Single-ion recycling reactions

A single ion is enough: Ion reaction rates and reaction product branching ratios could be determined through repeated regeneration of the original target ion by photodissociation after each reaction. The product molecule was identified through nondestructive mass spectrometry. Finally, the target ion was regenerated through photodissociation of the molecular ion.     

Comparing spiro-OMeTAD and P3HT hole conductors in efficient solid state dye-sensitized solar cells

Two hole conductor materials, spiro-OMeTAD and P3HT, were compared in solid-state dye-sensitized solar cells. Two organic dyes containing one anchor unit (D35) or two anchor units (M3) were used in the comparison. Absorbed photon to current conversion efficiency close to unity was obtained for the devices with spiro-OMeTAD. Energy conversion efficiencies of 4.7% and 4.9% were measured for the devices with spiro-OMeTAD and the dyes D35 and M3, respectively. For the devices using the P3HT hole conductor the results were rather different comparing the two dye molecules, with energy conversion efficiencies of 3.2% and 0.5% for D35 and M3, respectively. Photo-induced absorption measurements suggest that the regeneration of the dyes, and the polymer infiltration, is not complete using P3HT, while spiro-OMeTAD regenerates the dyes efficiently. However, the TiO(2)/D35/P3HT system shows rather high energy conversion efficiency and electrochemical oxidation of the dyes on TiO(2) indicates that D35 have a more efficient dye to dye hole conduction than M3, which thereby might explain the higher performance. The dye hole conduction may therefore be of significant importance for optimizing the energy conversion in such hybrid TiO(2)/dye/polymer systems.     

Droplet-based interfacial capacitive sensing

This paper presented a novel droplet-based pressure sensor using elastic and capacitive electrode-electrolyte interfaces to achieve ultrahigh mechanical-to-electrical sensitivity (1.58 μF kPa(-1)) and resolution (1.8 Pa) with a simple device architecture. The miniature transparent droplet sensors, fabricated by one-step laser micromachining, consisted of two flexible polymer membranes with conductive coating and a separation layer hosting a sensing chamber for an electrolyte droplet. The sensing principle primarily relied on high elasticity of the sensing droplet and large capacitance presented at the electrode-electrolyte interface. A simple surface modification scheme was introduced to the conductive coating, which reduced hysteresis of the droplet deformation without substantially compromising the interfacial capacitance. Moreover, the major concern of liquid evaporation was addressed by a mixture of glycerol and electrolyte with long-term stability in a laboratory environment. Theoretical analyses and experimental investigations on several design parameters (i.e., the dimensions of the sensing chamber and the droplet size) were thoroughly conducted to characterize and optimize the overall sensitivity of the device. Moreover, the environmental influences (e.g., temperature and humidity) on the capacitive measurement were further investigated. Finally, the simply constructed and mechanically flexible droplet sensor was successfully applied to detect minute blood pressure variations on the skin surface (with the maximum value less than 100 Pa) throughout cardiovascular cycles.     

Control and femtosecond time-resolved imaging of torsion in a chiral molecule

We study how the combination of long and short laser pulses can be used to induce torsion in an axially chiral biphenyl derivative (3,5-difluoro-3',5'-dibromo-4'-cyanobiphenyl). A long, with respect to the molecular rotational periods, elliptically polarized laser pulse produces 3D alignment of the molecules, and a linearly polarized short pulse initiates torsion about the stereogenic axis. The torsional motion is monitored in real-time by measuring the dihedral angle using femtosecond time-resolved Coulomb explosion imaging. Within the first 4 picoseconds (ps), torsion occurs with a period of 1.25 ps and an amplitude of 3° in excellent agreement with theoretical calculations. At larger times, the quantum states of the molecules describing the torsional motion dephase and an almost isotropic distribution of the dihedral angle is measured. We demonstrate an original application of covariance analysis of two-dimensional ion images to reveal strong correlations between specific ejected ionic fragments from Coulomb explosion. This technique strengthens our interpretation of the experimental data.     

Nitric oxide adsorbed on zeolites: EPR studies

CW-EPR studies of NO adsorbed on sodium ion-exchanged zeolites were focused on the geometrical structure of NO monoradical and (NO)2 biradical formed on zeolites. The EPR spectrum of NO monoradical adsorbed on zeolite can be characterized by the three different g-tensor components and the resolved y-component hyperfine coupling with the 14N nucleus. Among the g-tensor components, the value of g(zz) is very sensitive to the local environment of zeolite and becomes a measure of the electrostatic field in zeolite. The temperature dependence of the g-tensor demonstrated the presence of two states of the Na-NO adduct, in rigid and rotational states. The EPR spectra of NO adsorbed on alkaline metal ion-exchanged zeolite and their temperature dependency are essentially the same as that on sodium ion-exchanged zeolite. On the other hand, for NO adsorbed on copper ion-exchanged zeolite it is known that the magnetic interaction between NO molecule and paramagnetic copper ion are observable in the spectra recorded at low temperature. The signals assigned to (NO)2 biradical were detected for EPR spectrum of NO adsorbed on Na-LTA. CW-EPR spectra as well as their theoretical calculation suggested that the two NO molecules are aligned along their N-O bond axes. A new procedure for automatical EPR simulation is described which makes it possible to analyze EPR spectrum easily. In the last part of this paper, some instances when other nitrogen oxides were used as a probe molecule to characterize the zeolite structure, chemical properties of zeolites, and dynamics of small molecules were described on the basis of selected literature data reported recently.     

Concentrated Kondo systems

This review considers the experimental and theoretical studies of concentrated Kondo systems (CKS), Kondo lattices, substitutional solid solutions and their transition from Kondo impurity to Kondo lattice, and ‘intermediate valence compounds’ which are, in fact, high T _K CKS (T _K is the Kondo temperature). The anomalous low temperature properties of CKS are related to the formation of the narrow (～k _B T _K) high-amplitude Abrikosov-Suhl resonance E _R in the vicinity of the Fermi level E _F. This resonance is situated exactly at E _F in low T _K CKS with T _K < Δ_CF and near E _F in high T _K CKS with T _K > Δ_CF (Δ_CF is the crystal field splitting). In low T _K ‘j=1/2’ CKS the condition E _R=E _F leads to an increase of the density of states at E _F, which is large enough to induce heavy fermion superconductivity in CeCu₂Si₂, UBe₁₃. We demonstrate that the transition from low T _K (E _R=E _F) to high T _K CKS (E _R≠E _F) might be what was formerly considered as a ‘Kondo-lattice-intermediate valence state’ transition. It appears that in many cases the essentially non-integer valence state of the rare-earth elements in metallic compounds is thermodynamically unstable with respect to a transition to an almost integer valence state, because it realizes the maximum gain in free energy from the Kondo condensation.     

Irradiation-induced defect states in Pb1−xSnxTe under high pressure

Abstract

The galvanomagnetic properties of electron-irradiate n^? and P-Pb_1?x,Sn_xTe (x=O.2) under high hydrostatic Pressure have been investigated. In the irradiated samples the “soft” stabilisation of Fermi level under the irradiation has been revealed and the model of the energy spectrum of irradiated Pb_1?x,Sn_xTe (x=O.2) proposed. The obtained experimental results were used to aetermine the Parameters of radiation-induced resonant band situated slightly below the valence band top.     

A classification of smooth convex 3-polytopes with at most 16 lattice points

We provide a complete classification up to isomorphism of all smooth convex lattice 3-polytopes with at most 16 lattice points. There exist in total 103 different polytopes meeting these criteria. Of these, 99 are strict Cayley polytopes and the remaining four are obtained as inverse stellar subdivisions of such polytopes. We derive a classification, up to isomorphism, of all smooth embeddings of toric threefolds in ? ^N where N≤15. Again we have in total 103 such embeddings. Of these, 99 are projective bundles embedded in ? ^N and the remaining four are blow-ups of such toric threefolds.