Atomistic Multiscale Modeling of Colloidal Plasmonic Nanoparticles

Area of Science:

• Computational Chemistry
• Materials Science
• Nanotechnology

Background:

• Plasmonic nanoparticles (NPs) exhibit unique optical properties crucial for various applications.
• Accurately modeling the optical response of solvated NPs requires accounting for complex NP-solvent interactions.
• Existing methods may lack the accuracy or efficiency for real-size, solvated plasmonic systems.

Purpose of the Study:

• To present a novel, fully atomistic multiscale classical approach for modeling the optical response of solvated plasmonic nanoparticles.
• To incorporate mutual interactions between plasmonic substrates and surrounding solvent molecules.
• To provide a flexible and reliable method for simulating diverse plasmonic systems.

Main Methods:

• Coupling the Frequency Dependent Fluctuating Charges and Fluctuating Dipoles (ωFQFμ) model for plasmonic substrates.
• Utilizing the polarizable Fluctuating Charges (FQ) classical force field for the solvating environment.
• Integrating NP-radiation and NP-solvent interactions within a unified ωFQFμ/FQ framework.

Main Results:

• The ωFQFμ/FQ approach demonstrates remarkable accuracy in reproducing optical responses.
• The model accurately predicts plasmon resonance frequency shifts, especially for sub-quantum-size NPs.
• Successful simulations of homogeneous and bimetallic NPs in various solvents showcase the method's flexibility.

Conclusions:

• The developed ωFQFμ/FQ approach offers a powerful tool for simulating optical properties of solvated plasmonic nanoparticles.
• This method provides high accuracy and flexibility, advancing the computational study of plasmonic systems.
• The approach is validated and ready for application to complex NP-solvent systems.