A stable free tetragermacyclobutadiene incorporating fused-ring bulky EMind groups.

The first free cyclobutadiene (CBD) germanium analogue was obtained as room-temperature stable dark red crystals via the reaction of the bulky EMind-substituted 1,2-dichlorodigermene with lithium naphthalenide. The cyclic 4π-electron antiaromaticity is essentially stabilized by the polar Jahn-Teller distortion in the germanium CBD producing a planar rhombic-shaped charge-separated structure.

Magnetic Field-Induced Insulator-Semimetal Transition in a Pyrochlore Nd2Ir2O7.

We investigate magnetotransport properties in a single crystal of pyrochore-type Nd2Ir2O7. The metallic conduction is observed on the antiferromagnetic domain walls of the all-in-all-out-type Ir 5d moment ordered insulating bulk state that can be finely controlled by an external magnetic field along [111]. On the other hand, an applied field along [001] induces the bulk phase transition from insulator to semimetal as a consequence of the field-induced modification of the Nd 4f and Ir 5d moment configurations.

Majorana bound states and nonlocal spin correlations in a quantum wire on an unconventional superconductor.

We study theoretically the proximity effect of a one-dimensional metallic quantum wire (in the absence of spin-orbit interaction) lying on top of an unconventional superconductor. Three different material classes are considered as a substrate: (i) a chiral superconductor in class D with broken time-reversal symmetry and a class DIII superconductor (ii) with and (iii) without a nontrivial Z(2) number. Interestingly, we find degenerate zero energy Majorana bound states at both ends of the wire for all three cases.

Transcriptome tomography for brain analysis in the web-accessible anatomical space.

Increased information on the encoded mammalian genome is expected to facilitate an integrated understanding of complex anatomical structure and function based on the knowledge of gene products. Determination of gene expression-anatomy associations is crucial for this understanding. To elicit the association in the three-dimensional (3D) space, we introduce a novel technique for comprehensive mapping of endogenous gene expression into a web-accessible standard space: Transcriptome Tomography.

"Up" versus "down" alignment and hydration structures of solutes at the air/water interface revealed by heterodyne-detected electronic sum frequency generation with classical molecular dynamics simulation.

We unambiguously demonstrate the "up" versus "down" alignment of a pair of prototypical solute molecules adsorbed at the air/water interface for the first time using heterodyne-detected electronic sum frequency generation spectroscopy. This molecular alignment is also reproduced by classical molecular dynamics (MD) simulation theoretically. Furthermore, the MD simulation indicates distinctly different interface-specific hydration structures around the two solute molecules, which dictate the molecular alignment at the interface.

Electric quadrupole contribution to the nonresonant background of sum frequency generation at air/liquid interfaces.

We study an electric quadrupole contribution to sum frequency generation (SFG) at air∕liquid interfaces in an electronically and vibrationally nonresonant condition. Heterodyne-detected electronic sum frequency generation spectroscopy of air∕liquid interfaces reveals that nonresonant χ((2)) (second-order nonlinear susceptibility) has a negative sign and nearly the same value for all eight liquids studied. This result is rationalized on the basis of the theoretical expressions of χ((2)) with an electric quadrupole contribution taken into account.

Coherent nuclear dynamics in ultrafast photoinduced structural change of bis(diimine)copper(I) complex.

The photoinduced structural change of a prototype metal complex, [Cu(dmphen)(2)](+) (dmphen = 2,9-dimethyl-1,10-phenanthroline), was studied by ultrafast spectroscopy with time resolution as high as 30 fs. Time-resolved absorption measured with direct S(1) excitation clearly showed spectral changes attributable to the D(2d) (perpendicular) → D(2) (flattened) structural change occurring in the metal-to-ligand charge transfer singlet excited state ((1)MLCT) and the subsequent S(1) → T(1) intersystem crossing. It was confirmed that the two processes occur with time constants of ~0.

Tracking of the nuclear wavepacket motion in cyanine photoisomerization by ultrafast pump-dump-probe spectroscopy.

Understanding ultrafast reactions, which proceed on a time scale of nuclear motions, requires a quantitative characterization of the structural dynamics. To track such structural changes with time, we studied a nuclear wavepacket motion in photoisomerization of a prototype cyanine dye, 1,1'-diethyl-4,4'-cyanine, by ultrafast pump-dump-probe measurements in solution. The temporal evolution of wavepacket motion was examined by monitoring the efficiency of stimulated emission dumping, which was obtained from the recovery of a ground-state bleaching signal.

Resolving inhomogeneity using lifetime-weighted fluorescence correlation spectroscopy.

Fluorescence correlation spectroscopy (FCS) was extended by incorporating information of the fluorescence lifetime. This new experimental approach, called lifetime-weighted FCS, enables us to observe fluorescence lifetime fluctuations in the nano- to millisecond time region. The potential of this method for resolving inhomogeneity in complex systems was demonstrated.

"Half-hydration" at the air/water interface revealed by heterodyne-detected electronic sum frequency generation spectroscopy, polarization second harmonic generation, and molecular dynamics simulation.

A solute-solvent interaction at the air/water interface was investigated both experimentally and theoretically, by studying a prototypical surface-active polarity indicator molecule, coumarin 110 (C110), adsorbed at the air/water interface with heterodyne-detected electronic sum frequency generation (HD-ESFG) spectroscopy, polarization second harmonic generation (SHG), and a molecular dynamics (MD) simulation. The second-order nonlinear optical susceptibility (chi((2))) tensor elements of C110 at the air/water interface were determined experimentally by HD-ESFG and polarization SHG, and information on "intermediate" polarity sensed by C110 at the interface was obtained by HD-ESFG. An MD simulation and a time-dependent density functional theory calculation were used to theoretically evaluate the chi((2)) tensor elements, which were in good agreement with the experimental results of HD-ESFG and polarization SHG.