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We find that in the ordinary smectic-A phase, the spatial distribution of the counterions of the mesogens is approximately uniform, whereas in the wide smectic-A phase, the small counterions accumulate in between the smectic layers. Due to this phenomenology, the wide smectic-A phase could be interesting for applications, which hinge on the presence of conductivity channels for mobile ions.Using self-consistent field theory, we systematically explore the microphase separation in the class of two-component miktoarm star copolymers containing a single conjunction point between different blocks by considering an extended list of candidate microphases. We plot mean-field phase diagrams in the plane of segregation strength and composition for an array of representative star copolymers. Three principal phase diagram topologies, dictated by different phase stabilities, are exposed, displaying a hierarchy in complexity by increasing the molecular asymmetry. Our investigation indicates that the phase diagram topology depends on the ratios of arm numbers and Kuhn segment lengths, which highlights the role of the coordination number ratio between different polymers at the domain interface. These findings reveal the simplicity of the general phase behavior and suggest a complete list of stable microphases for the entire class, which provide useful insight into studying copolymers with more complicated architectures and conformational properties.We study supercooled dynamics in a quantum hard-sphere liquid using quantum mode-coupling formulation. In the moderate quantum regime, classical cage effects lead to slower dynamics compared to the strongly quantum regime, where tunneling overcomes classical caging, leading to faster relaxation. As a result, the glass transition critical density can become significantly higher than for the classical liquids. A perturbative approach is used to solve time dependent quantum mode-coupling equations to study in detail the dynamics of the supercooled liquid in the moderate quantum regime. Similar to the classical case, the relaxation time shows the power-law increase with the increase in the density in the supercooled regime. However, the power-law exponent is found to be dependent on the quantumness; it increases linearly as the quantumness is increased in the moderate quantum regime.Bimetallic alloys have attracted considerable attention due to the tunable catalytic activity and selectivity that can be different from those of pure metals. Here, we study the superior catalytic behaviors of the Pt3Ni nanowire (NW) over each individual, Pt and Ni NWs during the reverse Water Gas Shift (rWGS) reaction, using density functional theory. The results show that the promoted rWGS activity by Pt3Ni strongly depends on the ensemble effect (a particular arrangement of active sites introduced by alloying), while the contributions from ligand and strain effects, which are of great importance in electrocatalysis, are rather subtle. As a result, a unique Ni-Pt hybrid ensemble is observed at the 110/111 edge of the Pt3Ni NW, where the synergy between Ni and Pt sites is active enough to stabilize carbon dioxide on the surface readily for the rWGS reaction but moderate enough to allow for the facile removal of carbon monoxide and hydrogenation of hydroxyl species. Our study highlights the importance of the ensemble effect in heterogeneous catalysis of metal alloys, enabling selective binding-tuning and promotion of catalytic activity.Plasmonic cavities (PCs) made of metallic nanostructures can concentrate electromagnetic radiation into an ultrasmall volume, where it might strongly interact with quantum emitters. In recent years, there has been much interest in studying such a strong coupling in the limit of single emitters. However, the lossy nature of PCs, reflected in their broad spectra, limits their quality factors and hence their performance as cavities. Here, we study the effect of the adhesion layer used in the fabrication of metal nanostructures on the spectral linewidths of bowtie-structured PCs. Using dark-field microspectroscopy, as well as electron energy loss spectroscopy, it is found that a reduction in the thickness of the chromium adhesion layer we use from 3 nm to 0.1 nm decreases the linewidths of both bright and dark plasmonic modes. We further show that it is possible to fabricate bowtie PCs without any adhesion layer, in which case the linewidth may be narrowed by as much as a factor of 2. Linewidth reduction increases the quality factor of these PCs accordingly, and it is shown to facilitate reaching the strong-coupling regime with semiconductor quantum dots.We propose a strategy for enabling photodissociation of a normally photostable molecule through coupling to a nanoparticle plasmon. The large possible coupling on the single-molecule level combined with the highly lossy nature of plasmonic modes, with lifetimes on the order of femtoseconds, opens an ultrafast decay channel for the molecule. For plasmon mode frequencies below the vertical photoexcitation energy of the molecule, the difference between the excitation and emission energies is converted into vibrational energy on the molecular ground state in a Raman-like process. Under the correct conditions, this energy can be high enough to enable efficient photodissociation on the electronic ground state. We demonstrate the concept using numerical simulations of the Lindblad master equation for the hydrogen molecule in the vicinity of an aluminum nanoparticle and explore the photodissociation efficiency as a function of various system parameters.The role of water in the formation of particles from atmospheric trace gases is not well understood, in large part due to difficulties in detecting its presence under atmospheric conditions and the variety of possible structures that must be screened computationally. Here, we use infrared spectroscopy and variable-temperature ion trap mass spectrometry to investigate the structural motifs adopted by water bound to ammonium bisulfate clusters and their temperature dependence. For clusters featuring only acid-base linkages, water adopts a bridging arrangement spanning an adjacent ammonium and bisulfate. For larger clusters, water can also insert into a bisulfate-bisulfate hydrogen bond, yielding hydration isomers with very similar binding energies. The population of these isomers shows a complex temperature evolution, as an apparent third isomer appears with a temperature dependence that is difficult to explain using simple thermodynamic arguments. (E/Z)-BCI in vitro These observations suggest that the thermodynamics of water binding to atmospheric clusters such as these may not be straightforward.
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