A review of computational studies of bottlebrush polymers

Mohammadi, Esmat; Joshi, Soumil Y.; Deshmukh, Sanket A.

doi:10.1016/j.commatsci.2021.110720

Cited by 35 publications

(42 citation statements)

References 227 publications

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“…While commonly used in biophysical and biochemical studies, 107 MD simulations is an emergent tool to design soft materials. 108 − 111 However, realizing the full potential of this method requires new approaches to reduce the computational cost of multiscale modeling required to predict the properties of desired materials. 22 , 112 − 115 As shown here, the integration of machine learning can provide insights into design principles—a thermodynamically grounded understanding of the contribution of molecular syntax to a programmable assembly of hybrid materials.…”

Section: Discussionmentioning

confidence: 99%

“…Traditional brute-force material design, synthesis, and characterization strategies to elucidate the design principles of these hybrid materials are impractical given the large design space resulting from the orthogonality of protein, lipidation, and branching “building blocks.” Our proposed alternative strategy is to use MD simulations and data analytics to survey quickly and less expensively the hybrid design space and then experimentally verify results. While commonly used in biophysical and biochemical studies, MD simulations is an emergent tool to design soft materials. − However, realizing the full potential of this method requires new approaches to reduce the computational cost of multiscale modeling required to predict the properties of desired materials. ,− As shown here, the integration of machine learning can provide insights into design principlesa thermodynamically grounded understanding of the contribution of molecular syntax to a programmable assembly of hybrid materials. Elucidating these principles will foster the development of next-generation biomaterials and therapeutics whose forms and functions rival the exquisite hierarchy and capabilities of biological systems.…”

Section: Discussionmentioning

confidence: 99%

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Adaptive Recombinant Nanoworms from Genetically Encodable Star Amphiphiles

Hossain

Lynch

et al. 2021

Biomacromolecules

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Recombinant nanoworms are promising candidates for materials and biomedical applications ranging from the templated synthesis of nanomaterials to multivalent display of bioactive peptides and targeted delivery of theranostic agents. However, molecular design principles to synthesize these assemblies (which are thermodynamically favorable only in a narrow region of the phase diagram) remain unclear. To advance the identification of design principles for the programmable assembly of proteins into well-defined nanoworms and to broaden their stability regimes, we were inspired by the ability of topologically engineered synthetic macromolecules to acess rare mesophases. To test this design principle in biomacromolecular assemblies, we used post-translational modifications (PTMs) to generate lipidated proteins with precise topological and compositional asymmetry. Using an integrated experimental and computational approach, we show that the material properties (thermoresponse and nanoscale assembly) of these hybrid amphiphiles are modulated by their amphiphilic architecture. Importantly, we demonstrate that the judicious choice of amphiphilic architecture can be used to program the assembly of proteins into adaptive nanoworms, which undergo a morphological transition (sphere-to-nanoworms) in response to temperature stimuli.

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Adaptive Recombinant Nanoworms from Genetically Encodable Star Amphiphiles

Hossain

Lynch

et al. 2021

Biomacromolecules

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“…However, due to the limited resolution of available experimental techniques [53,54], it remains challenging to distinguish the bottlebrushes within clusters and characterize their conformations. Computational modeling allows one to understand and predict bottlebrush conformations under various conditions [5,22,23,51,52,[55][56][57][58][59][60][61][62][63][64]; current modeling efforts focusing on characterizing self-assembly of bottlebrushes are surveyed in a recent review by Mohmmadi et al [65].…”

Section: Introductionmentioning

confidence: 99%

Mesoscale Modeling of Agglomeration of Molecular Bottlebrushes: Focus on Conformations and Clustering Criteria

Choudhury

Giltner

et al. 2022

Polymers

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Using dissipative particle dynamics, we characterize dynamics of aggregation of molecular bottlebrushes in solvents of various qualities by tracking the number of clusters, the size of the largest cluster, and an average aggregation number. We focus on a low volume fraction of bottlebrushes in a range of solvents and probe three different cutoff criteria to identify bottlebrushes belonging to the same cluster. We demonstrate that the cutoff criteria which depend on both the coordination number and the length of the side chain allows one to correlate the agglomeration status with the structural characteristics of bottlebrushes in solvents of various qualities. We characterize conformational changes of the bottlebrush within the agglomerates with respect to those of an isolated bottlebrush in the same solvents. The characterization of bottlebrush conformations within the agglomerates is an important step in understanding the relationship between the bottlebrush architecture and material properties. An analysis of three distinct cutoff criteria to identify bottlebrushes belonging to the same cluster introduces a framework to identify both short-lived transient and long-lived agglomerates; the same approach could be further extended to characterize agglomerates of various macromolecules with complex architectures beyond the specific bottlebrush architecture considered herein.

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“…Molecular dynamics (MD) simulations have been routinely used as a powerful tool in studying the atomic-level structure and interactions between water and various substrates, including metals, polymers, and 2-D materials. − To successfully and reliably capture these atomic-level details, accurate force-field (FF) parameters between water and the substrate of interest must be utilized. Failure to capture accurate interactions between solvent and substrate can create unrealistically superhydrophilic or superhydrophobic surfaces .…”

Section: Introductionmentioning

confidence: 99%

Determination of Accurate Interaction Parameters between the Molybdenum Disulfide and Water to Investigate Their Interfacial Properties

et al. 2022

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Molybdenum disulfide (MoS 2 ), due to its many potential applications such as energy storage material, sensor, and lubricant, has attracted much attention from the scientific community. However, the environmental conditions like temperature, pressure, and, especially, humidity affect the performance of MoS 2 . Therefore, understanding the structure of water at the MoS 2 −water interface is critical to improve and design novel MoS 2 -based devices. In this study, we develop precise nonbonded interactions between MoS 2 represented by the Stillinger−Weber (SW) potential and three water models to reproduce its experimental macroscopic contact angle and the binding energies of water molecules obtained from quantum calculations. The forcefield (FF) parameter development was accelerated by integrating particle swarm optimization (PSO) algorithm with molecular dynamics (MD) simulations. Our systematic approach to develop these intermolecular potentials enabled us to reproduce the macroscopic contact angle of ∼63°−70°, which was in good agreement with experimental contact angles reported in the literature. Additionally, the structural properties of water such as z-density profile, orientation of O−H bonds near the MoS 2 surface, and hydrogen-bond distribution in different regions of a droplet were studied to gain the molecular level insights of the MoS 2 −water interface. This study not only provides a novel hybrid approach that integrated experimental and quantum calculations data to develop accurate FF parameters to study wettability of surfaces but also sheds a new light on structure of water at the MoS 2 −water interface.

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A review of computational studies of bottlebrush polymers

Cited by 35 publications

References 227 publications

Adaptive Recombinant Nanoworms from Genetically Encodable Star Amphiphiles

Adaptive Recombinant Nanoworms from Genetically Encodable Star Amphiphiles

Mesoscale Modeling of Agglomeration of Molecular Bottlebrushes: Focus on Conformations and Clustering Criteria

Determination of Accurate Interaction Parameters between the Molybdenum Disulfide and Water to Investigate Their Interfacial Properties

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