131 research outputs found
Роль маркетинга в сфере культуры
Сегодня все мы ощущаем завершение очередного этапа развития нашего общества, который выражается в многочисленных кризисах (политическом, экономическом, экологическом и т.д.), что в полной мере
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Introduction: Deep carbon cycle through five reactions
What are the key reactions driving the global carbon cycle in Earth, the only known habitable planet in the Solar System? And how do chemical reactions govern the transformation and movement of carbon? The special collection “Earth in Five Reactions: A Deep Carbon Perspective” features review articles synthesizing knowledge and findings on the role of carbon-related reactions in Earth's dynamics and evolution. These integrative studies identify gaps in our current understanding and establish new frontiers to motivate and guide future research in deep carbon science. The collection also includes original experimental and theoretical investigations of carbon-bearing phases and the impact of chemical and polymorphic reactions on Earth's deep carbon cycle
Tuning the nonlinear optical absorption of reduced graphene oxide by chemical reduction
Reduced graphene oxides with varying degrees of reduction have been produced by hydrazine reduction of graphene oxide. The linear and nonlinear optical properties of both graphene oxide as well as the reduced graphene oxides have been measured by single beam Z-scan measurement in the picosecond region. The results reveal both saturable absorption and two-photon absorption, strongly dependent on the intensity of the pump pulse: saturable absorption occurs at lower pump pulse intensity (~1.5 GW/cm2 saturation intensity) whereas two-photon absorption dominates at higher intensities (≥5.7 GW/cm2). Intriguingly, we find that the two-photon absorption coefficient (from 1.5 cm/GW to 4.5cm/GW) and the saturation intensity (from 1 GW/cm2 to 2 GW/cm2) vary with chemical reduction, which is ascribed to the varying concentrations of sp2 domains and sp2 clusters in the reduced graphene oxides. Our results not only provide an insight into the evolution of the nonlinear optical coefficient in reduced graphene oxide, but also suggest that chemical engineering techniques may usefully be applied to tune the nonlinear optical properties of various nano-materials, including atomically thick graphene sheets
Pressure-induced structural modulations in coesite
Silica phases, SiO2, have attracted significant attention as important phases in the fields of condensed-matter physics, materials science, and (in view of their abundance in the Earth's crust) geoscience. Here, we experimentally and theoretically demonstrate that coesite undergoes structural modulations under high pressure. Coesite transforms to a distorted modulated structure, coesite-II, at 22–25 GPa with modulation wave vector q=0.5b∗. Coesite-II displays further commensurate modulation along the y axis at 36–40 GPa and the long-range ordered crystalline structure collapses beyond ∼40GPa and starts amorphizing. First-principles calculations illuminate the nature of the modulated phase transitions of coesite and elucidate the modulated structures of coesite caused by modulations along the y-axis direction. The structural modulations are demonstrated to result from phonon instability, preceding pressured-induced amorphization. The recovered sample after decompression develops a rim of crystalline coesite structure, but its interior remains low crystalline or partially amorphous. Our results not only clarify that the pressure-induced reversible phase transitions and amorphization in coesite originate from structural modulations along the y-axis direction, but also shed light on the densification mechanism of silica under high pressure
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Thermal Behavior of Iron Arsenides Under Non-Oxidizing Conditions.
Fe2As has been studied in situ by synchrotron powder X-ray diffraction (PXRD) over the range of temperatures 25-850 °C and under a neutral atmosphere to understand its thermal behavior, which is potentially important for gold extraction. For the first time, incongruent high-temperature reactions of Fe2As are observed as it breaks down and the existence of a previously undiscovered high-temperature FeAs phase with an NiAs-type structure has been determined experimentally. No evidence has been found for the existence of the high-temperature Fe3As2 phase. Hence, the previously published phase diagram for the Fe-As system has to be modified accordingly
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Thermal behaviour of iron arsenides under non-oxidising conditions
Fe2As has been studied in situ by synchrotron powder X-ray diffraction (PXRD) over the range of temperatures 25–850 °C and under a neutral atmosphere to understand its thermal behavior, which is potentially important for gold extraction. For the first time, incongruent high-temperature reactions of Fe2As are observed as it breaks down and the existence of a previously undiscovered high-temperature FeAs phase with an NiAs-type structure has been determined experimentally. No evidence has been found for the existence of the high-temperature Fe3As2 phase. Hence, the previously published phase diagram for the Fe–As system has to be modified accordingly
Carbon network evolution from dimers to sheets in superconducting ytrrium dicarbide under pressure
Carbon-bearing compounds display intriguing structural diversity, due to variations in hybrid bonding of carbon. Here, first-principles calculations and unbiased structure searches on yttrium dicarbide at pressure reveal four new structures with varying carbon polymerisation, in addition to the experimentally observed high-temperature low-pressure I4/mmm dimer phase. At low pressures, a metallic C2/m phase (four-member single-chain carbide) is stable, which transforms into a Pnma phase (single-chain carbide) upon increasing pressure, with further transformation to an Immm structure (double-chain carbide) at 54 GPa and then to a P6/mmm phase (sheet carbide) at 267 GPa. Yttrium dicarbide is structurally diverse, with carbon bonded as dimers (at lowest pressure), four-member single chains, infinite single chains, double chains and eventually sheet structures on compression. Electron–phonon coupling calculations indicate that the high-pressure phases are superconducting. Our results aid the understanding and design of new superconductors and illuminate pressure-induced carbon polymerisation in carbides
Phase Transitions in Zeolitic Imidazolate Framework 7: The Importance of Framework Flexibility and Guest-Induced Instability
A study of the phase transitions in ZIF-7 (zeolitic imidazolate frameworks- (Zn(PhIm)2, PhIm = benzimidazolate)) as a function of guest occupancy and temperature was reported. Raman spectra of an as-synthesized sample were collected in air between 297 and 421 K. The major contributions of the spectra come from the vibrational modes of the benzimidazolate ligand. Upon heating, most of the Raman bands remain similar and keep the same frequencies until 357 K, indicating that the structure of ZIF-7 seems to be stable in this temperature range. Above 357 K, strong modifications are observed in the regions corresponding to the lattice modes. The formation of ZIF-7-II is attributed to the loss of dimethylformamide (DMF) solvent molecules from the ZIF-7-I framework. This can be confirmed by the differential scanning calorimetry and thermogravimetric analysis traces of ZIF-7-I. The highly-distorted and locally-strained nature of ZIF-7-II leads to its poor crystallinity, reflected by X-ray powder diffraction and scanning electron microscope
A scaling law for distinct electrocaloric cooling performance in low-dimensional organic, relaxor and anti-ferroelectrics
Electrocaloric (EC) materials show promise in eco-friendly solid-state refrigeration and integrable on-chip thermal management. While direct measurement of EC thin-films still remains challenging, a generic theoretical framework for quantifying the cooling properties of rich EC materials including normal-, relaxor-, organic- and anti-ferroelectrics is imperative for exploiting new flexible and room-temperature cooling alternatives. Here, we present a versatile theory that combines Master equation with Maxwell relations and analytically relates the macroscopic cooling responses in EC materials with the intrinsic diffuseness of phase transitions and correlation characteristics. Under increased electric fields, both EC entropy and adiabatic temperature changes increase quadratically initially, followed by further linear growth and eventual gradual saturation. The upper bound of entropy change (∆Smax) is limited by distinct correlation volumes (V cr ) and transition diffuseness. The linearity between V cr and the transition diffuseness is emphasized, while ∆Smax = 300 kJ/(K.m3) is obtained for Pb0.8Ba0.2ZrO3. The ∆Smax in antiferroelectric Pb0.95Zr0.05TiO3, Pb0.8Ba0.2ZrO3 and polymeric ferroelectrics scales proportionally with V cr −2.2, owing to the one-dimensional structural constraint on lattice-scale depolarization dynamics; whereas ∆Smax in relaxor and normal ferroelectrics scales as ∆Smax ~ V cr −0.37, which tallies with a dipolar interaction exponent of 2/3 in EC materials and the well-proven fractional dimensionality of 2.5 for ferroelectric domain walls
Water incorporation in synthetic and natural MgAl2O4 spinel
The solubility and incorporation mechanisms of water in synthetic and natural MgAl2O4 spinel have been investigated in a series of high-pressure/temperature annealing experiments. In contrast to most other nominally anhydrous minerals, natural spinel appears to be completely anhydrous. On the other hand, non-stoichiometric Al-rich synthetic (defect) spinel can accommodate several hundred ppm water in the form of structurally-incorporated hydrogen. Infrared (IR) spectra of hydrated defect spinel contain one main O-H stretching band at 3343-3352 cm-1 and a doublet consisting of two distinct O-H bands at 3505-3517 cm-1 and 3557-3566 cm-1. IR spectra and structural refinements based on single-crystal X-ray data are consistent with hydrogen incorporation in defect spinel onto both octahedral and tetrahedral O-O edges. Fine structure of O-H bands in IR spectra can be explained by partial coupling of interstitial hydrogen with cation vacancies, or by the effects of Mg-Al disorder on the tetrahedral site. The concentration of cation vacancies in defect spinel is a major control on hydrogen affinity. The commercial availability of large single crystals of defect spinel coupled with high water solubility and similarities in water incorporation mechanisms between hydrous defect spinel and hydrous ringwoodite (Mg2SiO4) suggests that synthetic defect spinel may be a useful low-pressure analogue material for investigating the causes and consequences of water incorporation in the lower part of Earth's mantle transition zone
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