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821.
Reaction mechanisms of the ultrafast photoisomerization between cyclohexadiene and hexatriene have been elucidated by the quantum dynamics on the ab initio potential energy surfaces calculated by multireference configuration interaction method. In addition to the quantum wave-packet dynamics along the two-dimensional reaction coordinates, the semiclassical analyses have also been carried out to correctly estimate the nonadiabatic transition probabilities around conical intersections in the full-dimensional space. The reaction time durations of radiationless decays in the wave-packet dynamics are found to be generally consistent with the femtosecond time-resolution experimental observations. The nonadiabatic transition probabilities among the ground (S0), first (S1), and second (S2) excited states have been estimated by using the semiclassical Zhu-Nakamura formula considering the full-dimensional wave-packet density distributions in the vicinity of conical intersections under the harmonic normal mode approximation. The cyclohexadiene (CHD) ring-opening process proceeds descending on the S1(1 1B) potential after the photoexcitation. The major part of the wave-packet decays from S1(1 1B) to S1(2 1A) by the first seam line crossing along the C2-symmetry-breaking directions. The experimentally observed ultrafast S1-S0 decay can be explained by the dynamics through the S1-S0 conical intersection along the direction toward the five-membered ring. The CHD: hexatriene (HT) branching ratio is estimated to be approximately 5:5, which is in accordance with the experiment in solution. This branching ratio is found to be mainly governed by the location of the five-membered ring S1-S0 conical intersection along the ground state potential ridge between CHD and HT. 相似文献
822.
Ito H Takegawa Y Deguchi K Nagai S Nakagawa H Shinohara Y Nishimura S 《Rapid communications in mass spectrometry : RCM》2006,20(23):3557-3565
Mass spectrometric analyses of various N-glycans binding to proteins and peptides are highly desirable for elucidating their biological roles. An approach based on collision-induced dissociation (CID) MS(n) spectra acquired by electrospray ionization linear ion trap time-of-flight mass spectrometry (ESI-LIT-TOFMS) in the positive- and negative-ion modes has been proposed as a direct method of assigning N-glycans without releasing them from N-glycopeptides. In the positive-ion mode of this approach, the MS(2) spectrum of N-glycopeptide was acquired so that a glycoside-bond cleavage occurs in the chitobiose residue (i.e., GlcNAcbeta1-4GlcNAc, GlcNAc: N-acetylglucosamine) attached to asparagine (N), and two charges on the [M+H+Na](2+) precursor ion are shared with both of the resulting fragments. These fragments are sodiated B(n)-type fragment ions of oligosaccharide (N-glycan) and a protonated peptide ion retaining one GlcNAc residue on the asparagine (N) residue. The structure of N-glycan was assigned by comparing MS(3) spectra derived from both the sodiated B(n)-type fragment ions of N-glycopeptide and the PA (2-aminopyridine) N-glycan standard (i.e., MS(n) spectral matching). In a similar manner, the structural assignment of sialylated N-glycan was performed by employing the negative-ion CID MS(n) spectra of deprotonated B(n)-type fragment ions of N-glycopeptide and the PA N-glycan standard. The efficacy of this approach was tested with chicken egg yolk glycopeptides with a neutral and a sialylated N-glycan, and human serum IgG glycopeptides with neutral N-glycan isomers. These results suggest that the approach based on MS(n) spectral matching is useful for the direct and simple structural assignment of neutral and sialylated N-glycans of glycopeptides. 相似文献
823.
Phelan D Louca D Kamazawa K Lee SH Ancona SN Rosenkranz S Motome Y Hundley MF Mitchell JF Moritomo Y 《Physical review letters》2006,97(23):235501
The perovskite LaCoO3 evolves from a nonmagnetic Mott insulator to a spin cluster ferromagnet (FM) with the substitution of Sr2+ for La3+ in La1-xSrxCoO3. The clusters increase in size and number with x and the charge percolation through the clusters leads to a metallic state. Using elastic neutron scattering on La1-xSrxCoO3 single crystals, we show that an incommensurate spin superstructure coexists with the FM spin clusters. The incommensurability increases continuously with x, with the intensity rising in the insulating phase and dropping in the metallic phase as it directly competes with the commensurate FM, itinerant clusters. The spin incommensurability arises from local order of Co3+-Co4+ clusters but no long-range static or dynamic spin stripes develop. The coexistence and competition of the two magnetic phases explain the residual resistivity at low temperatures in samples with metalliclike transport. 相似文献
824.
Hiroki Sasaki 《Algebras and Representation Theory》2010,13(4):445-465
Let k be an algebraically closed field of characteristic p. We shall discuss the cohomology algebras of a block ideal B of the group algebra kG of a finite group G and a block ideal C of the block ideal of kH of a subgroup H of G which are in Brauer correspondence and have a common defect group, continuing (Kawai and Sasaki, Algebr Represent Theory
9(5):497–511, 2006). We shall define a (B,C)-bimodule L. The k-dual L
* induces the transfer map between the Hochschild cohomology algebras of B and C, which restricts to the inclusion map of the cohomology algebras of B into that of C under some condition. Moreover the module L induces a kind of refinement of Green correspondence between indecomposable modules lying in the blocks B and C; the block varieties of modules lying in B and C which are in Green correspondence will also be discussed. 相似文献
825.
In this paper, we study the Jarque–Bera test for a class of univariate parametric stochastic differential equations (SDE) dX t = b(X t , α)dt + dZ t , constructed based on the sample observed at discrete time points \({t^{n}_{i}=ih_{n}}\) , i = 1, 2, . . . , n, where Z is a nondegenerate Lévy process with finite moments and h is a sequence of positive real numbers with nh n → ∞ and \({nh_{n}^{2} \to 0}\) as n → ∞. It is shown that under proper conditions, the Jarque–Bera test statistic based on the Euler residuals can be used to test for the normality of the unobserved Z and the proposed test is consistent against the presence of any nontrivial jump components. Our result indicates that the Jarque–Bera test is easy to implement and asymptotically distribution-free with no fine-tuning parameters. Simulation results to validate the test are given for illustration. 相似文献
826.
Thierry Giordano Hiroki Matui Ian F. Putnam Christian F. Skau 《Inventiones Mathematicae》2010,179(1):119-158
We show that every minimal action of any finitely generated abelian group on the Cantor set is (topologically) orbit equivalent to an AF relation. As a consequence, this extends the classification up to orbit equivalence of minimal dynamical systems on the Cantor set to include AF relations and ? d -actions. 相似文献
827.
Akira Ono Hiroki Kanazawa Hikari Ito Misato Goto Koudai Nakamura Hisao Saneyoshi Jiro Kondo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(47):16991-16994
Numerous applications of metal‐mediated base pairs (metallo‐base‐pairs) to nucleic acid based nanodevices and genetic code expansion have been extensively studied. Many of these metallo‐base‐pairs are formed in DNA and RNA duplexes containing Watson–Crick base pairs. Recently, a crystal structure of a metal–DNA nanowire with an uninterrupted one‐dimensional silver array was reported. We now report the crystal structure of a novel DNA helical wire containing HgII‐mediated T:T and T:G base pairs and water‐mediated C:C base pairs. The Hg‐DNA wire does not contain any Watson–Crick base pairs. Crystals of the Hg‐DNA wire, which is the first DNA wire structure driven by HgII ions, were obtained by mixing the short oligonucleotide d(TTTGC) and HgII ions. This study demonstrates the potential of metallo‐DNA to form various structural components that can be used for functional nanodevices. 相似文献
828.
Tatsuhiro Sakaiya Hidenori Terasaki Kosaku Akimoto Hiroki Kato Taichi Ueda Ryota Hosogi 《高压研究》2019,39(1):150-159
The Rayleigh–Taylor (RT) instability of liquid iron alloys is important for understanding the core formation mechanism in the Earth. Here we first report the measurement of RT instability growth for a liquid iron–silicon (Fe–Si) alloy, which is one of the major candidate for the material of the Earth’s core, using a high power laser. We optimized the measurement setup and analytical technique to observe the growth of perturbation on an Fe–Si sample surface. The growth of perturbation amplitude on the Fe–Si alloy under high pressure and temperature was successfully observed using in situ X-ray radiography. The growth rate of the RT instability for the Fe–Si alloy on about 1000?GPa was estimated to be 0.3 ns?1. 相似文献
829.
Takuya Morozumi Hideaki Okane Hiroki Sakamoto Yusuke Shimizu Kenta Takagi Hiroyuki Umeeda 《中国物理C(英文版)》2018,(2)
We discuss a supersymmetric model with discrete flavor symmetry A_4×Z_3. The additional scalar fields which contribute masses of leptons in the Yukawa terms are introduced in this model. We analyze their scalar potential and find that they have various vacuum structures. We show the relations among 24 different vacua and classify them into two types. We derive expressions of the lepton mixing angles, Dirac CP violating phase and Majorana phases for the two types. The model parameters which are allowed by the experimental data of the lepton mixing angles are different for each type. We also study the constraints on the model parameters which are related to Majorana phases. The different allowed regions of the model parameters for the two types are shown numerically for a given region of two combinations of the CP violating phases. 相似文献
830.
Takesue H 《Physical review letters》2008,101(17):173901
The frequency distinguishability of two single photons was successfully erased using single photon frequency up-conversion. A frequency nondegenerate photon pair generated via spontaneous four-wave mixing in a dispersion shifted fiber was used to emulate two telecom-band single photons that were in the same temporal mode but in different frequency modes. The frequencies of these photons were converted to the same frequency by using the sum-frequency generation process in periodically poled lithium niobate waveguides, while maintaining their temporal indistinguishability. As a result, the two converted photons exhibited a nonclassical dip in a Hong-Ou-Mandel quantum interference experiment. The present scheme will add flexibility to networking quantum information systems that use photons with various wavelengths. 相似文献