Related papers: Towards First-principles Electrochemistry
In what has been described as the fourth age of Quantum Chemistry, variational nuclear motion programs are now routinely being used to obtain the vibration-rotation levels and corresponding wavefunctions of small molecules to the sort of…
In bulk systems, molecules are routinely identified by their vibrational spectrum using Raman or infrared spectroscopy. In recent years, vibrational excitation lines have been observed in low-temperature conductance measurements on single…
By employing single charge injections with an atomic force microscope, we investigated redox reactions of a molecule on a multilayer insulating film. First, we charged the molecule positively by attaching a single hole. Then we neutralized…
We theoretically investigate optical absorption of molecules embedded nearby metallic antennas by using discrete dipole approximation method. It is found that the spectral peak of the absorption is shifted due to the radiation-induced…
We propose an approach to sensitively probe the chirality of molecules by measuring their coherent optical absorption spectra. It is shown that quantum dynamics of the cyclic three-level chiral molecules driven by appropriately-designed…
We study the spectrum of vibrational modes in metal nanoparticles with a dielectric core. Vibrational modes are excited by the rapid heating of the particle lattice that takes place after laser excitation, and can be monitored by means of…
The theory of statistical-mechanical lattice-gas modeling of adsorption is reviewed and shown to be applicable to a range of electrochemical problems dominated by effective, lateral adsorbate--adsorbate interactions. A general strategy for…
As per the Franck-Condon principle, absorption spectroscopy reveals changes in nuclear geometry in molecules or solids upon electronic excitation. It is often assumed these changes cannot be resolved beyond the ground vibrational…
We present first-principles calculations of the rate of energy exchanges between electrons and ions in nonequilibrium warm dense plasmas, liquid metals and hot solids, a fundamental property for which various models offer diverging…
We have measured the electric field modulated absorption of a sample of single-walled nanotubes (SWNT) suspended in a solid polyvinyl alcohol matrix. The electroabsorption (EA) spectrum roughly follows the first derivative of the absorption…
In this work, we investigate the relative importance of electronic and phononic energy dissipation during the molecular adsorption of CO on Cu(110). Initial sticking probabilities as a function of impact energy for CO impinging at normal…
From ultraviolet to mid-infrared region, light-matter interaction mechanisms in semiconductors progressively shift from electronic transitions to phononic resonances and are affected by temperature. Here, we present a parallel…
Over the past decade, experimental microscopy and spectroscopy have made significant progress in the study of the morphological, optical, electronic and transport properties of materials. These developments include higher spatial…
The Stark effect provides a powerful method to shift the spectra of molecules, atoms and electronic transitions in general, becoming one of the simplest and most straightforward way to tune the frequency of quantum emitters by means of a…
In surface catalysis, the adsorption of carbon monoxide on transition-metal electrodes represents the prototype of strong chemisorption. Notwithstanding significant changes in the molecular orbitals of adsorbed CO, spectroscopic experiments…
Theoretical descriptions of the spectrum of electronic excitations in real metals have not yet reached a fully predictive, "first-principles" stage. In this paper we begin by presenting brief highlights of recent progress made in the…
We propose a computationally lean, two-stage approach that reliably predicts self-assembly behavior of complex charged molecules on a metallic surfaces under electrochemical conditions. Stage one uses ab initio simulations to provide…
The control and observation of reactants forming a chemical bond at the single-molecule level is a longstanding challenge in quantum physics and chemistry. Using a single CO molecule adsorbed at the apex of an atomic force microscope tip…
Linear and non-linear spectroscopies are powerful tools used to investigate the energetics and dynamics of electronic excited states of both molecules and crystals. While highly accurate \emph{ab initio} calculations of molecular spectra…
We perform all-electron path integral Monte Carlo (PIMC) and density functional theory molecular dynamics (DFT-MD) calculations to explore warm dense matter states of oxygen. Our simulations cover a wide density-temperature range of…