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Results for “Electronic properties and materials”

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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

In-situ observation of trapped carriers in organic metal halide perovskite films with ultra-fast temporal and ultra-high energetic resolutions

Abstract We in-situ observe the ultrafast dynamics of trapped carriers in organic methyl ammonium lead halide perovskite thin films by ultrafast photocurrent spectroscopy with a sub-25 picosecond time resolution. Upon ultrafast laser excitation, trapped carriers follow a phonon assisted tunneling mechanism and a hopping transport mechanism along ultra-shallow to shallow trap states ranging from 1.72–11.51 millielectronvolts and is demonstrated by time-dependent and independent activation energies. Using temperature as an energetic ruler, we map trap states with ultra-high energy resolution down to < 0.01 millielectronvolt. In addition to carrier mobility of ~4 cm 2 V −1 s −1 and lifetime of ~1 nanosecond, we validate the above transport mechanisms by highlighting trap state dynamics, including trapping rates, de-trapping rates and trap properties, such as trap density, trap levels, and capture-cross sections. In this work we establish a foundation for trap dynamics in high defect-tolerant perovskites with ultra-fast temporal and ultra-high energetic resolution.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Electronic transport properties of a lithium-decorated ZrTe 5 thin film

Through a combination of single crystal growth, experiments involving in situ deposition of surface adatoms, and complimentary modeling, we examine the electronic transport properties of lithiumdecorated ZrTe 5 thin films. We observe that the surface states in ZrTe 5 are robust against Li adsorption. Both the surface electron density and the associated Berry phase are remarkably robust to adsorption of Li atoms. Fitting to the Hall conductivity data reveals that there exist two types of bulk carriers: those for which the carrier density is insensitive to Li adsorption, and those whose density decreases during initial Li depositions and then saturates with further Li adsorption. We propose this dependence is due to the gating effect of a Li-adsorption-generated dipole layer at the ZrTe 5 surface.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Emergence of distinct electronic states in epitaxially-fused PbSe quantum dot superlattices

Abstract Quantum coupling in arrayed nanostructures can produce novel mesoscale properties such as electronic minibands to improve the performance of optoelectronic devices, including ultra-efficient solar cells and infrared photodetectors. Colloidal PbSe quantum dots (QDs) that self-assemble into epitaxially-fused superlattices (epi-SLs) are predicted to exhibit such collective phenomena. Here, we show the emergence of distinct local electronic states induced by crystalline necks that connect individual PbSe QDs and modulate the bandgap energy across the epi-SL. Multi-probe scanning tunneling spectroscopy shows bandgap modulation from 0.7 eV in the QDs to 1.1 eV at their necks. Complementary monochromated electron energy-loss spectroscopy demonstrates bandgap modulation in spectral mapping, confirming the presence of these distinct energy states from necking. The results show the modification of the electronic structure of a precision-made nanoscale superlattice, which may be leveraged in new optoelectronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Tunable spin and valley excitations of correlated insulators in Γ-valley moiré bands

Moiré superlattices formed from transition metal dichalcogenides (TMDs) have been shown to support a variety of quantum electronic phases that are highly tunable using applied electromagnetic fields. While the valley character of the low-energy states dramatically affects optoelectronic properties in the constituent TMDs, this degree of freedom has yet to be fully explored in moiré systems. Here, we establish twisted double bilayer WSe 2 as an experimental platform to study electronic correlations within Γ-valley moiré bands. Through a combination of local and global electronic compressibility measurements, we identify charge-ordered phases at multiple integer and fractional moiré band fillings ν. By measuring the magnetic field dependence of their energy gaps and the chemical potential upon doping, we reveal spin-polarized ground states with novel spin polaron quasiparticle excitations. In addition, an applied displacement field allows us to realize a new mechanism of metal-insulator transition at ν=–1 driven by tuning between Γ- and K-valley moiré bands. Together, our results demonstrate control over both the spin and valley character of the correlated ground and excited states in this system.

36 MATERIALS SCIENCE↗
DOE OSTI2020

DC Hall coefficient of the strongly correlated Hubbard model

The Hall coefficient is related to the effective carrier density and Fermi surface topology in non-interacting and weakly interacting systems. In strongly correlated systems, the relation between the Hall coefficient and single-particle properties is less clear. Clarifying this relation would give insight into the nature of transport in strongly correlated materials that lack well-formed quasiparticles. In this work, we investigate the DC Hall coefficient of the Hubbard model using determinant quantum Monte Carlo in conjunction with a recently developed expansion of magneto-transport coefficients in terms of thermodynamic susceptibilities. At leading order in the expansion, we observe a change of sign in the Hall coefficient as a function of temperature and interaction strength, which we relate to a change in the topology of the apparent Fermi surface. We also combine our Hall coefficient results with optical conductivity values to evaluate the Hall angle, as well as effective mobility and effective mass based on Drude theory of metals.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Nonreciprocal directional dichroism at telecom wavelengths

Magnetoelectrics with ultra-low symmetry and spin-orbit coupling are well known to display a number of remarkable properties including nonreciprocal directional dichroism. As a polar and chiral magnet, Ni 3 TeO 6 is predicted to host this effect in three fundamentally different configurations, although only two have been experimentally verified. Inspired by the opportunity to unravel the structure-property relations of such a unique light-matter interaction, we combined magneto-optical spectroscopy and first-principles calculations to reveal nonreciprocity in the toroidal geometry and compared our findings with the chiral configurations. We find that formation of Ni toroidal moments is responsible for the largest effects near 1.1 eV—a tendency that is captured by our microscopic model and computational implementation. At the same time, we demonstrate deterministic control of nonreciprocal directional dichroism in Ni 3 TeO 6 across the entire telecom wavelength range. This discovery will accelerate the development of photonics applications that take advantage of unusual symmetry characteristics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Emergent topological quantum orbits in the charge density wave phase of kagome metal CsV 3 Sb 5

The recently discovered kagome materials AV 3 Sb 5 (A = K, Rb, Cs) attract intense research interest in intertwined topology, superconductivity, and charge density waves (CDW). Although the in-plane 2 × 2 CDW is well studied, its out-of-plane structural correlation with the Fermi surface properties is less understood. In this work, we advance the theoretical description of quantum oscillations and investigate the Fermi surface properties in the three-dimensional CDW phase of CsV 3 Sb 5 . We derived Fermi-energy-resolved and layer-resolved quantum orbits that agree quantitatively with recent experiments in the fundamental frequency, cyclotron mass, and topology. We reveal a complex Dirac nodal network that would lead to a π Berry phase of a quantum orbit in the spinless case. However, the phase shift of topological quantum orbits is contributed by the orbital moment and Zeeman effect besides the Berry phase in the presence of spin-orbital coupling (SOC). Therefore, we can observe topological quantum orbits with a π phase shift in otherwise trivial orbits without SOC, contrary to common perception. Our work reveals the rich topological nature of kagome materials and paves a path to resolve different topological origins of quantum orbits.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Many-body enhancement of high-harmonic generation in monolayer MoS2

Abstract Many-body effects play an important role in enhancing and modifying optical absorption and other excited-state properties of solids in the perturbative regime, but their role in high harmonic generation (HHG) and other nonlinear response beyond the perturbative regime is not well-understood. We develop here an ab initio many-body method to study nonperturbative HHG based on the real-time propagation of the non-equilibrium Green’s function with the GW self energy. We calculate the HHG of monolayer MoS 2 and obtain good agreement with experiment, including the reproduction of characteristic patterns of monotonic and nonmonotonic harmonic yield in the parallel and perpendicular responses, respectively. Here, we show that many-body effects are especially important to accurately reproduce the spectral features in the perpendicular response, which reflect a complex interplay of electron-hole interactions (or exciton effects) in tandem with the many-body renormalization and Berry curvature of the independent quasiparticle bandstructure.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Pressure-induced concomitant topological and metal-insulator quantum phase transitions in Ce3Pd3Bi4

Abstract The electronic property and magnetic susceptibility of Ce 3 Pd 3 Bi 4 were systemically investigated from 18 to 290 K for varying values of cell volume using dynamic mean-field theory coupled with density functional theory. By extrapolating to zero temperature, the ground state of Ce 3 Pd 3 Bi 4 at ambient pressure is found to be a correlated semimetal due to insufficient hybridization. Upon applying pressure, the hybridization strength increases and a crossover to the Kondo insulator is observed at finite temperatures. The characteristic temperature signaling the formation of Kondo singlet, as well as the characteristic temperature associated with f -electron delocalization–localization change, simultaneously vanishes around a critical volume of 0.992 V 0 , suggesting that such metal–insulator transition is possibly associated with a quantum critical point. Finally, Wilson’s loop calculations indicate that the Kondo insulating side is topologically trivial, thus a topological transition also occurs across the quantum critical point.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Kramers nodal lines and Weyl fermions in SmAlSi

Kramers nodal lines (KNLs) have recently been proposed theoretically as a special type of Weyl line degeneracy connecting time-reversal invariant momenta. KNLs are robust to spin orbit coupling and are inherent to all non-centrosymmetric achiral crystal structures, leading to unusual spin, magneto-electric, and optical properties. However, their existence in in real quantum materials has not been experimentally established. Here we gather the experimental evidence pointing at the presence of KNLs in SmAlSi, a non-centrosymmetric metal that develops incommensurate spin density wave order at low temperature. Using angle-resolved photoemission spectroscopy, density functional theory calculations, and magneto-transport methods, we provide evidence suggesting the presence of KNLs, together with observing Weyl fermions under the broken inversion symmetry in the paramagnetic phase of SmAlSi. We discuss the nesting possibilities regarding the emergent magnetic orders in SmAlSi. Our results provide a solid basis of experimental observations for exploring correlated topology in SmAlSi.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Fermi-crossing Type-II Dirac fermions and topological surface states in NiTe 2

Transition-metal dichalcogenides (TMDs) offer an ideal platform to experimentally realize Dirac fermions. However, typically these exotic quasiparticles are located far away from the Fermi level, limiting the contribution of Dirac-like carriers to the transport properties. Here we show that NiTe 2 hosts both bulk Type-II Dirac points and topological surface states. The underlying mechanism is shared with other TMDs and based on the generic topological character of the Te p-orbital manifold. However, unique to NiTe 2 , a significant contribution of Ni d orbital states shifts the energy of the Type-II Dirac point close to the Fermi level. In addition, one of the topological surface states intersects the Fermi energy and exhibits a remarkably large spin splitting of 120 meV. Our results establish NiTe 2 as an exciting candidate for next-generation spintronics devices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Mott insulators with boundary zeros

The topological classification of electronic band structures is based on symmetry properties of Bloch eigenstates of single-particle Hamiltonians. In parallel, topological field theory has opened the doors to the formulation and characterization of non-trivial phases of matter driven by strong electron-electron interaction. Even though important examples of topological Mott insulators have been constructed, the relevance of the underlying non-interacting band topology to the physics of the Mott phase has remained unexplored. Here, we show that the momentum structure of the Green’s function zeros defining the “Luttinger surface" provides a topological characterization of the Mott phase related, in the simplest description, to the one of the single-particle electronic dispersion. Considerations on the zeros lead to the prediction of new phenomena: a topological Mott insulator with an inverted gap for the bulk zeros must possess gapless zeros at the boundary, which behave as a form of “topological antimatter” annihilating conventional edge states. Placing band and Mott topological insulators in contact produces distinctive observable signatures at the interface, revealing the otherwise spectroscopically elusive Green’s function zeros.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Observation of spin-momentum locked surface states in amorphous Bi 2 Se 3

Crystalline symmetries have played a central role in the identification and understanding of quantum materials. Here we investigate whether an amorphous analogue of a well-known three-dimensional strong topological insulator has topological properties in the solid state. We show that amorphous Bi 2 Se 3 thin films host a number of two-dimensional surface conduction channels. Our angle-resolved photoemission spectroscopy data are consistent with a dispersive two-dimensional surface state that crosses the bulk gap. Spin-resolved photoemission spectroscopy shows this state has an anti-symmetric spin texture, confirming the existence of spin-momentum locked surface states. We discuss these experimental results in light of theoretical photoemission spectra obtained with an amorphous topological insulator tight-binding model, contrasting it with alternative explanations. In conclusion, the discovery of spin-momentum locked surface states in amorphous materials opens a new avenue to characterize amorphous matter and triggers the search for an overlooked subset of quantum materials outside of current classification schemes.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Observation of electron orbital signatures of single atoms within metal-phthalocyanines using atomic force microscopy

Resolving the electronic structure of a single atom within a molecule is of fundamental importance for understanding and predicting chemical and physical properties of functional molecules such as molecular catalysts. However, the observation of the orbital signature of an individual atom is challenging. We report here the direct identification of two adjacent transition-metal atoms, Fe and Co, within phthalocyanine molecules using high-resolution noncontact atomic force microscopy (HR-AFM). HR-AFM imaging reveals that the Co atom is brighter and presents four distinct lobes on the horizontal plane whereas the Fe atom displays a “square” morphology. Pico-force spectroscopy measurements show a larger repulsion force of about 5 pN on the tip exerted by Co in comparison to Fe. Our combined experimental and theoretical results demonstrate that both the distinguishable features in AFM images and the variation in the measured forces arise from Co’s higher electron orbital occupation above the molecular plane. The ability to directly observe orbital signatures using HR-AFM should provide a promising approach to characterizing the electronic structure of an individual atom in a molecular species and to understand mechanisms of certain chemical reactions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Imaging gate-tunable Tomonaga–Luttinger liquids in 1H-MoSe 2 mirror twin boundaries

One-dimensional electron systems exhibit fundamentally different properties than higher-dimensional systems. For example, electron-electron interactions in one-dimensional electron systems have been predicted to induce Tomonaga-Luttinger liquid behaviour. Naturally occurring grain boundaries in single-layer transition metal dichalcogenides exhibit one-dimensional conducting channels that have been proposed to host Tomonaga-Luttinger liquids, but charge density wave physics has also been suggested to explain their behaviour. Clear identification of the electronic ground state of this system has been hampered by an inability to electrostatically gate such boundaries and tune their charge carrier concentration. Here we present a scanning tunnelling microscopy and spectroscopy study of gate-tunable mirror twin boundaries in single-layer 1H-MoSe 2 devices. Gating enables scanning tunnelling microscopy and spectroscopy for different mirror twin boundary electron densities, thus allowing precise characterization of electron-electron interaction effects. Visualization of the resulting mirror twin boundary electronic structure allows unambiguous identification of collective density wave excitations having two velocities, in quantitative agreement with the spin-charge separation predicted by finite-length Tomonaga-Luttinger liquid theory.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Existence of La-site antisite defects in LaMO 3 (M = Mn, Fe, and Co) predicted with many-body diffusion quantum Monte Carlo

The properties of LaMO 3 (M: 3d transition metal) perovskite crystals are significantly dependent on point defects, whether introduced accidentally or intentionally. The most studied defects in La-based perovskites are the oxygen vacancies and doping impurities on the La and M sites. Here, we identify that intrinsic antisite defects, the replacement of La by the transition metal, M, can be formed under M-rich and O-poor growth conditions, based on results of an accurate many-body ab initio approach. Our fixed-node diffusion Monte Carlo (FNDMC) calculations of LaMO 3 (M = Mn, Fe, and Co) find that such antisite defects can have low formation energies and are magnetized. Complementary density functional theory (DFT)-based calculations show that Mn antisite defects in LaMnO 3 may cause the p-type electronic conductivity. These features could affect spintronics, redox catalysis, and other broad applications. Our bulk validation studies establish that FNDMC reproduces the antiferromagnetic state of LaMnO 3 , whereas DFT with PBE (Perdew–Burke–Ernzerhof), SCAN (strongly constrained and appropriately normed), and the LDA+U (local density approximation with Coulomb U) functionals all favor ferromagnetic states, at variance with experiment.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Hopping frustration-induced flat band and strange metallicity in a kagome metal

The introduction of localized electronic states into a metal can alter its physical properties, for example enabling exotic metal physics including heavy fermion and strange metal behaviour. A common source of localized states in such systems are partially filled 4f and 5f shells because of the inherently compact nature of those orbitals. The interaction of electrons in these orbitals with the conduction sea is well described by the Kondo framework. However, there have also been observations of Kondo-like behaviour in 3d transition metal oxides and in 4d- and 5d-containing van der Waals heterostructures. This calls for a broader consideration of the physical requirements for Kondo systems. Here we show transport and thermodynamic hallmarks of heavy fermion and strange metal behaviour that arise in the kagome metal Ni3In, wherein the source of localized states is destructive interference-induced band flattening of partially filled Ni 3d states. With magnetic field and pressure tuning, here we also find evidence that the system is proximate to quantum criticality, extending the analogy to f-electron Kondo lattices. These observations highlight the role of hopping frustration in metallic systems as a potential source for strong correlations. Additionally, this suggests a lattice-driven approach to realizing correlated metals with non-trivial band topology.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Absence of Y-pocket in 1-Fe Brillouin zone and reversed orbital occupation imbalance in FeSe

The FeSe nematic phase has been the focus of recent research on iron-based superconductors (IBSs) due to its unusual properties, which are distinct from those of the pnictides. A series of theoretical/experimental studies were performed to determine the origin of the nematic phase. However, they yielded conflicting results and caused additional controversies. Here, we report the results of angle-resolved photoemission and X-ray absorption spectroscopy studies on FeSe detwinned by a piezo stack. We fully resolved band dispersions with orbital characters near the Brillouin zone (BZ) corner, and revealed an absence of any Fermi pocket at the Y point in the 1-Fe BZ. In addition, the occupation imbalance between d xz and d yz orbitals was the opposite of that of iron pnictides, consistent with the identified band characters. These results resolve issues associated with the FeSe nematic phase and shed light on the origin of the nematic phase in IBSs.

36 MATERIALS SCIENCE↗