The Art of Building Small: From Molecular Switches to Motors (Nobel Lecture)

Feringa, Ben L.

doi:10.1002/anie.201702979

Cited by 629 publications

(547 citation statements)

References 141 publications

(149 reference statements)

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“…Nonetheless,i tis ac hallenge that the chemistry community has embraced increasingly during the past two decades with much of the teaching of the fundamental theory coming from the physics community,and, in particular, one very prominent physicist from the University of Maine,n amely Dean Astumian [45][46][47][48] with whom we have collaborated as well as published several reviews [49][50][51] that stand alongside acrop [52][53][54][55][56][57][58][59][60][61][62][63][64][65][66][67][68][69] that can be traced back for at least two decades from the present day.I nm yN obel Lecture,Ichose to highlight the progress [50,51] we have made in recent times on the design and synthesis of artificial molecular pumps,based on the building blocks that found their origins almost 40 years ago in the ICI Corporate Laboratory and were used by us [21][22][23][24][25][26][27] to put the mechanical bond on afirm footing before introducing [28] them into molecular switches in the first instance.…”

Section: Molecular Machinesmentioning

confidence: 99%

Mechanically Interlocked Molecules (MIMs)—Molecular Shuttles, Switches, and Machines (Nobel Lecture)

2017

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Section: Molecular Machinesmentioning

confidence: 99%

Mechanically Interlocked Molecules (MIMs)—Molecular Shuttles, Switches, and Machines (Nobel Lecture)

2017

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“…Although the push toward application of synthetic molecular machines (69)(70)(71) remains in its infancy (72), there have already been important insights provided to the fundamental aspects of the principles by which molecules use energy input from the environment to carry out mechanical and chemical tasks (73), including self-assembly of complex structures from simpler starting materials. A very important step has recently been taken by the research group of David Leigh.…”

Section: Prospective and Conclusionmentioning

confidence: 99%

Stochastically pumped adaptation and directional motion of molecular machines

Astumian

2018

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

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Recent developments in synthetic molecular motors and pumps have sprung from a remarkable confluence of experiment and theory. Synthetic accomplishments have facilitated the ability to design and create molecules, many of them featuring mechanically bonded components, to carry out specific functions in their environment-walking along a polymeric track, unidirectional circling of one ring about another, synthesizing stereoisomers according to an external protocol, or pumping rings onto a long rod-like molecule to form and maintain high-energy, complex, nonequilibrium structures from simpler antecedents. Progress in the theory of nanoscale stochastic thermodynamics, specifically the generalization and extension of the principle of microscopic reversibility to the single-molecule regime, has enhanced the understanding of the design requirements for achieving strong unidirectional motion and high efficiency of these synthetic molecular machines for harnessing energy from external fluctuations to carry out mechanical and/or chemical functions in their environment. A key insight is that the interaction between the fluctuations and the transition state energies plays a central role in determining the steady-state concentrations. Kinetic asymmetry, a requirement for stochastic adaptation, occurs when there is an imbalance in the effect of the fluctuations on the forward and reverse rate constants. Because of strong viscosity, the motions of the machine can be viewed as mechanical equilibrium processes where mechanical resonances are simply impossible but where the probability distributions for the state occupancies and trajectories are very different from those that would be expected at thermodynamic equilibrium. molecular machine | stochastic pumping | kinetic asymmetry The molecular machines necessary for life must carry out their function in the fluctuating environment of a biological cell. Nowhere is the dynamic aspect of biology at the molecular level more evident than in the bilayer membrane surrounding most cells and organelles, a small portion of which is shown schematically in Fig. 1. Three transmembrane proteins are included in the depiction: (i) an ion channel that provides a conduit for conduction of ions across the membrane; (ii) a molecule that facilitates the transport of some substance, S, across the membrane; and (iii), an NaATPase that uses energy from ATP hydrolysis to maintain ion gradients across the membrane. The transporter acts as a catalyst to reduce the barrier for transport of S. In and of itself, the transporter cannot drive the substance S from low to high chemical potential. The transporter, however, is near a possible source of energy, the ion channel. The ion channel provides a path for conduction of ions from high to low electrochemical potential, thus dissipating energy. Every time the ion channel opens or closes, the local electric field across the membrane changes, and because the flow of ions down the electrochemical gradient when the channel is open dissipates energy, the resulting ...

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“…[1][2][3] Fundamental developments have discovered fascinating phenomena and enabled a wealth of applications in the gas phase, [4][5][6][7][8] in solution, 4,[9][10][11] in crystals, 4,12 on surfaces, [4][5][6][13][14][15] and in biosystems. 16 Here we use a molecular model rotor to demonstrate the way from molecular quantum dynamics to explicitly time dependent statistical thermodynamics.…”

mentioning

confidence: 99%

“…The potential wells support thirty equivalent global minimum structures that are arranged in cyclic order, GM 1 , GM 2 , ..., GM 30 . These are separated from each other by thirty equivalent transition states, again in cyclic order, TS 1,2 , TS 2,3 , ..., TS 30,1 , and all with the same low potential barrier (V b ≈ 106.4 h c cm -1 ).…”

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confidence: 99%

From coherent quasi-irreversible quantum dynamics towards the second law of thermodynamics: The model boron rotor B13+

2018

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The planar boron cluster B13+ provides a model to investigate the microscopic origin of the second law of thermodynamics in a small system. It is a molecular rotor with an inner wheel that rotates in an outer bearing. The cyclic reaction path of B13+ passes along thirty equivalent global minimum structures (GMi, i = 1, 2, ..., 30). The GMs are embedded in a cyclic thirty-well potential. They are separated by thirty equivalent transition states with potential barrier Vb. If the boron rotor B13+ is prepared initially in one of the thirty GMs, with energy below Vb, then it tunnels sequentially to its nearest, next-nearest etc. neighbors (520 fs per step) such that all the other GMs get populated. As a consequence, the entropy of occupying the GMs takes about 6 ps to increases from zero to a value close to the maximum value for equi-distribution. Perfect recurrences are practically not observable.

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The Art of Building Small: From Molecular Switches to Motors (Nobel Lecture)

Cited by 629 publications

References 141 publications

Mechanically Interlocked Molecules (MIMs)—Molecular Shuttles, Switches, and Machines (Nobel Lecture)

Mechanically Interlocked Molecules (MIMs)—Molecular Shuttles, Switches, and Machines (Nobel Lecture)

Stochastically pumped adaptation and directional motion of molecular machines

From coherent quasi-irreversible quantum dynamics towards the second law of thermodynamics: The model boron rotor B13+

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