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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 1,585 records · Page 88
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Alkali triel chalcogenide nanocrystals: a molecular reactivity approach to ternary phase selectivity

Alkali-metal-based materials are promising building blocks for energy conversion and storage technologies. Here, we use a molecular reactivity-based solution-phase approach to selectively synthesize multiple phases and specific polymorphs of lithium- and sodium-containing triel chalcogenide nanocrystals, LiTrCh 2 , NaTrCh 2 , and NaTr 3 Ch 5 , where Tr = Ga and In and Ch = S, Se, and Te. Analogous to the case of binary II–VI and III–V tetrahedral semiconductors, where the two commonly isolated zinc blende and wurtzite polymorphs are separated by only 1–50 meV f.u. −1 , we find that LiTrCh 2 nanocrystals easily adopt tetragonal (chalcopyrite) and orthorhombic polymorphs separated by only 2.7–6.2 meV f.u. −1 Because of this small energy difference, soft colloidal synthesis succeeds in accessing either one of these polymorphs, depending on the specific dichalcogenide precursor used. Highly reactive diethyl diselenide favors the thermodynamically more stable tetragonal I$\bar{4}2$d phase, whereas mildly reactive diphenyl diselenide favors the kinetic, metastable orthorhombic Pna2 1 phase. Density functional theory calculations confirm the relative energies among multiple LiTrCh 2 polymorphs and also model the observed powder X-ray diffraction pattern of a new C2 NaIn 3 Te 5 phase. 7 Li, 69 Ga, and 77 Se solid-state NMR spectra are consistent with phase-pure ternary LiGaSe 2 nanocrystals. A majority of the nanocrystal compositions are visible-light emitters. This work opens the door to new Li/Na-based ternary triel chalcogenide nanostructures for energy storage and conversion applications.

Pavel, Md Riad Sarkar [Iowa State Univ., Ames, IA ↗
DOE OSTI2019

Electrostatic subframing and compressive-sensing video in transmission electron microscopy

We present kilohertz-scale video capture rates in a transmission electron microscope, using a camera normally limited to hertz-scale acquisition. An electrostatic deflector rasters a discrete array of images over a large camera, decoupling the acquisition time per subframe from the camera readout time. Total-variation regularization allows features in overlapping subframes to be correctly placed in each frame. Moreover, the system can be operated in a compressive-sensing video mode, whereby the deflections are performed in a known pseudorandom sequence. Compressive sensing in effect performs data compression before the readout, such that the video resulting from the reconstruction can have substantially more total pixels than that were read from the camera. This allows, for example, 100 frames of video to be encoded and reconstructed using only 15 captured subframes in a single camera exposure. We demonstrate experimental tests including laser-driven melting/dewetting, sintering, and grain coarsening of nanostructured gold, with reconstructed video rates up to 10 kHz. The results exemplify the power of the technique by showing that it can be used to study the fundamentally different temporal behavior for the three different physical processes. Both sintering and coarsening exhibited self-limiting behavior, whereby the process essentially stopped even while the heating laser continued to strike the material. We attribute this to changes in laser absorption and to processes inherent to thin-film coarsening. In contrast, the dewetting proceeded at a relatively uniform rate after an initial incubation time consistent with the establishment of a steady-state temperature profile.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Semicoherent oxide heterointerfaces: Structure, properties, and implications

In the quest for enhanced functionality of all sorts, nanostructured materials are becoming ever more common. This is particularly true of oxide/oxide heterostructures in which the high density of interfaces has been implicated in enhanced properties and used to engineer strain in oxide composite structures. These interfaces are often characterized by a network of misfit dislocations that relieve the lattice mismatch strain between the two materials, and these dislocations themselves are often suggested as the source of either enhancements or degradation of properties. Despite the importance and pervasiveness of misfit dislocations, however, there is still much that is unknown about their structure and properties, particularly in oxide/oxide heterostructures. Here, we give a perspective on the importance of these dislocation networks and the need to interrogate their impact on functionality.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer

Covalent functionalization of semiconducting single-wall carbon nanotubes (CNTs) introduces new photoluminescent emitting states. These states are spatially localized around functionalization sites and strongly red-shifted relative to the emission commonly observed from the CNT band-edge exciton state. A particularly important feature of these localized exciton states is that because the exciton is no longer free to diffusively sample photoluminescent quenching sites along the CNT length, its lifetime is significantly extended. We have recently demonstrated that an important relaxation channel of such localized excitons is the electronic-to-vibrational energy transfer (EVET). This process is analogous to the Förster resonance energy transfer except the final state of this process is not electronically, but vibrationally excited molecules of the surrounding medium (e.g., solvent). In this work, we develop a theory of EVET for a nanostructure of arbitrary shape and apply it to the specific case of EVET-mediated relaxation of defect-localized excitons in a covalently functionalized CNT. Here, the resulting EVET relaxation times are in good agreement with experimental data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Nanoshell quantum dots: Quantum confinement beyond the exciton Bohr radius

Nanoshell quantum dots (QDs) represent a novel class of colloidal semiconductor nanocrystals (NCs), which supports tunable optoelectronic properties over the extended range of particle sizes. Traditionally, the ability to control the bandgap of colloidal semiconductor NCs is limited to small-size nanostructures, where photoinduced charges are confined by Coulomb interactions. A notorious drawback of such a restricted size range concerns the fact that assemblies of smaller nanoparticles tend to exhibit a greater density of interfacial and surface defects. This presents a potential problem for device applications of semiconductor NCs where the charge transport across nanoparticle films is important, as in the case of solar cells, field-effect transistors, and photoelectrochemical devices. Furthermore, the morphology of nanoshell QDs addresses this issue by enabling the quantum-confinement in the shell layer, where two-dimensional excitons can exist, regardless of the total particle size. Such a geometry exhibits one of the lowest surface-to-volume ratios among existing QD architectures and, therefore, could potentially lead to improved charge-transport and multi-exciton characteristics. The expected benefits of the nanoshell architecture were recently demonstrated by a number of reports on the CdS bulk /CdSe nanoshell model system, showing an improved photoconductivity of solids and increased lifetime of multi-exciton populations. Along these lines, this perspective will summarize the recent work on CdS bulk /CdSe nanoshell colloids and discuss the possibility of employing other nanoshell semiconductor combinations in light-harvesting and lasing applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Long-lived charge separation in two-dimensional ligand-perovskite heterostructures

Rational design of heterojunctions using nanostructured materials is a useful strategy for achieving efficient interfacial charge separation in photovoltaics. Heterojunctions can be constructed between organic ligands and inorganic layer in two-dimensional (2D) perovskites, taking advantage of their highly programmable structures. We investigate electron and hole transfer at the interface between the thiophene-based semiconducting ligands and the lead halide inorganic sublattices using time-resolved photoluminescence and transient reflection spectroscopy in single 2D perovskite crystals. Here, these measurements demonstrate charge transfer time of ~ 10 ps and long-lived charge-separated state over the nanosecond timescale in 2D ligand-perovskite heterostructures. The efficient charge transfer processes with slow charge recombination suggest the potential for improving exciton dissociation and charge transport in 2D perovskite solar cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Thermal transport in nanoporous holey silicon membranes investigated with optically induced transient thermal gratings

In this study, we use transient thermal gratings—a non-contact, laser-based thermal metrology technique with intrinsically high accuracy—to investigate room-temperature phonon-mediated thermal transport in two nanoporous holey silicon membranes with limiting dimensions of 120 nm and 250 nm, respectively. We compare the experimental results with ab initio calculations of phonon-mediated thermal transport according to the phonon Boltzmann transport equation (BTE) using two different computational techniques. We find that the calculations conducted within the Casimir framework, i.e., based on the BTE with the bulk phonon dispersion and diffuse scattering from surfaces, are in quantitative agreement with the experimental data and thus conclude that this framework is adequate for describing phonon-mediated thermal transport in silicon nanostructures with feature sizes of the order of 100 nm.

Duncan, Ryan A. (ORCID:0000000328318099)↗
DOE OSTI2020

ABINIT: Overview and focus on selected capabilities

ABINIT is probably the first electronic-structure package to have been released under an open-source license about 20 years ago. It implements density functional theory, density-functional perturbation theory (DFPT), many-body perturbation theory (GW approximation and Bethe–Salpeter equation), and more specific or advanced formalisms, such as dynamical mean-field theory (DMFT) and the “temperature-dependent effective potential” approach for anharmonic effects. Relying on planewaves for the representation of wavefunctions, density, and other space-dependent quantities, with pseudopotentials or projector-augmented waves (PAWs), it is well suited for the study of periodic materials, although nanostructures and molecules can be treated with the supercell technique. The present article starts with a brief description of the project, a summary of the theories upon which ABINIT relies, and a list of the associated capabilities. It then focuses on selected capabilities that might not be present in the majority of electronic structure packages either among planewave codes or, in general, treatment of strongly correlated materials using DMFT; materials under finite electric fields; properties at nuclei (electric field gradient, Mössbauer shifts, and orbital magnetization); positron annihilation; Raman intensities and electro-optic effect; and DFPT calculations of response to strain perturbation (elastic constants and piezoelectricity), spatial dispersion (flexoelectricity), electronic mobility, temperature dependence of the gap, and spin-magnetic-field perturbation. The ABINIT DFPT implementation is very general, including systems with van der Waals interaction or with noncollinear magnetism. Community projects are also described: generation of pseudopotential and PAW datasets, high-throughput calculations (databases of phonon band structure, second-harmonic generation, and GW computations of bandgaps), and the library libpaw. ABINIT has strong links with many other software projects that are briefly mentioned.

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

Low-temperature nanoscale heat transport in a gadolinium iron garnet heterostructure probed by ultrafast x-ray diffraction

Time-resolved x-ray diffraction has been used to measure the low-temperature thermal transport properties of a Pt/Gd3Fe5O12//Gd3Ga5O12 metal/oxide heterostructure relevant to applications in spin caloritronics. A pulsed femtosecond optical signal produces a rapid temperature rise in the Pt layer, followed by heat transport into the Gd3Fe5O12 (GdIG) thin film and the Gd3Ga5O12 (GGG) substrate. The time dependence of x-ray diffraction from the GdIG layer was tracked using an accelerator-based femtosecond x-ray source. The ultrafast diffraction measurements probed the intensity of the GdIG (1 −1 2) x-ray reflection in a grazing-incidence x-ray diffraction geometry. The comparison of the variation of the diffracted x-ray intensity with a model including heat transport and the temperature dependence of the GdIG lattice parameter allows the thermal conductance of the Pt/GdIG and GdIG//GGG interfaces to be determined. Complementary synchrotron x-ray diffraction studies of the low-temperature thermal expansion properties of the GdIG layer provide a precise calibration of the temperature dependence of the GdIG lattice parameter. The interfacial thermal conductance of the Pt/GdIG and GdIG//GGG interfaces determined from the time-resolved diffraction study is of the same order of magnitude as previous reports for metal/oxide and epitaxial dielectric interfaces. The thermal parameters of the Pt/GdIG//GGG heterostructure will aid in the design and implementation of thermal transport devices and nanostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Anodic arc discharge: Why pulsed?

Pulsed anodic arc discharge is a novel synthesis method of nanomaterials by means of low-temperature atmospheric plasma. The technique consists in periodically supplying DC power to two vertically aligned electrodes in the form of short unipolar pulses with peak currents of a few hundred Amperes in helium atmosphere. The pulsed arc plasmas are sustained at frequencies of the order of 1 Hz with around 10% of duty cycle. It constitutes a versatile technique thanks to a series of advantages compared to continuous DC arc processes, in particular: flexibility in the experimental conditions, process stability and repeatability, better utilization of ablating anode material, lower production of macroparticles, and lower thermal loads. Such features are discussed in this article. A brief overview concerning the recent accomplishments of pulsed arc discharge on deposition of carbon nanostructures (graphene and carbon nanotubes) and few-layer flakes of molybdenum disulphide (MoS 2 ) is provided, as well as an outlook on future applications of this method for the discovery of new materials with tailored functional properties.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Tracking nanoparticle growth in pulsed carbon arc discharge

The dynamics of nanoparticle growth in pulsed anodic arc discharge has been studied in time-resolved mode. To this end, a fast moving probe was employed to extract the material generated in a pulsed arc plasma held between two graphite electrodes. The probe motion was synchronized with the pulse phase and the exposure time to the plasma was set to 10 ms. The graphite anode was eroded in a helium atmosphere (300 Torr) by an arc plasma pulsed at 1 Hz with a 10% duty cycle and showing 250 A of peak current. The structure and morphology of the probe depositions were characterized by Raman spectroscopy, scanning electron microscopy, and focused ion beam. A maximal deposition rate of 260 μm/s was measured 5 mm away from the arc core during the active 0.1 s of the pulse. Such a rate yields a growth flux of 1.3 × 10 21 cm –2 s –1 , rich in carbon nanostructures (graphene platelets, nanotubes) with a characteristic aggregate size within 1–10 μm. The deposition during the inactive 0.9 s of the pulse was several orders of magnitude slower and consisted of amorphous carbon traces. Furthermore, the nanoparticle distribution along the collecting probe is correlated with the pulse phase, thereby providing information on particle transport. Pulsed nanosynthesis can be modeled as a periodical growth process, where the volume and propagation velocity of the growth region can be adjusted through modulation of the pulse signal waveform. The proposed model constitutes a suitable framework to investigate the pulsed arc synthesis of nanomaterials with tailored physical and chemical properties.

42 ENGINEERING↗
DOE OSTI2020

Effect of Many Modes on Self-Polarization and Photochemical Suppression in Cavities

The standard description of cavity-modified molecular reactions typically involves a single (resonant) mode, while in reality the quantum cavity supports a range of photon modes. In this work we demonstrate that as more photon modes are accounted for, physico-chemical phenomena can dramatically change, as illustrated by the cavity-induced suppression of the important and ubiquitous process of proton-coupled electron-transfer. Using a multi-trajectory Ehrenfest treatment for the photonmodes, we find that self-polarization effects become essential, and we introduce the concept of selfpolarization- modified Born-Oppenheimer surfaces as a new construct to analyze dynamics. As the number of cavity photon modes increases, the increasing deviation of these surfaces from the cavityfree Born-Oppenheimer surfaces, together with the interplay between photon emission and absorption inside the widening bands of these surfaces, leads to enhanced suppression. The present findings are general and will have implications for the description and control of cavity-driven physical processes of molecules, nanostructures and solids embedded in cavities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Metal-ion-controlled growth and nanoindentation response of 3D, bicontinuous Cu–Fe thin films

Bicontinuous, nanocomposite thin film morphologies depend largely on the deposition conditions applied during physical vapor deposition. With the introduction of high power impulse magnetron sputtering (HiPIMS), the range of potential morphologies achieved during deposition has been increased. In this work, we compare the deposition outcomes between traditional direct-current magnetron sputtering (DCMS) and HiPIMS for a thin film co deposit of Cu and Fe. Modular control of the columnarity, porosity and roughness was achieved by varying the Cu and Fe metal ion currents during deposition. The directionality of the nanostructured phase-separated morphology was also controlled as the ion current increased. At zero ion current for both Cu and Fe sputtered species during DCMS, the film exhibited lateral concentration modulations of Cu and Fe. The directionality of the Cu- and Fe-rich phases shifted to vertical concentration modulations at low ion currents of I Fe = 1A and I Cu = 0:1A and to lateral concentration modulations at relatively moderate ion currents of I Fe = 5A and I Cu = 2A: At high ion currents of I Fe = 18A and I Cu = 2A; a more randomized phase domain structure was observed on the nanoscale. This structural shift is rationalized using an interdiffusion model. Here, the role of different kinds of phase separated morphologies, achieved during DCMS deposition, on the mechanical properties has also been studied. Results indicated increase in hardness, indentation modulus and flow strength values with the increase in indentation strain rates. Bicontinuous Cu-Fe nanocomposites are found to be stronger than multilayer Cu-Fe samples.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ligand structure and adsorption free energy of nanocrystals on solid substrates

In this paper, we present an investigation on the absorption of alkylthiolated nanocrystals on a solid substrate. We calculate adsorption free energies and report a number of effects induced by the substrate. Nearest neighbor distances and bonding free energies are significantly different than for a free floating case, there is a weakening of bonding free energies among nanocrystals, and the adsorption is manifestly anisotropic, i.e., stronger along certain directions of the nanocrystal core. We contend that this last result accounts for the Bain transition (fcc → bcc) observed in experimental results. We report the presence of vortices induced by the substrate, which explain the increased nearest neighbor distance among nanocrystals, which is in excellent quantitative agreement with experimental results and with the predictions of the Orbifold Topological Model. Implications for the assembly of nanostructures and future experiments are also discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Spontaneous emission dynamics of Eu 3+ ions coupled to hyperbolic metamaterials

We show that sub-wavelength nanostructured systems with tunable electromagnetic properties, such as hyperbolic metamaterials (HMMs), provide a useful platform to tailor spontaneous emission processes. Here, we investigate a system comprising Eu 3+ (NO 3 ) 3 ·6H 2 O nanocrystals on an HMM structure featuring a hexagonal array of Ag nanowires in a porous Al2O 3 matrix. The HMM-coupled Eu 3+ ions exhibit up to a 2.4 fold increase in their decay rate, accompanied by an enhancement of the emission rate of the 5 D 0 → 7 F 2 transition. Using finite-difference time-domain modeling, we corroborate these observations with the increase in the photonic density of states seen by the Eu 3+ ions in the proximity of the HMM. Our results indicate that HMMs can serve as a valuable tool to control the emission from weak transitions and, hence, hint at a route toward more practical applications of rare-earth ions in nanoscale optoelectronics and quantum devices.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Absolute laser energy absorption measurement of relativistic 0.7 ps laser pulses in nanowire arrays

Laser absorption is one of the most important parameters governing laser–matter interactions. The laser energy absorption on nanowire array targets is measured for the first time in the relativistic regime at intensities of 10 19 W=cm 2 and compared to foil targets. The results show that the laser energy absorption of 0.7 ps frequency doubled (527 nm) pulses on Au nanowire targets varies widely with nanowire parameters, reaching laser energy absorption values up to 71% of the incident energy, significantly exceeding those of solid flat targets obtained in similar irradiation conditions. The analysis shows that the increase in absorption strongly correlates with larger effective target surface area over a broad range of nanowire parameters explored. These direct absorption measurements provide valuable data to benchmark simulations of the relativistic laser pulse interactions with nanostructures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Second-harmonic generation in nonlinear plasmonic lattices enhanced by quantum emitter gain medium

In this work, we report on a theoretical study of second-harmonic generation (SHG) in plasmonic nanostructures interacting with two-level quantum emitters (QEs) under incoherent energy pump. We generalize the driven-dissipative Tavis–Cummings model by introducing the anharmonic surface plasmon-polariton (SPP) mode coupled to QEs and examine physical properties of corresponding SPP-QE polariton states. Our calculations of the SHG efficiency for strong QE-SPP coupling demonstrate orders of magnitude enhancement facilitated by the polariton gain. We further discuss time-domain numerical simulations of SHG in a square lattice comprising Ag nanopillars coupled to QEs utilizing a fully vectorial nonperturbative nonlinear hydrodynamic model for conduction electrons coupled to Maxwell–Bloch equations for QEs. The simulations support the idea of gain enhanced SHG and show orders of magnitude increase in the SHG efficiency as the QEs are tuned in resonance with the lattice plasmon mode and brought above the population inversion threshold by incoherent pumping. By varying pump frequency and tuning QEs to a localized plasmon mode, we demonstrate further enhancement of the SHG efficiency facilitated by strong local electric fields. The incident light polarization dependence of the SHG is examined and related to the symmetries of participating plasmon modes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Suppression of thermal conductivity and electronic correlations in Fe 1– x Ru x Sb 2 (0 ≤ x ≤ 0.6)

We present simultaneous suppression of FeSb 2 thermal conductivity and electronic correlations in Fe 1– x Ru x Sb 2 (0 ≤ x ≤ 0.6) single crystal alloys. Small energy gap Δ 1 in Kondo-insulator-like semiconductor FeSb 2 associated with impurity in-gap state increases whereas the intrinsic bandgap Δ 2 decreases upon Ru substitution on Fe atomic site. Thermopower is suppressed along with the intrinsic bandgap and with the thermal conductivity. The more delocalized 4 d character of atomic orbital of Ru brings suppression of electronic correlations, but also an increase in impurity density which reduces phonon mean free path and surface scattering length. Our results indicate a range of Ru doping x where nanostructuring could be used to suppress thermal conductivity further, potentially toward the amorphous limit.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗