Nonlinear vibrational spectroscopies such as visible-infrared sum-frequency spectroscopy may serve as powerful probes of interfacial structure. Obtaining quantitative orientation information, however, has been limited by the required knowledge of the corresponding molecular-level nonlinear optical properties. We provide a general scheme for calculating the vibrational hyperpolarizability of any...

In this combined theoretical and experimental study we report a full analysis of the resonant inelastic X-ray scattering (RIXS) spectra of H2O, D2O and HDO. We demonstrate that electronically-elastic RIXS has an inherent capability to map the potential energy surface and to perform vibrational analysis of the electronic ground state in multimode systems. We show that the control and selection o...

Vibrational degrees of freedom in trapped-ion systems have recently been gaining attention as a quantum resource, beyond the role mediator for entangling operations on internal freedom, because large available Hilbert space. The vibrational modes can be represented harmonic oscillators and thus offer space with infinite dimension. Here we review recent theoretical experimental progress coherent...

The lifetime of the antisymmetric stretch mode of interstitial oxygen in crystalline Si is measured directly by time-resolved, transient bleaching spectroscopy to be T1 = 229 ± 16 ps at 10 K. The temperature dependence of the lifetime shows that the stretch mode decays into eight vibrational modes of 142 ± 20 cm. The low-temperature width of the FTIR (IR) absorption line due to the stretch mode...

The shift and broadening of the vibrational frequency of a diatomic molecule adsorbed on a metal surface are calculated on the basis of electromagnetic interactions. Finite molecular size and nonlocal metal response are included in a calculation of the response function, whose pole is the complex normal mode frequency. Finite molecular size is described by a model of a point-like vibrational mo...

Electronic transport through an alkanedithiol self-assembled monolayer (SAM) is investigated using a nanometer scale device. Temperature-independent current-voltage characteristics are observed, indicating tunneling is the main conduction mechanism. The measured current-voltage characteristics are analyzed with a metal-insulator-metal tunneling model. The inelastic electron tunneling spectrosco...

Experiments explore the influence of different C-H stretching eigenstates of CH3D on the reaction of CH3D with Cl(2P3/2). We prepare the mid |110>|0>(A1,E), mid |200>|>0(E), and mid |100>|0> +nu3 +nu5 eigenstates by direct midinfrared absorption near 6000 cm(-1). The vibrationally excited molecules react with photolytic Cl atoms, and we monitor the vibrational states of the CH2D or CH3 radical ...

Photoinduced intramolecular charge separation (CS) in a polar polymer glass, cyanoethylated pullulan (CN-PUL), was studied below the glass transition temperature (Tg=395 K). A series of three carbazole (Cz: donor)-cyclohexane (S: spacer)-acceptor (A: acceptor) molecules (Cz-S-A) was used as intramolecular donor-acceptor dyads. The photoinduced CS rate was evaluated by the fluorescence decay mea...

In one-dimensional Lie algebraic framework, we calculated the vibrational frequencies of oxygen difluoride (F2O) molecule in fundamental mode, higher overtones and their combinational bands.