Сибирский федеральный университет

Тип публикации: статья из журнала

Год издания: 2020

Идентификатор DOI: 10.1111/php.13280

Аннотация: Calcium-regulated photoproteins are found in at least five phyla of organisms. The light emitted by those photoproteins can be tuned by mutating the photoprotein and/or by modifying the substrate coelenterazine (CTZ). Thirty years ago, Shimomura observed that the luminescence activity of aequorin was dramatically reduced when the substrate CTZ was replaced by its analog v-CTZ. The latter is formed by adding a phenyl ring to the π-conjugated moiety of CTZ. The decrease in luminescence activity has not been understood until now. In this paper, through combined quantum mechanics and molecular mechanics calculations as well as molecular dynamics simulations, we discovered the reason for this observation. Modification of the substrate changes the conformation of nearby aromatic residues and enhances the π-π stacking interactions between the conjugated moiety of v-CTZ and the residues, which weakens the charge transfer to form light emitter and leads to a lower luminescence activity. The microenvironments of CTZ in obelin and in aequorin are very similar, so we predicted that the luminescence activity of obelin will also dramatically decrease when CTZ is replaced by v-CTZ. This prediction has received strong evidence from currently theoretical calculations and has been verified by experiments.

Журнал: Photochemistry and Photobiology

Выпуск журнала: Т. 96, № 5

Номера страниц: 1047-1060

ISSN журнала: 00318655

Издатель: American Society for Photobiology

• Ding B.W. (Key Laboratory of Theoretical and Computational Photochemistry,Ministry of Education,College of Chemistry,Beijing Normal University)
• Liu Y.J. (Key Laboratory of Theoretical and Computational Photochemistry,Ministry of Education,College of Chemistry,Beijing Normal University)
• Eremeeva E.V. (Photobiology Laboratory,Institute of Biophysics SB RAS,Federal Research Center “Krasnoyarsk Science Center SB RAS”)
• Vysotski E.S. (Photobiology Laboratory,Institute of Biophysics SB RAS,Federal Research Center “Krasnoyarsk Science Center SB RAS”)

• Ядро РИНЦ (eLIBRARY.RU)