Optical absorption of water: coulomb effects versus hydrogen bonding.
The optical spectrum of water is not well understood. For example, the main absorption peak shifts upwards by 1.3 eV upon condensation, which is contrary to the behavior expected from aggregation-induced broadening of molecular levels. We investigate theoretically the effects of electron-electron and electron-hole correlations, finding that condensation leads to delocalization of the exciton onto nearby hydrogen-bonded molecules. This reduces its binding energy and has a dramatic impact on the line shape. The calculated spectrum is in excellent agreement with experiment.
Hahn
P H
PH
Institut für Festkörpertheorie und -optik, Friedrich-Schiller-Universität, Max-Wien-Platz 1, 07743 Jena, Germany.
Schmidt
W G
WG
Seino
K
K
Preuss
M
M
Bechstedt
F
F
Bernholc
J
J