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DOE OSTI2020

Lightwave terahertz quantum manipulation of nonequilibrium superconductor phases and their collective modes

In this work, we present a gauge-invariant density matrix description of nonequilibrium superconductor (SC) states with spatial and temporal correlations driven by intense terahertz (THz) lightwaves. We derive superconductor Bloch-Maxwell equations of motion that extend Anderson pseudospin models to include the Cooper pair center-of-mass motion and electromagnetic propagation effects. We thus describe quantum control of dynamical phases, collective modes, quasiparticle coherence, and high nonlinearities during cycles of carrier wave oscillations, which relates to our recent experiments. Coherent photogeneration of a nonlinear supercurrent with a dc component, achieved via condensate acceleration by an effective lightwave field, dynamically breaks the equilibrium inversion symmetry. Experimental signatures include high harmonic light emission at equilibrium-symmetry-forbidden frequencies, Rabi-Higgs collective modes and quasiparticle coherence, and nonequilibrium moving condensate states tuned by few-cycle THz fields. We use such lightwaves as an oscillating accelerating force that drives strong nonlinearities and anisotropic quasiparticle populations to control and amplify different classes of collective modes, e.g., damped oscillations, persistent oscillations, and overdamped dynamics via Rabi flopping. Recent phase-coherent nonlinear spectroscopy experiments can be modeled by solving the full nonlinear quantum dynamics including self-consistent light-matter coupling.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Examining Cloud Feedback Components in the Simple Cloud-Resolving E3SM Atmosphere Model (SCREAM)

Cloud feedback remains the main source of uncertainty in climate sensitivity estimated by global climate models (GCMs), largely because subgrid cloud responses are parameterized in GCMs due to their coarse resolution. Here, this study examines cloud feedback in the global 3.25-km Simple Cloud-Resolving Energy Exascale Earth System Model (E3SM) Atmosphere Model (SCREAM 3 km) through a pair of 1-yr atmosphere-only simulations with control and +4-K sea surface temperature perturbations. SCREAM 3 km produces a positive cloud feedback that falls within but at the upper end of the range of Coupled Model Intercomparison Project phase 5 (CMIP5) and CMIP phase 6 (CMIP6) models and expert judgment. The positive cloud feedback arises from positive contributions from both high- and low-level clouds, with increases in high-cloud altitude and decreases in low-cloud amount and optical depth playing key roles. The stronger-than-CMIP-average feedback is mainly attributable to the high-cloud altitude feedback, owing to cloud tops rising nearly isothermally in SCREAM 3 km. The positive low-cloud amount feedback is weaker in SCREAM than in GCMs because estimated inversion strength (EIS) increases more dramatically with warming. A coarser 12-km resolution version of SCREAM exhibits a weaker positive cloud feedback than SCREAM 3 km, mainly because its low-cloud-radiative flux is more sensitive to EIS, leading to a stronger negative low-cloud amount feedback. With this process-level assessment of cloud feedback, this study reveals where SCREAM aligns with and diverges from conventional GCMs and expert assessment, providing insights to inform further model improvement and future expert assessment.

Cloud radiative effects↗

DOE OSTI2022

In-Operando XRD Study of the Effects of Water Vapor on Phase Formation in LSM/YSZ SOFC Cathodes

Here, in-operando XRD was conducted on anode supported SOFC button cells with LSM-YSZ cathodes operated at varying cathode air compositions under constant current conditions for over 1000 h. 1-hour XRD scans were continuously collected throughout the entire operation duration. By taking the sum of measured intensities from all of the collected patterns, the resulting cumulative XRD count times allowed the identification of minor phases present at concentrations as low as <0.1 wt%. In dry air with no contaminants, the cathode exhibited improving power output during the first couple of hundred hours, followed by stable operation. The effect of 3% H 2 O + 12% CO 2 on the LSM-YSZ cathode was very similar to the effect of 3% H 2 O alone, exhibiting performance degradation. Increasing contaminants in the cathode air were found to decrease the performance of the cells. In-operando XRD discovered an increase in MnO concentration and decrease in La 2 O 3 . A gradual expansion of the LSM lattice resulting from loss of Sr or O was discovered in the LSM/YSZ cathodes tested in humid cathode air. The inverse relationship between the unit cell volume and operating voltage suggests a possible correlation between Sr segregation and performance degradation in the LSM/YSZ cathodes.

25 ENERGY STORAGE↗

DOE OSTI2021

Observable proton decay in flipped SU(5)

We explore proton decay in a class of realistic supersymmetric flipped SU(5) models supplemented by a U(1) R symmetry which plays an essential role in implementing hybrid inflation. Two distinct neutrino mass models, based on inverse seesaw and type I seesaw, are identified, with the latter arising from the breaking of U(1) R by nonrenormalizable superpotential terms. Depending on the neutrino mass model an appropriate set of intermediate scale color triplets from the Higgs superfields play a key role in proton decay channels that include p → (e + , μ + ) π 0 , p → (e + , μ + ) K 0 , p → $\bar v$π + , and p → $\bar v$K + . We identify regions of the parameter space that yield proton lifetime estimates which are testable at Hyper-Kamiokande and other next generation experiments. We discuss how gauge coupling unification in the presence of intermediate scale particles is realized, and a Z 4 symmetry is utilized to show how such intermediate scales can arise in flipped SU(5). Finally, we compare our predictions for proton decay with previous work based on SU(5) and flipped SU(5).

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Strong electron-phonon coupling driven pseudogap modulation and density-wave fluctuations in a correlated polar metal

Abstract There is tremendous interest in employing collective excitations of the lattice, spin, charge, and orbitals to tune strongly correlated electronic phenomena. We report such an effect in a ruthenate, Ca 3 Ru 2 O 7 , where two phonons with strong electron-phonon coupling modulate the electronic pseudogap as well as mediate charge and spin density wave fluctuations. Combining temperature-dependent Raman spectroscopy with density functional theory reveals two phonons, B 2 P and B 2 M , that are strongly coupled to electrons and whose scattering intensities respectively dominate in the pseudogap versus the metallic phases. The B 2 P squeezes the octahedra along the out of plane c -axis, while the B 2 M elongates it, thus modulating the Ru 4d orbital splitting and the bandwidth of the in-plane electron hopping; Thus, B 2 P opens the pseudogap, while B 2 M closes it. Moreover, the B 2 phonons mediate incoherent charge and spin density wave fluctuations, as evidenced by changes in the background electronic Raman scattering that exhibit unique symmetry signatures. The polar order breaks inversion symmetry, enabling infrared activity of these phonons, paving the way for coherent light-driven control of electronic transport.

36 MATERIALS SCIENCE↗

NASA NTRS1987

Single-state selection system for hydrogen masers

The design and operation of a single-state selection system based on the adiabatic fast-passage technique for atomic state inversion is described. The system uses a variable-pitch dc solenoid and orthogonal four-wire RF coil to create the state-changing magnetic fields, and a half-wavelength state selection magnet to remove the inverted state atoms from the hydrogen beam. The system's performance was determined by measuring maser power as a function of line Q. The system removes more than 85 percent of undesired atoms from the beam. The potential effects of improvements in the maser on its frequency stability have been calculated. The use of single-state selection combined with increased RF coupling to the cavity and increased storage bulb collimation offers the possibility of frequency stability in the 10 to the -17th regime over intervals on the order of 60,000 s.

Mattison, Edward M.↗

DOE OSTI2024

Monitoring spatiotemporal evolution of fractures during hydraulic stimulations at the first EGS collab testbed using anisotropic elastic-waveform inversion

The EGS Collab project acquired continuous active-source seismic monitoring (CASSM) data before, during, and after hydraulic stimulations at the first testbed at the depth of 4850 ft (1478 m) at the Sanford Underground Research Facility in Lead, South Dakota, for monitoring fracture creation and evolution. CASSM acquisition was conducted using 24 hydrophones, 18 accelerometers, and 17 piezoelectric sources within four fracture-parallel wells and two orthogonal wells. 3D anisotropic traveltime tomography and anisotropic elastic-waveform inversion of the campaign cross-borehole seismic data show that the rock within the stimulation region is a heterogeneous horizontal transverse isotropic medium. Here we use these inversion results as the initial models and apply 3D anisotropic first-arrival traveltime tomography and 3D anisotropic elastic-waveform inversion to the CASSM data acquired after each stimulation in May, 2018 and December, 2018. We observe the spatiotemporal evolution of seismic velocities and anisotropic parameters caused by hydraulic fracture stimulations, showing the regions of rock alternation caused by hydraulic fracture stimulation.

15 GEOTHERMAL ENERGY↗

DOE OSTI2020

Singlet fission

Singlet fission (SF) is a process whereby a photo-excited singlet exciton spontaneously splits into lower energy triplet excitons. This process has been known to occur in select organic materials for over 50 years but in the past was viewed as a curiosity and not as a problem worthy of focused attention. Over the past decade, this viewpoint has changed as the promising use of SF to improve photovoltaic efficiency has spurred vast activity, which has revealed the richness of the phenomenon. Currently, our understanding of the role played by various bright and dark states and their couplings to vibrations and to each other and by chemical composition and packing, among other factors, has enabled a large increase in the number of viable SF systems as well as a far deeper understanding of the process itself. These advances have allowed for the demonstration of proof-of-concept increases in the solar cell efficiency via the use of SF materials in simple tandem cells and as sensitizers in conjunction with conventional photovoltaics. Indeed, concepts surrounding the field have now invaded other fields, with a prominent example being the use of photon upconversion associated with triplet–triplet fusion (the inverse process to SF) in organic chemistry and photocatalysis. The 23 research articles in this special topic showcase recent cutting-edge advances in the field and highlight the diverse new directions being explored in the field of SF.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Fermiology and transport properties of the candidate topological crystalline insulator SrAg 4 ⁢Sb 2

Compared to time-reversal symmetry-protected ℤ 2 topological insulators and Dirac/Weyl semimetals, there are significantly fewer candidates for topological crystalline insulators. SrAg 4 ⁢Sb 2 is predicted to exhibit topological crystalline insulator behavior when considering spin-orbit coupling. In this study, we systematically investigate single crystals of SrAg 4 ⁢Sb 2 using electrical transport and magnetic torque measurements, along with first-principles calculations. Our transport data reveals its compensated semimetal nature with a magnetoresistance up to around 700% at 2 K and 9 T. Analysis of de Haas–van Alphen oscillations uncovers a Fermi surface consisting of three distinct Fermi pockets with light effective masses. Comparison between the three-dimensional fermiology obtained from our oscillation data and the first-principles calculations demonstrates excellent agreement. This confirms the accuracy of the calculations, which indicate a band inversion centered at the 𝑇 point and identify the existence of nontrivial tube and needle hole Fermi pockets at Γ, alongside one trivial diamond electron pocket at the 𝐹 point in the Brillouin zone. Furthermore, symmetry and topology analysis results in two potential sets of topological invariants, suggesting the emergence of two-dimensional gapless Dirac surface states either on the 𝑎⁢𝑏 planes or on both the 𝑎⁢𝑏 planes and mirror planes, protected by crystal symmetries. Therefore, SrAg 4 ⁢Sb 2 emerges as a promising candidate topological crystalline insulator.

36 MATERIALS SCIENCE↗

DOE OSTI2023

β + Gamow-Teller Strengths from Unstable 14 O via the (d, 2 He) Reaction in Inverse Kinematics

For the first time, the (d, 2 He) reaction was successfully used in inverse kinematics to extract the Gamow-Teller transition strength in the β + direction from an unstable nucleus. The new technique was made possible by the use of an active-target time-projection chamber and a magnetic spectrometer, and opens a path to addressing a range of scientific challenges, including in astrophysics and neutrino physics. Here, in this Letter, the nucleus studied was 14 O, and the Gamow-Teller transition strength to 14 N was extracted up to an excitation energy of 22 MeV. The data were compared to shell-model and state-of-the-art coupled-cluster calculations. Shell-model calculations reproduce the measured Gamow-Teller strength distribution up to about 15 MeV reasonably well, after the application of a phenomenological quenching factor. In a significant step forward to better understand this quenching, the coupled-cluster calculation reproduces the full strength distribution well without such quenching, owing to the large model space, the inclusion of strong correlations, and the coupling of the weak interaction to two nucleons through two-body currents.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Diurnal evolution of non-precipitating marine stratocumuli in a large-eddy simulation ensemble

Abstract. We explore the cloud system evolution of non-precipitating marine stratocumuli with a focus on the impacts of the diurnal cycle and free-tropospheric (FT) humidity based on an ensemble of 244 large-eddy simulations generated by perturbing initial thermodynamic profiles and aerosol conditions. Cases are categorized based on their degree of decoupling and the cloud liquid water path (LWPc, based on model columns with cloud optical depths greater than one). A budget analysis method is proposed to analyze the evolution of cloud water in both coupled and decoupled boundary layers. More coupled clouds start with a relatively low LWPc and cloud fraction (fc) but experience the least decrease in LWPc and fc during the daytime. More decoupled clouds undergo greater daytime reduction in LWPc and fc, especially those with higher LWPc at sunrise because they suffer from faster weakening of net radiative cooling. During the nighttime, a positive correlation between FT humidity and the LWPc emerges, consistent with higher FT humidity reducing both radiative cooling and the humidity jump, both of which reduce entrainment and increase LWPc. The LWPc is more likely to decrease during the nighttime for a larger LWPc and greater inversion base height (zi), conditions under which entrainment dominates as turbulence develops. In the morning, the rate of the LWPc reduction depends on the LWPc at sunrise, zi, and the degree of decoupling, with distinct contributions from subsidence and radiation.

Chen, Yao-Sheng (ORCID:0000000208354132)↗

DOE OSTI2020

Strong spin–orbit quenching via the product Jahn–Teller effect in neutral group IV qubits in diamond

Abstract Artificial atom qubits in diamond have emerged as leading candidates for a range of solid-state quantum systems, from quantum sensors to repeater nodes in memory-enhanced quantum communication. Inversion-symmetric group IV vacancy centers, comprised of Si, Ge, Sn, and Pb dopants, hold particular promise as their neutrally charged electronic configuration results in a ground-state spin triplet, enabling long spin coherence above cryogenic temperatures. However, despite the tremendous interest in these defects, a theoretical understanding of the electronic and spin structure of these centers remains elusive. In this context, we predict the ground-state and excited-state properties of the neutral group IV color centers from first principles. We capture the product Jahn–Teller effect found in the excited state manifold to second order in electron–phonon coupling, and present a nonperturbative treatment of the effect of spin–orbit coupling. Importantly, we find that spin–orbit splitting is strongly quenched due to the dominant Jahn–Teller effect, with the lowest optically-active 3 E u state weakly split into m s -resolved states. The predicted complex vibronic spectra of the neutral group IV color centers are essential for their experimental identification and have key implications for use of these systems in quantum information science.

Materials Science↗

DOE OSTI2022

Large bilinear magnetoresistance from Rashba spin-splitting on the surface of a topological insulator

In addition to the topologically protected linear dispersion, a band-bending-confined two-dimensional electron gas with tunable Rashba spin-splitting (RSS) was found to coexist with the topological surface states on the surface of topological insulators (TIs). Here, in this paper, we report the observation of large bilinear magnetoresistance (BMR) in Bi 2 ⁢Se 3 films decorated with transition-metal atoms. The magnitude of the BMR sensitively depends on the type and amount of atoms deposited, with a maximum achieved value close to those of strong Rashba semiconductors. Our first-principles calculations reproduce the quantum well states and reveal sizable RSS in all Bi 2 ⁢Se 3 heterostructures with broken inversion symmetry. Our results show that charge-spin interconversion through RSS states in TIs can be fine tuned through surface atom deposition and easily detected via BMR for potential spintronic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Relating storm-snow avalanche instabilities to data collected from the Differential Emissivity Imaging Disdrometer (DEID)

Storm-snow avalanches are challenging to forecast due to complex alpine terrain and during rapidly changing weather conditions. They can result in loss of lives and significant economic impact. We describe how a new device that continuously measures with high-frequency snowflake mass, size, density, and type, the Differential Emissivity Imaging Disdrometer (DEID), and show how the DEID can be used to aid avalanche forecasting when coupled with a storm-snow stability model. DEID measurements of snow accumulation, snow water equivalent (SWE), and snow density obtained during seventeen storms taken at the mid-Collins Snow-Study Plot at Alta Ski Area in Utah's Central Wasatch mountain range during winter 2020–2021 show excellent agreement with infrequent manual measurements. Additionally, two new variables, the Shape Density Index (SDI) and Complexity, are proposed and used to classify snowflake habit and estimate storm-snow shear strength. We illustrate how these DEID-derived data can be used to identify layers of concern in the storm snow such as density inversions, in real-time without digging snow pits. Furthermore, the DEID-data are used to run four variations of the SNOw Slope Stability model (SNOSS) for the storms investigated. The results are evaluated with data collected from tilt-board tests, infrasound measurements, and visual observations of avalanches. For a total fourteen storms analyzed, the DEID-driven SNOSS-modeled minimum stability index predicts the general stability of the storm-snow as indicated by observed avalanches, both natural and of unknown cause. Finally, the results provide a promising approach for nowcasting instabilities within storm-snow layers with a single instrument.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Effects of filling, strain, and electric field on the Néel vector in antiferromagnetic CrSb

CrSb is a layered antiferromagnet (AFM) with perpendicular magnetic anisotropy, a high Néel temperature, and large spin-orbit coupling (SOC), which makes it interesting for AFM spintronic applications. To elucidate the various mechanisms of Néel vector control, the effects of strain, band filling, and electric field on the magnetic anisotropy energy (MAE) of bulk and thin-film CrSb are determined and analyzed using density functional theory. The MAE of the bulk crystal is large (1.2 meV per unit cell). Due to the significant ionic nature of the Cr-Sb bond, finite slabs are strongly affected by end termination. Truncation of the bulk crystal to a thin film with one surface terminated with Cr and the other surface terminated with Sb breaks inversion symmetry, creates a large charge dipole and average electric field across the film, and breaks spin degeneracy, such that the thin film becomes a ferrimagnet. The MAE is reduced such that its sign can be switched with realistic strain, and the large SOC gives rise to an intrinsic voltage controlled magnetic anisotropy. A slab terminated on both faces with Cr remains a compensated AFM, but with the compensation occurring nonlocally between mirror-symmetric Cr pairs. In-plane alignment of the moments is preferred, the magnitude of the MAE remains large, similar to that of the bulk, and it is relatively insensitive to filling.

36 MATERIALS SCIENCE↗

NASA NTRS1999

Coherent Pump-Probe Interactions and Terahertz Intersubband Gain in Semiconductor Quantum Wells

In recent years there has been considerable interest in intersubband-transition-based infrared semiconductor quantum well (QW) lasers because of their potential applications. In the mid-infrared range, both electrically-injected quantum cascade lasers [1] and optically-pumped multiple QW lasers [2] have been experimentally realized. In these studies, optical gain is due to population inversion between the lasing subbands. It was also proposed that stimulated Raman scattering in QW systems can produce net infrared optical gain [3j. In such a nonlinear optical scheme, the appearance of optical gain that may lead to intersubband Raman lasers does not rely on the population inversion. Since, in tile resonant Raman process (Raman gain is the largest in this case), the pump field induces population redistribution among subbands in the QW s ystem, it seems that a realistic estimate of the optical gain has to include this effect. Perturbative calculations used in the previous work [3] may overestimate the Raman gain. In this paper we present a nonperturbative calculation of terahertz gain of optically-pumped semiconductor step quantum wells. Limiting optical transitions within the conduction band of QW, we solve the pump-field-induced nonequilibrium distribution function for each subband of the QW system from a set of coupled rate equations. Both intrasubband and intersubband relaxation processes in the quantum well system are included. Taking into account the coherent interactions between pump and THz (signal) waves, we we derive the susceptibility of the QW system for the THz field. For a GaAs/AlGaAs step QW, we calculate the Thz gain spectrum for different pump frequencies and intensities. Under moderately strong pumping (approximately 0.3 MW/sq cm), a significant THz gain (approximately 300/m) is predicted. It is also shown that the coherent wave interactions (resonant stimulated Raman processes) contribute significantly to the THz gain.

Liu, Ansheng↗

NASA NTRS2007

Carbon Nanotubes for Space Photovoltaic Applications

Carbon nanotubes (CNTs) can be envisioned as an individual graphene sheet rolled into a seamless cylinder (single-walled, SWNT), or concentric sheets as in the case of a multi-walled carbon nanotube (MWNT) (1). The role-up vector will determine the hexagonal arrangement and "chirality" of the graphene sheet, which will establish the nanotube to be metallic or semiconducting. The optoelectronic properties will depend directly on this chiral angle and the diameter of the SWNT, with semiconductor types exhibiting a band gap energy (2). Characteristic of MWNTs are the concentric graphene layers spaced 0.34 nm apart, with diameters from 10-200 nm and lengths up to hundreds of microns (2). In the case of SWNTs, the diameters range from 0.4 - 2 nm and lengths have been reported up to 1.5 cm (3). SWNTs have the distinguishable property of "bundling" together due to van der Waal's attractions to form "ropes." A comparison of these different structural types is shown in Figure 1. The use of SWNTS in space photovoltaic (PV) applications is attractive for a variety of reasons. Carbon nanotubes as a class of materials exhibit unprecedented optical, electrical, mechanical properties, with the added benefit of being nanoscale in size which fosters ideal interaction in nanomaterial-based devices like polymeric solar cells. The optical bandgap of semiconducting SWNTs can be varied from approx. 0.4 - 1.5 eV, with this property being inversely proportional to the nanotube diameter. Recent work at GE Global Research has shown where a single nanotube device can behave as an "ideal" pn diode (5). The SWNT was bridged over a SiO2 channel between Mo contacts and exhibited an ideality factor of 1, based on a fit of the current-voltage data using the diode equation. The measured PV efficiency under a 0.8 eV monochromatic illumination showed a power conversion efficiency of 0.2 %. However, the projected efficiency of these junctions is estimated to be > 5 %, especially when one considers the enhanced absorption (from nanotubes whose bandgap is tailored to illumination) and electromagnetic coupling in a network of nanotubes.

Efstathiadis, Harry↗

DOE OSTI2023

Probing Majorana wavefunctions in Kitaev honeycomb spin liquids with second-order two-dimensional spectroscopy

Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response $\chi^{(2)}_{yzx}(\omega_1, \omega_2)$ when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by $\mathbb{Z}_2$ flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.

Qiang, Yihua↗