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Title: Time-resolved fluctuation during the photochemical reaction of a photoreceptor protein: Phototropin1LOV2-linker
Authors: Kuroi, Kunisato
Sato, Francielle
Nakasone, Yusuke
Zikihara, Kazunori
Tokutomi, Satoru
Terazima, Masahide
Author's alias: 寺嶋, 正秀
Issue Date: 27-Jan-2016
Publisher: Royal Society of Chemistry
Journal title: Physical Chemistry Chemical Physics
Volume: 18
Start page: 6228
End page: 6238
Abstract: Although the relationship between structural fluctuations and reactions is important for elucidating reaction mechanisms, experimental data describing such fluctuations of reaction intermediates are sparse. In order to investigate structural fluctuations during a protein reaction, the compressibilities of intermediate species after photoexcitation of a phot1LOV2-linker, which is a typical LOV domain protein with the C-terminal linker including the J-α helix and used recently for optogenetics, were measured in the time-domain by the transient grating and transient lens methods with a high pressure optical cell. The yield of covalent bond formation between the chromophore and a Cys residue (S state formation) relative to that at 0.1 MPa decreased very slightly with increasing pressure. The fraction of the reactive species that yields the T state (linker-unfolded state) decreased almost proportionally with pressure (0.1-200 MPa) to about 65%. Interestingly, the volume change associated with the reaction was much more pressure sensitive. By combining these data, the compressibility changes for the short lived intermediate (S state) and the final product (T state) formation were determined. The compressibility of the S state was found to increase compared with the dark (D) state, and the compressibility decreased during the transition from the S state to the T state. The compressibility change is discussed in terms of cavities inside the protein. By comparing the crystal structures of the phot1LOV2-linker at dark and light states, we concluded that the cavity volumes between the LOV domain and the linker domain increase in the S state, which explains the enhanced compressibility.
Rights: This is the accepted version of the following article, which has been published in final form at http://dx.doi.org/10.1039/c5cp07472j.
This is not the published version. Please cite only the published version. この論文は出版社版でありません。引用の際には出版社版をご確認ご利用ください。
URI: http://hdl.handle.net/2433/218348
DOI(Published Version): 10.1039/c5cp07472j
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