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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

How additives for tin halide perovskites influence the Sn 4+ concentration

Tin halide perovskite (Sn-HPs) photovoltaics could potentially equal or exceed the performance of their more toxic Pb-based analogues if defect state densities, particularly originating from the presence of Sn 4+ , can be significantly decreased. Numerous additives are incorporated into Sn-HPs to minimize the amount of Sn 4+ , including SnF 2 , reducing agents such as hydrazine derivatives, and various antioxidants. However, despite the frequent use of additives to reduce Sn 4+ content, there is limited understanding of how they function and consequently limited guidance for the development of new additives. Herein, we use cyclic voltammetry to probe the redox behavior of SnI 2 , SnI 4 , Sn-HP precursor solutions, and 18 different additives. Through 119 Sn NMR measurements we show that hydrochloride containing additives undergo halide exchange with SnI 4 to form SnI x Cl y , which results in decreased Sn 4+ concentrations and less p-type character in the Sn-HP films. We find that the most effective additive at lowering the Sn 4+ content in FASnI 3 is not capable of reducing SnI 4 or forming SnI x Cl y , but rather it acts as a sacrificial and coordinating antioxidant. In general, when selecting additives for Sn-HPs it is important to account for the redox potential, coordination with Sn species, ability to react with oxygen, and the potential for halide exchange.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Excited State Orbital Optimization via Minimizing the Square of the Gradient: General Approach and Application to Singly and Doubly Excited States via Density Functional Theory

We present a general approach to converge excited state solutions to any quantum chemistry orbital optimization process, without the risk of variational collapse. The resulting square gradient minimization (SGM) approach only requires analytic energy/Lagrangian orbital gradients and merely costs 3 times as much as ground state orbital optimization (per iteration), when implemented via a finite difference approach. SGM is applied to both single determinant ΔSCF and spin-purified restricted open-shell Kohn-Sham (ROKS) approaches to study the accuracy of orbital optimized DFT excited states. It is found that SGM can converge challenging states where the maximum overlap method (MOM) or analogues either collapse to the ground state or fail to converge. We also report that ΔSCF/ROKS predict highly accurate excitation energies for doubly excited states (which are inaccessible via TDDFT). Singly excited states obtained via ROKS are also found to be quite accurate, especially for Rydberg states that frustrate (semi)local TDDFT. Our results suggest that orbital optimized excited state DFT methods can be used to push past the limitations of TDDFT to doubly excited, charge-transfer, or Rydberg states, making them a useful tool for the practical quantum chemist's toolbox for studying excited states in large systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Hot droughts in the Amazon provide a window to a future hypertropical climate

Tropical forests represent the warmest and wettest of Earth’s biomes, but with continued anthropogenic warming, they will be pushed to climate states with no current analogue. Droughts in the tropics are already becoming more intense as they occur at successively higher temperatures. Here, in this study, we synthesize multiple datasets to assess the effects of hot droughts on a central Amazon forest. First, a more than 30-year record of annually resolved forest demographic data from a selective logging experiment showed higher tree mortality during intense droughts, particularly among fast-growing pioneer species with low wood density. Second, analysis of ecophysiological field measurements from the 2015 and 2023 El Niño droughts identified a soil moisture threshold beyond which transpiration rates rapidly declined. As rainless days beyond this threshold continued, drought conditions intensified, increasing the potential for tree mortality from hydraulic failure and carbon starvation. Third, analyses from the Coupled Model Intercomparison Project Phase 6 demonstrated that under high-emission scenarios, a large area of tropical forest will shift to a hotter ‘hypertropical’ climate by 2100. Last, under a hypertropical climate, temperature and moisture conditions during typical dry season months will more frequently exceed identified drought mortality thresholds, elevating the risk of forest dieback. Present-day hot droughts are harbingers of this emerging climate, offering a window for studying tropical forests under expected extreme future conditions.

drought↗
DOE OSTI2022

Harnessing Intermolecular Interactions to Promote Long-Lived Photoinduced Charge Separation from Copper Phenanthroline Chromophores

In this study, facilitating photoinduced electron transfer (PET) while minimizing rapid charge-recombination processes to produce a long-lived charge-separated (CS) state represents a primary challenge associated with achieving efficient solar fuel production. Natural photosynthetic systems employ intermolecular interactions to arrange the electron-transfer relay in reaction centers and promote a directional flow of electrons. This work explores a similar tactic through the synthesis and ground- and excited-state characterization of two Cu(I)bis(phenanthroline) chromophores with homoleptic and heteroleptic coordination geometries and which are functionalized with negatively charged sulfonate groups. The addition of sulfonate groups enables solubility in pure water, and it also induces assembly with the dicationic electron acceptor methyl viologen (MV 2+ ) via bimolecular, dynamic electrostatic interactions. The effect of the sulfonate groups on the ground- and excited-state properties was evaluated by comparison with the unsulfonated analogues in 1:1 acetonitrile/water. The excited-state lifetimes for all sulfonated complexes are similar to what we expect from previous literature, with the exception of the sulfonated heteroleptic complex whose metal-to-ligand charge-transfer (MLCT) lifetime in water has two components that are fit to 10 and 77 ns. For the sulfonated complexes, we detected reduced MV +$\bullet$ in both solvent environments following MLCT excitation, but control measurements in 1:1 acetonitrile/water with the unsulfonated analogues showed no PET to MV 2+ , indicating that electrostatically driven supramolecular assemblies of the sulfonated complexes with MV 2+ facilitate the observed PET. Additionally, the strength of the intermolecular interactions driving the formation of these assemblies changes drastically with the solvent environment. In 1:1 acetonitrile/water, PET occurred from both sulfonated complexes with quantum yields (Φ ET ) of 2-3% but increased to a remarkable 98% for the sulfonated heteroleptic complex with a 3 μs CS-state lifetime in water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Fractional Chern insulators in magic-angle twisted bilayer graphene

Fractional Chern insulators (FCIs) are lattice analogues of fractional quantum Hall states that may provide a new avenue towards manipulating non-Abelian excitations. Early theoretical studies have predicted their existence in systems with flat Chern bands and highlighted the critical role of a particular quantum geometry. However, FCI states have been observed only in Bernal-stacked bilayer graphene (BLG) aligned with hexagonal boron nitride (hBN), in which a very large magnetic field is responsible for the existence of the Chern bands, precluding the realization of FCIs at zero field. By contrast, magic-angle twisted BLG supports flat Chern bands at zero magnetic field and therefore offers a promising route towards stabilizing zero-field FCIs. Here we report the observation of eight FCI states at low magnetic field in magic-angle twisted BLG enabled by high-resolution local compressibility measurements. The first of these states emerge at 5 T, and their appearance is accompanied by the simultaneous disappearance of nearby topologically trivial charge density wave states. We demonstrate that, unlike the case of the BLG/hBN platform, the principal role of the weak magnetic field is merely to redistribute the Berry curvature of the native Chern bands and thereby realize a quantum geometry favourable for the emergence of FCIs. Our findings strongly suggest that FCIs may be realized at zero magnetic field and pave the way for the exploration and manipulation of anyonic excitations in flat moiré Chern bands.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Controlling Tautomerization in Pyridine-Fused Phosphorus-Nitrogen Heterocycles

Inclusion of a second nitrogen atom in the aromatic core of phosphorus-nitrogen (PN) heterocycles results in unexpected tautomerization to a nonaromatic form. This tautomerization, initially observed in the solid state through X-ray crystallography, is also explained by computational analysis. We prepared an electron deficient analogue (2 e) with a fluorine on the pyridine ring and showed that the weakly basic pyridine resisted tautomerization, providing key insights to why the transformation occurs. To study the difference in solution vs. solid-state heterocycles, alkylated analogues that lock in the quinoidal tautomer were synthesized and their different 1 H NMR and UV/Vis spectra studied. Ultimately, we determined that all heterocycles are the aromatic tautomer in solution and all but 2 e switch to the quinoidal tautomer in the solid state. Better understanding of this transformation and under what circumstances it occurs suggest future use in a switchable on/off hydrogen-bond-directed receptor that can be tuned for complementary hydrogen bonding.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Stoichiometric Lanthanide Compounds with Diglycolamides: A Synthetic Approach toward Understanding Rare-Earth Speciation in Solution

A fundamental understanding of coordination chemistry across the lanthanide series is essential for explaining the chemical behavior of rare-earth metals in complex liquid–liquid extraction processes. Probing the exact bonding between the extractant and the metal is sometimes done through the synthesis of solid-state compounds that can serve as models for metal speciation in solution. In the case of diglycolamide (DGA), a commonly used neutral diamide extractant, extensive studies identify the stepwise formation of 1:1 [Ln(DGA)(H 2 O) 6 ] 3+ , 1:2 [Ln(DGA) 2 (H 2 O) 3 ] 3+ , and 1:3 [Ln(DGA) 3 ] 3+ complexes in solution. The crystallographic reports, however, exclusively show a 1:3 [Ln(DGA) 3 ] 3+ moiety in the solid state, while the structures of 1:1 and 1:2 complexes are yet to be isolated and comprehensively studied. In this work, we report the synthesis and characterization of three new families of stoichiometric N,N,N′,N’ -tetramethyldiglycolamide (TMDGA) compounds: [Ln(TMDGA)(H 2 O) 5 Cl]Cl 2 ·2H 2 O, [Ln(TMDGA) 2 (H 2 O) 3 ]Cl 3 ·3H 2 O, and [Ln(TMDGA) 3 ]Cl 3 ·7H 2 O, where Ln = Nd, Eu, Gd, with Ln:TMDGA ratios of 1:1, 1:2, and 1:3, respectively. Further, the compounds have been analyzed using vibrational spectroscopy (both Raman and FT-IR), as well as variable temperature fluorescence spectroscopy. A spectrophotometric titration of Eu(III) was performed to confirm the presence of the [Eu(TMDGA) n ] 3+ ( n = 1, 2, and 3) species in solution and to compare the individual solid-state emission spectra to their respective analogues in solution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Wabash CarbonSAFE (Subtask 3.1 - Application of the NRAP Tools to the Wabash CarbonSAFE Site for Risk Assessment Associated with Geologic Carbon Storage Activities)

This report documents a risk assessment of CO 2 containment loss and induced shear failure due to geologic carbon storage at the Wabash CarbonSAFE site. The operator, Wabash Valley Resources, has proposed adapting the onsite integrated gasification combined cycle (IGCC) facilities to produce hydrogen and injecting the byproduct CO 2 stream into the subsurface Potosi dolomite formation. The purpose of this study is to assess (1) CO 2 sequestration performance relative to the CarbonSAFE goals of storing 50 Mt over 30 years, (2) the risk of containment loss due to leakage along a wellbore and into an overlying aquifer, and (3) the state of stress and risk of reactivating existing fractures. This study relied upon the initial site characterization work performed by the Illinois State Geologic Survey (ISGS) along with analogue data collected from other carbon sequestration projects in the region.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2023

Sterically Encumbered Heteroleptic Copper(I) β-Diketiminate Complexes with Extended Excited-State Lifetimes

One of the main challenges in developing effective copper(I) photosensitizers is their short excited-state lifetimes, usually attributed to structural distortion upon light excitation. We have previously introduced copper(I) charge-transfer chromophores of the general formula Cu(N^N)(ArNacNac), where N^N is a conjugated diimine ligand and ArNacNac is a substituted β-diketiminate ligand. These chromophores were promising regarding their tunable redox potentials and intense visible absorption but were ineffective as photosensitizers, presumably due to short excited-state lifetimes. Here, we introduce sterically crowded analogues of these heteroleptic chromophores with bulky alkyl substituents on the N^N and/or ArNacNac ligand. Structural analysis was combined with electrochemical and photophysical characterization, including ultrafast transient absorption (UFTA) spectroscopy to investigate the effects of the alkyl groups on the excited-state lifetimes of the complexes. The molecular structures determined by single-crystal X-ray diffraction display more distortion in the ground state as alkyl substituents are introduced into the phenanthroline or the NacNac ligand, showing smaller τ 4 values due to the steric hindrance. UFTA measurements were carried out to determine the excited-state dynamics. Sterically encumbered Cu5 and Cu6 display excited-state lifetimes 15–20 times longer than unsubstituted complex Cu1, likely indicating that the incorporation of bulky alkyl substituents inhibits the pseudo-Jahn–Teller (PJT) flattening distortion in the excited state. Furthermore, this work suggests that the steric properties of these heteroleptic copper(I) charge-transfer chromophores can be readily modified and that the excited-state dynamics are strongly responsive to these modifications.

14 SOLAR ENERGY↗
DOE OSTI2026

Tetrel Bond-Mediated Photophysical Modulation and Fluoride Recognition in Carbazole-Organosilanes

Silicon-centered orbitals are typically regarded as electronically inert in donor–acceptor systems. Here, we show that silole-based carbazole–silane architectures can render these orbitals electronically relevant, enabling modulation of excited-state behavior and anion-responsive photophysics. Two carbazole–Dipp–silanes exhibit identical carbazole-localized LE singlet emission in solution yet diverge markedly in the solid state: one compound displays a broad long-wavelength emission band in the prompt spectrum and enhanced long-lived emission consistent with a triplet-derived excited state, likely arising from a combination of intramolecular structural locking and solid-state packing effects, whereas the more flexible analogue remains predominantly LE-emissive. Fluoride coordination further differentiates the two systems, producing ratiometric red-shifted emission in one case and fluorescence quenching in the other through a fully reversible coordination process. These results identify σ*(Si–Ar) orbitals as tunable contributors to excited-state landscapes in organosilane luminophores and suggest a broader design strategy for controlling excited-state behavior in tetrel-based photofunctional systems.

Haque, Md Hasanul↗
DOE OSTI2021

Spectroscopy of the T = 2 mirror nuclei 48 Fe/ 48 Ti using mirrored knockout reactions

A sequence of excited states has been established for the first time in the proton-rich nucleus 48 Fe (Z=26, N=22). The technique of mirrored (i.e. analogue) one-nucleon knockout reactions was applied, in which the T z = ±2 mirror pair, 48 Fe/ 48 Ti were populated via one-neutron/one-proton knockout from the secondary beams 49 Fe/ 49 V, respectively. The analogue properties of the reactions were used to help establish the new level scheme of 48 Fe. The inclusive and exclusive cross sections were determined for the populated states. Large differences between the cross sections for the two mirrored reactions were observed and have been interpreted in terms of different degrees of binding of the mirror nuclei and in the context of the recent observations of suppression of spectroscopic strength as a function of nuclear binding, for knockout reactions on light solid targets. Mirror energy differences (MED) have been determined between the analogue T = 2 states and compared with the shell model predictions. MED for this mirror pair, due to their location in the shell, are especially sensitive to excitations out of the f 7/2 shell, and present a stringent test of the shell-model prescription.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Quantum spin nematic phase in a square-lattice iridate

Spin nematic is a magnetic analogue of classical liquid crystals, a fourth state of matter exhibiting characteristics of both liquid and solid. Particularly intriguing is a valence-bond spin nematic, in which spins are quantum entangled to form a multipolar order without breaking time-reversal symmetry, but its unambiguous experimental realization remains elusive. Here, in this study, we establish a spin nematic phase in the square-lattice iridate Sr 2 IrO 4 , which approximately realizes a pseudospin one-half Heisenberg antiferromagnet in the strong spin-orbit coupling limit. Upon cooling, the transition into the spin nematic phase at T C approximate to 263 K is marked by a divergence in the static spin quadrupole susceptibility extracted from our Raman spectra and concomitant emergence of a collective mode associated with the spontaneous breaking of rotational symmetries. The quadrupolar order persists in the antiferromagnetic phase below TN approximate to 230 K and becomes directly observable through its interference with the antiferromagnetic order in resonant X-ray diffraction, which allows us to uniquely determine its spatial structure. Further, we find using resonant inelastic X-ray scattering a complete breakdown of coherent magnon excitations at short-wavelength scales, suggesting a many-body quantum entanglement in the antiferromagnetic state. Taken together, our results reveal a quantum order underlying the Neel antiferromagnet that is widely believed to be intimately connected to the mechanism of high-temperature superconductivity. We establish a spin nematic phase in the square-lattice iridate Sr 2 IrO 4 and find a complete breakdown of coherent magnon excitations at short-wavelength scales, suggesting a many-body quantum entanglement in the antiferromagnetic state.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Frictional properties of Opalinus Clay: influence of humidity, normal stress and grain size on frictional stability

SUMMARY The Opalinus Clay (OPA) is a clay-rich formation considered as a potential host rock for radioactive waste repositories and as a caprock for carbon storage in Switzerland. Its very low permeability (10−19 to 10−21 m2) makes it a potential sealing horizon, however the presence of faults that may be activated during the lifetime of a repository project can compromise the long-term hydrological confinement, and lead to mechanical instability. Here, we have performed laboratory experiments to test the effect of relative humidity (RH), grain size (g.s.) and normal stress on rate-and-state frictional properties and stability of fault laboratory analogues corresponding to powders of OPA shaly facies. The sifted host rock powders at different grain size fractions (<63 μm and 63 < g.s. < 125 μm), at room (∼25 per cent) and 100 per cent humidity, were slid in double-direct shear configuration, under different normal stresses (5–70 MPa). We observe that peak friction, μpeak and steady-state friction, μss, depend on water vapour content and applied normal stress. Increasing relative humidity from ∼25 per cent RH (room humidity) to 100 per cent RH causes a decrease of frictional coefficient from 0.41 to 0.35. The analysis of velocity-steps in the light of rate-and-state friction framework shows that the stability parameter (a–b) is always positive (velocity-strengthening), and it increases with increasing sliding velocity and humidity. The dependence of (a–b) on slip rate is lost as normal stress increases, for each humidity condition. By monitoring the variations of the layer thickness during the velocity steps, we observe that dilation (Δh) is directly proportional to the sliding velocity, decreases with normal stress and is unaffected by humidity. Microstructural analysis shows that most of the deformation is accommodated within B-shear zones, and the increase of normal stress (σn) promotes the transition from strain localization and grain size reduction to distributed deformation on a well-developed phyllosilicate network. These results suggest that: (1) the progressive loss of velocity dependence of frictional stability parameter (a–b) at σn > 35 MPa is dictated by a transition from localized to distributed deformation and (2) water vapour content does not affect the deformation mechanisms and dilation, whereas it decreases steady-state friction (μss), and enhances fault stability.

58 GEOSCIENCES↗
DOE OSTI2020

Experimental Investigation of Hydraulic Fracturing and Stress Sensitivity of Fracture Permeability Under Changing Polyaxial Stress Conditions

Understanding and predicting fracture propagation and subsequent fluid flow characteristics is critical to geoenergy technologies that engineer and/or utilize favorable geological conditions to store or extract fluids from the subsurface. Fracture permeability decreases nonlinearly with increasing normal stress, but the relationship between shear displacement and fracture permeability is less well understood. We utilize the new Geo–Reservoir Experimental Analogue Technology (GREAT cell), which can apply polyaxial stress states and realistic reservoir temperatures and pressures to cylindrical samples and has the unique capability to alter both the magnitude and orientation of the radial stress field by increments of 11.25° during an experiment. We load synthetic analogue materials and real rock samples to stress conditions representative of 500–1,000 m depth, investigate the hydraulic stimulation process, and then conduct flow experiments while changing the fluid pressure and the orientation of the intermediate and minimum principal stresses. High–resolution circumferential strain measurements combined with fluid pressure data indicate fracture propagation can be both stable (no fluid pressure drop) and unstable (fluid pressure drop). The induced fractures exhibit both opening and shear displacements during their creation and/or during fluid flow with changing radial stress states. Flow tests during radial stress field rotation reveal that fracture normal effective stress has first–order control on fracture permeability but increasing fracture offset can lead to elevated permeabilities at maximum shear stress. Here, the results have implications for our conceptual understanding of fracture propagation as well as fluid flow and deformation around fractures.

58 GEOSCIENCES↗
DOE OSTI2021

Observation and control of the weak topological insulator state in ZrTe5

Abstract A quantum spin Hall (QSH) insulator hosts topological states at the one-dimensional (1D) edge, along which backscattering by nonmagnetic impurities is strictly prohibited. Its 3D analogue, a weak topological insulator (WTI), possesses similar quasi-1D topological states confined at side surfaces. The enhanced confinement could provide a route for dissipationless current and better advantages for applications relative to strong topological insulators (STIs). However, the topological side surface is usually not cleavable and is thus hard to observe. Here, we visualize the topological states of the WTI candidate ZrTe 5 by spin and angle-resolved photoemission spectroscopy (ARPES): a quasi-1D band with spin-momentum locking was revealed on the side surface. We further demonstrate that the bulk band gap is controlled by external strain, realizing a more stable WTI state or an ideal Dirac semimetal (DS) state. The highly directional spin-current and the tunable band gap in ZrTe 5 will provide an excellent platform for applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Investigation of a bacteriochlorin-containing pentad array for panchromatic light-harvesting and charge separation

A new pentad array designed to exhibit panchromatic absorption and charge separation has been synthesized and characterized. The array is composed of a triad panchromatic absorber (a bis(perylene-monoimide)-porphyrin) to which are appended an electron acceptor (perylene-diimide) and an electron donor/hole acceptor (bacteriochlorin) in a crossbar arrangement. The motivation for incorporation of the bacteriochlorin versus a free-base or zinc chlorin utilized in prior constructs was to facilitate hole transfer to this terminal unit and thereby achieve a higher yield of charge separation across the array. The intense S 0 → S 1 (Q y ) band of the bacteriochlorin also enhances absorption in the near-infrared spectral region. Due to synthetic constraints, a phenylethyne linker was used to join the bacteriochlorin to the core porphyrin of the panchromatic triad rather than the diphenylethyne linker employed for the prior chlorin-containing pentads. Static and time-resolved photophysical studies reveal enhanced excited-state quenching for the pentad in benzonitrile and dimethyl sulfoxide compared to the prior chlorin-containing analogues. Success was only partial, however, as a long-lived charge separated state was not observed despite the improved energetics for the final ground-state hole/electron-shift reaction. The apparent reason is more facile competing charge-recombination due to the shorter bacteriochlorin – porphyrin linker that increases electronic coupling for this process. Furthermore, the studies highlight design criteria for balancing panchromatic absorption and long-lived charge separation in molecular architectures for solar-energy conversion.

14 SOLAR ENERGY↗
DOE OSTI2025

Thermalization and criticality on an analogue–digital quantum simulator

Abstract Understanding how interacting particles approach thermal equilibrium is a major challenge of quantum simulators 1,2 . Unlocking the full potential of such systems towards this goal requires flexible initial state preparation, precise time evolution and extensive probes for final state characterization. Here we present a quantum simulator comprising 69 superconducting qubits that supports both universal quantum gates and high-fidelity analogue evolution, with performance beyond the reach of classical simulation in cross-entropy benchmarking experiments. This hybrid platform features more versatile measurement capabilities compared with analogue-only simulators, which we leverage here to reveal a coarsening-induced breakdown of Kibble–Zurek scaling predictions 3 in theXYmodel, as well as signatures of the classical Kosterlitz–Thouless phase transition 4 . Moreover, the digital gates enable precise energy control, allowing us to study the effects of the eigenstate thermalization hypothesis 5–7 in targeted parts of the eigenspectrum. We also demonstrate digital preparation of pairwise-entangled dimer states, and image the transport of energy and vorticity during subsequent thermalization in analogue evolution. These results establish the efficacy of superconducting analogue–digital quantum processors for preparing states across many-body spectra and unveiling their thermalization dynamics.

Science & Technology - Other Topics↗