Affiliation:
1. State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, and College of Chemistry and Chemical Engineering Xiamen University Xiamen People's Republic of China
2. Energy Materials & Devices Key Laboratory of Anhui Province, School of Physics and Photoelectric Engineering Anhui University Hefei People's Republic of China
3. College of Chemistry and Chemical Engineering Zhoukou Normal University Zhoukou People's Republic of China
Abstract
AbstractPlasmonic metal nanoparticles (PMNPs) are capable of localized surface plasmon resonance (LSPR) and have become an important component in many experimental settings, such as the surface‐enhanced spectroscopy and plasmonic photocatalysts, in which PMNPs are used to regulate the nearby molecular photophysical and photochemical behaviors by means of the complex interplay between the plasmon and molecular quantum transitions. Building computational models of these coupled plasmon‐molecule systems can help us better understand the bound molecular properties and reactivity, and make better decisions to design and control such systems. Ab initio modeling the nanosystem remains highly challenging. Many hybrid quantum‐classical (or ‐quantum) computing models have thus been developed to model the coupled systems, in which the molecular system of interest is designated as the quantum mechanical (QM) sub‐region and treated by the excited‐state electronic structure approaches such as the time‐dependent density functional theory (TDDFT), while the electromagnetic response of PMNPs is usually described using either a computational/classical electrodynamic (CED) model, polarizable continuum model(PCM), a polarizable molecular mechanics (MM) force field, or a collective of optical oscillators in QED model, leading to many hybrid approaches, such as QM/CED, QM/PCM, QM/MM or ab initio QED. In this review, we summarize recent advances in the development of these hybrid models as well as their advantages and limitations, with a specific emphasis on the TDDFT‐based approaches. Some numerical simulations on the plasmon‐enhanced absorption and Raman spectroscopy, plasmon‐driven water splitting reaction and interfacial electronic injection dynamics in dye‐sensitized solar cell are demonstrated.This article is categorized under:
Electronic Structure Theory > Ab Initio Electronic Structure Methods
Theoretical and Physical Chemistry > Spectroscopy
Software > Quantum Chemistry
Electronic Structure Theory > Combined QM/MM Methods
Funder
National Natural Science Foundation of China
Subject
Materials Chemistry,Computational Mathematics,Physical and Theoretical Chemistry,Computer Science Applications,Biochemistry