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At least 361 records · Page 20

A silicon singlet–triplet qubit driven by spin-valley coupling

Spin–orbit effects, inherent to electrons confined in quantum dots at a silicon heterointerface, provide a means to control electron spin qubits without the added complexity of on-chip, nanofabricated micromagnets or nearby coplanar striplines. Here, we demonstrate a singlet–triplet qubit operating mode that can drive qubit evolution at frequencies in excess of 200 MHz. This approach offers a means to electrically turn on and off fast control, while providing high logic gate orthogonality and long qubit dephasing times. We utilize this operational mode for dynamical decoupling experiments to probe the charge noise power spectrum in a silicon metal-oxide-semiconductor double quantum dot. In addition, we assess qubit frequency drift over longer timescales to capture low-frequency noise. We present the charge noise power spectral density up to 3 MHz, which exhibits a 1/ f α dependence consistent with α ~ 0.7, over 9 orders of magnitude in noise frequency.

97 MATHEMATICS AND COMPUTING↗

Two-color-driven enhanced high-order harmonic generation in solids

We theoretically investigate the emission of high-harmonic (HH) radiation in model crystals by bichromatic few-cycle driving pulses that are composed as the phase-coherent superposition of a mid-infrared fundamental pulse and its second harmonic. Adjusting the model-crystal parameters to reproduce the lowest band gap of MgO, we examine the extent to which distinct domains of the HH spectrum can be controlled and enhanced by tuning the temporal profile of the bichromatic driving laser electric field. We change the driving-pulse shape by varying its fundamental-versus-second-harmonic pulse amplitude ratio and delay, while keeping the energy of the driving laser pulse fixed. For suitable amplitude ratios and delays, we find an up to fivefold enhancement of the spectral HH yield and significant shifts of the HH cutoff frequency.

74 ATOMIC AND MOLECULAR PHYSICS↗

Controlling the Manifold of Polariton States Through Molecular Disorder

Exciton polaritons, arising from the interaction of electronic transitions with confined electromagnetic fields, have emerged as a powerful tool to manipulate the properties of organic materials. However, standard experimental and theoretical approaches overlook the significant energetic disorder present in most materials now studied. Using the conjugated polymer P3HT as a model platform, the degree of energetic disorder is systematically tuned and a corresponding redistribution of photonic character within the polariton manifold is observed. Based on these subtle spectral features, a more generalized approach is developed to describe strong light–matter coupling in disordered systems that captures the key spectroscopic observables and provides a description of the rich manifold of states intermediate between bright and dark. Finally, applied to a wide range of organic systems, the method challenges prevailing notions about ultrastrong coupling and whether it can be achieved with broad, disordered absorbers.

36 MATERIALS SCIENCE↗

Strongly Anharmonic Phonons and Their Role in Superionic Diffusion and Ultralow Thermal Conductivity of Cu 7 PSe 6

We report the quest for advanced superionic materials requires understanding their complex atomic dynamics, but detailed studies of the interplay between lattice vibrations and ionic diffusion remain scarce. Here inelastic and quasielastic neutron scattering measurements in the superionic argyrodite Cu 7 PSe 6 are reported, combined with molecular dynamics (MD) based on ab initio and machine-learned potentials, providing critical insights into the atomistic mechanisms underlying fast ion conduction. The results reveal how long-range Cu diffusion is limited by intercluster hopping, controlled by selective anharmonic phonons of the crystalline framework. Further, the Green–Kubo simulations reproduce the ultralow lattice thermal conductivity and identify contributions from mobile ions, phonons, and their cross-correlations. The mode resolved analysis shows that the thermal conductivity is dominated by low-energy acoustic phonon modes of the overall crystal framework. The analysis of mode-resolved spectral functions further show that vibrational modes with significant Cu contributions are strongly damped, corresponding to the breakdown of associated phonon quasiparticles. These results highlight the importance of strongly anharmonic effects in superionic systems, in which the traditional quasiharmonic phonon picture is insufficient, and pave the way toward combining machine-learning accelerated simulations with neutron scattering experiments to rationalize the complex atomic dynamics underlying ionic and thermal transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Laser beam pointing stabilization using analog position-sensitive diodes

Laser wire scanners have been used for ion beam profile and emittance measurements at the Spallation Neutron Source linear accelerator. Due to propagation distances exceeding 100 m, reliable measurements require laser beam stabilization, previously accomplished with a feedback control loop using a digital camera as a position sensor [Hardin et al., Opt. Express 19, 2874 (2011)]. Here, this paper presents an upgraded pointing stabilization system utilizing analog position-sensitive diodes (PSDs) as the position detector, optimized with an optical diffuser. The new system significantly surpasses the previous system by offering an order-of-magnitude improvement in radiation tolerance and a bandwidth limited only by the burst repetition rate of the laser beam. Operating with a 60-Hz burst mode laser, the new system effectively suppresses laser beam drifts up to 30 Hz, compared to the previous system’s 4 Hz limit. In addition, the amplitude of spectral components below 0.1 Hz was reduced by a factor of more than 100, which is over seven times greater than was achieved by the previous system.

Data acquisition↗

Simulation of high-frequency dissolved oxygen dynamics in a shallow estuary, the Corsica River, Chesapeake Bay

Understanding shallow water biogeochemical dynamics is a challenge in coastal regions, due to the presence of highly variable land-water interface fluxes, tight coupling with sediment processes, tidal dynamics, and diurnal variability in biogeochemical processes. While the deployment of continuous monitoring devices has improved our understanding of high-frequency (12 - 24 hours) variability and spatial heterogeneity in shallow regions, mechanistic modeling of these dynamics has lagged behind conceptual and empirical models. The inherent complexity of shallow water systems is represented in the Corsica River estuary, a small basin within the Chesapeake Bay ecosystem, where abundant monitoring data have been collected from long-term monitoring stations, continuous monitoring sensors, synoptic sensor surveys, and measurements of sediment-water fluxes. A state-of-the-art modeling system, the Semi-implicit Cross-scale Hydroscience Integrated System Model (SCHISM), was applied to the Corsica domain with a high-resolution grid and nutrient loads from the most recent version of the Chesapeake Bay watershed model. The Corsica SCHISM model reproduced observed high-frequency variability in dissolved oxygen, as well as seasonal variability in chlorophyll-a and sediment-water fluxes. Time-series signal analyses using Empirical Model Decomposition and spectral analysis revealed that the diurnal and M2 tide frequencies are the dominant high-frequency modes and physical transport contributes a larger share to dissolved oxygen budgets than biogeochemical processes on an hourly time scale. Heterogeneity and patchiness in dissolved oxygen resulting from phytoplankton distributions and geometry-driven eddies amplify the physical transport effect, and on longer time scales oxygen is controlled more by photosynthesis and respiration. Our simulation demonstrates that interactions among physical and biological dynamics generate complex high-frequency variability in water quality and non-linear reposes to nutrient loading and environmental forcing in shallow water systems.

54 ENVIRONMENTAL SCIENCES↗

Real-time confinement regime detection in fusion plasmas with convolutional neural networks and high-bandwidth edge fluctuation measurements

Abstract A real-time detection of the plasma confinement regime can enable new advanced plasma control capabilities for both the access to and sustainment of enhanced confinement regimes in fusion devices. For example, a real-time indication of the confinement regime can facilitate transition to the high-performing wide-pedestal (WP) quiescent H-mode, or avoid unwanted transitions to lower confinement regimes that may induce plasma termination. To demonstrate real-time confinement regime detection, we use the 2D beam emission spectroscopy (BES) diagnostic system to capture localized density fluctuations of long wavelength turbulent modes in the edge region at a 1 MHz sampling rate. BES data from 330 discharges in either L-mode, H-mode, quiescent H (QH)-mode, or WP QH-mode were collected from the DIII-D tokamak and curated to develop a high-quality database to train a deep-learning classification model for real-time confinement detection. We utilize the 6×8 spatial configuration with a time window of 1024 µ s and recast the input to obtain spectral-like features via fast Fourier transform preprocessing. We employ a shallow 3D convolutional neural network for the multivariate time-series classification task and utilize a softmax in the final dense layer to retrieve a probability distribution over the different confinement regimes. Our model classifies the global confinement state on 44 unseen test discharges with an average F 1 score of 0.94, using only ∼1 ms snippets of BES data at a time. This activity demonstrates the feasibility for real-time data analysis of fluctuation diagnostics in future devices such as ITER, where the need for reliable and advanced plasma control is urgent.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Multidimensional coherent spectroscopy of light-driven states and their collective modes in multiband superconductors

We present a comprehensive theory of light-controlled multiband superconductivity, and apply it to predict distinctive signatures of light-driven superconducting (SC) states in terahertz multidimensional coherent spectroscopy (THz-MDCS) experiments. We first derive gauge-invariant Maxwell-Bloch equations for multiband BCS superconductors with spatial fluctuations. We consider driving electromagnetic fields determined self-consistently by Maxwell's equations. By calculating the THz-MDCS spectra measured experimentally in the clean SC limit, we identify unique signatures of finite-momentum Cooper-pairing states that live longer than the laser pulse. They are controlled by a pair of THz laser pulses with well-defined relative phase (pulse pair). The pseudospin oscillators that describe the properties of these SC states are parametrically driven by both finite-momentum Cooper pairing and by time oscillations of the order-parameter relative phase. We show that such strong parametric driving leads to drastic changes in the THz-MDCS spectral shape from the predictions of third-order nonlinear susceptibility calculations. These spectral changes strongly depend on the interband-to-intraband interaction ratio and on the collective modes of the light-driven state. For negligible interband interaction, the spectra show a transition with increasing field, from traditional pump-probe, four-wave-mixing, and third-harmonic generation peaks determined by the laser frequency to sidebands determined by the excitations of the driven system. These sidebands emerge from difference-frequency Raman processes in the nonequilibrium SC state. For interband couplings weaker than the intraband pairing, we show that the Leggett phase collective mode leads to harmonic sidebands around the traditional pump-probe peaks. Additional Higgs collective mode peaks result from light-induced inversion-symmetry breaking in a thin-film geometry. For strong interband coupling, we find a transition from a nonequilibrium finite Cooper-pair momentum state characterized by hybrid-Higgs amplitude mode peaks in THz-MDCS spectra to a driven state identified experimentally by the emergence of Floquet-type sidebands at bi-Higgs frequencies. Those dominant bi-Higgs-frequency satellites are manifestations of a new order parameter relative phase collective mode that characterizes the nonequilibrium SC state. The predicted interaction- and field-dependent transitions in the spectral profile allow us to propose THz-MDCS experiments for quantum tomography of light-driven superconductivity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Cation and Anion Channelrhodopsins: Sequence Motifs and Taxonomic Distribution

Cation and anion channelrhodopsins (CCRs and ACRs, respectively) primarily from two algal species, Chlamydomonas reinhardtii and Guillardia theta, have become widely used as optogenetic tools to control cell membrane potential with light. We mined algal and other protist polynucleotide sequencing projects and metagenomic samples to identify 75 channelrhodopsin homologs from four channelrhodopsin families, including one revealed in dinoflagellates in this study. We carried out electrophysiological analysis of 33 natural channelrhodopsin variants from different phylogenetic lineages and 10 metagenomic homologs in search of sequence determinants of ion selectivity, photocurrent desensitization, and spectral tuning in channelrhodopsins. Our results show that association of a reduced number of glutamates near the conductance path with anion selectivity depends on a wider protein context, because prasinophyte homologs with a glutamate pattern identical to that in cryptophyte ACRs are cation selective. Desensitization is also broadly context dependent, as in one branch of stramenopile ACRs and their metagenomic homologs, its extent roughly correlates with phylogenetic relationship of their sequences. Regarding spectral tuning, we identified two prasinophyte CCRs with red-shifted spectra to 585 nm. They exhibit a third residue pattern in their retinal-binding pockets distinctly different from those of the only two types of red-shifted channelrhodopsins known (i.e., the CCR Chrimson and RubyACRs). In cryptophyte ACRs we identified three specific residue positions in the retinal-binding pocket that define the wavelength of their spectral maxima. Lastly, we found that dinoflagellate rhodopsins with a TCP motif in the third transmembrane helix and a metagenomic homolog exhibit channel activity. Channelrhodopsins are widely used in neuroscience and cardiology as research tools and are considered prospective therapeutics, but their natural diversity and mechanisms remain poorly characterized. Genomic and metagenomic sequencing projects are producing an ever-increasing wealth of data, whereas biophysical characterization of the encoded proteins lags behind. In this study, we used manual and automated patch clamp recording of representative members of four channelrhodopsin families, including a family in dinoflagellates that we report in this study. Our results contribute to a better understanding of molecular determinants of ionic selectivity, photocurrent desensitization, and spectral tuning in channelrhodopsins.

59 BASIC BIOLOGICAL SCIENCES↗

Toward inclusive observables with staggered quarks: the smeared $R$~ratio

Inclusive hadronic observables are ubiquitous in particle and nuclear physics. Computation of these observables using lattice QCD is challenging due the presence of a difficult inverse problem. As a stepping stone to more complicated observables, we report on progress to compute the smeared $R$~ratio with staggered quarks using the spectral reconstruction algorithm of Hansen, Lupo, and Tantalo. We compare staggered-quark results on two ensembles to domain-wall results on a single ensemble and to the Bernecker-Meyer parameterization. This work utilizes two ensembles generated by the MILC collaboration using highly improved staggered quarks and one ensemble generated by the RBC/UKQCD collaboration using domain-wall quarks. Possible strategies for controlling opposite-parity effects associated with staggered quarks are discussed.

Blum, Thomas↗

High-performance light-driven heterogeneous CO 2 catalysis with near-unity selectivity on metal phosphides

Akin to single-site homogeneous catalysis, a long sought-after goal is to achieve reaction site precision in heterogeneous catalysis for chemical control over patterns of activity, selectivity and stability. Herein, we report on metal phosphides as a class of material capable of realizing these attributes and unlock their potential in solar-driven CO 2 hydrogenation. Selected as an archetype, Ni 12 P 5 affords a structure based upon highly dispersed nickel nanoclusters integrated into a phosphorus lattice that harvest light intensely across the entire solar spectral range. Motivated by its panchromatic absorption and unique linearly bonded nickel-carbonyl-dominated reaction route, Ni 12 P 5 is found to be a photothermal catalyst for the reverse water gas shift reaction, offering a CO production rate of 960 ± 12 mmol g cat –1 h –1 , near 100% selectivity and long-term stability. Successful extension of this idea to Co2P analogs implies that metal phosphide materials are poised as a universal platform for high-rate and highly selective photothermal CO 2 catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-temperature Majorana fermions in magnet-superconductor hybrid systems

Magnet-superconductor hybrid (MSH) structures represent one of the most promising platforms to realize, control, and manipulate Majorana modes using scanning tunneling methods. By depositing either chains or islands of magnetic atoms on the surface of a conventional, elemental superconductor such as Pb or Re, topological superconducting phases can emerge. They feature either localized Majorana bound states at the chain ends or dispersing chiral Majorana modes at the island's boundary. However, some of these experiments have not reached the spectral resolution to clearly distinguish between topological Majorana and trivial Shiba states due to very small superconducting gap sizes and experiments performed at sub-Kelvin temperatures. Here we consider superconducting substrates with unconventional spin-singlet pairing, including high-temperature d -wave and extended s -wave superconductors. We derive topological phase diagrams and compute edge states for cylinder and island geometries and discuss their properties. Several time-reversal invariant topological superconducting phases of the Zhang-Kane-Mele type are found and discussed. Addiotnally, we review one-dimensional MSH structures and show that parameters to realize topologically nontrivial magnetic chains embedded into a larger, two-dimensional substrate differ from the purely one-dimensional case. Quite generally we find that unconventional superconducting substrates work as well as the conventional s -wave substrates to realize topological phases. In particular, iron-based pnictide and chalcogenide superconductors are the most promising class of substrates for future high-temperature MSH systems.

36 MATERIALS SCIENCE↗

Reduced Energetic Disorders in Dion–Jacobson Perovskites for Efficient and Spectral Stable Blue LEDs

Metal halide perovskites have witnessed great success in green, red, and near-infrared light-emitting diodes (LEDs), yet blue LEDs still lag behind. Reducing undesired energetic disorders – broad n -phases and halide segregation – is considered as the most critical strategy to further improve the performances. Here, the study reports a newly designed and synthesized di-ammonium ligand with rigid π -conjugated rings and additional methyl groups to construct Dion–Jacobson (DJ) structure. Augmented coordination from the extra ammonium site and increased effective bulkiness from methyl groups lead to better distribution control over conventional mono-ammonium ligands. This enhances the radiative recombination of blue emissions in the film with homogeneous energy landscape and improved surface morphology, as evidenced by a series of imaging and mapping techniques. As a result, it demonstrates DJ perovskite LEDs (PeLEDs) with peak external quantum efficiencies of ≈4% at 484 nm and ≈11% at 494 nm, which are among the top reported for pure DJ phase-based PeLEDs in the corresponding wavelength regions. The results deepen the understanding of regulating energetic disorders in perovskite materials via molecular engineering.

36 MATERIALS SCIENCE↗

Broadband THz Modulation via Solid–State Organic Electrochemical Devices

The sub-Terahertz and Terahertz bands play a critical role in next-generation wireless communication and sensing technologies, thanks to the large amount of available bandwidth in this spectral regime. While long-wavelength (microwave to mm-Wave) and short-wavelength (near-infrared to ultraviolet) devices are well-established and studied, the sub-THz to THz regime remains relatively underexplored and underutilized. Traditional approaches used in the aforementioned spectral regions are more difficult to replicate in the THz band, leading to the need for the development of novel devices and structures that can manipulate THz radiation effectively. Herein a novel organic, solid-state electrochemical device is presented, capable of achieving modulation depths of over 90% from ≈500 nm of a conducting polymer that switches conductivity over a large dynamic range upon application of an electronically controllable external bias. The stability of such devices under long-term, repeated voltage switching, as well as continuous biasing at a single voltage, is also explored. Switching stabilities and long-term bias stabilities are achieved over two days for both use cases. Additionally, both depletion mode (always “ON”) and accumulation mode (always “OFF”) operation are demonstrated. These results suggest applications of organic electrochemical THz modulators in large area and flexible implementations.

36 MATERIALS SCIENCE↗

Appearance versus disappearance of broad absorption line troughs in quasars

ABSTRACT We present a new set of 84 broad absorption line (BAL) quasars (1.7 < zem < 4.4) exhibiting an appearance of C iv BAL troughs over 0.3–4.8 rest-frame years by comparing the Sloan Digital Sky Survey Data Release (SDSSDR)-7, SDSSDR-12, and SDSSDR-14 quasar catalogues. We contrast the nature of BAL variability in this appearing BAL quasar sample with a disappearing BAL quasar sample studied in the literature by comparing the quasar’s intrinsic, BAL trough, and continuum parameters between the two samples. We find that appearing BAL quasars have relatively higher redshift and smaller probed time-scales as compared to the disappearing BAL quasars. To mitigate the effect of any redshift bias, we created control samples of appearing and disappearing BAL quasars that have similar redshift distribution. We find that the appearing BAL quasars are relatively brighter and have shallower and wider BAL troughs compared to the disappearing BAL sample. The distribution of quasar continuum variability parameters between the two samples is clearly separated, with the appearance of the BAL troughs being accompanied by the dimming of the continuum and vice versa. Spectral index variations in the two samples also point to the anticorrelation between the BAL trough and continuum variations consistent with the ‘bluer when brighter’ trend in quasars. We show that the intrinsic dust model is less likely to be a favourable scenario in explaining BAL appearance/disappearance. Our analysis suggests that the extreme variations of BAL troughs like BAL appearance/disappearance are mainly driven by changes in the ionization conditions of the absorbing gas.

Mishra, Sapna↗

Etching-Chemistry-Driven Ruthenium Doping on Ti 3 C 2 T x MXene for Optimizing Electrochemical Performance

We demonstrate that the etching chemistry used during MXene synthesis from Ti 3 AlC 2 MAX phase significantly influences surface functionalization and structural vacancies, which in turn affect ruthenium (Ru) ion interactions. Using hydrofluoric acid (HF) and ammonium bifluoride (NH 4 HF 2 ) as etchants, we obtained MXene surfaces with distinct functional groups and Ti vacancies that impact Ru ion interactions and electrochemical performance. Both MXene variants (labeled MX(H) and MX(N), respectively) exhibited negative zeta potentials in their pristine state, but upon the addition of Ru the zeta potential for MX(H) reached 12.9 mV while that for MX(N) remained negative at −6.4 mV. This adsorption resulted in a 14.4-fold increase in the specific capacitance of MX(H)/Ru compared to pristine MX(H), whereas MX(N)/Ru exhibited only a 4.4-fold increase over its pristine counterpart. X-ray diffraction analysis identified the formation of ammonium titanium oxide fluoride, (NH 4 ) 3 TiOF 5 , on MX(N), which likely contributed to its reduced Ru adsorption. X-ray photoelectron spectroscopy suggested the presence of Ti vacancies in both MXene variants; however, their behavior toward Ru accommodation differed markedly, with MX(H) showing the most obvious shift in the Ti 2p peak in the XPS survey spectrum, while MX(N) showed the most obvious shift in the C 1s peak. Electron paramagnetic resonance spectroscopy further demonstrated a distinct alteration in the spectral signatures of MX(H) upon Ru addition, in contrast to the negligible changes in MX(N), indicating effective passivation of the Ti defect sites in MX(H) via vacancy-assisted Ru doping. Cyclic voltammetry showed that Ru-incorporated MX(H) nanocomposites exhibit more efficient redox-active sites, as reflected in their higher capacitance values. These findings highlight the pivotal role of MXene surface chemistry in controlling cation adsorption, providing valuable insights for the rational design of high-performance electrodes.

2D surface engineering↗

Strain-Induced Trapping of Indirect Excitons in MoSe 2 /WSe 2 Heterostructures

Understanding and control of excitons in transition metal dichalcogenide (TMD) materials are essential for the exploration of the rich many-body physics in TMDs and their applications in photonic and optoelectronic devices. Local strain modulation has been utilized as an effective approach for creating potential traps and localizing intralayer excitons in TMD monolayers. Here, we investigate the effect of strains on indirect excitons in TMD heterostructures. The emergence of narrow spectral peaks from the strained sites together with their drastically reduced lifetimes indicates the formation of potential traps in the heterostructures and the trapping of indirect excitons in them. The absence of photon-antibunching from these trapped indirect excitons further reveals their weak localization in the potential traps. Here, our study indicates that, compared to the case of intralayer excitons, narrower potential traps are required for obtaining highly localized indirect excitons due to their unique properties. These findings have important implications for creating long-wavelength quantum emitters in TMD heterostructures and the exploration of indirect exciton condensation and motion in TMDs.

36 MATERIALS SCIENCE↗

Enhancing Graphene Plasmonic Device Performance via its Dielectric Environment

Graphene plasmons provide a compelling avenue toward chip-scale dynamic tuning of infrared light. Dynamic tunability emerges through controlled alterations in the optical properties of the system defining graphene’s plasmonic dispersion. Typically, electrostatic induced alterations of the carrier concentration in graphene working in conjunction with mobility have been considered the primary factors dictating plasmonic tunability. We find here that the surrounding dielectric environment also plays a primary role, dictating not just the energy of the graphene plasmon but so too the magnitude of its tuning and spectral width. To arrive at this conclusion, poles in the imaginary component of the reflection coefficient are used to efficiently survey the effect of the surrounding dielectric on the tuning of the graphene plasmon. By investigating several common polar materials, optical phonons (i.e., the Reststrahlen band) of the dielectric substrate are shown to appreciably affect not only the plasmon’s spectral location but its tunability, and its resonance shape as well. In particular, tunability is maximized when the resonances are spectrally distant from the Reststrahlen band, whereas sharp resonances (i.e., high-Q) are achievable at the band’s edge. Overall, these observations both underscore the necessity of viewing the dielectric environment in aggregate when considering the plasmonic response derived from two-dimensional materials and provide heuristics to design dynamically tunable graphene-based infrared devices.

36 MATERIALS SCIENCE↗