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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Electronic mobility, doping, and defects in epitaxial BaZrS 3 chalcogenide perovskite thin films

We present the electronic transport properties of BaZrS 3 thin films grown epitaxially by gas-source molecular beam epitaxy. We observe n-type behavior in all samples, with carrier concentration ranging from 4 × 10 18 to 4 × 10 20 cm −3 at room temperature (RT). We observe a champion RT Hall mobility of 11.1 cm 2 V −1 s −1 , which is competitive with established thin-film photovoltaic absorbers. Temperature-dependent Hall mobility data show that phonon scattering dominates at room temperature, in agreement with computational predictions. X-ray diffraction data illustrate a correlation between mobility and antiphase boundary concentration, illustrating how microstructure can affect transport. Despite the well-established environmental stability of chalcogenide perovskites, we observe significant changes to electronic properties as a function of storage time in ambient conditions. With the help of secondary ion mass spectrometry measurements, we propose and support a defect mechanism that explains this behavior: as-grown films have a high concentration of sulfur vacancies that are shallow donors (V ⋅ S or V ⋅⋅ S ), which are converted into neutral oxygen defects (O$^{×}_{S}$) upon air exposure. We discuss the relevance of this defect mechanism within the larger context of chalcogenide perovskite research, and we identify means to stabilize the electronic properties.

Van Sambeek, Jack [Massachusetts Institute of Tech↗
DOE OSTI2023

Non-Markovian Hole Excess Noise in Avalanche Amorphous Selenium Thin Films

Enhancing the signal-to-noise ratio in avalanche photodiodes by utilizing impact ionization gain requires materials exhibiting low excess noise factors. Amorphous selenium (a-Se) as a wide bandgap at ~2.1 eV, a solid-state avalanche layer, demonstrates single-carrier hole impact ionization gain and manifests ultralow thermal generation rates. A comprehensive study of the history dependent and non-Markovian nature of hot hole transport in a-Se was modeled using a Monte Carlo (MC) random walk of single hole free flights, interrupted by instantaneous phonon, disorder, hole–dipole, and impact-ionization scattering interactions. The hole excess noise factors were simulated for 0.1–15 μm a-Se thin-films as a function of mean avalanche gain. The hole excess noise factors in a-Se decreases with an increase in electric field, impact ionization gain, and device thickness. The history dependent nature of branching of holes is explained using a Gaussian avalanche threshold distance distribution and the dead space distance, which increases determinism in the stochastic impact ionization process. An ultralow non-Markovian excess noise factor of ~1 was simulated for 100 nm a-Se thin films corresponding to avalanche gains of 1000. Future detector designs can utilize the nonlocal/non-Markovian nature of the hole avalanche in a-Se, to enable a true solid-state photomultiplier with noiseless gain.

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

Scale-invariant machine-learning model accelerates the discovery of quaternary chalcogenides with ultralow lattice thermal conductivity

We design an advanced machine-learning (ML) model based on crystal graph convolutional neural network that is insensitive to volumes (i.e., scale) of the input crystal structures to discover novel quaternary chalcogenides, AMM'Q 3 (A/M/M' = alkali, alkaline earth, post-transition metals, lanthanides, and Q = chalcogens). These compounds are shown to possess ultralow lattice thermal conductivity (κ l ), a desired requirement for thermal-barrier coatings and thermoelectrics. Upon screening the thermodynamic stability of ~1 million compounds using the ML model iteratively and performing density-functional theory (DFT) calculations for a small fraction of compounds, we discover 99 compounds that are validated to be stable in DFT. Taking several DFT-stable compounds, we calculate their κ l using Peierls–Boltzmann transport equation, which reveals ultralow κ l (<2 Wm -1 K -1 at room temperature) due to their soft elasticity and strong phonon anharmonicity. Our work demonstrates the high efficiency of scale-invariant ML model in predicting novel compounds and presents experimental-research opportunities with these new compounds.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Crystalline Structure-Dependent Mechanical and Thermoelectric Performance in Ag 2 Se 1–x S x System

Self-powered wearable electronics require thermoelectric materials simultaneously with a high dimensionless figure of merit (zT) and good flexibility to convert the heat discharged by the human body into electricity. Ag 2 (S,Se)-based semiconducting materials can well satisfy these requirements, and thus, they are attracting great attention in thermoelectric society recently. Ag 2 (S,Se) crystalizes in an orthorhombic structure or monoclinic structure, depending on the detailed S/Se atomic ratio, but the relationship between its crystalline structure and mechanical/thermoelectric performance is still unclear to date. In this study, a series of Ag 2 Se 1–x S x (x = 0, 0.1, 0.2, 0.3, 0.4, and 0.45) samples were prepared and their mechanical and thermoelectric performance dependence on the crystalline structure was systematically investigated. x = 0.3 in the Ag 2 Se 1–x S x system was found to be the transition boundary between orthorhombic and monoclinic structures. Mechanical property measurement shows that the orthorhombic Ag 2 Se 1–x S x samples are brittle while the monoclinic Ag 2 Se 1–x S x samples are ductile and flexible. In addition, the orthorhombic Ag 2 Se 1–x S x samples show better electrical transport performance and higher zT than the monoclinic samples under a comparable carrier concentration, most likely due to their weaker electron-phonon interactions. This study sheds light on the further development of flexible inorganic TE materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Significant phase-space-driven thermal transport suppression in BC8 silicon

The BC8 silicon allotrope has a lattice thermal conductivity 1–2 orders of magnitude lower than that of diamond-cubic silicon. In the current work, the phonon density of states, phonon dispersion, and lattice thermal conductivity are investigated by inelastic neutron scattering measurements and first-principles calculations. Flat phonon bands are found to play a critical role in the reduction of lattice thermal conductivity in BC8–Si. Such bands in the low-energy range enhance the phonon scattering between acoustic and low-energy optical phonons, while bands in the intermediate-energy range act as a scattering bridge between the high- and low-energy optical phonons. Further, they significantly enlarge the phonon-phonon scattering phase space and reduces the lattice thermal conductivity in this novel silicon allotrope. This work provides insights into the significant reduction of the lattice thermal conductivity in BC8–Si, thus expanding the understanding of novel silicon allotropes and their development for electronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2025

High-throughput computational framework for high-order anharmonic thermal transport in cubic and tetragonal crystals

Accurate first-principles prediction of lattice thermal conductivity (κL) remains challenging in identifying materials with extreme thermal behavior. While the harmonic approximation with three-phonon scattering (HA + 3ph) is now routine, reliable κL prediction often requires higher-order anharmonic effects, including self-consistent phonon renormalization, three- and four-phonon scattering, and off-diagonal heat flux (SCPH + 3, 4ph + OD). We present a state-of-the-art high-throughput workflow that unifies these effects and apply it to 773 cubic and tetragonal crystals spanning diverse chemistries and structures. From 562 dynamically stable compounds, we assess the hierarchical impacts of higher-order anharmonicity. For around 60% of materials, HA + 3ph predictions closely match those from SCPH + 3, 4ph + OD. SCPH generally increases κ L , by over 8 times in extreme cases, whereas four-phonon scattering universally suppresses κ L , sometimes to 15% of the HA + 3ph value. Off-diagonal contributions are negligible in high-κ L systems but can rival diagonal terms in highly anharmonic low-κ L compounds. We highlight four case studies, Rb 2 TlAlH 6 , Cu 3 VSe 4 , CuBr, and KTlCl 4 , that exhibit distinct extreme behaviors. This work delivers not only a robust workflow for high-fidelity κL dataset but also a quantitative framework to determine when higher-order effects are essential. The hierarchy of κ L results, from the HA + 3ph to SCPH + 3, 4ph + OD level, offers a scalable, interpretable route to discovering next-generation extreme thermal materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Magnetosynthesis effect on magnetic order, phonons, and magnons in single-crystal Sr 2 ⁢ IrO 4

It was shown earlier that applying a magnetic field during the growth of Sr 2 IrO 4 , also known as “field-alteration”, induces significant changes to its structural, magnetic, and transport properties. However, the microscopic nature of these changes is enigmatic. Here, in this study, we employed resonant elastic and inelastic x-ray scattering, as well as Raman scattering, to investigate samples from two batches of Sr 2 IrO 4 grown in magnetic fields of different strengths. Our findings reveal that samples grown in a weaker magnetic field have similar magnetic order to non-altered samples, whereas those grown in a stronger field show a different stacking of weak in-plane ferromagnetic moments. Additionally, we observed significant softening and broadening of select Raman-active phonons in the field altered samples, with a stronger effect in the samples grown in the stronger field. We discuss insights that our results provide into the microscopic nature of field-alteration in Sr 2 IrO 4 .

36 MATERIALS SCIENCE↗
DOE OSTI2023

Extended linear-in- T resistivity due to electron-phason scattering in moiré superlattices

Due to its incommensurate nature, moiré superlattices host not only acoustic phonons but also another type of soft collective modes called phasons. Here, we investigate the impact of electron-phason scattering on the transport properties of moiré systems. We show that the resistivity can scale linearly with temperature down to temperatures much lower than the Bloch-Grüneisen scale defined by electron kinematics on the Fermi surface. This result stems from the friction between layers, which transfers phason spectral weight to a broad diffusive low-energy peak in the mechanical response of the system. As a result, phason scattering becomes a very efficient channel for entropy production at low temperatures. We also consider the contributions of phasons to thermodynamic properties at low temperatures and find a “metallic-like” linear-in-T behavior for the specific heat, despite the fact that this behavior is due to mechanical and not electronic degrees of freedom. Finally, we discuss the implications of this finding to reports of linear-in-T resistivity in the phase diagram of twisted bilayer graphene.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Accelerated discovery of a large family of quaternary chalcogenides with very low lattice thermal conductivity

The development of efficient thermal energy management devices such as thermoelectrics and barrier coatings often relies on compounds having low lattice thermal conductivity (κ l ). Here, we present the computational discovery of a large family of 628 thermodynamically stable quaternary chalcogenides, AMM'Q 3 (A = alkali/alkaline earth/post-transition metals; M/M' = transition metals, lanthanides; Q = chalcogens) using high-throughput density functional theory (DFT) calculations. We validate the presence of low κ l in these materials by calculating κ l of several predicted stable compounds using the Peierls–Boltzmann transport equation. Our analysis reveals that the low κ l originates from the presence of either a strong lattice anharmonicity that enhances the phonon-scatterings or rattler cations that lead to multiple scattering channels in their crystal structures. Our thermoelectric calculations indicate that some of the predicted semiconductors may possess high energy conversion efficiency with their figure-of-merits exceeding 1 near 600 K. Our predictions suggest experimental research opportunities in the synthesis and characterization of these stable, low κ l compounds.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Simultaneous thickness and thermal conductivity measurements of thinned silicon from 100 nm to 17 μm

Studies of size effects on thermal conductivity typically necessitate the fabrication of a comprehensive film thickness series. In this Letter, we demonstrate how material fabricated in a wedged geometry can enable similar, yet higher-throughput measurements to accelerate experimental analysis. Frequency domain thermoreflectance (FDTR) is used to simultaneously determine the thermal conductivity and thickness of a wedged silicon film for thicknesses between 100 nm and 17 μm by considering these features as fitting parameters in a thermal model. FDTR-deduced thicknesses are compared to values obtained from cross-sectional scanning electron microscopy, and corresponding thermal conductivity measurements are compared against several thickness-dependent analytical models based upon solutions to the Boltzmann transport equation. Our results demonstrate how the insight gained from a series of thin films can be obtained via fabrication of a single sample.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Persistent hot carrier diffusion in boron arsenide single crystals imaged by ultrafast electron microscopy

Cubic boron arsenide (BAs) is promising for microelectronics thermal management because of its high thermal conductivity. Recently, its potential as an optoelectronic material is also being explored. However, it remains challenging to measure its photocarrier transport properties because of small sizes of available high-quality crystals. Here, we use scanning ultrafast electron microscopy (SUEM) to directly visualize the diffusion of photocarriers in BAs single crystals. Surprisingly, we observed ambipolar diffusion at low optical fluence with persistent hot carrier dynamics for above 200 ps, which can likely be attributed to the large frequency gap between acoustic and optical phonons, the same feature that is responsible for the high thermal conductivity. At higher optical fluence, we observed spontaneous electron-hole separation. Our results show BAs is an attractive optoelectronic material combining high thermal conductivity and excellent photocarrier transport properties. Finally, our study also demonstrates the capability of SUEM to probe photocarrier transport in emerging materials.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Comment on “Superconductivity at low density near a ferroelectric quantum critical point: Doped SrTiO 3 ”

Wölfle and Balatsky have proposed a microscopic pairing mechanism for doped SrTiO 3 (STO) based on the gradient coupling of electronic density to the soft transverse optical (TO) phonon mode. Since this coupling to TO phonons is usually weak, this conclusion is surprising, especially for a low-density superconductor such as STO, where the density of states is small. A crucial step in the argument made by Wölfle and Balatsky is that the displacement vector of the TO mode is not strictly perpendicular to the momentum vector, making a deformation coupling possible. We show that they have made a mistake in computing the eigenvector and have grossly overestimated this lack of orthogonality. When corrected, the coupling is negligible. We also use transport data to put upper bounds on the coupling constant which are much smaller than the estimate by Wölfle and Balatsky. Lastly, we also object to their use of the Eliashberg equation when the phonon frequency is larger than the Fermi energy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Effective theory of superconductivity in strongly coupled amorphous materials

A theory of phonon-mediated superconductivity in strong-coupling amorphous materials is developed based on an effective description of structural disorder and its effect on the vibrational spectrum. The theory accounts for the diffusivelike transport of vibrational excitations due to disorder-induced scattering within the Eliashberg theory of strong-coupling superconductivity. The theory provides a good analytical description of the Eliashberg function $α^2F(ω)$ in comparison with experiments and allows one to disentangle the effects of transverse and longitudinal excitations on the Eliashberg function. In particular, it shows that the transverse excitations play a crucial role in driving an increase or excess in the Eliashberg function at low energy, which is related to the boson peak phenomenon in vibrational spectra of glasses. This low-energy excess, on the one hand, drives an enhancement of the electron-phonon coupling but at the same time reduces the characteristic energy scale $ω_{\text{log}}$ in the Allen-Dynes formula. As a consequence, the nonmonotonicity of $T_c$ as a function of alloying (disorder) in Pb-based systems can be rationalized. Further, the case of Al-based systems, where disorder increases $T_c$ from the start, is also analyzed. General material-design principles for enhancing $T_c$ in amorphous superconductors are presented.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Hot Carrier Dynamics in Low-Dimensional Systems

This program aimed on a fundamental level to understand the nature of hot carrier transport and thermalization in both hybrid metal halide perovskites and type-II inorganic semiconductors; as well as, to assess the role of confinement, electron phonon interactions, and the dynamic nature of these systems under external perturbations.

14 SOLAR ENERGY↗
NASA NTRS2009

Computer Code for Nanostructure Simulation

Due to their small size, nanostructures can have stress and thermal gradients that are larger than any macroscopic analogue. These gradients can lead to specific regions that are susceptible to failure via processes such as plastic deformation by dislocation emission, chemical debonding, and interfacial alloying. A program has been developed that rigorously simulates and predicts optoelectronic properties of nanostructures of virtually any geometrical complexity and material composition. It can be used in simulations of energy level structure, wave functions, density of states of spatially configured phonon-coupled electrons, excitons in quantum dots, quantum rings, quantum ring complexes, and more. The code can be used to calculate stress distributions and thermal transport properties for a variety of nanostructures and interfaces, transport and scattering at nanoscale interfaces and surfaces under various stress states, and alloy compositional gradients. The code allows users to perform modeling of charge transport processes through quantum-dot (QD) arrays as functions of inter-dot distance, array order versus disorder, QD orientation, shape, size, and chemical composition for applications in photovoltaics and physical properties of QD-based biochemical sensors. The code can be used to study the hot exciton formation/relation dynamics in arrays of QDs of different shapes and sizes at different temperatures. It also can be used to understand the relation among the deposition parameters and inherent stresses, strain deformation, heat flow, and failure of nanostructures.

Filikhin, Igor↗
DOE OSTI2020

Anomalous phonon-mode dependence in polarized Raman spectroscopy of the topological Weyl semimetal TaP

Topological Weyl semimetals (WSMs) have attracted widespread interest due to the chiral Weyl fermions and surface Fermi arcs that enable unique optical and transport phenomena. In this work, we present angle-resolved Raman spectroscopy of TaP, a prototypical noncentrosymmetric WSM, for five excitation wavelengths ranging from 364 to 785 nm. The Raman-active modes, $A_1$, $B^1_1$, and $B^2_1$ modes, exhibit two main unique features beyond the conventional Raman theory. First, the relative intensities of Raman-active modes change as a function of the excitation wavelength. Second, angle-resolved polarized Raman spectra show systematic deviation from the Raman tensor theory. In particular, the $B^1_1$ mode is absent for 633-nm excitation, whereas the $B^2_1$ mode shows an unusual twofold symmetry instead of a fourfold symmetry for 488-, 532-, and 633-nm excitations. Finally, these unconventional phenomena are attributed to the interference effect in the Raman process owing to the existence of multiple carrier pockets with almost the same energy but different symmetries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. In this paper, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron–phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron–phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Boosting Thermoelectric Performance in Nanocrystalline Ternary Skutterudite Thin Films through Metallic CoTe 2 Integration

Metal–semiconductor nanocomposites have emerged as a viable strategy for concurrently tailoring both thermal and electronic transport properties of established thermoelectric materials, ultimately achieving synergistic performance. In this investigation, a series of nanocomposite thin films were synthesized, embedding metallic cobalt telluride (CoTe 2 ) nanophase within the nanocrystalline ternary skutterudite (Co(Ge 1.22 Sb 0.22 )Te 1.58 or CGST) matrix. Our approach harnessed composition fluctuation-induced phase separation and in situ growth during thermal annealing to seamlessly integrate the metallic phase. The distinctive band structures of both materials have developed an ohmic-type contact characteristic at the interface, which raised carrier density considerably yet negligibly affected the mobility counterpart, leading to a substantial improvement in electrical conductivity. The intricate balance in transport properties is further influenced by the metallic CoTe 2 phase’s role in diminishing lattice thermal conductivity. The presence of the metallic phase instigates enhanced phonon scattering at the interface boundaries. Consequently, a 2-fold enhancement in the thermoelectric figure of merit (zT ~ 1.30) is attained with CGST-7 wt. % CoTe 2 nanocomposite film at 655 K compared to that of pristine CGST.

36 MATERIALS SCIENCE↗