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Huynh A Lanzillotti-Kimura ND Jusserand B Perrin B Fainstein A Pascual-Winter MF Peronne E Lemaître A 《Physical review letters》2006,97(11):115502
We report a direct determination of the dynamic behavior of confined acoustic phonons in nanocavities by picosecond acoustics. We provide the broadband, high resolution transmission amplitude curve in the subterahertz range, and we give evidence of resonant transmission peaks in three successive stop bands, in quantitative agreement with acoustic simulations. We furthermore demonstrate transit times in the nanosecond range at the cavity peaks reflecting the strong confinement of resonant phonons within the cavity layer. On the other hand, picosecond transit times are measured in the stop band, shorter than in any of the constituting materials, a tunneling effect well known both in photonic crystals and in macroscopic phononic systems. 相似文献
84.
Huynh Le Thanh Nguyen Tran Thi Thuy Dung Nguyen Hoang Hai Au Nguyen Thi Thu Trang Tran Van Man Grag Akhil Le My Loan Phung 《Journal of Solid State Electrochemistry》2018,22(7):2247-2254
Journal of Solid State Electrochemistry - Olivine LiFePO4 (LFP) is a promising cathode material for high-rated lithium-ion batteries. However, olivine faced a severe disadvantage of low... 相似文献
85.
Dennis R Livesay Dang H Huynh Sargis Dallakyan Donald J Jacobs 《Chemistry Central journal》2008,2(1):1-20
Background
Gram-negative bacteria use periplasmic-binding proteins (bPBP) to transport nutrients through the periplasm. Despite immense diversity within the recognized substrates, all members of the family share a common fold that includes two domains that are separated by a conserved hinge. The hinge allows the protein to cycle between open (apo) and closed (ligated) conformations. Conformational changes within the proteins depend on a complex interplay of mechanical and thermodynamic response, which is manifested as an increase in thermal stability and decrease of flexibility upon ligand binding.Results
We use a distance constraint model (DCM) to quantify the give and take between thermodynamic stability and mechanical flexibility across the bPBP family. Quantitative stability/flexibility relationships (QSFR) are readily evaluated because the DCM links mechanical and thermodynamic properties. We have previously demonstrated that QSFR is moderately conserved across a mesophilic/thermophilic RNase H pair, whereas the observed variance indicated that different enthalpy-entropy mechanisms allow similar mechanical response at their respective melting temperatures. Our predictions of heat capacity and free energy show marked diversity across the bPBP family. While backbone flexibility metrics are mostly conserved, cooperativity correlation (long-range couplings) also demonstrate considerable amount of variation. Upon ligand removal, heat capacity, melting point, and mechanical rigidity are, as expected, lowered. Nevertheless, significant differences are found in molecular cooperativity correlations that can be explained by the detailed nature of the hydrogen bond network.Conclusion
Non-trivial mechanical and thermodynamic variation across the family is explained by differences within the underlying H-bond networks. The mechanism is simple; variation within the H-bond networks result in altered mechanical linkage properties that directly affect intrinsic flexibility. Moreover, varying numbers of H-bonds and their strengths control the likelihood for energetic fluctuations as H-bonds break and reform, thus directly affecting thermodynamic properties. Consequently, these results demonstrate how unexpected large differences, especially within cooperativity correlation, emerge from subtle differences within the underlying H-bond network. This inference is consistent with well-known results that show allosteric response within a family generally varies significantly. Identifying the hydrogen bond network as a critical determining factor for these large variances may lead to new methods that can predict such effects. 相似文献86.
In this paper we report on the kinetics of hydrogen abstraction for the OH + alkene reaction class, using the reaction class transition state theory (RC-TST) combined with the linear energy relationship (LER) and the barrier height grouping (BHG) approaches. Parameters for the RC-TST were derived from theoretical calculations using a set of 15 reactions representing the hydrogen abstractions from the terminal and nonterminal carbon sites of the double bond of alkene compounds. Both the RC-TST/LER, where only reaction energy is needed at either density functional theory BH&HLYP or semiempirical AM1 levels, and RC-TST/BHG, where no additional information is required, are found to be promising methods for predicting rate constants for a large number of reactions in this reaction class. Detailed error analyses show that, when compared to explicit theoretical calculations, the averaged systematic errors in the calculated rate constants using both the RC-TST/LER and RC-TST/BHG methods are less than 25% in the temperature range 300-3000 K. The estimated rate constants using these approaches are in good agreement with available data in the literature. 相似文献
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Swarbhanu Sarkar Yeong Su Ha Nisarg Soni Gwang Il An Woonghee Lee Min Hwan Kim Phuong Tu Huynh Heesu Ahn Nikunj Bhatt Yong Jin Lee Jung Young Kim Kwon Moo Park Isao Ishii Shin‐Geol Kang Jeongsoo Yoo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2016,128(32):9511-9516
Hydrogen sulfide (H2S) has multifunctional roles as a gas signaling molecule in living systems. However, the efficient detection and imaging of H2S in live animals is very challenging. Herein, we report the first radioisotope‐based immobilization technique for the detection, quantification, and in vivo imaging of endogenous H2S. Macrocyclic 64Cu complexes that instantly reacted with gaseous H2S to form insoluble 64CuS in a highly sensitive and selective manner were prepared. The H2S concentration in biological samples was measured by a thin‐layer radiochromatography method. When 64Cu–cyclen was injected into mice, an elevated H2S concentration in the inflamed paw was clearly visualized and quantified by Cerenkov luminescence and positron emission tomography (PET) imaging. PET imaging was also able to pinpoint increased H2S levels in a millimeter‐sized infarcted lesion of the rat heart. 相似文献
89.
All higher life forms use oxygen and respiration as their primary energy source. The oxygen comes from water by solar-energy conversion in photosynthetic membranes. In green plants, light absorption in photosystem II (PSII) drives electron-transfer activation of the oxygen-evolving complex (OEC). The mechanism of water oxidation by the OEC has long been a subject of great interest to biologists and chemists. With the availability of new molecular-level protein structures from X-ray crystallography and EXAFS, as well as the accumulated results from numerous experiments and theoretical studies, it is possible to suggest how water may be oxidized at the OEC. An integrated sequence of light-driven reactions that exploit coupled electron-proton transfer (EPT) could be the key to water oxidation. When these reactions are combined with long-range proton transfer (by sequential local proton transfers), it may be possible to view the OEC as an intricate structure that is "wired for protons". 相似文献
90.