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At least 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Orientation-Driven Chirality Funnels in Chiral Low-Dimensional Lead-Halide Perovskite Heterostructures

Chiral hybrid metal-halide perovskites show low-symmetry crystal structures, large Rashba splitting, spin-filtering, and strong chiroptical activity. Circular dichroism and circularly polarized photoluminescence have been investigated in chiral perovskites with increasingly distorted chiral structures. Here, we report the fabrication of chiral (R/S)-EBAPbI3 (EBA = α-ethylbenzylamine) single crystals, which possess highly distorted octahedral structures with a high angle variance value of ∼68 degree2. Using control in the fabrication conditions, we transfer chiral single crystals to thin films and achieve different crystal orientation preferences that induce tunable chiroptical properties to their heterostructures with PbI2 nanodomains, which we characterize with in situ X-ray diffraction and grazing-incidence wide-angle X-ray scattering measurements. Using transient chiroptical spectroscopies, we resolve photoexcited charge carrier dynamics and chirality transfer processes in such heterostructures down to cryogenic temperatures. We observe rapid carrier transfer along the in-plane (002) facets in chiral perovskite phases to PbI2 nanostructures within the initial few picoseconds, while carrier transfer along the out-of-plane (002) facets occurs at a slower rate. This fast transfer process leads to high photoluminescence intensities and large degrees of circular polarization in the emission from PbI2 nanodomains at cryogenic temperatures. Our findings report a multidimensional chiral-achiral heterostructure which takes advantage of controllable chirality transfer and offers new routes for future spintronic and chiroptical applications.

Liu, Shangpu↗
DOE OSTI2025

Unconventional Superlattice Ordering in Intercalated Transition Metal Dichalcogenide V1/3NbS2

The interplay between symmetry and topology in magnetic materials makes it possible to engineer exotic phases and technologically useful properties. A key requirement for these pursuits is achieving control over local crystallographic and magnetic structure, usually through sample morphology (such as synthesis of bulk crystals versus thin films) and application of magnetic or electric fields. Here we show that V1/3NbS2 can be crystallized in two ordered superlattices, distinguished by the periodicity of out-of-plane magnetic intercalants. Whereas one of these structures is metallic and displays the hallmarks of altermagnetism, the other superlattice, which has not been isolated before in this family of intercalation compounds, is a semimetallic noncollinear antiferromagnet that may enable access to topologically nontrivial properties. This observation of an unconventional superlattice structure establishes a powerful route for tailoring the tremendous array of magnetic and electronic behaviors hosted in related materials and may expand their use in low-power spintronic or topological quantum devices.

Fender, Shannon S↗
DOE OSTI2025

Highly Conjugated Porphyrin Arrays Enable Optical Resolution of Ferromagnetic and Antiferromagnetic Aligned States of the Triplet Exciton and an Incorporated Stable Radical

Well-defined photogenerated molecular spin systems have potential utility in spintronics and quantum information science (QIS). Because molecular magnetic, optical, and electronic properties can be controlled by design, diverse spin systems can be prepared at modest temperatures. Photogenerated molecular spin systems often involve states prepared from the interaction of excitons and charges. Resolving the nature of electron spin alignment in photogenerated spin states described by the coupling of a triplet exciton and a stable radical commonly relies on EPR spectroscopy. Here, we describe ethyne-bridged (porphinato)metal ( PM n ) oligomers that incorporate a macrocycle-bound Cu(II) radical center. Upon photoexcitation of such PM n arrays, a singdoublet ( 2 S 1 ) state is formed; ultrafast internal conversion (IC) then produces a tripdoublet ( 2 T 1 ) state, which undergoes intersystem crossing (ISC) to produce a tripquartet ( 4 T 1 ) state, before relaxation to the ground state ( 2 S 0 ). These highly conjugated Cu(II) radical-containing PMn arrays enable direct observation of copper porphyrin 2 T 1 → 4 T 1 ISC dynamics from the biexponential decay of the near-infrared (NIR) 2,4 T 1 → 2,4 T n transient absorption manifold. Multireference n-electron valence perturbation theory (NEVPT2) computations illuminate how PM n electronic structure controls the relaxation dynamics of these long-lived (>10 ns) electronically excited multiplet states. These studies show that highly conjugated and polarizable porphyrin arrays incorporating stable spin centers provide rare π-delocalized systems where the ferromagnetic and antiferromagnetic alignment between a triplet exciton and a stable radical are both spectrally resolved and addressable using transient optical spectroscopy at wavelengths exceeding 1 μm, providing new opportunities to QIS.

14 SOLAR ENERGY↗
DOE OSTI2025

Discovery and Synthesis of a Family of Boride Altermagnets

Borides are a rich material family. To push the boundaries of borides’ properties and applications into broader fields, we have conducted systematic theoretical and experimental searches for synthesizable phases in ternary borides TM 2 B 2 (T = 3d, M = 4d/5d transition metals). We find that TM 2 B 2 in the FeMo 2 B 2 -type and CoW 2 B 2 -type structures form a large family of stable/metastable materials of 120 members. Among them, we identify 40 materials with stable magnetic solutions. Further, we discover 11 altermagnets in the FeMo 2 B 2 -type structure. So far, boride altermagnets are rare. In these altermagnets, T = Fe or Mn atoms are arranged in parallel T-chains with strong ferromagnetic intrachain couplings and antiferromagnetic interchain couplings. They simultaneously exhibit electronic band spin splitting, typical of ferromagnetism, and zero net magnetization, typical of antiferromagnetism. They also exhibit magnonic band chiral splitting. Both effects originate from the unique altermagnetic symmetries crucially constrained by the nonmagnetic atoms in the structure. Transport properties of relevance to spintronic applications, including the strain-induced spin-splitter effect and anomalous Hall effect, are predicted. An iodine-assisted synthesis method for TM 2 B 2 is developed, using which 7 of the predicted low-energy phases are experimentally synthesized and characterized, including 4 altermagnets. This work expands the realm of borides by offering new opportunities for studying altermagnetism and altermagnons in borides. It also provides valuable insights into the discovery and design of altermagnets. Here, by demonstrating that altermagnets can exist as families sharing a common motif, this work paves a feasible route for discovering altermagnets by elemental substitutions and high-throughput computations.

Chemical structure↗
DOE OSTI2025

Skyrmion-like Spin Textures Emerging in the Material Derived from Structural Frustration

Magnetic materials with complex spin textures present both fundamental and practical appeal. The complex patterns of magnetic moments emerging on underlying crystal lattices hold potential for robust information storage and processing, including the promise of topological quantum computing. The scope of materials that host such patterns, however, remains rather limited. Here, in this study, we report a discovery of a complex spin texture in a noncentrosymmetric material that emerges from the structural frustration at the boundary between centrosymmetric parent structures MnCoGe (the hexagonal Ni 2 In or the orthorhombic TiNiSi structure type) and MnCoAs (the TiNiSi structure type). Our findings demonstrate that such structural frustration provides a powerful handle for identifying compositional spaces where complex magnetic behavior and associated nontrivial magnetic structures are likely to emerge. Thus, the new phase MnCoGe 1/3 As 2/3 exhibits a modulated cycloidal antiferromagnetic arrangement of electron spins on a noncentrosymmetric lattice (of the hexagonal ZrNiAl type) that materializes in the space between centrosymmetric collinear ferromagnets. This work provides a pathway for discovering novel materials with exotic spin textures for next-generation spintronics and quantum technologies.

Wang, YiXu [Florida State University, Tallahassee,↗
DOE OSTI2025

Spin Glass Behavior and Giant Magnetoresistance via Aliovalent Fe/Ni Alloying in Amorphous Tetrathiafulvalene-Tetrathiolate Coordination Polymers

The discovery of materials with programmable combinations of charge transport and magnetic properties is a major goal in synthetic chemistry. Molecular materials, such as coordination polymers (CPs), are emerging candidates in this field due to their synthetic modularity. While there are many conductive or magnetic CPs, single-component examples with both properties are still emerging. Here, in this work, we demonstrate how alloying paramagnetic Fe(III) centers into a highly conductive Ni-based CP results in novel amorphous materials with high conductivity and giant magnetoresistance. Aliovalent doping with paramagnetic Fe centers engenders spin-glass transitions, while Ni and the strong π-stacking interactions of tetrathiafulvalene-2,3,6,7-tetrathiolate (TTFtt) ligands support conductivity. Ni 0.69 Fe 0.31 TTFtt has σ ≈ 200 S/cm and a 1.8 K magnetoresistance of −52% at 5 T, among the largest for any coordination solid. This work demonstrates not only how magnetic properties can be rationally incorporated into conductive CPs, but also an unexpected potential for amorphous materials in spintronic applications.

amorphous materials↗
DOE OSTI2025

Mechanistic Insight into Tunable Spin Relaxation in Two-Dimensional Type-II Ligand-Perovskite Heterostructures

Two-dimensional (2D) metal-halide perovskites with spin-dependent optical properties hold great promise for spintronic and quantum applications. However, their spin lifetimes, especially for n = 1 2D perovskites, are typically limited to subpicosecond time scales due to rapid spin relaxation driven by strong spin−orbit coupling (SOC), electron−hole exchange interactions, and phonon-mediated scattering. Here, we demonstrate that type-II ligand-perovskite heterostructures overcome these constraints by reducing electron−hole wave function overlap and exciton binding energy. Compared to the type-I 2D perovskite (PEA) 2 PbI 4 with a spin lifetime of 0.29 ps at room temperature, our engineered type-II systems achieve substantially extended spin lifetimes, ∼6.37 ps for (4Tm) 2 PbI 4 and ∼18.47 ps for (4TCNm) 2 PbI 4 . In both materials, spatial charge separation across the perovskite−ligand interface mitigates the Bir−Aronov− Pikus (BAP) mechanism. Temperature- and fluence-dependent measurements reveal Elliott−Yafet (EY)-dominated spin relaxation in (4Tm) 2 PbI 4 , consistent with the observation of coherent phonon oscillation, whereas (4TCNm) 2 PbI 4 exhibits D’yakonov−Perel (DP)-dominated spin relaxation, with weaker phonon coupling further suppressing the EY relaxation, enabling spin lifetimes up to ∼126.81 ps at 5 K. Our findings establish a structural design framework for tailoring spin dynamics in 2D perovskites, offering a promising strategy to engineering spin and optoelectronic properties via rational ligand engineering.

Excitons↗
DOE OSTI2019

Antiferromagnetic Semiconductor BaFMn 0.5 Te with Unique Mn Ordering and Red Photoluminescence

Semiconductors possessing both magnetic and optoelectronic properties are rare and promise applications in opto-spintronics. In this work, we report the mixed-anion semiconductor BaFMn 0.5 Te with a band gap of 1.76 eV and a work function of 5.08 eV, harboring both antiferromagnetism (AFM) and strong red photoluminescence (PL). The synthesis of BaFMn 0.5 Te in quantitative yield was accomplished using the "panoramic synthesis" technique and synchrotron radiation to obtain the full reaction map, from which we determined that the compound forms upon heating at 850 degrees C via an intermediate unknown phase. The structure refinement required the use of a (3+1)-dimensional superspace group Cmme(alpha 01/2)0ss. The material crystallizes into a ZrCuSiAs-like structure with alternating [BaF] + and [Mn0.5Te] - layers and has a commensurately modulated structure with the q-vector of 1/6a* + 1/6b* + 1/2c* at room temperature arising from the unique ordering pattern of Mn 2+ cations. Long-range AFM order emerges below 90 K, with two-dimensional short-range AFM correlations above the transition temperature. First-principles calculations suggest that BaFMn 0.5 Te is an indirect band gap semiconductor with the gap opening between Te 5p and Mn 3d orbitals, and the magnetic interactions between nearest-neighbor Mn 2+ atoms are antiferromagnetic. Steady-state PL spectra show a broad strong emission centered at similar to 700 nm, which we believe originates from the energy manifolds of the modulated Mn 2+ sublattice and its defects. Time-resolved PL measurements reveal an increase in excited-state lifetimes with longer probe wavelengths, from 93 ns (at 650 nm) to 345 ns (at 800 nm), and a delayed growth (6.5 ± 0.3 ns) in the kinetics at 800 nm with a concomitant decay (4.1 ± 0.1 ns) at 675 nm. Together, these observations predict that there are multiple emissive states, with higher energy states populating lower energy states by energy transfer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals

The realization of long-range ferromagnetic order in two-dimensional van der Waals crystals, combined with their rich electronic and optical properties, could lead to new magnetic, magnetoelectric and magneto-optic applications1,2,3,4. In two-dimensional systems, the long-range magnetic order is strongly suppressed by thermal fluctuations, according to the Mermin–Wagner theorem5; however, these thermal fluctuations can be counteracted by magnetic anisotropy. Previous efforts, based on defect and composition engineering6,7,8,9,10, or the proximity effect, introduced magnetic responses only locally or extrinsically. Here we report intrinsic long-range ferromagnetic order in pristine Cr2Ge2Te6 atomic layers, as revealed by scanning magneto-optic Kerr microscopy. In this magnetically soft, two-dimensional van der Waals ferromagnet, we achieve unprecedented control of the transition temperature (between ferromagnetic and paramagnetic states) using very small fields (smaller than 0.3 tesla). This result is in contrast to the insensitivity of the transition temperature to magnetic fields in the three-dimensional regime. We found that the small applied field leads to an effective anisotropy that is much greater than the near-zero magnetocrystalline anisotropy, opening up a large spin-wave excitation gap. We explain the observed phenomenon using renormalized spin-wave theory and conclude that the unusual field dependence of the transition temperature is a hallmark of soft, two-dimensional ferromagnetic van der Waals crystals. Cr2Ge2Te6 is a nearly ideal two-dimensional Heisenberg ferromagnet and so will be useful for studying fundamental spin behaviours, opening the door to exploring new applications such as ultra-compact spintronics.

Gong, Cheng↗
DOE OSTI2017

Observation of stable Néel skyrmions in cobalt/palladium multilayers with Lorentz transmission electron microscopy

Néel skyrmions are of high interest due to their potential applications in a variety of spintronic devices, currently accessible in ultrathin heavy metal/ferromagnetic bilayers and multilayers with a strong Dzyaloshinskii–Moriya interaction. Here in this paper we report on the direct imaging of chiral spin structures including skyrmions in an exchange-coupled cobalt/palladium multilayer at room temperature with Lorentz transmission electron microscopy, a high-resolution technique previously suggested to exhibit no Néel skyrmion contrast. Phase retrieval methods allow us to map the internal spin structure of the skyrmion core, identifying a 25 nm central region of uniform magnetization followed by a larger region characterized by rotation from in- to out-of-plane. The formation and resolution of the internal spin structure of room temperature skyrmions without a stabilizing out-of-plane field in thick magnetic multilayers opens up a new set of tools and materials to study the physics and device applications associated with chiral ordering and skyrmions.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Voltage-controlled interlayer coupling in perpendicularly magnetized magnetic tunnel junctions

Magnetic interlayer coupling is one of the central phenomena in spintronics. It has been predicted that the sign of interlayer coupling can be manipulated by electric fields, instead of electric currents, thereby offering a promising low energy magnetization switching mechanism. Here we present the experimental demonstration of voltage-controlled interlayer coupling in a new perpendicular magnetic tunnel junction system with a GdO x tunnel barrier, where a large perpendicular magnetic anisotropy and a sizable tunnelling magnetoresistance have been achieved at room temperature. Owing to the interfacial nature of the magnetism, the ability to move oxygen vacancies within the barrier, and a large proximity-induced magnetization of GdO x , both the magnitude and the sign of the interlayer coupling in these junctions can be directly controlled by voltage. Lastly, these results pave a new path towards achieving energy-efficient magnetization switching by controlling interlayer coupling.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Magnetic quantum phase transition in Cr-doped Bi 2 (Se x Te 1-x ) 3 driven by the Stark effect

The interplay between magnetism and topology, as exemplified in the magnetic skyrmion systems, has emerged as a rich playground for finding novel quantum phenomena and applications in future information technology. Magnetic topological insulators (TI) have attracted much recent attention, especially after the experimental realization of quantum anomalous Hall effect. Future applications of magnetic TI hinge on the accurate manipulation of magnetism and topology by external perturbations, preferably with a gate electric field. In this work, we investigate the magneto transport properties of Cr doped Bi 2 (Se x Te 1-x ) 3 TI across the topological quantum critical point (QCP). We find that the external gate voltage has negligible effect on the magnetic order for samples far away from the topological QCP. However, for the sample near the QCP, we observe a ferromagnetic (FM) to paramagnetic (PM) phase transition driven by the gate electric field. Theoretical calculations show that a perpendicular electric field causes a shift of electronic energy levels due to the Stark effect, which induces a topological quantum phase transition and consequently a magnetic phase transition. Finally, the in situ electrical control of the topological and magnetic properties of TI shed important new lights on future topological electronic or spintronic device applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Toward tunable quantum transport and novel magnetic states in Eu 1– x Sr x Mn 1– z Sb 2 ( z < 0.05)

Magnetic semimetals are very promising for potential applications in novel spintronic devices. Nevertheless, realizing tunable topological states with magnetism in a controllable way is challenging. Here, we report novel magnetic states and the tunability of topological semimetallic states through the control of Eu spin reorientation in Eu 1–x Sr x Mn 1–z Sb 2 . Increasing the Sr concentration in this system induces a surprising reorientation of noncollinear Eu spins to the Mn moment direction and topological semimetallic behavior. The Eu spin reorientations to distinct collinear antiferromagnetic orders are also driven by the temperature/magnetic field and are coupled to the transport properties of the relativistic fermions generated by the 2D Sb layers. These results suggest that nonmagnetic element doping at the rare earth element site may be an effective strategy for generating topological electronic states and new magnetic states in layered compounds involving spatially separated rare earth and transition metal layers.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Deterministic and robust room-temperature exchange coupling in monodomain multiferroic BiFeO 3 heterostructures

Exploiting multiferroic BiFeO 3 thin films in spintronic devices requires deterministic and robust control of both internal magnetoelectric coupling in BiFeO 3 , as well as exchange coupling of its antiferromagnetic order to a ferromagnetic overlayer. Previous reports utilized approaches based on multi-step ferroelectric switching with multiple ferroelectric domains. Because domain walls can be responsible for fatigue, contain localized charges intrinsically or via defects, and present problems for device reproducibility and scaling, an alternative approach using a monodomain magnetoelectric state with single-step switching is desirable. Here we demonstrate room temperature, deterministic and robust, exchange coupling between monodomain BiFeO 3 films and Co overlayer that is intrinsic (i.e., not dependent on domain walls). Direct coupling between BiFeO 3 antiferromagnetic order and Co magnetization is observed, with ~90° in-plane Co moment rotation upon single-step switching that is reproducible for hundreds of cycles. Finally, this has important consequences for practical, low power non-volatile magnetoelectric devices utilizing BiFeO 3 .

36 MATERIALS SCIENCE↗
DOE OSTI2018

Discovery of a magnetic conductive interface in PbZr 0.2 Ti 0.8 O 3 /SrTiO 3 heterostructures

Here, emergent physical properties often arise at interfaces of complex oxide heterostructures due to the interplay between various degrees of freedom, especially those with polar discontinuities. It is desirable to explore if these structures may generate pure and controllable spin currents, which are needed to attain unmatched performance and energy efficiency in the next-generation spintronic devices. Here we report the emergence of a spin-polarized two-dimensional electron gas (SP-2DEG) at the interface of two insulators, SrTiO 3 and PbZr 0.2 Ti 0.8 O 3 . This SP-2DEG is strongly localized at the interfacial Ti atoms, due to the interplay between Coulomb interaction and band bending, and can be tuned by the ferroelectric polarization. Our findings open a door for engineering ferroelectric/insulator interfaces to create tunable ferroic orders for magnetoelectric device applications and provide opportunities for designing multiferroic materials in heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Accessing valley degree of freedom in bulk Tin(II) sulfide at room temperature

The field of valleytronics has promised greater control of electronic and spintronic systems with an additional valley degree of freedom. However, conventional and two-dimensional valleytronic systems pose practical challenges in the utilization of this valley degree of freedom. Here we show experimental evidences of the valley effect in a bulk, ambient, and bias-free model system of Tin(II) sulfide. We elucidate the direct access and identification of different sets of valleys, based primarily on the selectivity in absorption and emission of linearly polarized light by optical reflection/transmission and photoluminescence measurements, and demonstrate strong optical dichroic anisotropy of up to 600% and nominal polarization degrees of up to 96% for the two valleys with band-gap values 1.28 and 1.48 eV, respectively; the ease of valley selection further manifested in their non-degenerate nature. Such discovery enables a new platform for better access and control of valley polarization.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Large quantum-spin-Hall gap in single-layer 1T' WSe 2

Two-dimensional (2D) topological insulators (TIs) are promising platforms for low-dissipation spintronic devices based on the quantum-spin-Hall (QSH) effect, but experimental realization of such systems with a large band gap suitable for room-temperature applications has proven difficult. Here, we report the successful growth on bilayer graphene of a quasi-freestanding WSe 2 single layer with the 1T' structure that does not exist in the bulk form of WSe 2 . Using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy/spectroscopy (STM/STS), we observe a gap of 129 meV in the 1T' layer and an in-gap edge state located near the layer boundary. The system's 2D TI characters are confirmed by first-principles calculations. The observed gap diminishes with doping by Rb adsorption, ultimately leading to an insulator-semimetal transition. The discovery of this large-gap 2D TI with a tunable band gap opens up opportunities for developing advanced nanoscale systems and quantum devices.

36 MATERIALS SCIENCE↗