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Chemical Mapping of Nanoparticle–Ligand Interfaces in Optical Nanocavities

Year: 2025
Type: article
Abstract: Understanding processes in photon-phonon scattering, absorption, and chemical reactions in optical nanocavities is important for single-molecule sensors, single-photon emitters, and photocatalysis. However, the influence of electromagnetic fields, charge transfer, and molecular geometry is challenging to probe by ensemble-averaged spectroscopic techniques over multiple nanocavities. Photoinduced force microscopy (PiFM), which measures photoinduced polarizability under infrared excitation of a sample in the nanocavity between the scanning probe microscopy tip and sample surface, is used here for simultaneous nanoscale topological and chemical characterization. First-principles density functional theory (DFT) simulations of the vibrational spectra of gold nanoparticle surfaces functionalized with benzenedithiol (Au-BDT) elucidate molecular orientation, charge transfer, and oxidation state for understanding molecular and adatom reconfiguration in optical nanocavities in response to external fields.
DOI: 10.1021/jacs.5c05582
Authors: Chloe E. Groome, Hector Pascual-Herrero, Meagan E. Hill, Zhe Wang, Mariia Stepanova, Sahar Sharifzadeh, Maxim R. Shcherbakov, Ruqian Wu, Regina Ragan
Language: English
Open Access status: hybrid
Estimated APC paid: $4,500
Funders: National Science Foundation, University of California, Irvine, Division of Materials Research, Office of Advanced Cyberinfrastructure, Division of Chemical, Bioengineering, Environmental, and Transport Systems, Division of Electrical, Communications and Cyber Systems
Awards: G1135980590, G1422720434, G1453181110, UCI MRSEC: Materials Discovery Through Atomic Level Structural Design and Charge Control, G3526003852, Track 1: ACCESS Resource Allocations Marketplace and Platform Services (RAMPS), G4010157413, G4228951661, G4358414136, G5212984984, A Next-Generation Sensing Platform for Bacterial Metabolomics, G6965887028, G7360388406, G8243525310, Track 2: Customized Multi-tier Assistance, Training, and Computational Help (MATCH) for End User ACCESS to CI, CAREER: Bridging Infrared and Visible Photonics with Chip-ready Nonlinear and Quantum Metadevices, G8801403457, G97908232
OpenAlex ID: W4411284276
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Cites: 32
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