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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

The role of electron irradiation history in liquid cell transmission electron microscopy

In situ liquid cell transmission electron microscopy (LC-TEM) allows dynamic nanoscale characterization of systems in a hydrated state. Although powerful, this technique remains impaired by issues of repeatability that limit experimental fidelity and hinder the identification and control of some variables underlying observed dynamics. We detail new LC-TEM devices that improve experimental reproducibility by expanding available imaging area and providing a platform for investigating electron flux history on the sample. Irradiation history is an important factor influencing LC-TEM results that has, to this point, been largely qualitatively and not quantitatively described. We use these devices to highlight the role of cumulative electron flux history on samples from both nanoparticle growth and biological imaging experiments and demonstrate capture of time zero, low-dose images on beam-sensitive samples. In particular, the ability to capture pristine images of biological samples, where the acquired image is the first time that the cell experiences significant electron flux, allowed us to determine that nanoparticle movement compared to the cell membrane was a function of cell damage and therefore an artifact rather than visualizing cell dynamics in action. Lastly, these results highlight just a subset of the new science that is accessible with LC-TEM through the new multiwindow devices with patterned focusing aides.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2019

Gold Nanocrystal Etching as a Means of Probing the Dynamic Chemical Environment in Graphene Liquid Cell Electron Microscopy

Graphene liquid cell electron microscopy has the needed temporal and spatial resolution to enable the in situ observation of nanoscale dynamics in solution. Yet, the chemistry of the solution in the liquid cell during imaging is as yet poorly understood due to the generation of a complex mixture of radiolysis products by the electron beam. In this work, the etching trajectories of nanocrystals were used as a probe to determine the effect of the electron beam dose rate and preloaded etchant, FeCl 3 , on the chemistry of the liquid cell. Initially, illuminating the sample at a low electron beam dose rate generates hydrogen bubbles, providing a reservoir of sacrificial reductant. Increasing the electron beam dose rate leads to a constant etching rate that varies linearly with the electron beam dose rate. Comparing these conclusions with the oxidation potentials of the species in solution, the electron beam likely controls the total concentration of oxidative species in solution and FeCl 3 likely controls the relative ratio of oxidative species, independently determining the etching rate and chemical potential of the reaction, respectively. Correlating these liquid cell etching results with the ex situ oxidative etching of gold nanocrystals using FeCl 3 provides further insight into the liquid cell chemistry while corroborating the liquid cell dynamics with ex situ synthetic behavior. This understanding of the chemistry in the liquid cell will allow researchers to better control the liquid cell electron microscopy environment, enabling new nanoscale materials science experiments to be conducted systematically in a reproducible manner.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Upper critical solution temperature polymer assemblies via variable temperature liquid phase transmission electron microscopy and liquid resonant soft X-ray scattering

Abstract Here, we study the upper critical solution temperature triggered phase transition of thermally responsive poly(ethylene glycol)- block -poly(ethylene glycol) methyl ether acrylate- co -poly(ethylene glycol) phenyl ether acrylate- block -polystyrene nanoassemblies in isopropanol. To gain mechanistic insight into the organic solution-phase dynamics of the upper critical solution temperature polymer, we leverage variable temperature liquid-cell transmission electron microscopy correlated with variable temperature liquid resonant soft X-ray scattering. Heating above the upper critical solution temperature triggers a reduction in particle size and a morphological transition from a spherical core shell particle with a complex, multiphase core to a micelle with a uniform core and Gaussian polymer chains attached to the surface. These correlated solution phase methods, coupled with mass spectral validation and modeling, provide unique insight into these thermoresponsive materials. Moreover, we detail a generalizable workflow for studying complex, solution-phase nanomaterials via correlative methods.

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

Structure retrieval in liquid-phase electron scattering

Electron scattering on liquid samples has been enabled recently by the development of ultrathin liquid sheet technologies. The data treatment of liquid-phase electron scattering has been mostly reliant on methodologies developed for gas electron diffraction, in which theoretical inputs and empirical fittings are often needed to account for the atomic form factor and remove the inelastic scattering background. In this work, we present an alternative data treatment method that is able to retrieve the radial distribution of all the charged particle pairs without the need of either theoretical inputs or empirical fittings. Here, the merits of this new method are illustrated through the retrieval of real-space molecular structure from experimental electron scattering patterns of liquid water, carbon tetrachloride, chloroform, and dichloromethane.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Conductive Liquid Metal Vitrimer Composites for Reconfigurable and Recyclable Flexible Electronics

Liquid metal (LM) elastomer composites exhibit excellent functionality for stretchable electronics and wearables, but limited recycling and reuse pathways constrain their sustainable use. Here, to address these challenges amid growing concerns over electronic waste, a conductive LM–vitrimer composite is presented that enables recyclable and reconfigurable electronics. This soft and stretchable composite features uniformly distributed LM inclusions that enhance thermal conductivity by 6.53× and enable the formation of conductive traces with electrical self-healing, while the vitrimer provides structural restoration. The dynamic covalent bonds of the vitrimer matrix are leveraged for both reprocessing the composite and chemically recovering 94% of the LM. This liquid-state filler slightly reduces the vitrimer's stiffness to 2.63 MPa (≈20% lower), while maintaining its high stretchability (>135% strain) and thermal stability. It is further examined how ultrasonicated LM inclusions interact with the vitrimer matrix and demonstrate the composite's self-healing and recyclability through two distinct approaches: 1) thermomechanical reprocessing, which restores fragmented composites under heat and compression for circuit reconfiguration; and 2) chemical recycling, which recovers the embedded LM for reuse in fabricating new composites and redesigned circuitry. With the integration of recyclability and diverse functional capabilities, LM–vitrimer composites emerge as a promising material platform for sustainable, flexible electronics.

Han, Youngshang [Univ. of Washington, Seattle, WA ↗
DOE OSTI2019

Electron–hole liquid in a van der Waals heterostructure photocell at room temperature

In semiconductors, photo-excited charge carriers exist as a gas of electrons and holes, bound electron–hole pairs (excitons), biexcitons and trions. At sufficiently high densities, the non-equilibrium system of electrons (e-) and holes (h + ) may merge into an electronic liquid droplet. Here, we report on the electron–hole liquid in ultrathin MoTe2 photocells revealed through multi-parameter dynamic photoresponse microscopy (MPDPM). By combining rich visualization with comprehensive analysis of very large data sets acquired through MPDPM, we find that ultrafast laser excitation at a graphene–MoTe 2 –graphene interface leads to the abrupt formation of ring-like spatial patterns in the photocurrent response as a function of increasing optical power at T = 297 K. The sudden onset to these patterns, together with extreme sublinear power dependence and picosecond-scale photocurrent dynamics, provide strong evidence for the formation of a two-dimensional electron–hole liquid droplet. The electron–hole liquid, which features a macroscopic population of correlated electrons and holes, may offer a path to room-temperature optoelectronic devices that harness collective electronic phenomena.

phonons, thermal conductivity, thermoelectric, spi↗
DOE OSTI2023

All‐Liquid Reconfigurable Electronics Using Jammed MXene Interfaces

Abstract Rigid, solid‐state components represent the current paradigm for electronic systems, but they lack post‐production reconfigurability and pose ever‐increasing challenges to efficient end‐of‐life recycling. Liquid electronics may overcome these limitations by offering flexible in‐the‐field redesign and separation at end‐of‐life via simple liquid phase chemistries. Up to now, preliminary work on liquid electronics has focused on liquid metal components, but these devices still require an encapsulating polymer and typically use alloys of rare elements like indium. Here, using the self‐assembly of jammed 2D titanium carbide (Ti 3 C 2 T x ) MXene nanoparticles at liquid–liquid interfaces, “all‐liquid” electrically conductive sheets, wires, and simple functional devices are described including electromechanical switches and photodetectors. These assemblies combine the high conductivity of MXene nanosheets with the controllable form and reconfigurability of structured liquids. Such configurations can have applications not only in electronics, but also in catalysis and microfluidics, especially in systems where the product and substrate have affinity for solvents of differing polarity.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Evidence of a coupled electron-phonon liquid in NbGe 2

Whereas electron-phonon scattering relaxes the electron’s momentum in metals, a perpetual exchange of momentum between phonons and electrons may conserve total momentum and lead to a coupled electron-phonon liquid. Such a phase of matter could be a platform for observing electron hydrodynamics. Here we present evidence of an electron-phonon liquid in the transition metal ditetrelide, NbGe 2 , from three different experiments. First, quantum oscillations reveal an enhanced quasiparticle mass, which is unexpected in NbGe 2 with weak electron-electron correlations, hence pointing at electron-phonon interactions. Second, resistivity measurements exhibit a discrepancy between the experimental data and standard Fermi liquid calculations. Third, Raman scattering shows anomalous temperature dependences of the phonon linewidths that fit an empirical model based on phonon-electron coupling. We discuss structural factors, such as chiral symmetry, short metallic bonds, and a low-symmetry coordination environment as potential design principles for materials with coupled electron-phonon liquid.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Room-Temperature Electron–Hole Liquid in Monolayer MoS 2

Excitons in semiconductors are usually noninteracting and behave like an ideal gas, but may condense to a strongly correlated liquid-like state, i.e., electron–hole liquid (EHL), at high density and appropriate temperature. An EHL is a macroscopic quantum state with exotic properties and represents the ultimate attainable charge excitation density in steady states. It bears great promise for a variety of fields such as ultra-high-power photonics and quantum science and technology. However, the condensation of gas-like excitons to an EHL has often been restricted to cryogenic temperatures, which significantly limits the prospect of EHLs for use in practical applications. Herein we demonstrate the formation of an EHL at room temperature in monolayer MoS 2 by taking advantage of the monolayer’s extraordinarily strong exciton binding energy. Here, this work demonstrates the potential for the liquid-like state of charge excitations to be a useful platform for the studies of macroscopic quantum phenomena and the development of optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2019

MoS 2 Liquid Cell Electron Microscopy Through Clean and Fast Polymer-Free MoS 2 Transfer

Two dimensional (2D) materials have found various applications because of their unique physical properties. For example, graphene has been used as the electron transparent membrane for liquid cell transmission electron microscopy (TEM) due to its high mechanical strength and flexibility, single-atom thickness, chemical inertness, etc. Here, we report using 2D MoS 2 as a functional substrate as well as the membrane window for liquid cell TEM, which is enabled by our facile and polymer-free MoS 2 transfer process. This provides the opportunity to investigate the growth of Pt nanocrystals on MoS 2 substrates, which elucidates the formation mechanisms of such heterostructured 2D materials. We find that Pt nanocrystals formed in MoS 2 liquid cells have a strong tendency to align their crystal lattice with that of MoS 2 , suggesting a van der Waals epitaxial relationship. Importantly, we can study its impact on the kinetics of the nanocrystal formation. Here, the development of MoS 2 liquid cells will allow further study of various liquid phenomena on MoS 2 , and the polymer-free MoS 2 transfer process will be implemented in a wide range of applications.

36 MATERIALS SCIENCE↗
DOE OSTI2019

A Demonstration of Light-Augmented Calorimetry For Low-Energy Electrons in Liquid Argon.

The ability to resolve electrons with energies as low as 5 MeV in liquid argon (LAr) is important for future studies of astrophysical neutrinos in liquid argon time projection chambers (LArTPCs). Existing methods for measuring the energy of electromagnetic showers in LArTPCs rely solely on charge-based reconstruction which requires correcting for assumed electron-ion recombination. However, LAr scintillation light has the potential to improve energy reconstruction over charge-based measurements alone. Here we present a demonstration of a light-augmented calorimetric technique for low-energy electrons in LAr that foregoes the need to correct for recombination. A sample of Michel electrons from stopping cosmic muons is collected in LArIAT (Liquid Argon In A Testbeam), a single-phase LArTPC at Fermilab’s Test Beam Facility. Michel electron energy spectra are reconstructed using both a traditional charge-based approach as well as a more holistic approach that incorporates both charge and light. A maximum-likelihood fitter, using LArIAT’s well-tuned simulation, is developed for combining these quantities to achieve optimal energy resolution. A sample of isolated electrons with Ee < 60 MeV is then simulated to better determine the energy resolution of this topology. Due to LArIAT’s low wire noise, the addition of light is not found to significantly improve upon the achieved charged-based resolution of σ/E ≃ 9%/√E ⊕ 1%. However, additional samples are generated with varying wire noise levels and light yields to gauge the impact of light-augmented calorimetry in large LArTPCs such as DUNE and SBND. At a charge-readout signal-to-noise of ≈10, the energy resolution for low-energy electrons is improved by ∼15%, ∼25%, and ∼45% over charge-only calorimetry for average light yields of 10, 20, and 100 pe/MeV, respectively.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2019

Quasi-Two-Dimensional Electron-Hole Liquid in an Electric Field

The density functional theory is used to determine the ground state of quasi-two-dimensional electron-hole liquid in an external electric field. The Schrödinger equations for electrons and holes are solved numerically. The equilibrium density of electron-hole liquid in SiO{sub 2}/Si/SiO{sub 2} quantum wells is found as a function of the quantum well width and electric field strength.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Electron-beam-driven chemical processes during liquid phase transmission electron microscopy

Liquid phase (or liquid cell) transmission electron microscopy (LP-TEM) has been established as a powerful tool for observing dynamic processes in liquids at nanometer to atomic length scales. However, the simple act of observation using electrons irreversibly alters the nature of the sample. A clear understanding of electron beam-driven processes during LP-TEM is required to interpret in situ observations and utilize the electron beam as a stimulus to drive nanoscale dynamic processes. In this review, we discuss recent advances toward understanding, quantifying, mitigating, and harnessing electron beam-driven chemical processes occurring during LP-TEM. We will highlight progress in several research areas, including modeling electron beam-induced radiolysis near interfaces, electron beam-induced nanocrystal formation, and radiation damage of soft materials and biomolecules.

Woehl, Taylor J.↗
DOE OSTI2017

Theoretical Phase Diagram for the Room-Temperature Electron–Hole Liquid in Photoexcited Quasi-Two-Dimensional Monolayer MoS 2

Strong correlations between electrons and holes can drive the existence of an electron–hole liquid (EHL) state, typically at high carrier densities and low temperatures. The current emergence of quasi-two-dimensional (2D) monolayer transition metal dichalcogenides (TMDCs) provides ideal systems to explore the EHL state since ineffective screening of the out-of-plane field lines in these quasi-2D systems allows for stronger charge carrier correlations in contrast to conventional 3D bulk semiconductors and enables the existence of the EHL at high temperatures. In this work, we construct the phase diagram for the photoinduced first-order phase transition from a plasma of electron–hole pairs to a correlated EHL state in suspended monolayer MoS 2 . We illustrate that the quasi-2D nature of monolayer TMDCs and the ineffective screening of the out-of-plane field lines allow for this phase transition to occur at and above room temperature, thereby opening avenues for studying many-body phenomena without the constraint of cryogenics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Hydrodynamic electron transport in graphene Hall-bar devices

Here we consider hydrodynamic electron transport in the Hall-bar geometry. The theory is developed for systems with non-Galilean-invariant electron liquids. We show that inhomogeneity of the electron density induced by long-range disorder and gating leads to mixing between the hydrodynamic transport mode and transport relative to the electron liquid. For graphene systems near charge neutrality, these effects lead to strong coupling of the hydrodynamic flow to charge transport. As a result, the effective electrical conductivity of the system may significantly exceed the intrinsic conductivity of the electron liquid. We obtain analytic expressions for the thermoelectric transport coefficients of the system as a function of density in the full crossover region between clean and disorder-dominated regimes.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Amorphous-Phase-Mediated Crystallization of Ni Nanocrystals Revealed by High-Resolution Liquid-Phase Electron Microscopy

Nonclassical features of crystallization in solution have been recently identified both experimentally and theoretically. In particular, an amorphous-phase-mediated pathway is found in various crystallization systems as an important route, different from the classical nucleation and growth model. In this paper, we utilize high-resolution in situ transmission electron microscopy with graphene liquid cells to study amorphous-phase-mediated formation of Ni nanocrystals. An amorphous phase is precipitated in the initial stage of the reaction. Within the amorphous particles, crystalline domains nucleate and eventually form nanocrystals. In addition, unique crystallization behaviors, such as formation of multiple domains and dislocation relaxation, are observed in amorphous-phase-mediated crystallization. Theoretical calculations confirm that surface interactions can induce amorphous precipitation of metal precursors, which is analogous to the surface-induced amorphous-to-crystalline transformation occurring in biomineralization. In conclusion, our results imply that an unexplored nonclassical growth mechanism is important for the formation of nanocrystals.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Quasi-Two-Dimensional Electron–Hole Liquid in Si/SiO{sub 2} Quantum Wells

To calculate the energy and equilibrium density of electron-hole pairs in SiO{sub 2}/Si/SiO{sub 2} quantum wells (QWs), nonlinear Schrödinger equations for electrons and holes were numerically solved. Calculations were carried out for (100) and (111) silicon surfaces and various values of the QW width. It is shown that the binding energy of electron-hole pairs in a quasi-two-dimensional electron-hole liquid (EHL) is much higher than the binding energy in a three-dimensional EHL. The results of calculations are compared with the experimental results for a wide range of QW widths.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Quasi-Two-Dimensional Electron-Hole Liquid in a Magnetic Field

An analytical expression is derived for the energy of a three-component electron-hole liquid (EHL) in a magnetic field. Results of calculations of the EHL properties in Si/Si{sub 1–x}Ge{sub x}/Si quantum wells are presented. The influence of the magnetic field on the EHL properties and stability depending on the germanium concentration in the SiGe layer is revealed. It is found that the equilibrium electron-hole pair density strongly increases with the magnetic field. It is shown that the dependences of the filling factors of the Landau levels on the magnetic field are shaped as plateaus.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗