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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,045 records · Page 58
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Understanding the origin of Tabula Rasa-induced defects in n-type Cz c-Si: The case of nitrogen atmosphere

Phosphorus-doped Czochralski-grown silicon (Cz-Si) has been gaining market share in the large-scale manufacturing of high-efficiency silicon (Si)-based photovoltaic (PV) devices thanks to higher carrier lifetimes than their boron-doped counterpart. However, the fabrication of n-type Cz-Si based solar cells often requires process steps with much higher temperatures and longer times than p-type Silicon. Defect interaction with the high temperatures during such processes tend to be detrimental to the n-type Cz-Si carrier lifetime, therefore limiting the final device efficiency. Short thermal anneals before cell processing, known as Tabula Rasa (TR), have been proposed to mitigate the thermally induced lifetime degradation during n-type Cz-Si solar cell fabrication. This work thoroughly investigates the defects responsible for the lifetime degradation after TR in a N 2 atmosphere treatment. We use temperature-injection-dependent lifetime spectroscopy and the thickness variation method to decouple the effects of TR treatment in the bulk and the surface of the n-type Cz-Si wafers. Using the defect parameter contour mapping (DPCM), we identify the defect energy level (E t ) and the capture cross-section ratio (k) of the most likely process-induced defect, which aligns with previously proposed Si vacancy-associated defects. The DPCM reveals that these vacancy-associated defects have a shallow energy level E t - E v ~0.13 eV and very efficient electron capture cross section k~600. Unexpectedly, the bulk degradation due to vacancy defects in the volume of the wafer, is accompanied by a significant increase in the surface recombination as well. Through evaluating the surface recombination velocity temperature- and injection dependence, we show that after TR, at room temperature and for an injection level of 10 15 cm -3 , in a wafer passivated with a-Si:H(i) the surface recombination dominates the overall lifetime response. Here we hypothesize that the near surface vacancy-associated bulk defects play a role in lowering the electron diffusion current into the a-Si:H(i) from the c-Si(n) reducing the field-effect passivation.

14 SOLAR ENERGY↗
DOE OSTI2022

Optimizing lane reversals in transportation networks to reduce traffic congestion: A global optimization approach

This paper studies how to reduce the overall travel time of commuters in a transportation network by reversing the direction of some lanes in the network using a macroscopic network-wide perspective. Similar to the Network Design Problem, the lane reversal problem has been shown to be NP-hard given the dependence of the users’ route selection on the lane direction decision. Herein, we propose and compare three efficient methods to solve the routing and lane reversal problem jointly. First, we introduce an alternating method that decouples the routing and lane assignment problems. Second, we propose a Frank–Wolfe method that jointly takes gradient steps to adjust both the lane assignment and routing decisions. Third, we propose a convex approximation method that uses a threshold-based approach to convexify the joint routing and lane reversal objective. The convex approximation method is advantageous since it finds a global optimum solution for the approximated problem and it enables the possibility to include linear constraints. Using this method, we extend the main formulation to be able to limit a maximum number of reversed lanes, as well as to incorporate multiple origin–destination (OD) patterns. We test the proposed methods in a case study using the transportation network of Eastern Massachusetts where our results indicate an overall reduction in travel times of 4.7% by selecting the best 15 reversals. Moreover, using a small test network, we investigate the performance of the lane reversal strategies as a function of the OD demand symmetry. As expected, we observe that when the OD demand is very asymmetric (e.g., for a single OD pair, evacuations, large events), the reduction in travel times is larger than the symmetric case, reaching travel time reductions of 60%.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

The exit-wave power-cepstrum transform for scanning nanobeam electron diffraction: robust strain mapping at subnanometer resolution and subpicometer precision

Scanning nanobeam electron diffraction (NBED) with fast pixelated detectors is a valuable technique for rapid, spatially resolved mapping of lattice structure over a wide range of length scales. However, intensity variations caused by dynamical diffraction and sample mistilts can hinder the measurement of diffracted disk centers as necessary for quantification. Robust data processing techniques are needed to provide accurate and precise measurements for complex samples and non-ideal conditions. Here we present an approach to address these challenges using a transform, called the exit wave power cepstrum (EWPC), inspired by cepstral analysis in audio signal processing. The EWPC transforms NBED patterns into real-space patterns with sharp peaks corresponding to inter-atomic spacings. We describe a simple analytical model for interpretation of these patterns that cleanly decouples lattice information from the intensity variations in NBED patterns caused by tilt and thickness. With tracking the inter-atomic spacing peaks in EWPC patterns, strain mapping is demonstrated for two practical applications: mapping of ferroelectric domains in epitaxially strained PbTiO 3 films and mapping of strain profiles in arbitrarily oriented core-shell Pt-Co nanoparticle fuel-cell catalysts. The EWPC transform enables lattice structure measurement at sub-pm precision and sub-nm resolution that is robust to small sample mistilts and random orientations.

42 ENGINEERING↗
DOE OSTI2024

Mechanisms of proton transport in aqueous acid solutions

The fundamental understanding of proton transport, specifically the Grotthuss-like mechanism, is critical for many technological applications. The present study presents a comprehensive analysis of proton transport in aqueous solutions of sulfuric and phosphoric acids using quasielastic neutron and light scattering, broadband dielectric spectroscopy, rheology, pulsed-field gradient-NMR measurements, and ab initio molecular dynamic simulations. Results show that in all systems, proton transport occurs through short “jumps” of ~0.5 Å that are faster than structural relaxation. However, proton hopping appears to be coupled to structural relaxation in aqueous solutions of sulfuric acid, while these processes are decoupled in phosphoric acid. Neutron scattering indicates that all protons have the same fast mobility in phosphoric acid systems, while at least one proton per sulfuric molecule remains slower than other protons. Analysis reveals correlated proton jumps, but these correlations suppress conductivity, suggesting that expected Grotthuss-like enhancement of conductivity is unlikely in bulk liquids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Determining the domain-level reaction-diffusion properties of an actin-binding protein transgelin-2 within cells

Proteins in cells undergo repeated binding to other molecules, thereby reducing the apparent extent of their intracellular diffusion. While much effort has been made to analytically decouple these combined effects of pure diffusion and chemical binding, it is difficult with conventional approaches to attribute the measured quantities to the nature of specific domains of the proteins. Motivated by the common goal in cell signaling research aimed at identifying the domains responsible for particular intermolecular interactions, here we describe a framework for determining the local physicochemical properties of cellular proteins associated with immobile scaffolds. To validate this new approach, we apply it to transgelin-2, an actin-binding protein whose intracellular dynamics remains elusive. We develop a fluorescence recovery after photobleaching (FRAP)-based framework, in which comprehensive combinations of domain-deletion mutants are created, and the difference among them in FRAP response is analyzed. We demonstrate that transgelin-2 in actin stress fibers (SFs) interacts with F-actin via two separate domains, and the chemical properties are determined for the individual domains. Its pure diffusion properties independent of the association to F-actin is also obtained. Our approach will thus be useful, as presented here for transgelin-2, in addressing the signaling mechanism of cellular proteins associated with SFs.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2026

Prediction of dynamic behavior of a system undergoing an exchange of components using a transmission simulator method

In systems with modular design, it is of interest to perform component exchanges to upgrade components and explore new system configurations. If the dynamics of the components are known, then dynamic substructuring can be used to obtain a prediction of system performance for the new configuration. The transmission simulator method is a substructuring technique that utilizes an additional fixture to apply an elastic boundary condition to a test article such that an appropriate dynamic response can be obtained for a given substructuring application, and the technique has been used widely for performing coupling and decoupling operations. Here, in this work, a modified transmission simulator method is proposed that allows a direct exchange of components to be performed. In a numerical demonstration, the proposed method is shown to accurately predict the dynamics of an assembly that has undergone a component exchange in which the exchanged components have different material properties and different geometric properties. This approach can be applied to dynamic qualification frameworks in which structures undergo modifications or upgrades rather than complete redesigns.

Component exchange↗
DOE OSTI2025

Tailoring coherent beam combined laser pulse trains for high peak and average power applications

Laser systems based on coherent beam combination (CBC) that rely on tiled pupil architecture intrinsically carry digital capabilities independently applicable to all three essential characteristics of a laser pulse: amplitude, phase and polarization. Those capabilities allow the far-field energy distribution to be flexibly tailored in real time. Operation in the femtosecond regime at high repetition rates gives access to a wide range of applications requiring both high peak and average powers. We address the task of independent peak versus average power adjustment needed for applications seeking to decouple nonlinear phenomena associated with GW peak power from the thermal load inherent to kW average power operation. The technical solutions proposed are presented in the framework of the Ecole Polytechnique XCAN CBC laser platform (61 independent channels) with an emphasis on thermal management measures implemented to ensure its nominal operation.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Beryllium-10 dating of the Foothills Erratics Train in Alberta, Canada, indicates detachment of the Laurentide Ice Sheet from the Rocky Mountains at ~15 ka

The Foothills Erratics Train consists of large quartzite blocks of Rocky Mountains origin deposited on the eastern slopes of the Rocky Mountain Foothills in Alberta between ~53.5°N and 49°N. The blocks were deposited in their present locations when the western margin of the Laurentide Ice Sheet (LIS) detached from the local ice masses of the Rocky Mountains, which initiated the opening of the southern end of the ice-free corridor between the Cordilleran Ice Sheet and the LIS. In this study, we use 10 Be exposure dating to constrain the beginning of this decoupling. Based on a group of 12 samples well-clustered in time, we date the detachment of the western LIS margin from the Rocky Mountain front to ~14.9 ± 0.9 ka. This is ~1000 years later than previously assumed, but a lack of a latitudinal trend in the ages over a distance of ~500 km is consistent with the rapid opening of a long wedge of unglaciated terrain portrayed in existing ice-retreat reconstructions. Finally, a later separation of the western LIS margin from the mountain front implies higher ice margin–retreat rates in order to meet the Younger Dryas ice margin position near the boundary of the Canadian Shield ~2000 years later.

10Be exposure dating↗
DOE OSTI2023

A general infrastructure for data-driven control design and implementation in tokamaks

A general infrastructure for tokamak controllers based on data-driven neural net models is presented. The paradigm allows for more flexible choices of both the underlying model and the desired controlled variables and targets. The system is implemented and tested on the DIII-D tokamak, enacting simultaneous pressure and temperature control via a finite-set model-predictive controller. Traditional control methods such as proportional–integral–derivative (PID) have proven effective for decoupled control tasks, but scale poorly when trying to achieve more complicated goals such as full state control. This is exactly where model-based controllers succeed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

The structure of 3-D collisional magnetized bow shocks in pulsed-power-driven plasma flows

Here we investigate three-dimensional (3-D) bow shocks in a highly collisional magnetized aluminium plasma, generated during the ablation phase of an exploding wire array on the MAGPIE facility (1.4 MA, 240 ns). Ablation of plasma from the wire array generates radially diverging, supersonic ($M_S$ $\sim 7$), super-Alfvénic ($M_A>1$) magnetized flows with frozen-in magnetic flux $(R_M\gg1)$. These flows collide with an inductive probe placed in the flow, which serves both as the obstacle that generates the magnetized bow shock, and as a diagnostic of the advected magnetic field. Laser interferometry along two orthogonal lines of sight is used to measure the line-integrated electron density. A detached bow shock forms ahead of the probe, with a larger opening angle in the plane parallel to the magnetic field than in the plane normal to it. Since the resistive diffusion length of the plasma is comparable to the probe size, the magnetic field decouples from the ion fluid at the shock front and generates a hydrodynamic shock, whose structure is determined by the sonic Mach number, rather than the magnetosonic Mach number of the flow. The 3-D simulations performed using the resistive magnetohydrodynamic (MHD) code Gorgon confirm this picture, but under-predict the anisotropy observed in the shape of the experimental bow shock, suggesting that non-MHD mechanisms may be important for modifying the shock structure.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Observation of subcritical shocks in a collisional laboratory plasma: scale dependence near the resistive length

We present a study of subcritical shocks in a highly collisional laboratory plasma with a dynamically significant magnetic field. Shocks were produced by placing cylindrical obstacles into the supermagnetosonic ( $M_{{\rm MS}} \sim 1.9$ ) outflow from an inverse wire array z-pinch at the MAGPIE pulsed power facility ( $n_{e} \sim 8.5 \times 10^{17}\,{\rm cm}^{-3}$ , $v \sim 45\,{\rm km}\,{\rm s}^{-1}$ ). We demonstrate the existence of subcritical shocks in this regime and find that secondary stagnation shocks form in the downstream which we infer from interferometry and optical Thomson scattering measurements are hydrodynamic in nature. The subcritical shock width is found to be approximately equal to the resistive diffusion length and we demonstrate the absence of a jump in hydrodynamic parameters. Temperature measurements by collective optical Thomson scattering showed little temperature change across the subcritical shock ( ${<}10\,\%$ of the ion kinetic energy) which is consistent with a balance between adiabatic and Ohmic heating and radiative cooling. We demonstrate the absence of subcritical shocks when the obstacle diameter is less than the resistive diffusion length due to decoupling of the magnetic field from the plasma. These findings are supported by magnetohydrodynamic simulations using the Gorgon and AstroBEAR codes and discrepancies between the simulations and experiment are discussed.

Physics↗
DOE OSTI2026

From Weibel seeds to dynamo beyond pair-plasmas

Bridging the spatiotemporal scales of magnetic seed field generation and subsequent dynamo amplification in the weakly collisional intracluster medium presents an extreme numerical challenge. We perform collisionless turbulence simulations with initially unmagnetised electrons that capture both magnetic seed generation via the electron Weibel instability and the ensuing dynamo amplification. Going beyond existing pair-plasma studies, we use an ion-to-electron mass ratio of 100 for which we find electron and ion dynamics are sufficiently decoupled. These simulations are enabled by the 10-moment collisionless fluid solver of Gkeyll, which evolves the full pressure tensor for all species. The electron heat-flux closure regulates pressure isotropisation and effectively sets the magnetic Reynolds number. We investigate how the strength of the closure influences the transition between a regime reminiscent of previous kinetic pair-plasma simulations and a regime exhibiting dynamo behaviour qualitatively similar to magnetohydrodynamics.

astrophysical plasmas↗
DOE OSTI2024

Characterization of MoS 2 films via simultaneous grazing incidence X-ray diffraction and grazing incidence X-ray fluorescence (GIXRD/GIXRF)

Physical vapor deposited (PVD) molybdenum disulfide (nominal composition MoS 2 ) is employed as a thin film solid lubricant for extreme environments where liquid lubricants are not viable. The tribological properties of MoS 2 are highly dependent on morphological attributes such as film thickness, orientation, crystallinity, film density, and stoichiometry. These structural characteristics are controlled by tuning the PVD process parameters, yet undesirable alterations in the structure often occur due to process variations between deposition runs. Nondestructive film diagnostics can enable improved yield and serve as a means of tuning a deposition process, thus enabling quality control and materials exploration. Grazing incidence X-ray diffraction (GIXRD) for MoS 2 film characterization provides valuable information about film density and grain orientation (texture). However, the determination of film stoichiometry can only be indirectly inferred via GIXRD. The combination of density and microstructure via GIXRD with chemical composition via grazing incidence X-ray fluorescence (GIXRF) enables the isolation and decoupling of film density, composition, and microstructure and their ultimate impact on film layer thickness, thereby improving coating thickness predictions via X-ray fluorescence. We have augmented an existing GIXRD instrument with an additional X-ray detector for the simultaneous measurement of energy-dispersive X-ray fluorescence spectra during the GIXRD analysis. This combined GIXRD/GIXRF analysis has proven synergetic for correlating chemical composition to the structural aspects of MoS 2 films provided by GIXRD. We present the usefulness of the combined diagnostic technique via exemplar MoS 2 film samples and provide a discussion regarding data extraction techniques of grazing angle series measurements.

MoS2↗
DOE OSTI2022

Understanding the Influence of Receptive Field and Network Complexity in Neural Network-Guided TEM Image Analysis

Abstract Trained neural networks are promising tools to analyze the ever-increasing amount of scientific image data, but it is unclear how to best customize these networks for the unique features in transmission electron micrographs. Here, we systematically examine how neural network architecture choices affect how neural networks segment, or pixel-wise separate, crystalline nanoparticles from amorphous background in transmission electron microscopy (TEM) images. We focus on decoupling the influence of receptive field, or the area of the input image that contributes to the output decision, from network complexity, which dictates the number of trainable parameters. For low-resolution TEM images which rely on amplitude contrast to distinguish nanoparticles from background, we find that the receptive field does not significantly influence segmentation performance. On the other hand, for high-resolution TEM images which rely on both amplitude and phase-contrast changes to identify nanoparticles, receptive field is an important parameter for increased performance, especially in images with minimal amplitude contrast. Rather than depending on atom or nanoparticle size, the ideal receptive field seems to be inversely correlated to the degree of nanoparticle contrast in the image. Our results provide insight and guidance as to how to adapt neural networks for applications with TEM datasets.

42 ENGINEERING↗
DOE OSTI2018

Equilibria and Rate Phenomena from Atomistic to Mesoscale: Simulation Studies of Magnetite

Batteries are complex devices composed of multiple components that operate far from equilibrium and may operate under extreme stress and varying loads. Research of isolated battery components are valuable to the fundamental understanding of the physical processes occurring within each constituent element. When the components are integrated into a full device and operated under realistic conditions, it can be difficult to decouple the physical processes that occur across multiple interfaces and multiple length scales. Thus, the physical processes studied in isolated components may change in a full battery setup or may be irrelevant to performance. Simulation studies on many length scales play a key role in the analysis of experiments and in the elucidation of the relevant physical processes impacting performance. In this Account, we aim to highlight the use of modeling on multiple length scales to identify rate limiting phenomena in lithium-ion batteries. To illustrate the utility of modeling, we examine lithium-ion batteries with nanostructured magnetite, Fe 3 O 4 , as the positive electrode active material against a solid Li 0 negative electrode. Due to continuous operation away from equilibrium, batteries exhibit highly nonideal behavior, and a model that aims to reproduce behavior under realistic operating conditions must be able to capture the physics occurring on the length scales relevant to the performance of the system. It is our experience that limiting behavior in lithium-ion batteries can be observed on the atomic scale and up through the electrode scale and thus, predictive models must be capable of integrating and communicating physics across multiple length scales. Magnetite is studied as an electrode material for lithium-ion batteries, but it is found to suffer from slow solid-state transport of lithium, slow reaction kinetics, and poor cycling. Magnetite (Fe 3 O 4 ) is a material capable of undergoing multiple electron transfers (MET), and can accept up to eight lithium per formula unit (Li 8 Fe 3 O 4 ). Magnetite, (Fe 8a 3+ )[Fe 3+ Fe 2+ ] 16d O 4,32e 2– , has a close-packed inverse spinel structure and undergoes intercalation, structural rearrangement, and conversion reactions upon full lithiation. To overcome solid-state transport resistances, magnetite can be nanostructured to decrease Li + diffusion lengths, and this has been shown to increase capacity. Additionally, unique architectures incorporating both carbon and Fe 3 O 4 have shown to alleviate transport and cycling issues in the material. Here, we solely address traditional composite electrodes, in which Fe 3 O 4 is synthesized as nanoparticles and combined with additives to fabricate the electrode. In the case of nanoparticulate magnetite, it has been found that the electrode fabrication process results in the formation of micrometer-sized agglomerates of the Fe 3 O 4 nanoparticles, introducing a secondary structural motif. The agglomerates may form in one or more fabrication processes, and their elimination may not be straightforward or warranted. Here, we highlight the impact of these secondary formations on the performance of the Fe 3 O 4 lithium-ion battery. We illustrate how simulations can be used to design experiments, prioritize research efforts, and predict performance.

25 ENERGY STORAGE↗
DOE OSTI2019

Anisotropic Vapor-Deposited Glasses: Hybrid Organic Solids

CONSPECTUS: The term "organic solids" encompasses both crystals and glasses. Organic crystals are commonly grown for purification and structure determination and are being extensively explored for applications in organic electronics including field effect transistors. The ability to control the packing of one molecule relative to its neighbors is of critical importance for most uses of organic crystals. Often, anisotropic packing is also highly desirable as it enhances charge transport and optimizes light absorption/emission. When compared to crystals, the local packing in organic glasses is highly disordered and often isotropic. Glasses, however, offer two key advantages with respect to crystals. First, glasses typically lack grain boundaries and thus exhibit better macroscopic homogeneity. Second, glass composition can often be varied over a wide range while maintaining homogeneity. Besides electronic materials, many modern plastics used in a wide range of technologies are organic glasses, and the glassy state is being increasingly utilized to deliver pharmaceuticals because of higher bioavailability. In this article, we introduce vapor-deposited organic glasses as hybrid materials that combine some of the useful features of crystals and traditional liquid-cooled glasses. Physical vapor deposition produces glasses by directly condensing molecules from the gas phase onto a temperature-controlled substrate and allows film thickness to be controlled with nanometer precision. Just as liquid-cooled glasses, vapor-deposited glasses have smooth surfaces and lack grain boundaries. These attributes are critical for applications such as organic light emitting diodes (OLEDs), in which vapor-deposited glasses of organic semiconductors form the active layers. In common with crystals, vapor-deposited glasses can exhibit anisotropic packing, and the extent of anisotropy can be comparable to that of the typical organic crystal. For vapor-deposited glasses, in contrast to crystals, anisotropic packing can generally be controlled as a continuous variable. Deposition conditions can be chosen to produce glasses with significant molecular orientation (molecules "standing up" or "lying down" relative to the substrate), and pr-stacking can be directed along different directions relative to the substrate. Over the last five years, we have gained a fundamental understanding of the mechanism that controls the anisotropy of vapor-deposited glasses and learned how to control many aspects of anisotropic packing. Two key elements that enable such control are the high mobility present at the surface of an organic glass and the tendency of the surface to promote anisotropic packing of molecules. In contrast to traditional epitaxial growth, for vapor-deposited glasses, the free surface (not the substrate) acts as a template that controls the structure of a growing film. Lastly, the structure of any given layer is decoupled from those beneath it, thereby providing considerable freedom in producing layered glassy structures.

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

Tuning Perovskites’ Hydration-Induced Chemical Expansion with Octahedral Tilt Angles

Hydration-induced strains in proton-conducting oxides compromise chemo-mechanical stability when these materials are applied in protonic ceramic electrochemical cells. Here, to develop design principles for zero-strain materials, we systematically studied the hydration coefficients of chemical expansion (CCEs) in perovskite (Sr, Ba)(Ce, Zr, Y)O 3–x solid solutions with in situ dilatometry and thermogravimetric analysis in the range of 430–630 °C. By including and decoupling a wide range of tolerance factors and lattice parameters, we were able to identify a minimum in hydration CCEs (0–0.02) at intermediate tolerance factor values (t ≈ 0.95). Conversely, despite expectations of lower CCEs in larger unit cells, no general trend in CCE versus lattice parameter was found, and opposite trends could be seen for Sr(Ce, Zr, Y)O 3–x versus Ba(Ce, Zr, Y)O 3–x separately. In situ neutron diffraction (ND) enabled atomistic insight. Upon decreasing t, chemical strain anisotropy increased, but this trend did not match the U-shaped dependence of macroscopic CCEs on t. Instead, perovskites with intermediate t, hosting intermediate octahedral tilt angles in the nominally dry state, underwent the largest change in the B–O–B angles during hydration. Accommodating hydration through decreasing B–O–B angles is beneficial because it does not result in large lattice parameter changes. We propose an intermediate tolerance factor as a simple structural descriptor to enable near-zero hydration strains in proton-conducting perovskites.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Orbital-Selective Instabilities and Spin Fluctuations at the Verge of Superconductivity in Interlayer-Expanded Iron Selenide

Understanding electron correlation-driven instabilities and their coupling to structural phases is essential for deciphering multiorbital pairing in unconventional superconductors. We investigate Li x (C 5 H 5 N) y Fe 2 Se 2 (x ∼ 0.6; y ∼ 0.7−0.9), a tetragonal β-FeSe intercalate with a superconducting transition temperature (T c = 39 K) closely tied to an expanded Fe-layer spacing (∼11.4 Å). High-resolution synchrotron Xray diffraction and core-level absorption spectroscopy reveal subtle lattice distortions on cooling without a symmetry-breaking transition. Instead, the material exhibits negative thermal expansion (NTE) in the two-dimensional Fe network below T S ∼ 70 K, and stiffening of local Se−Fe−Se bond dynamics near T c . The spatially incoherent rearrangement of FeSe 4 tetrahedra and the site-local fluctuations, signal reduced electron correlations compared to those of parent β-FeSe (T c = 8 K). Complementary X-ray emission spectroscopy, a fast local probe of Fe 3d valence states, detects persistent local Fe spin moments below T S , unlike quenching in related systems. These findings indicate that decoupling of Fe planes leads to an electronically driven lattice instability. The latter emerges as NTE induced from weak, orbital-selective localization of in-plane Fe 3d states rather than conventional transverse vibrations. Governed by Hund’s coupling, this selectivity permits coexistence of local spin fluctuations with itinerant d-electrons critical for enhancing T c . These results suggest that intercalation-driven d-orbital differentiation moderates electron correlations, providing a pathway to optimize the superconductivity in low-dimensional quantum materials.

36 MATERIALS SCIENCE↗