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At least 1,711 records · Page 95
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Anisotropic time-domain electronic response in cuprates driven by midinfrared pulses

Superconductivity in the cuprates is characterized by an anisotropic electronic gap of d -wave symmetry. The aim of this study is to understand how this anisotropy affects the nonequilibrium electronic response of high-T c superconductors. Here we use a polarization selective time domain experiment to address the dynamics of electronic excitation of different symmetry in optimally doped Bi 2 Sr 2 Y 0.08 Ca 0.92 Cu 2 O 8+δ and measure the nodal and antinodal nonequilibrium response resulting from photoexcitations with ultrashort pulses with photon energy comparable to the superconducting gap. The response to long wavelength photoexcitation with pump polarization along the Cu-Cu axis of the sample is discussed with the support of an effective d-wave BCS model which suggests that such transient response could be ascribed to an increase of pair coherence in the antinodal region.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Rationally Engineered Vertically Aligned β ‐Ga 2− x W x O 3 Nanocomposites for Self‐Biased Solar‐Blind Ultraviolet Photodetectors with Ultrafast Response

Abstract With the astonishing advancement of present technology and increasing energy consumption, there is an ever‐increasing demand for energy‐efficient multifunctional sensors or transducers based on low‐cost, eco‐friendly material systems. In this context, self‐assembled vertically aligned β ‐Ga 2− x W x O 3 nanocomposite (GWO‐VAN) architecture‐assisted self‐biased solar‐blind UV photodetection on a silicon platform, which is the heart of traditional electronics is presented. Utilizing precisely controlled growth parameters, the formation of W‐enriched vertical β ‐Ga 2− x W x O 3 nanocolumns embedded into the W‐deficient β ‐Ga 2− x W x O 3 matrix is reached. Detailed structural and morphological analyses evidently confirm the presence of β ‐Ga 2− x W x O 3 nanocomposite with a high structural and chemical quality. Furthermore, absorption and photoluminescence spectroscopy explains photo‐absorption dynamics and the recombination through possible donor–acceptor energy states. The proposed GWO‐VAN framework facilitates evenly dispersed nanoregions with asymmetric donor energy state distribution and thus forms build‐in potential at the vertical β ‐Ga 2− x W x O 3 interfaces. As a result, the overall heterostructure evinces photovoltaic nature under the UV irradiation. A responsivity of ≈30 A/W is observed with an ultrafast response time (≈350 µs) under transient triggering conditions. Corresponding detectivity and external quantum efficiency are 7.9 × 10 12 Jones and 1.4 × 10 4 %, respectively. It is believed that, while this is the first report exploiting GWO‐VAN architecture to manifest self‐biased solar‐blind UV photodetection, the implication of the approach is enormous in designing electronics for extreme environment functionality and has immense potential to demonstrate drastic improvement in low‐cost UV photodetector technology.

Das, Debabrata↗
DOE OSTI2021

Photophysical properties of zero-dimensional perovskites studied by PBE0 and GW+BSE methods

Due to the exceptional photophysical properties and great potential applications in solid state lighting, zero-dimensional halide perovskites with broadband emitting have recently attracted much attention. In this work, to reveal the origin of the broadband absorption and emission spectra of 0D (C 4 N 2 H 14 Br) 4 SnBr x I 6-x (x = 3), the ground state and exciton dynamics properties have been studied by hybrid PBE0 functional and the GW+BSE method. Different self-trapped excitons (STEs) are obtained, and their emission energies by PBE0 are consistent well with experimental data. By considering the vibrational broadening of emission, our calculated full width at half maximum of emission accords well with the experiment. The absorption of free exciton and STEs is also calculated by considering the quasiparticle and excitonic effect. Our results show that these light-induced trapped states can be observed by experiments, as confirmed in other similar systems by the femtosecond transient absorption spectra.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Full information acquisition in piezoresponse force microscopy

The information flow from the tip-surface junction to the detector electronics during the piezoresponse force microscopy (PFM) imaging is explored using the recently developed general mode (G-mode) detection. Information-theory analysis suggests that G-mode PFM in the non-switching regime, close to the first resonance mode, contains a relatively small (100–150) number of components containing significant information. The first two primary components are similar to classical PFM images, suggesting that classical lock-in detection schemes provide high veracity information in this case. At the same time, a number of transient components exhibit contrast associated with surface topography, suggesting pathway to separate the two. The number of significant components increases considerably in the non-linear and switching regimes and approaching cantilever resonances, precluding the use of classical lock-in detection and necessitating the use of band excitation or G-mode detection schemes. The future prospects of full information imaging in scanning probe microscopy are discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2019

AT2018cow: A Luminous Millimeter Transient

We present detailed submillimeter- through centimeter-wave observations of the extraordinary extragalactic transient AT2018cow. The apparent characteristics—the high radio luminosity, the rise and long-lived emission plateau at millimeter bands, and the sub-relativistic velocity—have no precedent. A basic interpretation of the data suggests E(k) ≳ 4 X 10^(48) erg coupled to a fast but sub-relativistic (v ≈ 0.13c) shock in a dense (n(e) ≈ 3 X 10^(5) per cu. cm) medium. We find that the X-ray emission is not naturally explained by an extension of the radio-submm synchrotron spectrum, nor by inverse Compton scattering of the dominant blackbody UV/optical/IR photons by energetic electrons within the forward shock. By ∆t ≈ 20 days, the X-ray emission shows spectral softening and erratic inter-day variability. Taken together, we are led to invoke an additional source of X-ray emission: the central engine of the event. Regardless of the nature of this central engine, this source heralds a new class of energetic transients shocking a dense medium, which at early times are most readily observed at millimeter wavelengths

Anna Y. Q. Ho↗
DOE OSTI2025

Correlated solvent coordinates accelerate multi-donor proton-coupled electron transfer

The rate of charge transfer within a discrete donor–acceptor (D/A) pair is well-described by semi-classical electron transfer theory, but the effects of multiple equivalent redox sites remain less understood. We report a series of ground-state intramolecular proton-coupled electron transfer (PCET) complexes designed to isolate the effects of donor number, N, while holding geometry, coupling, and driving forces constant. The [Ru(L) 3−N (OH) N ] 2+ complexes incorporate one, two, or three identical phenolic electron donors linked to Ru through rigid phenanthroline bridges (OH = 2,4-di-tert-butyl-6-(1-methyl-1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl)phenol). Upon flash photolysis and oxidative quenching with methyl viologen (MV 2+ ), the transient Ru(III) oxidizes an appended phenol by PCET with the hydrogen-bonded imidazole nitrogen atom functioning as the base. The rate increased by 3.4-fold and 5.7-fold (1.7-fold and 1.9-fold after statistical correction) for two- and three-donor complexes compared to the single-donor system. The supra-statistical acceleration is attributed to a reduced effective outer sphere reorganization energy (λ m ) modeled by a partially shared solvent reaction coordinate, in which a subset of solvent dipoles is already oriented to stabilize charge from any donor. The final phenoxyl radical state is localized due to the transfer of a proton, and the recombination reaction with the viologen radical is not accelerated. These results demonstrate the effects of solvent dynamics on intramolecular PCET rates, offering a new strategy for the design of synthetic charge transfer systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Enhancement of carrier lifetimes in type-II quantum dot/quantum well hybrid structures

We investigate optical transitions and carrier dynamics in hybrid structures containing type-I GaAs/AlGaAs quantum wells (QWs) and type-II GaSb/AlGaAs quantum dots (QDs). We show that the optical recombination of photocreated electrons confined in the QWs with holes in the QDs and wetting layer can be modified according to the QW/QD spatial separation. In particular, for low spacer thicknesses, the QW optical emission can be suppressed due to the transference of holes from the QW to the GaSb layer, favoring the optical recombination of spatially separated carriers, which can be useful for optical memory and solar cell applications. Time-resolved photoluminescence (PL) measurements reveal non-exponential recombination dynamics. We demonstrate that the PL transients can only be quantitatively described by considering both linear and quadratic terms of the carrier density in the bimolecular recombination approximation for type-II semiconductor nanostructures. We extract long exciton lifetimes from 700 ns to 5 μs for QDs depending on the spacer layer thickness.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Formation mechanism of anodic titanium oxide in mixed electrolytes

Highlights: • Compact anodic titanium oxide (CATO) and anodic TiO{sub 2} nanotubes (ATNTs) were compared. • A distinct transform from CATO films into the porous ATNTs was observed firstly. • FESEM evidences for oxygen bubble mould effect were provided firstly. • Formation mechanisms for different titanium oxide films are confirmed consistent. - Abstract: The formation mechanism of anodic TiO{sub 2} nanotubes (ATNTs) remains mysterious and complicated. Usually, ATNTs are fabricated in pure NH{sub 4}F electrolytes rather than mixed electrolytes and Ti anodizations are carried out under potentiostatic rather than galvanostatic conditions. In this work, anodizations under the potentiostatic and galvanostatic conditions are conducted. The formation processes of titanium oxide film in different mixed electrolytes are explored in detail. By changing the mass ratios of oxalic acid and ammonium fluoride, different kinds of anodic titanium oxide films are fabricated: the compact anodic titanium oxide (CATO) films, transient-state anodic titanium oxide films and porous films (ATNTs). A distinct transform from CATO films into ATNTs was observed. Cavities within oxide and hemispheric bottoms are found, confirming the presence of oxygen bubble mould. Based on the electronic current and ionic current model, a consistent formation mechanism for three kinds of anodic titanium oxide films in mixed electrolytes is proposed.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Positional Effects from σ-Bonded Platinum(II) on Intersystem Crossing Rates in Perylenediimide Complexes: Synthesis, Structures, and Photophysical Properties

In this research, the synthesis and photophysical properties of a series of new chromophores featuring Pt(II) σ-bonded to perylenediimide (PDI) cores are reported. A Pt(PPh 3 ) 2 X (X = Cl, Br) moiety was attached to PDI in either the ortho or the bay position (2- or 1-positions respectively) or a Pt(PPh 3 ) 2 subunit was used to bridge two bay positions (1- and 12-positions) forming a Pt(II) cyclometalate. Through a combination of steady-state and transient absorption and photoluminescence spectroscopy, the excited-state dynamics of these molecules were revealed, indicating that the Pt atom location on the PDI has a substantial impact on observed intersystem crossing (ISC) rates. The ISC time constants for the bay-substituted and cyclometalated PDIs are between 2.67 and 1.29 ns, respectively, determined by the singlet fluorescence decays from the initially populated singlet excited states. In the case of the ortho -substituted PDI, ISC to the triplet state occurs on the ultrafast time scale with a time constant of 345 fs, determined through ultrafast transient absorption spectroscopy. In all examples, the measured PDI-based fluorescence quantum yields quantitatively correlate with the measured ISC rates leaving little doubt that variation in the Pt(II) substitution position(s) markedly influence the resultant photophysics. Electronic structure calculations suggest differing amounts of metal-based contributions in the lowest excited states as a function of substitution position, supporting the trend of the observed ISC rates.

14 SOLAR ENERGY↗
DOE OSTI2017

Vibronically coherent ultrafast triplet-pair formation and subsequent thermally activated dissociation control efficient endothermic singlet fission

Singlet exciton fission (SF), the conversion of one spin-singlet exciton (S 1 ) into two spin-triplet excitons (T 1 ), could provide a means to overcome the Shockley-Queisser limit in photovoltaics. SF as measured by the decay of S 1 has been shown to occur efficiently and independently of temperature even when the energy of S1 is as much as 200 meV less than 2T 1 . Here, we study films of TIPS-tetracene using transient optical spectroscopy and show that the initial rise of the triplet pair state (TT) occurs in 300 fs, matched by rapid loss of S1 stimulated emission, and that this process is mediated by the strong coupling of electronic and vibrational degrees of freedom. This is followed by a slower 10 ps morphology-dependent phase of S1 decay and TT growth. Here we observe the TT to be thermally dissociated on 10-100 ns timescales to form free triplets. This provides a model for "temperature independent", efficient TT formation and thermally activated TT separation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Ultrafast vertical photoconductive intrinsic diamond switch with high current (17.1 A at 1 kV)

Here, this Letter reports on a vertical, bulk-conducting photoconductive semiconductor switch (PCSS) fabricated on an intrinsic Type IIa single-crystal diamond substrate. Under near-bandgap excitation at 225 nm with a 20 μ J pulse, a strong photocurrent response of 17.1 A at 1 kV DC bias magnitude is obtained by (i) tuning the optical trigger wavelength to the “matched-absorption” window (224–235 nm) near the band edge, where the optical penetration depth becomes comparable to the 500 μ m substrate thickness, and (ii) choosing the bias polarity ensuring electron-dominant conduction, given that electrons have a higher mobility than holes in diamond. The PCSS has an area-normalized responsivity of 54.2 mA W −1 cm −2 and an effective on-resistance of 8.48 Ω, with a fast 90%–10% transient fall time of 25 ns, attributed to carrier sweep-out. These results support vertical, bulk-conducting intrinsic diamond PCSS as a promising platform for high-power optical switching and provide new insight into intrinsic photoconductivity in diamond.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2015

Modeling and Analysis of Hybrid Pixel Detector Deficiencies for Scientific Applications

Semiconductor hybrid pixel detectors often consist of a pixellated sensor layer bump bonded to a matching pixelated readout integrated circuit (ROIC). The sensor can range from high resistivity Si to III-V materials, whereas a Si CMOS process is typically used to manufacture the ROIC. Independent, device physics and electronic design automation (EDA) tools are used to determine sensor characteristics and verify functional performance of ROICs respectively with significantly different solvers. Some physics solvers provide the capability of transferring data to the EDA tool. However, single pixel transient simulations are either not feasible due to convergence difficulties or are prohibitively long. A simplified sensor model, which includes a current pulse in parallel with detector equivalent capacitor, is often used; even then, spice type top-level (entire array) simulations range from days to weeks. In order to analyze detector deficiencies for a particular scientific application, accurately defined transient behavioral models of all the functional blocks are required. Furthermore, various simulations, such as transient, noise, Monte Carlo, inter-pixel effects, etc. of the entire array need to be performed within a reasonable time frame without trading off accuracy. The sensor and the analog front-end can be modeling using a real number modeling language, as complex mathematical functions or detailed data can be saved to text files, for further top-level digital simulations. Parasitically aware digital timing is extracted in a standard delay format (sdf) from the pixel digital back-end layout as well as the periphery of the ROIC. For any given input, detector level worst-case and best-case simulations are performed using a Verilog simulation environment to determine the output. Each top-level transient simulation takes no more than 10-15 minutes. The impact of changing key parameters such as sensor Poissonian shot noise, analog front-end bandwidth, jitter due to clock distribution etc. can be accurately analyzed to determine ROIC architectural viability and bottlenecks. Hence the impact of the detector parameters on the scientific application can be studied.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2018

Highly mobile charge-transfer excitons in two-dimensional WS 2 /tetracene heterostructures

Charge-transfer (CT) excitons at heterointerfaces play a critical role in light to electricity conversion using organic and nanostructured materials. However, how CT excitons migrate at these interfaces is poorly understood. We investigate the formation and transport of CT excitons in two-dimensional WS 2 /tetracene van der Waals heterostructures. Electron and hole transfer occurs on the time scale of a few picoseconds, and emission of interlayer CT excitons with a binding energy of ~0.3 eV has been observed. Transport of the CT excitons is directly measured by transient absorption microscopy, revealing coexistence of delocalized and localized states. Trapping-detrapping dynamics between the delocalized and localized states leads to stretched-exponential photoluminescence decay with an average lifetime of ~2 ns. The delocalized CT excitons are remarkably mobile with a diffusion constant of ~1 cm 2 s -1 . These highly mobile CT excitons could have important implications in achieving efficient charge separation.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Oxide Interfaces: emergent structure and dynamics

This Final Report describes the scientific accomplishments that have been achieved with support from grant DE-FG02-06ER46273 during the period 6/1/2012– 5/31/2016. The overall goals of this program were focused on the behavior of epitaxial oxide heterostructures at atomic length scales (Ångstroms), and correspondingly short time-scales (fs -ns). The results contributed fundamentally to one of the currently most active frontiers in condensed matter physics research, namely to better understand the intricate relationship between charge, lattice, orbital and spin degrees of freedom that are exhibited by complex oxide heterostructures. The findings also contributed towards an important technological goal which was to achieve a better basic understanding of structural and electronic correlations so that the unusual properties of complex oxides can be exploited for energy-critical applications. Specific research directions included: probing the microscopic behavior of epitaxial interfaces and buried layers; novel materials structures that emerge from ionic and electronic reconfiguration at epitaxial interfaces; ultrahigh-resolution mapping of the atomic structure of heterointerfaces using synchrotron-based x-ray surface scattering, including direct methods of phase retrieval; using ultrafast lasers to study the effects of transient strain on coherent manipulation of multi-ferroic order parameters; and investigating structural ordering and relaxation processes in real-time.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Grid-Connected Modular Soft-Switching Solid State Transformers (M-S4T)

The objective of this project is to develop and verify the concept of a flexible and modular soft-switching solid-state transformer (M-S4T) for direct grid-connected applications. The ability to directly connect power electronics converters to the medium voltage grid (4 kV – 13 kV), and to potentially replace the passive and bulky, but ubiquitous 60 hertz service transformer in the 25 kVA to 100 kVA range, with a more flexible and controllable device, has been regarded as the ‘holy grail’ in grid control. However, this has proven to be extremely difficult. This project has developed the solutions to several key challenges of the direct grid-connected power electronics and realized a 7.2 kV M-S4T prototype. First, a protection method to protect the M-S4T from the high voltages (110 kV for the 13 kV system) that occur on the grid due to transients and lightning strikes have been developed and experimentally verified. Second, the realization and the operation of the M-S4T based on high-voltage SiC devices (>3.3 kV) and a medium-frequency medium-voltage low-leakage transformer in a single-stage solid-state transformer with zero-voltage switching, low dv/dt, and low electromagnetic interference has been successfully demonstrated up to 7.5 kV peak. Third, an oil-cooling system and stable communication and distributed control system for converter module voltage sharing have been developed and experimentally verified. The developed M-S4T has realized a modular universal high-performance power conversion system. This conversion system is scalable to different voltage and power levels and adaptable to four-quadrant bidirectional operation. Moreover, the use of passive cooling techniques meets the equipment life requirements, and the lightning protection scheme fulfills the basic insulation level specifications for direct grid connection. Such power conversion system opens up near-term opportunities, including energy storage, solar PV, or electric vehicle charging with significant cost and footprint savings. In the longer term, the possibility of replacing the utility distribution transformer with an M-S4T will be transformative for future distribution grids with a compact footprint and full controllability to enable high renewable energy and storage penetration. In addition to the main project, this report expands on the Plus-Up projected including as part of the main award. This project developed and demonstrated the technology for autonomous collaborative inverters that can be connected in an ad hoc manner to the grid. The aim of the project was to: (1) evaluate the existing techniques for grid-connected inverters and find their limitations; (2) develop detailed requirements for grid-connected inverters in the modern grid with millions of active nodes; (3) design a unified control strategy that brings more autonomy and intelligence to grid-connected inverters, and addresses parts of the issues with the existing techniques. The proposed technique, called UniCon, enables inverters to 1) connect/disconnect to/from the grid in an ad hoc manner; (2) work based on local sensing. Slow communication could be used for a more optimized behavior; (3) work automatically in both grid-forming/grid-following mode; (4) handle large disturbances, e.g., big load step and fault, in an oscillation-free manner; (5) work collaboratively with other inverters in steady-state and during transients. UniCon can be implemented in the middle-level control; hence it is agnostic to the vendor and to the implementation of the inner voltage/current and protection loops. Furthermore, a new synchronization scheme, based on deep learning, was developed that can extract the grid voltage phase and amplitude in a stable manner. The method is cheap to implement can improve the dynamic performance of the grid-connected inverters during fast transients, e.g., fault. The proposed control scheme was validated by (1) MATLAB/Simulink; (2) hardware-in-the-loop results, and; (3) experimental results using three inverters that form a microgrid in a down-scaled feeder. Lastly, both the M-S4T and UniCon have achieved promising tangible paths to markets. In the case of the M-S4T, the underlying technology — the Soft Switching Solid State Transformer (S4T) developed at the Georgia Tech Center for Distributed Energy (GT-CDE) has been licensed by GridBlock from the Georgia Tech Research Corporation, and GridBlock has been working with manufacturing partner Jabil (one of the largest US-based contract manufacturers) and system integrator Power Secure (largest deployer of microgrids in the US with 4.7 GW under management), to meet the strong initial demand. Similarly, GridBlock has an exclusive license to the UniCon technology, developed under this award by GT-CDE. The UniCon provides an intermediate control layer that enables the implementation of the higher-level ‘transactive’ control commands for the system. The architecture of the system - slow communications with the cloud for system optimization and setpoints, and the use of locally measured quantities for real-time control, provide a very robust and secure way of implementing a real-time must-run grid that is also secure and stable. This is a brand-new functionality that is critical for the future grid and key to GridBlock’s business model.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2025

Design and validation of a nanosecond short-wave infrared streak camera using gaseous detonation experiments

A custom short-wave infrared (SWIR) galvanometric streak camera was developed to provide nanosecond- scale, time-resolved optical diagnostics. The system was designed as a compact, mechanically driven alternative to traditional tube-based streak cameras, using a galvanometer mirror and multiple-reflection optical path to achieve high temporal resolution while maintaining electronic synchronization for trigger sequencing. Temporal resolution achieved 139.5 ns/px, allowing direct conversion of image-slope gradients to physical wave velocities. The instrument was validated using hydrogen-oxygen-argon detonations within a modular detonation tube, capturing transient emission structures and post-detonation decay behavior with microsecond precision. Although signal levels in filtered configurations were limited by lens transmission and detector sensitivity, the system successfully resolved intensity rise and decay characteristics across 10-60 % argon mixtures. The observed trends demonstrate the feasibility of compact galvanometer-based streak systems for high-speed SWIR imaging in reactive environments!

42 ENGINEERING↗
NASA NTRS1976

Effects of 1- and 2-MeV electrons on photomultiplier tubes

Various types of photomultiplier tubes useful for space applications were irradiated with 1- and 2-MeV electrons at Van Allen radiation belt fluxes of 100,000 to 10 millions electrons/sq cm-sec. The increase in the dark current due to electron irradiation was observed at various bias voltages under worst-case conditions (no shielding). Results were presented in the form of dark current plotted against electron flux. All the tubes tested showed extremely large increases in dark current. Tube types 541A, 6217, 6199, and 6903 exhibited the largest increases under irradiation, whereas type 1P22 was affected the least. All the damage observed was transient. The luminescence produced in the optical window probably accounts for a large part of the dark-current increases, but there were some effects possibly due to direct irradiation of the photocathode and dynode chain.

Beatty, M. E., III↗
NASA NTRS1980

Radiation tolerance of boron doped dendritic web silicon solar cells

The potential of dendritic web silicon for giving radiation hard solar cells is compared with the float zone silicon material. Solar cells with n(+)-p-P(+) structure and approximately 15% (AMl) efficiency were subjected to 1 MeV electron irradiation. Radiation tolerance of web cell efficiency was found to be at least as good as that of the float zone silicon cell. A study of the annealing behavior of radiation-induced defects via deep level transient spectroscopy revealed that E sub v + 0.31 eV defect, attributed to boron-oxygen-vacancy complex, is responsible for the reverse annealing of the irradiated cells in the temperature range of 150 to 350 C.

Rohatgi, A.↗