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Daniel Jost

Publications and source records attributed to Daniel Jost.

At least 19 recordsLinked to original sources

X-ray Driven Trihydrogen Formation on Silica Nanosurfaces

The trihydrogen cation ($\mathrm{H_3^+}$) initiates the ion-molecule reactions that build molecular complexity in interstellar space. Whether its canonical formation reaction, $\mathrm{H_2^+ + H_2 \rightarrow H_3^+ + H}$, proceeds on inorganic surfaces under radiation-driven ionization has remained untested. Here we drive $\mathrm{H_3^+}$ formation on hydrated silica nanoparticles using intense 1.88 keV X-ray pulses, combining ion velocity map imaging, electron time-of-flight spectroscopy, and single-particle coherent diffractive imaging to resolve this chemistry on individual particles. The self-induced surface electric field on the V/nm scale drives interfacial charge transfer and water fragmentation. This field is the dominant parameter governing the relative yields of $\mathrm{H^+}$, $\mathrm{H_2^+}$, and $\mathrm{H_3^+}$ across particle size, composition, and aggregation. Density functional theory and nonadiabatic quantum molecular dynamics simulations trace this field-driven charge transfer, directly analogous to band bending at semiconductor photoelectrodes. These results establish surface-field-driven charge transfer as a unifying mechanism between radiation dominated astrophysical environments and field-driven surface catalysis.

physics.chem-ph

Beyond Self-Play and Scale: A Behavior Benchmark for Generalization in Autonomous Driving

Recent Autonomous Driving (AD) works such as GigaFlow and PufferDrive have unlocked Reinforcement Learning (RL) at scale as a training strategy for driving policies. Yet such policies remain disconnected from established benchmarks, leaving the performance of large-scale RL for driving on standardized evaluations unknown. We present BehaviorBench -- a comprehensive test suite that closes this gap along three axes: Evaluation, Complexity, and Behavior Diversity. In terms of Evaluation, we provide an interface connecting PufferDrive to nuPlan, which, for the first time, enables policies trained via RL at scale to be evaluated on an established planning benchmark for autonomous driving. Complementarily, we offer an evaluation framework that allows planners to be benchmarked directly inside the PufferDrive simulation, at a fraction of the time. Regarding Complexity, we observe that today's standardized benchmarks are so simple that near-perfect scores are achievable by straight lane following with collision checking. We extract a meaningful, interaction-rich split from the Waymo Open Motion Dataset (WOMD) on which strong performance is impossible without multi-agent reasoning. Lastly, we address Behavior Diversity. Existing benchmarks commonly evaluate planners against a single rule-based traffic model, the Intelligent Driver Model (IDM). We provide a diverse suite of interactive traffic agents to stress-test policies under heterogeneous behaviors, beyond just using IDM. Overall, our benchmarking analysis uncovers the following insight: despite learning interactive behaviors in an emergent manner, policies trained via pure self-play under standard reward functions overfit to their training opponents and fail to generalize to other traffic agent behaviors. Building on this observation, we propose a hybrid planner that combines a PPO policy with a rule-based planner.

cs.RO

Super Agents and Confounders: Influence of surrounding agents on vehicle trajectory prediction

In highly interactive driving scenes, trajectory prediction is conditioned on information from surrounding traffic participants such as cars and pedestrians. Our main contribution is a comprehensive analysis of state-of-the-art trajectory predictors, which reveals a surprising and critical flaw: many surrounding agents degrade prediction accuracy rather than improve it. Using Shapley-based attribution, we rigorously demonstrate that models learn unstable and non-causal decision-making schemes that vary significantly across training runs. Building on these insights, we propose to integrate a Conditional Information Bottleneck (CIB), which does not require additional supervision and is trained to effectively compress agent features as well as ignore those that are not beneficial for the prediction task. Comprehensive experiments using multiple datasets and model architectures demonstrate that this simple yet effective approach not only improves overall trajectory prediction performance in many cases but also increases robustness to different perturbations. Our results highlight the importance of selectively integrating contextual information, which can often contain spurious or misleading signals, in trajectory prediction. Moreover, we provide interpretable metrics for identifying non-robust behavior and present a promising avenue towards a solution.

cs.LG

The chemRIXS Instrument for the LCLS-II X-Ray Free Electron Laser

The chemRIXS instrument at the Linac Coherent Light Source offers new opportunities for studying solution-phase systems with time-resolved soft X-ray spectroscopy through the recently commissioned high-repetition-rate LCLS-II X-ray free electron laser. The orders-of-magnitude X-ray flux improvement provided by the superconducting accelerator, combined with corresponding advances in the optical laser system and the liquid jet recirculation system, enables studies on dilute systems with high signal-to-noise compared to what was possible with the LCLS-I copper accelerator. These capabilities open up time-resolved X-ray absorption spectroscopy and resonant inelastic X-ray scattering to entirely new classes of samples, as well as enabling the development of new soft X-ray spectroscopies on liquid samples. An overview of the beamline components and the first LCLS-II commissioning results are presented.

physics.ins-det

Collective Magnetic Excitations in a Photo-excited Electron-doped Cuprate Superconductor

Elucidating the microscopic behavior of cuprates under ultrafast photoexcitation offers critical insights into their highly correlated out-of-equilibrium states. Although quasiparticle dynamics have been investigated extensively, the behavior of collective magnetic excitations remains comparatively unexplored. Here, we use time-resolved resonant inelastic X-ray scattering (trRIXS) at the Cu $L_3$-edge to track the collective magnetic excitations (paramagnons) in an optimally electron-doped cuprate driven out-of-equilibrium by a femtosecond pump laser pulse. Upon pumping, we observed an anti-Stokes signal associated with paramagnon generation, which modifies the paramagnon dispersion near the zone center, although the bandwidth remained unchanged. Moreover, the spectral weight exhibits a momentum-dependent variation across the Brillouin zone. The light-driven boost of the paramagnon population and the resulting spectral-weight transfer could provide new leverage to manipulate the properties of cuprates.

cond-mat.mtrl-sci

Direct Observation of the Lindhard Continuum using Resonant Inelastic X-ray Scattering

Understanding the excitations of quantum materials is essential for unraveling how their microscopic constituents interact. Among these, particle-hole excitations form a particularly important class, as they govern fundamental processes such as screening, dissipation, and transport. In metals, the continuum of electron-hole excitations is described by the Lindhard function. Although central to the theory of Fermi liquids, the corresponding Lindhard continuum has remained experimentally elusive. Here, we report its direct observation in the weakly correlated metal MgB$_{2}$ using ultra-soft resonant inelastic X-ray scattering (RIXS). We resolve a linearly dispersing excitation with velocity comparable to the Fermi velocity and find quantitative agreement with simulations of the non-interacting charge susceptibility. A detailed analysis and decomposition of the simulations reveal the intra-band origin of this low-energy excitation, confirming it as the Lindhard continuum. Our results establish ultra-soft RIXS as a momentum-resolved probe of the fermiology in metals and call for deeper investigations of continuum features in RIXS and related spectroscopy of other materials beyond MgB$_{2}$.

cond-mat.str-el

Doping dependence of 2-spinon excitations in the doped 1D cuprate Ba$_2$CuO$_{3+{\delta}}$

Recent photoemission experiments on the quasi-one-dimensional Ba-based cuprates suggest that doped holes experience an attractive potential not captured using the simple Hubbard model. This observation has garnered significant attention due to its potential relevance to Cooper pair formation in high-$T_c$ cuprate superconductors. To scrutinize this assertion, we examined signatures of such an attractive potential in doped 1D cuprates Ba$_2$CuO$_{3+\delta}$ by measuring the dispersion of the 2-spinon excitations using Cu $L_3$-edge resonant inelastic X-ray scattering (RIXS). Upon doping, the 2-spinon excitations appear to weaken, with a shift of the minimal position corresponding to the nesting vector of the Fermi points, $q_F$. Notably, we find that the energy scale of the 2-spinons near the Brillouin zone boundary is substantially softened compared to that predicted by the Hubbard model in one-dimension. Such a discrepancy implies missing ingredients, which lends support for the presence of an additional attractive potential between holes.

cond-mat.str-el

Detection of chiral spin fluctuations driven by frustration in Mott insulators

Topologically ordered states, such as chiral spin liquids, have been proposed as candidates that host fractionalized excitations. However, detecting chiral character or proximity to these non-trivial states remains a challenge. Resonant Raman scattering can be a powerful tool for detecting chiral fluctuations, as the $A_{2g}$ channel probes excitations with broken time-reversal symmetry and local chiral order. Here, we use exact diagonalization to characterize the resonant $A_{2g}$ channel, alongside two-magnon scattering in $B_{1g}$ and $E_g$ channels, for the Hubbard model on lattices with increasing levels of geometric spin frustration, where tuning the incident energy near the Mott gap reveals strong chiral spin excitation intensity. Increased spin frustration in the Mott insulator results in an overall softening of the Raman $A_{2g}$ response, indicating a tendency toward low energy chiral-chiral fluctuations in Mott insulators with magnetic frustration and proximity to chiral spin liquid states that can potentially be tuned by external perturbations.

cond-mat.str-el

Chiral Altermagnon in MnTe

Altermagnetism has surfaced as a novel magnetic phase, bridging the properties of ferro- and anti-ferromagnetism. The momentum-dependent spin-splitting observed in these materials reflects their unique symmetry characteristics, which also establish the conditions for chiral magnons to emerge. Here we provide the first direct experimental evidence for a chiral magnon in the altermagnetic candidate MnTe revealed by circular-dichroism resonant inelastic X-ray scattering (CD-RIXS). This mode which we term chiral altermagnon exhibits a distinct momentum dependence of its spin polarization consistent with the proposed altermagnetic $g-$wave symmetry of MnTe. Our polarization-resolved results corroborate the existence of a new class of magnetic excitations, demonstrating how altermagnetic order shapes spin dynamics and paves the way for advances in spintronic and quantum technologies.

cond-mat.mtrl-sci

Orbital inversion and emergent lattice dynamics in infinite layer CaCoO$_2$

The layered cobaltate CaCoO$_2$ exhibits a unique herringbone-like structure. Serving as a potential prototype for a new class of complex lattice patterns, we study the properties of CaCoO$_2$ using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Our results reveal a significant inter-plane hybridization between the Ca $4s-$ and Co $3d-$orbitals, leading to an inversion of the textbook orbital occupation of a square planar geometry. Further, our RIXS data reveal a strong low energy mode, with anomalous intensity modulations as a function of momentum transfer close to a quasi-static response suggestive of electronic and/or orbital ordering. These findings indicate that the newly discovered herringbone structure exhibited in CaCoO$_2$ may serve as a promising laboratory for the design of materials having strong electronic, orbital and lattice correlations.

cond-mat.str-el

Time-resolved X-ray Spectroscopy from the Atomic Orbital Ground State Up

X-ray spectroscopy has been a key method to determine ground and excited state properties of quantum materials with atomic specificity. Now, new x-ray facilities are opening the door to the study of pump-probe x-ray spectroscopy - specifically time-resolved x-ray absorption (trXAS) and time-resolved resonant inelastic x-ray scattering (trRIXS). In this paper we will present simulations of each of these spectroscopies using a time-domain full atomic multiplet, charge transfer Hamiltonian, adapted to study the properties of a generalized cluster model including a central transition metal ion caged by ligand atoms in a planar geometry. The numerically evaluated trXAS and trRIXS cross-sections for representative electron configurations $3d^9$ and $3d^8$ demonstrate the insights that can be obtained from charge transfer pumping, and how this nonequilibrium process affects ground and excited state properties. The straightforward characterization of the excitations in these systems, based on our analysis of the simulations, can serve as a benchmark for future experiments, as access to these time-resolved spectroscopic techniques becomes more widely available.

cond-mat.str-el

The Influence of Extended Interactions on Spin Dynamics in One-dimensional Cuprates

Quasi-one-dimensional (1D) materials provide a unique platform for understanding the importance and influence of extended interactions on the physics of strongly correlated systems due to their relative structural simplicity and the existence of powerful theoretical tools well-adapted to one spatial dimension. Recently, this was highlighted by anomalous observations in the single-particle spectral function $A(q,\omega)$ of 1D cuprate chain compounds, measured by angle-resolved photoemission spectroscopy (ARPES), which were explained by the presence of a long-range attractive interaction. Such an extended interaction should leave its fingerprints on other observables, notably the dynamical spin structure factor $S(q,\omega)$, measured by neutron scattering or resonant inelastic x-ray scattering (RIXS). Starting from a simple Hubbard Hamiltonian in 1D and using time-dependent density matrix renormalization group (tDMRG) methods, we show that the presence of long-range attractive coupling, directly through an instantaneous Coulomb interaction $V$ or retarded electron-phonon ({\it el-ph}) coupling, can introduce significant spectral weight redistribution in $S(q,\omega)$ across a wide range of doping. This underscores the significant impact that extended interactions can have on dynamical correlations among particles, and the importance of properly incorporating this influence in modeling. Our results demonstrate that $S(q,\omega)$ can provide a sensitive experimental constraint, which complements ARPES measurements, in identifying key interactions in 1D cuprates, beyond the standard Hubbard model.

cond-mat.str-el

Univariate Radial Basis Function Layers: Brain-inspired Deep Neural Layers for Low-Dimensional Inputs

Deep Neural Networks (DNNs) became the standard tool for function approximation with most of the introduced architectures being developed for high-dimensional input data. However, many real-world problems have low-dimensional inputs for which standard Multi-Layer Perceptrons (MLPs) are the default choice. An investigation into specialized architectures is missing. We propose a novel DNN layer called Univariate Radial Basis Function (U-RBF) layer as an alternative. Similar to sensory neurons in the brain, the U-RBF layer processes each individual input dimension with a population of neurons whose activations depend on different preferred input values. We verify its effectiveness compared to MLPs in low-dimensional function regressions and reinforcement learning tasks. The results show that the U-RBF is especially advantageous when the target function becomes complex and difficult to approximate.

cs.NE

Low temperature dynamic polaron liquid in a manganite exhibiting colossal magnetoresistance

Polarons - fermionic charge carriers bearing a strong companion lattice deformation - exhibit a natural tendency for self-localization due to the recursive interaction between electrons and the lattice. While polarons are ubiquitous in insulators, how they evolve in transitions to metallic and superconducting states in quantum materials remains an open question. Here, we use resonant inelastic x-ray scattering (RIXS) to track the electron-lattice coupling in the colossal magneto-resistive bi-layer manganite La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ across its metal-to-insulator transition. The response in the insulating high-temperature state features harmonic emissions of a dispersionless oxygen phonon at small energy transfer. Upon cooling into the metallic state, we observe a drastic redistribution of spectral weight from the region of these harmonic emissions to a broad high energy continuum. In concert with theoretical calculations, we show that this evolution implies a shift in electron-lattice coupling from static to dynamic lattice distortions that leads to a distinct polaronic ground state in the low temperature metallic phase - a dynamic polaron liquid.

cond-mat.str-el

Polarized tip-enhanced Raman spectroscopy at liquid He temperature in ultrahigh vacuum using an off-axis parabolic mirror

Tip-enhanced Raman spectroscopy (TERS) combines inelastic light scattering well below the diffraction limit down to the nanometer range and scanning probe microscopy and, possibly, spectroscopy. In this way, topographic and spectroscopic as well as single- and two-particle information may simultaneously be collected. While single molecules can now be studied successfully, bulk solids are still not meaningfully accessible. It is the purpose of the work presented here to outline approaches toward this objective. We describe a home-built, liquid helium cooled, ultrahigh vacuum tip-enhanced Raman spectroscopy system (LHe-UHV-TERS). The setup is based on a scanning tunneling microscope and, as an innovation, an off-axis parabolic mirror having a high numerical aperture of approximately $0.85$ and a large working distance. The system is equipped with a fast load-lock chamber, a chamber for the \textit{in situ} preparation of tips, substrates, and samples, and a TERS chamber. Base pressure and temperature in the TERS chamber were approximately $3\times 10^{-11}$~mbar and 15~K, respectively. Polarization dependent tip-enhanced Raman spectra of the vibration modes of carbon nanotubes were successfully acquired at cryogenic temperature. Enhancement factors in the range of $10^7$ were observed. The new features described here including very low pressure and temperature and the external access to the light polarizations, thus the selection rules, may pave the way towards the investigation of bulk and surface materials.

cond-mat.supr-con

Orientational wetting and topological transitions in confined solutions of semi-flexible polymers

Despite their considerable practical and biological applications, the link between molecular properties, assembly conditions and self-organized structure in confined polymer solutions remains elusive. Here, we explore the lyotropic nematic ordering of semi-flexible chains in spherical confinement for multiple contour lengths across a wide regime of concentrations. We uncover an original crossover from two distinct quadrupolar states, both characterized by regular tetrahedral patterns of surface topological defects, to either longitudinal, latitudinal or spontaneously-twisted bipolar structures with increasing densities. These transitions, along with the intermediary arrangements that they involve, are attributed to the combination of orientational wetting with subtle variations in their liquid-crystal (LC) elastic anisotropies. Our molecular simulations are corroborated by density functional calculations, and are quantified through the introduction of several order parameters as well as an unsupervised learning scheme for the localization of topological defects. Our results agree quantitatively with the predictions of continuum nematic elasticity theories, and evidence the extent to which the folding of macromolecules and the self-assembly of low-molecular-weight LCs may be guided by the same, universal principles.

cond-mat.soft

A Broken Translational Symmetry State in an Infinite-Layer Nickelate

A defining signature of strongly correlated electronic systems is the existence of competing phases with similar ground state energies, resulting in a rich phase diagram. While in the recently discovered nickelate superconductors, a high antiferromagnetic exchange energy has been reported, which implies the existence of strong electronic correlations, signatures of competing phases have not yet been observed. Here, we uncover a charge order (CO) in infinite-layer nickelates La1-xSrxNiO2 using resonant x-ray scattering across the Ni L-edge. In the parent compound, the CO arranges along the Ni-O bond direction with an incommensurate wave vector (0.344+/-0.002, 0) r.l.u., distinct from the stripe order in other nickelates which propagates along a direction 45 degree to the Ni-O bond. The CO resonance profile indicates that CO originates from the Ni 3d states and induces a parasitic charge modulation of La electrons. Upon doping, the CO diminishes and the ordering wave vector shifts toward a commensurate value of 1/3 r.l.u., indicating that the CO likely arises from strong correlation effects and not from Fermi surface nesting.

cond-mat.supr-con

Quantum critical fluctuations in an Fe-based superconductor

Quantum critical fluctuations may prove to play an instrumental role in the formation of unconventional superconductivity. Here, we show that the characteristic scaling of a marginal Fermi liquid is present in inelastic light scattering data of an Fe-based superconductor tuned through a quantum critical point (QCP) by chemical substitution or doping. From the doping dependence of the imaginary time dynamics we are able to distinguish regions dominated by quantum critical behavior from those having classical critical responses. This dichotomy reveals a connection between the marginal Fermi liquid behavior and quantum criticality. In particular, the overlap between regions of high superconducting transition temperatures and quantum critical scaling suggests a contribution from quantum fluctuations to the formation of superconductivity.

cond-mat.supr-con