high pressure

高压
  • 文章类型: Journal Article
    红藻紫菜,俗称Nori,由于其高营养成分,在世界各地被广泛用作食品,包括大量的彩色藻胆蛋白(PBPs)。其中,R-藻蓝蛋白(R-PC)因其鲜艳的紫色和众多生物活性而脱颖而出,使其成为食品工业的有价值的蛋白质。然而,R-PC有限的热稳定性需要替代加工方法来保持其颜色和生物活性。我们的研究旨在研究低聚R-PC在高压(HP)条件下(高达4000bar)的原位稳定性,荧光,和小角度X射线散射(SAXS)技术。R-PC的展开是多相过程。最初,低压诱导R-PC寡聚形式(三聚体)的构象变化。当压力增加到1600巴以上时,这些三聚体解离成单体,在3000巴以上的压力下,子单元开始展开。当恢复到大气压力时,R-PC部分折叠,保留其原始颜色吸光度的50%。相比之下,热处理会对R-PC颜色产生不可逆和有害的影响,与热处理相比,强调了HP处理在保持R-PC的颜色和生物活性方面的优势。
    The red macroalgae Porphyra, commonly known as Nori, is widely used as food around the world due to its high nutrient content, including the significant abundance of colored phycobiliproteins (PBPs). Among these, R-phycocyanin (R-PC) stands out for its vibrant purple color and numerous bioactive properties, making it a valuable protein for the food industry. However, R-PC\'s limited thermal stability necessitates alternative processing methods to preserve its color and bioactive properties. Our study aimed to investigate the in-situ stability of oligomeric R-PC under high pressure (HP) conditions (up to 4000 bar) using a combination of absorption, fluorescence, and small-angle X-ray scattering (SAXS) techniques. The unfolding of R-PC is a multiphase process. Initially, low pressure induces conformational changes in the R-PC oligomeric form (trimers). As pressure increases above 1600 bar, these trimers dissociate into monomers, and at pressures above 3000 bar, the subunits begin to unfold. When returned to atmospheric pressure, R-PC partially refolds, retaining 50% of its original color absorbance. In contrast, heat treatment causes irreversible and detrimental effects on R-PC color, highlighting the advantages of HP treatment in preserving both the color and bioactive properties of R-PC compared to heat treatment.
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  • 文章类型: Journal Article
    由于辐射途径竞争,同时增强自由激子(FE)发射和自陷激子(STE)发射仍然具有极大的挑战性。这里,显著的荧光改善,与FEs和STEs的辐射复合相关的首先是在非常规ACI型杂化钙钛矿中实现的,具有{PbI6}八面体单元的(ACA)(MA)PbI4(ACA=乙脒)晶体,通过静水压力处理。请注意,(ACA)(MA)PbI4在1atm至2.5GPa的温和压力间隔内表现出91.5倍的发射增强和从绿色到红色的显着压色性。在高压下,单个卤化物八面体的实质性畸变和两个卤化物八面体之间的Pb-I-Pb角确实决定了压力调节的局部激子行为。在更高的压力下,还观察到光电流增强,这归因于(ACA)(MA)PbI4中促进的电子连通性。各向异性压缩减少了相邻有机分子和{PbI6}八面体之间的距离,导致氢键相互作用的增强。这项工作不仅提供了对ACI型钙钛矿的结构-光学关系的深刻理解,但也提出了通过压力抑制非辐射复合来打破发光效率极限的见解。
    Simultaneous enhancement of free excitons (FEs) emission and self-trapped excitons (STEs) emission remains greatly challenging because of the radiative pathway competition. Here, a significant fluorescence improvement, associated with the radiative recombination of both FEs and STEs is firstly achieved in an unconventional ACI-type hybrid perovskite, (ACA)(MA)PbI4 (ACA=acetamidinium) crystals with {PbI6} octahedron units, through hydrostatic pressure processing. Note that (ACA)(MA)PbI4 exhibits a 91.5-fold emission enhancement and considerable piezochromism from green to red in a mild pressure interval of 1 atm to 2.5 GPa. The substantial distortion of both individual halide octahedron and the Pb-I-Pb angles between two halide octahedra under high pressure indeed determines the pressure-tuning localized excitons behavior. Upon higher pressure, photocurrent enhancement is also observed, which is attributed to the promoted electronic connectivity in (ACA)(MA)PbI4. The anisotropic compaction reduces the distance between neighboring organic molecules and {PbI6} octahedra, leading to the enhancement of hydrogen bonding interactions. This work not only offers a deep understanding of the structure-optical relationships of ACI-type perovskites, but also presents insights into breaking the limits of luminescent efficiency by pressure-suppressed nonradiative recombination.
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  • 文章类型: Journal Article
    我们开发了一种HPLC系统,其中相分离多相流在分离柱中作为洗脱液工作。我们将新型分离机制称为相分离模式。水/乙腈/乙酸乙酯三元混合溶液,这是两相分离混合溶液之一,通过温度效应(从20到0°C)从均质到非均质的相变引起相分离多相流。在这项研究中,我们试图用压力效应代替温度效应进行相分离多相流。将熔融石英毛细管(长度为50厘米,内径为50μm)与色谱柱的下游相连,以对系统施加5.5MPa的压力。研究了2,6-萘二磺酸(2,6-NDS)和1-萘酚(1-NA)的模型分析物。例如,溶液(体积%的水/乙腈/乙酸乙酯;20:55:25,富含有机物)和(60:30:10,富含水)用作洗脱剂。在1.5MPa和20°C的压力下用两种溶液不分离模型分析物。但是有了富含有机物的溶液,1-NA和2,6-NDS按此顺序分离,并与富含水的溶液,它们在5.5MPa和20°C的压力下以相反的顺序分离。相分离模式可以在高压下甚至在室温下进行。
    We have developed a HPLC system where phase-separation multiphase flow works in the separation column as an eluent. We call the novel separation mechanism a phase-separation mode. The ternary mixed solution of water/acetonitrile/ethyl acetate, which is one of the two-phase-separation mixed solutions, caused the phase-separation multiphase flow via phase change from homogeneous to heterogeneous with the temperature effect (from 20 to 0 °C). In this study, we tried to perform phase-separation multiphase flow with the pressure effect instead of the temperature one. The fused-silica capillary tube (50 cm length and 50 µm inner diameter) was allied to the downstream of the column to apply the pressure of 5.5 MPa to the system. Model analytes of 2,6-naphthalenedisulfonic acid (2,6-NDS) and 1-naphthol (1-NA) were examined. For example, solutions (the volume% of water/acetonitrile/ethyl acetate; 20:55:25, organic-rich) and (60:30:10, water-rich) were used as eluent. The model analytes were not separated with both solutions at the pressure of 1.5 MPa and 20 °C. But with the organic-rich solution, 1-NA and 2,6-NDS were separated in this order and with the water-rich solution, they were separated in the reverse order at the pressure of 5.5 MPa and 20 °C. The phase-separation mode could be performed at the high pressure even at the room temperature.
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  • 文章类型: Journal Article
    从了解地壳和俯冲带Na辅助碳循环的地球化学过程的角度出发,研究高P-T条件下Na碳酸盐稳定性及其在含水碳酸盐流体中的转化是相关的。在高P-T条件下对金刚石砧室(DAC)中含Na的碳酸盐-水-Fe-金属系统的原位拉曼研究表明,碳酸盐分解时会形成甲酸盐和其他有机化合物,这与碳酸盐在干燥中的行为不同系统。另外使用XRD和FTIR方法来确定相组成。含水流体中的含钠碳酸盐(NahcoliteNaHCO3,短铁矿Na2Ca2(CO3)3和松质岩Na7Ca[(CO3)1.5Al6Si6O24]·2H2O)在中等P-T参数下分解形成简单的碳酸盐和甲酸盐(作为主要的有机分子)(高于0.2GPa,200°C)。我们的实验结果直接证实了Horita和Berndt(Science,1999)关于碳酸盐-水-金属体系中有机甲酸酯的可能产率。在Fe金属存在的情况下,水性流体中的NahcoliteNaHCO3分解为无水相:natriteγ-Na2CO3,菱铁矿,磁铁矿(由于Fe钢垫片的溶解),甲酸钠和可能的甲酸钠和甲酸甲酯的有机分子结晶溶剂化物。短铁矿衰变为无水相:文石CaCO3,Na-Ca-甲酸盐和无定形相。Cancrinite分解为未识别的碳酸盐-铝硅酸盐相,Na-Ca-甲酸盐和未知的有机分子晶体。由于DAC中使用的Fe钢垫片的溶解,该系统中还形成了磁铁矿。本研究为地壳和上地幔中碳酸盐对有机物的非生物形成过程提供了新的见解。
    The study of Na-carbonates stability and their transformations in aqueous carbonate fluid under high P-T conditions is relevant from the point of view of the understanding geochemical processes of the Na-assisted carbon circulation in the Earth\'s crust and subduction zones. In situ Raman study of Na-bearing carbonate-water-Fe-metal system in diamond anvil cell (DAC) at high P-T conditions revealed that carbonates decompose with abiogenic formation of formates and other organic compounds that differs from behavior of carbonates in dry system. XRD and FTIR methods have been used additionally to determine the phase composition. Na-bearing carbonates (nahcolite NaHCO3, shortite Na2Ca2(CO3)3 and cancrinite Na7Ca[(CO3)1.5Al6Si6O24]⋅2H2O) in aqueous fluid decompose to form simple carbonates and formates (as dominant organic molecules) at moderate P-T parameters (above ∼0.2 GPa, 200 °C). Our experimental results directly confirm the hypothesis of Horita and Berndt (Science, 1999) about possible yield of organic formates in the carbonate-water-metal system. Nahcolite NaHCO3 in aqueous fluid in the presence of Fe metal decomposes into anhydrous phases: natrite γ-Na2CO3, siderite, magnetite (due to dissolution of Fe steel gasket), Na-formate and likely organic molecular crystalline solvate of Na-formate and methyl formate. Shortite decays into anhydrous phases: aragonite CaCO3, Na-Ca-formates and an amorphous phase. Cancrinite decomposes to unidentified carbonate-alumonosilicate phases, Na-Ca-formates and unknown organic molecular crystal. Magnetite is also formed in this system due to dissolution of Fe steel gasket used in DAC. The present study provides a new insight in processes of abiogenic formation of organic matter from carbonates in the crust and upper mantle.
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  • 文章类型: Journal Article
    在室温(RT)下实现超导性是物理学中的圣杯。关于高压下二元氢化物H3S和LaH10的高Tc超导性的最新发现已指导寻找RT超导体以常规电子-声子机制压缩氢化物。这里,在高压下预测了一个特殊的超氢化物家族,MH12(M=Mg,Sc,Zr,Hf,Lu),所有都表现出RT超导性,计算出的Tcs范围为313至398K。与H3S和LaH10相反,MH12中的氢亚晶格排列为准原子H2单元。这种独特的配置与高Tc密切相关,归因于费米能级上H2反键合态的高电子密度以及与H2和H-M-H的弯曲振动有关的强电子-声子耦合。值得注意的是,MgH12和ScH12即使在低于100GPa的压力下也保持动态稳定。这些发现为实现RT超导性提供了重要见解,并为实验研究的创新方向铺平了道路。
    Achieving superconductivity at room temperature (RT) is a holy grail in physics. Recent discoveries on high-Tc superconductivity in binary hydrides H3S and LaH10 at high pressure have directed the search for RT superconductors to compress hydrides with conventional electron-phonon mechanisms. Here, an exceptional family of superhydrides is predicated under high pressures, MH12 (M = Mg, Sc, Zr, Hf, Lu), all exhibiting RT superconductivity with calculated Tcs ranging from 313 to 398 K. In contrast to H3S and LaH10, the hydrogen sublattice in MH12 is arranged as quasi-atomic H2 units. This unique configuration is closely associated with high Tc, attributed to the high electronic density of states derived from H2 antibonding states at the Fermi level and the strong electron-phonon coupling related to the bending vibration of H2 and H-M-H. Notably, MgH12 and ScH12 remain dynamically stable even at pressure below 100 GPa. The findings offer crucial insights into achieving RT superconductivity and pave the way for innovative directions in experimental research.
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  • 文章类型: Journal Article
    过渡金属二硫属TiSe2在2-4GPa的低压范围内表现出超导圆顶,其峰值的最大转变温度Tc为≈1.8K。据报道,施加高压会在TiSe2中引起新的超导状态,该状态从≈16GPa开始,Tc高得多,在≈21.5GPa时达到5.6K,没有下降的迹象。结合高通量第一原理结构搜索,X射线衍射,和高达30GPa的拉曼光谱测量,发现TiSe2经历了从环境压力下的1T相到高压下新的4O相的一阶结构转变。从头算的比较计算表明,尽管常规的声子介导的配对机制可以解释在低压下在1T-TiSe2中观察到的超导性,4O-TiSe2的电子-声子耦合太弱,无法在高压下诱导转变温度高达5.6K的超导状态。在加压TiSe2中发现的新超导状态需要进一步研究其潜在机理。
    Transition metal dichalcogenide TiSe2 exhibits a superconducting dome within a low pressure range of 2-4 GPa, which peaks with the maximal transition temperature Tc of ≈1.8 K. Here it is reported that applying high pressure induces a new superconducting state in TiSe2, which starts at ≈16 GPa with a substantially higher Tc that reaches 5.6 K at ≈21.5 GPa with no sign of decline. Combining high-throughput first-principles structure search, X-ray diffraction, and Raman spectroscopy measurements up to 30 GPa, It is found that TiSe2 undergoes a first-order structural transition from the 1T phase under ambient pressure to a new 4O phase under high pressure. Comparative ab initio calculations reveal that while the conventional phonon-mediated pairing mechanism may account for the superconductivity observed in 1T-TiSe2 under low pressure, the electron-phonon coupling of 4O-TiSe2 is too weak to induce a superconducting state whose transition temperature is as high as 5.6 K under high pressure. The new superconducting state found in pressurized TiSe2 requires further study on its underlying mechanism.
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  • 文章类型: Journal Article
    PdSe2是一种起皱的过渡金属二硫属化物,据报道在压力下经历二维到三维的结构转变。这里,我们使用泵浦探针光谱法研究了高压下PdSe2的电子和声子演化。我们观察到Pd的d轨道中发生的电子带内和带间跃迁,揭示了高压下Jahn-Teller效应的消失。此外,我们发现带间重组和带内弛豫寿命的衰减速率在3和7GPa变化,分别。第一性原理计算表明,带隙闭合减慢了3GPa后带间复合的衰减速率,声子-声子散射的饱和是相对恒定的带内弛豫寿命的主要原因。我们的工作为理解压力下声子对电子的演化和载流子动力学的调制提供了新的视角。
    PdSe2 is a puckered transition metal dichalcogenide that has been reported to undergo a two-dimensional to three-dimensional structural transition under pressure. Here, we investigated the electronic and phononic evolution of PdSe2 under high pressure using pump-probe spectroscopy. We observed the electronic intraband and interband transitions occurring in the d orbitals of Pd, revealing the disappearance of the Jahn-Teller effect under high pressure. Furthermore, we found that the decay rates of interband recombination and intraband relaxation lifetimes change at 3 and 7 GPa, respectively. First-principles calculations suggest that the bandgap closure slows the decay rate of interband recombination after 3 GPa, while the saturation of phonon-phonon scattering is the main reason for the relatively constant intraband relaxation lifetime. Our work provides a novel perspective for understanding the evolution of the electron and modulation of the carrier dynamics by phonons under pressure.
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  • 文章类型: Journal Article
    通过单晶X射线衍射和拉曼光谱研究了黄原酸锂水合物在冷却至100K和压缩至5.3GPa时的晶体结构。观察到4GPa的相变。冷却时不发生相变。比较了晶格应变的各向异性和分子间相互作用的变化。
    The crystal structure of lithium xanthinate hydrate was studied by single crystal X-ray diffraction and Raman spectroscopy on cooling to 100 K and under compression to 5.3 GPa. A phase transition at ∼4 GPa is observed. No phase transitions occur on cooling. Anisotropy of lattice strain and changes in intermolecular interactions are compared.
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  • 文章类型: Journal Article
    高压既是深海生物学必须适应的环境挑战,和高度敏感的热力学工具,可用于触发生物分子和组件的结构变化。脂膜是最压敏的生物组件之一,压力可能对其结构和性能产生很大影响。在这一章中,我们将探索使用高压小角X射线衍射和高压显微镜来测量和量化在平衡高压条件下和响应压力跳跃的脂质膜横向结构的变化。
    High pressure is both an environmental challenge to which deep sea biology has to adapt, and a highly sensitive thermodynamic tool that can be used to trigger structural changes in biological molecules and assemblies. Lipid membranes are amongst the most pressure sensitive biological assemblies and pressure can have a large influence on their structure and properties. In this chapter, we will explore the use of high pressure small angle X-ray diffraction and high pressure microscopy to measure and quantify changes in the lateral structure of lipid membranes under both equilibrium high pressure conditions and in response to pressure jumps.
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  • 文章类型: Journal Article
    2D范德华(vdW)磁体最近已成为自旋电子器件创新的有前途的材料系统,因为它们在尺寸减小和磁性异质结构简单集成方面具有有趣的现象,而不受晶格匹配的限制。然而,对于二维vdW磁性材料中的自旋电子学应用,实现远高于室温的居里温度和可控的磁各向异性仍然具有挑战性。在这项工作中,报道了铁基2D层状铁磁体Fe3GaTe2中的压力调谐圆顶状铁磁-顺磁相图。通过施加压力实现从平面外到平面内方向的连续可调磁各向异性。这种行为归因于层内和层间交换相互作用之间的竞争以及费米能级附近的DOS增强。该研究提出了压力工程二维铁磁材料的突出特性,可用于下一代自旋电子器件。
    2D van der Waals (vdW) magnets have recently emerged as a promising material system for spintronic device innovations due to their intriguing phenomena in the reduced dimension and simple integration of magnetic heterostructures without the restriction of lattice matching. However, it is still challenging to realize Curie temperature far above room temperature and controllable magnetic anisotropy for spintronics application in 2D vdW magnetic materials. In this work, the pressure-tuned dome-like ferromagnetic-paramagnetic phase diagram in an iron-based 2D layered ferromagnet Fe3GaTe2 is reported. Continuously tunable magnetic anisotropy from out-of-plane to in-plane direction is achieved via the application of pressure. Such behavior is attributed to the competition between intralayer and interlayer exchange interactions and enhanced DOS near the Fermi level. The study presents the prominent properties of pressure-engineered 2D ferromagnetic materials, which can be used in the next-generation spintronic devices.
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