Journal of the American Chemical Society, volume 144, issue 1, pages 69-73

Light Driven Ultrafast Bioinspired Molecular Motors: Steering and Accelerating Photoisomerization Dynamics of Retinal

Publication typeJournal Article
Publication date2021-12-27
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor15
ISSN00027863, 15205126
General Chemistry
Catalysis
Biochemistry
Colloid and Surface Chemistry
Abstract
Photoisomerization of retinal protonated Schiff base in microbial and animal rhodopsins are strikingly ultrafast and highly specific. Both protein environments provide conditions for fine-tuning the photochemistry of their chromophores. Here, by combining time-resolved action absorption spectroscopy and high-level electronic structure theory, we show that similar control can be gained in a synthetically engineered retinal chromophore. By locking the dimethylated retinal Schiff base at the C11═C12 double bond in its trans configuration (L-RSB), the excited-state decay is rendered from a slow picosecond to an ultrafast subpicosecond regime in the gas phase. Steric hindrance and pretwisting of L-RSB are found to be important for a significant reduction in the excited-state energy barriers, where isomerization of the locked chromophore proceeds along C9═C10 rather than the preferred C11═C12 isomerization path. Remarkably, the accelerated excited-state dynamics also becomes steered. We show that L-RSB is capable of unidirectional 360° rotation from all-trans to 9-cis and from 9-cis to all-trans in only two distinct steps induced by consecutive absorption of two 600 nm photons. This opens a way for the rational design of red-light-driven ultrafast molecular rotary motors based on locked retinal chromophores.

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Gruber E. et al. Light Driven Ultrafast Bioinspired Molecular Motors: Steering and Accelerating Photoisomerization Dynamics of Retinal // Journal of the American Chemical Society. 2021. Vol. 144. No. 1. pp. 69-73.
GOST all authors (up to 50) Copy
Gruber E., Kabylda A., Nielsen M. L., Rasmussen A. P., Teiwes R., Kusochek P. A., Bochenkova A. V., Andersen L. P. Light Driven Ultrafast Bioinspired Molecular Motors: Steering and Accelerating Photoisomerization Dynamics of Retinal // Journal of the American Chemical Society. 2021. Vol. 144. No. 1. pp. 69-73.
RIS |
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RIS Copy
TY - JOUR
DO - 10.1021/jacs.1c10752
UR - https://doi.org/10.1021%2Fjacs.1c10752
TI - Light Driven Ultrafast Bioinspired Molecular Motors: Steering and Accelerating Photoisomerization Dynamics of Retinal
T2 - Journal of the American Chemical Society
AU - Rasmussen, Anne P
AU - Teiwes, Ricky
AU - Kusochek, Pavel A
AU - Gruber, Elisabeth
AU - Kabylda, Adil
AU - Nielsen, Mogens Lykkegaard
AU - Bochenkova, Anastasia V.
AU - Andersen, L P
PY - 2021
DA - 2021/12/27 00:00:00
PB - American Chemical Society (ACS)
SP - 69-73
IS - 1
VL - 144
SN - 0002-7863
SN - 1520-5126
ER -
BibTex |
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BibTex Copy
@article{2021_Gruber
author = {Anne P Rasmussen and Ricky Teiwes and Pavel A Kusochek and Elisabeth Gruber and Adil Kabylda and Mogens Lykkegaard Nielsen and Anastasia V. Bochenkova and L P Andersen},
title = {Light Driven Ultrafast Bioinspired Molecular Motors: Steering and Accelerating Photoisomerization Dynamics of Retinal},
journal = {Journal of the American Chemical Society},
year = {2021},
volume = {144},
publisher = {American Chemical Society (ACS)},
month = {dec},
url = {https://doi.org/10.1021%2Fjacs.1c10752},
number = {1},
pages = {69--73},
doi = {10.1021/jacs.1c10752}
}
MLA
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MLA Copy
Gruber, Elisabeth, et al. “Light Driven Ultrafast Bioinspired Molecular Motors: Steering and Accelerating Photoisomerization Dynamics of Retinal.” Journal of the American Chemical Society, vol. 144, no. 1, Dec. 2021, pp. 69-73. https://doi.org/10.1021%2Fjacs.1c10752.
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