Progress toward a Rationally Designed Molecular Motor

Kelly, T. Ross

doi:10.1021/ar000167x

Cited by 247 publications

(121 citation 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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“…Synthetic motor-molecules (7)(8)(9)(10)(11), which are designed to excel where their biological counterparts fall short, also have been investigated. Whereas devices powered by biological molecules require (4-6) chemical diffusion for actuation stimulus, synthetic molecules have been shown (2,9) to operate with a variety of different stimuli, thereby lending much greater flexibility to a particular system's design.…”

Section: Olecular Motors Have Recently Garnered Considerable In-mentioning

confidence: 99%

Evaluation of synthetic linear motor-molecule actuation energetics

Brough¹,

Northrop

Schmidt

et al. 2006

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

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By applying atomic force microscope (AFM)-based force spectroscopy together with computational modeling in the form of molecular force-field simulations, we have determined quantitatively the actuation energetics of a synthetic motor-molecule. This multidisciplinary approach was performed on specifically designed, bistable, redox-controllable [2]rotaxanes to probe the steric and electrostatic interactions that dictate their mechanical switching at the single-molecule level. The fusion of experimental force spectroscopy and theoretical computational modeling has revealed that the repulsive electrostatic interaction, which is responsible for the molecular actuation, is as high as 65 kcal⅐mol ؊1 , a result that is supported by ab initio calculations.computational modeling ͉ force spectroscopy ͉ molecular motors ͉ switchable rotaxanes M olecular motors have recently garnered considerable interest within the domains of microsciences and nanosciences (1, 2). Harnessing the ability to selectively, cooperatively, and repeatedly induce structural changes in molecules may hold the promise of engineered systems that operate with the same complexity, elegance, and efficiency as biological motors function in the human body. In natural systems, it has become apparent that both macro and micro processes are initiated and controlled by nanoscale molecular motors (3). For example, myosin and kinesin are associated with muscle contraction and intracellular trafficking, respectively, and have recently found their ways into engineered devices (4, 5). Moreover, initial work has been performed that demonstrates the ability of natural nanoscale molecular motors to power microfabricated systems (6).Synthetic motor-molecules (7-11), which are designed to excel where their biological counterparts fall short, also have been investigated. Whereas devices powered by biological molecules require (4-6) chemical diffusion for actuation stimulus, synthetic molecules have been shown (2, 9) to operate with a variety of different stimuli, thereby lending much greater flexibility to a particular system's design. Moreover, a synthetic nanoscale actuating molecule carries with it an inherent ability to be modified and optimized precisely for a specific task.Switchable, bistable rotaxanes (2, 9), compounds comprised of a dumbbell-shaped component containing two different recognition sites for an encircling ring-shaped component, show particular promise as molecular actuators, given their ability to undergo controllable, reversible mechanical switching with the appropriate chemical, electrochemical, or photochemical stimulus in solution. Toward the goal of device applications, switching has been shown to operate in condensed phases such as in a polymer electrolyte gel (12), on a self-assembled monolayer (SAM) (13), on the solid supports of engineered systems (14), and in molecular switch tunnel junctions (15). Bistable rotaxanes benefit from their synthesis being highly modular, a virtue that allows for a considerable degree of flexibility in their des...

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“…However, complexation of both bipyridyl nitrogens to a metal (normally Hg 2+ ) forces a pyridine ring hydrogen in between two of the blades of the paddlewheel and breaks its three-fold symmetry, as shown in Scheme 19 [64]. …”

Section: Triptycenes As Components Of Molecular Brakesmentioning

confidence: 99%

Symmetry Breaking in NMR Spectroscopy: The Elucidation of Hidden Molecular Rearrangement Processes

McGlinchey¹

2014

Symmetry

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Variable-temperature NMR spectroscopy is probably the most convenient and sensitive technique to monitor changes in molecular structure in solution. Rearrangements that are rapid on the NMR time-scale exhibit simplified spectra, whereby non-equivalent nuclear environments yield time-averaged resonances. At lower temperatures, when the rate of exchange is sufficiently reduced, these degeneracies are split and the underlying "static" molecular symmetry, as seen by X-ray crystallography, becomes apparent. Frequently, however, such rearrangement processes are hidden, even when they become slow on the NMR time-scale, because the molecular point group remains unchanged. Judicious symmetry breaking, such as by substitution of a molecular fragment by a similar, but not identical moiety, or by the incorporation of potentially diastereotopic (chemically non-equivalent) nuclei, allows the elucidation of the kinetics and energetics of such processes. Examples are chosen that include a wide range of rotations, migrations and other rearrangements in organic, inorganic and organometallic chemistry.

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Progress toward a Rationally Designed Molecular Motor

Cited by 247 publications

References 11 publications

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

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

Evaluation of synthetic linear motor-molecule actuation energetics

Symmetry Breaking in NMR Spectroscopy: The Elucidation of Hidden Molecular Rearrangement Processes

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