Photoefficient 2<sup>nd</sup> generation molecular motors responsive to visible light

Pfeifer, Lukas; Scherübl, Maximilian; Fellert, Maximilian; Danowski, Wojciech; Cheng, Jinling; Pol, J.A. Fernandez; Feringa, Ben L.

doi:10.1039/c9sc02150g

Cited by 44 publications

(70 citation statements)

References 41 publications

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“…Tuning of the S 1 electronic structure and photoreaction properties of neutral stilbenoid molecular motors was already explored via introducing electron-donating or electron-withdrawing substituents. 76 In particular, the graing of an electron-poor CN group on the rotor moiety improved the isomerisation QY up to 20% for a 2 nd generation Feringa-type motor also characterized by a longer-lived ($10 ps) S 1 dark state proposed to feature enhanced pyramidalization. 72,77 Here, we observe that the isomerisation QY of 1 increases four-fold compared to the originally reported oxindoles (QYs ca.…”

Section: Discussionmentioning

confidence: 99%

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Effect of charge-transfer enhancement on the efficiency and rotary mechanism of an oxindole-based molecular motor

et al. 2021

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Effect of charge-transfer enhancement on the efficiency and rotary mechanism of an oxindole-based molecular motor

et al. 2021

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“…Bacteria and active colloids, for example, are propelled along trajectories that appear diffusive at long timescales but are more persistent and superdiffusive at shorter timescales ( 1 ). Recent reports of “enhanced” or “boosted” diffusion of various molecules extend this notion down to the molecular scale, raising questions about the shared and distinguishing features of equilibrium and nonequilibrium, not only for protein molecular motors where the phenomenon was first identified ( 2 ), but also for synthetic molecular motors ( 3 – 5 ), active fluctuations in the cell ( 6 , 7 ), optically trapped colloids ( 8 ), common chemical reactions ( 9 ), and enzymes ( 10 – 18 ). Regarding enzymes, however, experiments have not tackled the basic question of how the reaction rate and the free energy released affect mobility.…”

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Master curve of boosted diffusion for 10 catalytic enzymes

Jee

Tlusty

Granick

2020

Proc. Natl. Acad. Sci. U.S.A.

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Molecular agitation more rapid than thermal Brownian motion is reported for cellular environments, motor proteins, synthetic molecular motors, enzymes, and common chemical reactions, yet that chemical activity coupled to molecular motion contrasts with generations of accumulated knowledge about diffusion at equilibrium. To test the limits of this idea, a critical testbed is the mobility of catalytically active enzymes. Sentiment is divided about the reality of enhanced enzyme diffusion, with evidence for and against. Here a master curve shows that the enzyme diffusion coefficient increases in proportion to the energy release rate—the product of Michaelis-Menten reaction rate and Gibbs free energy change (ΔG)—with a highly satisfactory correlation coefficient of 0.97. For 10 catalytic enzymes (urease, acetylcholinesterase, seven enzymes from the glucose cascade cycle, and one other), our measurements span from a roughly 40% enhanced diffusion coefficient at a high turnover rate and negativeΔGto no enhancement at a slow turnover rate and positiveΔG. Moreover, two independent measures of mobility show consistency, provided that one avoids undesirable fluorescence photophysics. The master curve presented here quantifies the limits of both ideas, that enzymes display enhanced diffusion and that they do not within instrumental resolution, and has possible implications for understanding enzyme mobility in cellular environments. The striking linear dependence of ΔGfor the exergonic enzymes (ΔG<0), together with the vanishing effect for endergonic enzyme (ΔG>0), are consistent with a physical picture in which the mechanism boosting the diffusion is an active one, utilizing the available work from the chemical reaction.

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“…To this end, it becomes crucial to shift the operation wavelength of molecular motors toward the visible and even near-infrared spectral regions because of the harmful nature and low penetrability of UV light. Despite the recent emergence of several successful examples of visible-light-driven molecular motors, 22,90,91 challenges still remain regarding how to apply these visible-light-driven molecular motors in responsive materials, whose realization might arouse several exciting projects such as sunlight-driven motorized materials and energy-storage materials.…”

Section: Perspectives and Challengesmentioning

confidence: 99%

Bottom-Up: Can Supramolecular Tools Deliver Responsiveness from Molecular Motors to Macroscopic Materials?

Zhang

Tian

et al. 2020

Matter

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Motion is omnipresent, as is obvious from the artificial machines in the macro-world and the biomolecular motors in living systems, controlling dynamic behavior along many length scales. With the emergence of molecular machines in the past decades, a major step has been made toward responsive materials and dynamic molecular systems. Photochemical rotary molecular motors hold a unique position, as embedding nanoscale motors in macroscopic materials enables light-driven responsive and adaptive properties. Although the synthesis and engineering of discrete molecular motors in the solution phase are well understood, the design and construction of motorized smart materials that operate at the supramolecular and macroscopic levels provide several fundamental challenges. This Review highlights emerging methodologies that take advantage of the supramolecular toolbox for the bottom-up assembly of responsive materials. Illustrative examples include muscle-like actuators, motor-based metal-organic frameworks, and motorized liquid crystal films and droplets. Emphasis is on how the lightresponsive behavior and motion of rotary molecular motors can be communicated, delivered, and amplified to result in a specific dynamic output ranging from the nanoscale and molecular level all the way to the macroscopic scale and materials level. Furthermore, general guidelines for the supramolecular amplification of molecular motion and challenges and perspectives for the development of future motorized smart materials are presented.

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Photoefficient 2^nd generation molecular motors responsive to visible light

Abstract: A new series of visible light-driven artificial rotary molecular motors is presented including the most red-shifted example to date.

Cited by 44 publications

References 41 publications

Effect of charge-transfer enhancement on the efficiency and rotary mechanism of an oxindole-based molecular motor

Effect of charge-transfer enhancement on the efficiency and rotary mechanism of an oxindole-based molecular motor

Master curve of boosted diffusion for 10 catalytic enzymes

Bottom-Up: Can Supramolecular Tools Deliver Responsiveness from Molecular Motors to Macroscopic Materials?

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Photoefficient 2nd generation molecular motors responsive to visible light

Abstract: A new series of visible light-driven artificial rotary molecular motors is presented including the most red-shifted example to date.

Cited by 44 publications

References 41 publications

Effect of charge-transfer enhancement on the efficiency and rotary mechanism of an oxindole-based molecular motor

Effect of charge-transfer enhancement on the efficiency and rotary mechanism of an oxindole-based molecular motor

Master curve of boosted diffusion for 10 catalytic enzymes

Bottom-Up: Can Supramolecular Tools Deliver Responsiveness from Molecular Motors to Macroscopic Materials?

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Product

Resources

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Photoefficient 2^nd generation molecular motors responsive to visible light