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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Detection of a pair density wave state in UTe2

Abstract Spin-triplet topological superconductors should exhibit many unprecedented electronic properties, including fractionalized electronic states relevant to quantum information processing. Although UTe 2 may embody such bulk topological superconductivity 1–11 , its superconductive order parameter Δ( k ) remains unknown 12 . Many diverse forms for Δ( k ) are physically possible 12 in such heavy fermion materials 13 . Moreover, intertwined 14,15 density waves of spin (SDW), charge (CDW) and pair (PDW) may interpose, with the latter exhibiting spatially modulating 14,15 superconductive order parameter Δ( r ), electron-pair density 16–19 and pairing energy gap 17,20–23 . Hence, the newly discovered CDW state 24 in UTe 2 motivates the prospect that a PDW state may exist in this material 24,25 . To search for it, we visualize the pairing energy gap with μeV-scale energy resolution using superconductive scanning tunnelling microscopy (STM) tips 26–31 . We detect three PDWs, each with peak-to-peak gap modulations of around 10 μeV and at incommensurate wavevectors P i =1,2,3 that are indistinguishable from the wavevectors Q i =1,2,3 of the prevenient 24 CDW. Concurrent visualization of the UTe 2 superconductive PDWs and the non-superconductive CDWs shows that every P i : Q i pair exhibits a relative spatial phase δϕ ≈ π. From these observations, and given UTe 2 as a spin-triplet superconductor 12 , this PDW state should be a spin-triplet PDW 24,25 . Although such states do exist 32 in superfluid 3 He, for superconductors, they are unprecedented.

Science & Technology - Other Topics↗
DOE OSTI2023

Smectic pair-density-wave order in EuRbFe 4 As 4

The pair density wave (PDW) is a superconducting state in which Cooper pairs carry centre-of-mass momentum in equilibrium, leading to the breaking of translational symmetry. Experimental evidence for such a state exists in high magnetic field and in some materials that feature density-wave orders that explicitly break translational symmetry. However, evidence for a zero-field PDW state that exists independent of other spatially ordered states has so far been elusive. Here we show that such a state exists in the iron pnictide superconductor EuRbFe 4 As 4 , a material that features co-existing superconductivity (superconducting transition temperature ( T c ) ≈ 37 kelvin) and magnetism (magnetic transition temperature ( T m ) ≈ 15 kelvin). Using spectroscopic imaging scanning tunnelling microscopy (SI-STM) measurements, we show that the superconducting gap at low temperature has long-range, unidirectional spatial modulations with an incommensurate period of about eight unit cells. Upon increasing the temperature above Tm, the modulated superconductor disappears, but a uniform superconducting gap survives to T c . When an external magnetic field is applied, gap modulations disappear inside the vortex halo. The SI-STM and bulk measurements show the absence of other density-wave orders, indicating that the PDW state is a primary, zero-field superconducting state in this compound. FInally, both four-fold rotational symmetry and translation symmetry are recovered above T m , indicating that the PDW is a smectic order.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Quantum textures of the many-body wavefunctions in magic-angle graphene

Interactions among electrons create novel many-body quantum phases of matter with wavefunctions that often reflect electronic correlation effects, broken symmetries, and novel collective excitations. A wide range of quantum phases has been discovered in MATBG, including correlated insulating, unconventional superconducting, and magnetic topological phases. The lack of microscopic information, including precise knowledge of possible broken symmetries, has thus far hampered our understanding of MATBG's correlated phases. Here we use high-resolution scanning tunneling microscopy to directly probe the wavefunctions of the correlated phases in MATBG. The squares of the wavefunctions of gapped phases, including those of the correlated insulators, pseudogap, and superconducting phases, show distinct patterns of broken symmetry with a √3 x √3 super-periodicity on the graphene atomic lattice that has a complex spatial dependence on the moiré superlattice scale. We introduce a symmetry-based analysis to describe our measurements of the wavefunctions of MATBG's correlated phases with a set of complex-valued local order parameters. For the correlated insulators in MATBG, at fillings of ±2 electrons per moiré unit cell relative to charge neutrality, we compare the observed quantum textures to those expected for proposed theoretical ground states. In typical MATBG devices, the textures of correlated insulators' wavefunctions closely match those of the theoretically proposed IKS order, while in ultra-low-strain samples our data has local symmetries like those of a T-IVC phase. Here, we also study the wavefunction of MATBG's superconducting state, revealing strong signatures of intervalley coherence that can only be distinguished from those of the insulator with our phase-sensitive measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Two-dimensional heavy fermions in the van der Waals metal CeSiI

Heavy-fermion metals are prototype systems for observing emergent quantum phases driven by electronic interactions. A long-standing aspiration is the dimensional reduction of these materials to exert control over their quantum phases, which remains a significant challenge because traditional intermetallic heavy-fermion compounds have three-dimensional atomic and electronic structures. Here we report comprehensive thermodynamic and spectroscopic evidence of an antiferromagnetically ordered heavy-fermion ground state in CeSiI, an intermetallic comprising two-dimensional (2D) metallic sheets held together by weak interlayer van der Waals (vdW) interactions. Owing to its vdW nature, CeSiI has a quasi-2D electronic structure, and we can control its physical dimension through exfoliation. The emergence of coherent hybridization of f and conduction electrons at low temperature is supported by the temperature evolution of angle-resolved photoemission and scanning tunnelling spectra near the Fermi level and by heat capacity measurements. Electrical transport measurements on few-layer fakes reveal heavy-fermion behaviour and magnetic order down to the ultra-thin regime. Importantly, our work establishes CeSiI and related materials as a unique platform for studying dimensionally confined heavy fermions in bulk crystals and employing 2D device fabrication techniques and vdW heterostructures to manipulate the interplay between Kondo screening, magnetic order and proximity effects.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Tuning commensurability in twisted van der Waals bilayers

Moiré superlattices based on van der Waals bilayers created at small twist angles lead to a long wavelength pattern with approximate translational symmetry. At large twist angles ( θ t ), moiré patterns are, in general, incommensurate except for a few discrete angles. Here we show that large-angle twisted bilayers offer distinctly different platforms. More specifically, by using twisted tungsten diselenide bilayers, we create the incommensurate dodecagon quasicrystals at θ t = 30° and the commensurate moiré crystals at θ t = 21.8° and 38.2°. Further, valley-resolved scanning tunnelling spectroscopy shows disparate behaviours between moiré crystals (with translational symmetry) and quasicrystals (with broken translational symmetry). In particular, the K valley shows rich electronic structures exemplified by the formation of mini-gaps near the valence band maximum. These discoveries demonstrate that bilayers with large twist angles offer a design platform to explore moiré physics beyond those formed with small twist angles.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Spectroscopy of the fractal Hofstadter energy spectrum

Hofstadter’s butterfly, the predicted energy spectrum for non-interacting electrons confined to a two-dimensional lattice in a magnetic field, is one of the most remarkable fractal structures in nature. At rational ratios of magnetic flux quanta per lattice unit cell, this spectrum shows self-similar distributions of energy levels that reflect its recursive construction. For most materials, Hofstadter’s butterfly is predicted under experimental conditions that are unachievable using laboratory-scale magnetic fields. More recently, electrical transport studies have provided evidence for Hofstadter’s butterfly in materials engineered to have artificially large lattice constants, such as those with moiré superlattices. Yet, so far, direct spectroscopy of the fractal energy spectrum predicted by Hofstadter nearly 50 years ago has remained out of reach. Here, in this work, we use high-resolution scanning tunnelling microscopy/spectroscopy (STM/STS) to investigate the flat electronic bands in twisted bilayer graphene (TBG) near the predicted second magic angle, an ideal setting for spectroscopic studies of Hofstadter’s spectrum. Our study shows the fractionalization of flat moiré bands into discrete Hofstadter subbands and discerns experimental signatures of self-similarity of this spectrum. Moreover, our measurements uncover a spectrum that evolves dynamically with electron density, showing phenomena beyond that of Hofstadter’s original model owing to the combined effects of strong correlations, Coulomb interactions and the quantum degeneracy of electrons in TBG.

electronic properties and materials↗
DOE OSTI2025

Cooper-pair density modulation state in an iron-based superconductor

Superconducting (SC) states that break space-group symmetries of the underlying crystal can exhibit nontrivial spatial modulation of the order parameter. Previously, such states were intimately associated with the breaking of translational symmetry, resulting in the density-wave orders, with wavelengths spanning several unit cells. However, a related basic concept has long been overlooked: when only intra-unit-cell symmetries of the space group are broken, the SC states can show a distinct type of nontrivial modulation preserving long-range lattice translation. Here, in this study, we refer to this new concept as the pair density modulation (PDM) and report the first observation of a PDM state in exfoliated thin flakes of the iron-based superconductor FeTe 0.55 Se 0.45 . Using scanning tunnelling microscopy (STM), we discover robust SC gap modulation with the wavelength corresponding to the lattice periodicity and the amplitude exceeding 30% of the gap average. Notably, we find that the observed modulation originates from the large difference in SC gaps on the two nominally equivalent iron sublattices. The experimental findings, backed up by model calculations, suggest that, in contrast to the density-wave orders, the PDM state is driven by the interplay of sublattice symmetry breaking and a peculiar nematic distortion specific to the thin flakes. Our results establish new frontiers for exploring the intertwined orders in strong-correlated electronic systems and open a new chapter for iron-based superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Visualizing interaction-driven restructuring of quantum Hall edge states

Many topological phases host gapless boundary modes that can be dramatically modified by electronic interactions. Even for the long-studied edge modes of quantum Hall phases, forming at the boundaries of two-dimensional (2D) electron systems, the nature of such interaction-induced changes has been elusive. Despite advances made using local probes, key experimental challenges persist: the lack of direct information about the internal structure of edge states on microscopic scales, and complications from edge disorder. Here, we use scanning tunneling microscopy (STM) to image pristine electrostatically defined quantum Hall edge states in graphene with high spatial resolution and demonstrate how correlations dictate the structures of edge channels on both magnetic and atomic length scales. For integer quantum Hall states in the zeroth Landau level, we show that interactions renormalize the edge velocity, dictate the spatial profile for copropagating modes, and induce unexpected edge valley polarization that differ from those of the bulk. While some of our findings can be understood by mean-field theory, others show breakdown of this picture, highlighting the roles of edge fluctuations and inter-channel couplings. We also extend our measurements to spatially resolve the edge state of fractional quantum Hall phases and detect spectroscopic signatures of interactions in this chiral Luttinger liquid. Furthermore, our study establishes STM as a promising tool for exploring edge physics of the rapidly expanding 2D topological phases, including newly realized fractional Chern insulators.

Electronic properties and materials↗
DOE OSTI2026

Limitations of probing field-induced response with STM

The kagome superconductors AV 3 Sb 5 (where A = K, Cs, Rb) exhibit intertwined density waves, unconventional superconductivity and time-reversal symmetry breaking without spin magnetism, with scanning tunnelling microscopy (STM) studies reporting, albeit not universally, magnetic-field-dependent changes in the apparent chirality of the 2 × 2 charge density wave (CDW). Related to this, Xing et al. investigated the effects of magnetic and electric fields on the 2 × 2 CDW state and the lattice structure of kagome superconductor RbV3Sb5, reporting a field-induced ~1% change in the in-plane lattice constants, concomitant with the CDW intensity modification, controlled by the field direction. Here we demonstrate how the apparent magnetic field induced lattice and CDW intensity change can be explained as a consequence of two independent experimental artifacts: a reconfiguration of atoms at the STM tip apex that alters the amplitudes of CDW modulations, and piezo creep, hysteresis and thermal drift, which artificially distort STM topographs. Here, we argue that the reported piezomagnetism could be attributed to experimental artifacts rather than an intrinsic magnetic-field-induced change of the sample.

Candelora, Christopher [Boston College, Chestnut H↗
DOE OSTI2026

Visualizing the impact of quenched disorder on 2D electron Wigner solids

Electron Wigner solids (WSs) provide an ideal system for understanding the competing effects of electron–electron and electron–disorder interactions, a central unsolved problem in condensed matter physics. Progress in this topic has been limited by a lack of single-defect-resolved experimental measurements as well as accurate theoretical tools to enable realistic experiment/theory comparison. Here, in this study, we overcome these limitations by combining atomically resolved scanning tunnelling microscopy (STM) with neural-quantum-state quantum Monte Carlo (NQS-QMC) simulation of disordered 2D electron WSs to discover new disorder-induced physical regimes of correlated electron behaviour. STM was used to image the electron density (n e )-dependent evolution of electron WSs in gate-tunable bilayer MoSe 2 (BL-MoSe 2 ) devices with varying long-range (n LR ) and short-range (n SR ) disorder densities. These images were compared with NQS-QMC simulations using realistic disorder maps extracted from experiment, thus allowing the roles of different disorder types to be disentangled. We identify two distinct physical regimes for disordered electron WSs that depend on n SR . For n SR ≲ n e , the WS behaviour is dominated by long-range disorder and features extensive mixed solid–liquid phases, a new type of local re-entrant melting/crystallization and prominent Friedel oscillations. By contrast, when n SR ≫ n e , these features are suppressed and a more robust amorphous WS phase emerges that persists to higher n e , highlighting the importance of short-range disorder in this regime. Our work establishes a powerful framework for studying disordered quantum solids through a combined experimental–theoretical approach.

Ge, Zhehao [University of California, Berkeley, CA↗
DOE OSTI2022

Visualizing the unusual spectral weight transfer in DyBa2Cu3O7–δ thin film

Abstract We report a Spectroscopic Imaging Scanning Tunneling Microscopy (SI-STM) study of a DyBa 2 Cu 3 O 7-δ (DBCO) thin film ( T c ~ 79 K) synthesized by the molecular beam epitaxy (MBE). We observed an unusual transfer of spectral weight in the local density of states (LDOS) spectra occurring only within the superconducting gap. By a systematic control of the tip-sample distance and the junction resistance, we demonstrate that the spectral weight transfer can be switched at a nano-meter length scale. These results suggest that an interaction between the STM tip and the sample alters the electronic configurations in the film. This probably originates from a combination of an intrinsic band bending at the interface between the surface and the bulk, and a tip-induced band bending. These results may open a new avenue for band engineering and applications of thin films of high- T c cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Spin-polarized imaging of the antiferromagnetic structure and field-tunable bound states in kagome magnet FeSn

Abstract Kagome metals are an exciting playground for the explorations of novel phenomena at the intersection of topology, electron correlations and magnetism. The family of FeSn-based kagome magnets in particular attracted a lot of attention for simplicity of the layered crystal structure and tunable topological electronic band structure. Despite a significant progress in understanding their bulk properties, surface electronic and magnetic structures are yet to be fully explored in many of these systems. In this work, we focus on a prototypical kagome metal FeSn. Using a combination of spin-averaged and spin-polarized scanning tunneling microscopy, we provide the first atomic-scale visualization of the layered antiferromagnetic structure at the surface of FeSn. In contrast to the field-tunable electronic structure of cousin material Fe 3 Sn 2 that is a ferromagnet, we find that electronic density-of-states of FeSn is robust to the application of external magnetic field. Interestingly, despite the field insensitive electronic band structure, FeSn exhibits bound states tied to specific impurities with large effective moments that strongly couple to the magnetic field. Our experiments provide microscopic insights necessary for theoretical modeling of FeSn and serve as a spring board for spin-polarized measurements of topological magnets in general.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Vibrational and electronic properties of Np 2 O 5 from experimental spectroscopy and first principles calculations

High-valence actinide oxides are critical to understanding the behavior of 5f-electrons, yet their structural and electronic properties remain poorly understood due to challenges in synthesis and handling. We report the first Raman spectroscopic study of single-crystalline Np 2 O 5 and the first scanning tunneling spectroscopy (STS) measurement on any neptunium-containing material. Hydrothermally synthesized crystals were structurally verified by X-ray diffraction. Raman spectra revealed sharply resolved vibrational features, including previously unreported low-frequency modes. STS measurements revealed a band gap of 1.5 eV. Density functional theory (DFT) enables vibrational mode assignments, reveals neptunium-dominated low-frequency phonons, oxygen-dominated high-frequency modes, and predicts an indirect band gap of 1.68 eV. This predicted value is in excellent agreement with the experimentally measured STS gap. This combined Raman, DFT, and STS approach provides a robust framework for correlating lattice dynamics and electronic structure in actinide materials, providing benchmark data for Np 2 O 5 , and opening new avenues for probing structure–property relationships in complex f-electron materials.

36 - MATERIALS SCIENCE↗
DOE OSTI2024

Unraveling the mechanism of tip-enhanced molecular energy transfer

Electronic Energy Transfer (EET) between chromophores is fundamental in many natural light-harvesting complexes, serving as a critical step for solar energy funneling in photosynthetic plants and bacteria. The complicated role of the environment in mediating this process in natural architectures has been addressed by recent scanning tunneling microscope experiments involving EET between two molecules supported on a solid substrate. These measurements demonstrated that EET in such conditions has peculiar features, such as a steep dependence on the donor-acceptor distance, reminiscent of a short-range mechanism more than of a Förster-like process. By using state of the art hybrid ab initio/electromagnetic modeling, here we provide a comprehensive theoretical analysis of tip-enhanced EET. In particular, we show that this process can be understood as a complex interplay of electromagnetic-based molecular plasmonic processes, whose result may effectively mimic short range effects. Therefore, the established identification of an exponential decay with Dexter-like effects does not hold for tip-enhanced EET, and accurate electromagnetic modeling is needed to identify the EET mechanism.

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

Deposition temperature-mediated growth of helically shaped polymers and chevron-type graphene nanoribbons from a fluorinated precursor

Graphene nanoribbons (GNRs) of precise size and shape, critical for controlling electronic properties and future device applications, can be realized via precision synthesis on surfaces using rationally designed molecular precursors. Fluorine-bearing precursors have the potential to form GNRs on nonmetallic substrates suitable for device fabrication. Here, we investigate the deposition temperature-mediated growth of a new fluorine-bearing precursor, 6,11-diiodo-1,4-bis(2-fluorophenyl)-2,3-diphenyltriphenylene (C 42 H 24 F 2 I 2 ), into helically shaped polymer intermediates and chevron-type GNRs on Au(111) by combining scanning tunneling microscopy, X-ray photoelectron spectroscopy, and density functional theory simulations. The fluorinated precursors do not adsorb on the Au(111) surface at lower temperatures, necessitating an optimum substrate temperature to achieve maximum polymer and GNR lengths. We compare the adsorption behavior with that of pristine chevron precursors and discuss the effects of C-H and C-F bonds. The results elucidate the growth mechanism of GNRs with fluorine-bearing precursors and establish a foundation for future synthesis of GNRs on nonmetallic substrates.

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

Sign changing pairing in single layer FeSe/SrTiO3 revealed by nonmagnetic impurity bound states

Abstract The discovery of high-temperature superconductivity in single layer FeSe epitaxially grown on SrTiO 3 (001) substrates has instigated extensive debate over whether its pairing symmetry is conventional sign-preserving s -wave or unconventional sign-changing. Here, we probe the pairing state for single layer FeSe/SrTiO 3 grown by molecular beam epitaxy using scanning tunneling microscopy/spectroscopy. We observe robust in-gap bound states induced by non-magnetic Fe-vacancy defects within the Fe-plane, which exhibit strong spatial electron-hole asymmetry with two-fold symmetry in hole states and four-fold in electron states. The bound states exhibit no energy shift or splitting under an applied magnetic field, consistent with a sign-changing order parameter. This is further confirmed by defect bound state quasiparticle interference that shows a sign-changing behavior with a pair of corresponding peaks at the positive and negative energies near the impurity bound states. Our findings provide unambiguous evidence for a sign-changing pairing symmetry for single layer FeSe/SrTiO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Atomic-scale manipulation of buried graphene–silicon carbide interface by local electric field

Abstract Precision of scanning tunneling microscopy (STM) enables control of matter at scales of single atoms. However, transition from atomic-scale manipulation strategies to practical devices encounters fundamental problems in protection of the designer structures formed atop the surface. In this context, STM manipulation of subsurface structures on technologically relevant materials is encouraging. Here, we propose a material platform and protocols for precise manipulation of a buried graphene interface. We show that an electric field from the STM tip reversibly controls breaking and restoring of covalent bonds between the graphene buffer layer and the SiC substrate. The process involves charge redistribution at the atomically sharp interface plane under the epitaxial graphene layer(s). This buried manipulation platform is laterally defined by unit cells from the corresponding (6×6) SiC moiré lattice of the epitaxial graphene. Local and reversible electric-field-induced patterning of graphene heterostructures from the bottom interface creates an alternative architecture concept for their applications.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Large bandgap observed on the surfaces of EuZn 2 As 2 single crystals

EuM 2 As 2 (M = Zn, Cd, In, Sn etc.) is an excellent material system for studying magnetism-tuned topological properties. However, discrepancies exist between experimental data and theoretical calculations regarding the bulk and surface bandgaps. In this work, cleaved EuZn 2 As 2 crystals are studied using scanning tunneling microscopy/spectroscopy and density functional theory calculations. Triangular-shaped defect-induced modifications in the local density of states help distinguish between Eu-terminated and AsZn-terminated surfaces. While large bandgaps (~1.5 eV at 77 K) are observed on both pristine surfaces, the bandgap size is found to be highly sensitive to local heterogeneity, tending to decrease. By combining experimental observations with theoretical simulations, we conclude that the reduced bandgap in heterogeneous regions arises from Zn vacancies and/or substitution by As atoms, both impacting greater in the Eu surface electronic properties than those in the AsZn surface. This demonstrates the intimate relationship between the electronic structure and magnetism in EuZn 2 As 2 .

interfaces↗