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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 955 records · Page 53
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

All-optical control of charge transfer and interlayer excitons in transition metal dichalcogenide heterostructures

An all-optical approach to control interlayer charge transfer and interlayer exciton dynamics is demonstrated using transition metal dichalcogenide heterostructures of MoSe 2 /MoS 2 and MoSe 2 /WS 2 as examples. In the three-pulse pump-probe experiments, a control pulse injects photocarriers and produces an electric field due to the interlayer charge separation. A pump pulse excites new carriers and their dynamics under the influence of the control-injected carriers and field is time-resolved by measuring differential reflectance of a third probe pulse. In MoSe 2 /MoS 2 , the interlayer electron transfer time from MoSe 2 to MoS 2 decreases with increasing the control-injected carrier density and electric field. The dipole moment of the interlayer excitons is reduced by the control pulse, which can be utilized for ultrafast and all-optical control of interlayer excitons. The recombination of the interlayer excitons is enhanced by the control pulse, which increases the spatial overlap of the electron and hole wave functions. The effect of the control pulse on the interlayer excitons is confirmed in the MoSe 2 /WS 2 heterostructure, although its effect on the electron transfer time is not resolvable. Furthermore, these results reveal useful information to understand and control interlayer charge transfer dynamics and provide tools for ultrafast manipulation of electrons in van der Waals heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Characterization and Failure Analysis of 650-V Enhancement-Mode GaN HEMT for Cryogenically Cooled Power Electronics

In order to evaluate the feasibility of newly developed gallium nitride (GaN) devices in a cryogenically cooled converter, this article characterizes a 650-V enhancement-mode GaN high-electron mobility transistor (GaN HEMT) at cryogenic temperatures. The characterization includes both static and dynamic behaviors. The results show that this GaN HEMT is an excellent device candidate to be applied in cryogenic-cooled applications. For example, transconductance at cryogenic temperature (93 K) is 2.5 times higher than one at room temperature (298 K), and accordingly, peak di / dt during turn-on transients at cryogenic temperature is around 2 times of that at room temperature. Moreover, the ON-resistance of the channel at the cryogenic temperature is only one-fifth of that at room temperature. The corresponding explanations of performance trends at cryogenic temperatures are also given from the view of semiconductor physics. In addition, several device failures were observed during the dynamic characterization of GaN HEMTs at cryogenic temperatures. Additionally, the ultrafast switching speed-induced high di / dt and dv / dt at cryogenic temperatures amplify the negative effects of parasitics inside the switching loop. Based on failure waveforms, two failure modes were classified, and detailed failure mechanisms caused by ultrafast switching speed are given in this article.

42 ENGINEERING↗
DOE OSTI2023

Investigation of AlGaN-Delta–GaN-Based UV Photodiodes in a Metal–Semiconductor–Metal Configuration for Efficient and Fast Solar Blind UV Sensing

Metal–semiconductor–metal (MSM) configured UV photodiodes (PD’s) were designed and fabricated on an AlGaN/GaN–based substrate for efficient and ultrafast UV detection. The purpose was to investigate the feasibility of obtaining efficient and ultrafast temporal response from these devices in the UV given the challenges associated with the formation of Schottky contacts on laterally oriented AlGaN/GaN thin films. Two sets of devices were implemented using Pt and Au as metal contacts with 5-µm finger width, 5-µm finger spacing, and a 50-µm x 50-µm active area. Spectral and voltage bias studies were done to establish the spectral profile and the effect of bias voltage on the responsivity of the detectors at 265 nm. Here, the best vertical MSM PD’s produced 0.6-A/W responsivity under 10-V bias voltage at 265 nm. Peak spectral responsivities were recorded as 1.35 A/W and 1.25 A/W at 240 nm for Pt and Au PD’s, respectively.

42 ENGINEERING↗
DOE OSTI2021

Optical current generation in graphene: CEP control vs. ω + 2 ω control

The injection of directional currents in solids with strong optical fields has attracted tremendous attention as a route to realize ultrafast electronics based on the quantum-mechanical nature of electrons at femto- to attosecond timescales. Such currents are usually the result of an asymmetric population distribution imprinted by the temporal symmetry of the driving field. Here we compare two experimental schemes that allow control over the amplitude and direction of light-field-driven currents excited in graphene. Both schemes rely on shaping the incident laser field with one parameter only: either the carrier-envelope phase (CEP) of a single laser pulse or the relative phase between pulses oscillating at angular frequencies ω and 2ω, both for comparable laser parameters. We observe that the efficiency in generating a current via two-color-control exceeds that of CEP control by more than two orders of magnitude (7 nA vs. 18 pA), as the ω + 2ω field exhibits significantly more asymmetry in its temporal shape. We support this finding with numerical simulations that clearly show that two-color current control in graphene is superior, even down to single-cycle pulse durations. We expect our results to be relevant to experimentally access fundamental properties of any solid at ultrafast timescales, as well as for the emerging field of petahertz electronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Soliton Generation in Negative Thermal Expansion Materials

Strain solitons have been observed statically in several 2D materials and dynamically in substrate materials using ultrafast laser pulses. The latter case relies on lattice relaxation in response to ultrafast heating in a light-absorbing transducer material, a process which is sensitive to the thermal expansion coefficient. Here we consider an unusual case where the sign of the thermal expansion coefficient is negative, a scenario which is experimentally feasible in light of rapid and recent advances in the discovery of negative thermal expansion materials. We present numerical solutions to a nonlinear differential equation which has been repeatedly demonstrated to quantitatively model experimental data and discuss the salient results using realistic parameters for material linear and nonlinear elasticity. The solitons that emerge from the initial value problem with negative and positive thermal expansion are qualitatively different in several ways. The new case of negative thermal expansion gives rise to a nearly-periodic soliton train with chirped profile and free of an isolated shock front. We suggest this unanticipated result may be realized experimentally and assess the potential for certain applications of this generic effect.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Dark-field x-ray microscopy for 2D and 3D imaging of microstructural dynamics at the European x-ray free-electron laser

Dark field x-ray microscopy (DXFM) can visualize microstructural distortions in bulk crystals. Using the femtosecond x-ray pulses generated by x-ray free-electron lasers (XFELs), DFXM can achieve sub-μm spatial resolution and <100 fs time resolution simultaneously. In this paper, we demonstrate ultrafast DFXM measurements at the European XFEL to visualize an optically driven longitudinal strain wave propagating through a diamond single crystal. We also present two DFXM scanning modalities that are new to the XFEL sources: spatial 3D and 2D axial-strain scans with sub-μm spatial resolution. With this progress in XFEL-based DFXM, we discuss new opportunities to study multi-timescale spatiotemporal dynamics of microstructures.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodi.de Perovskites

Hybrid organic-inorganic perovskites such as methylammonium lead iodide have emerged as promising semiconductors for energy-relevant applications. The interactions between charge carriers and lattice vibrations, giving rise to polarons, have been invoked to explain some of their extraordinary optoelectronic properties. Here, time-resolved optical spectroscopy is performed, with off-resonant pumping and electronic probing, to examine several representative lead iodide perovskites. The temporal oscillations of electronic bandgaps induced by coherent lattice vibrations are reported, which is attributed to antiphase octahedral rotations that dominate in the examined 3D and 2D hybrid perovskites. The off-resonant pumping scheme permits a simplified observation of changes in the bandgap owing to the A(g) vibrational mode, which is qualitatively different from vibrational modes of other symmetries and without increased complexity of photogenerated electronic charges. The work demonstrates a strong correlation between the lead-iodide octahedral framework and electronic transitions, and provides further insights into the manipulation of coherent optical phonons and related properties in hybrid perovskites on ultrafast timescales.

coherent optical phonons↗
DOE OSTI2019

Nanoimaging and Nanospectroscopy of Polaritons with Time Resolved s ‐SNOM

Abstract The development of electronics and photonics is entering a new era of ultrahigh speed sensing, data processing, and telecommunication. The carrier frequencies of the next‐generation electronic devices inevitably extend beyond radio frequencies, marching toward the nominally photonics‐dominated territories, e.g., terahertz and beyond. As a result, electronic and photonic techniques naturally merge and seek common ground. At the forefront of this technical trend is the field of polaritonics, where polaritons are half‐light, half‐matter quasiparticles that carry the properties of both “bare” photons and “bare” dipole‐carrying excitations. The Janus‐faced nature of polaritons renders the unique capability of operando control using photoexcitation or applied electric field. Here, state‐of‐the‐art ultrafast polaritonic phenomena probed by scattering‐type scanning near‐field optical microscope ( s ‐SNOM) techniques is reviewed. The ultrafast dynamical control and loss‐reduction of the polariton propagation are discussed with special emphasis on the creation and probing of the tip or edge induced plasmon– and phonon–polaritons in low‐dimensional systems. The detailed technical aspects of s ‐SNOM and its possible future development are also presented.

Yao, Ziheng↗
DOE OSTI2022

Terahertz Detection Using Enhanced Two‐Step Absorption in Photoconductive Metasurfaces Gated at λ = 1.55 µm

Abstract Superior ultrafast photoconductive properties make low temperature grown (LT) GaAs one of the best materials for photoconductive terahertz (THz) detection. However, the large bandgap of LT‐GaAs limits its operation to gating at wavelengths shorter than 870 nm. Here, it is demonstrated for the first time that nanostructuring the LT‐GaAs into a highly absorbing metasurface enables THz photoconductive detection with a pulsed laser at λ = 1.55 µm. The very weak sub‐bandgap absorption mediated by midgap states in LT‐GaAs is strongly enhanced using the concept of perfect absorption via degenerate critical coupling. Integrated with a THz antenna, the LT‐GaAs metasurface enables high sensitivity THz detection with a high dynamic range of 60 dB and large bandwidth up to 4.5 THz. The LT‐GaAs metasurface has the potential to serve as a universal ultrafast switching element for THz applications, enabling low‐cost, turn‐key THz systems for a variety of real‐world applications.

Jung, Hyunseung↗
DOE OSTI2025

Efficient Broadband Terahertz Generation by Above‐Band‐Gap Excitation of the Pyroelectric ZnSnN 2

Terahertz (THz) radiation is a powerful probe of low-energy excitations in all phases of matter. However, it remains a challenge to find materials that efficiently generate THz radiation in a broad range of frequencies following optical excitation. Here, we investigate a pyroelectric material, ZnSnN 2 , and find that its above-band-gap excitation results in the efficient formation of an ultrafast photocurrent generating THz radiation. The resulting THz electric field spans a frequency range from below 1 THz to above 30 THz. The results suggest that the photocurrent is primarily driven by an ultrafast pyroelectric effect where the photo-excited carriers screen the spontaneous electric polarization of ZnSnN 2 . Strong structural disorder reduces the photocarrier lifetime significantly and, thus, enables broadband operation. ZnSnN2 shows a similar THz-emitter performance as the best spintronic THz emitters regarding bandwidth and amplitude. The study unveils the large potential of pyroelectric materials as efficient and broadband THz emitters with built-in bias fields.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Single-shot switching in Tb/Co-multilayer based nanoscale magnetic tunnel junctions

Magnetic tunnel junctions (MTJs) are elementary units of magnetic memory devices. For high-speed and low-power data storage and processing applications, fast reversal of the magnetization by an ultrashort laser pulse is extremely important. Here we demonstrate single-shot switching of Tb/Co-multilayer based nanoscale MTJs by combining the optical writing and the electrical read-out methods. A 90-fs-long laser pulse switches the magnetization of the storage layer (SL). The change in the tunneling magnetoresistance (TMR) between the SL and a reference layer (RL) is probed electrically across the oxide barrier. Single-shot switching is demonstrated by varying the cell diameter from 300 nm to 20 nm. The anisotropy, magnetostatic coupling, and switching probability exhibit cell-size dependence. By suitable association of laser fluence and magnetic field, successive commutation between high-resistance and low-resistance states is achieved. The nature of the magnetization reversal of both SL and RL in a continuous film is probed with a depth-resolved magneto-optical Kerr effect (MOKE) magnetometry. The ultrafast dynamics in the continuous full-MTJ stack is investigated with the time-resolved pump–probe technique. Our experimental findings provide strong support for the growing interest in ultrafast spintronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Structural and spectroscopic characterization of photoactive yellow protein and photoswitchable fluorescent protein constructs containing heavy atoms

Photo-induced structural rearrangements of chromophore-containing proteins are essential for various light-dependent signaling pathways and optogenetic applications. Ultrafast structural and spectroscopic methods have offered insights into these structural rearrangements across many timescales. However, questions still remain about exact mechanistic details, especially regarding photoisomerization of the chromophore within these proteins femtoseconds to picoseconds after photoexcitation. Instrumentation advancements for time-resolved crystallography and ultrafast electron diffraction provide a promising opportunity to study these reactions, but achieving enough signal-to-noise is a constant challenge. In this work, we present four new photoactive yellow protein constructs and one new fluorescent protein construct that contain heavy atoms either within or around the chromophore and can be expressed with high yields. Structural characterization of these constructs, most at atomic resolution, show minimal perturbation caused by the heavy atoms compared to wild-type structures. Spectroscopic studies report the effects of the heavy atom identity and location on the chromophore’s photophysical properties. None of the substitutions prevent photoisomerization, although certain rates within the photocycle may be affected. Overall, these new proteins containing heavy atoms are ideal samples for state-of-the-art time-resolved crystallography and electron diffraction experiments to elucidate crucial mechanistic information of photoisomerization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Initial assessment of multilayer silicon detectors for hard X-ray imaging

Silicon detectors with lower material budget, ultrafast readout and radiation hardness are under developments. These unique features make pixelized silicon sensors a good option for hard X-ray imaging. To verify the performance of spatial resolution and energy sensitivity of silicon sensors to hard X-rays, a two layer setup of Pixelink PL-D725MU sensors has been tested at the Argonne National Laboratory Advanced Photon Source (APS) ID-10 sector with 29.2 keV high photon flux (4.5 x 10(8) to 4.5 x 10(10) photons per second) X-rays. Better than 3 mu m spatial resolution and clear energy characterization have been achieved by both layers. Commercial CMOS sensors with superior spatial resolution could be used for phase contrast imaging in current synchrotrons. These studies pave the path for future multilayer ultrafast silicon sensor development with ns to sub-ns readout speeds in hard X-ray imaging at synchrotrons and XFEL beamlines.

Hard X-ray imaging↗
DOE OSTI2019

Saddle point approaches in strong field physics and generation of attosecond pulses

Attoscience is the emerging field that accesses the fastest electronic processes occurring at the atomic and molecular length scales with attosecond (1 as = 10 –18 s) time resolution having wide ranging physical, chemical, material science and biological applications. The quintessential and one of the most fundamental processes in this domain is the generation of phase locked XUV attosecond pulses. The theoretical approach to understand the process incorporates a fully quantum or semi classical or relativistic description of coherent charge dynamics in intense ultrashort electromagnetic fields driving a quantum system (an atom, a molecule, solid band gap materials or surface plasmas). Modelling of such physical and dynamical systems in science and also in many other branches often leads to equations represented in terms of complex multi-dimensional integrals. These integrals can often be solved using the stationary phase approximation, which leads to a series of equations identifying the points in the multi-dimensional space, having most significant contributions in their evaluation. These points are usually indicated as saddle points. The description of the dynamics of quantum mechanical or relativistic systems that results from such an approach enables near to classical physics intuitive perceptions of the processes under investigation. Thus, the saddle point methods are very powerful and valuable general theoretical tools to obtain asymptotic expressions of such solutions and help also to gain physical insights on the underlying phenomena. Such techniques developed in the past have been adapted to study the emission of as pulses by different physical systems and have been widely employed in calculating and estimating the response of matter to intense electromagnetic pulses on ultrafast time scales. Here we provide an extensive disposition of the saddle point approaches unifying their ubiquitous applications within the domain of attoscience valid for simple atomic to more complex condensed matter systems undergoing ultrafast dynamics and present current trends and advancements in the field. In this review we would delineate the methodology, present a synthesis of seminal works and describe the state of the art applications. Finally we also address ultrashort time dynamics of novel materials that have gained much attention recently, namely lower dimensional material systems and micro-plasma systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

From Coherence to Function: Exploring the Connection in Chemical Systems

The role of quantum mechanical coherences or coherent superposition states in excited state processes has received considerable attention in the last two decades largely due to advancements in ultrafast laser spectroscopy. These coherence effects hold promise for enhancing the efficiency and robustness of functionally relevant processes, even when confronted with energy disorder and environmental fluctuations. Understanding coherence deeply drives us to unravel mechanisms and dynamics controlled by order and synchronization at a quantum mechanical level, envisioning optical control of coherence to enhance functions or create new ones in molecular and material systems. In this frontier, the interplay between electronic and vibrational dynamics, specifically the influence of vibrations in directing electronic dynamics, has emerged as the leading principle. Here, two energetically disparate quantum degrees of freedom work in-sync to dictate the trajectory of an excited state reaction. Moreover, with the vibrational degree being directly related to the structural composition of molecular or material systems, new molecular designs could be inspired by tailoring certain structural elements. In the realm of chemical kinetics, our understanding of the dynamics of chemical transformations is underpinned by fundamental theories, such as transition state theory, activated rate theory, and Marcus theory. These theories elucidate reaction rates by considering the energy barriers that must be overcome for reactants to transform into products. Those barriers are surmounted by the stochastic nature of energy gap fluctuations within reacting systems, emphasizing that the reaction coordinate, the pathway from reactants to products, is not rigidly defined by a specific vibrational motion but encompasses a diverse array of molecular motions. While less is known about the involvement of specific intramolecular vibrational modes, their significance in certain cases cannot be overlooked. In this Account, we summarize key experimental findings that offer deeper insights into the complex electronic–vibrational trajectories encompassing excited states afforded from state-of-the-art ultrafast laser spectroscopy in three exemplary processes: photoinduced electron transfer, singlet–triplet intersystem crossing, and intramolecular vibrational energy flow in molecular systems. We delve into the rapid decoherence, or loss of phase and amplitude correlations, of vibrational coherences along promoter vibrations during subpicosecond intersystem crossing dynamics in a series of binuclear platinum complexes. This rapid decoherence illustrates the vibration-driven reactive pathways from the Franck–Condon state to the curve crossing region. We also explore the generation of new vibrational coherences induced by impulsive reaction dynamics rather than by the laser pulse in these systems, which sheds light on specific energy dissipation pathways and thereby on the progression of the reaction trajectory in the vicinity of the curve crossing on the product side. Another property of vibrational coherences, amplitude, reveals how energy can flow from one vibration to another in the electronic excited state of a terpyridine–molybdenum complex hosting a nonreactive dinitrogen substrate. In conclusion, a slight change in vibrational energy triggers a quasi-resonant interaction, leading to constructive wavepacket interference and ultimately intramolecular vibrational redistribution from a Franck–Condon active terpyridine vibration to a dinitrogen stretching vibration, energizing the dinitrogen bond.

Electrical energy↗
DOE OSTI2020

Energy Migration Processes in Re(I) MLCT Complexes Featuring a Chromophoric Ancillary Ligand

We present herein the synthesis, structural characterization, electronic structure calculations, and ultrafast and supra-nanosecond photophysical properties of a series of five Re(I) bichromophores exhibiting metal to ligand charge transfer (MLCT) excited states based on the general formula fac -[Re(N ^ N)(CO) 3 (PNI-py)]PF 6, where PNI-py is 4-piperidinyl-1,8-naphthalimidepyridine and N ^ N is a diimine ligand ( Re1 – 5 ), along with their corresponding model chromophores where 4-ethylpyridine was substituted for PNI-py ( Mod1 – 5 ). The diimine ligands used include 1,10-phenanthroline (phen, 1 ), 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline (bcp, 2 ), 4,4'-di- tert -butyl-2,2'-bipyridine (dtbb, 3 ), 4,4'-diethyl ester-2,2'-bipyridine (deeb, 4 ), and 2,2'-biquinoline (biq, 5 ). In these metal–organic bichromophores, structural modification of the diimine ligand resulted in substantial changes to the observed energy transfer efficiencies between the two chromophores as a result of the variation in 3 MLCT excited-state energies. The photophysical properties and energetic pathways of the model chromophores were explored in parallel to accurately track the changes that arose from introduction of the organic chromophore pendant on the ancillary ligand. All relevant photophysical and energy transfer processes were probed and characterized using time-resolved photoluminescence spectroscopy, ultrafast and nanosecond transient absorption spectroscopy, and time-dependent density functional theory calculations. Of the five bichromophores in this study, four ( Re1 – 4 ) exhibited a thermal equilibrium between the 3 PNI-py and the 3 MLCT excited state, drastically extending the lifetimes of the parent model chromophores.

14 SOLAR ENERGY↗
DOE OSTI2021

An Ab Initio Multiple Cloning Method for Non-Adiabatic Excited-State Molecular Dynamics in NWChem

The recently developed ab-initio multiple cloning (AIMC) approach based on the multicongurational Ehrenfest (MCE) method provides a powerful and accurate way of describing the excited-state dynamics of molecular systems. The AIMC method is a controlled approximation to non-adiabatic dynamics with a particular strength in the proper description of decoherence effects due to branching of vibrational wavepackets at a level crossing. In this work, we report a new implementation of the AIMC algorithm in the open source NWChem computational chemistry program. The framework combines linear-response time-dependent density functional theory with Ehrenfest mean-eld theory to determine the equations of motion for classical trajectories. The multi-dimensional wave function is decomposed into a superposition of Gaussian coherent states guided by Ehrenfest trajectories (i.e., MCE approach), which can clone with fully quantum mechanical amplitudes and phases. By using an efficient time-derivative based non-adiabatic coupling approach within the AIMC method, all observable are calculated on-the-y in the non-adiabatic molecular dynamics process. As a representative example, we apply our implementation to study the ultrafast photoinduced electronic and vibrational energy transfer in a pyridine molecule. The effects of the cloning procedure on electronic and vibrational coherence, relaxation and unidirectional energy transfer are discussed. This new AIMC implementation provides a high-level non-adiabatic molecular dynamics framework for simulating photoexcited dynamics in complex molecular systems and experimentally relevant ultrafast spectroscopic probes, such as nonlinear coherent optical and X-ray signals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Resolving the Impact of Hydrogen Bonding on the Phylloquinone Cofactor through Two-Dimensional Infrared Spectroscopy

Phylloquinone (PhQ) is a molecule involved in photosynthetic electron transfer, where the local protein environment is known to tune the properties of PhQ through various noncovalent interactions. In this work, we determine how hydrogen bonding, one of these noncovalent interactions, alters the vibrational potential energy surface of PhQ. In addition, this work demonstrates how hydrogen bonding to PhQ manifests in ultrafast multidimensional vibrational spectra, which is an important step towards using ultrafast vibrational based spectroscopies to probe PhQ embedded in the binding pocket of photosynthetic reaction centers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗