SIMES Publications

Abstract

Abstract

Inactive components and safety hazards are two critical challenges in realizing high-energy lithium-ion batteries. Metal foil current collectors with high density are typically an integrated part of lithium-ion batteries yet deliver no capacity. Meanwhile, high-energy batteries can entail increased fire safety issues. Here we report a composite current collector design that simultaneously minimizes the ‘dead weight’ within the cell and improves fire safety. An ultralight polyimide-based current collector (9 μm thick, specific mass 1.54 mg cm−2) is prepared by sandwiching a polyimide embedded with triphenyl phosphate flame retardant between two superthin Cu layers (~500 nm). Compared to lithium-ion batteries assembled with the thinnest commercial metal foil current collectors (~6 µm), batteries equipped with our composite current collectors can realize a 16–26% improvement in specific energy and rapidly self-extinguish fires under extreme conditions such as short circuits and thermal runaway.

Abstract

A combination of neutron diffraction and angle-resolved photoemission spectroscopy measurements on a pure antiferromagnetic stripe ${\mathrm{Rb}}_{1-\delta }{\mathrm{Fe}}_{1.5-\sigma }{S}_2$ is reported. A neutron diffraction experiment on a powder sample shows that a $98\%$ volume fraction of the sample is in the antiferromagnetic stripe phase with rhombic iron vacancy order and a refined composition of ${\mathrm{Rb}}_{0.66}{\mathrm{Fe}}_{1.36}{S}_2$, and that only $2\%$ of the sample is in the block antiferromagnetic phase with $\sqrt{5}\times \sqrt{5}$ iron vacancy order. Furthermore, a neutron diffraction experiment on a single crystal shows that there is only a single phase with the stripe antiferromagnetic order with the refined composition of ${\mathrm{Rb}}_{0.78}{\mathrm{Fe}}_{1.35}{S}_2$, while the phase with block antiferromagnetic order is absent. Angle-resolved photoemission spectroscopy measurements on the same crystal with the pure stripe phase reveal that the electronic structure is gapped at the Fermi level with a gap larger than 0.325 eV. The data collectively demonstrate that the extra $10\%$ iron vacancies in addition to the rhombic iron vacancy order effectively impede the formation of the block antiferromagnetic phase; the data also suggest that the stripe antiferromagnetic phase with rhombic iron vacancy order is a Mott insulator.

Abstract

Copper oxide high-T_C superconductors possess a number of exotic orders that coexist with or are proximal to superconductivity. Quantum fluctuations associated with these orders may account for the unusual characteristics of the normal state, and possibly affect the superconductivity^1,2,3,4. Yet, spectroscopic evidence for such quantum fluctuations remains elusive. Here, we use resonant inelastic X-ray scattering to reveal spectroscopic evidence of fluctuations associated with a charge order^{5,6,7,8,9,10,11,12,13,14} in nearly optimally doped Bi₂Sr₂CaCu₂O_8+δ. In the superconducting state, while the quasielastic charge order signal decreases with temperature, the interplay between charge order fluctuations and bond-stretching phonons in the form of a Fano-like interference increases, an observation that is incompatible with expectations for competing orders. Invoking general principles, we argue that this behaviour reflects the properties of a dissipative system near an order–disorder quantum critical point, where the dissipation varies with the opening of the pseudogap and superconducting gap at low temperatures, leading to the proliferation of quantum critical fluctuations, which melt charge order.

Abstract

We report in situ structural measurements of shock‐compressed single crystal orthoenstatite up to 337 ± 55 GPa on the Hugoniot, obtained by coupling ultrafast X‐ray diffraction to laser‐driven shock compression. Shock compression induces a disordering of the crystalline structure evidenced by the appearance of a diffuse X‐ray diffraction signal at nanosecond timescales at 80 ± 13 GPa on the Hugoniot, well below the equilibrium melting pressure (>170 GPa). The formation of bridgmanite and post‐perovskite have been indirectly reported in microsecond‐scale plate‐impact experiments. Therefore, we interpret the high‐pressure disordered state we observed at nanosecond scale as an intermediate structure from which bridgmanite and post‐perovskite crystallize at longer timescales. This evidence of a disordered structure of MgSiO₃ on the Hugoniot indicates that the degree of polymerization of silicates is a key parameter to constrain the actual thermodynamics of shocks in natural environments.

Abstract

We report the phase diagram of Nd_1−xSr_xNiO₂ infinite layer thin films grown on SrTiO₃. A superconducting dome spanning 0.125<x<0.25 is found, remarkably similar to cuprates, albeit over a narrower doping window. However, while cuprate superconductivity is bounded by an insulator for underdoping and a metal for overdoping, here we observe weakly insulating behavior on either side of the dome. Furthermore, the normal state Hall coefficient is always small and proximate to a continuous zero crossing in doping and in temperature, in contrast to the ∼1/x dependence observed for cuprates. This suggests the presence of both electronlike and holelike bands, consistent with band structure calculations.

Abstract

The resistance of a conventional insulator diverges as temperature approaches zero. The peculiar low-temperature resistivity saturation in the 4f Kondo insulator (KI) SmB₆ has spurred proposals of a correlation-driven topological Kondo insulator (TKI) with exotic ground states. However, the scarcity of model TKI material families leaves difficulties in disentangling key ingredients from irrelevant details. Here we use angle-resolved photoemission spectroscopy (ARPES) to study FeSb₂, a correlated d-electron KI candidate that also exhibits a low-temperature resistivity saturation. On the (010) surface, we find a rich assemblage of metallic states with two-dimensional dispersion. Measurements of the bulk band structure reveal band renormalization, a large temperature-dependent band shift, and flat spectral features along certain high-symmetry directions, providing spectroscopic evidence for strong correlations. Our observations suggest that exotic insulating states resembling those in SmB₆ and YbB₁₂ may also exist in systems with d instead of f electrons.

Abstract

Solid-state Li−S batteries are attractive due to their high energy density and safety. However, it is unclear whether the concepts from liquid electrolytes are applicable in the solid state to improve battery performance. Here, we demonstrate that the nanoscale encapsulation concept based on Li₂S@TiS₂ core−shell particles, originally developed in liquid electrolytes, is effective in solid polymer electrolytes. Using in situ optical cell and sulfur Kedge X-ray absorption, we find that polysulfides form and are welltrapped inside individual particles by the nanoscale TiS₂ encapsulation. This TiS₂ encapsulation layer also functions to catalyze the oxidation reaction of Li₂S to sulfur, even in solid-state electrolytes, proven by both experiments and density functional theory calculations. A high cell-level specific energy of 427 W·h· kg⁻¹ is achieved by integrating the Li₂S@TiS₂ cathode with a poly(ethylene oxide)-based electrolyte and a lithium metal anode. This study points to the fruitful direction of borrowing concepts from liquid electrolytes into solid-state batteries.

Abstract

Experiments using a THz pump and an X-ray probe at an X-ray free-electron laser (XFEL) facility like the Linac Coherent Light Source II (LCLS II) require frequency-tunable (3 to 20 THz), narrow bandwidth (~10%), carrier-envelopephase-stable THz pulses that produce high fields (>1 MV cm^-1) at the repetition rate of the X-rays and are well synchronized with them. In this paper, a two-bunch scheme to generate THz radiation at LCLS II is studied: the first bunch produces THz radiation in an electromagnet wiggler immediately following the LCLS II undulator that produces X-rays from the second bunch. The initial time delay between the two bunches is optimized to compensate for the path difference in THz transport. The two-bunch beam dynamics, the THz wiggler and radiation are described, as well as the transport system bringing the THz pulses from the wiggler to the experimental hall.

Abstract

We have performed an angle-resolved photoemission spectroscopy (ARPES) study of BaNi ₂P₂  that shows a superconducting transition at T_c  ∼ 2.5 K. We observed hole and electron Fermi surfaces (FSs) around the Brillouin zone center and corner, respectively, and the shapes of the hole FSs dramatically changed with photon energy, indicating strong three dimensionality. The observed FSs are consistent with band-structure calculations and de Haas-van Alphen measurements. The mass enhancement factors estimated in the normal state were m ∗/m_b ≤2, indicating weak electron correlation compared to typical iron-pnictide superconductors. An electronlike Fermi surface around the Z point was observed in contrast with BaNi ₂As₂ and may be related to the higher T_c of BaNi₂P₂.