Sunlight-powered kHz rotation of a hemithioindigo-based molecular motor

Guentner, Manuel; Schildhauer, Monika; Thumser, Stefan; Mayer, Péter; Stephenson, David S.; Dube, Henry

doi:10.1038/ncomms9406

Cited by 205 publications

(226 citation statements)

References 43 publications

(46 reference statements)

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“…For example, the second-generation overcrowded-alkene motors, the hemithioindigo motor of Dube and co-workers [29] and the N-alkyl imine motors of Lehn and co-workers [32,33] all contain a (single) stereocenter. Owing to the stereocenter, the respective excited-state PES is asymmetric with respect to the two possible directions-CW or CCW-for the Z/E photoisomerizations that underlie the light-induced rotary motion.…”

Section: Other Mother Designs: Fewer Chiral Featuresmentioning

confidence: 99%

“…As for rotary speed, it was reported that 3 is capable of kHz frequencies at ambient temperatures. [29] The dibenzofulvene motors, in turn, lack a stereocenter but incorporate an axially chiral trityl moiety. Designed and synthesized by Bell and co-workers, [30,31] these systems appear promising motor candidates because their Z/E photoisomerizations around the central double bond are unidirectional and can attain high quantum yields (QYs) by appropriate substitutions (X in motor 4).…”

Section: R Ota R Y M Ol Ecu L a R Mot Orsmentioning

confidence: 99%

“…The hemithioindigo motor, developed by Dube and co-workers, [29] has a stereogenic sulfur atom and parallels the behavior of the overcrowdedalkene motors by yielding a full 3608 rotation from consecutive photochemical and thermal isomerization steps. However, rather than being powered by UV light, the photochemical steps of this motor are powered by non-destructive visible light, which is an advantage from the viewpoint of applications.…”

Section: R Ota R Y M Ol Ecu L a R Mot Orsmentioning

confidence: 99%

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Quantum chemical design of rotary molecular motors

Oruganti

Wang

Durbeej

2017

Int J of Quantum Chemistry

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This tutorial review describes how recent quantum chemical calculations and non-adiabatic molecular dynamics simulations have provided valuable guidelines and insights for the design of more powerful synthetic rotary molecular motors. Following a brief overview of the various types of rotary motors synthesized to date, we present computationally identified steric and electronic approaches to significantly reduce the free-energy barriers of the critical thermal isomerization steps of chiral overcrowded alkenes, a main class of motors whose potential for many different kinds of applications is well documented. Furthermore, we describe how computational research in this field has provided new motor designs that differ from overcrowded alkenes by either (1) completing a full 3608 rotation through fewer steps, (2) exhibiting more efficient photochemical steps, or (3) requiring fewer chiral features for their function, including a design that even in the absence of a stereocenter achieves unidirectional rotary motion from two Z/E photoisomerizations alone.chirality, molecular motors, non-adiabatic molecular dynamics, photoisomerization, steric interactions | I N TR ODU C TI ONIn this tutorial review, we give an account of how quantum chemical research has contributed to advance the field of artificial molecular machines.This field [1][2][3][4][5][6][7][8][9][10][11] is devoted to the fabrication of molecular systems capable of performing the same type of machine-like functions that Nature-made protein complexes carry out in order to, among other things, propel cells, store energy in cells, equip cells with transport systems, and generate biomechanical forces. [12][13][14] Although artificial molecular machines are yet to make an impact on our everyday lives, the field is currently undergoing a rapid expansion both in terms of what man-made molecules can accomplish and the areas of expertise of the scientists drawn to the field. In many ways, this development, envisioned already in 1959 by Richard Feynman in his prophetic "There's Plenty of Room at the Bottom" lecture, [15] is testament to the groundbreaking work on the design and synthesis of molecular machines [16][17][18][19][20][21][22][23][24][25] for which Jean-Pierre Sauvage, Sir J. Fraser Stoddart and Bernard (Ben) L. Feringa were awarded the Nobel Prize in Chemistry 2016.While a molecular machine can be defined as "an assembly of a discrete number of molecular components designed to perform mechanical-like movements (output) as a consequence of appropriate external stimuli (input)," [2] this tutorial review focuses on the subset of such systems known as molecular motors. Loosely speaking, molecular motors are molecules that can produce net work by absorbing external energy and converting the energy into directed (non-random) mechanical motion in a controllable fashion. The ability to produce net work is the distinguishing feature of molecular motors vis-a-vis molecular switches, the latter of which sustain back-and-forth motion but not the continuous m...

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Section: Other Mother Designs: Fewer Chiral Featuresmentioning

confidence: 99%

Section: R Ota R Y M Ol Ecu L a R Mot Orsmentioning

confidence: 99%

Section: R Ota R Y M Ol Ecu L a R Mot Orsmentioning

confidence: 99%

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Quantum chemical design of rotary molecular motors

Oruganti

Wang

Durbeej

2017

Int J of Quantum Chemistry

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“…Directional movement has been demonstrated in artificial molecular machines (1)(2)(3)(4), using photoexcitation (5)(6)(7)(8)(9)(10)(11) and/or the sequential addition of chemical reagents (12)(13)(14)(15)(16)(17)(18)(19)(20)(21)(22), and an autonomous chemically-driven molecular rotary motor that operates through a bio-inspired (23) information ratchet mechanism has been described (24,25). Here we report on an alternative class of ratchet mechanism, based on acid-base oscillations, that powers both rotary and linear molecular motors.…”

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confidence: 99%

Rotary and linear molecular motors driven by pulses of a chemical fuel

Erbaş-Çakmak

Fielden

Karaca

et al. 2017

Science

359

274

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Acid fuels the motion of a threaded ring A central goal in the construction of molecular-scale machines is the efficient achievement of one-way motion. Erbas-Cakmak et al. developed a class of machines that transmit pH changes into the two-stage guided motion of molecular rings threaded on a linear or cyclic axle. The design relies on temporary blocking groups and landing sites along the axle that toggle between active and passive states in response to acid or base. Trichloroacetic acid initiates the first stage of motion until it is decomposed by base in the solution, spurring the second phase. Science , this issue p. 340

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“…An important factor in the enhanced performances of this metasurface comes from the blackbody nature of the nanoparticles, whose darkness is maintained regardless light input conditions, [29] yielding an extremely high thermal efficiency. The combination of excellent stability to saline corrosion, [35] large scale fabrication, [30] ultralight weight (only 3.8 g of gold for 1 m 2 of metasurface) and 98% recyclability provides an ideal platform for solar steam generation in both industrial and academic oriented applications, which range from large scales desalination power plants and sterilization systems to steamdriven nanorachets, [42][43][44][45] demonstrating new possible concepts of plasmonic blackbody materials that could enrich our world in innovative ways.…”

Section: Discussionmentioning

confidence: 99%

High‐Performance Large‐Scale Solar Steam Generation with Nanolayers of Reusable Biomimetic Nanoparticles

Liu

Huang

Hsiung

et al. 2017

Advanced Sustainable Systems

160

119

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is currently based on structures floating on water. [11,13,17,[19][20][21][22] By using graphite membranes, the highest solar thermal efficiency (see Equation (4)) of 85% has been reported under an equivalent solar intensity of 10 suns. [13] One of the main drawback of this approach, besides the large light intensity requirement, lies in the fact that carbon-based systems (both graphite and graphene) are vulnerable to the contamination of pollutants or salt in the water, thus limiting the recyclability of the membrane after prolonged use.In this article, we developed a different approach, which makes use of a flat-optics metasurface [23][24][25][26][27][28] composed of suitably engineered plasmonic nanoparticles. [29,30] Plasmonics structures, thanks to the possibility of localizing light energy at the nanoscale, have demonstrated a great potential in converting light energy into heat for a variety of photothermal applications. [31][32][33][34] In plasmonic steam generation, the best results have been obtained with porous films, which reported efficiencies of ≈60% under 1 sun. [19,20] The efficiency limits of these structures originate from the resonant nature of classical plasmonic materials, which usually harvest energy only at characteristic frequencies of the solar spectrum. In our metasurface, we overcome this problem by using a completely new mechanism of heat generation supported by biomimetic nanoparticles that behave as an almost ideal blackbody. These nanoparticles mimic the shell of an Asian specie of beetle that possesses an exceptional ability in controlling light reflection. [29] Even when these nanoparticles are used in extremely small volumes, they completely absorb input photons at all frequencies and polarizations. By suitably dispersing these nanoparticles in a paper film, we created a metasurface with a remarkable ability in transforming light energy into heat, leading to a dramatic increase of solar thermal generation efficiency if compared to classical structures. Our nanoparticles are fully recyclable from the paper substrate and invulnerable to saline water corrosion, representing an ideal system for solar steam generation. [35] 2. Results Sample Design and Fabrication

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Sunlight-powered kHz rotation of a hemithioindigo-based molecular motor

Cited by 205 publications

References 43 publications

Quantum chemical design of rotary molecular motors

Quantum chemical design of rotary molecular motors

Rotary and linear molecular motors driven by pulses of a chemical fuel

High‐Performance Large‐Scale Solar Steam Generation with Nanolayers of Reusable Biomimetic Nanoparticles

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