Dissipative Self‐Assembly of Photoluminescent Silicon Nanocrystals

Biological assemblies such as chromosomes, membranes, and the cytoskeleton are driven out of equilibrium at the nanoscale by enzymatic activity and molecular motors. Similar non-equilibrium dynamics can be realized in synthetic systems, such as chemically fueled colloidal particles. Characterizing the stochastic non-equilibrium dynamics of such active soft assemblies still remains a challenge. Recently, new non-invasive approaches have been proposed to determine non-equilibrium behavior, which are based on detecting broken detailed balance in the stochastic trajectories of several coordinates of the system. Inspired by the method of two-point microrheology, in which the equilibrium fluctuations of a pair of probe particles reveal the viscoelastic response of an equilibrium system, here we investigate whether we can extend such an approach to non-equilibrium assemblies: can one extract information on the nature of the active driving in a system from the analysis of a two-point non-equilibrium measure? We address this question theoretically in the context of a class of elastic systems, driven out of equilibrium by a spatially heterogeneous stochastic internal driving. We consider several scenarios for the spatial features of the internal driving that may be relevant in biological and synthetic systems, and investigate how such features of the active noise may be reflected in the long-range scaling behavior of two-point non-equilibrium measures.

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“…(5). The simple configuration of a one-dimensional case allows us to replace the double index of the dipoles amplitudes {α D 12 , α D 23 , .…”

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confidence: 99%

Mesoscopic non-equilibrium measures can reveal intrinsic features of the active driving

2019

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“…Fourth, it will be interesting to develop NPs capable of responding simultaneously to light and other external stimuli (such as the recently developed “dual‐responsive” NPs assembling in response to light and magnetic fields). In this context, NPs self‐assembling in response to chemical fuels and light are particularly interesting. Fifth, in virtually all of the examples covered in this review, light‐induced self‐assembly of NPs was carried out in bulk solution.…”

Section: Discussionmentioning

confidence: 99%

The Many Ways to Assemble Nanoparticles Using Light

2019

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The ability to reversibly assemble nanoparticles using light is both fundamentally interesting and important for applications ranging from reversible data storage to controlled drug delivery. Here, the diverse approaches that have so far been developed to control the self-assembly of nanoparticles using light are reviewed and compared. These approaches include functionalizing nanoparticles with monolayers of photoresponsive molecules, placing them in photoresponsive media capable of reversibly protonating the particles under light, and decorating plasmonic nanoparticles with thermoresponsive polymers, to name just a few. The applicability of these methods to larger, micrometer-sized particles is also discussed. Finally, several perspectives on further developments in the field are offered.

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“…From a translational point of view, we expect to see exciting developments towards materials for the field of healthcare. To that end, we have recently demonstrated the use of time‐regulated nanoparticle assemblies to regulate the uptake of compounds by biological cells . In the future, such materials can be used to regulate cell behavior with temporal control thereby the field of regenerative medicine.…”

Section: Discussionmentioning

confidence: 99%

“…The field of synthetic molecular dissipative self‐assembly is still young, yet different types of molecular structures have been explored including vesicles, liquid crystals and assemblies of nanoparticles . Given the diversity of the assemblies that peptides can form, peptides and peptide‐derivatives have been a successful class of molecules to serve as building blocks for dissipative self‐assembly.…”

Section: Dissipative Self‐assembly Of Peptidesmentioning

confidence: 99%

Dissipative Self‐Assembly of Peptides

Tena‐Solsona

Boekhoven

2019

Israel Journal of Chemistry

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In molecular self‐assembly, molecules interact with each other by non‐covalent interactions to form larger structures. The process occurs in‐equilibrium, which means that molecules can leave the assembly and reassemble elsewhere, but that occurs on average with equal rates. For self‐assembly, peptides have proven to be a particularly useful building block, in part because of their versatility. Biology also uses self‐assembly to create functional materials. For example, components of the cytoskeleton, like actin filament and microtubules, are self‐assembled proteins. In other words, biology uses the same building blocks and design rules as supramolecular chemists to create functional structures. However, biological assemblies are vastly more complex than their synthetic counterparts. The discrepancy is in part because proteins are more complex than the peptides we use as building blocks. Another contributing factor to the difference in complexity is that most assemblies in living systems exist out of equilibrium. To use peptides for complex functions as biology does, we should understand and be able to create peptide assemblies out of equilibrium. In this work, we review recent advances towards the creation of peptide assemblies that exist out of equilibrium driven by an external energy source.

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Dissipative Self‐Assembly of Photoluminescent Silicon Nanocrystals

Cited by 100 publications

References 42 publications

Mesoscopic non-equilibrium measures can reveal intrinsic features of the active driving

Mesoscopic non-equilibrium measures can reveal intrinsic features of the active driving

The Many Ways to Assemble Nanoparticles Using Light

Dissipative Self‐Assembly of Peptides

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