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DOE OSTI2024

Microscopic Derivation of Transition-state Theory for Complex Quantum Systems

The decay of quantum complex systems through a potential barrier is often described with transition-state theory, also known as RRKM theory in chemistry. Here we derive the basic formula for transition-state theory based on a generic Hamiltonian as might be constructed in a configuration-interaction basis. Two reservoirs of random Hamiltonians from Gaussian orthogonal ensembles are coupled to intermediate states representing the transition states at a barrier. Under the condition that the decay of the reservoirs to open channels is large, an analytic formula for reaction rates is derived. Here, the transition states act as independent Breit–Wigner resonances which contribute additively to the total transition probability, as is well known for electronic conductance through resonant tunneling states. It is also found that the transition probability is independent of the decay properties of the states in the second reservoir over a wide range of decay widths.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Summary Analysis of Different Offshore Wind Capacity Density Drivers in Proposed U.S. Projects and Impacts on Progress Towards State and Federal Deployment Targets

Understanding the density of offshore wind development - or the "capacity density" - is important for state and federal offshore wind planning efforts and to track progress towards policy goals. NREL has traditionally assumed a capacity density of 3 megawatts per square kilometer (MW/km2) when estimating the U.S. project pipeline (Musial et al. 2022), but capacity densities for existing European offshore wind farms ranged from 2-19 MW/km2 (Borrmann et al. 2018). We track the expected capacity densities of the proposed U.S. projects in the East Coast and make an analysis by state and by developer to identify what are the capacity density norms in the industry and whether the state in which the development efforts are taking place has some impact on capacity density. We also analyze the effects of the area occupied by station keeping systems on capacity density for lease areas dedicated to floating projects and provide a list of main capacity density drivers. This summary analysis sets a baseline to study how different capacity density drivers could impact the progress towards state and federal deployment targets. Given the currently delineated Renewable Energy Areas in the Outer Continental Shelf (OCS) and the basis from the summary analysis, we estimate the expected offshore wind deployment over time federally and by state and compare it to the state and federal deployment targets. The proposed analysis helps identify gaps and needs to meet state and federal targets, which provides sufficient information to propose strategic supply chain and policy planning with the objective of meeting deployment goals.

capacity density↗

DOE OSTI2025

Enhancing Acidic Oxygen Evolution Activity by Controlling Oxidation State of Iridium

Iridium oxides with high oxidation states have been reported to be effective in enhancing the acidic oxygen evolution reaction (OER) performance. Herein, we develop ultrasmall IrO x nanoparticles (NPs) over titanium nitride (TiN), which undergoes surface oxidation under oxidative conditions to form oxygen-modified TiN (oxi-TiN), enabling the formation of highly oxidized Ir δ+ (δ > 4). This IrO x /oxi-TiN catalyst delivers higher Ir mass activity than commercial IrO 2 , while comparable stability is maintained. The superior OER activity of IrO x /oxi-TiN is further demonstrated in a proton exchange membrane water electrolyzer (PEMWE), requiring only 1.88 V to reach 3 A cm −2 , achieving the U.S. Department of Energy 2025 target (1.90 V at 3 A cm −2 ). In situ X-ray absorption spectroscopy (XAS) confirms that the superior OER activity of IrO x /oxi-TiN originates from highly oxidized Ir δ+ under OER conditions. Further, density functional theory (DFT) calculations reveal a general correlation between the oxidation state of Ir and OER overpotential. Specifically, the introduction of interfacial oxygen at the Ir/TiN interface increases the oxidation state of deposited Ir δ+ from δ < 4 to δ > 4, decreasing the OER overpotential. This study highlights the critical role of high oxidation states of Ir δ+ in enhancing OER activity, providing guidance for the development of advanced acidic OER catalysts.

In situ measurements↗

DOE OSTI2025

Enhancing Acidic Oxygen Evolution Activity by Controlling Oxidation State of Iridium

Iridium oxides with high oxidation states have been reported to be effective in enhancing the acidic oxygen evolution reaction (OER) performance. In this work, we develop ultrasmall IrO x nanoparticles (NPs) over titanium nitride (TiN), which undergoes surface oxidation under oxidative conditions to form oxygen‐modified TiN (oxi‐TiN), enabling the formation of highly oxidized Ir δ+ (δ > 4). This IrO x /oxi‐TiN catalyst delivers higher Ir mass activity than commercial IrO 2 , while comparable stability is maintained. The superior OER activity of IrO x /oxi‐TiN is further demonstrated in a proton exchange membrane water electrolyzer (PEMWE), requiring only 1.88 V to reach 3 A cm −2 , achieving the U.S. Department of Energy 2025 target (1.90 V at 3 A cm −2 ). In situ X‐ray absorption spectroscopy (XAS) confirms that the superior OER activity of IrO x /oxi‐TiN originates from highly oxidized Ir δ+ under OER conditions. Density functional theory (DFT) calculations reveal a general correlation between the oxidation state of Ir and OER overpotential. Specifically, the introduction of interfacial oxygen at the Ir/TiN interface increases the oxidation state of deposited Ir δ+ from δ < 4 to δ > 4, decreasing the OER overpotential. This study highlights the critical role of high oxidation states of Ir δ+ in enhancing OER activity, providing guidance for the development of advanced acidic OER catalysts.

58 GEOSCIENCES↗

DOE OSTI2026

Locally purified maximally mixed states at scale: Entanglement pruning and symmetries

Locally Purified Density Operators (LPDOs) are state-of-the-art tensor network ansatze candidates that efficiently represent mixed quantum states at scale. However, given their non-uniqueness, their representational complexity is generally sub-optimal in practical computations. Here, in this work we perform a comprehensive numerical and analytical analysis and resolve this issue in the experimentally relevant limit where noise depolarizes the density operator into a maximally mixed state. To resolve the sub-optimality issue, we analyze two numerical tools, one analytic method, and detail the relations between them. The numerical tools used are fidelity-preserving truncations and isometric gauge transformations leveraging Riemannian optimizations over entropic objective functions. In addition, by invoking the injectivity and symmetry constraints of the maximally mixed LPDO, we also present analytical closed-form expressions for the disentangler and discuss their relation to numerical optimizers. Further, away from the maximally mixed state, our simulations highlight how the truncation threshold smoothly interpolate, as a function of depolarization, between established matrix product results and our new results. Our work shows how, by minimizing the resources required to represent key states of practical interest in experiment, the efficiency of tensor network algorithms can be substantially increased. This paves the path for uncovering tensor network’s fundamental scalability limits and latent potential in representing the wide locus of mixed quantum states that are accessible on near-term quantum devices.

Gangapuram, Amit Jamadagni [Oak Ridge National Lab↗

DOE OSTI2025

Graph-Learning-Assisted State and Event Tracking for Solar-Penetrated Power Grids with Heterogeneous Data Sources

Unlike transmission systems, distribution systems do not typically contain sufficient metering to enable real-time state estimation. The lack of sufficient real-time measurements prohibits accurate and timely monitoring of the state of distribution systems. As a result, control and optimal operation of distribution systems, especially those containing large numbers of renewable generation units are not possible without proper data and information about the current state of the system. The main motivation of this project is to address this shortcoming by developing an approach which provides “predicted” real-time measurements so that they can be used to execute a distribution system state estimator. Thus, the objective of the project is to make the distribution systems fully observable, such that the hosting capacity for solar generation can be accurately estimated, and unnecessary solar curtailments can be avoided. In order to accomplish this goal, the project investigated the use of a grid-model-informed machine learning (ML) tool which integrates heterogeneous data streams obtained from AMI meters, SCADA as well as PMU measurements and created synchronous measurement snapshots for the state estimator (SE); and developed a hybrid robust SE which provides not only accurate state estimates but also real-time feedback for the ML model refinement.

14 SOLAR ENERGY↗

DOE OSTI2025

Aerosol Particle Mixing State and Composition at AMF3 (Interim Field Campaign Report)

The campaign is designed to support deployment of aerosol sampling equipment at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s third ARM Mobile Facility (AMF3) to enable both singe-particle and bulk characterization of the aerosol particles at the field site in Bankhead National Forest, northern Alabama. We are proposing to do this work as part of our proposal “Generalizing aerosol mixing state: synthesis from observations and connection to models,” which has the pre-proposal tracking number PRE-0000035878. The full proposal has Dr. Rachel O’Brien as the Principal Investigator (PI) and Dr. Andy Ault and Dr. Nicole Riemer as Co-PIs. We sought to deploy instruments in winter 2025 and summer 2025 to obtain samples in different seasons, but were delayed by AMF3 set-up and availability of students and PIs. We just completed our first deployment this summer (2025) and we are interested in obtaining samples during this upcoming fall and winter to see the seasonal trends in aerosol mixing state at the site. This will provide a comparison of the impact of biogenic emissions on the mixing state and the chemical composition of the aerosol particles. Overall, the proposed study will provide key information regarding the mixing state of aerosol particles at AMF3 with direct ties to impacts of the particles on cloud formation and light scattering/absorption. From our deployment that ended las week we have some visible observations from our samples. We are observing a regular amount of black carbon on stage 6 of our Micro-Orifice Uniform Deposit Impactor (MOUDI) and we have also observed some short, large increases in aerosol loading. We hope to continue observations of these two features to determine the sources/aging for the black carbon and the physical mixing state as well as the sources for the short (a few minutes) increases in the aerosol loading and determine if the source for these is dust or sea salt or another source. We are also interested in comparing the black carbon we see here to samples collected during the agriculture burns in January/February and in comparing the larger particles to bioaerosols in the spring. To obtain these comparisons, we will need to collect more samples in the other seasons. Finally, we have some size-resolved particle collectors that can be deployed at the same time as the tethered balloon launches. We have discussed with Swarup China about trying to get the timing to work in August and we are interested in coordinating again later, if possible. This will give us ground-level and vertical aerosol mixing state sample sets that will be very exciting to analyze.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

An Ab Initio Electronic Structure Investigation of the Ground and Excited States of ScH + , YH + , and LaH +

Multireference configuration interaction (MRCI), Davidson-corrected MRCI (MRCI+Q), coupled-cluster singles, doubles, and perturbative triples [CCSD(T)], and frozen-core full configuration interaction (fcFCI) calculations were carried out using large, correlation-consistent basis sets to investigate the excited states of the Sc atom and the spin–free and spin–orbit coupled potential energy profiles, energetics, spectroscopic constants, and electron populations of low-lying states of MH + (M = Sc, Y, La). The core electron correlation effects, complete basis set effects, and spin–orbit coupling effects were also evaluated. The first four electronic states of all MH + are 1 2 Δ, 1 2 Σ + , 1 2 Π, and 2 2 Σ + with 1σ 2 1δ 1 , 1σ 2 2σ 1 , 1σ 2 1π 1 , and 1σ 2 3σ 1 single-reference electron configurations, respectively. These states of MH + can be represented by the M 2+ H – ionic structure. The ground states of ScH + , YH + , and LaH + are 1 2 Δ 3/2 , 1 2 Σ + 1/2 , and 1 2 Δ 3/2 with 55.45, 60.54, and 62.34 kcal/mol bond energies, respectively. The core electron correlation was found to be vital for gaining accurate predictions on the ground and excited state properties of MH + . The spin–orbit coupling effects are minor for ScH + but become substantial moving to YH + and LaH + . Overall, the results of this work are in good agreement with the limited set of experimental findings of MH + available in the literature and will be of use for future investigations. Furthermore, the theoretical approaches, findings, and trends reported here are expected to aid studies of similar species.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2025

DOUBLY-STRANGE BARYON SPECTROSCOPY WITH THE GLUEX EXPERIMENT: GROUND STATE ¿(1320) PHOTOPRODUCTION CROSS SECTION AND PROPERTIES

In the light-quark sector, traditional quark models and, more recently, lattice QCD calculations have predicted many more baryon states than have been experimentally observed. The hyperons, baryons with strange-quark content, in particular abundantly lack these observed states, and past observations are statistically limited. For multi-strange hyperons the matter is much worse and the production mechanisms of these states in photoproduction are very poorly understood. By capitalizing on the narrow peaks, as compared to the broad and overlapping N* and ¿* states, characteristic of the lowest lying ¿ resonances, the systematic aspects of the spectrum can be analyzed. In addition, we can measure experimental observables such as the production cross section to study the production mechanisms of the ¿ resonances. By accumulating various experimental observables, this goal could be accomplished through Partial Wave Analysis (PWA). The main body of work presented in this dissertation is the physics analysis and systematic study of the production cross section for the doubly strange octet ground state baryon (¿(1320)) in the exclusive t-channel photoproduction reaction ¿p ¿ K+Y* ¿ K+(K+¿-)Y* where ¿- ¿ ¿p- and ¿ ¿ pp-. The spin quantum number of ¿(1320) is also extracted and discussed. A preliminary result to extract the mass of ¿(1320) is also explored as a result of the statistical limitations of current measurements. Furthermore, the spectrum of the excited ¿* baryons are explored and discussed in the ¿*- ¿ K-¿ decay channel. The studies on the ground state and excited ¿ baryon are performed using the GlueX Phase-I (GlueX-I) data set. We have extracted differential cross sections from seven beam photon energy bins for E¿ ¿ [6.4,11.4] GeV1 and for -t < 2.4 GeV2 in the production of K+Y*. 1Natural units (c = 1) are used for the entire body of work.

Hernandez, Jesse [Florida State Univ., Tallahassee↗

DOE OSTI2025

Structure–Activity Relationships in Ether-Functionalized Solid-State Metal–Organic Framework Electrolytes

The structure–property relationships of metal–organic framework (MOF)-based solid-state electrolytes are not well understood. Herein, a systematic investigation of 12 Zr(IV)-based UiO-66 MOFs with varying ether-chain functional groups was carried out to elucidate the critical microscopic interactions that facilitate improved solid-state electrolyte performance. Enhanced sampling molecular dynamics (MD) simulations were employed and revealed a three-tier ion hopping mechanism: linker–linker hopping, linker-counterion hopping, and counterion-counterion hopping. Detailed structural analysis of the MD trajectories revealed that the chemistry and morphology of the linker groups affect the relative stability and population distribution of the electrolyte components, such that crown-ether-based linker groups enhance the probability of extended, low-barrier ion percolation pathways. As a result, we were able to tune the ionic conductivities by rationally manipulating the counterion distributions, linker binding strengths, and the configurational entropy (multivariability of the linkers). The resulting performance of these MOF-based solid-state electrolytes was significantly enhanced, with a methoxy-functionalized framework (UiO-66-L1 100 ) achieving high ionic conductivities of 2.32 × 10 –4 S/cm and 2.07 × 10 –3 S/cm at 30 °C and 90 °C, respectively, an order of magnitude greater than other all-solid-state MOF electrolyte systems. The electrolyte stability was evaluated with LiIn|LPSCl|MOF:LiTFSI|LPSCl|LiIn symmetric cells, showing excellent Li plating/stripping processes for over 2 months.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Discharge Rate‐Driven Li 2 O 2 Growth Exhibits Unconventional Morphology Trends in Solid‐State Li‐O 2 Batteries

Solid-state lithium oxygen batteries (LOBs) are known for their enhanced safety, higher electrochemical stability, and improved energy density compared to liquid-state LOBs. However, the investigation of solid-state LOBs is limited with little understanding of their discharge and charge processes. In this work, a polymer-based solid-state LOB is used to investigate the effect of discharge rate on lithium peroxide (Li 2 O 2 ) formation, the oxygen evolution reaction (OER), and cycle performance. Notably, we observe a counterintuitive trend: Li 2 O 2 particle size increases with increasing discharge current density, in contrast to liquid systems. This behavior arises from inherent space charge layers that restrict Li⁺ transport under high current, and spatially heterogeneous active sites at the solid electrolyte–cathode interface, directly evidenced by small angle X-ray scattering (SAXS), which govern nucleation accessibility and promote site-selective Li 2 O 2 growth. Furthermore, higher current densities improve ORR and OER efficiency but accelerate anode degradation, while lower currents promote side reactions. These opposing effects result in a trade-off that defines an optimal discharge rate (0.1 mA cm -2 ) for maximizing cycle life. This study provides a new mechanistic perspective on discharge-driven processes in solid-state LOBs and offers practical guidelines for performance optimization in future high-energy battery systems.

Discharge current density↗

DOE OSTI2025

The effect of ion pairing on speciation and transport in ion exchange membranes at varying hydration levels: A four-state model

Understanding ion pairing in ion exchange membranes (IEMs) is essential for advancing IEM applications in energy and environmental technologies. Here, this study introduces a four-state molecular dynamics model to quantify speciation and transport within Nafion-117, specifically examining the role of ion pairing in monovalent and divalent counterions (NaCl, Na 2 SO 4 , and MgSO 4 ). By analyzing radial distribution functions (RDFs) and molecular snapshots, we distinguish ion pairing modes and classify counterions into four states: condensed counterion, condensed ion pair, free ion pair, and free counterion. A key finding is that while divalent counterions (e. g., Mg 2+ ) maintain stable speciation across hydration levels, monovalent counterions (e.g., Na + ) show notable speciation shifts with hydration. Both monovalent and divalent counterions are not diffusive when condensed onto the polymer (sorbed to membrane functional groups). In contrast, free counterions are diffusive across all hydration levels. To evaluate the overall diffusivity of counterions, four-state fractions and diffusivities are computed, each contributing to counterion transport. The condensed/free ion speciation for multivalent sulfate salts aligns with previous revisions to the Donnan-Manning framework that include ion pairing, thereby validating its relevance to established membrane theories. The four-state model's diffusivity results support several current ion exchange assumptions, including that the condensed counterions are immobile, while uncondensed counterions are mobile. The four-state model offers insights into contact ion pairing within IEMs, highlighting its potential even when undetected in aqueous solution experiments. This work advances the theoretical understanding of counterion speciation in IEMs while identifying model limitations that suggest avenues for refinement, such as distinguishing water-mediated ion pairs between fully hydrated ions.

Ion exchange membranes↗

DOE OSTI2025

Tuning Excited-State Charge Transfer Character in Cofacial Core-Substituted Perylenediimide Dimers

Understanding the interplay between excimer formation and symmetry-breaking charge separation is important for optimizing charge separation in organic photovoltaic materials. To explore this connection, we synthesized four 1,6,7,12-tetrakis( p -X-phenoxy)perylene-(3,4:9,10)-bisdicarboximide cofacially stacked dimers, where X = MeO, tert -butyl, Br, and CF 3 . Steady-state spectroscopy reveals H-type aggregation and excimer formation in all four dimers, while transient absorption spectroscopy shows relatively small changes in their excited-state absorptions. However, time-resolved fluorescence (TRF) spectroscopy shows that relaxation occurs from an initial Frenkel exciton-dominated excimer state to one in which charge transfer (CT) character contributes. Relaxation to the lower-lying state with CT character is attributed to a combination of structural and charge distribution changes elicited by varying the substituents. Finally, this study illustrates how subtle changes in charge distribution and structure can combine to influence the excited state dynamics that influence charge separation in molecular dimers.

fluorescence↗

DOE OSTI2025

Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms

Rare-earth adatoms on surfaces have been studied for potential atomic-scale magnetic storage, quantum sensing, and quantum computing applications. Despite accumulating experimental efforts, a comprehensive description of the electronic configurations of the adatoms remains elusive. Here, we investigate two charge states and several electronic configurations, including 5d and 6s valence shells, for a Sm adatom on a MgO substrate using multiconfigurational ab initio methods, for the possibility of using the Sm nuclear spin levels as qubits. For the configurations in a neutral charge state, we find that the electronic ground state is a singlet, and thus the hyperfine interaction associated with the 147 Sm nucleus is absent, which may greatly enhance nuclear spin coherence time. The degeneracy of the nuclear levels is lifted by the nuclear quadrupole interaction. We show that the splitting of the nuclear levels can be controlled by a static electric field, and that Rabi oscillations between the nuclear levels can be induced by a time-dependent electric field. For the configurations in a singly charged state, electronic Kramers doublets are formed. The electronic configurations including an unpaired 6s orbital exhibit a strong hyperfine Stark effect due to a large Fermi contact contribution to the hyperfine interaction. In these configurations, electric-field-induced Rabi oscillations between the electronic-nuclear levels can occur at frequencies up to 3 orders of magnitude higher than those for the neutral charge state. The proposed system may be experimentally observed within scanning tunneling microscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

The dynamical state of eROSITA clusters and its impact on the brightest cluster galaxy luminosity

The first Spectrum-Roentgen-Gamma (SRG) eROSITA public release contains 12 247 clusters and groups from its first 6 months of operation. We used the offset between the brightest cluster galaxy (BCG) and the X-ray peak ( D BCG − X ) to classify the cluster dynamical state of 3946 galaxy clusters and groups. We aim to investigate the evolution of the merger and relaxed cluster distributions with redshift and mass, and the distributions’ impact on the BCG. We used the X-ray peak from the eROSITA survey and the BCG position from the LS DR10 optical data, which includes the DECam eROSITA Survey optical data, to measure the D BCG − X offset. We modelled the distribution of D BCG − X , in units of R 500 , as the sum of two Rayleigh distributions representing the cluster’s relaxed and disturbed populations, and explored their evolution with redshift and mass. To explore the impact of the cluster’s dynamical state on the BCG luminosity, we separated the main sample according to the dynamical state. We defined clusters as relaxed if D BCG − X < 0.25R500, disturbed if D BCG − X > 0.5R500, and ‘diverse’ if 0.25R500 < D BCG − X < 0.5R500. We find no evolution of the merging fraction with redshift or mass. The width of the relaxed distribution increases with redshift, while the width of the two Rayleigh distributions decreases with mass. The analysis reveals that BCGs in relaxed clusters are brighter than BCGs in both the disturbed and diverse cluster populations. The most significant differences are found for high-mass clusters at higher redshifts. The results suggest that BCGs in low-mass clusters are less centrally bound than those in high-mass systems, irrespective of the dynamical state. Over time, BCGs in relaxed clusters progressively align with the potential centre. This alignment correlates with their luminosity growth relative to BCGs in dynamically disturbed clusters, underscoring the critical role of the cluster’s dynamical state in regulating BCG evolution.

galaxy clusters↗

DOE OSTI2026

The impact of aerosol mixing state on immersion freezing: insights from classical nucleation theory and particle-resolved simulations

Immersion freezing, initiated by ice-nucleating particles (INPs) in supercooled aqueous droplets, plays an important role in the formation of ice crystals within clouds. The efficiency of immersion freezing depends strongly on INP composition and, crucially, on the mixing state – how chemical species are distributed across the particle population. Here, we quantify the impact of aerosol mixing state on immersion freezing using a combined theoretical and particle-resolved modeling approach. We derive analytical expressions for the frozen fraction of internally and externally mixed INP populations based on classical nucleation theory, showing that the frozen fraction is sensitive to whether ice-active species are present in all particles or only in a subset of the population. We introduce a multi-species immersion freezing scheme into the particle-resolved model PartMC, using the water activity-based immersion freezing model (ABIFM) to compute freezing probabilities for mixed-composition particles. To improve computational efficiency, we implement a Binned Tau-Leaping algorithm and demonstrate an order-of-magnitude speedup with minimal accuracy loss. Simulations reproduce the analytical trends in limiting cases and extend the analysis to more general aerosol populations, where mixing state continues to exert a substantial control on frozen fraction. Sensitivity analyses across particle size, species type, and cooling condition reveal that the mixing state effect is most pronounced when small amounts of highly efficient INPs are mixed with less efficient materials. These findings underscore the need to represent aerosol mixing state explicitly in models of heterogeneous ice nucleation to reduce uncertainty in cloud-phase partitioning.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Single-Determinant Ground State in Ce 4+ Imidophosphorane Complexes

X-ray spectroscopy techniques are critical in the electronic structure analysis of high-valent lanthanides. The interpretation of multipeaked features at the lanthanide L 3 -edge has remained a challenging question, as it is observed across a range of material classes. A series of structurally related Ce 4+ complexes were prepared to probe the potential ligand field perturbation of the ground state within the series. The tuning of relative 4f and ligand orbital energies in homoleptic and heteroleptic tetravalent Ce imidophosphorane complexes is achieved through ligand derivatization and is clearly demonstrated by UV−vis spectroscopy and electrochemically measured redox potentials. However, Ce L 3 - edge high-energy resolution fluorescence-detected (HERFD) X-ray absorption near-edge structure (XANES) spectra present features at consistent numbers and energies across the range of complexes. Resonant inelastic X-ray scattering (RIXS) is employed to visualize the observed features in the HERFD-XANES spectra. Large complete active space configuration interaction singles and doubles (CASCISD) calculations demonstrate that the ground-state wave function of all complexes can be described employing a single determinant. As a result, the multielectron feature at the L 3 -edge observed in this study for the Ce 4+ imidophosphorane complexes is described as excited-state multiconfigurational behavior that is independent of ligand variation, in systems where the ground state is described using the simple single determinant wave function.

Lanthanides↗

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↗