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91.
    
A synthetic strategy to construct large geodesic structures of phenine (1,3,5‐trisubstituted benzene) was devised. In this strategy, five pentagons were assembled on an omphalos pentagon, and bridging peripheral pentagons furnished five additional hexagons. Thirty phenine units were synthetically assembled to afford a large C220H180 molecule with a phenine framework isoreticular to a hemispherical, bisected segment of C60. Although a hemispherical structure of the phenine framework was suggested by solution‐phase NMR spectra, crystallographic analysis revealed an oval‐like deformation of the molecular shape. In‐depth structural analyses, including theoretical calculations, showed that structural fluctuations observed as variations in the biaryl torsion angles allowed structural deformations and, at the same time, that the dynamic fluctuations resulted in the spectroscopic observation of a hemisphere as a time‐averaged structure.  相似文献   
92.
We introduce a way to selectively probe local vibration modes at nanostructured asperities such as tips of carbon nanohorns. Our observations benefit from signal amplification in surface-enhanced Raman scattering (SERS) at sites near a silver surface. We observe nanohorn tip vibration modes in the range 200-500 cm(-1), which are obscured in regular Raman spectra. Ab initio density functional calculations assign modes in this frequency range to local vibrations at the nanohorn cap resembling the radial breathing mode of fullerenes. Careful interpretation of our SERS spectra indicates presence of caps with 5 or 6 pentagons, which are chemically the most active sites. Changes in the peak intensities and frequencies with time indicate that exposure to laser irradiation may cause structural rearrangements at the cap.  相似文献   
93.
    
Organic structure-directing agents (OSDAs) are often employed for synthesis of zeolites with desired frameworks. A priori prediction of such OSDAs has mainly relied on the interaction energies between OSDAs and zeolite frameworks, without cost considerations. For practical purposes, the cost of OSDAs becomes a critical issue. Therefore, the development of a computational de novo prediction methodology that can speed up the trial-and-error cycle in the search for less expensive OSDAs is desired. This study utilized a nature-inspired ant colony optimization method to predict physicochemically and/or economically preferable OSDAs, while also taking molecular similarity and heuristics of zeolite synthesis into consideration. The prediction results included experimentally known OSDAs, candidates having structures closely related to known OSDAs, and novel ones, suggesting the applicability of this approach.

Inspired by the exploratory methods of ant colonies, adaptive optimization was employed to explore the chemical space for organic molecules that guide zeolite crystallization, giving both physicochemically and economically promising molecules.  相似文献   
94.
In this paper we review studies on spin-dependent transport in systems containing ferromagnetic nanoparticles. In a tunnel junction with a nanometer-scale-island, the charging effect leads to an electric current blockade phenomenon in which a single electron charge plays a significant role in electron transport, resulting in single-electron tunneling (SET) properties such as Coulomb blockade and Coulomb staircase. In a tunnel junction with a ferromagnetic nano-island and electrode, it was expected that the interplay of spin-dependent tunneling (SDT) and SET, i.e., spin-dependent single-electron tunneling (SD-SET), would give rise to remarkable tunnel magnetoresistance (TMR) phenomena. We investigated magnetotransport properties in both sequential tunneling and cotunneling regimes of SET and found the enhancement and oscillation of TMR. The self-assembled ferromagnetic nanoparticles we have employed in this study consisted of a Co–Al–O granular film with cobalt nanoparticles embedded in an Al–O insulating matrix. A Co36Al22O42Co36Al22O42 film prepared by a reactive sputtering method produced a TMR ratio reaching 10% and superparamagnetic behavior at room temperature. The TMR ratio exhibited an anomalous increase at low temperatures but no indication of change with bias voltage. In Section 4, we show that the anomalous increase of the MR provided evidence for higher-order tunneling (cotunneling) between large granules through intervening small granules. We emphasize that the existence of higher-order tunneling is a natural consequence of the granular structure, since broad distribution of granule size is an intrinsic property of granular systems. In Section 5, we concentrate on SD-SET properties in sequential tunneling regimes. We fabricated two types of device structures with Co–Al–O film using focused ion-beam milling or electron-beam lithography techniques. One had a granular nanobridge structure: point-shaped electrodes separated by a very narrow lateral gap filled with the Co–Al–O granular film. The other had a current-perpendicular-to-plane (CPP) geometry structure: a thin Co–Al–O granular film sandwiched by ferromagnetic electrodes with the current flowing in the direction perpendicular to the film plane through a few Co particles. We found the enhancement and oscillation of TMR due to spin-dependent SET in sequential tunneling regimes. In Section 6, we report experimental evidence of a spin accumulation effect in Co nanoparticles leading to the oscillation of TMR with alternate sign changes. Furthermore, we discovered that the spin relaxation time in the nanoparticles is unprecedentedly enhanced up to the order of more than hundreds of nanoseconds, compared to that evaluated from the spin-diffusion length of ferromagnetic layers in previous CPP-GMR studies, i.e., the order of tens of picoseconds.  相似文献   
95.
An experimental study was performed on the combustion characteristics of a jet diffusion flame of Mg vapor injected through a small nozzle into CO2 atmospheres at low pressures from 8 to 48 kPa with a view to using Mg as fuel for a CO2-breathing turbojet engine in the Mars atmosphere. The Mg vapor jet produced three types of the flame. At lower pressures and higher injection velocities, a red-heated jet flame formed, in which the injected Mg vapor was heated by spontaneous reactions, turning red. At medium pressures and injection velocities, a stable luminous lifted-like flame developed above the rim of the chimney, a tube-like combustion product for the Mg vapor passage that grew on the nozzle during combustion. The flame had similar flame length properties to laminar jet diffusion flames of gaseous fuels. At higher pressures and lower injection velocities, a stable luminous attached flame developed at the rim of the chimney. The same reactions, producing MgO(g), CO and MgO(c), proceeded preferentially for all flames and chimneys. Carbon was only subordinately generated. Burning behavior of Mg vapor jets in a CO2 atmosphere has been represented, including the homogeneous reaction of Mg vapor with CO2, the diffusion of CO2, and the condensation and deposit of MgO. The injection velocity of Mg vapor at the rim of the chimney and the exothermic reactions with diffused CO2 that occur there play a crucial role in the attachment and development of the flames. The flame structure may be explained in terms of the relatively low gas-phase reaction rate of Mg with CO2.  相似文献   
96.
Yoshida  Koki  Konishi  Keiji  Hara  Naoyuki 《Nonlinear dynamics》2021,104(3):2363-2388
Nonlinear Dynamics - Stochastic synchrony, also known as noise-induced synchronization that leads to phase coherence, arises when a set of uncoupled neurons synchronizes to a common white noise...  相似文献   
97.
Crystalline-to-amorphous transformation of cellulose in water, just like that for starch upon cooking called gelatinisation, is revealed at 320 degrees C and 25 MPa.  相似文献   
98.
An efficient algorithm is proposed for finding all solutions of systems of nonlinear equations with separable mappings. This algorithm is based on interval analysis, the dual simplex method, the contraction method, and a special technique which makes the algorithm not require large memory space and not require copying tableaus. By numerical examples, it is shown that the proposed algorithm could find all solutions of a system of 2000 nonlinear equations in acceptable computation time. AMS subject classification (2000)  65H10, 65G10  相似文献   
99.
All-solid-state batteries (ASSBs) with inorganic solid electrolytes (SEs) have attracted significant interest as next-generation energy storage. Halides such as Li3YCl6 are promising candidates for SE because they combine high oxidation stability and deformability. However, the ionic conductivities of halide SEs are not as high as those of other SEs, especially sulfides. Here, we discover new lithium-metal-oxy-halide materials, LiMOCl4 (M=Nb, Ta). They exhibit extremely high ionic conductivities of 10.4 mS cm−1 for M=Nb and 12.4 mS cm−1 for M=Ta, respectively, even in cold-pressed powder forms at room temperature, which are comparable to or surpass those of organic liquid electrolytes used in lithium-ion batteries. Bulk-type ASSB cells using the oxyhalides as the cathode SE demonstrate an outstanding rate capability with a capacity retention of 80 % at 5 C/0.1 C. We believe that the proposed oxyhalides are promising SE candidates for the practical applications of ASSBs.  相似文献   
100.
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