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Analysis of the Mode-Specific Excited-State Energy Distribution and Wavelength-Dependent Photoreaction Quantum Yield in Rhodopsin

Department of Chemistry, University of California at Berkeley, Berkeley, California 94720 USA

Correspondence: Address reprint requests to Richard A. Mathies, Fax: 510-642-3599; E-mail: rich{at}zinc.cchem.berkeley.edu.

The photoreaction quantum yield of rhodopsin is wavelength dependent: () is reduced by up to 5% at wavelengths to the red of 500 nm but is invariant ( = 0.65 ± 0.01) between 450 and 500 nm (Kim et al., 2001). To understand this nonstatistical internal conversion process, these results are compared with predictions of a Landau-Zener model for dynamic curve crossing. The initial distribution of excess photon energy in the 28 Franck-Condon active vibrational modes of rhodopsin is defined by a fully thermalized sum-over-states vibronic calculation. This calculation reveals that absorption by high-frequency unreactive modes (e.g., C=C stretches) increases as the excitation wavelength is shifted from 570 to 450 nm whereas relatively less energy is deposited into reactive low-frequency modes. This result qualitatively explains the experimentally observed wavelength dependence of () for rhodopsin and reveals the importance of delocalized, torsional modes in the reactive pathway.

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