) complexes, in particular, offer long-lived emissive doublet states and chemical robustness, making them attractive for room-temperature spin control. Here we investigate the spin-state dynamics of tris(2,4-pentanedionato)chromium(III), [Cr(acac)3], a photochemically stable d3 complex with minimal vibrational congestion. Using ultrafast transient grating and two dimensional electronic spectroscopy with ~10 fs resolution, we directly probe vibrational and electronic dynamics associated with the 4T2 -> 2E intersystem crossing (ISC). These measurements reveal coherent vibrational modes implicated in mediating nonadiabatic spin transitions. Complementary theoretical modelling shows that vibronic coupling and spin orbit interactions promote the formation of multiple conical intersections, providing ultrafast channels for spin-flip dynamics. Metal-ligand bending and stretching modes serve as tuning and coupling coordinates, enabling ISC despite weak spin-orbit coupling in 3d transition metal. Our study provides mechanistic insight into spin-vibronic dynamics in Cr(III) complexes and establishes a design framework for achieving ultrafast molecular spin switching, advancing the development of optically addressable spin centres for future spintronic and quantum technologies. △ Less

Submitted 30 June, 2026; originally announced June 2026.

Stochastic Cluster Expansion for Excited State Energies

Authors: Annabelle Canestraight, Russell Miller, Libor Veis, Vojtech Vlcek

Abstract: Excited-state electronic structure in strongly correlated systems remains challenging due to the exponential scaling of the many-body Hilbert space and the difficulty of constructing systematically controlled active spaces. Building on the stochastic cluster expansion (SCE) framework previously developed for ground-state correlation energies, we extend the formalism to excitation gaps by expressin… ▽ More Excited-state electronic structure in strongly correlated systems remains challenging due to the exponential scaling of the many-body Hilbert space and the difficulty of constructing systematically controlled active spaces. Building on the stochastic cluster expansion (SCE) framework previously developed for ground-state correlation energies, we extend the formalism to excitation gaps by expressing energy differences directly as a hierarchy of orbital-space cluster contributions. In this formulation, excitation energies are reconstructed from reduced-rank calculations involving a minimal frontier chemical subspace (FCS), treated exactly, together with stochastic sampling of the remaining orbital environment. This approach eliminates the need for large or chemically preselected active spaces. We demonstrate the method on charge-transfer complexes and polyacenes, where accurate singlet-triplet gaps are obtained that agree with full-system results. The method converges with low-order cluster terms and provides a systematically improvable framework for excited states in correlated systems. △ Less

Submitted 1 May, 2026; originally announced May 2026.

Electroluminescence Yield Measurements in Xenon Gas with the NEXT-DEMO++ Detector

Authors: NEXT Collaboration, J. Renner, J. D. Villamil, N. López-March, K. Mistry, P. Novella, A. Simón, V. Álvarez, J. M. Benlloch-Rodríguez, M. Cid, C. Cortes-Parra, R. Esteve, F. Kellerer, J. Martín-Albo, A. Martínez, G. Martínez-Lema, M. Martínez-Vara, M. Querol, P. Saharia, M. Sorel, S. Teruel-Pardo, H. Almazán, L. Arazi, I. J. Arnquist, F. Auria-Luna , et al. (89 additional authors not shown)

Abstract: The NEXT-DEMO++ detector, a high-pressure xenon gas time projection chamber serving as a prototype for the NEXT-100 experiment, was used to measure the electroluminescence (EL) yield as a function of reduced electric field ($E/p$) across pressures from 2.0 to 9.4 bar, utilizing the 41.5 keV de-excitation peak of $^{83m}$Kr. These measurements were made to examine the pressure dependence of the slo… ▽ More The NEXT-DEMO++ detector, a high-pressure xenon gas time projection chamber serving as a prototype for the NEXT-100 experiment, was used to measure the electroluminescence (EL) yield as a function of reduced electric field ($E/p$) across pressures from 2.0 to 9.4 bar, utilizing the 41.5 keV de-excitation peak of $^{83m}$Kr. These measurements were made to examine the pressure dependence of the slope of the reduced EL yield $Y/p$, which has shown inconsistencies in the literature. The reduced yield was fitted with a linear model, revealing a modest ($\sim$5%) change in slope, beginning around 5 bar and increasing with pressure up to 9.4 bar. △ Less

Submitted 17 April, 2026; originally announced April 2026.

Comments: 8 pages, 5 figures

Increasing ultrasound field-of-view with reduced element count arrays containing large elements

Authors: Mick Gardner, Rita J. Miller, Michael L. Oelze

Abstract: Several applications of medical ultrasound can benefit from a larger field of view (FOV). This study is aimed at increasing the FOV of linear array probes by increasing the element width. Coupled elements were used to imitate a larger element width. Through Fourier analysis, theoretical pressure amplitudes, and bandwidth estimates, coupled elements are shown to be close approximations of large ele… ▽ More Several applications of medical ultrasound can benefit from a larger field of view (FOV). This study is aimed at increasing the FOV of linear array probes by increasing the element width. Coupled elements were used to imitate a larger element width. Through Fourier analysis, theoretical pressure amplitudes, and bandwidth estimates, coupled elements are shown to be close approximations of large elements. The effects of coupling on resolution, contrast, and speckle signal-to-noise ratio are investigated through phantom images and in-vivo images of a rabbit tumor reconstructed with plane-wave compounding. Furthermore, a positioning system was used to acquire data from a virtual large aperture with 120 mm FOV and 128 elements, collected in sections with a single probe. The Null Subtraction Imaging (NSI), Sign Coherence Factor (SCF), and Minimum Variance (MV) beamformers are compared for regaining resolution lost by an increased F-number. The NSI beamformer decreased Full-Width at Half-Max (FWHM) estimates of wire targets by 79% with coupling by 2 compared to uncoupled DAS. The MV beamformer was best for maintaining speckle statistics while improving resolution. Our results demonstrate how increased element width can increase FOV with no increase to element count. △ Less

Submitted 16 April, 2026; v1 submitted 15 February, 2026; originally announced February 2026.

Loss Landscape Geometry and the Learning of Symmetries: Or, What Influence Functions Reveal About Robust Generalization

Authors: James Amarel, Robyn Miller, Nicolas Hengartner, Benjamin Migliori, Emily Casleton, Alexei Skurikhin, Earl Lawrence, Gerd J. Kunde

Abstract: We study how neural emulators of partial differential equation solution operators internalize physical symmetries by introducing an influence-based diagnostic that measures the propagation of parameter updates between symmetry-related states, defined as the metric-weighted overlap of loss gradients evaluated along group orbits. This quantity probes the local geometry of the learned loss landscape… ▽ More We study how neural emulators of partial differential equation solution operators internalize physical symmetries by introducing an influence-based diagnostic that measures the propagation of parameter updates between symmetry-related states, defined as the metric-weighted overlap of loss gradients evaluated along group orbits. This quantity probes the local geometry of the learned loss landscape and goes beyond forward-pass equivariance tests by directly assessing whether learning dynamics couple physically equivalent configurations. Applying our diagnostic to autoregressive fluid flow emulators, we show that orbit-wise gradient coherence provides the mechanism for learning to generalize over symmetry transformations and indicates when training selects a symmetry compatible basin. The result is a novel technique for evaluating if surrogate models have internalized symmetry properties of the known solution operator. △ Less

Submitted 27 January, 2026; originally announced January 2026.

Controlling Nonadiabatic Transitions Through Engineered Ultrafast Laser Fields at Conical Intersections

Authors: Xuanchao Zhang, Yang-Cheng Ye, Panpan Zhang, Xiangmei Duan, R. J. Dwayne Miller, Fulu Zheng, Ajay Jha, Hong-Guang Duan

Abstract: In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of… ▽ More In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of wave-packets as they traverse the degeneracy region with strong nonadiabatic coupling. By systematically varying pulse parameters, we demonstrate that both chirp and pulse duration modulate vibrational coherence and alter branching between competing pathways, leading to controlled changes in quantum yield. Our results elucidate the dynamical mechanisms underlying pulse-shaped control near conical intersections and establish a general framework for manipulating ultrafast nonadiabatic processes. △ Less

Submitted 31 December, 2025; v1 submitted 28 December, 2025; originally announced December 2025.

Demonstration of Sub-Percent Energy Resolution in the NEXT-100 Detector

Authors: NEXT Collaboration, M. Pérez Maneiro, M. Martínez-Vara, S. Torelli, G. Martínez-Lema, P. Novella, J. A. Hernando Morata, J. J. Gómez-Cadenas, C. Adams, H. Almazán, V. Álvarez, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, Y. Ayyad, C. D. R. Azevedo, K. Bailey, F. Ballester, J. E. Barcelon, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez, F. I. G. M. Borges , et al. (89 additional authors not shown)

Abstract: NEXT-100 is a high-pressure xenon time projection chamber with electroluminescent amplification, designed to operate with up to approximately 70.5 kg at 13.5 bar. It is the most recent detector developed by the NEXT collaboration to search for the neutrinoless double-beta decay ($ββ0ν$) of Xe-136. The NEXT gas TPC technology offers the best energy resolution near the Q-value of the decay (… ▽ More NEXT-100 is a high-pressure xenon time projection chamber with electroluminescent amplification, designed to operate with up to approximately 70.5 kg at 13.5 bar. It is the most recent detector developed by the NEXT collaboration to search for the neutrinoless double-beta decay ($ββ0ν$) of Xe-136. The NEXT gas TPC technology offers the best energy resolution near the Q-value of the decay ($Q_{ββ}$ = 2458 keV) among xenon detectors, which is set by design to be <1% FWHM. We report here the high-energy calibration of the detector using a Th-228 source, demonstrating linear response and an energy resolution of $(0.90 \pm 0.02)$% FWHM at the Tl-208 photopeak (2615 keV). This performance extrapolates to a resolution at the double-beta decay end-point of $R(Q_{ββ})$ = $(0.93 \pm 0.02)$% FWHM, confirming the detector's capability for precision energy measurement in the search for $ββ0ν$. △ Less

Submitted 12 January, 2026; v1 submitted 4 November, 2025; originally announced November 2025.

First results of the NEXT-100 detector using $^{83m}$Kr decays

Authors: NEXT Collaboration, G. Martínez-Lema, C. Hervés Carrete, S. Torelli, M. Cid Laso, P. Vázquez Cabaleiro, B. Palmeiro, J. A. Hernando Morata, J. J. Gómez-Cadenas, C. Adams, H. Almazán, V. Álvarez, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, Y. Ayyad, C. D. R. Azevedo, K. Bailey, F. Ballester, J. E. Barcelon, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez , et al. (91 additional authors not shown)

Abstract: The NEXT collaboration is investigating the double beta decay of $^{136}$Xe using high-pressure gas electroluminescent time projection chambers, which provide excellent energy resolution together with a robust topological signature. Operating at the Laboratorio Subterráneo de Canfranc (LSC) and building on the success of the NEXT-White detector, the NEXT-100 apparatus began commissioning in May 20… ▽ More The NEXT collaboration is investigating the double beta decay of $^{136}$Xe using high-pressure gas electroluminescent time projection chambers, which provide excellent energy resolution together with a robust topological signature. Operating at the Laboratorio Subterráneo de Canfranc (LSC) and building on the success of the NEXT-White detector, the NEXT-100 apparatus began commissioning in May 2024 and started operation with xenon at a pressure of 4 bar in October 2024. We report here the first results obtained with NEXT-100 using low-energy calibration data from $^{83m}$Kr decays, which allow mapping of the detector response in the active volume and monitoring of its stability over time. After homogenizing the light response, we achieve an energy resolution of 4.37% FWHM at 41.5 keV for $^{83m}$Kr point-like energy deposits contained in a radius of 425 mm. In a fiducial region representing the operating conditions of NEXT-100 at 10 bar we obtain an improved energy resolution of 4.16% FWHM. These results are in good agreement with that obtained in NEXT-White, and an $E^{-1/2}$ extrapolation to $Q_{ββ}$ yields an energy resolution close to 0.5% FWHM, well below the 1% FWHM design target. △ Less

Submitted 8 January, 2026; v1 submitted 3 November, 2025; originally announced November 2025.

Comments: 13 pages, 11 figures

Technical assessment of a novel vertical CT system for upright radiotherapy simulation and treatment planning

Authors: Jordan M. Slagowski, Yuhao Yan, Jessica R. Miller, John W. Hayes, Carson A. Hoffman, Minglei Kang, Carri K. Glide-Hurst

Abstract: Purpose: To characterize image quality, imaging dose, and dose calculation accuracy for an upright CT scanner with a six-degree-of-freedom patient positioning system. Methods: Imaging dose (CTDIvol) was measured at 120 kVp and 200 mAs. Image quality was evaluated using an ACR-464 phantom. Mean CT number accuracy was assessed within inserts of known material and uniformity as the difference in valu… ▽ More Purpose: To characterize image quality, imaging dose, and dose calculation accuracy for an upright CT scanner with a six-degree-of-freedom patient positioning system. Methods: Imaging dose (CTDIvol) was measured at 120 kVp and 200 mAs. Image quality was evaluated using an ACR-464 phantom. Mean CT number accuracy was assessed within inserts of known material and uniformity as the difference in values at the center and periphery of uniform phantoms. High-contrast resolution was assessed by visible line pairs and modulation transfer function (MTF). Low-contrast performance was quantified by contrast-to-noise-ratio (CNR). Spatial integrity was evaluated between fiducials 100 mm apart. Hounsfield unit to mass density and stopping-power-ratio calibrations were performed. Proton and photon treatment plans were optimized on upright CT scans of a thorax phantom in heterogenous and homogeneous regions. Dose was forward computed on a registered recumbent CT scan and agreement evaluated using 3D gamma analysis. Results: CT imaging dose (CTDIvol) was 23.5 mGy for the 16 cm head phantom and 10.1 mGy for the 32 cm body phantom. Mean CT numbers (HU) were within the expected range for water (1.7) and acrylic (120.8). CT numbers were slightly (5-27 HU) out-of-range for air (-950.4), polyethylene (-78.8), and bone (823.0). Image uniformity was 20.2 HU and 35.0 HU for 20 cm and 48 cm diameter phantoms, respectively. Eight high-contrast line pairs were visualized. The MTF equaled 4.4 cm-1 at 50% and 7.1 cm-1 at 10%. The median CNR was 0.93, below the 1.0 tolerance. Spatial integrity was 0.36 mm. Gamma pass rates were 99.8% for photon and 90.6% for proton plans with 1%/1mm criteria, and greater than or equal to 98.0% for all plans with 3%/2mm criteria. Conclusion: Upright CT image quality and dose calculation accuracy are acceptable for photon and proton radiotherapy. △ Less

Submitted 24 October, 2025; originally announced October 2025.

Local Order Average-Atom Interatomic Potentials

Authors: Chloe A. Zeller, Ronald E. Miller, Ellad B. Tadmor

Abstract: This article describes an extension to the effective Average-Atom (AA) method for random alloys to account for local ordering (short-range order) effects by utilizing information from partial radial distribution functions. The new Local Order Average-Atom (LOAA) method is rigorously derived based on statistical mechanics arguments and validated for non-stoichiometric binary 2D hexagonal crystals a… ▽ More This article describes an extension to the effective Average-Atom (AA) method for random alloys to account for local ordering (short-range order) effects by utilizing information from partial radial distribution functions. The new Local Order Average-Atom (LOAA) method is rigorously derived based on statistical mechanics arguments and validated for non-stoichiometric binary 2D hexagonal crystals and 3D FeNiCr and NiAl alloys whose ground state is obtained through Monte Carlo sampling. Material properties for these alloys computed from atomistic simulations using standard interatomic potentials (IPs) exhibit a strong dependence on local ordering that is captured by simulations with effective LOAA IPs, but not the original AA method. The advantage of LOAA is that it requires smaller system sizes to achieve statistically converged results and therefore enables the simulation of complex materials, such as high-entropy alloys, at a fraction of the computational cost of standard IPs. △ Less

Submitted 6 July, 2026; v1 submitted 7 October, 2025; originally announced October 2025.

Excitonic Energy Transfer in Red Algal Photosystem I Reveals an Evolutionary Bridge between Cyanobacteria and Plants

Authors: Mengyuan Cui, Zihui Liu, Miriam Izzo, Junhua Zhou, Enhu He, Vandana Tiwari, Petar H. Lambrev, R. J. Dwayne Miller, Joanna Kargu, Fulu Zheng, Ajay Jha, Hong-GuangDuan

Abstract: Photosystem I converts light into chemical energy with near-unity quantum efficiency,yet its energy-transfer and charge-separation mechanisms remain debated. Evolution has diversified PSI architectures. The unicellular red algae Cyanidioschyzon merolae represents a key evolutionary intermediate,featuring a cyanobacterial-like monomeric core surrounded by three to five LHCR subunits. This hybrid or… ▽ More Photosystem I converts light into chemical energy with near-unity quantum efficiency,yet its energy-transfer and charge-separation mechanisms remain debated. Evolution has diversified PSI architectures. The unicellular red algae Cyanidioschyzon merolae represents a key evolutionary intermediate,featuring a cyanobacterial-like monomeric core surrounded by three to five LHCR subunits. This hybrid organization provides a unique system to bridge mechanistic models across lineages. We applied two-dimensional electronic spectroscopy at ultralow temperatures to disentangle overlapping excitation pathways in C. merolae PSI. Cryogenic measurements suppressed thermal broadening, resolving five dynamical components: sub-picosecond equilibration acrossthe core-LHCR interface, subsequent population transfer into progressively lowerenergy manifolds, and slower feeding into red pools distributed across both core and antenna. On the longest timescales, a persistent ground-state bleach signifies excitons stabilised in terminal sinks. Notably, comparison of 8 K and 80 K spectra reveals that excitations are heterogeneously partitioned among multiple sinks at low disorder, whereas modest thermal activation promotes selective convergence into core-associated red chlorophylls. To interpret these dynamics, we employed atomistic excitonic Hamiltonians with time-nonlocal master equations, providing a quantitative framework for exciton migration and thermal redistribution. Together, these results demonstrate that C. merolae PSI broadens the kinetic funnel by distributing sinks across core and antenna, an evolutionary adaptation that extends spectral coverage whilst ensuring efficient trapping. These insights reconcile cyanobacterial and plant paradigms and illuminate how antenna expansion reshaped PSI function during the course of photosynthetic evolution. △ Less

Submitted 29 September, 2025; originally announced September 2025.

Generalization vs. Memorization in Autoregressive Deep Learning: Or, Examining Temporal Decay of Gradient Coherence

Authors: James Amarel, Nicolas Hengartner, Robyn Miller, Kamaljeet Singh, Siddharth Mansingh, Arvind Mohan, Benjamin Migliori, Emily Casleton, Alexei Skurikhin, Earl Lawrence, Gerd J. Kunde

Abstract: Foundation models trained as autoregressive PDE surrogates hold significant promise for accelerating scientific discovery through their capacity to both extrapolate beyond training regimes and efficiently adapt to downstream tasks despite a paucity of examples for fine-tuning. However, reliably achieving genuine generalization - a necessary capability for producing novel scientific insights and ro… ▽ More Foundation models trained as autoregressive PDE surrogates hold significant promise for accelerating scientific discovery through their capacity to both extrapolate beyond training regimes and efficiently adapt to downstream tasks despite a paucity of examples for fine-tuning. However, reliably achieving genuine generalization - a necessary capability for producing novel scientific insights and robustly performing during deployment - remains a critical challenge. Establishing whether or not these requirements are met demands evaluation metrics capable of clearly distinguishing genuine model generalization from mere memorization. We apply the influence function formalism to systematically characterize how autoregressive PDE surrogates assimilate and propagate information derived from diverse physical scenarios, revealing fundamental limitations of standard models and training routines in addition to providing actionable insights regarding the design of improved surrogates. △ Less

Submitted 17 January, 2026; v1 submitted 18 August, 2025; originally announced September 2025.

The NEXT-100 Detector

Authors: NEXT Collaboration, C. Adams, H. Almazán, V. Álvarez, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, Y. Ayyad, C. D. R. Azevedo, K. Bailey, F. Ballester, J. E. Barcelon, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez, F. I. G. M. Borges, A. Brodoline, N. Byrnes, A. Castillo, E. Church, L. Cid, M. Cid, X. Cid , et al. (92 additional authors not shown)

Abstract: The NEXT collaboration is dedicated to the study of double beta decays of $^{136}$Xe using a high-pressure gas electroluminescent time projection chamber. This advanced technology combines exceptional energy resolution ($\leq 1\%$ FWHM at the $Q_{ββ}$ value of the neutrinoless double beta decay) and powerful topological event discrimination. Building on the achievements of the NEXT-White detector,… ▽ More The NEXT collaboration is dedicated to the study of double beta decays of $^{136}$Xe using a high-pressure gas electroluminescent time projection chamber. This advanced technology combines exceptional energy resolution ($\leq 1\%$ FWHM at the $Q_{ββ}$ value of the neutrinoless double beta decay) and powerful topological event discrimination. Building on the achievements of the NEXT-White detector, the NEXT-100 detector started taking data at the Laboratorio Subterráneo de Canfranc (LSC) in May of 2024. Designed to operate with xenon gas at 13.5 bar, NEXT-100 consists of a time projection chamber where the energy and the spatial pattern of the ionising particles in the detector are precisely retrieved using two sensor planes (one with photo-multiplier tubes and the other with silicon photo-multipliers). The detector has been operating at stable conditions using argon and xenon gases at $\sim$4 bar and drift fields of 74 V/cm and 118 V/cm, respectively. Alpha decays from the $^{222}$Rn chain have been used to test and monitor the stability of the detector, showing a constant electron lifetime in the drift volume. In this paper, in addition to reporting the results of the commissioning run, we provide a detailed description of the NEXT-100 detector, describe its assembly, and present the current estimation of the radiopurity budget. △ Less

Submitted 10 December, 2025; v1 submitted 23 May, 2025; originally announced May 2025.

Measuring $\mathbb{Z}_2$ invariants in dimer models and cross-coupled ladders with a programmable photonic molecule

Authors: Sashank Kaushik Sridhar, Rohith Srikanth, Alexander R. Miller, Ferguson J. McComb, Avik Dutt

Abstract: Topological models are characterized by a quantized topological invariant and provide a description of novel phases of matter that can exhibit localized edge states, corner modes, and chiral transport. We experimentally realize two 1-D lattices supporting symmetry-protected topology - the Su-Schrieffer-Heeger (SSH) and extended SSH models using the synthetic frequency dimension of coupled fiber ri… ▽ More Topological models are characterized by a quantized topological invariant and provide a description of novel phases of matter that can exhibit localized edge states, corner modes, and chiral transport. We experimentally realize two 1-D lattices supporting symmetry-protected topology - the Su-Schrieffer-Heeger (SSH) and extended SSH models using the synthetic frequency dimension of coupled fiber ring resonators. We introduce and experimentally demonstrate cascaded heterodyning as a technique for low-noise, single-shot winding number measurements through the mean chiral displacement and band structure measurements. Through our robust setup and detection techniques we can extend our capability to realizing 1-D ladder models, demonstrating a modified Creutz ladder with a staggered flux with each plaquette. This highly reconfigurable and compact fiber optics platform for Hamiltonian simulation, along with a low-noise detection scheme, provides a path forward for chip-scale realizations. △ Less

Submitted 7 May, 2025; originally announced May 2025.

Comments: 7 pages, 4 figures

High Voltage Delivery and Distribution for the NEXT-100 Time Projection Chamber

Authors: NEXT Collaboration, C. Adams, H. Almazán, V. Álvarez, K. Bailey, R. Guenette, B. J. P. Jones, S. Johnston, K. Mistry, F. Monrabal, D. R. Nygren, B. Palmeiro, L. Rogers, J. Waldschmidt, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, F. Ballester, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez , et al. (86 additional authors not shown)

Abstract: A critical element in the realization of large liquid and gas time projection chambers (TPCs) is the delivery and distribution of high voltages into and around the detector. Such experiments require of order tens of kilovolts to enable electron drift over meter-scale distances. This paper describes the design and operation of the cathode feedthrough and high voltage distribution through the field… ▽ More A critical element in the realization of large liquid and gas time projection chambers (TPCs) is the delivery and distribution of high voltages into and around the detector. Such experiments require of order tens of kilovolts to enable electron drift over meter-scale distances. This paper describes the design and operation of the cathode feedthrough and high voltage distribution through the field cage of the NEXT-100 experiment, an underground TPC that will search for neutrinoless double beta decay $0νββ$. The feedthrough has been demonstrated to hold pressures up to 20~bar and sustain voltages as high as -65~kV, and the TPC is operating stably at its design high voltages. The system has been realized within the constraints of a stringent radiopurity budget and is now being used to execute a suite of sensitive double beta decay analyses. △ Less

Submitted 18 September, 2025; v1 submitted 2 May, 2025; originally announced May 2025.

Journal ref: JINST 21 P07001 (2026)

Tumor monitoring and detection of lymph node metastasis using quantitative ultrasound and immune cytokine profiling in dogs undergoing radiation therapy: a pilot study

Authors: Mick Gardner, Audrey Billhymer, Rebecca Kamerer, Joanna Schmit, Trevor Park, Julie Nguyen-Edquilang, Rita Miller, Kim A Selting, Michael Oelze

Abstract: Quantitative ultrasound (QUS) characterizes the composition of cells to distinguish diseased from healthy tissue. QUS can reflect the complexity of the tumor and detect early lymph node (LN) metastasis ex vivo. The objective in this study was to gather preliminary QUS and cytokine data from dogs undergoing radiation therapy and correlate QUS data with both LN metastasis and tumor response. Spontan… ▽ More Quantitative ultrasound (QUS) characterizes the composition of cells to distinguish diseased from healthy tissue. QUS can reflect the complexity of the tumor and detect early lymph node (LN) metastasis ex vivo. The objective in this study was to gather preliminary QUS and cytokine data from dogs undergoing radiation therapy and correlate QUS data with both LN metastasis and tumor response. Spontaneous solid tumors were evaluated with QUS before and up to one year after receiving RT. Additionally, regional LNs were evaluated with QUS in vivo, then excised and examined with histopathology to detect metastasis. Paired t-tests were used to compare QUS data of metastatic and non-metastatic LNs within patients. Furthermore, paired t-tests compared pre- versus post-RT QUS data. Serum was collected at each time point for cytokine profiles. Most statistical tests were underpowered to produce significant $p$ values, but interesting trends were observed. The lowest $p$ values for LN tests were found with the envelope statistics $K$ ($p = 0.142$) and $μ$ ($p = 0.181$), which correspond to cell structure and number of scatterers. For tumor response, the lowest $p$ values were found with $K$ ($p = 0.115$) and $μ$ ($p = 0.127$) when comparing baseline QUS data with QUS data 1 week after RT. Monocyte chemoattractant protein 1 (MCP-1) was significantly higher in dogs with cancer when compared to healthy controls ($p = 1.12$e-4). A weak correlation was found between effective scatterer diameter (ESD) and Transforming growth factor beta 1 (TGF$β$-1). While statistical tests on the preliminary QUS data alone were underpowered to detect significant differences among groups, our methods create a basis for future studies. △ Less

Submitted 24 March, 2025; originally announced March 2025.

Comments: 8 pages, 5 figures

Performance of an Optical TPC Geant4 Simulation with Opticks GPU-Accelerated Photon Propagation

Authors: NEXT Collaboration, I. Parmaksiz, K. Mistry, E. Church, C. Adams, J. Asaadi, J. Baeza-Rubio, K. Bailey, N. Byrnes, B. J. P. Jones, I. A. Moya, K. E. Navarro, D. R. Nygren, P. Oyedele, L. Rogers, F. Samaniego, K. Stogsdill, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet , et al. (91 additional authors not shown)

Abstract: We investigate the performance of Opticks, a NVIDIA OptiX API 7.5 GPU-accelerated photon propagation tool compared with a single-threaded Geant4 simulation. We compare the simulations using an improved model of the NEXT-CRAB-0 gaseous time projection chamber. Performance results suggest that Opticks improves simulation speeds by between 58.47+/-0.02 and 181.39+/-0.28 times relative to a CPU-only G… ▽ More We investigate the performance of Opticks, a NVIDIA OptiX API 7.5 GPU-accelerated photon propagation tool compared with a single-threaded Geant4 simulation. We compare the simulations using an improved model of the NEXT-CRAB-0 gaseous time projection chamber. Performance results suggest that Opticks improves simulation speeds by between 58.47+/-0.02 and 181.39+/-0.28 times relative to a CPU-only Geant4 simulation and these results vary between different types of GPU and CPU. A detailed comparison shows that the number of detected photons, along with their times and wavelengths, are in good agreement between Opticks and Geant4. △ Less

Submitted 9 July, 2025; v1 submitted 18 February, 2025; originally announced February 2025.

Comments: 12 pages, 8 Figures

Journal ref: NEXT Collaboration. Performance of an optical TPC Geant4 simulation with opticks GPU-accelerated photon propagation. Eur. Phys. J. C 85, 910 (2025)

Reconstructing neutrinoless double beta decay event kinematics in a xenon gas detector with vertex tagging

Authors: NEXT Collaboration, M. Martínez-Vara, K. Mistry, F. Pompa, B. J. P. Jones, J. Martín-Albo, M. Sorel, C. Adams, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, K. Bailey, F. Ballester, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez, F. I. G. M. Borges, A. Brodolin, N. Byrnes , et al. (86 additional authors not shown)

Abstract: If neutrinoless double beta decay is discovered, the next natural step would be understanding the lepton number violating physics responsible for it. Several alternatives exist beyond the exchange of light neutrinos. Some of these mechanisms can be distinguished by measuring phase-space observables, namely the opening angle $\cosθ$ among the two decay electrons, and the electron energy spectra,… ▽ More If neutrinoless double beta decay is discovered, the next natural step would be understanding the lepton number violating physics responsible for it. Several alternatives exist beyond the exchange of light neutrinos. Some of these mechanisms can be distinguished by measuring phase-space observables, namely the opening angle $\cosθ$ among the two decay electrons, and the electron energy spectra, $T_1$ and $T_2$. In this work, we study the statistical accuracy and precision in measuring these kinematic observables in a future xenon gas detector with the added capability to precisely locate the decay vertex. For realistic detector conditions (a gas pressure of 10 bar and spatial resolution of 4 mm), we find that the average $\overline{\cosθ}$ and $\overline{T_1}$ values can be reconstructed with a precision of 0.19 and 110 keV, respectively, assuming that only 10 neutrinoless double beta decay events are detected. △ Less

Submitted 12 June, 2025; v1 submitted 14 February, 2025; originally announced February 2025.

Numerically Stable Resonating Hartree-Fock

Authors: Ericka Roy Miller, Shane M. Parker

Abstract: The simulation of excited states at low computational cost remains an open challenge for electronic structure (ES) methods. While much attention has been given to orthogonal ES methods, relatively little work has been done to develop nonorthogonal ES methods for excited states, particularly those involving nonorthogonal orbital optimization. We present here a numerically stable formulation of the… ▽ More The simulation of excited states at low computational cost remains an open challenge for electronic structure (ES) methods. While much attention has been given to orthogonal ES methods, relatively little work has been done to develop nonorthogonal ES methods for excited states, particularly those involving nonorthogonal orbital optimization. We present here a numerically stable formulation of the Resonating Hartree-Fock (ResHF) method that uses the matrix adjugate to remove numerical instabilities in ResHF arising from nearly orthogonal orbitals, and we demonstrate improvements to ResHF wavefunction optimization as a result. We then benchmark the performance of ResHF against Complete Active Space Self-Consistent Field in the avoided crossing of LiF, the torsional rotation of ethene, and the singlet-triplet energy gaps of a selection of small molecules. ResHF is a promising excited state method because it incorporates the orbital relaxation of state-specific methods, while retaining the correct state crossings of state-averaged approaches. Our open-source ResHF implementation, yucca, is available on GitLab. △ Less

Submitted 12 March, 2025; v1 submitted 1 November, 2024; originally announced November 2024.

Comments: 12 pages, 4 figures

Journal ref: Journal of Chemical Physics, 162, 104115 (2025)

Fluorescence Imaging of Individual Ions and Molecules in Pressurized Noble Gases for Barium Tagging in $^{136}$Xe

Authors: NEXT Collaboration, N. Byrnes, E. Dey, F. W. Foss, B. J. P. Jones, R. Madigan, A. McDonald, R. L. Miller, K. E. Navarro, L. R. Norman, D. R. Nygren, C. Adams, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, J. E. Barcelon, K. Bailey, F. Ballester, M. del Barrio-Torregrosa , et al. (90 additional authors not shown)

Abstract: The imaging of individual Ba$^{2+}$ ions in high pressure xenon gas is one possible way to attain background-free sensitivity to neutrinoless double beta decay and hence establish the Majorana nature of the neutrino. In this paper we demonstrate selective single Ba$^{2+}$ ion imaging inside a high-pressure xenon gas environment. Ba$^{2+}$ ions chelated with molecular chemosensors are resolved at t… ▽ More The imaging of individual Ba$^{2+}$ ions in high pressure xenon gas is one possible way to attain background-free sensitivity to neutrinoless double beta decay and hence establish the Majorana nature of the neutrino. In this paper we demonstrate selective single Ba$^{2+}$ ion imaging inside a high-pressure xenon gas environment. Ba$^{2+}$ ions chelated with molecular chemosensors are resolved at the gas-solid interface using a diffraction-limited imaging system with scan area of 1$\times$1~cm$^2$ located inside 10~bar of xenon gas. This new form of microscopy represents an important enabling step in the development of barium tagging for neutrinoless double beta decay searches in $^{136}$Xe, as well as a new tool for studying the photophysics of fluorescent molecules and chemosensors at the solid-gas interface. △ Less

Submitted 20 May, 2024; originally announced June 2024.

Measurement of Energy Resolution with the NEXT-White Silicon Photomultipliers

Authors: T. Contreras, B. Palmeiro, H. Almazán, A. Para, G. Martínez-Lema, R. Guenette, C. Adams, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, K. Bailey, F. Ballester, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez, F. I. G. M. Borges, A. Brodolin, N. Byrnes, S. Cárcel, A. Castillo , et al. (85 additional authors not shown)

Abstract: The NEXT-White detector, a high-pressure gaseous xenon time projection chamber, demonstrated the excellence of this technology for future neutrinoless double beta decay searches using photomultiplier tubes (PMTs) to measure energy and silicon photomultipliers (SiPMs) to extract topology information. This analysis uses $^{83m}\text{Kr}$ data from the NEXT-White detector to measure and understand th… ▽ More The NEXT-White detector, a high-pressure gaseous xenon time projection chamber, demonstrated the excellence of this technology for future neutrinoless double beta decay searches using photomultiplier tubes (PMTs) to measure energy and silicon photomultipliers (SiPMs) to extract topology information. This analysis uses $^{83m}\text{Kr}$ data from the NEXT-White detector to measure and understand the energy resolution that can be obtained with the SiPMs, rather than with PMTs. The energy resolution obtained of (10.9 $\pm$ 0.6) $\%$, full-width half-maximum, is slightly larger than predicted based on the photon statistics resulting from very low light detection coverage of the SiPM plane in the NEXT-White detector. The difference in the predicted and measured resolution is attributed to poor corrections, which are expected to be improved with larger statistics. Furthermore, the noise of the SiPMs is shown to not be a dominant factor in the energy resolution and may be negligible when noise subtraction is applied appropriately, for high-energy events or larger SiPM coverage detectors. These results, which are extrapolated to estimate the response of large coverage SiPM planes, are promising for the development of future, SiPM-only, readout planes that can offer imaging and achieve similar energy resolution to that previously demonstrated with PMTs. △ Less

Submitted 16 August, 2024; v1 submitted 30 May, 2024; originally announced May 2024.

Quantum tomography of molecules using ultrafast electron diffraction

Authors: Jiayang Jiang, Ming Zhang, Aosheng Gu, R. J. Dwayne Miller, Zheng Li

Abstract: We propose a quantum tomography (QT) approach to retrieve the temporally evolving reduced density matrix in elecotronic state basis, where the populations and coherence between ground state and excited state are reconstructed from the ultrafast electron diffraction signal. In order to showcase the capability of the proposed QT approach, we simulate the nuclear wavepacket dynamics and ultrafast ele… ▽ More We propose a quantum tomography (QT) approach to retrieve the temporally evolving reduced density matrix in elecotronic state basis, where the populations and coherence between ground state and excited state are reconstructed from the ultrafast electron diffraction signal. In order to showcase the capability of the proposed QT approach, we simulate the nuclear wavepacket dynamics and ultrafast electron diffraction of photoexcited pyrrole molecules using ab initio quantum chemical CASSCF method. From simulated time-resolved diffraction data, we retrieve the evolving density matrix in a crude diabatic representation basis and reveal the symmetry of the excited pyrrole wavepacket. Our QT approach opens the route to make quantum version of "molecular movie" that covers the electronic degree of freedom, and equips ultrafast electron diffraction with the power to reveal the coherence between electronic states, relaxation and dynamics of population transfer. △ Less

Submitted 8 March, 2024; originally announced March 2024.

Comments: 8 pages, 6 figures

Journal ref: J. Chem. Phys. 160, 104101 (2024)

Ultrafast Photochemistry and Electron Diffraction for Cyclobutanone in the S2 State: Surface Hopping with Time-Dependent Density Functional Theory

Authors: Ericka Roy Miller, Sean J. Hoehn, Abhijith Kumar, Dehua Jiang, Shane M. Parker

Abstract: We simulate the photodynamics of gas-phase cyclobutanone excited to the S$_2$ state using fewest switches surface hopping (FSSH) dynamics powered by time-dependent density functional theory (TDDFT). We predict a total C3+C2 photoproduct yield of 9%, with a C3:C2 product ratio of 1:8. Two primary S$_2$$\rightarrow$S$_1$ conical intersections are identified: $β$ stretch and CCH bend, with the higher… ▽ More We simulate the photodynamics of gas-phase cyclobutanone excited to the S$_2$ state using fewest switches surface hopping (FSSH) dynamics powered by time-dependent density functional theory (TDDFT). We predict a total C3+C2 photoproduct yield of 9%, with a C3:C2 product ratio of 1:8. Two primary S$_2$$\rightarrow$S$_1$ conical intersections are identified: $β$ stretch and CCH bend, with the higher energy $β$ stretch being associated with sub-picosecond S$_2$ decay. Excited state lifetimes computed with respect to electronic state populations were found to be 7.0 ps (S$_2$$\rightarrow$S$_1$) and 550 fs (S$_1$$\rightarrow$S$_0$). We also generate time-resolved difference pair distribution functions ($Δ$PDFs) from our TDDFT-FSSH dynamics results in order to generate direct comparisons to ultrafast electron diffraction experiment observables. Global and target analysis of time-resolved $Δ$PDFs produced a distinct set of lifetimes: i) a 0.462 ps decay, and ii) a 16.8 ps decay that both resemble the S$_2$ minimum, as well as iii) a long ($>$ nanosecond) decay that resembles the S$_1$ minimum geometry and the fully separated C3/C2 products. Finally, we contextualize our results by considering the impact of the most likely sources of significant errors. △ Less

Submitted 15 February, 2024; originally announced February 2024.

Comments: 10 pages, 9 figures, preprint before peer review

Journal ref: J. Chem. Phys. 161, 034105 (2024)

Design, characterization and installation of the NEXT-100 cathode and electroluminescence regions

Authors: NEXT Collaboration, K. Mistry, L. Rogers, B. J. P. Jones, B. Munson, L. Norman, C. Adams, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, K. Bailey, F. Ballester, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez, F. I. G. M. Borges, A. Brodolin, N. Byrnes, S. Cárcel , et al. (85 additional authors not shown)

Abstract: NEXT-100 is currently being constructed at the Laboratorio Subterráneo de Canfranc in the Spanish Pyrenees and will search for neutrinoless double beta decay using a high-pressure gaseous time projection chamber (TPC) with 100 kg of xenon. Charge amplification is carried out via electroluminescence (EL) which is the process of accelerating electrons in a high electric field region causing secondar… ▽ More NEXT-100 is currently being constructed at the Laboratorio Subterráneo de Canfranc in the Spanish Pyrenees and will search for neutrinoless double beta decay using a high-pressure gaseous time projection chamber (TPC) with 100 kg of xenon. Charge amplification is carried out via electroluminescence (EL) which is the process of accelerating electrons in a high electric field region causing secondary scintillation of the medium proportional to the initial charge. The NEXT-100 EL and cathode regions are made from tensioned hexagonal meshes of 1 m diameter. This paper describes the design, characterization, and installation of these parts for NEXT-100. Simulations of the electric field are performed to model the drift and amplification of ionization electrons produced in the detector under various EL region alignments and rotations. Measurements of the electrostatic breakdown voltage in air characterize performance under high voltage conditions and identify breakdown points. The electrostatic deflection of the mesh is quantified and fit to a first-principles mechanical model. Measurements were performed with both a standalone test EL region and with the NEXT-100 EL region before its installation in the detector. Finally, we describe the parts as installed in NEXT-100, following their deployment in Summer 2023. △ Less

Submitted 21 December, 2023; v1 submitted 6 November, 2023; originally announced November 2023.

Comments: 35 pages, 25 Figures, update includes accepted version in JINST

Journal ref: JINST 19 P02007 2024

Demonstration of Event Position Reconstruction based on Diffusion in the NEXT-White Detector

Authors: J. Haefner, K. E. Navarro, R. Guenette, B. J. P. Jones, A. Tripathi, C. Adams, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, K. Bailey, F. Ballester, M. del Barrio-Torregrosa, A. Bayo, J. M. BenllochRodríguez, F. I. G. M. Borges, A. Brodolin, N. Byrnes, S. Cárcel, J. V. Carrión , et al. (86 additional authors not shown)

Abstract: Noble element time projection chambers are a leading technology for rare event detection in physics, such as for dark matter and neutrinoless double beta decay searches. Time projection chambers typically assign event position in the drift direction using the relative timing of prompt scintillation and delayed charge collection signals, allowing for reconstruction of an absolute position in the dr… ▽ More Noble element time projection chambers are a leading technology for rare event detection in physics, such as for dark matter and neutrinoless double beta decay searches. Time projection chambers typically assign event position in the drift direction using the relative timing of prompt scintillation and delayed charge collection signals, allowing for reconstruction of an absolute position in the drift direction. In this paper, alternate methods for assigning event drift distance via quantification of electron diffusion in a pure high pressure xenon gas time projection chamber are explored. Data from the NEXT-White detector demonstrate the ability to achieve good position assignment accuracy for both high- and low-energy events. Using point-like energy deposits from $^{83\mathrm{m}}$Kr calibration electron captures ($E\sim45$keV), the position of origin of low-energy events is determined to $2~$cm precision with bias $< 1$mm. A convolutional neural network approach is then used to quantify diffusion for longer tracks (E$\geq$1.5MeV), yielding a precision of 3cm on the event barycenter. The precision achieved with these methods indicates the feasibility energy calibrations of better than 1% FWHM at Q$_{ββ}$ in pure xenon, as well as the potential for event fiducialization in large future detectors using an alternate method that does not rely on primary scintillation. △ Less

Submitted 6 November, 2023; originally announced November 2023.

Comments: 18 pages, 16 figures

Synthesis technique and electron beam damage study of nanometer-thin single-crystalline Thymine

Authors: Hazem Daoud, Sreelaja Pulleri Vadhyar, Ehsan Nikbin, Cheng Lu, R. J. Dwayne Miller

Abstract: Samples suitable for electron diffraction studies must satisfy certain characteristics such as having a thickness in the range of 10 - 100 nm. We report, to our knowledge, the first successful synthesis technique of nanometer-thin sheets of single-crystalline thymine suitable for electron diffraction and spectroscopy studies. This development provides a well defined system to explore issues relate… ▽ More Samples suitable for electron diffraction studies must satisfy certain characteristics such as having a thickness in the range of 10 - 100 nm. We report, to our knowledge, the first successful synthesis technique of nanometer-thin sheets of single-crystalline thymine suitable for electron diffraction and spectroscopy studies. This development provides a well defined system to explore issues related to UV photochemistry of DNA and high intrinsic stability essential to maintaining integrity of genetic information. The crystals are grown using the evaporation technique and the nanometer-thin sheets are obtained via microtoming. The sample is characterized via x-ray diffraction (XRD) and is subsequently studied using electron diffraction via a transmission electron microscope (TEM). Thymine is found to be more radiation resistant than similar molecular moieties (e.g., carbamazepine) by a factor of 5. This raises interesting questions about the role of the fast relaxation processes of electron scattering-induced excited states, extending the concept of radiation hardening beyond photoexcited states. The high stability of thymine in particular opens the door for further studies of these ultrafast relaxation processes giving rise to the high stability of DNA to UV radiation. △ Less

Submitted 12 January, 2024; v1 submitted 2 October, 2023; originally announced October 2023.

Unraveling Quantum Coherences Mediating Primary Charge Transfer Processes in Photosystem II Reaction Center

Authors: Ajay Jha, Pan-Pan Zhang, Vandana Tiwari, Lipeng Chen, Michael Thorwart, R. J. Dwayne Miller, Hong-Guang Duan

Abstract: Photosystem II (PSII) reaction center is a unique protein-chromophore complex that is capable of efficiently separating electronic charges across the membrane after photoexcitation. In the PSII reaction center, the primary energy- and charge-transfer (CT) processes occur on comparable ultrafast timescales, which makes it extremely challenging to understand the fundamental mechanism responsible for… ▽ More Photosystem II (PSII) reaction center is a unique protein-chromophore complex that is capable of efficiently separating electronic charges across the membrane after photoexcitation. In the PSII reaction center, the primary energy- and charge-transfer (CT) processes occur on comparable ultrafast timescales, which makes it extremely challenging to understand the fundamental mechanism responsible for the near-unity quantum efficiency of the transfer. Here, we elucidate the role of quantum coherences in the ultrafast energy and CT in the PSII reaction center by performing two-dimensional (2D) electronic spectroscopy at the cryogenic temperature of 20 K, which captures the distinct underlying quantum coherences. Specifically, we uncover the electronic and vibrational coherences along with their lifetimes during the primary ultrafast processes of energy and CT. We also examine the functional role of the observed quantum coherences. To gather further insight, we construct a structure-based excitonic model that provided evidence for coherent energy and CT at low temperature in the 2D electronic spectra. The principles, uncovered by this combination of experimental and theoretical analyses, could provide valuable guidelines for creating artificial photosystems with exploitation of system-bath coupling and control of coherences to optimize the photon conversion efficiency to specific functions. △ Less

Submitted 24 July, 2023; originally announced July 2023.

Demonstration of neutrinoless double beta decay searches in gaseous xenon with NEXT

Authors: NEXT Collaboration, P. Novella, M. Sorel, A. Usón, C. Adams, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, K. Bailey, F. Ballester, M. del Barrio-Torregrosa, A. Bayo, J. M. Benlloch-Rodríguez, F. I. G. M. Borges, S. Bounasser, N. Byrnes, S. Cárcel, J. V. Carrión, S. Cebrián , et al. (90 additional authors not shown)

Abstract: The NEXT experiment aims at the sensitive search of the neutrinoless double beta decay in $^{136}$Xe, using high-pressure gas electroluminescent time projection chambers. The NEXT-White detector is the first radiopure demonstrator of this technology, operated in the Laboratorio Subterráneo de Canfranc. Achieving an energy resolution of 1% FWHM at 2.6 MeV and further background rejection by means o… ▽ More The NEXT experiment aims at the sensitive search of the neutrinoless double beta decay in $^{136}$Xe, using high-pressure gas electroluminescent time projection chambers. The NEXT-White detector is the first radiopure demonstrator of this technology, operated in the Laboratorio Subterráneo de Canfranc. Achieving an energy resolution of 1% FWHM at 2.6 MeV and further background rejection by means of the topology of the reconstructed tracks, NEXT-White has been exploited beyond its original goals in order to perform a neutrinoless double beta decay search. The analysis considers the combination of 271.6 days of $^{136}$Xe-enriched data and 208.9 days of $^{136}$Xe-depleted data. A detailed background modeling and measurement has been developed, ensuring the time stability of the radiogenic and cosmogenic contributions across both data samples. Limits to the neutrinoless mode are obtained in two alternative analyses: a background-model-dependent approach and a novel direct background-subtraction technique, offering results with small dependence on the background model assumptions. With a fiducial mass of only 3.50$\pm$0.01 kg of $^{136}$Xe-enriched xenon, 90% C.L. lower limits to the neutrinoless double beta decay are found in the T$_{1/2}^{0ν}>5.5\times10^{23}-1.3\times10^{24}$ yr range, depending on the method. The presented techniques stand as a proof-of-concept for the searches to be implemented with larger NEXT detectors. △ Less

Submitted 22 September, 2023; v1 submitted 16 May, 2023; originally announced May 2023.

Journal ref: JHEP 09 (2023) 190

NEXT-CRAB-0: A High Pressure Gaseous Xenon Time Projection Chamber with a Direct VUV Camera Based Readout

Authors: NEXT Collaboration, N. K. Byrnes, I. Parmaksiz, C. Adams, J. Asaadi, J Baeza-Rubio, K. Bailey, E. Church, D. González-Díaz, A. Higley, B. J. P. Jones, K. Mistry, I. A. Moya, D. R. Nygren, P. Oyedele, L. Rogers, K. Stogsdill, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, S. Ayet, C. D. R. Azevedo , et al. (94 additional authors not shown)

Abstract: The search for neutrinoless double beta decay ($0νββ$) remains one of the most compelling experimental avenues for the discovery in the neutrino sector. Electroluminescent gas-phase time projection chambers are well suited to $0νββ$ searches due to their intrinsically precise energy resolution and topological event identification capabilities. Scalability to ton- and multi-ton masses requires read… ▽ More The search for neutrinoless double beta decay ($0νββ$) remains one of the most compelling experimental avenues for the discovery in the neutrino sector. Electroluminescent gas-phase time projection chambers are well suited to $0νββ$ searches due to their intrinsically precise energy resolution and topological event identification capabilities. Scalability to ton- and multi-ton masses requires readout of large-area electroluminescent regions with fine spatial resolution, low radiogenic backgrounds, and a scalable data acquisition system. This paper presents a detector prototype that records event topology in an electroluminescent xenon gas TPC via VUV image-intensified cameras. This enables an extendable readout of large tracking planes with commercial devices that reside almost entirely outside of the active medium.Following further development in intermediate scale demonstrators, this technique may represent a novel and enlargeable method for topological event imaging in $0νββ$. △ Less

Submitted 3 August, 2023; v1 submitted 12 April, 2023; originally announced April 2023.

Comments: 30 Pages, 22 figures, Updated to match current JINST submission

A Compact Dication Source for Ba$^{2+}$ Tagging and Heavy Metal Ion Sensor Development

Authors: K. E. Navarro, B. J. P. Jones, J. Baeza-Rubio, M. Boyd, A. A. Denisenko, F. W. Foss, S. Giri, R. Miller, D. R. Nygren, M. R. Tiscareno, F. J. Samaniego, K. Stogsdill, C. Adams, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, S. Ayet, C. D. R. Azevedo, K. Bailey, F. Ballester, J. M. Benlloch-Rodríguez, F. I. G. M. Borges , et al. (85 additional authors not shown)

Abstract: We present a tunable metal ion beam that delivers controllable ion currents in the picoamp range for testing of dry-phase ion sensors. Ion beams are formed by sequential atomic evaporation and single or multiple electron impact ionization, followed by acceleration into a sensing region. Controllability of the ionic charge state is achieved through tuning of electrode potentials that influence the… ▽ More We present a tunable metal ion beam that delivers controllable ion currents in the picoamp range for testing of dry-phase ion sensors. Ion beams are formed by sequential atomic evaporation and single or multiple electron impact ionization, followed by acceleration into a sensing region. Controllability of the ionic charge state is achieved through tuning of electrode potentials that influence the retention time in the ionization region. Barium, lead, and cobalt samples have been used to test the system, with ion currents identified and quantified using a quadrupole mass analyzer. Realization of a clean $\mathrm{Ba^{2+}}$ ion beam within a bench-top system represents an important technical advance toward the development and characterization of barium tagging systems for neutrinoless double beta decay searches in xenon gas. This system also provides a testbed for investigation of novel ion sensing methodologies for environmental assay applications, with dication beams of Pb$^{2+}$ and Cd$^{2+}$ also demonstrated for this purpose. △ Less

Submitted 2 March, 2023; originally announced March 2023.

Reflectance and fluorescence characteristics of PTFE coated with TPB at visible, UV, and VUV as a function of thickness

Authors: J. Haefner, A. Fahs, J. Ho, C. Stanford, R. Guenette, C. Adams, H. Almazán, V. Álvarez, B. Aparicio, A. I. Aranburu, L. Arazi, I. J. Arnquist, F. Auria-Luna, S. Ayet, C. D. R. Azevedo, K. Bailey, F. Ballester, J. M. Benlloch-Rodríguez, F. I. G. M. Borges, S. Bounasser, N. Byrnes, S. Cárcel, J. V. Carrión, S. Cebrián, E. Church , et al. (78 additional authors not shown)

Abstract: Polytetrafluoroethylene (PTFE) is an excellent diffuse reflector widely used in light collection systems for particle physics experiments. In noble element systems, it is often coated with tetraphenyl butadiene (TPB) to allow detection of vacuum ultraviolet scintillation light. In this work this dependence is investigated for PTFE coated with TPB in air for light of wavelengths of 200~nm, 260~nm,… ▽ More Polytetrafluoroethylene (PTFE) is an excellent diffuse reflector widely used in light collection systems for particle physics experiments. In noble element systems, it is often coated with tetraphenyl butadiene (TPB) to allow detection of vacuum ultraviolet scintillation light. In this work this dependence is investigated for PTFE coated with TPB in air for light of wavelengths of 200~nm, 260~nm, and 450~nm. The results show that TPB-coated PTFE has a reflectance of approximately 92\% for thicknesses ranging from 5~mm to 10~mm at 450~nm, with negligible variation as a function of thickness within this range. A cross-check of these results using an argon chamber supports the conclusion that the change in thickness from 5~mm to 10~mm does not affect significantly the light response at 128~nm. Our results indicate that pieces of TPB-coated PTFE thinner than the typical 10~mm can be used in particle physics detectors without compromising the light signal. △ Less

Submitted 10 January, 2023; v1 submitted 9 November, 2022; originally announced November 2022.

Review of foundational concepts and emerging directions in metamaterial research: Design, phenomena, and applications

Authors: Jade E. Holliman Jr, H. Todd Schaef, B. Peter McGrail, Quin R. S. Miller

Abstract: In the past two decades, artificial structures known as metamaterials have been found to exhibit extraordinary material properties that enable the unprecedented manipulation of electromagnetic waves, elastic waves, molecules, and particles. Phenomena such as negative refraction, bandgaps, near perfect wave absorption, wave focusing, negative Poissons ratio, negative thermal conductivity, etc., all… ▽ More In the past two decades, artificial structures known as metamaterials have been found to exhibit extraordinary material properties that enable the unprecedented manipulation of electromagnetic waves, elastic waves, molecules, and particles. Phenomena such as negative refraction, bandgaps, near perfect wave absorption, wave focusing, negative Poissons ratio, negative thermal conductivity, etc., all are possible with these materials. Metamaterials were originally theorized and fabricated in electrodynamics, but research into their applications has expanded into acoustics, thermodynamics, seismology, classical mechanics, and mass transport. In this Research Update we summarize the history, current state of progress, and emerging directions of metamaterials by field, focusing the unifying principles at the foundation of each discipline. We discuss the different designs and mechanisms behind metamaterials as well as the governing equations and effective material parameters for each field. Also, current and potential applications for metamaterials are discussed. Finally, we provide an outlook on future progress in the emerging field of metamaterials. △ Less

Submitted 6 November, 2022; originally announced November 2022.

Comments: 22 pages, 3 figures, 1 table

Novel applications of Generative Adversarial Networks (GANs) in the analysis of ultrafast electron diffraction (UED) images

Authors: Hazem Daoud, Dhruv Sirohi, Endri Mjeku, John Feng, Saeed Oghbaey, R. J. Dwayne Miller

Abstract: Inferring transient molecular structural dynamics from diffraction data is an ambiguous task that often requires different approximation methods. In this paper we present an attempt to tackle this problem using machine learning. While most recent applications of machine learning for the analysis of diffraction images apply only a single neural network to an experimental dataset and train it on the… ▽ More Inferring transient molecular structural dynamics from diffraction data is an ambiguous task that often requires different approximation methods. In this paper we present an attempt to tackle this problem using machine learning. While most recent applications of machine learning for the analysis of diffraction images apply only a single neural network to an experimental dataset and train it on the task of prediction, our approach utilizes an additional generator network trained on both synthetic data and experimental data. Our network converts experimental data into idealized diffraction patterns from which information is extracted via a convolutional neural network (CNN) trained on synthetic data only. We validate this approach on ultrafast electron diffraction (UED) data of bismuth samples undergoing thermalization upon excitation via 800 nm laser pulses. The network was able to predict transient temperatures with a deviation of less than 6% from analytically estimated values. Notably, this performance was achieved on a dataset of 408 images only. We believe employing this network in experimental settings where high volumes of visual data are collected, such as beam lines, could provide insights into the structural dynamics of different samples. △ Less

Submitted 7 July, 2023; v1 submitted 13 October, 2022; originally announced October 2022.

Smart Quantum Statistical Imaging beyond the Abbe-Rayleigh Criterion

Authors: Narayan Bhusal, Mingyuan Hong, Nathaniel R. Miller, Mario A Quiroz-Juarez, Roberto de J. Leon-Montiel, Chenglong You, Omar S. Magana-Loaiza

Abstract: The manifestation of the wave nature of light through diffraction imposes limits on the resolution of optical imaging. For over a century, the Abbe-Rayleigh criterion has been utilized to assess the spatial resolution limits of optical instruments. Recently, there has been an enormous impetus in overcoming the Abbe-Rayleigh resolution limit by projecting target light beams onto spatial modes. Thes… ▽ More The manifestation of the wave nature of light through diffraction imposes limits on the resolution of optical imaging. For over a century, the Abbe-Rayleigh criterion has been utilized to assess the spatial resolution limits of optical instruments. Recently, there has been an enormous impetus in overcoming the Abbe-Rayleigh resolution limit by projecting target light beams onto spatial modes. These conventional schemes for superresolution rely on a series of spatial projective measurements to pick up phase information that is used to boost the spatial resolution of optical systems. Unfortunately, these schemes require a priori information regarding the coherence properties of "unknown" light beams. Furthermore, they require stringent alignment and centering conditions that cannot be achieved in realistic scenarios. Here, we introduce a smart quantum camera for superresolving imaging. This camera exploits the self-learning features of artificial intelligence to identify the statistical fluctuations of unknown mixtures of light sources at each pixel. This is achieved through a universal quantum model that enables the design of artificial neural networks for the identification of quantum photon fluctuations. Our camera overcomes the inherent limitations of existing superresolution schemes based on spatial mode projection. Thus, our work provides a new perspective in the field of imaging with important implications for microscopy, remote sensing, and astronomy. △ Less

Submitted 11 October, 2021; originally announced October 2021.

Comments: 10 pages, 5 figures

Quantum state tomography of molecules by ultrafast diffraction

Authors: Ming Zhang, Shuqiao Zhang, Yanwei Xiong, Hankai Zhang, Anatoly A. Ischenko, Oriol Vendrell, Xiaolong Dong, Xiangxu Mu, Martin Centurion, Haitan Xu, R. J. Dwayne Miller, Zheng Li

Abstract: Ultrafast electron diffraction and time-resolved serial crystallography are the basis of the ongoing revolution in capturing at the atomic level of detail the structural dynamics of molecules. However, most experiments employ the classical "ball-and-stick" depictions, and the information of molecular quantum states, such as the density matrix, is missing. Here, we introduce a framework for the pre… ▽ More Ultrafast electron diffraction and time-resolved serial crystallography are the basis of the ongoing revolution in capturing at the atomic level of detail the structural dynamics of molecules. However, most experiments employ the classical "ball-and-stick" depictions, and the information of molecular quantum states, such as the density matrix, is missing. Here, we introduce a framework for the preparation and ultrafast coherent diffraction from rotational wave packets of molecules, and we establish a new variant of quantum state tomography for ultrafast electron diffraction to characterize the molecular quantum states. The ability to reconstruct the density matrix of molecules of arbitrary degrees of freedom will provide us with an unprecedentedly clear view of the quantum states of molecules, and enable the visualization of effects dictated by the quantum dynamics of molecules. △ Less

Submitted 28 July, 2021; originally announced July 2021.

Comments: arXiv admin note: substantial text overlap with arXiv:2012.11899

Video-Streaming Biomedical Implants using Ultrasonic Waves for Communication

Authors: Gizem Tabak, Jae Won Choi, Rita J. Miller, Michael L. Oelze, Andrew C. Singer

Abstract: The use of wireless implanted medical devices (IMDs) is growing because they facilitate continuous monitoring of patients during normal activities, simplify medical procedures required for data retrieval and reduce the likelihood of infection associated with trailing wires. However, most of the state-of-the-art IMDs are passive and offline devices. One of the key obstacles to an active and online… ▽ More The use of wireless implanted medical devices (IMDs) is growing because they facilitate continuous monitoring of patients during normal activities, simplify medical procedures required for data retrieval and reduce the likelihood of infection associated with trailing wires. However, most of the state-of-the-art IMDs are passive and offline devices. One of the key obstacles to an active and online IMD is the infeasibility of real-time, high-quality video broadcast from the IMD. Such broadcast would help develop innovative devices such as a video-streaming capsule endoscopy (CE) pill with therapeutic intervention capabilities. State-of-the-art IMDs employ radio-frequency electromagnetic waves for information transmission. However, high attenuation of RF-EM waves in tissues and federal restrictions on the transmit power and operable bandwidth lead to fundamental performance constraints for IMDs employing RF links, and prevent achieving high data rates that could accomodate video broadcast. In this work, ultrasonic waves were used for video transmission and broadcast through biological tissues. The proposed proof-of-concept system was tested on a porcine intestine ex vivo and a rabbit in vivo. It was demonstrated that using a millimeter-sized, implanted biocompatible transducer operating at 1.1-1.2 MHz, it was possible to transmit endoscopic video with high resolution (1280 pixels by 720 pixels) through porcine intestine wrapped with bacon, and to broadcast standard definition (640 pixels by 480 pixels) video near real-time through rabbit abdomen in vivo. A media repository that includes experimental demonstrations and media files accompanies this paper. The accompanying media repository can be found at this link: https://bit.ly/3wuc7tk. △ Less

Submitted 27 June, 2021; v1 submitted 25 June, 2021; originally announced June 2021.

Comments: arXiv admin note: text overlap with arXiv:1909.13172

Utilizing relativistic time dilation for time-resolved studies

Authors: Hazem Daoud, R. J. Dwayne Miller

Abstract: Time-resolved studies have so far relied on rapidly triggering a photo-induced dynamic in chemical or biological ions or molecules and subsequently probing them with a beam of fast moving photons or electrons that crosses the studied samples in a short period of time. Hence, the time resolution of the signal is mainly set by the pulse duration of the pump and probe pulses. In this paper we propose… ▽ More Time-resolved studies have so far relied on rapidly triggering a photo-induced dynamic in chemical or biological ions or molecules and subsequently probing them with a beam of fast moving photons or electrons that crosses the studied samples in a short period of time. Hence, the time resolution of the signal is mainly set by the pulse duration of the pump and probe pulses. In this paper we propose a different approach to this problem that has the potential to consistently achieve orders of magnitude higher time resolutions than what is possible with laser technology or electron beam compression methods. Our proposed approach relies on accelerating the sample to a high speed to achieve relativistic time dilation. Probing the time-dilated sample would open up previously inaccessible time resolution domains. △ Less

Submitted 12 March, 2021; v1 submitted 13 November, 2020; originally announced November 2020.

Journal ref: J. Chem. Phys. 154, 111107 (2021)

Serial Electron Diffraction Data Processing with diffractem and CrystFEL

Authors: Robert Bücker, Pascal Hogan-Lamarre, R. J. Dwayne Miller

Abstract: Serial electron diffraction (SerialED) is an emerging technique, which applies the snapshot data-collection mode of serial X-ray crystallography to three-dimensional electron diffraction (3D ED), forgoing the conventional rotation method. Similarly to serial X-ray crystallography, this approach leads to almost complete absence of radiation damage effects even for the most sensitive samples, and al… ▽ More Serial electron diffraction (SerialED) is an emerging technique, which applies the snapshot data-collection mode of serial X-ray crystallography to three-dimensional electron diffraction (3D ED), forgoing the conventional rotation method. Similarly to serial X-ray crystallography, this approach leads to almost complete absence of radiation damage effects even for the most sensitive samples, and allows for a high level of automation. However, SerialED also necessitates new techniques of data processing, which combine existing pipelines for rotation electron diffraction and serial X-ray crystallography with some more particular solutions for challenges arising in SerialED specifically. Here, we introduce our analysis pipeline for SerialED data, and its implementation using the CrystFEL and diffractem program packages. Detailed examples are provided in extensive supplementary code. △ Less

Submitted 5 November, 2020; originally announced November 2020.

Comments: 21 pages, 9 figures

Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite

Authors: Hong-Guang Duan, Vandana Tiwari, Ajay Jha, Golibjon R. Berdiyorov, Alexey Akimov, Oriol Vendrell, Pabitra K. Nayak, Henry J. Snaith, Michael Thorwart, Zheng Li, Mohamed E. Madjet, R. J. Dwayne Miller

Abstract: Organic-inorganic perovskites have shown great promise towards their application in optoelectronics. The success of this class of material is dictated by the complex interplay between various underlying microscopic phenomena. The structural dynamics of organic cations and the inorganic sublattice after photoexcitation is hypothesized to have a direct effect on the material properties, thereby affe… ▽ More Organic-inorganic perovskites have shown great promise towards their application in optoelectronics. The success of this class of material is dictated by the complex interplay between various underlying microscopic phenomena. The structural dynamics of organic cations and the inorganic sublattice after photoexcitation is hypothesized to have a direct effect on the material properties, thereby affecting the overall device performance. Here, we use two-dimensional (2D) electronic spectroscopy to reveal impulsively excited vibrational modes of methylammonium (MA) lead iodide perovskite, which drive the structural distortion after photoexcitation. The vibrational analysis of the measured data allows us to directly monitor the time evolution of the librational motion of the MA cation along with the vibrational coherences of inorganic sublattice. Wavelet analysis of the observed vibrational coherences uncovers the interplay between these two types of phonons. It reveals the coherent generation of the librational motion of the MA cation within ~300 fs, which is complemented by the coherent evolution of the skeletal motion of the inorganic sublattice. We have employed time-dependent density functional theory (TDDFT) to study the atomic motion of the MA cation and the inorganic sublattice during the process of photoexcitation. The TDDFT calculations support our experimental observations of the coherent generation of librational motions in the MA cation and highlight the importance of the anharmonic interaction between the MA cation and the inorganic sublattice. Our calculations predict the transfer of the photoinduced vibrational coherence from the MA cation to the inorganic sublattice, which drives the skeleton motion to form a polaronic state leading to long lifetimes of the charge carriers. This work may lead to novel design principles for next generation of solar cell materials. △ Less

Submitted 10 April, 2020; originally announced April 2020.

Intermolecular Vibrations Drive Ultrafast Singlet Fission

Authors: Hong-Guang Duan, Ajay Jha 1, Xin Li, Vandana Tiwari, Hanyang Ye, Pabitra K. Nayak, Xiao-Lei Zhu, Zheng Li, Todd J. Martinez, Michael Thorwart, R. J. Dwayne Miller

Abstract: Singlet fission is a spin-allowed exciton multiplication process in organic semiconductors that converts one spin-singlet exciton to two triplet excitons. It offers the potential to enhance solar energy conversion by circumventing the Shockley-Queisser limit on efficiency. Recently, the mechanism of the primary singlet fission process in pentacene and its derivatives have been extensively investig… ▽ More Singlet fission is a spin-allowed exciton multiplication process in organic semiconductors that converts one spin-singlet exciton to two triplet excitons. It offers the potential to enhance solar energy conversion by circumventing the Shockley-Queisser limit on efficiency. Recently, the mechanism of the primary singlet fission process in pentacene and its derivatives have been extensively investigated, however, the nature of the primary ultrafast process in singlet fission is still a matter of debate. Here, we study the singlet fission process in a pentacene film by employing a combination of transient-grating (TG) and two-dimensional (2D) electronic spectroscopy complemented by quantum chemical and nonadiabatic dynamics calculations. The high sensitivity of heterodyne detected TG spectroscopy enabled us to capture the vibrational coherence and to show that it mediates the transition from the singlet excited electronic state to the triplet-pair state. This coherent process is further examined by 2D electronic spectroscopy. Detailed analysis of the experimental data reveals that significant vibronic couplings of a few key modes in the low- and high-frequency region connect the excited singlet and triplet-pair states. Based on quantum chemical calculations, we identify these key intermolecular rocking modes along the longitudinal molecular axis between the pentacene molecules. They play the essential role of an electronic bridge between the singlet and triplet-pair states. Along with high-frequency local vibrations acting as tuning modes, these rocking motions drive the ultrafast dynamics at the multidimensional conical intersection in the singlet fission process. △ Less

Submitted 8 October, 2019; originally announced October 2019.

Effect of Oxygen on Hydrogen Diffusivity in hcp-Zirconium

Authors: Manura Liyanage, Ronald Miller, R. K. N. D. Rajapakse

Abstract: Zirconium and its alloys are extensively used as cladding material in nuclear reactors. They are vulnerable to hydrogen degradation under the harsh service conditions of the reactors, which necessitates continuous monitoring for the hydride concentration. The presence of hydride denuded zones in the latter stages of the pressure tube's life hinders the monitoring process, which is carried out by s… ▽ More Zirconium and its alloys are extensively used as cladding material in nuclear reactors. They are vulnerable to hydrogen degradation under the harsh service conditions of the reactors, which necessitates continuous monitoring for the hydride concentration. The presence of hydride denuded zones in the latter stages of the pressure tube's life hinders the monitoring process, which is carried out by scrape samples taken from the surface of pressure tubes. We investigated the effect of oxygen on diffusivity of hydrogen in hcp-Zr, to check the hypothesis that oxygen slows the diffusion of hydrogen and thereby encourages the occurrence of hydride denuded zones. From the study we found that oxygen indeed decreases the diffusivity of hydrogen in hcp-Zr for moderate O concentrations, supporting the hypothesis. We investigated the diffusion processes of individual H atoms, which showed that the reduction in diffusivity is caused by a decrease in the hopping rates and the formation of hydrogen traps by the combination of several interstitial sites. △ Less

Submitted 5 September, 2019; originally announced September 2019.

Does electronic coherence enhance anticorrelated pigment vibrations under realistic conditions?

Authors: Hong-Guang Duan, Michael Thorwart, R. J. Dwayne Miller

Abstract: The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom. Here, we reexamine two recently formulated concepts that a coherent vibronic coupling between molecular states would either extend the electronic coherence lifet… ▽ More The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom. Here, we reexamine two recently formulated concepts that a coherent vibronic coupling between molecular states would either extend the electronic coherence lifetime or enhance the amplitude of the anticorrelated vibrational mode at longer times. For this, we study a vibronically coupled dimer and calculate the nonlinear two-dimensional (2D) electronic spectra which directly reveal electronic coherence. The timescale of electronic coherence is initially extracted by measuring the anti-diagonal bandwidth of the central peak in the 2D spectrum at zero waiting time. Based on the residual analysis, we identify small-amplitude long-lived oscillations in the cross-peaks, which, however, are solely due to groundstate vibrational coherence, regardless of having resonant or off-resonant conditions. Our studies neither show an enhancement of the electronic quantum coherence nor an enhancement of the anticorrelated vibrational mode by the vibronic coupling under ambient conditions. △ Less

Submitted 25 March, 2019; originally announced April 2019.

High-temperature Ultraviolet Photodetectors: A Review

Authors: Ruth A. Miller, Hongyun So, Thomas A. Heuser, Debbie G. Senesky

Abstract: Wide bandgap semiconductors have become the most attractive materials in optoelectronics in the last decade. Their wide bandgap and intrinsic properties have advanced the development of reliable photodetectors to selectively detect short wavelengths (i.e., ultraviolet, UV) in high temperature regions (up to 300°C). The main driver for the development of high-temperature UV detection instrumentatio… ▽ More Wide bandgap semiconductors have become the most attractive materials in optoelectronics in the last decade. Their wide bandgap and intrinsic properties have advanced the development of reliable photodetectors to selectively detect short wavelengths (i.e., ultraviolet, UV) in high temperature regions (up to 300°C). The main driver for the development of high-temperature UV detection instrumentation is in-situ monitoring of hostile environments and processes found within industrial, automotive, aerospace, and energy production systems that emit UV signatures. In this review, a summary of the optical performance (in terms of photocurrent-to-dark current ratio, responsivity, quantum efficiency, and response time) and uncooled, high-temperature characterization of III-nitride, SiC, and other wide bandgap semiconductor UV photodetectors is presented. △ Less

Submitted 19 September, 2018; originally announced September 2018.

Reduced-Order Modeling through Machine Learning Approaches for Brittle Fracture Applications

Authors: A. Hunter, B. A. Moore, M. K. Mudunuru, V. T. Chau, R. L. Miller, R. B. Tchoua, C. Nyshadham, S. Karra, D. O. Malley, E. Rougier, H. S. Viswanathan, G. Srinivasan

Abstract: In this paper, five different approaches for reduced-order modeling of brittle fracture in geomaterials, specifically concrete, are presented and compared. Four of the five methods rely on machine learning (ML) algorithms to approximate important aspects of the brittle fracture problem. In addition to the ML algorithms, each method incorporates different physics-based assumptions in order to reduc… ▽ More In this paper, five different approaches for reduced-order modeling of brittle fracture in geomaterials, specifically concrete, are presented and compared. Four of the five methods rely on machine learning (ML) algorithms to approximate important aspects of the brittle fracture problem. In addition to the ML algorithms, each method incorporates different physics-based assumptions in order to reduce the computational complexity while maintaining the physics as much as possible. This work specifically focuses on using the ML approaches to model a 2D concrete sample under low strain rate pure tensile loading conditions with 20 preexisting cracks present. A high-fidelity finite element-discrete element model is used to both produce a training dataset of 150 simulations and an additional 35 simulations for validation. Results from the ML approaches are directly compared against the results from the high-fidelity model. Strengths and weaknesses of each approach are discussed and the most important conclusion is that a combination of physics-informed and data-driven features are necessary for emulating the physics of crack propagation, interaction and coalescence. All of the models presented here have runtimes that are orders of magnitude faster than the original high-fidelity model and pave the path for developing accurate reduced order models that could be used to inform larger length-scale models with important sub-scale physics that often cannot be accounted for due to computational cost. △ Less

Submitted 5 June, 2018; originally announced June 2018.

Comments: 25 pages, 8 figures

Exploring vibrational ladder climbing in vibronic coupling models: Toward experimental observation of a geometric phase signature of a conical intersection

Authors: Hazem Daoud, Loic Joubert-Doriol, Artur F. Izmaylov, R. J. Dwayne Miller

Abstract: Conical intersections (CIs) have been widely studied using spectroscopic techniques. However, CIs have mainly been identified by rapid internal conversion transitions that take place after the photoexcitation. Such identifications cannot distinguish various types of intersections as well as to separate the actual intersection from an avoided crossing. In this paper, we investigate how ultrafast IR… ▽ More Conical intersections (CIs) have been widely studied using spectroscopic techniques. However, CIs have mainly been identified by rapid internal conversion transitions that take place after the photoexcitation. Such identifications cannot distinguish various types of intersections as well as to separate the actual intersection from an avoided crossing. In this paper, we investigate how ultrafast IR laser pulses can be utilized to stimulate nuclear dynamics revealing geometric phase features associated with CIs. We consider two low-dimensional nonadiabatic models to obtain optimal two- and three-pulse laser sequences for stimulating nuclear dynamics necessary for the CI identification. Our results provide insights on designing non-linear spectroscopic schemes for subsequent probes of the nuclear wavepackets by ultrafast electron diffraction techniques to unambiguously detect CIs in molecules. △ Less

Submitted 15 August, 2018; v1 submitted 25 April, 2018; originally announced April 2018.

Smaller desert dust cooling effect estimated from analysis of dust size and abundance

Authors: Jasper F. Kok, David A. Ridley, Qing Zhou, Ron L. Miller, Chun Zhao, Colette L. Heald, Daniel S. Ward, Samuel Albani, Karsten Haustein

Abstract: Desert dust aerosols affect Earth's global energy balance through direct interactions with radiation, and through indirect interactions with clouds and ecosystems. But the magnitudes of these effects are so uncertain that it remains unclear whether atmospheric dust has a net warming or cooling effect on global climate. Consequently, it is still uncertain whether large changes in atmospheric dust l… ▽ More Desert dust aerosols affect Earth's global energy balance through direct interactions with radiation, and through indirect interactions with clouds and ecosystems. But the magnitudes of these effects are so uncertain that it remains unclear whether atmospheric dust has a net warming or cooling effect on global climate. Consequently, it is still uncertain whether large changes in atmospheric dust loading over the past century have slowed or accelerated anthropogenic climate change, or what the effects of potential future changes in dust loading will be. Here we present an analysis of the size and abundance of dust aerosols to constrain the direct radiative effect of dust. Using observational data on dust abundance, in situ measurements of dust optical properties and size distribution, and climate and atmospheric chemical transport model simulations of dust lifetime, we find that the dust found in the atmosphere is substantially coarser than represented in current global climate models. Since coarse dust warms climate, the global dust direct radiative effect is likely to be less cooling than the ~-0.4 W/m2 estimated by models in a current global aerosol model ensemble. Instead, we constrain the dust direct radiative effect to a range between -0.48 and +0.20 W/m2, which includes the possibility that dust causes a net warming of the planet. △ Less

Submitted 20 October, 2017; originally announced October 2017.

Comments: Published as article in Nature Geoscience

Journal ref: Nature Geoscience, 10, 274-278

Mechanical and optical nanodevices in single-crystal quartz

Authors: Young-Ik Sohn, Rachel Miller, Vivek Venkataraman, Marko Lončar

Abstract: Single-crystal α-quartz, one of the most widely used piezoelectric materials, has enabled a wide range of timing applications. Owing to the fact that integrated thin-film based quartz platform is not available, most of these applications rely on macroscopic, bulk crystal-based devices. Here we show that the Faraday cage angled-etching technique can be used to realize nanoscale electromechanical an… ▽ More Single-crystal α-quartz, one of the most widely used piezoelectric materials, has enabled a wide range of timing applications. Owing to the fact that integrated thin-film based quartz platform is not available, most of these applications rely on macroscopic, bulk crystal-based devices. Here we show that the Faraday cage angled-etching technique can be used to realize nanoscale electromechanical and photonic devices in quartz. Using this approach, we demonstrate quartz nanomechanical cantilevers and ring resonators featuring Qs of 4,900 and 8,900, respectively. △ Less

Submitted 9 October, 2017; originally announced October 2017.

Comments: 10 pages, 4 figures

Low-dose cryo electron ptychography via non-convex Bayesian optimization

Authors: Philipp Michael Pelz, Wen Xuan Qiu, Robert Bücker, Günther Kassier, R. J. Dwayne Miller

Abstract: Electron ptychography has seen a recent surge of interest for phase sensitive imaging at atomic or near-atomic resolution. However, applications are so far mainly limited to radiation-hard samples because the required doses are too high for imaging biological samples at high resolution. We propose the use of non-convex, Bayesian optimization to overcome this problem and reduce the dose required fo… ▽ More Electron ptychography has seen a recent surge of interest for phase sensitive imaging at atomic or near-atomic resolution. However, applications are so far mainly limited to radiation-hard samples because the required doses are too high for imaging biological samples at high resolution. We propose the use of non-convex, Bayesian optimization to overcome this problem and reduce the dose required for successful reconstruction by two orders of magnitude compared to previous experiments. We suggest to use this method for imaging single biological macromolecules at cryogenic temperatures and demonstrate 2D single-particle reconstructions from simulated data with a resolution of 7.9 Å$\,$ at a dose of 20 $e^- / Å^2$. When averaging over only 15 low-dose datasets, a resolution of 4 Å$\,$ is possible for large macromolecular complexes. With its independence from microscope transfer function, direct recovery of phase contrast and better scaling of signal-to-noise ratio, cryo-electron ptychography may become a promising alternative to Zernike phase-contrast microscopy. △ Less

Submitted 19 February, 2017; originally announced February 2017.