Related papers: Hot electron mediated desorption rates calculated …
We present a modification of the $\Delta$SCF method of calculating energies of excited states, in order to make it applicable to resonance calculations of molecules adsorbed on metal surfaces, where the molecular orbitals are highly…
A general approach to calculate the diabatic surfaces for electron-transfer reactions is presented, based on first-principles molecular dynamics of the active centers and their surrounding medium. The excitation energy corresponding to the…
A new scenario of thermalization process of the adsorbate attached at solid surfaces is proposed. The scenario is based on existence of electric dipole layer in which the electron wavefunctions extend over the positive ions. Thus the strong…
Accurate and efficient simulation of excited state properties is an important and much aspired cornerstone in the study of adsorbate dynamics on metal surfaces. To this end, the recently proposed linear expansion \Delta Self-Consistent…
A wide range of experiments have established that certain chemical reactions at metal surfaces can be driven by multiple hot electron mediated excitations of adsorbates. A high transient density of hot electrons is obtained by means of…
Electron-stimulated desorption (ESD) of cryosorbed molecules on surfaces is a process of relevance to fields as varied as vacuum dynamics in accelerators and astrochemistry. While desorption from such molecular systems induced by keV…
The behavior of a polyelectrolyte adsorbed on a charged surface of high-dielectric constant is studied by both Monte-Carlo simulation and analytical methods. It is found that in a low ionic strength medium, the transition is first-order…
We show that a simple first-principles correction based on the difference between the singlet-triplet CO excitation energy values obtained by DFT and high-level quantum chemistry methods yields accurate CO adsorption properties on a variety…
Inelastic electron scattering by the adsorbate covered Pt(100) single crystal surface is studied by Disappearance Potential Spectroscopy and density of states (DOS) calculations. Two peculiar channels of elastic electron consumption are…
Non-adiabatic molecular dynamics simulations are used to analyze the role of different solvent degrees of freedom in the non-radiative relaxation of the first excited state of the hydrated electron. The relaxation occurs through a…
We use density functional theory (DFT) with the generalized gradient approximation (GGA) and our first-principles extrapolation method for accurate chemisorption energies {[Mason {\em et al.}, Phys. Rev. B {\bf 69}, 161401R (2004)]} to…
We present a model intended for rapid sampling of ground and excited state potential energy surfaces for first-row transition metal active sites. The method is computationally inexpensive and is suited for dynamics simulations where (1)…
Photo-induced excited-state energy transfer (EET) processes play an important role in the solar energy conversions. The phenylene ethynylene (PE) dendrimers display great potential in improving the efficiency of solar cells, because of…
We study phonon-mediated adsorption and desorption of an electron at dielectric surfaces with deep polarization-induced surface potentials where multi-phonon transitions are responsible for electron energy relaxation. Focusing on…
We present a dynamical simulation scheme to model the highly correlated excited state dynamics of linear polyenes. We apply it to investigate the internal conversion processes of carotenoids following their photoexcitation. We use the…
Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several…
Accurate description of nonadiabatic dynamics of molecules at metal surfaces involving electron transfer has been a longstanding challenge for theory. Here, we tackle this problem by first constructing high-dimensional neural network…
Electron injection from an adsorbed molecule to the substrate (heterogeneous electron transfer) is studied. One reaction coordinate is used to model this process. The surface phonons and/or the electron-hole pairs together with the internal…
An accurate description of nonadiabatic energy relaxation is crucial for modeling atomistic dynamics at metal surfaces. Interfacial energy transfer due to electron-hole pair excitations coupled to motion of molecular adsorbates is often…
In a dense plasma environment, the energy levels of an ion shift relative to the isolated ion values. This shift is reflected in the optical spectrum of the plasma and can be measured in, for example, emission experiments. In this work, we…