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Hybrid metal halides (HMHs) with typical host–guest structures exhibit intentional, unique, and synergistic features of organic and inorganic components. Here, a novel 2D HMH with a conjugated polyacetylene skeleton is synthesized by pressure-induced solid-state topochemical polymerization (SSTP) of (C3H6N)2CdCl4(C3H6N+= propargylamine cation, PA-CdCl). Compared with the faint emission of PA-CdCl, polymerized (C3H6N)2CdCl4(P-PA-CdCl) exhibits a strong yellow emission from the helical polyacetylene skeletons. Furthermore, P-PA-CdClexhibits a narrowed bandgap of 2.26 eV, almost half the initial PA-CdCl. Theoretical calculations reveal that the transformation of optical properties is due to the reconstruction of the band alignment from type-I to reverse type-I via SSTP. Such an SSTP can be replicated in other 2D HMHs to yield polymerized HMHs with identical emissive polyacetylene skeletons. This study showcases the potential of pressure-induced SSTP in developing novel materials with intriguing properties, establishing it as a valuable platform for the structural regulation of HMHs and polymer synthesis.

The properties of pavement bitumen deteriorates when exposed to complicated environmental factors. This study developed a multi-environment simulation device to apply multi-factor coupling on asphalt mixtures. The physicochemical properties of recovered bitumen were analysed by traditional technical indicators, tensile strength, fourier transform infrared spectroscopy, and contact angle tests. The ageing index and target functional group index ratio were proposed to quantify the interactions of environmental factors. The results indicated that surface morphology of mixtures was severely affected by multi-factor coupling. The multi-factor coupling exacerbated the deterioration of physical properties and increased tensile strength, surface free energy, and adhesion work. However, the sulfoxide index was more affected by thermal ageing than the carbonyl index, and its change under ultraviolet and multi-factor actions was not obvious. The ageing index and target functional group index ratio indicated that the effect of ultraviolet-thermal coupling had the largest effect on the physicochemical properties of bitumen.

Lithium (Li) metal solid-state batteries feature high energy density and improved safety and thus are recognized as promising alternatives to traditional Li-ion batteries. In practice, using Li metal anodes remains challenging because of the lack of a superionic solid electrolyte that has good stability against reduction decomposition at the anode side. Here, we propose a new electrolyte design with an antistructure (compared to conventional inorganic structures) to achieve intrinsic thermodynamic stability with a Li metal anode. Li-rich antifluorite solid electrolytes are designed and synthesized, which give a high ionic conductivity of 2.1 × 10–4S cm–1at room temperature with three-dimensional fast Li-ion transport pathways and demonstrate high stability in Li–Li symmetric batteries. Reversible full cells with a Li metal anode and LiCoO2cathode are also presented, showing the potential of Li-rich antifluorites as Li metal-compatible solid electrolytes for high-energy-density solid-state batteries.

The development of cutting-edge solid-state electrolytes (SSEs) entails a deep understanding of the underlying correlation between the structure and ionic conductivity. Generally, the structure of SSEs encompasses several interconnected crystal parameters, and their collective influence on Li+transport can be challenging to discern. Here, we systematically investigate the structure–function relationship of halide spinel LixMgCl2+x(2 ≥ x≥ 1) SSEs. A nonmonotonic trend in the ionic conductivity of LixMgCl2+xSSEs has been observed, with the maximum value of 8.69 × 10–6S cm–1achieved at x= 1.4. The Rietveld refinement analysis, based on neutron diffraction data, has revealed that the crystal parameters including cell parameters, Li+vacancies, Debye–Waller factor, and Li–Cl bond length assume diverse roles in influencing ionic conductivity of LixMgCl2+xat different stages within the range of xvalues. Besides, mechanistic analysis demonstrates Li+transport along three-dimensional pathways, which primarily governs the contribution to ionic conductivity of LixMgCl2+xSSEs. This study has shed light on the collective influence of crystal parameters on Li+transport behaviors, providing valuable insights into the intricate relationship between the structure and ionic conductivity of SSEs.

Because the modulation accuracy and precision of liquid crystal spatial light modulator (LC-SLM) are strongly influenced by difference in operation conditions and the manufacturing errors of spatial light modulator, it is an essential procedure to measure and calibrate its phase modulation characteristics such as phase errors and nonlinear compensation quality. In this letter, we propose a novel method based on Quadriwave lateral shearing interferometry to obtain these phase modulation characteristics for LC-SLM, which in theory presents obvious advantages over conventional methods such as high precision, excellent noise immunity, and the requirement of only one interferogram during reconstructing modulation phase. The validity of our proposed method has been verified by comparing the experimental results with those obtained from Twyman-Green Interferometry and Optical Power interferometry.

The rational design of solid electrolytes for the next-generation batteries entails an accurate understanding of ionic transport mechanisms. To elucidate the detailed ion hopping processes in different coordinate environments, two solid electrolytes, LiTi2(PO4)3and Li3Ti2(PO4)3, with the same NASICON-type framework but different sites for accommodating mobile ions, were synthesized and investigated by in situneutron diffraction and theoretical calculations. The temperature-dependent anisotropic thermal vibrational ellipsoids and migration paths from the maximum entropy method (MEM) indicated that Li ions move faster at higher coordinate architectures, exhibiting three-dimensional (3D) diffusion pathways. In this rhombohedral structure, “one” node (M1 site) out of “three” interconnected transition sites was found to be the lithium configuration of NASICON. Li ions located at the nodes along the 3D pathway in LiTi2(PO4)3can only drive out another Li-ion species at the node site, while Li ions located at transition sites between two nodes in Li3Ti2(PO4)3have repulsive force from their five surrounding Li ions. These different configurations lead to distinct overall transport modes. In LiTi2(PO4)3, concerted Li ions transport along a separated chain, while in Li3Ti2(PO4)3, concerted motion occurs along multiple cooperating chains in the 3D channels. Theoretical calculations further indicated that a larger diffusion bottleneck size of Li3Ti2(PO4)3enables lower hopping energy compared to LiTi2(PO4)3. This study clarifies the detailed ionic hopping processes and the underlying structure–conductivity relationships. Overall, these results elucidate the synergistic events in Li-ion hopping from thermodynamic and kinetic points of view, which will greatly benefit the rational design of solid electrolytes for next-generation batteries.

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Diffusion-mediated assembly of octahedral PbS nanocrystals (NCs) in a confined antisolvent environment displays a primary burst nucleation and Ostwald ripening growth of rhombic bcc supercrystals, followed by a secondary seed-based nucleation and oriented attachment growth of triangle fcc supercrystals. As the diffusion proceeds from ethanol across a sharp interface into NC-suspended toluene, a burst nucleation of supercrystal seeds occurs, and such supercrystals are quickly developed into rhombic grains that have a bcc structure. At a critical size of 10 μm, an Ostwald ripening event appears to guide the supercrystal growth. Upon grain growth above 30 μm, the fcc supercrystals start a nucleation at two symmetrical tips of individual rhombic crystals. Such fcc supercrystals are developed with a triangle shape, and two triangles are combined with one bcc rhombus in-between to form a butterfly-like bowtie stacking structure. The fcc triangle wings grow larger at a reduction of bcc rhombus cores. As the bcc cores gradually fade, such butterfly-like bowtie crystals aggregate and undergo an oriented attachment process, leading to the formation of freestanding 3D triangle crystals that have a single fcc lattice. Analysis of experimental observations and defined diffusion parameters reveals that fast solvent diffusion and high-NC concentration promote the growth of rhombic bcc supercrystals, while slow solvent diffusion and low-NC concentration accelerate the development of triangle fcc supercrystals. Upon succeeding in designable growth of 3D fcc supercrystals, this study provides designing principles for controlled fabrication of supercrystals with desired superlattices for additional engineering and applications.

By partial fluorination, the crystal phase of antiperovskite is changed; the Li+migration is accelerated; and the stability with electrodes is improved.

This work illustrates the effect of voids in LiRAP pellets on lithium dendrite growth and shows that reducing the voids can effectively suppress lithium dendrite growth.

The comparison of different stereoisomeric organic compounds under high pressure has been less investigated. Here, we chose different stereochemical configurations of cis/trans-stilbene to study the luminescence properties, polymerization reaction, and structural changes at 0–20 GPa by spectroscopy and XRD. No fluorescence enhancement occurred in cis-stilbene due to π–π stacking. At 16 GPa, the IR, UV–vis, and sample color changes show that it undergoes an irreversible polymerization, that C(sp2)–H changes to C(sp2+ sp3)–H. However, trans-stilbene undergoes fluorescence enhancement at 0–4 GPa due to the reduction of the torsion angle of the benzene ring and the C═C bond leading to the formation of rigid planar molecules, which is further confirmed by the IR and XRD results. At 8 GPa, the new peaks in UV–vis and XRD results show the formation of new substances by structural change. However, the structure of trans-stilbene is more stable, which leads to the return to the raw state after releasing the pressure, and a reversible transformation occurs at high pressure. The cis-trans isomerization under high pressure was also briefly investigated by combining heating and laser irradiation. The cis → trans-stilbene transition can only happen under a fixed-range light irradiation, and the trans → cis-stilbene transition could not happen even under irradiation with a 360 nm laser, which may provide a new idea for synthesizing trans isomers with a higher purity.

Recently, halide materials for solid electrolytes have received modest research interest. A variety of new halide electrolytes, such as Li3YCl6, Li3InCl6, and Li2Sc2/3Cl4halospinel structure, and LiAlCl4, have been experimentally prepared with high Li-ionic conductivities close to 10–3S/cm and low activation energies. Although much effort (experimental and theoretical) has been devoted to uncovering the best combination of Li–M–X, less attention has been paid to the structural effects on the ionic conductivities and electrochemical stabilities. In this article, DFT and AIMD simulations are performed to do a comparative study on several halide electrolytes with selected structures, including the most common rock-salt Li3MCl6, spinel Li2M2/3Cl4, and LiMCl4. It is revealed that halospinel Li2M2/3Cl4structures with cubic symmetry are three-dimensionally conducting and mechanically stable superionic conductors. They exhibit an excellent Li-ionic conductivity within the range 0.26–19.0 mS/cm with an activation energy lower than 0.20 eV (0.342–0.195 eV). Among them, Li2Sm2/3Cl4is predicted to have an outstanding balance between the ionic conductivity and stability. The room-temperature ionic conductivity is calculated to be as high as 15.3 mS/cm, whereas the band gap and electrochemical stability window vs Li/Li+reach 4.26 V, respectively, making it a promising candidate for practical applications as a superionic conductor in solid-state batteries.

Byline: Kun. Zhang, Min. Zhang, Jinlong. Zhu, Wang. Hong Objective: The objective of this study is to assess the gene mutation of advanced nonsmall cell lung cancer (NSCLC) patients with [...]

Multi-level programmable photonic integrated circuits (PICs) and optical metasurfaces have gained widespread attention in many fields, such as neuromorphic photonics, optical communications, and quantum information. In this paper, we propose pixelated programmable Si3N4PICs with record-high 20-level intermediate states at 785 nm wavelength. Such flexibility in phase or amplitude modulation is achieved by a programmable Sb2S3matrix, the footprint of whose elements can be as small as 1.2 μm, limited only by the optical diffraction limit of an in-house developed pulsed laser writing system. We believe our work lays the foundation for laser-writing ultra-high-level (20 levels and even more) programmable photonic systems and metasurfaces based on phase change materials, which could catalyze diverse applications such as programmable neuromorphic photonics, biosensing, optical computing, photonic quantum computing, and reconfigurable metasurfaces.

Superhard semiconductors have been long sought after for electronic device applications enduring extreme conditions, such as astronautics, due to their intrinsic toughness, high thermal and chemical stability. Here, we report the superhard p-type semiconductor Al2.69B50single crystal with the determined Vickers hardness of ∼40.5 GPa under the load of 0.49 N, which is one of the hardest semiconductor compounds that have been ever found. With the direct band gap of 2.3 eV, Al2.69B50exhibits excellent optical transmittance (>90%), covering the visible range from 459 nm to 760 nm and part of the infrared range, and also shows the high intensity of the photon emission in the visible light. Al2.69B50is very stable, thermally and chemically, with an ultra-low density of ∼2.52 g cm−3, allowing for further extension of its applications. Such an assembly of various excellent properties within one material has great implication for high power electronic design and applications.

All-solid-state lithium-metal batteries, with their high energy density and high-level safety, are promising next-generation energy storage devices. Their current performance is however compromised by lithium dendrite formation. Although using 3D-structured metal-based electrode materials as hosts to store lithium metal has the potential to suppress the lithium dendrite growth by providing a high surface area with lithiophilic sites, their rigid and ragged interface with solid-state electrolytes is detrimental to the battery performance. Herein, we show that Li2OHBr-containing poly(ethylene oxide) (PEO) polymer electrolytes can be used as a flexible solid-state electrolyte to mitigate the interfacial issues of 3D-structured metal-based electrodes and suppress the lithium dendrite formation. The presence of Li2OHBr in a PEO matrix can simultaneously improve the mechanical strength and lithium ion conductivity of the polymer electrolyte. It is confirmed that Li2OHBr does not only induce the PEO transformation of a crystalline phase to an amorphous phase but also serves as an anti-perovskite superionic conductor providing additional lithium ion transport pathways and hence improves the lithium ion conductivity. The good interfacial contact and high lithium ion conductivity provide sufficient lithium deposition sites and uniform lithium ion flux to regulate the lithium deposition without the formation of lithium dendrites. Consequently, the Li2OHBr-containing PEO polymer electrolyte in a lithium-metal battery with a 3D-structured lithium/copper mesh composite anode is able to improve the cycle stability and rate performance. The results of this study provide the experimental proof of the beneficial effects of the Li2OHBr-containing PEO polymer electrolyte on the 3D-structured lithium metal anode.

Understanding ice nucleation and growth is of great interest to researchers due to its importance in the biological, cryopreservation, and environmental fields. However, microstructural investigations of ice on the molecular scale are still lacking. In this paper, a simple method is proposed to prepare quasi-2-dimensional ice Ihfilms, which have been characterized via cryogenic transmission electron microscope. The intersecting stacking faults of basal (BSF) and prismatic (PSF) types have been directly visualized and resolved with a notable first-time report of PSF in ice Ih. Moreover, the possible growth pathways of BSF, namely, the Icphase, were elucidated by the theoretical calculations and the chair conformation of H2O molecules. This study offers valuable insights that can enhance researchers’ understanding of the growth kinetics of crystalline ice.

Crystallization and growth of anisotropic nanocrystals (NCs) into distinct superlattices were studied in real time, yielding kinetic details and designer parameters for scale-up fabrication of functional materials. Using octahedral PbS NC blocks, we discovered that NC assembly involves a primary lamellar ordering of NC-detached Pb(OA)2molecules on the front-spreading solvent surfaces. Upon a spontaneous increase of NC concentration during solvent processing, PbS NCs preferentially self-assembled into an orientation-disordered face-centered cubic (fcc) superlattice, which subsequently transformed into a body-centered cubic (bcc) superlattice with single NC-orientational ordering across individual domains. Unlike the deformation-based transformation route claimed previously, this solid–solid phase transformation involved a hidden intermediate formation of a lamellar-confined liquid interface at cost of the disassembly (melting) of small fcc grains. Such highly condensed and liquidized NCs recrystallized into the stable bcc phase with an energy reduction of 1.16 kBT. This energy-favorable and high NC-fraction-driven bcc phase grew as a 2D film at a propagation rate of 0.74 μm/min, smaller than the 1.23 μm/min observed in the early nucleated fcc phase under a dilute NC environment. Taking such insights and defined parameters, we designed experiments to manipulate the NC assembly pathway and achieved scalable fabrication of a large/single bcc supercrystal with coherent ordering of NC translation and atomic plane orientation. This study not only provides a design avenue for controllable fabrication of a large supercrystal with desired superlattices for application but also sheds new light on the nature of crystal nucleation/growth and phase transformation by extending the lengths from the nanoscale into the atomic scale, molecular scale, and microscale levels.

Solid-state electrolytes (SSEs) with high ionic conductivities are the key components in solid-state batteries, and the ionic conductivities of SSEs are strongly related to their underlying crystal structures. However, the current structural descriptions mainly focus on static average structure, with certain limitations due to an incomplete understanding of the ionic conduction mechanism in solid electrolytes. Herein, a relationship between ionic transport and local lattice dynamics at an atomic scale is presented. The local structural changes by altering the fractional occupancy of the halide anions in antiperovskite Li2OHX (Cl, Br) are investigated using atomic pair distribution function (PDF), and the corresponding Li+transport behaviors are obtained by electrochemical impedance spectroscopy (EIS). The increased lattice polarization and distortion are observed to decrease both activation barriers and Arrhenius prefactor upon changing the Br contents. It indicates that the synergistic effects of local structural changes on the activation barrier and Arrhenius prefactor both should be considered for promoting ionic transport. The investigation shows an in-depth understanding of ion conduction in solid electrolytes and delivers a new insight for developing new ionic conductors.

Lithium metal is considered to be the ultimate anode for lithium-ion batteries (LIBs) because of its ultrahigh capacity and lowest electrochemical potential. However, the high reactivity of the lithium metal triggers continuous electrolyte consumption and dendrite growth, resulting in short cycle lifetime and serious safety issues. Massive efforts have been made to stabilize the surface of the lithium metal anode. Here, we propose an amide-based passivation layer to serve as an electrochemically stable and highly tough SEI on the lithium metal anode by in situ generation. The SEI layer presents a high elasticity modulus of 10 GPa and enables stable cycling in 2500 h. Furthermore, based on our strategy, the Li/LiFePO4cell with a cathode loading of ∼19 mg cm–2exhibits a long lifespan of 400 cycles. Our approach establishes a meaningful guideline for building a highly strong electrolyte/electrode interface in high-energy density lithium metal batteries.

The report on the superconductivity of the two-legged spin ladders BaFe2S3and BaFe2Se3has established 123-type iron chalcogenides as a novel subgroup in the iron-based superconductor family and has stimulated the continuous exploration of other iron-based materials with new structures and potentially novel properties. In this paper, we report the systematic study of a new quasi-one-dimensional (1D) iron-based compound, Ba9Fe3Te15, including its synthesis and magnetic properties. The high-pressure synthesized Ba9Fe3Te15crystallized in a hexagonal structure that mainly consisted of face-sharing FeTe6octahedral chains running along the caxis, with a lattice constant of a= 10.23668 Å; this led to weak interchain coupling and an enhanced one-dimensionality. The systematic static and dynamic magnetic properties were comprehensively studied experimentally. The dc magnetic susceptibility showed typical 1D antiferromagnetic characteristics, with a Tmaxat 190 K followed by a spin glass (SG) state with freezing at Tf≈ 6.0 K, which were also unambiguously proved by ac susceptibility measurements. Additionally, X-ray magnetic circular dichroism (XMCD) experiments revealed an unexpected orbital moment for Fe2+, i.e., 0.84 μBper Fe in Ba9Fe3Te15. The transport property is electrically insulating, with a thermal activation gap of 0.32 eV. These features mark Ba9Fe3Te15as an alternative type of iron-based compound, providing a diverse candidate for high-pressure studies in order to pursue some emerging physics.

Nonuniform depolarization properties of ${\text{SiO}_2}$SiO_2 thin film, two-dimensional (2D) Si grating, and three-dimensional Si cylinder grating, were systematically investigated by Lu-Chipman decomposition. We find that introducing surface profiles with dimensions comparable to the detecting wavelengths can lead to obvious nonuniform depolarization, and control of the sample azimuth can manipulate the uniformity of the depolarizer components. The results indicate that the 2D nanostructure shows obvious nonuniform depolarization at 0° and 90° azimuths, while almost uniform depolarization at 45° azimuth. These discovered phenomena may give rise to some potential applications, such as the detection of the existence of nanostructures without a priori information about the sample, and the design of a uniform or nonuniform depolarizer.

Treatment failure in patients with liver hepatocellular carcinoma (LIHC) is primarily caused by tumor progression and therapy resistance. Tumor immunity plays a crucial role in regulating the homeostasis of cells through the process of programmed cell death (PCD). However, the expression profile and clinical significance of PCD-related genes in LIHC require further investigation. In this study, we analyzed twelve commonly observed PCD patterns to construct a prognostic model. We collected RNA-seq data, genomics, and clinical information from TCGA-LIHC and GSE14520 cohorts to validate the prognostic gene signature. We discovered 75 PCD-related differentially expressed genes (DEGs) with prognostic significance in LIHC. Using these genes, we constructed a PCD-related score (PCDscore) with an 11-gene signature through LASSO COX regression analysis. Validation in the GSE14520 cohort demonstrated that LIHC patients with high PCDscore had poorer prognoses. Unsupervised clustering based on the 11 model genes revealed 3 molecular subtypes of LIHC with distinct prognoses. By incorporating PCDscore with clinical features, we constructed a highly predictive nomogram. Additionally, PCDscore was correlated with immune checkpoint genes and immune cell infiltration. LIHC patients with high PCDscore exhibited sensitivity to common chemotherapy drugs (such as cisplatin and docetaxel). To summarize, our study developed a novel PCDscore model that comprehensively analyzed different cell death modes, providing an accurate prediction of clinical prognosis and drug sensitivity for LIHC patients.

Recently, topological insulators (TIs) KHgX (X = As, Sb, Bi) with hourglass-shaped dispersion have attracted great interest. Different from the TIs protected by either time-reversal or mirror crystal symmorphic symmetry tested in previous experiments, these materials were proposed as the first material class whose band topology relies on nonsymmorphic symmetries. As a result, KHgX shows many exotic properties, such as hourglass-shaped electronic channels and three-dimensional doubled quantum spin Hall effects. To date, high-pressure experimental studies on these nonsymmorphic TIs are minimal. Here, we carried out high-pressure electrical measurements up to 55 GPa, together with high-pressure X-ray diffraction measurements and high-pressure structure prediction on KHgAs. We found a pressure-induced semiconductor-metal transition between ~16 and 20 GPa, followed by the appearance of superconductivity with a Tcof ~3.5 K at approximately 21 GPa. The superconducting transition temperature was enhanced to a maximum of ~6.6 K at 31.8 GPa and then slowly decreased until 55 GPa. Furthermore, three high-pressure phases within 55 GPa were observed, and their crystal structures were established. Our results showed the high-pressure phase diagram of KHgAs and determined the pressure-induced superconductivity in nonsymmorphic TIs. Thus, our study can be used to facilitate further research on superconductivity and topologically nontrivial features protected by nonsymmorphic symmetries.

Lithium batteries have been essential technologies and become an integral part of our daily lives, powering a range of devices from phones to electric vehicles. To fully understand and optimize the performance of lithium batteries, it is necessary to investigate their internal states and processes through various characterization methods. Neutron imaging has been an indispensable complementary characterization technique to X-ray imaging or electron microscopy because of the unique interaction principle between neutrons and matter. It provides particular insights into the various states of matter inside lithium batteries, including the Li+concentration in solid electrodes, the Li plating/stripping behavior of Li-metal anodes, the Li+diffusion in solid ionic conductors, the distribution of liquid electrolytes and the generation of gases. This review aims to highlight the capabilities and advantages of neutron imaging in characterizing lithium batteries, as well as its current state of application in this field. Additionally, we discuss the potential of neutron imaging to contribute to the ongoing development of advanced batteries through its ability to visualize internal evolution.Neutron imaging is an indispensable technique for understanding batteries by providing unique insights into their internal states and processes, including lithium ion concentration, Li-metal anode behavior, electrolyte distribution, and gas generation.

Using light as a probe to investigate perturbations with deep subwavelength dimensions in large-scale wafers is challenging because of the diffraction limit and the weak Rayleigh scattering. In this Letter, we report on a nondestructive noninterference far-field imaging method, which is built upon electrodynamic principles (mechanical work and force) of the light-matter interaction, rather than the intrinsic properties of light. We demonstrate sensing of nanoscale perturbations with sub-10 nm features in semiconductor nanopatterns. This framework is implemented using a visible-light bright-field microscope with a broadband source and a through-focus scanning apparatus. This work creates a new paradigm for exploring light-matter interactions at the nanoscale using microscopy that can potentially be extended to many other problems, for example, bioimaging, material analysis, and nanometrology.

Environmental scanning electron microscopy (ESEM) is a broadly utilized nanoscale inspection technique capable of imaging wet or insulating samples. It extends the application of conventional scanning electron microscopy (SEM) and has been extensively used to study the behavior of liquid, polymer, and biomaterials by allowing for a gaseous environment. However, the presence of gas in the chamber can severely degrade the image resolution and contrast. This typically limits the ESEM operating pressure below 1000 Pa. The dynamic interactions, which require even-higher sensitivity and resolution, are particularly challenging to resolve at high-pressure conditions. Here, we present an enhanced ESEM technique using phase reconstruction to extend the limits of the ESEM operating pressure while improving the image quality, which is useful for sensing weak scattering from transparent or nanoscale samples. We applied this method to investigate the dynamics of condensing droplets, as an example case, which is of fundamental importance and has many industrial applications. We visualized dynamic processes such as single-droplet growth and droplet coalescence where the operating pressure range was extended from 1000 to 2500 Pa. Moreover, we detected the distribution of nucleation sites on the nanostructured surfaces. Such nanoscale sensing has been challenging previously due to the limitation of resolution and sensitivity. Our work provides a simple approach for high-performance ESEM imaging at high-pressure conditions without changes to the hardware and can be widely applied to investigate a broad range of static and dynamic processes.

Nanocube (NC) assemblies display complex superlattice behaviors, which require a systematic understanding of their nucleation and growth as well transformation toward construction of a consistent superlattice phase diagram. This work made use of Fe3O4NCs with controlled environments, and assembled NCs into three-dimensional (3D) superlattices of simple cubic (sc), body-centered cubic (bcc), and face-centered cubic (fcc), acute and obtuse rhombohedral (rh) polymorphs, and 2D superlattices of square and hexagon. Controlled experiments and computations of in situ and static small-angle X-ray scattering (SAXS) as well as electron microscopic imaging revealed that the fcc and bcc polymorphs preferred a primary nucleation at the early stage of NC assembly, which started from the high packing planes of fcc(111) and bcc(110), respectively, in both 3D and 2D cases. Upon continuous growth of superlattice grain (or domain), a confinement stress appeared and distorted fcc and bcc into acute and obtuse rh polymorphs, respectively. The variable magnitudes of competitive interactions between configurational and directional entropy determine the primary superlattice polymorph of either fcc or bcc, while emergent enhancement of confinement effect on enlarged grains attributes to late developed superlattice transformations. Differently, the formation of a sc polymorph requires a strong driving force that either emerges simultaneously or is applied externally so that one easy case of the sc formation can be achieved in 2D thin films. Unlike the traditional Bath deformation pathway that involves an intermediate body-centered tetragonal lattice, the observed superlattice transformations in NC assembly underwent a simple rhombohedral distortion, which was driven by a growth-induced in-plane compressive stress. Establishment of a consistent phase diagram of NC-based superlattices and reconstruction of their assembly pathways provide critical insight and a solid base for controlled design and scalable fabrication of nanocube-based functional materials with desired superlattices and collective properties for real-world applications.

Reducing pregnancy loss is important for improving reproductive efficiency for both human and mammalian animals. Our previous study demonstrates that maternal N-carbamylglutamate (NCG) supply during early pregnancy enhances embryonic survival in gilts. However, whether maternal NCG supply improves the pregnancy outcomes is still not known. Here we found maternal NCG supply during early pregnancy in sows significantly increased the numbers of total piglets born alive per litter (P< 0.05) and significantly changed the levels of metabolites in amniotic fluid and serum involved in metabolism of energy, lipid, and glutathione and immunological regulation. The expression of endometrial progesterone receptor membrane component 1 (PGRMC1) was significantly increased by NCG supplementation (P< 0.05) as well as the expression of PGRMC1, endothelial nitric oxide synthesases (eNOS), and lamin A/C in fetuses and placentae (P< 0.05). Among the NCG-associated amino acids, arginine and glutamine, markedly increased PGRMC1 and eNOS expression in porcine trophectoderm cells (P< 0.05), whereas glutamate could stimulate the expression of vimentin and lamin A/C in porcine trophectoderm (pTr) cells (P< 0.05) and proline stimulated lamin A/C expression (P< 0.05). Collectively, these data reveal the mechanisms of NCG in reducing early embryo loss. These findings have important implications that NCG has great potential to improve pregnancy outcomes in human and mammalian animals.

A novel solid sodium-ion conductor, Na2Mg2TeO6(NMTO) with a P2-type honeycomb-layered structure, has been synthesized for the first time by a simple solid-state synthetic route. The conductor of NMTO exhibits high conductivity of 2.3 × 10–4S cm–1at room temperature (RT) and a large electrochemical window of ∼4.2 V (versus Na+/Na). The conductor is remarkably stable, both in the ambient environment and within its metallic Na anode. This facile sodium-ion conductor displays potential for use in all-solid-state sodium-ion batteries (SS-SIBs).

Synchrotron-based in situ pressure small- and wide-angle X-ray scattering and associated strain analysis reveal a pressure-driven anisotropic strain distribution across a Pt nanocube (NC) assembled supercrystal that has an obtuse rhombohedral superlattice. This strain anisotropy is largely controlled by the rational interplay between soft organic molecules and hard NC cores localized at various ratios in the four types of decoded NC arrangements. Upon compression below 10 GPa, the strain appears as a superlattice shrinkage, which is developed mainly at molecule-rich regimes in the facet–facet and nondirect-contact configurations of NC arrangement. Above 10 GPa, an anisotropic strain enhances and accordingly starts an apparent superlattice shrinkage at molecule-poor regimes in the corner–corner and edge–edge configurations, whereas an unusual superlattice expansion is simultaneously triggered in molecule-rich regimes. Upon the release of pressure, a normal superlattice expansion arises only at molecule-rich regimes, but a constant superlattice remains at molecule-poor regions, and below 2 GPa, a discontinuous jump occurs. In situ electrical resistance measurements of single supercrystals under pressure and electron microscopy imaging of harvested samples further reveal a pressure-induced phase switching between the insulator and conductor in a low dimension (1D or 2D) as defined at 10 GPa under compression and 2 GPa under decompression. This typical phase switching originates from a pressure-driven NC attachment and weak fusion and subsequently a decompression-induced NC detachment. This consequence is largely controlled by the development of a stable 2D Maxwell-like topological lattice through a small fraction of facet–facet and edge–edge attachments between slightly deflected NCs. These results provide insights into the anisotropic interplay between soft and hard components in nanobased architectures with response to the enhancement and manifestation of material properties.

Pressure-induced emission enhancement is a new and effective way to manipulate the color of organic materials. However, the specific fluorescence enhancement mechanism and the causes of the color change have not been previously well explored. Herein, two rofecoxib derivatives, MOX2 and Y7, were synthesized with methyl sulfonyl and cyan as the terminal groups on the para-position of the benzene ring ② (Ph-②), and their fluorescence behavior was investigated at 0–20 GPa. The two compounds exhibit opposite pressure-tuned fluorescent behavior in the 0–3.1 GPa range. Theoretical calculation indicates that the −SO2CH3group of MOX2 directs the dihedral angle between the Ph-② and Ph-③ ring planes to an optimized steric position, producing a large steric hindrance and neutralizing the influence of pressure on the benzene ring, which results in the invariance of the fluorescence peak position. The change in this dihedral angle is mainly caused by the gradual formation of hydrogen bonds between the O atoms on −SO2and the H atoms of the benzene ring, resulting in a 6.3-fold increase in the fluorescence intensity. Conversely, the luminescence intensity of Y7 is monotonously suppressed as the pressure is increased due to the smaller size of the −C≡N substituent. This study provides a reference for regulating the luminescence properties of organic molecules.

All-solid-state sodium-ion batteries (ASSSIBs) are viewed as a potential alternative to Li-ion batteries due to the advantages in safety and cost. Na-ion electrolytes are the key component of ASSSIBs and required to possess low electronic conductivity, high ionic conductivity, wide electrochemical stable window, and good electrode compatibility. Framework structures, like Na8(AlSiO4)6X2(X = Cl, Br and I), receive broad research interest for catalysis, ion exchange and adsorption due to the interesting open structure. However, little attention is paid to such types of minerals for superionic conductors. In this investigation, a first-principles study using density functional theory and ab initio molecular dynamic simulations are carried out to predict electronic structure, thermodynamic interface stability and Na-ionic conductivity of Na8(AlSiO4)6X2, suggesting wide bandgaps (>6 eV) but extremely low ionic conductivity in perfect Na8(AlSiO4)6X2. By introducing artificial Na vacancy, three-dimensional diffusional pathway forms in the structure and generates significantly improved sodium conduction while maintaining the energetic and thermal stability, demonstrating the potential for ASSSIBs.

Van der Waals heterostructures have recently attracted great interest of the scientific community due to their rich exotic physical properties and extensive application prospects. Therefore, we conducted pressure-dependent Raman and photoluminescence spectroscopic studies on MoS2–WS2heterostructures in different twist angles (24.5 and 54°). Thus, it was confirmed that as the interlayer interaction increases under pressure, an electronic phase transition and a structural phase transition due to layer sliding are observed at ∼1.8 and ∼3.8 GPa in the HS-24.5° structures, while no phase transition is observed in the HS-54° structures. As a result of a larger tunable interlayer space in HS-24.5° structures, optical properties of HS-24.5° structures are more pressure-sensitive than those of the HS-54° structure. It is expected that this work will help comprehensively establish the correlation between the interlayer interactions and optical properties of vdW HSs at the atomic level. Understanding this correlation is crucial for the development of new excitonic devices.

Solid-state electrolytes (SSEs) play the most important role in the develo-pment of cutting-edge all-solid-state batteries (ASSBs). The lithium (sodium)-rich antiperovskite solid conductors have been considered as the promising SSEs due to the structural tolerance for lattice manipulation and the potential to improve ionic conductivity. In particular, lithium (sodium)-rich antiperovskite SSEs are mainly composed of light elements (e.g., Li, O, H), which are suitable for studying the structure and ionic transport mechanism through neutron diffraction techniques. This present review summarizes the progress of neutron diffraction in analyzing the structure and revealing the ionic transport mechanisms of antiperovskite SSEs. The structure-function relationships involved in ionic transport pathways, defect chemistry, anion disorder and lattice dynamics are introduced respectively. In addition, the possible future directions for the application of neutron diffraction in antiperovskite SSEs are suggested.

CO2capture is a viable solution for mitigating the global CO2emission in the atmosphere. Hydrate-based CO2capture is a promising technology. In this study, the CO2hydrate formation thermodynamics and kinetics, along with the factors that influence CO2capture in nanoporous silica gels (named S9, S26, and S77 with an average pore size of 9, 26 and 77 nm, respectively), with different degrees of nanoconfinement were investigated. The CO2hydrate phase equilibrium and dissociation heat were determined by heat flow analysis. The heat flow curves revealed the formation of both confined- and bulk-phase hydrates in S9 and only bulk-phase hydrate in S26 and S77. The phase equilibrium temperature of the confined-phase hydrate was about 10 K lower than that of the bulk-phase hydrate and the dissociation heat of confined phase hydrate is 285.81 J/g in S9. According to the pressure curves, the CO2hydrate formation time in S9 was 2–3.5 times longer than that in S26 and S77. Compared with dry silica gel, the supersaturated one was more conducive to CO2capture. Under the same water saturation condition, the CO2capture ability of S26 and S77 was stronger than that of S9, and the effect of water saturation was dominant over that of pressure. Thus, nanoconfinement in S9 has an adverse effect on hydrate-based CO2capture whereas that in S26 and S77 is advantageous to it. This study provides an important fundamental basis for enhancing the hydrate-based CO2capture ability via nanoconfinement in silica gel.

Critical dimension measurement accuracy in optical scatterometry relies not only on the systematic noise level of instruments and the reliability of forward modeling algorithms, but also heavily on the measurement configuration. To construct a set of potentially high-accuracy configurations, we apply a general measurement configuration optimization method based on error propagation theory and singular value decomposition, by which the measurement accuracy is approximated as a function of a pseudo Jacobian with respect to the measurement configurations. Simulations and experiments for the optical metrology of a sub-wavelength deep-etched multilayer grating establish the feasibility of the proposed method.

Na-rich antiperovskites are recently developed solid electrolytes with enhanced sodium ionic conductivity and show promising functionality as a novel solid electrolyte in an all solid-state battery. In this work, the sodium ionic transport pathways of the parent compound Na3OBr, as well as the modified layered antiperovskite Na4OI2, were studied and compared through temperature-dependent neutron diffraction combined with the maximum entropy method. In the cubic Na3OBr antiperovskite, the nuclear density distribution maps at 500 K indicate that sodium ions hop within and among oxygen octahedra, and Br–ions are not involved. In the tetragonal Na4OI2antiperovskite, Na ions, which connect octahedra in the abplane, have the lowest activation energy barrier. The transport of sodium ions along the caxis is assisted by I–ions.

The pathogenetic mechanism of Alzheimer’s disease (AD) is still unknown; however, gene polymorphism may play a critical role in the pathogenesis of AD. The aim of this meta-analysis was to evaluate the association between FAS gene A-670G polymorphism and AD. We searched all related subjects in PubMed, Embase, Cochrane Library, SinoMed, and the China Knowledge Resource Integrated Database and identified seven studies reporting a relationship between the A-670G polymorphism in the FAS gene and AD. A total of 1512 cases and 1707 controls were included in the seven studies. The meta-analyses results suggested no significant association between the A-670G polymorphism and AD in any genetic models. When a subgroup analysis was conducted by ethnicity, the A-670G polymorphism was also not relevant to AD. However, when stratified by age, the GG genotype increased the risk of early-onset AD. We also found that the A-670G polymorphism was related to patients with AD who carried the apolipoprotein-E ε4 allele in three genetic models. To sum up, our data suggested that the FAS gene A-670G polymorphism may not be associated with AD. When a subgroup analysis was conducted by ethnicity, the A-670G polymorphism was also not related with AD in Asian and Caucasian population. However, the FAS-670 GG genotype may increase the risk of AD in the younger population (age, ≤65 years). Furthermore, we found that the A-670G polymorphism was related to patients with AD who carried the APOE4 allele in dominant, allele and homozygous models.

The growing demand for electronic devices, smart devices, and the Internet of Things constitutes the primary driving force for marching down the path of decreased critical dimension and increased circuit intricacy of integrated circuits. However, as sub-10 nm high-volume manufacturing is becoming the mainstream, there is greater awareness that defects introduced by original equipment manufacturer components impact yield and manufacturing costs. The identification, positioning, and classification of these defects, including random particles and systematic defects, are becoming more and more challenging at the 10 nm node and beyond. Very recently, the combination of conventional optical defect inspection with emerging techniques such as nanophotonics, optical vortices, computational imaging, quantitative phase imaging, and deep learning is giving the field a new possibility. Hence, it is extremely necessary to make a thorough review for disclosing new perspectives and exciting trends, on the foundation of former great reviews in the field of defect inspection methods. In this article, we give a comprehensive review of the emerging topics in the past decade with a focus on three specific areas: (a) the defect detectability evaluation, (b) the diverse optical inspection systems, and (c) the post-processing algorithms. We hope, this work can be of importance to both new entrants in the field and people who are seeking to use it in interdisciplinary work.

Accurate, fast, and nondestructive reconstruction of the etched nanostructures is important for etching process control to achieve good fidelity, as well as high manufacturing yield. In this work, we have demonstrated the improved deep-etched multilayer grating reconstruction by simultaneously considering the model error of nonuniform side-wall angle (SWA) because of different etching anisotropies of various materials and by suppressing the abnormally distributed measurement errors using a robust statistics based method in optical scatterometry. More specifically, we introduce an additional parameter to perfect the profile model under measurement, and use a robust estimation procedure at the end of each iteration of the Gauss–Newton (GN) method to obtain the more accurate parameter departure vector. By applying the proposed methods, more accurate reconstructed results can be achieved.

We conducted in-situhigh-temperature neutron and X-ray diffraction studies on tetragonal PbTiO3. Using a combination of Rietveld analysis and Maximum Entropy Method, the nuclear and charge density distributions were determined as a function of temperature up to 460 °C. The ionic states obtained from charge density distributions reveal that the covalency of Pb–O2bonds gradually weakens with increasing temperature. The spontaneous polarizations calculated from the contributions of ionic state, ionic displacement, and nuclear polarization, are in good agreement with the experimental measurements. This method provides an effective approach to determine spontaneous polarizations in multiferroics with high-current leakage and low resistance.

We report discovery of ferromagnetism in (LaCa)(ZnMn)SbO isostructural to the well-studied iron-based superconductor LaFeAs(O1−xFx). Spin is induced by partial substitution of Mn2+for Zn2+, while charge is induced by substitution of Ca2+for La3+within the parent compound LaZnSbO. Ferromagnetism with Curie temperature (TC) is observed up to 40 K at the spin doping 0.15 by introducing Mn2+into the Zn2+sites for (La0.95Ca0.05)(Zn1−xMnx)SbO. The Hall coefficient measurement indicates p-type carrier for (La0.95Ca0.05)(Zn0.9Mn0.1)SbO with concentration of n∼1020cm−3showing anomalous Hall effect below TC.

Cooperative Jahn–Teller (JT) distortion accompanied by electromagnetic lattice coupling plays a crucial role in numerous important phenomena in materials science. The JT distortion occurring in high-spin 3d4and 3d9configurations in octahedral complexes is common, but similarly, large distortion due to lifting the degeneracy of t2gorbitals has so far seldomly been observed. Here, we report the discovery of the pressure-induced cooperative JT effect coupled with a large volume collapse of ∼12.8% and a magnetic moment collapse from S= 5/2 to S= 1/2 at ∼20.9 GPa in MnTe. The first-principles calculation indicates that weakened p–d hybridization and enhanced d state localization result in lifting t2gorbital degeneracy in Mn2+(d5), which induced a cooperative JT effect-triggered electromagnetic lattice coupling. These findings suggest a new mechanism for the cooperative JT distortion via pressure-induced ligand distortion in antiferromagnetic materials.