Molybdenum disulfide (MoS 2 ) is a layered material with outstanding electrical and optical properties. Numerous studies evaluate the performance in sensors, catalysts, batteries, and composites that can benefit from guidance by simulations in all-atom resolution. However, molecular simulations remain difficult due to lack of reliable models. We introduce an interpretable force field for MoS 2 with record performance that reproduces structural, interfacial, and mechanical properties in 0.1% to 5% agreement with experiments. The model overcomes structural instability, deviations in interfacial and mechanical properties by several 100%, and empirical fitting protocols in earlier models. It is compatible with several force fields for molecular dynamics simulation, including the interface force field (IFF), CVFF, DREIDING, PCFF, COMPASS, CHARMM, AMBER, and OPLS-AA. The parameters capture polar covalent bonding, X-ray structure, cleavage energy, infrared spectra, bending stability, bulk modulus, Young's modulus, and contact angles with polar and nonpolar solvents. We utilized the models to uncover the binding mechanism of peptides to the MoS 2 basal plane. The binding strength of several 7mer and 8mer peptides scales linearly with surface contact and replacement of surface-bound water molecules, and is tunable in a wide range from −86 to −6 kcal mol −1 . The binding selectivity is multifactorial, including major contributions by van-der-Waals coordination and charge matching of certain side groups, orientation of hydrophilic side chains towards water, and conformation flexibility. We explain the relative attraction and role of the 20 amino acids using computational and experimental data. The force field can be used to screen and interpret the assembly of MoS 2 -based nanomaterials and electrolyte interfaces up to a billion atoms with high accuracy, including multiscale simulations from the quantum scale to the microscale.
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Atomistic mechanisms of adhesion and shear strength in graphene oxide-polymer interfaces
Combining experimental and computational studies of nanocomposite interfaces is highly needed to gain insight into their performance. However, there are very few literature reports, combining well-controlled atomic force microscopy experiments with molecular dynamic simulations, which explore the role of polymer chemistry and assembly on interface adhesion and shear strength. In
this work, we investigate graphene oxide (GO)-polymer interfaces prevalent in nanocomposites based on a nacre-like architectures. We examine the interfacial strength resulting from van der Waals and hydrogen bonding interactions by comparing the out-of-plane separation and in-plane shear deformations of GO-polyethylene glycol (PEG) and GO-polyvinyl alcohol (PVA). The
investigation reveals an overall better mechanical performance for the anhydrous GO-PVA system in both out-of-plane and in-plane deformation modes, highlighting the benefits of the donor-acceptor hydrogen bond formation present in GO-PVA. Such bond formation results in interchain hydrogen bond networks leading to stronger interfaces. By contrast, PEG, a hydrogen
bond acceptor only, relies primarily on van der Waals inter-chain interactions, typically resulting in weaker interactions. The study also predicts that water addition increases the adhesion of GOPEG but decreases the adhesion of GO-PVA, and slightly increases the shear strength in both systems. Furthermore, by comparing simulations and experiments, we show that the CHARMM force field has enough accuracy to capture the effect of polymer content, water distribution, and to provide quantitative guidance for achieving optimum interfacial properties. Therefore, the study demonstrates an effective methodology, in the Materials Genome spirit, toward the design of 2D materials-polymer nanocomposites system for applications demanding mechanical robustness.
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- Award ID(s):
- 1953806
- NSF-PAR ID:
- 10333628
- Date Published:
- Journal Name:
- Journal of the mechanics and physics of solids
- Volume:
- 156
- ISSN:
- 0022-5096
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Van der Waals semiconductors (vdWS) offer superior mechanical and electrical properties and are promising for flexible microelectronics when combined with polymer substrates. However, the self‐passivated vdWS surfaces and their weak adhesion to polymers tend to cause interfacial sliding and wrinkling, and thus, are still challenging the reliability of vdWS‐based flexible devices. Here, an effective covalent vdWS–polymer lamination method with high stretch tolerance and excellent electronic performance is reported. Using molybdenum disulfide (MoS2)and polydimethylsiloxane (PDMS) as a case study, gold–chalcogen bonding and mercapto silane bridges are leveraged. The resulting composite structures exhibit more uniform and stronger interfacial adhesion. This enhanced coupling also enables the observation of a theoretically predicted tension‐induced band structure transition in MoS2. Moreover, no obvious degradation in the devices’ structural and electrical properties is identified after numerous mechanical cycle tests. This high‐quality lamination enhances the reliability of vdWS‐based flexible microelectronics, accelerating their practical applications in biomedical research and consumer electronics.
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Accepted Manuscript1.0
- Journal Article:
- The DOI is not currently available.
