Electronic coherence and collective optical excitations of conjugated molecules

Shaul Mukamel, Sergei Tretiak, Thomas Wagersreiter, Vladimir Chernyak

Research output: Contribution to journalArticlepeer-review

329 Citations (Scopus)

Abstract

Optical spectroscopy of conjugated molecules is described by using collective electronic coordinates, which represent the joint dynamics of electron-hole pairs. The approach relates the optical signals directly to the dynamics of charges and bond orders (electronic coherences) induced by the radiation field and uses only ground-state information, thus avoiding the explicit calculation of excited molecular states. The resulting real-space picture is reminiscent of the normal-mode analysis of molecular vibrations and offers a unified framework for the treatment of other types of systems including semiconductor nanostructures and biological complexes. Spatial coherence displayed in two-dimensional plots of the five electronic normal modes that dominate the optical response of poly(p-phenylene vinylene) oligomers with up to 50 repeat units (398 carbon atoms) in the 1.5- to 8- electronvolt frequency range suggests a saturation to bulk behavior at about five repeat units.

Original languageEnglish
Number of pages1
JournalScience
Volume277
Issue number5327
DOIs
Publication statusPublished - 8 Aug 1997
Externally publishedYes

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