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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 1,009 records · Page 56
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DOE OSTI2023

Electron Microscopy Studies of Soft Nanomaterials

This review highlights recent efforts on applying electron microscopy (EM) to soft (including biological) nanomaterials. We will show how developments of both the hardware and software of EM have enabled new insights into the formation, assembly, and functioning (e.g., energy conversion and storage, phonon/photon modulation) of these materials by providing shape, size, phase, structural, and chemical information at the nanometer or higher spatial resolution. Specifically, we first discuss standard real-space two-dimensional imaging and analytical techniques which are offered conveniently by microscopes without special holders or advanced beam technology. The discussion is then extended to recent advancements, including visualizing three-dimensional morphology of soft nanomaterials using electron tomography and its variations, identifying local structure and strain by electron diffraction, and recording motions and transformation by in situ EM. On these advancements, we cover state-of-the-art technologies designed for overcoming the technical barriers for EM to characterize soft materials as well as representative application examples. Here, the even more recent integration of machine learning and its impacts on EM are also discussed in detail. With our perspectives of future opportunities offered at the end, we expect this review to inspire and stimulate more efforts in developing and utilizing EM-based characterization methods for soft nanomaterials at the atomic to nanometer length scales in academic research and industrial applications.

Imaging↗
DOE OSTI2021

Precision measurement of electron-electron scattering in GaAs/AlGaAs using transverse magnetic focusing

Electron-electron (e-e) interactions assume a cardinal role in solid-state physics. Quantifying the e-e scattering length is hence critical. In this paper we show that the mesoscopic phenomenon of transverse magnetic focusing (TMF) in two-dimensional electron systems forms a precise and sensitive technique to measure this length scale. Conversely we quantitatively demonstrate that e-e scattering is the predominant effect limiting TMF amplitudes in high-mobility materials. Using high-resolution kinetic simulations, we show that the TMF amplitude at a maximum decays exponentially as a function of the e-e scattering length, which leads to a ready approach to extract this length from the measured TMF amplitudes. The approach is applied to measure the temperature-dependent e-e scattering length in high-mobility GaAs/AlGaAs heterostructures. The simulations further reveal current vortices that accompany the cyclotron orbits - a collective phenomenon counterintuitive to the ballistic transport underlying a TMF setting.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Development of a compact thermal lithium atom beam source for measurements of electron velocity distribution function anisotropy in electron cyclotron resonance plasmas

The anisotropy of the electron velocity distribution function (EVDF) in plasmas can be deduced from the polarization of emissions induced by anisotropic electron-impact excitation. In this paper, we develop a compact thermal lithium atom beam source for spatially resolved measurements of the EVDF anisotropy in electron cyclotron resonance (ECR) plasmas. The beam system is designed such that the ejected beam has a slab shape, and the beam direction is variable. The divergence and flux of the beam are evaluated by experiments and calculations. The developed beam system is installed in an ECR plasma device with a cusp magnetic field, and the LiI 2s–2p emission (670.8 nm) is observed in low-pressure helium plasma. The two-dimensional distributions of the degree and direction of the polarization in the LiI emission are measured by a polarization imaging system. The evaluated polarization distribution suggests the spatial variation of the EVDF anisotropy.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2013

Focused electron beam in pyroelectric electron probe microanalyzer

We report a method to focus the electron beam generated using a pyroelectric crystal. An electron beam with a spot size of 100 μm was achieved by applying an electrical field to an electroconductive needle tip set on a pyroelectric crystal. When the focused electron beam bombarded a sample, characteristic X-rays of the sample were only detected due to the production of an electric field between the needle tip and the sample.

43 PARTICLE ACCELERATORS↗
DOE OSTI2014

On the role of electron energy distribution function in double frequency heating of electron cyclotron resonance ion source plasmas

Double frequency heating (DFH) is a tool to improve the output of highly charged ions particularly from modern electron cyclotron resonance ion source installations with very high RF-frequencies. In order to gain information on the DFH-mechanism and on the role of the lower injected frequency we have carried out a series of dedicated experiments where we have put emphasis on the creation of a discrete resonance surface also for this lower frequency. Our well-established method of inserting an emissive MD (metal-dielectric) liner into the plasma chamber of the source is used in these experiments as a tool of investigation. In this way, the electron temperature and density for both ECR zones is increased in a controlled manner, allowing conclusions on the role of the change of the electron-energy-distribution function with and without DFH.

43 PARTICLE ACCELERATORS↗
DOE OSTI2013

Temperature dependence of diffusion length, lifetime and minority electron mobility in GaInP

The mobility of electrons in double heterostructures of p-type Ga{sub 0.50}In{sub 0.50}P has been determined by measuring minority carrier diffusion length and lifetime. The minority electron mobility increases monotonically from 300 K to 5 K, limited primarily by optical phonon and alloy scattering. Comparison to majority electron mobility over the same temperature range in comparably doped samples shows a significant reduction in ionized impurity scattering at lower temperatures, due to differences in interaction of repulsive versus attractive carriers with ionized dopant sites. These results should be useful in modeling and optimization for multi-junction solar cells and other optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Growth parameter optimization and interface treatment for enhanced electron mobility in heavily strained GaInAs/AlInAs high electron mobility transistor structures

The optimization of heavily strained Ga{sub 0.25}In{sub 0.75}As/Al{sub 0.48}In{sub 0.52}As high electron mobility transistor structures is discussed in detail. The growth parameters and the channel layer interfaces were optimized in order to maximize the mobility of the two-dimensional electron gas. Structures composed of an 11 nm thick channel layer and a 4 nm thick spacer layer exhibited electron mobilities as high as 15 100 cm{sup 2}/Vs and 70 000 cm{sup 2}/Vs at 300 and 77 K, respectively, for channels including InAs strained layers. The sheet carrier density was kept above 2.5 × 10{sup 12} cm{sup −2} throughout the entire study.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

University of Lodz an electron spectrometer—A new conversion-electron spectrometer for “in-beam” measurements

The designed and constructed at the University of Lodz an electron spectrometer is devoted to “in-beam” measurements. The apparatus is characterized by high efficiency up to 9%, good energy resolution (FWHM = 5 keV at 482 keV) and, what is very important good suppression of delta electrons, positrons, and photons emitted by the targets. This achievement was obtained using a combination of magnetic field in two different layouts: perpendicular and parallel to the axis of the spectrometer being orthogonal to the beamline. The conversion-electron spectrometer coupled to the EAGLE array was successfully tested in an “in-beam” measurement.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Pairing and unpairing electron densities in organic systems: Two-electron three center through space and through bonds interactions

Two-electron three-center bonding interactions in organic ions like methonium (CH{sub 5}{sup +}), ethonium (C{sub 2}H{sub 7}{sup +}), and protonated alkanes n−C{sub 4}H{sub 11}{sup +} isomers (butonium cations) are described and characterized within the theoretical framework of the topological analysis of the electron density decomposition into its effectively paired and unpaired contributions. These interactions manifest in some of this type of systems as a concentration of unpaired electron cloud around the bond paths, in contrast to the well known paradigmatic boron hydrids in which it is not only concentrated close to the atomic nucleus and the bond paths but out of them and over the region defined by the involved atoms as a whole. This result permits to propose an attempt of classification for these interactions based in such manifestations. In the first type, it is called as interactions through bonds and in the second type as interactions through space type.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Combining nanocalorimetry and dynamic transmission electron microscopy for in situ characterization of materials processes under rapid heating and cooling

Nanocalorimetry is a chip-based thermal analysis technique capable of analyzing endothermic and exothermic reactions at very high heating and cooling rates. Here, we couple a nanocalorimeter with an extremely fast in situ microstructural characterization tool to identify the physical origin of rapid enthalpic signals. More specifically, we describe the development of a system to enable in situ nanocalorimetry experiments in the dynamic transmission electron microscope (DTEM), a time-resolved TEM capable of generating images and electron diffraction patterns with exposure times of 30 ns–500 ns. The full experimental system consists of a modified nanocalorimeter sensor, a custom-built in situ nanocalorimetry holder, a data acquisition system, and the DTEM itself, and is capable of thermodynamic and microstructural characterization of reactions over a range of heating rates (10{sup 2} K/s–10{sup 5} K/s) accessible by conventional (DC) nanocalorimetry. To establish its ability to capture synchronized calorimetric and microstructural data during rapid transformations, this work describes measurements on the melting of an aluminum thin film. We were able to identify the phase transformation in both the nanocalorimetry traces and in electron diffraction patterns taken by the DTEM. Potential applications for the newly developed system are described and future system improvements are discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Study of beam transverse properties of a thermionic electron gun for application to a compact THz free electron laser

A novel thermionic electron gun adopted for use in a high power THz free electron laser (FEL) is proposed in this paper. By optimization of the structural and radiofrequency (RF) parameters, the physical design of the gun is performed using dynamic calculations. Velocity bunching is used to minimize the bunch's energy spread, and the dynamic calculation results indicate that high quality beams can be provided. The transverse properties of the beams generated by the gun are also analyzed. The novel RF focusing effects of the resonance cavity are investigated precisely and are used to establish emittance compensation, which enables the injector length to be reduced. In addition, the causes of the extrema of the beam radius and the normalized transverse emittance are analyzed and interpreted, respectively, and slice simulations are performed to illustrate how the RF focusing varies along the bunch length and to determine the effects of that variation on the emittance compensation. Finally, by observation of the variations of the beam properties in the drift tube behind the electron gun, prospective assembly scenarios for the complete THz-FEL injector are discussed, and a joint-debugging process for the injector is implemented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Controversial electronic structures and energies of Fe{sub 2}, Fe{sub 2}{sup +}, and Fe{sub 2}{sup −} resolved by RASPT2 calculations

The diatomic molecule Fe{sub 2} was investigated using restricted active space second-order perturbation theory (RASPT2). This molecule is very challenging to study computationally because predictions about the ground state and excited states depend sensitively on the choice of the quantum chemical method. For Fe{sub 2} we show that one needs to go beyond a full-valence active space in order to achieve even qualitative agreement with experiment for the dissociation energy, and we also obtain a smooth ground-state potential curve. In addition we report the first multireference study of Fe{sub 2}{sup +}, for which we predict an {sup 8}Σ{sub u}{sup −} ground state, which was not predicted by previous computational studies. By using an active space large enough to remove the most serious deficiencies of previous theoretical work and by explicitly investigating the interpretations of previous experimental results, this study elucidates previous difficulties and provides – for the first time – a qualitatively correct treatment of Fe{sub 2}, Fe{sub 2}{sup +}, and Fe{sub 2}{sup −}. Moreover, this study represents a record in terms of the number or active electrons and active orbitals in the active space, namely 16 electrons in 28 orbitals. Conventional CASPT2 calculations can be performed with at most 16 electrons in 16 orbitals. We were able to overcome this limit by using the RASPT2 formalism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

N-representability-driven reconstruction of the two-electron reduced-density matrix for a real-time time-dependent electronic structure method

Propagating the equations of motion (EOM) for the one-electron reduced-density matrix (1-RDM) requires knowledge of the corresponding two-electron RDM (2-RDM). We show that the indeterminacy of this expression can be removed through a constrained optimization that resembles the variational optimization of the ground-state 2-RDM subject to a set of known N-representability conditions. Electronic excitation energies can then be obtained by propagating the EOM for the 1-RDM and following the dipole moment after the system interacts with an oscillating external electric field. For simple systems with well-separated excited states whose symmetry differs from that of the ground state, excitation energies obtained from this method are comparable to those obtained from full configuration interaction computations. Although the optimized 2-RDM satisfies necessary N-representability conditions, the procedure cannot guarantee a unique mapping from the 1-RDM to the 2-RDM. This deficiency is evident in the mean-field-quality description of transitions to states of the same symmetry as the ground state, as well as in the inability of the method to describe Rabi oscillations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Interactions of nonlinear electron-acoustic solitary waves with vortex electron distribution

In the present work, based on a one dimensional model, we consider the head-on-collision of nonlinear electron-acoustic waves in a plasma composed of a cold electron fluid, hot electrons obeying a trapped/vortex-like distribution, and stationary ions. The analysis is based on the use of extended Poincare, Lighthill-Kuo method [C. H. Su and R. M. Mirie, J. Fluid Mech. 98, 509 (1980); R. M. Mirie and C. H. Su, J. Fluid Mech. 115, 475 (1982)]. It is shown that, for the first order approximation, the waves propagating in opposite directions are characterized by modified Korteweg-de Vries equations. In contrary to the results of previous investigations on this subject, we showed that the phase shifts are functions of both amplitudes of the colliding waves. The numerical results indicate that the waves with larger amplitude experience smaller phase shifts. Such a result seems to be plausible from physical considerations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Dissociative electron attachment to the gas-phase nucleobase hypoxanthine

We present high-resolution measurements of the dissociative electron attachment (DEA) to isolated gas-phase hypoxanthine (C{sub 5}H{sub 4}N{sub 4}O, Hyp), a tRNA purine base. The anion mass spectra and individual ion efficiency curves from Hyp were measured as a function of electron energy below 9 eV. The mass spectra at 1 and 6 eV exhibit the highest anion yields, indicating possible common precursor ions that decay into the detectable anionic fragments. The (Hyp − H) anion (C{sub 5}H{sub 3}N{sub 4}O{sup −}) exhibits a sharp resonant peak at 1 eV, which we tentatively assign to a dipole-bound state of the keto-N1H,N9H tautomer in which dehydrogenation occurs at either the N1 or N9 position based upon our quantum chemical computations (B3LYP/6-311+G(d,p) and U(MP2-aug-cc-pVDZ+)) and prior studies with adenine. This closed-shell dehydrogenated anion is the dominant fragment formed upon electron attachment, as with other nucleobases. Seven other anions were also observed including (Hyp − NH){sup −}, C{sub 4}H{sub 3}N{sub 4}{sup −}/C{sub 4}HN{sub 3}O{sup −}, C{sub 4}H{sub 2}N{sub 3}{sup −}, C{sub 3}NO{sup −}/HC(HCN)CN{sup −}, OCN{sup −}, CN{sup −}, and O{sup −}. Most of these anions exhibit broad but weak resonances between 4 and 8 eV similar to many analogous anions from adenine. The DEA to Hyp involves significant fragmentation, which is relevant to understanding radiation damage of biomolecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Impact of potassium doping on the electronic structure of tetracene and pentacene: An electron energy-loss study

We report the doping induced changes of the electronic structure of tetracene and pentacene probed by electron energy-loss spectroscopy in transmission. A comparison between the dynamic response of undoped and potassium-intercalated tetracene and pentacene emphasizes the appearance of a new excitation feature in the former gap upon potassium addition. Interestingly, the momentum dependency of this new excitation shows a negative dispersion. Moreover, the analysis of the C 1s and K 2p core-level excitation results in a significantly lower doping level compared to potassium doped picene, a recently discovered superconductor. Therefore, the present electronic structure investigations open a new pathway to better understand the exceptional differences between acenes and phenacene and their divergent behavior upon alkali doping.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Complete-active-space second-order perturbation theory (CASPT2//CASSCF) study of the dissociative electron attachment in canonical DNA nucleobases caused by low-energy electrons (0-3 eV)

Low-energy (0-3 eV) ballistic electrons originated during the irradiation of biological material can interact with DNA/RNA nucleobases yielding transient-anion species which undergo decompositions. Since the discovery that these reactions can eventually lead to strand breaking of the DNA chains, great efforts have been dedicated to their study. The main fragmentation at the 0-3 eV energy range is the ejection of a hydrogen atom from the specific nitrogen positions. In the present study, the methodological approach introduced in a previous work on uracil [I. González-Ramírez et al., J. Chem. Theory Comput. 8, 2769-2776 (2012)] is employed to study the DNA canonical nucleobases fragmentations of N–H bonds induced by low-energy electrons. The approach is based on minimum energy path and linear interpolation of internal coordinates computations along the N–H dissociation channels carried out at the complete-active-space self-consistent field//complete-active-space second-order perturbation theory level. On the basis of the calculated theoretical quantities, new assignations for the adenine and cytosine anion yield curves are provided. In addition, the π{sub 1}{sup −} and π{sub 2}{sup −} states of the pyrimidine nucleobases are expected to produce the temporary anions at electron energies close to 1 and 2 eV, respectively. Finally, the present theoretical results do not allow to discard neither the dipole-bound nor the valence-bound mechanisms in the range of energies explored, suggesting that both possibilities may coexist in the experiments carried out with the isolated nucleobases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗