Directional control of a processive molecular hopper

Qing, Yujia; Ionescu, Sandra A.; Pulcu, Gökçe Su; Bayley, Hagan

doi:10.1126/science.aat3872

Cited by 83 publications

(108 citation statements)

References 51 publications

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“…Interestingly, the electrostatic force from the ΔΨ can be sufficiently strong to break a disulfide bond, permitting a subsequent large conformational change in the MP, as shown experimentally in the VGIC . Recently, an artificially designed, ΔΨ‐driven molecular motor running inside a membrane‐embedded channel was reported to operate using a similar, disulfide‐bond hopping mechanism …”

Section: Two‐state Rigid‐body Motion Is a Common Way To Utilize Electmentioning

confidence: 90%

Interplay between the electrostatic membrane potential and conformational changes in membrane proteins

Zhang

2019

Protein Science

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Transmembrane electrostatic membrane potential is a major energy source of the cell. Importantly, it determines the structure as well as function of charge‐carrying membrane proteins. Here, we discuss the relationship between membrane potential and membrane proteins, in particular whether the conformation of these proteins is integrally connected to the membrane potential. Together, these concepts provide a framework for rationalizing the types of conformational changes that have been observed in membrane proteins and for better understanding the electrostatic effects of the membrane potential on both reversible as well as unidirectional dynamic processes of membrane proteins.

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Section: Two‐state Rigid‐body Motion Is a Common Way To Utilize Electmentioning

confidence: 90%

Interplay between the electrostatic membrane potential and conformational changes in membrane proteins

Zhang

2019

Protein Science

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“…The mechanism of plasmon‐induced chemical reaction, a key route in photocatalysis, remained controversial over years due to the difficulty in directly observing such a process. In a recent study, STM was applied to realize for the first time the real‐space and real‐time monitoring of plasmon‐induced chemical reaction at a single molecule level . Through the comparison of the spatial distribution of isolated dimethyl disulfide (CH 3 S) 2 molecule on Ag or Cu surfaces before and after localized surface plasmon excitation, Figure , it was found that those (CH 3 S) 2 near the tip position could indeed split into two identical ball shaped protrusions, although the majority remained as elliptical.…”

Section: Manipulation Of Single Molecule Reactionmentioning

confidence: 99%

Section: Manipulation Of Single Molecule Reactionmentioning

confidence: 99%

Toward Precision Measurement and Manipulation of Single‐Molecule Reactions by a Confined Space

Qiu

Fato

Yuan

et al. 2019

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All chemical reactions can be divided into a series of single molecule reactions (SMRs), the elementary steps that involve only isomerization of, dissociation from, and addition to an individual molecule. Analyzing SMRs is of paramount importance to identify the intrinsic molecular mechanism of a complex chemical reaction, which is otherwise implausible to reveal in an ensemble fashion, owing to the significant static and dynamic heterogeneity of real‐world chemical systems. The single‐molecule measurement and manipulation methods developed recently are playing an increasingly irreplaceable role to detect and recognize short‐lived intermediates, visualize their transient existence, and determinate the kinetics and dynamics of single bond breaking and formation. Notably, none of the above SMRs characterizations can be realized without the aid of a confined space. Therefore, this Review aims to highlight the recent progress in the development of confined space enabled single‐molecule sensing, imaging, and tuning methods to study chemical reactions. Future prospects of SMRs research are also included, including a push toward the physical limit on transduction of information to signals and vice versa, transmission and recording of signals, computational modeling and simulation, and rational design of a confined space for precise SMRs.

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“…Communications Figure 2. Excerpts of 400 MHz 1 HNMR spectra (323 Ki nCDCl 3 )showing the amide resonances of 2 at 1mm (a) and in the presence of 3equiv of 5 after:b)5min;c)60min. and d) at equilibrium.…”

Section: Angewandte Chemiementioning

confidence: 99%

“…[1] Miniature artificial walkers have also been described. [2,3] Tr anslation directionality can be imposed when changing the preferred position of macrocycles on am olecular rod by means of an external stimulus.B iased Brownian motion then allows the system to relax to its new preferred state leading to anet flux from one station to the other. [4] Reverting the preferred position back to its original state leads to ar eversal of translation and shuttling is observed.…”

mentioning

confidence: 99%

Directional Threading and Sliding of a Dissymmetrical Foldamer Helix on Dissymmetrical Axles

et al. 2019

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We have investigated the self-assembly of adissymmetrical aromatic oligoamide helix on linear amido-carbamate rods.Adissymmetric sequence bearing two differentiated ends is able to wrap around dissymmetric dumbbell guest molecules. Structural and thermodynamic investigations allowed us to decipher the mode of binding of the helix that can bind specifically to the amide and carbamate groups of the rod. In parallel kinetic studies of threading and sliding of the helix along linear axles were also monitored by 1 HNMR. Results show that threading of adissymmetrical host can be kinetically biased by the nature of the guest terminus allowing ap referential sense of sliding of the helix. The study presented below further demonstrates the valuable potential of foldaxanes to combine designed molecular recognition patterns with fine control of self-assembly kinetics to conceive complex supramolecular events.Inspired by the molecular biomachinery,chemists have long tried to reproduce the controlled directional translations observed, for example,i nt he motion of DNAp olymerases along DNAt emplates or of kinesin proteins along microtubules.A bundant literature thus exists on the translation of macrocycles on rod-like molecular axles. [1] Miniature artificial walkers have also been described. [2,3] Tr anslation directionality can be imposed when changing the preferred position of macrocycles on am olecular rod by means of an external stimulus.B iased Brownian motion then allows the system to relax to its new preferred state leading to anet flux from one station to the other. [4] Reverting the preferred position back to its original state leads to ar eversal of translation and shuttling is observed. [5] Besides the directionality of the motion, the relative inherent orientation of the axle and the component that slides along it is an intriguing aspect that has less often been addressed. [6][7][8] This stems from the fact that most macrocycles that have been used as molecular shuttles have as ymmetrical structure.I nc ontrast dissymmetrical macrocycles,for example,cone-shaped calixarenes [6] cylodextrins [7] and others, [8] may thread onto ad issymmetrical axle. Thelack of symmetry allows for the definition of afront and ar ear of the shuttle,a nd also of frontward and backward motions.B ye xtension, one could imagine chemical transformations that would occur exclusively at the rear and favor forward motion, for example via ar atcheting mechanism induced by processive catalysis (i.e., the installation of stoppers on the rod), or via as elf-propelling mechanism. [9] As preliminary steps towards this goal, we herein present ad issymmetrical helix-rod host-guest system with av ery strong thermodynamic preference for ap articular relative helix/rod orientation (Figure 1a). We also show that kinetic bias in threading the rod into the helix cavity allows for the implementation of the directional motion of an oriented helix along an oriented rod.We have previously introduced multi-turn helical aromatic oligoamide foldamers that for...

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Directional control of a processive molecular hopper

Cited by 83 publications

References 51 publications

Interplay between the electrostatic membrane potential and conformational changes in membrane proteins

Interplay between the electrostatic membrane potential and conformational changes in membrane proteins

Toward Precision Measurement and Manipulation of Single‐Molecule Reactions by a Confined Space

Directional Threading and Sliding of a Dissymmetrical Foldamer Helix on Dissymmetrical Axles

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