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DOE OSTI2026

Phonon-mediated ultrafast dynamics in self-assembled monolayers of 4-mercaptobenzoic acid on gold

Non-equilibrium interactions between plasmonic metals and adsorbed molecules lie at the heart of emerging applications such as plasmonic photocatalysis and sensing, though the ultrafast charge and energy transfer mechanisms arising from these interactions are not well understood. Herein, we investigate the ultrafast dynamics of Au nano-islands tethered with a self-assembled monolayer (SAM) of electron-withdrawing 4-mercaptobenzoic acid (4MBA) molecules. Ultrafast UV-visible transient absorption spectroscopy following excitation of the interband transition in Au reveals three well-known, characteristic time constants that quantify electron–electron (el–el), electron–phonon (el–ph) and phonon–phonon (ph–ph) scattering lifetimes. When comparing the dynamics of bare Au and 4MBA-Au, we find that the el–ph and ph–ph scattering lifetimes are notably longer in 4MBA-Au. Density functional perturbation theory calculations ascribe the elongation in el–ph lifetimes in 4MBA-Au to the significant coupling of acoustic phonon modes of Au with certain molecular vibrations of 4MBA, leading to decreased spatial overlap between carrier electronic states and the acoustic modes. We speculate that the elongation of ph–ph scattering lifetimes in 4MBA-Au arises due to poor thermal conductivity of the SAM which disrupts efficient energy dissipation from Au to the environment, thus slowing down the thermalization of phonons. This work provides a glimpse into how molecular adsorbates modify the charge carrier and phonon dynamics of Au and sets the stage for further systematic exploration of plasmonic metal–molecule interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Cold Spray Cobalt Magnetostrictive Electromagnetic Acoustic Transducers for High Temperature Structure Monitoring

The Department of Energy’s Advanced Sensors and Instrumentation program seeks to develop and qualify advanced sensors for the nuclear industry. Reliable high temperature and high radiation sensors for detection and characterization of structural flaws in pipes, vessels, and structurally critical components is a weakness for both conventional light water reactors with coolant T-hot approaching 350oC, and for advanced reactors with T-hot temperatures in excess of 500 to 800oC. Magnetostrictive Electromagnetic Acoustic Transducers using a cold spray cobalt coating have been proposed as a sensor design that can withstand these kinds of temperatures and radiation levels to serve as online sensors to detect flaws before cracks, pits, or erosion/corrosion flaws progress to through-wall failures. This report tests cold spray cobalt as part of a magnetostrictive EMAT for high temperature service. Cobalt is known to have strong magnetostrictive properties however the effect of cold spray application is not well studied. This program was surprised to discover that cold sprayed cobalt exhibited little or no magnetostrictive behavior until it was thermally annealed. Following annealing to 650oC however, cold spray cobalt did exhibit a magnetostrictive response. Work to date prior to this milestone report publication showed that magnetostrictive EMAT was successfully tested to 400oC with an alnico permanent magnet. The program plans to extend testing with an electromagnet to higher temperatures. This follow-on work will be reported under subsequent publications or as a revision to this report.

Glass, Samuel W.↗

DOE OSTI2026

Disorder-induced spin-cluster magnetism in a doped kagome spin liquid candidate

The search for new quantum spin liquid materials relies on systems with strong frustration such as spins on an ideal kagome lattice. However, lattice imperfections can have substantial effects which are as yet not well understood. In recent work, the two-dimensional kagome system YCu 3 ⁢(OH) 6 ⁢[(Cl 𝑥 ⁢Br (1−𝑥) ) 3−𝑦 ⁢(OH) 𝑦 ] has emerged as a leading candidate hosting a Dirac spin liquid which appears to survive at least for 𝑥 < 0.4, associated with alternating-bond-hexagon (ABH) disorder. Here in magnetic samples with 𝑥 = 0.58, 𝑦 = 0.1 we report unusual in-plane ferromagnetic canting (FM) of the in-plane antiferromagnet (AFM), with an unusually wide regime of short-ranged order, and propose theoretical models to explain this behavior. First, we show that Kitaev-type exchanges naturally arise on the kagome lattice to second order in the known Dzyaloshinskii-Moriya exchanges, and that these interactions can produce the unusual in-plane FM canting from antichiral AFM. Second, we propose a phenomenological model of weakly FM-canted spin clusters to describe the short-ranged regime and analyze quantum fluctuations in an ABH toy model to show how ABH disorder can stabilize this regime. Here, the combination of experimental observation and theory suggests that kagome-Kitaev interactions and ABH disorder are necessary for describing the magnetic fluctuations in this family of materials, with potential implications for the proposed proximate spin liquid phase.

Seth, Arnab [Georgia Institute of Technology, Atla↗

DOE OSTI2024

Phonon screening and dissociation of excitons at finite temperatures from first principles

The properties of excitons, or correlated electron–hole pairs, are of paramount importance to optoelectronic applications of materials. A central component of exciton physics is the electron–hole interaction, which is commonly treated as screened solely by electrons within a material. However, nuclear motion can screen this Coulomb interaction as well, with several recent studies developing model approaches for approximating the phonon screening of excitonic properties. While these model approaches tend to improve agreement with experiment, they rely on several approximations that restrict their applicability to a wide range of materials, and thus far they have neglected the effect of finite temperatures. Here, we develop a fully first-principles, parameter-free approach to compute the temperature-dependent effects of phonon screening within the ab initio GW -Bethe–Salpeter equation framework. We recover previously proposed models of phonon screening as well-defined limits of our general framework, and discuss their validity by comparing them against our first-principles results. We develop an efficient computational workflow and apply it to a diverse set of semiconductors, specifically AlN, CdS, GaN, MgO, and SrTiO 3 . We demonstrate under different physical scenarios how excitons may be screened by multiple polar optical or acoustic phonons, how their binding energies can exhibit strong temperature dependence, and the ultrafast timescales on which they dissociate into free electron–hole pairs.

Science & Technology - Other Topics↗

DOE OSTI2026

A Kinetic Model of the Long-Term Corrosion of Glass-Ceramic Materials

Multiphase waste forms show promise for increased waste loading and for the ability to dispose of contaminated solid and particulate waste through direct densification. However, achieving predictive capability for long-term durability of multiphase waste forms, and thus assessing their possible deployment, requires expanding the current, limited knowledge base. Here, we describe the development of a corrosion model of a two-phase waste form consisting of crystals of known volume fraction embedded in a glass matrix. This model accounts for the dissolution of both the crystalline and glass phases as well as the hydration of the glass phase through an ion exchange reaction. Because of the large difference in solubility between the two phases, the reactive surface of the crystalline phase is a function of the extent of dissolution of the glass phase in this model. Model parameterization was performed using corrosion data, such as from single-pass flow-through tests, for the individual phases. The parameterized corrosion model was evaluated against static dissolution test data for a glass-ceramic multiphase waste form. This evaluation demonstrated the model’s ability to reproduce the time-dependent release of key tracers of glass and crystalline phase dissolution. Hence, the development of a kinetic model provides a pathway for long-term durability predictions and thus the use of multiphase waste forms in nuclear cleanup missions.

Kerisit, Sebastien N.↗

DOE OSTI2026

Discovery of magnetic-field-tunable density modulations and spin tilting in a layered altermagnet

Altermagnets recently emerged as a new class of magnetic materials, arising from specific spin crystal symmetries. They exhibit a spin-polarized electronic band structure similar to ferromagnets, yet possess zero net magnetization, promising exotic properties. Here we study a layered triangular lattice altermagnet, cobalt-intercalated NbSe 2 using scanning tunneling microscopy and spectroscopy (STM/S). Spectroscopic-imaging STM and spin-polarized STM reveals emergent 2 a 0 tri-directional charge and spin density modulations on the selenium surface. Density functional theory simulations suggest these modulations reflect the underlying cobalt superstructure. We discover that an out-of-plane magnetic field tunes the modulation amplitudes and the electronic density-of-states in a manner dependent on the field direction and strength. This behavior is attributed to the field-induced tilting of cobalt spins, which can have profound implications on the electronic properties of the altermagnet. Our results provide atomic-scale insights to uncover a magnetic-field tunable altermagnetic band structure, highlight the importance of understanding spin canting in altermagnets.

condensed-matter physics↗

DOE OSTI2024

An Accreting Supermassive Black Hole Buried in a Faint Dwarf Galaxy

Abstract In the last decade, there have been several discoveries of active galactic nuclei (AGN) in dwarf galaxies including an AGN in an ultracompact dwarf galaxy with a black hole mass >10 6 M ⊙ . However, finding a supermassive black hole (SMBH) in a dwarf low surface brightness (LSB) galaxy is rare. We report the discovery of a Seyfert type 2 class AGN that is associated with a nuclear SMBH of mass ∼6.5 × 10 6 M ⊙ in a dwarf LSB galaxy (μ 0,r > 23.8 mag arcsec −2 ) that we denote by MJ0818+2257. The galaxy was previously thought to be an outlying emission blob around the large spiral galaxy LEDA 1678924. In our current analysis, which includes the detection of the optical counterpart of MJ0818+2257, we study its ionized gas kinematics and find that the dynamical mass within the ionized gas disk is ∼5.3 × 10 9 M ⊙ . This is comparable to its stellar mass, which is ∼3 × 10 9 M ⊙ , and suggests that MJ0818+2257 is moderately dark matter dominated within the stellar disk. The SMBH-mass-to-galaxy-stellar-mass ratio isM BH /M(*) > 0.022, which is high compared to disk galaxies. Our detection of an SMBH in a bulgeless LSB dwarf galaxy raises questions about the growth of SMBHs in low-luminosity galaxies and suggests the possibility of detecting heavy seed black holes from early epochs in LSB dwarf galaxies in the low-redshift Universe.

Astronomy & Astrophysics↗

DOE OSTI2026

HTGR Multiphysics Application Drivers FY26 Updates

This report summarizes FY26 progress under the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program's high-temperature gas-cooled reactor (HTGR) application driver work, covering a wide range of activities such as code validation and multi-physics code assessment. 1) A detailed SAM model of the High-Temperature Engineering Test Reactor (HTTR) was developed using a unique-block grouping approach, with an extended parallel thermal network method to capture block-to-block conduction and radiation heat transfer, and applied to steady-state simulations of the HTTR 30~MW and 9~MW cases. 2) In another activity, SAM's newly implemented multi-component gas flow model was validated against the Natural convection Shutdown heat removal Test Facility (NSTF) argon ingress experiment, correctly capturing the density-driven suppression and thermal recovery of natural circulation observed when argon is introduced into the air-cooled Reactor Cavity Cooling System (RCCS) loop. 3) For the OECD/NEA High Temperature Test Facility (HTTF) benchmark, we co-led the international benchmark activities as well as the OECD/NEA final benchmark report to be released at the end of this year. 4) Finally, the coupled Griffin-SAM modeling capability for pebble-bed HTGRs was advanced by verifying the Griffin neutronics solution against Serpent Monte Carlo for a realistic non-uniform temperature distribution, resolving several deficiencies in the SAM-to-Griffin temperature transfer scheme, and enabling distinct fuel kernel, moderator, and coolant temperatures for cross section feedback. These new features were demonstrated in a PBR load-following transient.

Lee, Alvin↗

DOE OSTI2024

Isotope engineering for spin defects in van der Waals materials

Abstract Spin defects in van der Waals materials offer a promising platform for advancing quantum technologies. Here, we propose and demonstrate a powerful technique based on isotope engineering of host materials to significantly enhance the coherence properties of embedded spin defects. Focusing on the recently-discovered negatively charged boron vacancy center ($${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − ) in hexagonal boron nitride (hBN), we grow isotopically purified h 10 B 15 N crystals. Compared to$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − in hBN with the natural distribution of isotopes, we observe substantially narrower and less crowded$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − spin transitions as well as extended coherence timeT 2 and relaxation timeT 1 . For quantum sensing,$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − centers in our h 10 B 15 N samples exhibit a factor of 4 (2) enhancement in DC (AC) magnetic field sensitivity. For additional quantum resources, the individual addressability of the$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − hyperfine levels enables the dynamical polarization and coherent control of the three nearest-neighbor 15 N nuclear spins. Our results demonstrate the power of isotope engineering for enhancing the properties of quantum spin defects in hBN, and can be readily extended to improving spin qubits in a broad family of van der Waals materials.

Science & Technology - Other Topics↗

DOE OSTI2024

Mitigating Sodium Ordering for Enhanced Solid Solution Behavior in Layered NaNiO 2 Cathodes

The O-type layered nickel oxides suffer from undesired cooperative Jahn–Teller distortion stemming from Ni 3+ ions and undergo multiple biphasic structural transformations during the insertion/extraction of large Na + ions, posing a significant challenge to stabilize the structural integrity. We present here a systematic investigation of the impact of substituting 5 % divalent (Mg 2+ ) or trivalent (Al 3+ or Co 3+ ) ions for Ni 3+ to alleviate Na + ion ordering and perturb the Jahn–Teller effect to enhance structural stability. Here, we gauge a fundamental understanding of the Mg−O and Na−O or Mg−O−Na bonding interactions, noting that the ionicity of the Mg−O bond deshields the electronic cloud of oxygen from Na + ions. Furthermore, calculations of the Van Vleck distortion modes reveal a relaxation of NiO 6 octahedra from Jahn–Teller distortion and a reduced electron density at the interlayer with Mg 2+ substitution. Long-range (operando X-ray diffraction) and short-range (magic angle spinning nuclear magnetic resonance) structural analyses provide insights into reduced ordering, allowing a stable continuous solid solution. Overall, Mg-substitution results in a high-capacity retention of ~96 % even after 100 cycles, showcasing the potential of this strategy for overcoming the structural instabilities and enhancing the performance of sodium-ion batteries.

25 ENERGY STORAGE↗

DOE OSTI2026

Effect of Oxidizing Impurities on the Corrosion Behavior of Structural Alloys Exposed to MgCl 2 Molten Salt Vapor

The corrosion behavior of structural alloys SS304 and IN617 when exposed to vapors of MgCl 2 molten salt at 764 °C for 100 h in an argon atmosphere was investigated as a function of the level of oxidizing impurities (e.g., NaOH) present in the salt. Increasing the concentration of oxidizing impurities in the salt caused an increase in corrosion in both structural alloys, as measured by Cr depletion layers. A poorly adhered oxide scale layer containing Mg, Al, and Cr was observed on the surface of the metals, and local attack was observed as well. The Ni-based IN617 showed lower Cr depletion and less scale formation than the Fe-based SS304. These results demonstrate that oxidizing impurities in the molten salt will impact the vapor phase corrosion for structural members exposed to the molten salt headspace. This finding is highly relevant for understanding the effects of the vapor phase in molten salt applications, including molten salt thermal energy storage, molten salt nuclear reactors, and molten salt electrochemistry.

25 ENERGY STORAGE↗

DOE OSTI2025

A topological superconductor tuned by electronic correlations

A topological superconductor, characterized by either a chiral order parameter or a topological surface state in proximity to bulk superconductivity, is foundational to topological quantum computing. A key open challenge is whether electron-electron interactions can tune such topological superconducting phases. Here, we provide experimental signatures of a unique topological superconducting phase in competition with electronic correlations in 10-unit-cell thick FeTe x Se 1-x films grown on SrTiO 3 substrates. When the Te content x exceeds 0.7, we observe a topological transition marked by the emergence of a superconducting surface state. Near the FeTe limit, the system undergoes another transition where the surface state disappears, and superconductivity is suppressed. Theory suggests that electron-electron interactions in the odd-parity xy− band drives this second topological transition. The flattening and eventual decoherence of d xy -derived bands track the superconducting dome, linking correlation effects directly to superconducting coherent transport. Our work establishes many-body electronic correlations as a sensitive knob for tuning topology and superconductivity, offering a pathway to engineer new topological phases in correlated materials.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Synthetic Tuning of Exciton–Phonon Coupling in Janus WS 2(1-x) Se 2x Monolayers Revealed by Resonant Raman Excitation Spectroscopy for Optoelectronic Applications

Janus monolayers, such as WSSe, have broken out-of-plane symmetry and an intrinsic dipole moment, impacting exciton transport, lifetime, and phonon interactions while imbuing piezoelectric, photocatalytic, and Rashba spin-splitting properties to transition metal dichalcogenides (TMDs). The new properties of this atomically thin material can be used for optoelectronic device applications. As TMDs are converted into Janus monolayers, e.g., top selenization of WS2 to WSSe, the bandgap and structure smoothly evolve, impacting not only the formation of excitons but also their complex interactions with different phonon modes. Resonant Raman excitation profiles (REPs) are uniquely well-suited to reveal both excitonic transitions and exciton–phonon coupling. Here, the resonant REPs of $A^{'}_{1}$ WS 2 and A 1 WSSe modes are measured to understand the strength of their coupling with the A, B, and C excitonic bands of a WS2 monolayer throughout its stepwise transformation into Janus WSSe by pulsed laser deposition (PLD) of energetic selenium species. In situ Raman spectroscopy during deposition is used to controllably prepare stable intermediate Janus structures, WS 2(1-x) Se 2x (0 ≤ x ≤ 0.5), for ex situ measurement of their resonant REPs. As x increases, REPs reveal not only pronounced excitonic bands that gradually shift toward lower photon energies but also strong, mode-selective exciton–phonon coupling. First-principles resonant Raman simulations independently predict this spectral behavior and are shown capable of matching the spectrally broadened, experimentally observed REP profiles in this model system, indicating their strong predictive capability for future experiments. The combination of controlled synthesis, REP characterization, and predictive theory employed here demonstrates a powerful pathway to understand and ultimately tune exciton–phonon interactions for future quantum optical devices.

Janus monolayers↗

DOE OSTI2023

High‐Entropy Lithium Argyrodite Solid Electrolytes Enabling Stable All‐Solid‐State Batteries

Abstract Superionic solid electrolytes (SEs) are essential for bulk‐type solid‐state battery (SSB) applications. Multicomponent SEs are recently attracting attention for their favorable charge‐transport properties, however a thorough understanding of how configurational entropy (ΔS conf ) affects ionic conductivity is lacking. Here, we successfully synthesized a series of halogen‐rich lithium argyrodites with the general formula Li 5.5 PS 4.5 Cl x Br 1.5‐x (0≤x≤1.5). Using neutron powder diffraction and 31 P magic‐angle spinning nuclear magnetic resonance spectroscopy, the S 2− /Cl − /Br − occupancy on the anion sublattice was quantitatively analyzed. We show that disorder positively affects Li‐ion dynamics, leading to a room‐temperature ionic conductivity of 22.7 mS cm −1 (9.6 mS cm −1 in cold‐pressed state) for Li 5.5 PS 4.5 Cl 0.8 Br 0.7 (ΔS conf =1.98R). To the best of our knowledge, this is the first experimental evidence that configurational entropy of the anion sublattice correlates with ion mobility. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors by tailoring the degree of compositional complexity. Moreover, the Li 5.5 PS 4.5 Cl 0.8 Br 0.7 SE allowed for stable cycling of single‐crystal LiNi 0.9 Co 0.06 Mn 0.04 O 2 (s‐NCM90) composite cathodes in SSB cells, emphasizing that dual‐substituted lithium argyrodites hold great promise in enabling high‐performance electrochemical energy storage.

Chemistry↗

DOE OSTI2026

Impacts of Multidimensional Progenitor Perturbations on Core-collapse Supernova Explosions

Numerical studies of core-collapse supernovae have demonstrated the importance of nonradial motions in precollapse progenitors on the explosion outcome. We use the Chimera neutrino radiation hydrodynamics code running seven two-dimensional simulations of 15 M⊙ progenitors with different progenitor structures introduced by different one- and two-dimensional precollapse stellar evolution environments to examine the impacts of stellar structure and nonspherical motion in the precollapse progenitor on the development of explosions. We compare the explosion evolution of these models in terms of shock dynamics, diagnostic energy, neutrino heating, accretion, explosion geometry, nuclear abundances, and turbulent convection. We also analyze how stochastic variation impacts our simulations. Contrary to results reported in prior studies examining the impacts of multidimensional progenitors, we observe similar shock revival times and explosion development in our simulations despite differences in initial compositions and structures. We find no discernible impact from the accretion of nonradial perturbations from a multi-D progenitor onto the stalled shock in the revival and strength of explosion, as fully developed neutrino-driven convection behind the stalled shock is similar for all our models. For models with physically sourced noise in the iron core, a strong oscillation of the shock occurs after bounce and deflects infall laterally, and accelerates the saturation of the lateral turbulent kinetic energy. An examination of model stochasticity shows that any prior expected impacts on explosive outcome due to convection-related perturbations lie below the detectable threshold of numerical variation.

Chen, Chien-Hui [North Carolina State University]↗

DOE OSTI2025

Dimensional Evolution Guides Property Control in the A n Cu 4– n TiS 4 Semiconductor Series

Through progressive reduction of the three-dimensional (3D) covalent network of Cu 4 TiS 4 , we isolate seven new members of the A n Cu 4–n TiS 4 family (A = alkali metal; n = 0–4), spanning 3D, 2D, 1D, and 0D structural fragments. The dimensional reduction is rational, as it preserves the edge-sharing connectivity between [CuS 4 ] 7– and [TiS 4 ] 4– tetrahedra across the series. This structural evolution is driven by the stepwise substitution of Cu with alkali metals, guiding the formation of fragments with reduced dimensionality. The effects of “n” and “A” on the crystal structures, stabilities, electronic structures, and optoelectronic properties are profound, demonstrating that the manipulation of alkali metal size and A n Cu 4–n TiS 4 stoichiometry enables predictable variations in structure and properties. For example, the n = 0 and n = 4 end members of the A n Cu 4–n TiS 4 family set the range of achievable band gaps with 2.00 eV for Cu 4 TiS 4 , 2.60 eV for Na 4 TiS 4 , and intermediate values for the n = 1–3 members. Notably, CsCu 3 TiS 4 exhibits exceptional air stability and congruent melting, with density functional theory (DFT) calculating moderate hole and electron effective masses in specific crystallographic directions (mh = 1.24m 0 , me = 0.87m 0 ). Additionally, A 3 CuTiS 4 (A = Na, K, Rb) displays direct band gap behavior and long photoluminescence lifetimes of 2.3–8.6 μs, and K 3 CuTiS 4 has a PLQY of 5.19%. These findings underscore the potential of the A n Cu 4–n TiS 4 family for applications in optoelectronics and demonstrate widely applicable design concepts that unveil rational stoichiometries within a given composition space to generate a series of crystal structures related through an evolving covalent dimensionality that corresponds to a predictable electronic structure and property progression.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Update on Radiochemical Assessment of High Burnup Commercially Irradiated Fuel

This work documents an effort to collect burnup measurements on a high burnup rod, designated 6XV, and first cycle accident tolerant fuel (ATF) rod, designated 47I, to enable benchmarking of fuel performance codes and neutronics codes. In addition to measurements, Virtual Environment for Reactor Applications (VERA) full-core-depletion analysis was also performed for the rods that were experimentally analyzed to provide an opportunity for code validation. This effort focuses on collecting data from rods irradiated at Byron Generating Station and shipped to the Oak Ridge National Laboratory (ORNL) hot-cells. This data will also anchor non-destructive examination evaluations of burnup of the various fuel rods undergoing postirradiation examination (PIE) at ORNL. Previous PIE of these fuel rods provides some guidance on the burnup trend across the fuel. Axial gamma spectroscopy scans provide a measure of relative changes in burnup across a fuel pin. Mass spectrometry based burnup measurements performed for this work at specific axial locations in the fuel are fully quantitative. By combining the mass spectrometry data with the gamma scans it is possible to more quantitatively evaluate axial variations in burnup across the entire fuel pin [1]. The combined set of burnup evaluations will be made available to other organizations that have an interest in high burnup radiochemistry data for validation of neutronic simulations and source term evaluation such as the Nuclear Regulatory Commission (NRC).

Harp, Jason [Oak Ridge National Laboratory (ORNL),↗

DOE OSTI2024

Tailoring Ion Transport in Li 3‐3y Ho 1+y Cl 6‐x Br x via Transition‐Metal Free Structural Planes and Charge Carrier Distribution

Abstract Localized atomistic disorder in halide‐based solid electrolytes (SEs) can be leveraged to boost Li + mobility. In this study, Li + transport in structurally modified Li 3 HoCl 6 , via Br − introduction and Li + deficiency, is explored. The optimized Li 3‐3 y Ho 1+ y Cl 6‐ x Br x achieves an ionic conductivity of 3.8 mS cm −1 at 25 °C, the highest reported for holmium halide materials. 6,7 Li nuclear magnetic resonance and relaxometry investigations unveil enhanced ion dynamics with bromination, attaining a Li + motional rate neighboring 116 MHz. X‐ray diffraction analyses reveal mixed‐anion‐induced phase transitions with disproportionate octahedral expansions and distortions, creating Ho‐free planes with favorable energetics for Li + migration. Bond valence site energy analysis highlights preferred Li + transport pathways, particularly in structural planes devoid of Ho 3+ blocking effects. Molecular dynamics simulations corroborate enhanced Li + diffusion with Br − introduction into Li 3 HoCl 6 . Li‐Ho electrostatic repulsions in the (001) plane presumably drive Li + diffusion into the Ho‐free (002) layer, enabling rapid intraplanar Li + motion and exchange between the 2d and 4h sites. Li 3‐3 y Ho 1+ y Cl 6‐ x Br x also demonstrates good battery cycling stability. These findings offer valuable insights into the intricate correlations between structure and ion transport and will help guide the design of high‐performance fast ion conductors for all‐solid‐state batteries.

Chemistry↗