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Type: Artigo de periódico
Title: Solvation of excess electrons in supercritical ammonia
Author: Rodriguez, J
Skaf, MS
Laria, D
Abstract: Molecular dynamics simulations have been performed to study equilibrium and dynamical aspects of solvation of excess electrons in supercritical ammonia along the T=450 K isotherm. The interval of supercritical densities investigated spans from typically dense liquid down to dilute vapor ambients. Equilibrium aspects of solvation were analyzed using combined path integral-molecular dynamics techniques. The transition from localized to quasifree states, described in terms of the isomorphic electron-polymer spatial extent, was observed at approximately one fourth of the triple point density, a value somewhat higher than that recently reported for supercritical water [D. Laria and M. Skaf, J. Phys. Chem. A 106, 8066 (2002)]. The density of electronic eigenstates shows typically one s- and three p-like bound states that gradually lose their symmetry characteristics as the density lowers. The computed ground state absorption spectrum exhibits redshifts in the absorption bands as the density decreases; these shifts are much larger than those reported by pulse radiolysis experiments. By performing adiabatic dynamics, we also investigate mechanisms for solvent relaxation at high and intermediate supercritical densities following a vertical excitation of the electron. (C) 2003 American Institute of Physics.
Country: EUA
Editor: Amer Inst Physics
Rights: aberto
Identifier DOI: 10.1063/1.1601215
Date Issue: 2003
Appears in Collections:Unicamp - Artigos e Outros Documentos

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