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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

BiCuI 4 (Pyridine) 5 a neutral ligand-supported compound of BiI 3 and CuI

Reaction of equimolar pyridine (Py) solutions BiI 3 and CuI produces the Py-supported 1:1 bimetallic complex BiCuI 4 (Py) 5 in quantitative yield. The title complex is only the second neutral complex to feature Cu–I–Bi bridging and shows an octahedral trans-[BiI 4 (Py) 2 ] unit joined to a distorted tetrahedral CuI(Py) 3 unit by an iodide bridge. The complex shows low thermal stability, decomposing under modest heating or vacuum to produce a mixture of BiI 3 and CuI. Thus, it is a potential entry/precursor to BiI 3 /CuI chemistry. Natural Localized Molecular Orbital (NLMO) calculations were performed to analyze the nature of the Cu–I–Bi bonds, revealing that the title compound lies on the cusp of being [Cu(Py) 3 ] + [BiI 4 (Py) 2 ] – . Diffuse reflectance spectroscopy measurements show a strong absorption band with an optical bandgap energy of 1.94 eV. Theoretical density of states (DOS) and time-dependent density functional theory (TD-DFT) experiments to map the electronic structure assign the primary electronic transition as a mixed halide/metal-to-ligand charge transfer between Cu–I–Bi donor orbitals and Py π* acceptor orbitals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Materials Data on BiI by Materials Project

BiI crystallizes in the monoclinic C2/m space group. The structure is one-dimensional and consists of eight BiI ribbons oriented in the (0, 1, 0) direction. there are two inequivalent Bi1+ sites. In the first Bi1+ site, Bi1+ is bonded in a rectangular see-saw-like geometry to four I1- atoms. There are two shorter (3.13 Å) and two longer (3.15 Å) Bi–I bond lengths. In the second Bi1+ site, Bi1+ is bonded in a single-bond geometry to one I1- atom. The Bi–I bond length is 3.82 Å. There are two inequivalent I1- sites. In the first I1- site, I1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms. In the second I1- site, I1- is bonded in a distorted L-shaped geometry to three Bi1+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on BiI by Materials Project

BiI crystallizes in the monoclinic C2/m space group. The structure is one-dimensional and consists of four BiI ribbons oriented in the (0, 1, 0) direction. there are two inequivalent Bi1+ sites. In the first Bi1+ site, Bi1+ is bonded in a distorted single-bond geometry to one I1- atom. The Bi–I bond length is 3.87 Å. In the second Bi1+ site, Bi1+ is bonded in a rectangular see-saw-like geometry to four I1- atoms. There are two shorter (3.13 Å) and two longer (3.15 Å) Bi–I bond lengths. There are two inequivalent I1- sites. In the first I1- site, I1- is bonded in an L-shaped geometry to three Bi1+ atoms. In the second I1- site, I1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ternary Complexes of BiI 3 /CuI and SbI 3 /CuI with Tetrahydrothiophene

Reactions of BiI 3 /CuI mixtures with tetrahydrothiophene (THT) in toluene produce 2-D sheet networks BiCu 3 I 6 (THT) n (n = 2, 3, or 4), depending on reaction conditions. All three structures are based on BiI 6 octahedra, which share pairs of (μ 2 -I) 2 with Cu 3 (THT) n units. BiCu 3 I 6 (THT) 2 features Cu 2 (μ 2 -I) 2 rhombs with close Cu···Cu interactions and is accompanied by formation of the very complex HBi 3 Cu 12 I 22 (THT) 8 . Reactions of SbI 3 /CuI with THT in toluene produced a SbCu 3 I 6 (THT) 2 network shows Cu 3 (μ 2 -THT) 2 units, like its Bi congener, but Cu 6 (μ 2 -I) 6 barrels rather than rhombs. Isolated SbI 3 units are stacked above the Cu 6 I 6 barrels. A molecular compound, Sb 3 Cu 3 I 12 (THT) 6 consists of a face-sharing Sb 3 I 12 stack, in which the Cu-THT units are bonded in asymmetric fashion about the central SbI 6 . Metal-halide bonds were investigated via QTAIM and NLMO analyses, demonstrating that these bonds are largely ionic and occur between the Bi/Sb and I p orbitals. Hirshfeld analysis shows significant H···H and H···I interactions. Diffuse reflectance spectroscopy (DRS) reveals band edges for the Bi species of 1.71–1.82 eV, while those for the neutral Sb complexes are in the range of 1.94–2.06 eV. Mapping of the electronic structure via density of state calculations indicates population of antibonding Bi/Sb–I orbitals in the excited state.

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

Viruses infecting a warm water picoeukaryote shed light on spatial co-occurrence dynamics of marine viruses and their hosts

The marine picoeukaryote Bathycoccus prasinos has been considered a cosmopolitan alga, although recent studies indicate two ecotypes exist, Clade BI (B. prasinos) and Clade BII. Viruses that infect Bathycoccus Clade BI are known (BpVs), but not that infect BII. We isolated three dsDNA prasinoviruses from the Sargasso Sea against Clade BII isolate RCC716. The BII-Vs do not infect BI, and two (BII-V2 and BII-V3) have larger genomes (~210 kb) than BI-Viruses and BII-V1. BII-Vs share ~90% of their proteins, and between 65% to 83% of their proteins with sequenced BpVs. Phylogenomic reconstructions and PolB analyses establish close-relatedness of BII-V2 and BII-V3, yet BII-V2 has 10-fold higher infectivity and induces greater mortality on host isolate RCC716. BII-V1 is more distant, has a shorter latent period, and infects both available BII isolates, RCC716 and RCC715, while BII-V2 and BII-V3 do not exhibit productive infection of the latter in our experiments. Global metagenome analyses show Clade BI and BII algal relative abundances correlate positively with their respective viruses. The distributions delineate BI/BpVs as occupying lower temperature mesotrophic and coastal systems, whereas BII/BII-Vs occupy warmer temperature, higher salinity ecosystems. Accordingly, with molecular diagnostic support, we name Clade BII Bathycoccus calidus sp. nov. and propose that molecular diversity within this new species likely connects to the differentiated host-virus dynamics observed in our time course experiments. Overall, the tightly linked biogeography of Bathycoccus host and virus clades observed herein supports species-level host specificity, with strain-level variations in infection parameters.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2026

Pyridine Complexes of Iodobismuthate(III) Anions

We report a rare family of pyridine-coordinated iodobismuthate(III) salts supported by alkyltriphenylphosphonium and tetraphenylphosphonium cations. Reactions of BiI 3 with Ph 3 PR + I − (R = Me, Et, n Pr, n Bu, Ph) in neat pyridine, followed by crystallization, yield structurally tunable bismuth-halide-pyridine anions dictated by reagent stoichiometry. Combination of BiI 3 and Ph 3 PR + I − in 2:1 ratio produced [Ph 3 PR] 2 [BiI 5 Py], 1 (R = Me, Et, n Pr, Ph), while combination in 1:1 ratio resulted in three compounds: [Ph 3 PR][cis-BiI 4 Py 2 ], 2 (R = n Pr, Ph), [Ph 3 PR][trans-BiI 4 Py 2 ], 3 (R = Me, Et, Ph), and [Ph 3 PR] 2 [transoid-Bi 2 I 8 Py 2 ], 4 (R = Me, Et, n Pr, n Bu, Ph). In many cases, the compounds were isolated as Py or Et 2 O solvates, and in some cases, multiple degrees of solvation or polymorphism were encountered. Hirshfeld analysis of 1–4 showed the major anion–cation/anion/solvent interactions to be H⋯I, H⋯H, and C⋯H. Diffuse reflectance measurements of representative compounds, all of which were yellow-orange to red-orange, revealed bandgaps in the range of 1.9–2.2 eV, where density-of-states KS-DFT calculations attribute the absorption to metal-centered charge transfer within the anionic unit. NLMO and QTAIM analyses further indicate predominantly ionic Bi(III)–I/pyridine bonding with robust inner-sphere coordination that is insensitive to anion speciation.

Bismuth Compounds↗
DOE OSTI2024

Pelletization with Spark Plasma Sintering and Characterization of Metal Iodides: An Assessment of Long-Term Radioiodine Immobilization Options

Four promising iodine “getter” materials (Ag, Cu, Bi, and Sn) for radioiodine capture were assessed in their pure metal-iodide (MI x ) pelletized forms to compare relative chemical durabilities. To study chemical durability, commercial MI x compounds of AgI, BiI 3 , BiOI, CuI, and SnI 4 were converted to dense monolithic pellets using spark plasma sintering. Semidynamic leach testing in the form of modified ASTM C1308 tests was then performed on the pellets in two different forms including unmounted (as-pressed) specimens (i.e., “U”) and epoxy-mounted specimens (i.e., “M”) with polished surfaces. The chemical durability results and sample characterizations showed that three of the five MI x compounds tested (i.e., AgI, CuI, and BiOI) displayed moderate to high leach resistances. Further, the remaining two MI x compounds (i.e., BiI 3 and SnI 4 ), which are both desirable iodine waste forms due to their high iodine loading capacities, readily decomposed during leach testing, indicated by crystallographic changes in the specimens as well as large amounts of iodine detected in the leachate solutions. The instabilities of BiI 3 and SnI 4 raise uncertainties for using the base metals/cations (i.e., Bi 0 /Bi 3+ and Sn 0 /Sn 4+ , respectively) as viable getters for radioiodine capture due to likely poor waste form chemical durabilities after capture and consolidation into waste forms.

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

Conformational flexibility is a critical factor in designing broad-spectrum human norovirus protease inhibitors

Human norovirus (HuNoV) is a leading cause of gastroenteritis worldwide and is associated with significant morbidity, mortality, and economic impact. There are currently no licensed antiviral drugs for the treatment of HuNoV-associated gastroenteritis. The HuNoV protease plays a critical role in the initiation of virus replication by cleaving the polyprotein. Thus, it is an ideal target for developing antiviral small-molecule inhibitors. While rupintrivir, a potent small-molecule inhibitor of several picornavirus proteases, effectively inhibits GI.1 protease, it is an order of magnitude less effective against GII protease. Other GI.1 protease inhibitors also tend to be less effective against GII proteases. To understand the structural basis for the potency difference, we determined the crystal structures of proteases of GI.1, pandemic GII.4 (Houston and Sydney), and GII.3 in complex with rupintrivir. These structures show that the open substrate pocket in GI protease binds rupintrivir without requiring significant conformational changes, whereas, in GII proteases, the closed pocket flexibly extends, reorienting arginine-112 in the BII-CII loop to accommodate rupintrivir. Structures of R112A protease mutants with rupintrivir, coupled with enzymatic and inhibition studies, suggest R112 is involved in displacing both substrate and ligands from the active site, implying a role in the release of cleaved products during polyprotein processing. Thus, the primary determinant for differential inhibitor potency between the GI and GII proteases is the increased flexibility in the BII-CII loop of the GII proteases caused by the H-G mutation in this loop. Therefore, the inherent flexibility of the BII-CII loop in GII proteases is a critical factor to consider when developing broad-spectrum inhibitors for HuNoV proteases.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Materials Data on BaBi4(IO2)2 by Materials Project

BaOBi2O3(BiI)2 crystallizes in the tetragonal I4/mmm space group. The structure is two-dimensional and consists of two BaOBi2O3 sheets oriented in the (0, 0, 1) direction and four BiI sheets oriented in the (0, 0, 1) direction. In each BaOBi2O3 sheet, Ba2+ is bonded in a body-centered cubic geometry to eight equivalent O2- atoms. All Ba–O bond lengths are 2.76 Å. Bi2+ is bonded to four equivalent O2- atoms to form distorted corner-sharing BiO4 trigonal pyramids. All Bi–O bond lengths are 2.24 Å. O2- is bonded to two equivalent Ba2+ and two equivalent Bi2+ atoms to form a mixture of distorted corner and edge-sharing OBa2Bi2 tetrahedra. In each BiI sheet, Bi2+ is bonded in a 4-coordinate geometry to four equivalent I1- atoms. All Bi–I bond lengths are 3.51 Å. I1- is bonded in a 4-coordinate geometry to four equivalent Bi2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Bi2IBr by Materials Project

(Bi)2(BiI)2BiBr2BiIBr crystallizes in the monoclinic C2/m space group. The structure is one-dimensional and consists of eight bismuth molecules; four BiBr2 ribbons oriented in the (0, 1, 0) direction; four BiI ribbons oriented in the (0, 1, 0) direction; and four BiIBr ribbons oriented in the (0, 1, 0) direction. In each BiBr2 ribbon, Bi1+ is bonded in a square co-planar geometry to four Br1- atoms. There are two shorter (2.95 Å) and two longer (2.96 Å) Bi–Br bond lengths. There are two inequivalent Br1- sites. In the first Br1- site, Br1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms. In the second Br1- site, Br1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms. In each BiI ribbon, there are two inequivalent Bi1+ sites. In the first Bi1+ site, Bi1+ is bonded in a square co-planar geometry to four I1- atoms. There are two shorter (3.13 Å) and two longer (3.14 Å) Bi–I bond lengths. In the second Bi1+ site, Bi1+ is bonded in a single-bond geometry to one I1- atom. The Bi–I bond length is 3.84 Å. There are two inequivalent I1- sites. In the first I1- site, I1- is bonded in an L-shaped geometry to three Bi1+ atoms. In the second I1- site, I1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms. In each BiIBr ribbon, Bi1+ is bonded in a rectangular see-saw-like geometry to two equivalent I1- and two equivalent Br1- atoms. Both Bi–I bond lengths are 3.12 Å. Both Bi–Br bond lengths are 2.97 Å. I1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms. Br1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Bi4I3Br by Materials Project

Bi(BiI)2BiIBr crystallizes in the orthorhombic Cmc2_1 space group. The structure is one-dimensional and consists of four bismuth molecules; four BiI ribbons oriented in the (1, 0, 0) direction; and four BiIBr ribbons oriented in the (1, 0, 0) direction. In each BiI ribbon, there are two inequivalent Bi1+ sites. In the first Bi1+ site, Bi1+ is bonded in a rectangular see-saw-like geometry to four I1- atoms. All Bi–I bond lengths are 3.13 Å. In the second Bi1+ site, Bi1+ is bonded in a distorted single-bond geometry to one I1- atom. The Bi–I bond length is 3.87 Å. There are two inequivalent I1- sites. In the first I1- site, I1- is bonded in an L-shaped geometry to three Bi1+ atoms. In the second I1- site, I1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms. In each BiIBr ribbon, Bi1+ is bonded in a rectangular see-saw-like geometry to two equivalent I1- and two equivalent Br1- atoms. Both Bi–I bond lengths are 3.13 Å. Both Bi–Br bond lengths are 2.96 Å. I1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms. Br1- is bonded in an L-shaped geometry to two equivalent Bi1+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Giant Apparent Optical Circular Dichroism in Thin Films of Bismuth-Based Hybrid Organic-Inorganic Metal Halide Semiconductor Through Preferred Orientation

Introducing chirality into organic/inorganic hybrid materials can impart chiroptical properties such as circular dichroism. The ability to tune chiroptical properties in self-assembled materials can have important implications for spintronic and optoelectronic applications. Here, a chiral organic cation, (R/S)-4-methoxy-a-methylbenzylammonium, is incorporated to synthesize the bismuth-based hybrid organic-inorganic metal halide semiconductor, (R/S-MeOMePMA)BiI4. Thin films of this Bi-based compound demonstrate large chiroptical responses, with circular dichroism anisotropy (gCD) values up to ˜0.1, close to the highest value observed in another chiral metal-halide semiconductor, (R-MBA2CuCl4). Detailed investigation reveals that this large gCD in (R/S-MeOMePMA)BiI4 is caused by the apparent CD effect. Careful selection of deposition conditions and the concomitant thin-film orientation enables the control of gCD, with maximum value observed when its thin film has a well-crystallized preferred (001) orientation parallel to the substrate. The results support a growing body of evidence that low symmetry plays an important role in achieving unusually large gCD in these chiral metal-halide materials and provides design rules for achieving large chiroptical response via morphology control.

chiroptic response↗
DOE OSTI2021

Line identification of boron and nitrogen emissions in EUV and VUV wavelength ranges in the impurity powder dropping experiments of LHD and its application to spectroscopic diagnostics

An impurity powder dropper was installed in the 21st campaign of the Large Helical Device experiment (Oct. 2019–Feb. 2020) under a collaboration between the National Institute for Fusion Science and the Princeton Plasma Physics Laboratory for the purposes of real-time wall conditioning and edge plasma control. In order to assess the effective injection of the impurity powders, spectroscopic diagnostics were applied to observe line emission from the injected impurity. Therefore, extreme-ultraviolet (EUV) and vacuum-ultraviolet (VUV) emission spectra were analyzed to summarize observable impurity lines with B and BN powder injection. Emission lines released from B and N ions were identified in the EUV wavelength range of 5–300 Å measured using two grazing incidence flat-field EUV spectrometers and in the VUV wavelength range of 300–2400 Å measured using three normal incidence 20 cm VUV spectrometers. BI–BV and NIII–NVII emission lines were identified in the discharges with the B and BN powder injection, respectively. Useful B and N emission lines which have large intensities and are isolated from other lines were successfully identified as follows: BI (1825.89, 1826.40) Å (blended), BII 1362.46 Å, BIII (677.00, 677.14, 677.16) Å (blended), BIV 60.31 Å, BV 48.59 Å, NIII (989.79, 991.51, 991.58) Å (blended), NIV 765.15 Å, NV (209.27, 209.31) Å (blended), NVI 1896.80 Å, and NVII 24.78 Å. Applications of the line identifications to the advanced spectroscopic diagnostics were demonstrated, such as the vertical profile measurements for the BV and NVII lines using a space-resolved EUV spectrometer and the ion temperature measurement for the BII line using a normal incidence 3 m VUV spectrometer.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Connectivity-Dependent Exciton–Phonon Coupling in Cesium Bismuth Halide Quantum Dots

Metal halide octahedra form the fundamental functional building blocks of metal halide perovskites, dictating their structures, optical properties, electronic structures, and dynamics. Here, in this study, we show that the connectivity of bismuth halide octahedra in Cs 3 Bi 2 Br 9 and Cs 3 Bi 2 I 9 quantum dots (QDs) changes with different halide elements. We use first-principles calculations to reveal the key role of the connectivity of bismuth halide octahedra on the wave function symmetry, Huang-Rhys factor, and exciton-phonon interaction strength. Following QD synthesis via a ligand-mediated transport method, the effect of connectivity is verified with transient absorption spectroscopy, where we contrast Cs 3 Bi 2 Br 9 and Cs 3 Bi 2 I 9 QD exciton dynamics. In photoexcited Cs 3 Bi 2 I 9 QDs, phonons related to the vibrational motions of face-sharing [BiI 6 ] 3- bioctahedra couple strongly to the electronic state and drive rapid carrier relaxation. Equivalent signals are not observed for photoexcited Cs 3 Bi 2 Br 9 QDs, implying a lack of phonon involvement in band-edge absorption and subsequent exciton relaxation. Our findings suggest that structural engineering can effectively tune the exciton-phonon coupling and therefore influence exciton relaxation and recombination in perovskite nanomaterials.

TDDFT↗
DOE OSTI2026

Ultrafast Carrier Self-Trapping Driven by Strong Exciton–Phonon Coupling in 2D MA 3 Bi 2 I 6 Cl 3 Perovskite

Two-dimensional (2D) hybrid bismuth halide perovskites have emerged as promising lead-free materials for optoelectronic applications due to their solution processability and tunable structures. Here, in this study, we investigate 2D layered hybrid perovskite MA 3 Bi 2 I 6 Cl 3 using temperature-dependent photoluminescence (PL) and femtosecond transient absorption spectroscopy. Our results reveal strong coupling between excitons and phonons, evidenced by giant Huang–Rhys factors, coherent phonon oscillations, and ultrafast carrier self-trapping into small-polaron and self-trapped exciton (STE) states. These processes appear as time-dependent ground-state bleach and photoinduced absorption features, highlighting the influence of the lattice in carrier dynamics. Wavelength- and time-resolved measurements reveal that PL emission is dominated by STEs, while free exciton emission is weak and short-lived. By comparing 2D MA 3 Bi 2 I 6 Cl 3 with 0D MA 3 Bi 2 I 9 , which contains molecularly isolated [BiI 6 ] 3− octahedra and 2D MA 3 Bi 2 Br 9 perovskites, we demonstrate how halide composition and structural dimensionality influence the balance between free exciton populations and carrier localization. These insights uncover the intrinsic kinetic landscape of photoexcited states in MA 3 Bi 2 I 6 Cl 3 . Overall, our study contributes to a mechanistic understanding of exciton–phonon interactions in lead-free 2D perovskites.

Pradeep, Kodimana Ramakrishnan [Northwestern Univ.↗
DOE OSTI2026

Magnetic order in the van der Waals magnet VCl 3

Here, we investigated the structural and magnetic properties of single-crystalline VCl 3 , a newly synthesized member of the vanadium trihalide family. High-quality single crystals were grown by the chemical vapor transport method, and their behavior was characterized using neutron diffraction and thermodynamic measurements. We show that VCl 3 crystallizes in the BiI 3 -type structure at room temperature and undergoes a structural phase transition at 𝑇 𝑆 = 103.7⁢(5)⁢K that lowers the lattice symmetry, followed by a zigzag antiferromagnetic order with a propagation vector 𝑘 = (0,0.5,1) below 𝑇 𝑁 = 21.8⁢(1)⁢K. Neutron diffraction experiments indicate that the ordered moments are canted by approximately 21° away from the 𝑐 axis toward the 𝑎 axis, yielding a total moment of approximately 1.09⁢(2) ⁢𝜇 B /V 3+ . Field-dependent magnetization along the 𝑐 axis exhibits a half magnetization plateau, indicative of a field-stabilized fractional state. These results establish VCl 3 as a new platform for exploring structural transitions, anisotropic magnetism, and field-induced phases in vanadium-based honeycomb magnets.

Kao, Zeyu [Fudan Univ., Shanghai (China)]↗
DOE OSTI2024

Lattice and magnetic structure in the van der Waals antiferromagnet VBr 3

Here, we report a comprehensive investigation of the lattice and magnetic structure in van der Waals antiferromagnet VBr 3 , characterized by a BiI 3 -type structure at room temperature. Neutron diffraction experiments were performed on both polycrystalline and single-crystalline VBr 3 samples, revealing clear magnetic Bragg peaks emerging below the Néel temperature of T N =26.5 K. These magnetic Bragg peaks can be indexed by k=(0, 0.5, 1) in hexagonal notation. Our refinement analysis suggests that the antiferromagnetic order in VBr 3 manifests as a zigzag structure. Moreover, we observed peak splitting for nuclear Bragg peaks in the HK plane below the structure transition temperature of T S =90.4 K, indicating the breaking of threefold symmetry within the ab plane.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗