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000904316 1001_ $$00000-0002-8525-5568$$aYaroshevich, Igor A.$$b0
000904316 245__ $$aRole of hydrogen bond alternation and charge transfer states in photoactivation of the Orange Carotenoid Protein
000904316 260__ $$aLondon$$bSpringer Nature$$c2021
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000904316 520__ $$aHere, we propose a possible photoactivation mechanism of a 35-kDa blue light-triggered photoreceptor, the Orange Carotenoid Protein (OCP), suggesting that the reaction involves the transient formation of a protonated ketocarotenoid (oxocarbenium cation) state. Taking advantage of engineering an OCP variant carrying the Y201W mutation, which shows superior spectroscopic and structural properties, it is shown that the presence of Trp201 augments the impact of one critical H-bond between the ketocarotenoid and the protein. This confers an unprecedented homogeneity of the dark-adapted OCP state and substantially increases the yield of the excited photoproduct S*, which is important for the productive photocycle to proceed. A 1.37 Å crystal structure of OCP Y201W combined with femtosecond time-resolved absorption spectroscopy, kinetic analysis, and deconvolution of the spectral intermediates, as well as extensive quantum chemical calculations incorporating the effect of the local electric field, highlighted the role of charge-transfer states during OCP photoconversion.
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000904316 7001_ $$00000-0001-6767-1501$$aMaksimov, Eugene G.$$b1$$eCorresponding author
000904316 7001_ $$00000-0002-8608-1416$$aSluchanko, Nikolai N.$$b2
000904316 7001_ $$0P:(DE-HGF)0$$aZlenko, Dmitry V.$$b3
000904316 7001_ $$00000-0003-1616-4408$$aStepanov, Alexey V.$$b4
000904316 7001_ $$aSlutskaya, Ekaterina A.$$b5
000904316 7001_ $$aSlonimskiy, Yury B.$$b6
000904316 7001_ $$aBotnarevskii, Viacheslav S.$$b7
000904316 7001_ $$aRemeeva, Alina$$b8
000904316 7001_ $$aGushchin, Ivan$$b9
000904316 7001_ $$aKovalev, Kirill$$b10
000904316 7001_ $$0P:(DE-Juel1)131964$$aGordeliy, Valentin I.$$b11
000904316 7001_ $$aShelaev, Ivan V.$$b12
000904316 7001_ $$aGostev, Fedor E.$$b13
000904316 7001_ $$aKhakhulin, Dmitry$$b14
000904316 7001_ $$aPoddubnyy, Vladimir V.$$b15
000904316 7001_ $$aGostev, Timofey S.$$b16
000904316 7001_ $$aCherepanov, Dmitry A.$$b17
000904316 7001_ $$aPolívka, Tomáš$$b18
000904316 7001_ $$aKloz, Miroslav$$b19
000904316 7001_ $$00000-0003-2835-2895$$aFriedrich, Thomas$$b20
000904316 7001_ $$aPaschenko, Vladimir Z.$$b21
000904316 7001_ $$aNadtochenko, Victor A.$$b22
000904316 7001_ $$aRubin, Andrew B.$$b23
000904316 7001_ $$aKirpichnikov, Mikhail P.$$b24
000904316 773__ $$0PERI:(DE-600)2919698-X$$a10.1038/s42003-021-02022-3$$gVol. 4, no. 1, p. 539$$n1$$p539$$tCommunications biology$$v4$$x2399-3642$$y2021
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