ArticleProceedings of the National Academy of Sciences of the United States of America2022
The dielectric function profile across the water interface through surface-specific vibrational spectroscopy and simulations.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2022. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 19 papers.
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19 citing papers in PubMed.
- Visible light leaves evaporation and interfacial structure of neat water unchanged at the air-water interface.Proceedings of the National Academy of Sciences of the United States of America · 2026Article
- When is nanoconfined water different from interfacial water?Faraday discussions · 2026Article
- Multipolar electric and magnetic contributions to sum-frequency generation spectra reveal biaxial interfacial water structure.Nature communications · 2026Article
- Electric fields at hydrophobic water interfaces: spectroscopic evidence, physical origin, and implications on reactivity.Chemical Society reviews · 2026Review
- Exposure of Selected Sunscreens to Artificial Sunlight Generates Persistent Free Radicals.Environmental science & technology letters · 2025Article
- Interfaces govern the structure of angstrom-scale confined water solutions.Nature communications · 2025Article
- Experimental quantification of nuclear quantum effects on the hydrogen bond of liquid water.Science advances · 2025Article
- Direct observation of carbon dioxide adsorption and binding at the air/aqueous interface.PNAS nexus · 2025Article
- Probing the Electric Double-Layer Capacitance to Understand the Reaction Environment in Conditions of Electrochemical Amination of Acetone.ACS applied materials & interfaces · 2025Article
- How Thick is the Air-Water Interface?─A Direct Experimental Measurement of the Decay Length of the Interfacial Structural Anisotropy.Langmuir : the ACS journal of surfaces and colloids · 2024Article
- Sum rule comparison of narrowband and broadband sum frequency generation spectra and comparison with theory.Proceedings of the National Academy of Sciences of the United States of America · 2024Article
- The role of charge in microdroplet redox chemistry.Nature communications · 2024Article
- Spontaneous Appearance of Triiodide Covering the Topmost Layer of the Iodide Solution Interface Without Photo-Oxidation.Environmental science & technology · 2024Article
- First-principles spectroscopy of aqueous interfaces using machine-learned electronic and quantum nuclear effects.Faraday discussions · 2024Article
- Fully First-Principles Surface Spectroscopy with Machine Learning.The journal of physical chemistry letters · 2023Article
- Article
- General Capacitance Upper Limit and Its Manifestation for Aqueous Graphene Interfaces.International journal of molecular sciences · 2023Article
- Ions Speciation at the Water-Air Interface.Journal of the American Chemical Society · 2023Article
- Polarization-Dependent Heterodyne-Detected Sum-Frequency Generation Spectroscopy as a Tool to Explore Surface Molecular Orientation and Ångström-Scale Depth Profiling.The journal of physical chemistry. B · 2022Review
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7 authors.
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Abstract
The dielectric properties of interfacial water on subnanometer length scales govern chemical reactions, carrier transfer, and ion transport at interfaces. Yet, the nature of the interfacial dielectric function has remained under debate as it is challenging to access the interfacial dielectric with subnanometer resolution. Here we use the vibrational response of interfacial water molecules probed using surface-specific sum-frequency generation (SFG) spectra to obtain exquisite depth resolution. Different responses originate from water molecules at different depths and report back on the local interfacial dielectric environment via their spectral amplitudes. From experimental and simulated SFG spectra at the air/water interface, we find that the interfacial dielectric constant changes drastically across an ∼1 Å thin interfacial water region. The strong gradient of the interfacial dielectric constant leads, at charged planar interfaces, to the formation of an electric triple layer that goes beyond the standard double-layer model.
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