Retinal chromophore charge delocalization and confinement explain the extreme photophysics of Neorhodopsin

Riccardo Palombo, Leonardo Barneschi, Laura Pedraza-González, Daniele Padula, Igor Schapiro, Massimo Olivucci*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

The understanding of how the rhodopsin sequence can be modified to exactly modulate the spectroscopic properties of its retinal chromophore, is a prerequisite for the rational design of more effective optogenetic tools. One key problem is that of establishing the rules to be satisfied for achieving highly fluorescent rhodopsins with a near infrared absorption. In the present paper we use multi-configurational quantum chemistry to construct a computer model of a recently discovered natural rhodopsin, Neorhodopsin, displaying exactly such properties. We show that the model, that successfully replicates the relevant experimental observables, unveils a geometrical and electronic structure of the chromophore featuring a highly diffuse charge distribution along its conjugated chain. The same model reveals that a charge confinement process occurring along the chromophore excited state isomerization coordinate, is the primary cause of the observed fluorescence enhancement.

Original languageAmerican English
Article number6652
JournalNature Communications
Volume13
Issue number1
DOIs
StatePublished - Dec 2022

Bibliographical note

Publisher Copyright:
© 2022, The Author(s).

Fingerprint

Dive into the research topics of 'Retinal chromophore charge delocalization and confinement explain the extreme photophysics of Neorhodopsin'. Together they form a unique fingerprint.

Cite this