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Active microrheology and dynamic phases for pattern-forming systems with competing interactions

We consider the driven dynamics of a probe particle moving through an assembly of particles with competing long-range repulsive and short-range attractive interactions, which form crystal, stripe, labyrinth, and bubble states as the ratio of attraction to repulsion is varied. We show that the probe particle exhibits a depinning-like threshold from an elastic regime, where the probe particle is trapped by interactions with the other particles, to a plastic flow regime, where the probe particle can break bonds in the surrounding medium. For a fixed particle density, the depinning threshold and sliding velocity of the probe particle vary nonmonotonically as the attraction term is increased. A velocity minimum appears near the crystal to stripe crossover, and there is a significant increase in the depinning threshold in the bubble regime when the probe particle is strongly confined inside the bubbles. For fixed attractive interaction but increasing particle density, the behavior is also nonmonotonic, and there are jumps and drops in the velocity and depinning threshold corresponding to points at which the system transitions between different structures. There are also several distinct flow states that can be characterized by the amount of plastic deformation induced by the probe particle in the surrounding medium. Each flow state generates a different amount of effective drag on the probe particle, and there can be jumps in the velocity-force curve at transitions between the states. In conclusion, we also find that when oriented stripes are present, the probe particle can move along the stripe in an edge transport state that has a finite Hall angle.

36 MATERIALS SCIENCE

Stripe and bubble ratchets on asymmetric substrates

We show that various nonmonotonic ratchet effects can arise when mesophase pattern-forming systems, which exhibit anisotropic crystal, stripe, and bubble regimes, are coupled to one-dimensional asymmetric substrates under ac driving. The patterns emerge in the absence of a substrate when the ratio of attraction to repulsion is varied for particles with competing short-range attraction and long-range repulsion potentials. In the presence of the substrate, we find that the ratchet efficiency varies nonmonotonically with increasing attraction, depending upon how well the mesophase morphology matches the substrate spacing and periodicity. For strong repulsion, there is a weak but finite ratchet effect, while at intermediate attraction, there is a robust ratchet effect in which the system forms stripes aligned with the substrate symmetry direction. For strong attraction, large bubbles appear that have weak or no ratchet effects when the bubble width exceeds the substrate lattice spacing, causing the bubble to be only weakly coupled to the substrate. For very strong attraction, small bubbles form and undergo a strong ratchet effect with an efficiency that oscillates as a function of ac drive amplitude. Although the small bubble regime is a strongly correlated regime in which each bubble contains many particles, the system behaves as if it is in a single-particle regime since the bubble width is much smaller than the substrate lattice spacing. We map out the different rectification phases as a function of the pattern morphology, substrate strength, and ac drive amplitude. The pronounced ratchet effects that we observe in some regimes can be exploited for pattern sorting in hard and soft matter systems. Published by the American Physical Society 2024

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC

Layered patterns of active scalar fields in a two-dimensional magnetohydrodynamic system

Here, we observe the formation of staircase patterns in the magnetic potential (𝐴) in a weakly magnetized two-dimensional magnetohydrodynamic system driven by a forced, fluctuating vortex array. Layering occurs due to inhomogeneous mixing of 𝐴 by vortex cells. Magnetic Reynolds number (𝑅 𝑚 )–dependent quenching of the turbulent diffusion of 𝐴 by weak magnetic fields increases the disparity between the (short) cell circulation time and the (long) time for intercell transport of magnetic potential. Thus, magnetic fields strengthen transport barriers between cells and reinforce the staircase, relative to its passive scalar counterpart. The analysis reveals a feedback mechanism, which promotes staircase formation. Magnetic staircases persist in both the flux expulsion (𝑅 𝑚 ⁢𝑣$^2_𝐴$/𝑈$^2_0$<1) and vortex disruption (𝑅 𝑚 ⁢𝑣$^2_𝐴$/𝑈$^2_0$≥1) limits. In the latter case, residual vortex cells homogenize 𝐴. Global layering morphology is shown to be well characterized by staircase curvature. Stochastic forcing of magnetic potential can support magnetic staircases against resistive decay.

magnetohydrodynamics

Understanding Oxide–Metal Interactions During Hot Isostatic Pressing to Diffusion Bond Aluminum Alloy 6061 Plates

The interaction between Mg, Si, and Al 2 O 3 during hot isostatic pressing diffusion bonding of aluminum alloy 6061 (AA6061) plates was investigated through thermodynamic calculations and experimental microstructural characterization. Thermodynamic calculations as functions of temperature, pressure, and composition revealed that the interaction among Mg, Si, and Al 2 O 3 yields Mg 2 Si and either MgO + Al or MgAl 2 O 4 + Al, facilitating the reduction of Al 2 O 3 and allowing Al/Al metallic bonds to form. Total pressure variation had a negligible influence on the oxygen partial pressure, and consequently, the reaction product formation. Oxygen partial pressure variation as a function of temperature and initial amount of Al 2 O 3 determined the formation of either MgO or MgAl 2 O 4 . Experimental Hot Isostatic Pressure (HIP) bonding at 723 K and 833 K under a constant pressure of 1017 atm documented the cooling rate-dependent formation of β–Mg 2 Si precipitates. High-resolution transmission electron microscopy imaging and selected area electron diffraction patterns verified the formation of β–Mg 2 Si and MgO at the interface but did not detect MgAl 2 O 4 . In conclusion, findings from this study clarify the role of thermochemical interactions in oxide disruption and bonding mechanisms during HIP diffusion bonding of AA6061 and provide guidance for optimizing joining processes for monolithic nuclear fuel assemblies.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Data-Driven Modeling and Control of Systems with Plasma-Surface Interactions (Final Technical Report)

This final technical report summarizes the activities and accomplishments in the period from February 2023 thru January 2026. The objective of the proposed research is to investigate the physical mechanisms and processes underlying the formation of structures and patterns in systems with plasma-surface interactions. In the past decades, there have been extensive studies on the interaction of glow discharges, dielectric barrier discharges, and arc discharges with confining or intervening surfaces. The advancement of the understanding of these phenomena is not only of fundamental scientific interest and relevance to the knowledge of the plasma state, but also with profound implications in various technological applications. The research will integrate theoretical, computational, and experimental work within an innovative framework of data assimilation, i.e., optimally combining model predictions with measurements. The scientific merit of this research has three aspects. Firstly, it extends the studies of plasma-surface interactions to systems with insulator surfaces and multi-layer systems, while existing studies are predominantly on electrode surfaces. Secondly, it expects to develop a novel data-driven modeling approach based on data assimilation to enhance the predictive and control capabilities, which could make transformative contributions to basic plasma research. Thirdly, it will shed new light on outstanding problems related to formation of patterns interfacing plasmas. This project also aims to launch an education and outreach initiative at Texas A&M University-Kingsville, a non-R1, minority-serving institution in South Texas. The initiative is structured as a four-tier pyramid. Tier one will be a webinar series for culture and capacity building to inform broader audience in the region about the research fields of plasma science and engineering. Tier two will be the creation and offering of an upper-level undergraduate course on introductory plasma physics, which will help with the recruitment for the upper tiers. On tier three, we will engage and mentor senior design students to conduct work toward the research goal of this project. There will also be a certificate program on general plasma science for undergrad and graduate students, part of which will be lab training at Princeton University. Tier four will be the supervision and mentoring of Ph.D. students. Therefore, this project will systematically expand the talent pipeline, broaden participation from communities historically and geographically underrepresented in DOE SC research portfolio, significantly improve the research and education capacity at the PI’s institution, and contribute to developing a diverse workforce in plasma science and engineering.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Real-time tracking and analysis of gas bubble dynamics in laser powder bed fusion using in-situ X-ray characterization and machine learning

Porosity defects remain a significant challenge in the laser powder bed fusion (LPBF) process, adversely affecting the mechanical properties and reliability of additively manufactured components. Here, this study investigates the real-time formation and trajectory of gas bubbles during LPBF of Al6061 alloy using advanced in-situ X-ray characterization and machine learning. The unsupervised Gaussian mixture model and particle tracking algorithm developed are able to precisely track and quantify the properties of gas bubbles and keyhole pores. Our analysis identified five distinct types of gas bubble formation and movement patterns, emphasizing the diverse origins and behaviors of these defects. It enables precise quantification of trajectories, velocities, and morphological changes of gas bubbles, offering a granular view of the subsurface dynamics within the melt pool. Additionally, we explored keyhole-induced pore dynamics, revealing the critical role of keyhole oscillation and collapse for the formation of both large and small gas pores. It defines four different regions of gas bubble movement within the melt pool, providing a clearer understanding of how local fluid dynamics affect pore behavior. The results underscore the importance of integrating in-situ experimental observation and automated machine learning to develop a more robust predictive model for defect formation in LPBF.

In-situ X-ray imaging

Emerging hierarchical dislocation structures: Insights from scanning electron microscopy-electron backscatter diffraction in situ tensile testing and multifractal analysis

Understanding the evolution of dislocation structures during plastic deformation is critical for predicting the mechanical performance of metallic materials. In this work, we applied in situ scanning electron microscopy/electron backscatter diffraction tensile testing combined with multifractal (MF) analysis to assess deformation-induced dislocation structure evolution in solution-annealed 304 L stainless steel, both in its as-received and neutron-irradiated states (5.4 displacements per atom). The analysis of kernel average misorientation patterns revealed the formation of hierarchical dislocation arrangements that exhibit clear MF scaling behavior. Despite pronounced visual differences between nonirradiated and irradiated specimens—most notably, the appearance of dislocation channels after irradiation—the singularity spectra suggest that both conditions give rise to similar underlying hierarchical structures. MF analysis provides a quantitative measure of the spatial complexity and self-organization of dislocation patterns, highlighting the accelerated emergence and evolution of the dislocation structures in irradiated polycrystalline materials, as well as the limitation of their spatial extent. The findings indicate that irradiation not only modifies microstructure but also alters correlation-driven dislocation organization. More generally, they demonstrate that MF analysis is a powerful tool for probing mesoscale deformation mechanisms.

Dislocation structures

Low-symmetry polymorph of GaP upends bonding paradigms of metallic high-pressure III–V compounds

Here, the pressure-induced polymorphism of binary octet compounds has long been considered a settled problem although the possible atomic disordering of some phases remains a puzzling observation. Taking GaP as a case study, we conclude, through x-ray microdiffraction and first-principles calculations, that its high-pressure metallic phase (previously reported as being disordered) adopts in fact an ordered base-centered monoclinic structure previously unknown in this class of compounds. The formation of layered patterns with variable degrees of interlayer dimerization, as observed in GaP, marks a paradigm shift of our understanding of ordering in octet high-pressure phases which calls for a more extensive re-examination. A rich polymorphism with fine tuning of chemical and physical properties can be envisioned.

36 MATERIALS SCIENCE

Integrated modeling of boron powder injection for real-time plasma-facing component conditioning

An integrated modeling framework for investigating the application of solid boron (B) powder injection for real-time surface conditioning of plasma-facing components (PFCs) in tokamak environments is presented. Utilizing the DIII-D impurity powder dropper (IPD) setup, this study simulates B powder injection scenarios ranging from milligrams to tens of milligrams per second, corresponding to boron flux rates of 10 20 –10 21 B/s in standard L-mode conditions. The comprehensive modeling approach combines EMC3-EIRENE for simulating the deuterium plasma background and the Dust Injection Simulator (DIS) for the ablation and transport of the boron powder particles. EMC3 trace impurity fluid modeling results show substantial boron transport to the inboard lower divertor, predominantly influenced by the main ion plasma flow. The dependency on powder particle size (5-250 µm) was found to be insignificant for the scenario considered. The effects of erosion and redeposition were considered to reconcile the discrepancies with experimental observations, which saw substantial deposition on the outer divertor plasma-facing components. For this purpose, the WallDYN3D code was updated to include boron sources within the plasma domain and integrated into the modeling framework. The mixed-material migration modeling shows evolving boron deposition patterns, suggesting the formation of mixed B-C layers or predominantly B coverage depending on the powder mass flow rate. While the modeling outcomes at lower B injection rates tend to align with DIII-D experimental observations, the prediction of near-pure boron layers at higher rates has yet to be experimentally verified in the carbon environment of the DIII-D tokamak. The extensive reach of boron layers found in the modeling suggests the need for modeling that encompasses the entire wall geometry for more accurate experimental correlations. This integrated approach sets a precedent for analyzing and applying real-time in-situ boron coating techniques in advanced tokamak scenarios, potentially extendable to ITER.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Roadmap for Photonics with 2D Materials

Triggered by advances in atomic-layer exfoliation and growth techniques, along with the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or a few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals now constitute a broad research field expanding in multiple directions through the combination of layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary subset of those directions, where 2D materials contribute remarkable nonlinearities, long-lived and ultraconfined polaritons, strong excitons, topological and chiral effects, susceptibility to external stimuli, accessibility, robustness, and a completely new range of photonic materials based on layer stacking, gating, and the formation of moiré patterns. These properties are being leveraged to develop applications in electro-optical modulation, light emission and detection, imaging and metasurfaces, integrated optics, sensing, and quantum physics across a broad spectral range extending from the far-infrared to the ultraviolet, as well as enabling hybridization with spin and momentum textures of electronic band structures and magnetic degrees of freedom. The rapid expansion of photonics with 2D materials as a dynamic research arena is yielding breakthroughs, which this Roadmap summarizes while identifying challenges and opportunities for future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

2D materials

Experimental Realization of Discrete Time Quasicrystals

Floquet (periodically driven) systems can give rise to unique nonequilibrium phases of matter without equilibrium analogs. The most prominent example is the realization of discrete time crystals. An intriguing question emerges: What other novel phases can manifest when the constraint of time periodicity is relaxed? In this study, we explore quantum systems subjected to a quasiperiodic drive. Leveraging a strongly interacting spin ensemble in diamond, we identify the emergence of long-lived discrete time quasicrystals. Unlike conventional time crystals, time quasicrystals exhibit robust subharmonic responses at multiple incommensurate frequencies. Furthermore, we show that the multifrequency nature of the quasiperiodic drive allows for the formation of diverse patterns associated with different discrete time quasicrystalline phases. Our findings demonstrate the existence of nonequilibrium phases in quasi-Floquet settings, significantly broadening the catalog of novel phenomena in driven many-body quantum systems.

Exotic phases of matter

Surface deformation coupled with self-organized pattern on a liquid anode of 1 atm DC glow discharge

Intricate, self-organized plasma structures observed above the surface of a liquid anode of atmospheric DC glow discharge were found to give rise to coherent, organized surface deformation and mechanical wave formation at the plasma–liquid interface. This new phenomenon indicates that the liquid is closely coupled to the plasma by the anode sheath’s electrohydrodynamic (EHD) force. A scientific question then arises: Do surface perturbations, coupled with the nonuniform surface charge distribution, enhance the electric field and induce self-organization? Using the reflective background-oriented schlieren technique, the liquid surface profile under the plasma pattern was measured for the first time. The results show that surface distortions are driven by the repulsive Coulomb force of nonuniform net-negative surface charge acted by the anode sheath field. The impacts of various operating parameters on the patterns and surface waves were examined, revealing the significance of gas heating and liquid charge relaxation time in the pattern formation mechanism. Time-resolved dynamics of a pulsed DC discharge indicated that the surface deformation only appeared after the establishment of plasma patterns. Statistically, the surface wave under the plasma has high wave numbers (8000–16000 m −1 ) and small amplitudes ($<$ 10 µm), generally found in the capillary wave regime. Yet the motion of surface deformations is in tandem with the plasma pattern and exhibits a nondispersive nature of constant phase velocity (0.1–0.4 m s −1 ), suggesting the dominant role of EHD force over the surface tension in the observed surface wave. These results indicate that the deformed liquid surface is driven by the EHD force of the plasma sheath. Although they share a similar geometry, the deformation and wave dynamics of the liquid surface do not stimulate a plasma pattern. Importantly, the complex EHD coupling in the plasma–liquid system raises awareness and new challenges for plasma control engineering, and the quantitative characteristics of the nondispersive surface wave are informative for advancing relevant theory and modeling.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Lanthanum-Promoted Electrocatalyst for the Oxygen Evolution Reaction: Unique Catalyst or Oxide Deconstruction?

A conventional performance metric for electrocatalysts that promote the oxygen evolution reaction (OER) is the current density at a given overpotential. However, the assumption that increased current density at lower overpotentials indicates superior catalyst design is precarious for OER catalysts in the working environment, as the crystalline lattice is prone to deconstruction and amorphization, thus greatly increasing the concentration of catalytic active sites. We show this to be the case for La 3+ incorporation into Co 3 O 4 . Powder X-ray diffraction (PXRD), Raman spectroscopy and extended X-ray absorption fine structure (EXAFS) reveal smaller domain sizes with decreased long-range order and increased amorphization for La-modified Co 3 O 4 . This lattice deconstruction is exacerbated under the conditions of OER as indicated by operando spectroscopies. The overpotential for OER decreases with increasing La 3+ concentration, with maximum activity achieved at 17% La incorporation. HRTEM images and electron diffraction patterns clearly show the formation of an amorphous overlayer during OER catalysis that is accelerated with La 3+ addition. O 1s XPS spectra after OER show the loss of lattice-oxide and an increase in peak intensities associated with hydroxylated or defective O-atom environments, consistent with Co(O) x (OH) y species in an amorphous overlayer. Furthermore, our results suggest that improved catalytic activity of oxides incorporated with La 3+ ions (and likely other metal ions) is due to an increase in the number of terminal octahedral Co(O) x (OH) y edge sites upon Co 3 O 4 lattice deconstruction, rather than enhanced intrinsic catalysis.

Catalysts

Anomalous and planar Hall effects in Co 1−x Ho x thin films across the magnetic sublattice compensation temperature

Metallic amorphous ferrimagnets derived from alloying 3d transition metals with 4f-electron rare earths host fascinating effects of compensation between the 3d and 4f magnetic sublattices. Here, a detailed study of the anisotropic magnetoresistance (Δρ xx ), planar Hall effect (ρ xy PHE ), and anomalous Hall effect (ρ xy AHE ) is reported on a series of Co 1−x Ho x thin films over a wide field–temperature (H–T) phase space. Close to the magnetic compensation temperature, the ρ xy AHE –H loops show a double sign reversal and signatures of spin-flop transition at higher fields. The Δρ xx and ρ xy PHE also display strong deviations from the classical angular dependence seen in soft ferromagnets like permalloy as the angle ϕ between in-plane current and magnetic field is scanned from 0 to 2π. It is argued that the non-zero orbital angular momentum of Ho ions in the lattice and stabilization of bubble domains below magnetic saturation may be responsible for such features. Direct imaging of magnetic textures with x-ray photoelectron microscopy shows the formation of stripe domain patterns in the regime of sublattice compensation. Such stripes are likely to transform into magnetic bubbles before full saturation is reached in a large magnetic field.

36 MATERIALS SCIENCE

Investigation of N 2 /O 2 plasma interaction with Pt-catalyst: effect of metastable adsorbates on product hysteresis

The coupling of catalysts and atmospheric-pressure plasma has the potential to improve the efficiency of certain catalytic reactions. Understanding the changes that the catalyst surface undergoes during exposure to plasma is key to improving plasma–catalytic performance. In this work, long term exposure of Pt–Al 2 O 3 powder catalyst to an Ar/N 2 /O 2 non-equilibrium atmospheric-pressure plasma-jet was investigated. Products produced by the interaction were analyzed downstream with Fourier-transform infrared spectroscopy while surface species were analyzed operandi with diffuse reflectance infrared Fourier transform spectroscopy. During exposure, the catalyst temperature was ramped cyclically between 100 °C and 350 °C to understand how substrate temperature affects the plasma–catalyst interaction. Long-lasting changes were revealed to take place on the catalyst surface during plasma exposure. At low temperatures, Pt–O and Pt–NO accumulate on the surface which react at elevated temperatures to form NO 2 . NO 2 initially appears to spill on to the Al 2 O 3 support as nitrites and nitrates instead of desorbing. Stable surface conditions are only achieved after prolonged plasma exposure, when nitrate sites on the Al 2 O 3 support are filled. By changing the catalyst temperature at various rates, the impact of total plasma species flux to the surface was analyzed. It was found that decreasing the heating rate increased the hysteresis in the pattern of NO 2 formation during thermal cycling. The variation with temperature demonstrates that plasma exposure results in a buildup of surface NO x and oxygen species which react or desorb at high temperatures. The observed changes are discussed from the generic viewpoint that a non-equilibrium plasma interacting with a catalyst at low temperature introduces metastable steady-state surface conditions. Upon heating above a threshold temperature, the introduced surface modifications can change either due to thermal effects, or, for a plasma environment, by additional interaction with the incident plasma species flux. The surface/material changes take place in a highly predictable fashion and after sufficient time above the threshold temperature reach a steady-state condition that is different from the transient behavior that is observed during initial heating. During cooling the plasma-surface interaction exhibits a different behavior than during heating, and this results in hysteresis of diverse observables. The metastability/hysteresis description appears quite generic and analogous to hysteresis behavior seen for different systems. Furthermore, it is expected to be useful for understanding the consequences of plasma–catalyst surface interactions for various systems.

36 MATERIALS SCIENCE

Dynamics of Thermally Driven Domain Transformation in Ferroelectric Thin Films

An important feature in ultrathin ferroelectric films is the spontaneous formation of nanoscale polarization domain patterns. Epitaxial strain can greatly increase the ferroelectric transition temperature such that films can be in the ferroelectric state during growth. On the other hand, depolarization fields compete with ferroelectricity in ultrathin films, and, consequently, the optimal domain configuration during growth is a moving target. Under these conditions it is readily possible for a grown film to be in a nonequilibrium domain configuration. As the energy landscape in the system is quite complex, the relaxation dynamics by which a system can evolve towards the true equilibrium configuration are also quite interesting. Here, to capture the details of this process we used Bragg-geometry x-ray photon correlation spectroscopy (XPCS), in which x-ray scattering speckle patterns contain the information from the domain arrangements inside the film. With modest heating (∼15⁢0 °C) domain relaxation from 𝑇 (tetragonal) to 𝑀 𝐶 (monoclinic) was observed in BaTiO 3 films grown on ultrathin ferroelectric PbTiO 3 layers. Two-time correlation analysis reveals fascinating details associated with sticking points and reversals in the process.

36 MATERIALS SCIENCE

X-Band Radar and Surface-Based Observations of Cold-Season Precipitation in Western Colorado’s Complex Terrain

Abstract Hydrologic processes associated with intermountain cold-season precipitation in the Upper Colorado River basin have important impacts on avalanche forecasting and water resource management. However, traditional weather radar networks struggle with observations in this complex terrain. Data collected during the Study of Precipitation, the Lower Atmosphere, and the Surface for Hydrometeorology (SPLASH) and its sister campaign, Surface Atmosphere Integrated Field Laboratory (SAIL) in the East River watershed of western Colorado, are used to examine a multistorm period from 23 December 2021 to 1 January 2022 that contributed 35% of the total winter precipitation in this watershed. Dual-polarization X-band radar and disdrometer measurements show ∼30-mm differences in precipitation amount at two sites in proximity over four distinct storm events within the period. Wind patterns, synoptic forcings, microphysical characteristics of precipitation, and surface meteorology are analyzed to explain the observed spatial variability of cold-season precipitation in complex mountainous terrain. Analysis shows that differences over time within this event are mainly accounted for by synoptic forcings, such as frontal passages; differences between sites are accounted for by the impact of variations in local wind patterns on precipitation microphysics. Patterns of surface precipitation intensity are compared and found to be correlated with X-band radar signatures; a relationship between a strong dendritic growth stage and intense low-density surface precipitation is reinforced by this study. This relationship demonstrates the importance of particle growth mechanisms on surface snowfall patterns in high-altitude complex terrain, underscoring the importance of realistic microphysical parameterizations. Significance Statement The amount and density of snowpack from western Colorado winter storms have significant impacts on water resources in the Upper Colorado River basin. Snowpack characteristics are affected by small-scale differences in how snow forms in the atmosphere. These differences are hard to study in the complex terrain of the Rockies, but data from the SPLASH and SAIL field campaigns allows us to investigate how snow crystal formation and mountain-driven wind patterns affect snow near the surface. Our study finds that snow crystal growth varies over small space and time scales and is likely controlled by the terrain beneath a given location and resultant local wind patterns. These results imply that predicting snowpack in the Rockies requires properly representing local wind patterns and crystal growth processes in models.

Heflin, Stella

A Visual Understanding of Circular Dichroism Spectroscopy

Mapping chemical and structural properties to electronic and magnetic responses is critical to many applications such as quantum information science, where the precise storage and transmission of unique information is paramount. Specifically, constructing molecules and materials that provide strong polarized responses at tunable frequencies and with large anisotropies is key to optical processing of quantum information. Chiral molecules provide chiroptical response to circularly polarized light, making them attractive for quantum information science and other applications related to sensing, polarized photodetectors, and spintronics. Predicting a molecular design, a priori, with large anisotropies to circularly polarized light is challenging due to the complex interplay between electric and magnetic components of the optical response. In this work, we explore a visual representation of the electronic chiroptical response by decomposing the rotary strength into its constituent components. Here, we make use of the intuitive electronic oscillator framework to develop classical intuition regarding the rotary strength and its constituents. We explore three model chemical systems that exhibit local and global chirality. Our analysis reveals that local chirality necessarily exhibits competition between the local chiral center and chirality induced in other fragments of the molecule, resulting in both unexpected nonmonotonic trends and sign flips in chemically adjacent geometries. Furthermore, we can visually distinguish between local and global chirality via examination of the transition chiral tensor. Interestingly, we make strong connections to ferromagnetic and antiferromagnetic spin systems in that chiroptically inactive transitions exhibit antiferromagnetic-like alternating orbital patterns while active transitions show domain formation in an ferromagnetic-like alignment that produces a net chiroptical response.

36 MATERIALS SCIENCE