The adsorption of active polymers on an attractive nanoparticle (NP) is studied using Langevin dynamics simulations. The active polymers consist of an active Brownian particle (ABP) at the head and a subsequent passive polymer chain. The ABP experiences an active force of magnitude . The interactions between the active polymer and NP are modeled as Lennard-Jones potential with a strength . We find the critical adsorption point * increases with increasing the active force . The increment of *, denoted as Δ*, due to can be expressed approximately as Δ* ∝ for the restricted rotating active polymer (RRAP) where the rotation of the head ABP is restricted and Δ* ∝ for the freely rotating active polymer (FRAP) where the ABP rotates freely. Meanwhile, the conformation of the adsorbed polymer, such as adsorbed trains on NP and the tail near the ABP, are also dependent on . When the tail near the ABP is short, the adsorption is significantly affected by the active force. However, when the tail is long, the whole polymer can be viewed as a long tail stretched by the active force and unperturbed adsorption monomers. Simulation results show that the active force has a direct and significant effect on * and the structure of the adsorbed active polymers.
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Proc Natl Acad Sci U S A
January 2025
Applied Mathematics Laboratory, Courant Institute of Mathematical Sciences, Department of Mathematics, New York University, New York, NY 10012.
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View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
Department of Chemistry, Chemical Theory Center, University of Minnesota, Minneapolis, MN 55455-0431.
Multiconfiguration pair-density functional theory (MC-PDFT) was proposed a decade ago, but it is still in the early stage of density functional development. MC-PDFT uses functionals that are called on-top functionals; they depend on the density and the on-top pair density. Most MC-PDFT calculations to date have been unoptimized translations of generalized gradient approximations (GGAs) of Kohn-Sham density functional theory (KS-DFT).
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, BioInspired Institute, Syracuse University, Syracuse, New York 13244, United States.
Understanding structure-mechanical activity relationships (SMARs) in polymer mechanochemistry is essential for the rational design of mechanophores with desired properties, yet SMARs in noncovalent mechanical transformations remain relatively underexplored. In this study, we designed a subset of diarylethene mechanophores based on a lever-arm hypothesis and systematically investigated their mechanical activity toward a noncovalent-yet-chemical conversion of atropisomer stereochemistry. Results from Density functional theory (DFT) calculations, single-molecule force spectroscopy (SMFS) measurements, and ultrasonication experiments collectively support the lever-arm hypothesis and confirm the exceptional sensitivity of chemo-mechanical coupling in these atropisomers.
View Article and Find Full Text PDFAdv Sci (Weinh)
January 2025
School of Resources and Environment, University of Electronic Science and Technology of China, Chengdu, 611731, China.
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr-CsPbBr polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface.
View Article and Find Full Text PDFAppl Biochem Biotechnol
January 2025
Department of Botany, Maharshi Dayanand University, Rohtak, 124001, India.
Cellulase was effectively immobilized onto an epoxy-bound chitosan-modified zinc metal-organic framework (epoxy/ZIF-8/CS/cellulase) support, yielding a conjugation rate of 0.64 ± 0.02 mg/cm2 and retaining 80.
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