Structural properties of contractile gels based on light-driven molecular motors: a small-angle neutron and X-ray study

Mariani, Giacomo; Colard-Itté, Jean-Rémy; Moulin, Émilie; Giuseppone, Nicolas

doi:10.1039/d0sm00031k

Cited by 7 publications

(9 citation statements)

References 48 publications

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“…Researchers looking for applications of artificial molecular machines have focused their attention on surfaces ,,− porous crystals, − metal–organic frameworks, − ,− and monolayers − of single molecules. Artificial molecular machines have been incorporated into liquid crystalline phases and gels. − Motorized contractile gels have been developed by Giuseppone − who has integrated molecular motors into polymer chains. Medical science is set to benefit from artificial molecular machines acting as molecular prosthetics. − …”

Section: Discussionmentioning

confidence: 99%

Molecular Pumps and Motors

et al. 2021

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Pumps and motors are essential components of the world as we know it. From the complex proteins that sustain our cells, to the mechanical marvels that power industries, much we take for granted is only possible because of pumps and motors. Although molecular pumps and motors have supported life for eons, it is only recently that chemists have made progress toward designing and building artificial forms of the microscopic machinery present in nature. The advent of artificial molecular machines has granted scientists an unprecedented level of control over the relative motion of components of molecules through the development of kinetically controlled, away-from-thermodynamic equilibrium chemistry. We outline the history of pumps and motors, focusing specifically on the innovations that enable the design and synthesis of the artificial molecular machines central to this Perspective. A key insight connecting biomolecular and artificial molecular machines is that the physical motions by which these machines carry out their function are unambiguously in mechanical equilibrium at every instant. The operation of molecular motors and pumps can be described by trajectory thermodynamics, a theory based on the work of Onsager, which is grounded on the firm foundation of the principle of microscopic reversibility. Free energy derived from thermodynamically non-equilibrium reactions kinetically favors some reaction pathways over others. By designing molecules with kinetic asymmetry, one can engineer potential landscapes to harness external energy to drive the formation and maintenance of geometries of component parts of molecules awayfrom-equilibrium, that would be impossible to achieve by standard synthetic approaches.

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Section: Discussionmentioning

confidence: 99%

Molecular Pumps and Motors

et al. 2021

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“…This Lorentzian-like component of the empirical correlation-length model is related for m = 2 to the Ornstein–Zernike scattering function, which characterizes the correlation length ξ of semidilute polymer solutions and is the same mathematical form of an exact theoretical structure factor derived from the random phase approximation (RPA) for gels in theta solvents . By fitting the scattering to this scattering function, the average mesh size ξ mesh of a polymer network can be obtained (at the mean-field level). ,, …”

Section: Network Structurementioning

confidence: 99%

“…191 By fitting the scattering to this scattering function, the average mesh size ξ mesh of a polymer network can be obtained (at the mean-field level). 15,192,193 Contrast variation in SANS additionally offers the opportunity to selectively label and thereby selectively "visualize" specific network components. Scattering from labeled strands can be measured and analyzed to measure the molecular dimensions of strand subchains, entire chains, or cross-link junctions.…”

Section: Scatteringmentioning

confidence: 99%

Molecular Characterization of Polymer Networks

et al. 2021

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Polymer networks are complex systems consisting of molecular components. Whereas the properties of the individual components are typically well understood by most chemists, translating that chemical insight into polymer networks themselves is limited by the statistical and poorly defined nature of network structures. As a result, it is challenging, if not currently impossible, to extrapolate from the molecular behavior of components to the full range of performance and properties of the entire polymer network. Polymer networks therefore present an unrealized, important, and interdisciplinary opportunity to exert molecular-level, chemical control on material macroscopic properties. A barrier to sophisticated molecular approaches to polymer networks is that the techniques for characterizing the molecular structure of networks are often unfamiliar to many scientists. Here, we present a critical overview of the current characterization techniques available to understand the relation between the molecular properties and the resulting performance and behavior of polymer networks, in the absence of added fillers. We highlight the methods available to characterize the chemistry and molecular-level properties of individual polymer strands and junctions, the gelation process by which strands form networks, the structure of the resulting network, and the dynamics and mechanics of the final material. The purpose is not to serve as a detailed manual for conducting these measurements but rather to unify the underlying principles, point out remaining challenges, and provide a concise overview by which chemists can plan characterization strategies that suit their research objectives. Because polymer networks cannot often be sufficiently characterized with a single method, strategic combinations of multiple techniques are typically required for their molecular characterization.

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“…Giuseppone and colleagues reported on the formation of chemical gels incorporating such molecular motors as active crosslinks and in which the work produced by each motor is directly stored as elastic energy in the network [85]. Because the rotation of the motors under UV irradiation induces a twisting of pairs of polymer chains, the increasing number of crosslinks from entanglements triggers a contraction of the material (through syneresis), together with an increase of its elastic modulus [86]. Interestingly, this elastic energy can be released by integrating light-triggered diarylethene moieties as additional crosslinking units and through unwinding of the polymer chains.…”

Section: Extracting Continuous Mechanical Work From Molecular Systems and Materials By Implementing Ratchet Mechanismsmentioning

confidence: 99%

Extraction of mechanical work from stimuli-responsive molecular systems and materials

Perrot

Moulin

Giuseppone

2021

Trends in Chemistry

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Structural properties of contractile gels based on light-driven molecular motors: a small-angle neutron and X-ray study

Abstract: The collective rotation of light-driven molecular motors actuates the structural changes and macroscopic contraction of the chemical gels.

Cited by 7 publications

References 48 publications

Molecular Pumps and Motors

Molecular Pumps and Motors

Molecular Characterization of Polymer Networks

Extraction of mechanical work from stimuli-responsive molecular systems and materials

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