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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Controlling thermoelectric transport via native defects in the diamond-like semiconductors Cu 2 HgGeTe 4 and Hg 2 GeTe 4

Diamond like semiconductors (DLS) have emerged as candidates for thermoelectric energy conversion. Towards understanding and optimizing performance, we present a comprehensive investigation of the electronic properties of two DLS phases, quaternary Cu 2 HgGeTe 4 and related ordered vacancy compound Hg 2 GeTe 4 , including thermodynamic stability, defect chemistry, and transport properties. To establish the thermodynamic link between the related but distinct phases, the stability region for both is visualized in chemical potential space. In spite of their similar structure and bonding, we show that the two materials exhibit reciprocal behaviors for dopability. Cu 2 HgGeTe 4 is degenerately p-type in all environments despite its wide stability region, due to the presence of low-energy acceptor defects V Cu and Cu Hg and is resistant to extrinsic n-type doping. Meanwhile Hg 2 GeTe 4 has a narrow stability region and intrinsic behavior due to the relatively high formation energy of native defects, but presents an opportunity for bi-polar doping. While these two compounds have similar structure, bonding, and chemical constituents, the reciprocal nature of their dopability emerges from significant differences in band edge positions. A Brouwer band diagram approach is utilized to visualize the role of native defects on carrier concentrations, dopability, and transport properties. Here this study elucidates the doping asymmetry between two solid-solution forming DLS phases Cu 2 HgGeTe 4 and Hg 2 GeTe 4 by revealing the defect chemistry of each compound, and suggests design strategies for defect engineering of DLS phases.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2024

First-principles calculation of lattice distortion, electronic structure, and bonding properties of GeTe-based and PbSe-based high-entropy chalcogenides

The massive amount of wasted heat energy from industry has pushed the development of thermoelectric (TE) materials that directly convert heat into electricity to a new level of concern. Recently, multicomponent alloys such as GeTe-based and PbSe-based high-entropy (HE) chalcogenides have attracted a great deal of attention due to their potential application as TE materials. The nature of the interatomic bonding, lattice distortion (LD), and the electronic structure in this class of materials is not fully understood. Herein, we report a comprehensive computational investigation of nine GeTe-based HE alloys with eight metallic elements (Ag, Pb, Sb, Bi, Cu, Cd, Mn, and Sn) with large supercells of 1080 atoms each; seven PbSe-based HE solid solutions: Pb0.99−ySb0.012SnySe1−2xTexSx (x = 0.1, 0.2, 0.25, 0.3, 0.35, 0.4, 0.45, with y = 0) with supercells of 1000 atoms each; and five Pb0.99−ySb0.012SnySe1−2xTexSx (y = 0.05, 0.1, 0.15, 0.2, 0.25 with x = 0.25) solid solutions with supercells of 1000 atoms each. All these HE models are theoretically investigated for the first time. The electronic structure, interatomic bonding, charge transfer, and lattice distortion (LD) are investigated by first-principles calculations based on density functional theory. Multicomponent HE alloys can cause a significant LD, which affects their mechanical, thermal, and TE properties. The calculations for the GeTe-based HE chalcogenides showed that they are semiconductors with a narrow bandgap, except for m8, which has a semi-metallic characteristic, and this makes them good candidates for TE applications. For most of these models, the Fermi level shifts upward and locates deeply in the conduction bands, resulting in the enhancement of the electrical conductivity (σ). The bonding properties showed that most bonds in m5 are more dispersed, indicating highest LD and lower lattice thermal conductivity. For PbSe-based HE solid solutions, the LD calculations showed that the models Pb0.99Sb0.012Se0.5Te0.25S0.25 and Pb0.89Sb0.012Sn0.1Se0.5Te0.25S0.25 have the higher LD, and thus a lower lattice thermal conductivity. Such investigations are in high demand since it enables us to design new HE chalcogenides for TE applications. We use the novel concept of total bond order density as a single quantum mechanical metric to characterize the internal cohesion of these HE alloys and correlate with calculated properties, especially the mechanical properties. This work provides a solid database for HE chalcogenides and a road map for many potential applications. Moreover, the computational procedure we developed can be used to design new HE chalcogenides for specific TE applications.

Physics↗
DOE OSTI2021

Tuning the room temperature ferromagnetism in Fe 5 GeTe 2 by arsenic substitution

In order to tune the magnetic properties of the cleavable high-Curie temperature ferromagnet Fe$_{5-x}$GeTe 2 , the effect of increasing the electron count through arsenic substitution has been investigated. Small additions of arsenic (2.5% and 5%) seemingly enhance ferromagnetic order in polycrystalline samples by quenching fluctuations on one of the three magnetic sublattices, whereas larger As concentrations decrease the ferromagnetic Curie temperature (T C ) and saturation magnetization. Furthermore, this work also describes the growth and characterization of Fe 4.8 AsTe 2 single crystals that are structurally analogous to Fe$_{5-x}$GeTe 2 but with some phase stability complications. Magnetization measurements reveal dominant antiferromagnetic behavior in Fe 4.8 AsTe 2 with a Néel temperature of $T_{\textrm{N}} \approx$ 42 K. A field-induced spin-flop below T N results in a switch from negative to positive magnetoresistance, with significant hysteresis causing butterfly-shaped resistance loops. In addition to reporting the properties of Fe 4.8 AsTe 2 , this work shows the importance of manipulating the individual magnetic sublattices in Fe$_{5-x}$GeTe 2 and motivates further efforts to control the magnetic properties in related materials by fine tuning of the Fermi energy or crystal chemistry.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Room-temperature in-plane ferromagnetism in Co-substituted Fe 5 GeTe 2 investigated by magnetic x-ray spectroscopy and microscopy

The exploration of two-dimensional (2D) van der Waals ferromagnets has revealed intriguing magnetic properties with significant potential for spintronics applications. In this study, we examine the magnetic properties of Co-doped Fe 5 GeTe 2 using x-ray photoemission electron microscopy (XPEEM) and x-ray magnetic circular dichroism (XMCD), complemented by density functional theory calculations. Our XPEEM measurements reveal that the Curie temperature (T c ) of a bilayer of (Co x Fe 1-x ) 5-δ GeTe 2 (with x = 0.28) reaches ∼300 K—a notable enhancement over most 2D ferromagnets in the ultrathin limit. Interestingly, the T c shows only a small dependence on film thickness (bulk T c ≈ 340 K), in line with the observed in-plane (IP) magnetic anisotropy and robust IP exchange coupling. XMCD measurements indicate that the spin moments for both Fe and Co are significantly reduced compared to the theoretical values. These insights highlight the potential of Co-doped Fe 5 GeTe 2 for stable, high-temperature ferromagnetic applications in 2D materials.

(Co0.28Fe0.72)5GeTe2↗
DOE OSTI2021

Tuning 2D magnetism in Fe 3+X GeTe 2 films by element doping

Two-dimensional (2D) ferromagnetic materials have been discovered with tunable magnetism and orbital-driven nodal-line features. Controlling the 2D magnetism in exfoliated nanoflakes via electric/magnetic fields enables a boosted Curie temperature (T C ) or phase transitions. One of the challenges, however, is the realization of high T C 2D magnets that are tunable, robust and suitable for large scale fabrication. Here, we report molecular-beam epitaxy growth of wafer-scale Fe 3+X GeTe 2 films with T C above room temperature. By controlling the Fe composition in Fe 3+X GeTe 2 , a continuously modulated T C in a broad range of 185–320 K has been achieved. This widely tunable T C is attributed to the doped interlayer Fe that provides a 40% enhancement around the optimal composition X = 2. We further fabricated magnetic tunneling junction device arrays that exhibit clear tunneling signals. Our results show an effective and reliable approach, i.e. element doping, to producing robust and tunable ferromagnetism beyond room temperature in a large-scale 2D Fe 3+X GeTe 2 fashion.

2D ferromagnetic material↗
DOE OSTI2020

Materials Data on GeTe by Materials Project

GeTe crystallizes in the orthorhombic Pbcn space group. The structure is one-dimensional and consists of four GeTe ribbons oriented in the (1, 0, 0) direction. Ge2+ is bonded in a 4-coordinate geometry to three equivalent Te2- atoms. There are two shorter (2.78 Å) and one longer (2.86 Å) Ge–Te bond lengths. Te2- is bonded in a 3-coordinate geometry to three equivalent Ge2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on GeTe by Materials Project

GeTe crystallizes in the orthorhombic Pnma space group. The structure is two-dimensional and consists of two GeTe sheets oriented in the (0, 0, 1) direction. Ge2+ is bonded in a 6-coordinate geometry to three equivalent Te2- atoms. There are one shorter (2.79 Å) and two longer (2.81 Å) Ge–Te bond lengths. Te2- is bonded in a 3-coordinate geometry to three equivalent Ge2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Writing and Detecting Topological Charges in Exfoliated Fe 5– x GeTe 2

Fe 5–x GeTe 2 is a promising two-dimensional (2D) van der Waals (vdW) magnet for practical applications, given its magnetic properties. These include Curie temperatures above room temperature, and topological spin textures–TST (both merons and skyrmions), responsible for a pronounced anomalous Hall effect (AHE) and its topological counterpart (THE), which can be harvested for spintronics. Here, we show that both the AHE and THE can be amplified considerably by just adjusting the thickness of exfoliated Fe 5–x GeTe 2 , with THE becoming observable even in zero magnetic field due to a field-induced unbalance in topological charges. Using a complementary suite of techniques, including electronic transport, Lorentz transmission electron microscopy, and micromagnetic simulations, we reveal the emergence of substantial coercive fields upon exfoliation, which are absent in the bulk, implying thickness-dependent magnetic interactions that affect the TST. We detected a “magic” thickness t ≈ 30 nm where the formation of TST is maximized, inducing large magnitudes for the topological charge density (~6.45 × 10 20 cm –2 ), and the concomitant anomalous (ρ xy A,max ≃22.6 μΩ cm) and topological (ρ xy u,T 1≃5 μΩ cm) Hall resistivities at T ≈ 120 K. These values for ρ xy A,max and ρ xy u,T are higher than those found in magnetic topological insulators and, so far, the largest reported for 2D magnets. Furthermore, the hitherto unobserved THE under zero magnetic field could provide a platform for the writing and electrical detection of TST aiming at energy-efficient devices based on vdW ferromagnets.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Anomalous lattice thermal conductivity increase with temperature in cubic GeTe correlated with strengthening of second-nearest neighbor bonds

Understanding thermal transport mechanisms in phase change materials is critical to elucidating the microscopic picture of phase transitions and advancing thermal energy conversion and storage. Experiments consistently show that cubic phase germanium telluride (GeTe) has an unexpected increase in lattice thermal conductivity with rising temperature. Despite its ubiquity, resolving its origin has remained elusive. In this work, we carry out temperature-dependent lattice thermal conductivity calculations for cubic GeTe through efficient, high-order machine-learned models and additional corrections for coherence effects. We corroborate the calculated phonon properties with our inelastic X-ray scattering measurements. Our calculated lattice thermal conductivity values agree well with experiments and show a similar increasing trend. Through additional bonding strength calculations, we propose that a major contributor to the increasing lattice thermal conductivity is the strengthening of second-nearest neighbor interactions. The findings herein serve to deepen our understanding of thermal transport in phase-change materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Dynamic crystallography reveals spontaneous anisotropy in cubic GeTe

Cubic energy materials such as thermoelectrics or hybrid perovskite materials are often understood to be highly disordered. In GeTe and related IV–VI compounds, this is thought to provide the low thermal conductivities needed for thermoelectric applications. Since conventional crystallography cannot distinguish between static disorder and atomic motions, we develop the energy-resolved variable-shutter pair distribution function technique. This collects structural snapshots with varying exposure times, on timescales relevant for atomic motions. In disagreement with previous interpretations, we find the time-averaged structure of GeTe to be crystalline at all temperatures, but with anisotropic anharmonic dynamics at higher temperatures that resemble static disorder at fast shutter speeds, with correlated ferroelectric fluctuations along the <100> c direction. We show that this anisotropy naturally emerges from a Ginzburg–Landau model that couples polarization fluctuations through long-range elastic interactions. By accessing time-dependent atomic correlations in energy materials, we resolve the long-standing disagreement between local and average structure probes and show that spontaneous anisotropy is ubiquitous in cubic IV–VI materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Surface magnetism in Fe 3 GeTe 2 van der Waals ferromagnet

The surface magnetization of Fe 3 GeTe 2 was examined by low-energy electron microscopy (LEEM) using an off-normal incidence electron beam. We found that the 180o domain walls are of Bloch type. Temperature-dependent LEEM measurements yield a surface magnetization with a surface critical exponent β1 = 0.79±0.02. This result is consistent with surface magnetism in the 3D semi-infinite Heisenberg (β1 = 0.84±0.01) or Ising (β1 = 0.78±0.02) models, which is distinctly different from the bulk exponent (β = 0.34±0.07). Further, the measurements reveal the power of LEEM with a tilted beam to determine magnetic domain structure in quantum materials, without need for the use of spin-polarized electrons. Single crystal diffraction measurements reveal inversion symmetry-breaking weak peaks and yield space group P-6m2. This Fe site defect-derived loss of inversion symmetry enables the formation of skyrmions in this Fe 3 GeTe 2 crystal.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Chemical control of the Rashba spin splitting size of α-GeTe(111) surface states by adjusting the potential at the topmost atomic layer

As control of the Rashba spin splitting size is highly desirable for spintronic devices, intensive studies have been performed to vary the splitting size by, for example, applying an electric field or designing novel heterostructures. However, direct observation of Rashba spin splitting size change via spectroscopic measurements has not been done so far. Here, we report results of angle-resolved photoemission studies on ferroelectric α-GeTe(111). We observe that the Rashba splitting size of α-GeTe(111) surface states is reduced upon dosing with potassium (K) which has a very low electron affinity. Based on density functional theory calculations, we find that the electric potential energy at the topmost atomic layer and the surface potential energy barrier is reduced upon K dosing. Furthermore, this change in the surface potential induces both delocalization of the surface states and reduction of the splitting size. We expect to increase the splitting size by dosing other elements or molecules with high electron affinity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Antiferromagnetic fluctuations and orbital-selective Mott transition in the van der Waals ferromagnet Fe 3–x GeTe 2

Fe 3–x GeTe 2 is a layered magnetic van der Waals material of interest for both fundamental and applied research. Despite the observation of intriguing physical properties, open questions exist even on the basic features related to magnetism: is it a simple ferromagnet or are there antiferromagnetic regimes, and are the moments local or itinerant. In this work, we demonstrate that antiferromagnetic spin fluctuations coexist with the ferromagnetism through comprehensive elastic and inelastic neutron scattering and thermodynamic measurements. Our realistic dynamical mean-field theory calculations reveal that the competing magnetic fluctuations are driven by an orbital selective Mott transition (OSMT), where only the plane-perpendicular a 1g orbital of the Fe(3d) manifold remains itinerant. Our results highlight the multi-orbital character in Fe 3–x GeTe 2 that supports a rare coexistence of local and itinerant physics within this material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Antiferromagnetic order in Co-doped Fe 5 GeTe 2 probed by resonant magnetic x-ray scattering

The quasi-two-dimensional van der Waals magnet Fe 5-δ GeTe 2 has emerged as a promising platform for electronic and spintronic functionalities at room temperature, owing to its large ferromagnetic ordering temperature T C ≈ 315 K. Interestingly, by cobalt (Co) substitution of iron in F5GT, i.e., (Fe 1-x Co x ) 5-δ GeTe 2 (Co-F5GT), not only can its magnetic transition temperature be further enhanced, but the magnetic and structural ground states can also be tuned. Specifically, an antiferromagnetic (AFM) order is induced beyond the Co doping level x ≥ 0.4. Here, in this work, we investigate the magnetic properties of a Co-F5GT single crystal at x = 0.45(1), by utilizing the element-specific, resonant magnetic x-ray scattering technique. Our study reveals an A-type, Ising-like AFM ground state, with a transition temperature T N ≈ 340 K. In addition, our work unveils an important contribution from Co magnetic moments to the magnetic order. The application of the in-plane magnetic fields gradually polarizes the spin moments along the field direction, but without inducing incommensurate spin texture(s).

36 MATERIALS SCIENCE↗
NASA NTRS1974

Vapor growth of GeTe single crystals in micro-gravity

The positive effects of micro-gravity on crystal growth and fundamental properties of the vapor transport reaction were established by analyzing the results of GeSe and GeTe vapor transport experiments performed on board Skylab. The analysis was based on a direct comparison of GeSe and GeTe crystals and of mass transport rate data obtained on earth and in space. For this purpose, a total of six transport experiments employing different concentrations of transport agent (GeI4) and two temperature gradients were performed during the Skylab 3 and 4 missions. Extensive ground-based studies demonstrated that the crystal morphology and the mass transport rates of the above systems are affected by the transport conditions, in particular by gravity-driven convection. The results demonstrate unambiguously a considerable improvement of the space crystals in terms of surface perfection, crystalline homogeneity and defect density. The observation of greater mass transport rates than expected in micro-gravity environment is of basic scientific and technological significance. This indicates that conventional transport models are incomplete and demonstrates that crystals of improved quality can be grown at reasonable rates by this technique in space. Results are of practical importance for the modification of crystal growth techniques on earth.

Wiedemeier, H.↗
DOE OSTI2025

Magnetic Phase Diagram of 2D Magnet Fe 5– x GeTe 2 Revealed by Cryogenic Lorentz 4D-STEM

A two-dimensional van der Waals ferromagnet Fe 5–x GeTe 2 (F5GT) exhibits room-temperature magnetic transition and magnetic anisotropy. Studies have identified diverse magnetic states, including stripe domains, skyrmionic type-I and topologically trivial type-II bubbles, depending on the magnetic and thermal history. Yet, the underlying micromagnetic energetics driving these states remains unclear. Here, we establish the magnetic phase diagram of bulk F5GT using cryogenic Lorentz four-dimensional scanning transmission electron microscopy. We reveal that stripe domains spontaneously form upon zero-field cooling, while metastable magnetic bubbles are stabilized by external fields. Transitions from type-I to type-II bubbles are driven by an oblique external field. Micromagnetic simulations confirm that these transitions arise from the interplay of uniaxial anisotropy, dipolar interactions, and external fields, without requiring significant Dzyaloshinskii–Moriya Interaction (DMI). In conclusion, these findings clarify the micromagnetic origin of spin textures of F5GT and establish it as a tunable platform for nanoscale topological magnetism.

2D Magnets↗
DOE OSTI2023

Above-Room-Temperature Ferromagnetism in Thin van der Waals Flakes of Cobalt-Substituted Fe 5 GeTe 2

Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying the fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling thin and highly tunable spintronic devices. To realize high-quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temperature that can be created via exfoliation. Here, in this paper, the study of exfoliated flakes of cobalt-substituted Fe 5 GeTe 2 (CFGT) exhibiting magnetism above room temperature is reported. Via quantum magnetic imaging with nitrogen-vacancy centers in diamond, ferromagnetism at room temperature was observed in CFGT flakes as thin as 16 nm corresponding to 16 layers. This result expands the portfolio of thin room-temperature 2D magnet flakes exfoliated from robust single crystals that reach a thickness regime relevant to practical spintronic applications. The Curie temperature T c of CFGT ranges from 310 K in the thinnest flake studied to 328 K in the bulk. To investigate the prospect of high-temperature monolayer ferromagnetism, Monte Carlo calculations were performed, which predicted a high value of T c of ~270 K in CFGT monolayers. Pathways toward further enhancing monolayer T c are discussed. These results support CFGT as a promising platform for realizing high-quality room-temperature 2D magnet devices.

2D magnetism↗
DOE OSTI2020

Materials Data on GeTe by Materials Project

GeTe is Halite, Rock Salt structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ge2+ is bonded to six equivalent Te2- atoms to form a mixture of edge and corner-sharing GeTe6 octahedra. The corner-sharing octahedral tilt angles are 0°. All Ge–Te bond lengths are 3.00 Å. Te2- is bonded to six equivalent Ge2+ atoms to form a mixture of edge and corner-sharing TeGe6 octahedra. The corner-sharing octahedral tilt angles are 0°.

36 MATERIALS SCIENCE↗