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At least 775 records · Page 43
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Solid-state NMR of unlabeled plant cell walls: high-resolution structural analysis without isotopic enrichment

Abstract Background Multidimensional solid-state nuclear magnetic resonance (ssNMR) spectroscopy has emerged as an indispensable technique for resolving polymer structure and intermolecular packing in primary and secondary plant cell walls. Isotope ( 13 C) enrichment provides feasible sensitivity for measuring 2D/3D correlation spectra, but this time-consuming procedure and its associated expenses have restricted the application of ssNMR in lignocellulose analysis. Results Here, we present a method that relies on the sensitivity-enhancing technique Dynamic Nuclear Polarization (DNP) to eliminate the need for 13 C-labeling. With a 26-fold sensitivity enhancement, a series of 2D 13 C– 13 C correlation spectra were successfully collected using the unlabeled stems of wild-type Oryza sativa (rice). The atomic resolution allows us to observe a large number of intramolecular cross peaks for fully revealing the polymorphic structure of cellulose and xylan. NMR relaxation and dipolar order parameters further suggest a sophisticated change of molecular motions in a ctl1 ctl2 double mutant: both cellulose and xylan have become more dynamic on the nanosecond and microsecond timescale, but the motional amplitudes are uniformly small for both polysaccharides. Conclusions By skipping isotopic labeling, the DNP strategy demonstrated here is universally extendable to all lignocellulose materials. This time-efficient method has landed the technical foundation for understanding polysaccharide structure and cell wall assembly in a large variety of plant tissues and species.

09 BIOMASS FUELS↗
DOE OSTI2025

Taylor limit studies for local helicity injection plasma startup

Solenoid-free tokamak startup techniques can simplify the design and reduce the cost of tokamak-based fusion energy systems. The newly commissioned Pegasus-III spherical tokamak provides a dedicated platform for developing a scalable solenoid-free startup approach. Local helicity injection (LHI) is one promising technique being developed on Pegasus-III, which uses compact edge current sources to drive open field line current I inj that is redistributed via helicity-conserving instabilities to initiate tokamak plasmas. These instabilities relax the system toward a minimum energy state described by Taylor relaxation theory. This relaxation process imposes a global current limit for LHI plasmas, referred to as the Taylor limit I TL ⁠, which can dictate the plasma current I p evolution. Experiments on Pegasus and Pegasus-III show that increasing this limit leads to more effective utilization of the available helicity input and higher I p plasmas. Initial Pegasus-III experiments have verified the expected I TL $\varpropto$ ( I inj B T ) 1/2 scaling holds for B T and I inj up to 0.3 T on axis and 12 kA ⁠, respectively. Additionally, data from different injector arrays show that the width of the injector aperture directly alters I TL and can be leveraged for future injector design optimization. Throughout these scaling studies, discharges were overdriven at I p = I TL by providing excess helicity input. Intermittent bursts of n = 1 magnetic activity consistent with large-scale reconnection events occurred more often as the system was increasingly overdriven leading to a flattening of the λ = μ 0 J ∥ / |B| profile, where J ∥ is the parallel current density.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS2000

Sigmoid CME Source Regions at the Sun: Some Recent Results

Identifying Coronal Mass Ejection (CME) precursors in the solar corona would be an important step in space weather forecasting, as well as a vital key to understanding the physics of CMEs. Twisted magnetic field structures are suspected of being the source of at least some CMEs. These features can appear sigmoid (S or inverse-S) shaped in soft X-ray (SXR) images. We review recent observations of these structures and their relation to CMEs, using soft X-ray (SXR) data from the Soft X-ray Telescope (SXT) on the Yohkoh satellite, and EUV data from the EUV Imaging Telescope (EIT) on the SOHO satellite. These observations indicate that the pre-eruption sigmoid patterns are more prominent in SXRs than in EUV, and that sigmoid precursors are present in over 50% of CMEs. These findings are important for CME research, and may potentially be a major component to space weather forecasting. So far, however, the studies have been subject to restrictions that will have to be relaxed before sigmoid morphology can be used as a reliable predictive tool. Moreover, some CMEs do not display a SXR sigmoid structure prior to eruption, and some others show no prominent SXR signature of any kind before or during eruption.

Sterling, Alphonse C.↗
DOE OSTI2023

Evolution of the Cellulose Microfibril through Gamma-Valerolactone-Assisted Co-Solvent and Enzymatic Hydrolysis

Biomass recalcitrance during deconstruction remains a key bottleneck to affordable biomass processing technologies. A clear connection between the cell wall structure and biomass deconstruction is necessary to understand how lignocellulosic material is broken down to valuable monomeric components. Here, we monitor changes in the cellulose microfibril domains of poplar, sorghum, and switchgrass throughout gamma-valerolactone (GVL)–water co-solvent pretreatment and enzymatic hydrolysis using solid-state 13 C cross-polarization magic angle spinning nuclear magnetic resonance spectroscopy (CP/MAS 13 C-NMR) and wide-angle X-ray scattering (WAXS). Spectral fitting of NMR peaks corresponding to different cellulose microenvironments at the C 4 carbon center suggests that a mildly acidic GVL–water co-solvent pretreatment of poplar leads to nearly full removal of xylan–cellulose linkages, which primes the cellulose for enzymatic attack. The spectral fitting also suggests that the pretreatment causes significant depletion of the inaccessible fibril surface domains with an increase in more thermally stable crystalline resonances (I β ). WAXS confirmed a decrease in the lattice spacing between (200) crystalline planes with increasing co-solvent pretreatment severity. These results are interpreted as an opening of bound microfibril surfaces previously inaccessible to the co-solvent system, which leaves behind a more thermally stable, crystalline domain that is potentially prone to relaxation and recrystallization. Full conversion of residual GVL-pretreated biomass was achieved after the GVL co-solvent pretreatment at 140 °C using a commercial enzyme cocktail, CTec2, which contains different cellulases and other enzymes. Spectral fitting of enzymatically hydrolyzed samples by a single engineered cellulase, CelR, suggests that the residual cellulose recalcitrance is mainly due to the inability of CelR to digest the I β crystalline domain present in pretreated samples. This work helps to provide new information regarding the structure of the cell wall and recalcitrance throughout GVL–water mild acidolysis and CelR enzymatic biomass deconstruction by tracking the evolution of structural domains within the cellulose microfibril. This work further directs recommendations for improving the conversion and sugar yields in future studies. Finally, our findings inform inquiry into larger questions of cellulose recalcitrance through GVL pretreatment and CelR enzymatic hydrolysis and give insight into subsequent required steps for full cellulose conversion with attention to the most recalcitrant cellulose structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

The weathered bedrock vadose zone: A hidden control on water availability in the western United States (Final Technical Report)

This report summarizes the research completed during the project entitled "The weathered bedrock vadose zone: A hidden control on water availability in the western United States" (Award: DE-SC0018039). The report covers work completed between 9/15/17 and 9/14/20. The objective of the exploratory project work was to evaluate the overarching hypothesis that the subsurface underlying actively eroding landscapes is systematically structured as a result of a balance between weathering and erosion and that this structure leads to dynamic moisture storage within weathered rock. To accomplish project objectives, we characterized hillslope weathering profile structure and conducted subsurface moisture monitoring across four study sites with comparable bedrock types but differing erosion rate and hydroclimate: The Angelo Coast Range Reserve (ACRR), Sagehorn-Russell Ranch (SRR), Antelope Valley Ranch (AVR), and the LBNL Watershed Function Scientific Focus Area (SFA). New characterization and monitoring infrastructure at the AVR and SFA sites was established through this project and enables long-term monitoring of hydrologic and carbon fluxes at the sites for comparison with long-term monitoring in other sites. Deep drilling, downhole logging, and characterization of chemistry and porosity of rock recovered from drilling reveals two weathering fronts across the sites. A shallower front is marked by the extent of pervasive fracturing and oxidation of pyrite and organic carbon. A deeper weathering front is marked by the appearance of open fractures and discoloration. At the AVR site, multiple ridge tops of different hillslope length were investigated to establish the relationship between the weathering front and topography. Drilling reveals that the fraction of the hillslope relief that is weathered scales with hillslope length, consistent with the theoretical framework that guided the project relating groundwater drainage with landscape evolution. With the establishment of new boreholes, we have documented significant water storage in weathered bedrock using low-field borehole nuclear magnetic resonance (NMR) across all four sites. In the upper 4 m of bedrock, the average water contents at ACRR, AVR, SRR, and SFA are approximately 25%, 16%, 25%, 23% respectively. At the ACRR site, where long-term monitoring via neutron probe surveys and time-domain transmission sensors are available, we have demonstrated that NMR reliably records moisture content and importantly, moisture content dynamics in weathered bedrock. Across all sites, our NMR monitoring has also revealed that a considerable fraction of the water storage occurs in fractures or pores that are significantly larger than the fine-grained bedrock matrix of the parent rock. To identify the proportion of water storage occurring in fractures and large pores, we analyzed the NMR signal by evaluating both the sum of echoes and an inversion of the NMR signal for a distribution of T2 relaxation times. Both methods reveal that at least 20% of the water storage occurs in fractures and larger pores across all sites. To constrain the interpretation of the in-situ field-scale NMR measurements, we compare the NMR response in the field to independent pore-structure information obtained via helium pycnometry. Results support the inference that dynamic seasonal water storage is dominantly restricted to the fracture network, which can reach 7% of the total volume. This dynamic range in water content is comparable to that of some soils, underscoring the need to understand how this region of the Earth System is structured, and functions as a hydrologic reservoir.

58 GEOSCIENCES↗
DOE OSTI2021

Ab initio ultrafast spin dynamics in solids

Spin relaxation and decoherence is at the heart of spintronics and spin-based quantum information science. Currently, theoretical approaches that can accurately predict spin relaxation of general solids including necessary scattering pathways and are capable of nanosecond to millisecond simulation time are urgently needed. We present a first-principles real-time density-matrix approach based on Lindblad dynamics to simulate ultrafast spin dynamics for general solid-state systems. Through the complete first-principles descriptions of pump, probe, and scattering processes including electron-phonon, electron-impurity, and electron-electron scatterings with self-consistent electronic spin-orbit couplings, our method can directly simulate the ultrafast pump-probe measurements for coupled spin and electron dynamics over nanoseconds at any temperatures and doping levels. We first apply this method to a prototypical system GaAs and obtain excellent agreement with experiments. We found that the relative contributions of different scattering mechanisms and phonon modes differ considerably between spin and carrier relaxation processes. In sharp contrast to previous work based on model Hamiltonians, we point out that the electron-electron scattering is negligible at room temperature but becomes dominant at low temperatures for spin relaxation in n-type GaAs. We further examine ultrafast dynamics in novel spin-valleytronic materials: monolayer and bilayer WSe 2 with realistic defects. We find that spin relaxation is highly sensitive to local symmetry and chemical bonds around defects. For the bilayer WSe 2 , we identify the scattering pathways in ultrafast dynamics and determine relevant dynamical properties, essential to its utilization of unique spin-valley-layer locking effects. In conclusion, our work provides a predictive computational platform for spin dynamics in solids, which has potential for designing new materials ideal for spintronics and quantum information technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2004

Finite Element Modeling Used to Study Stress Distribution on the Foot

A method to study the stress distribution inside the forefoot during walking was developed at the Cleveland Clinic Foundation by a researcher from the NASA Glenn Research Center. In this method, a semiautomated process was outlined to create a three-dimensional, patient-specific, finite element model (FEM) of the forefoot using magnetic resonance images (MRI). The images were processed in Matlab using the k-nearest neighbor (k-NN) classification algorithm and Sobel edge detection to separate the different tissue types: bone, skin, fat, and muscle. This information was used to create curves and surfaces that were exported to an FEM preprocessor known as Truegrid. In Truegrid, eight-noded or brick elements were created by using surface mapping. The FEM was processed and postprocessed in Abaqus. Material properties of the models were obtained from past experiments such as fat pad confined compression, skin axial and biaxial tests, muscle in vivo compressive tests, and reference literature (bone properties). Nonlinear (hyperelastic) material models were used for the skin (epidermis and dermis), fat, and muscles; and a linear elastic model was used for the bones. Muscle activation during walking yielded uncertainties in the muscle material model since contracted muscles are stiffer than relaxed muscles. These uncertainties were resolved by performing a sensitivity analysis of the muscle material properties. The original properties were multiplied by arbitrary factors of 2, 3, 0.5, and 0.33. The strain and stress distributions, as well as the locations of peak values, were similar in all cases. The peak contact pressure P obtained for each case varied with respect to the applied factor f as follows:

Morales, Nelson↗
DOE OSTI2025

Particle collisionality in scaled kinetic plasma simulations

Kinetic plasma processes, such as magnetic reconnection, collisionless shocks, and turbulence, are fundamental to the dynamics of astrophysical and laboratory plasmas. Simulating these processes often requires particle-in-cell (PIC) methods, but the computational cost of fully kinetic simulations can necessitate the use of artificial parameters, such as a reduced speed of light and ion-to-electron mass ratio, to decrease expense. While these approximations can preserve overall dynamics under specific conditions, they introduce nontrivial impacts on particle collisionality that are not yet well understood. In this work, we develop a method to scale particle collisionality in simulations employing an artificial speed of light and/or an artificial ion-to-electron mass ratio. By introducing species-dependent scaling factors, we independently adjust inter- and intra-species collision rates to better replicate the collisional properties of the physical system. Our approach maintains the fidelity of electron and ion transport properties while preserving critical relaxation rates, such as energy exchange timescales, within the limits of weakly collisional plasma theory. Furthermore, we demonstrate the accuracy of this scaling method through benchmarking tests against theoretical relaxation rates and connecting to fluid theory, highlighting its ability to retain key transport properties. Existing collisional PIC implementations can be easily modified to include this scaling, which will enable deeper insights into the behavior of marginally collisional plasmas across various contexts.

Totorica, S. R. [Princeton Univ., NJ (United State↗
NASA NTRS2007

Sintering of Lunar and Simulant Glass

Most oxygen-extraction techniques are temperature-dependent, with higher temperatures resulting in higher oxygen yield. An example is hydrogen reduction, in which the optimum process temperature is 1050 C. However, glass-rich lunar soil begins to show the effects of sintering at temperatures of 900 C or lower. Sintering welds particles together due to viscous relaxation of the glass in the sample. One approach to avoid problems related to sintering, such as difficulty in removing waste material from the reactor, is to keep the soil in motion. One of several methods being studied to accomplish this is fluidized-bed processing techniques, in which the grains are kept in motion by the action of flowing reductant gas. The spent material can be removed from the chamber while still fluidized, or the fluidizing motion can continue until the material has cooled below approx. 500 C. Until end-to-end prototypes are built that can remove the heated soil, the most practical option is to keep the bed fluidized while cooling the waste material. As ISRU technology advances, another option will become valuable, which is to intentionally sinter the material to a great enough extent that it becomes a brick. The free iron in lunar soil is magnetic, and ferromagnetic bricks can be manipulated by robotic systems using electromagnetic end effectors. Finally, if an electromagnetic field is applied to the soil while the brick is being formed, the brick itself will become a magnet. This property can be used to create self-aligning bricks or other building materials that do not require fasteners. Although sintering creates a challenge for early lunar surface systems, knowledge gained during prototype development will be valuable for the advanced lunar outpost.

Cooper, Bonnie L.↗
NASA NTRS1990

Transition from moving to stationary double layers in a single-ended Q machine

Large-amplitude (less than about 100 percent) relaxation oscillations in the plasma potential are known to be generated when the cold endplate of a single-ended Q machine is biased positively. These oscillations are associated with double layers that form near the hot plate (plasma source) and travel toward the endplate at about the ion-acoustic velocity. At the endplate they dissolve and then form again near the hot plate, the entire process repeating itself in a regular manner. By admitting a sufficient amount of neutral gas into the system, the moving double layers were slowed down and eventually stopped. The production of stationary double layers requires an ion source on the high-potential side of the double layers. These ions are provided by ionization of the neutral gas by electrons that are accelerated through the double layer. The dependence of the critical neutral gas pressure required for stationary double-layer formation on endplate voltage, magnetic field strength, and neutral atom mass has been examined. These results are discussed in terms of a simple model of ion production and loss, including ion losses across the magnetic field.

Song, Bin↗
DOE OSTI2022

A 9.2-GHz clock transition in a Lu(II) molecular spin qubit arising from a 3,467-MHz hyperfine interaction

Spins in molecules are particularly attractive targets for next-generation quantum technologies, enabling chemically programmable qubits and potential for scale-up via self-assembly. Here, we report observation of one of the largest hyperfine interactions for a molecular system, A iso = 3467±50 MHz, along with an associated clock transition of unprecedented magnitude. This is achieved through chemical control of the degree of s-orbital mixing into the spin-bearing d-orbital associated with a series of spin-½ La(II) and Lu(II) complexes. Increased s-orbital character reduces spin-orbit coupling and enhances the electron-nuclear Fermi contact interaction. Both outcomes are advantageous for quantum applications: the former reduces spin-lattice relaxation, while the latter maximizes the hyperfine interaction that, in turn, generates a 9 gigahertz clock transition, leading to an increase in phase memory time from 1.0±0.4 to 12±1 microseconds for one of the Lu(II) complexes. Furthermore, these findings suggest strategies for development of molecular quantum technologies, akin to trapped ion systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Real-time sparse-sampled Ptychographic imaging through deep neural networks

Ptychography has rapidly grown in the fields of X-ray and electron imaging for its unprecedented ability to achieve nano or atomic scale resolution while simultaneously retrieving chemical or magnetic information from a sample. A ptychographic reconstruction is achieved by means of solving a complex inverse problem that imposes constraints both on the acquisition and on the analysis of the data, which typically precludes real-time imaging due to computational cost involved in solving this inverse problem. In this work we propose PtychoNN, a novel approach to solve the ptychography reconstruction problem based on deep convolutional neural networks. We demonstrate how the proposed method can be used to predict real-space structure and phase at each scan point solely from the corresponding far-field diffraction data. The presented results demonstrate how PtychoNN can effectively be used on experimental data, being able to generate high quality reconstructions of a sample up to hundreds of times faster than state-of-the-art ptychography reconstruction solutions once trained. By surpassing the typical constraints of iterative model-based methods, we can significantly relax the data acquisition sampling conditions and produce equally satisfactory reconstructions. Besides drastically accelerating acquisition and analysis, this capability can enable new imaging scenarios that were not possible before, in cases of dose sensitive, dynamic and extremely voluminous samples.

Cherukara, Mathew J↗
DOE OSTI2021

Dynamics in Flexible Pillar[ n ]arenes Probed by Solid-State NMR

Pillar[n]arenes are supramolecular assemblies that can perform a range of technologically important molecular separations which are enabled by their molecular flexibility. Here, we probe dynamical behavior by performing a range of variable-temperature solid-state NMR experiments on microcrystalline perethylated pillar[n]arene (n = 5, 6) and the corresponding three pillar[6]arene xylene adducts in the 100–350 K range. This was achieved either by measuring site-selective motional averaged 13 C 1 H heteronuclear dipolar couplings and subsequently accessing order parameters or by determining 1 H and 13 C spin–lattice relaxation times and extracting correlation times based on dipolar and/or chemical shift anisotropy relaxation mechanisms. We demonstrate fast motional regimes at room temperature and highlight a significant difference in dynamics between the core of the pillar[n]arenes, the protruding flexible ethoxy groups, and the adsorbed xylene guest. Additionally, unexpected and sizable 13 C 1 H heteronuclear dipolar couplings for a quaternary carbon were observed for p-xylene adsorbed in pillar[6]arene only, indicating a strong host–guest interaction and establishing the p-xylene location inside the host, confirming structural refinements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2022

Low Frequency ULF Waves in the Earth’s Inner Magnetosphere: Power Spectra During High Speed Streams and Quiet Solar Wind and Seeding of EMIC Waves

Here we extend the scope of the Gamayunov and Engebretson (2021, hereinafter Paper 1) work by analyzing the low frequency ultra-low-frequency (ULF) wave power spectra in the Earth’s inner magnetosphere during high speed stream (HSS) and quiet solar wind (QSW) driving conditions in the upstream solar wind (SW) and comparing our results to the results of Paper 1, where the statistics of ULF wave power spectra during coronal mass ejections (CMEs) are presented. The most important results of our statistical and comparative analyses are as follows. (a) During CMEs, HSSs, and QSW, the magnetic field power spectra of the transverse and compressional fluctuations are well approximated by power-laws in the ∼ mHz - Hz frequency range, where on average the parameters of power-law fits during CMEs and HSSs are close, and those during QSW differ considerably from the respective parameters during CMEs and HSSs. (b) The dominance of the average compressional power over the average transverse power for the low frequency ULF waves during the 0 < SYM/H . 25 nT geomagnetic conditions may serve as a proxy of HSSs in the upstream SW, whereas the opposite relation between the average powers is an indication of CMEs. (c) Independently of the SW driving conditions, a turbulent energy cascade from low frequencies in the ULF wave frequency range into the higher frequency range exists in the Earth’s inner magnetosphere, supplying the nonthermal electromagnetic seed fluctuations needed for the growth of electromagnetic ion cyclotron (EMIC) waves (∼ Hz) due to relaxation of unstable distributions of energetic magnetospheric ions.

Konstantin V. Gamayunov↗
DOE OSTI2026

Insights into Rotational and Translational Dynamics in Mixtures of Ethylene Glycol and Choline Chloride Using Nuclear Magnetic Resonance Techniques

This work examines molecular dynamics and interactions in ethylene glycol–choline chloride (EG–ChCl) mixtures across 0–33 mol % ChCl, spanning the true eutectic region near 17–20 mol % and the commonly used 1:2 formulation. We combine pulsed-field-gradient (PFG) diffusion, fast-field-cycling (FFC) relaxometry, temperature-dependent 13 C T 1 , and nuclear Overhauser effect spectroscopy (NOESY) to disentangle local from macroscopic dynamics. PFG and FFC show that both translational and average rotational motions largely track the strong increase in viscosity with ChCl content, with ethylene glycol consistently diffusing faster than the choline cation and no global dynamical anomaly at the eutectic composition. More subtle, site-specific composition effects nevertheless emerge. The ratio of the diffusion coefficient of the hydroxyl group of choline to the diffusion coefficient of the methyl group of choline displays a shallow minimum in the 17–25 mol % region, indicating a modest change in how the hydroxyl-bearing end of choline samples the underlying translational motion relative to the methyl groups. 13 C T 1 analysis shows that rotational correlation times at 25 °C generally increase with ChCl, reflecting viscosity-coupled slowing, while the CH 2 –N α site exhibits a small but reproducible deviation from this monotonic trend near the eutectic. NOESY spectra at similar compositions reveal enhanced cross-relaxation between EG and choline protons, consistent with increased headgroup–solvent contact density rather than a wholesale structural rearrangement. Overall, our multitechnique study demonstrates that EG–ChCl dynamics are predominantly viscosity-dominated, with the eutectic region acting as a subtle dynamical crossover where specific choline segments become maximally coupled to the hydrogen-bond network. These insights refine the structure–dynamics picture of choline-chloride DESs and provide practical guidance for tuning composition in electrochemical, separation, and catalytic applications.

diffusion↗
DOE OSTI2021

Computation of linear MHD instabilities with the multi-region relaxed MHD energy principle

Over the last decade, a variational principle based on a generalisation of Taylor's relaxation, referred to as multi-region relaxed magnetohydrodynamics (MRxMHDs) has been developed. The numerical solutions of the MRxMHD equilibria have been constructed using the Stepped Pressure Equilibrium Code (SPEC) (Hudson et al 2012 Phys. Plasmas 19 112502). In principle, SPEC could also be established to describe the MRxMHD stability of an equilibrium. In this work, a theoretical framework is developed to relate the second variation of the energy functional to the so-called Hessian matrix, enabling the prediction of MHD linear instabilities of cylindrical plasmas, and is implemented in SPEC. The negative and positive eigenvalues of the Hessian matrix predict the stability of an equilibrium. Verification studies of SPEC stability results with the M3D-C 1 code and the tearing mode $\Delta^{^{\prime}}$ criterion have been conducted for ideal and resistive MHD instabilities, respectively, in a pressureless cylindrical tokamak, and have shown good agreement. Overall, our stability analysis is a critical step towards understanding the MHD stability of three-dimensional MHDs where nested flux surfaces, magnetic islands and stochastic regions co-exist.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Lifting Triplet Degeneracy Through Organic‐Cation Driven Structural Perturbation to Modulate Luminescence of Sb 3+ ‐Doped Double Perovskite

The spin-orbit coupling (SOC) and the Jahn-Teller effect (JTE) alter the orbital degeneracy in materials, leading to unique optical, electronic, and magnetic properties essential in spintronics, quantum computing, and light-emitting diodes (LEDs). Here, the study employs luminescent p-xylylenediammonium (PXA) instead of Cs+ in Cs2NaInCl6 to yield 2D Sb3+-doped (PXA)2NaInCl8 double perovskite and demonstrates a non-degenerate triplet state resulting from enhanced JTE in the strong SOC regime, featuring distinct emission centers. Consequently, a broadband emission from both PXA and [SbCl6]3− spans the entire spectrum (350–750 nm), representing a rare single-source multi-emissive 2D perovskite. With in-depth comparative structural, temperature-dependent photo-physical, and theoretical studies, it is elucidated that the synergistic effect of SOC and JTE on the Eg and T2g lattice modes modulate the electronic structure of [SbCl6]3− by splitting the doubly degenerate E levels of 3 T$^{*}_{1u}$ into non-degenerate states. The physical model, supported by theoretical studies, explains the energy level splitting required to realize two kinds of radiative minima in the relaxed excited state.

36 MATERIALS SCIENCE↗
NASA NTRS2003

Non-Thermal Hard X-Ray Emission in Galaxy Clusters Observed with the BeppoSAX PDS

We study the X-ray emission in a Sample of galaxy clusters using the BeppoSAX PDS instrument in the 20 - 80 keV energy band. We estimate the non-thermal hard X-ray cluster emission (HXR) by modeling the thermal contribution from the cluster gas and the non-thermal contamination from the unobscured AGN in the clusters. We also evaluate the systematic uncertainties due to the background fluctuations. Assuming negligible contamination from the obscured AGN, the resulting non-thermal component is detected at a 2 sigma level in approx. 50% of the non-significantly AGN-contaminated clusters: A2142, A2199, A2256, A3376, Coma, Ophiuchus and Virgo. The data are consistent with a scenario whereby relaxed clusters have no hard X-ray component of non-thermal origin, whereas merger clusters do. The co-added spectrum of the above clusters indicates a power-law spectrum for the HXR with a photon index of 2.8+0.3-0.4 in the 12 - 115 keV band, and we find indication that it has extended distribution. These indications argue against significant contamination from obscured AGN, which have harder spectra and centrally concentrated distribution. These results are supportive of the assumption of the merger shock acceleration of electrons in clusters, which has been proposed as a possible origin of the non-thermal hard X-ray emission models. Assuming that the Cosmic Microwave Background photons experience Inverse Compton scattering from the merger-accelerated relativistic electrons, and thus produce the observed HXR, the measured hard X-ray slope corresponds to a differential momentum spectra of the relativistic electrons with a slope of mu = 3.8 - 5.0. In presence of cluster magnetic fields this relativistic electron population produces synchrotron emission with a spectral index of 1.4 - 2.1, consistent with radio halo observations of merger clusters. Thus both hard X-ray and radio observations of merger clusters are consistent with the Inverse Compton model. The observed slope of HXR is also consistent with that predicted by the non-thermal bremsstrahlung, which chus cannot be ruled by the fit to the current data, even though this model requires an extreme, untenable cluster energetics. Assuming centrally concentrated distribution of HXR, the data requires a harder slope for the HXR spectrum, which is consistent with secondary electron models, but this model yields a worse fit to the PDS data and thus seems to be disfavored over the primary electron Inverse Compton model.

Nevalainen, J.↗