ArticleScience advances2021
Tracking interfacial single-molecule pH and binding dynamics via vibrational spectroscopy.
Article in Science advances, 2021. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 12 papers.
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Who cites it
12 citing papers in PubMed, 24 citations in OpenAlex.
- Machine learning-powered single-molecule cancer diagnosis using DNA origami tags.Science advances · 2026Article
- Optical control of single-atom dynamics in plasmonic nanogaps.Science advances · 2025Article
- Impact of Surface Enhanced Raman Spectroscopy in Catalysis.ACS nano · 2024Review
- Spearheading a new era in complex colloid synthesis with TPM and other silanes.Nature reviews. Chemistry · 2024Review
- Efficient optical plasmonic tweezer-controlled single-molecule SERS characterization of pH-dependent amylin species in aqueous milieus.Nature communications · 2023Article
- Mapping Atomic-Scale Metal-Molecule Interactions: Salient Feature Extraction through Autoencoding of Vibrational Spectroscopy Data.The journal of physical chemistry letters · 2023Article
- Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering.Nature communications · 2023Article
- Picocavities: a Primer.Nano letters · 2022Article
- Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature.Nature communications · 2022Article
- Optical suppression of energy barriers in single molecule-metal binding.Science advances · 2022Article
- A 4D x-ray computer microtomography for high-temperature electrochemistry.Science advances · 2022Article
- Locating Single-Atom Optical Picocavities Using Wavelength-Multiplexed Raman Scattering.ACS photonics · 2021Article
Corrections and comments
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Authors and funding
7 authors at 1 institution in 1 country.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Understanding single-molecule chemical dynamics of surface ligands is of critical importance to reveal their individual pathways and, hence, roles in catalysis, which ensemble measurements cannot see. Here, we use a cascaded nano-optics approach that provides sufficient enhancement to enable direct tracking of chemical trajectories of single surface-bound molecules via vibrational spectroscopy. Atomic protrusions are laser-induced within plasmonic nanojunctions to concentrate light to atomic length scales, optically isolating individual molecules. By stabilizing these atomic sites, we unveil single-molecule deprotonation and binding dynamics under ambient conditions. High-speed field-enhanced spectroscopy allows us to monitor chemical switching of a single carboxylic group between three discrete states. Combining this with theoretical calculation identifies reversible proton transfer dynamics (yielding effective single-molecule pH) and switching between molecule-metal coordination states, where the exact chemical pathway depends on the intitial protonation state. These findings open new domains to explore interfacial single-molecule mechanisms and optical manipulation of their reaction pathways.
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Registered trials
Read under generation 80e0d062 · epoch 390. Bibliography from PubMed, PubMed Central and OpenAlex; grants from NIH RePORTER; trial links from ClinicalTrials.gov; estimates, votes and beliefs from the OpenQuestion graph.