ArticleProceedings of the National Academy of Sciences of the United States of America2011
Adding a dimension to the infrared spectra of interfaces using heterodyne detected 2D sum-frequency generation (HD 2D SFG) spectroscopy.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2011. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 31 papers.
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31 citing papers in PubMed.
- Mixed Domain IR-Hyper-Raman Four Wave Mixing Spectroscopy.The journal of physical chemistry letters · 2026Article
- Frequency-Dependent Vibrational Relaxation Time of OH Stretch at the Air/Isotopically Diluted Water Interface.The journal of physical chemistry letters · 2025Article
- The Role of Sum-Frequency Generation Spectroscopy in Understanding On-Surface Reactions and Dynamics in Atmospheric Model-Systems.The journal of physical chemistry letters · 2024Review
- Unified picture of vibrational relaxation of OH stretch at the air/water interface.Nature communications · 2024Article
- Multimodal Nonlinear Hyperspectral Chemical Imaging Using Line-Scanning Vibrational Sum-Frequency Generation Microscopy.Journal of visualized experiments : JoVE · 2023Article
- Breaking Barriers in Ultrafast Spectroscopy and Imaging Using 100 kHz Amplified Yb-Laser Systems.Accounts of chemical research · 2023Article
- Development of Two-Dimensional Electronic-Vibrational Sum Frequency Generation (2D-EVSFG) for Vibronic and Solvent Couplings of Molecules at Interfaces and Surfaces.ACS physical chemistry Au · 2023Article
- Article
- An Evaluation of Maximum Determination Methods for Center Line Slope Analysis.The journal of physical chemistry. B · 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
- Two-dimensional electronic-vibrational sum frequency spectroscopy for interactions of electronic and nuclear motions at interfaces.Proceedings of the National Academy of Sciences of the United States of America · 2021Article
- Developments and Ongoing Challenges for Analysis of Surface-Bound Proteins.Annual review of analytical chemistry (Palo Alto, Calif.) · 2021Article
- The photochemical reaction of phenol becomes ultrafast at the air-water interface.Nature chemistry · 2021Article
- Spatially dependent H-bond dynamics at interfaces of water/biomimetic self-assembled lattice materials.Proceedings of the National Academy of Sciences of the United States of America · 2020Article
- Molecular Structure and Modeling of Water-Air and Ice-Air Interfaces Monitored by Sum-Frequency Generation.Chemical reviews · 2020Article
- Structure from Dynamics: Vibrational Dynamics of Interfacial Water as a Probe of Aqueous Heterogeneity.The journal of physical chemistry. B · 2018Article
- Recent advances in multidimensional ultrafast spectroscopy.Royal Society open science · 2018Review
- Second-order spectral lineshapes from charged interfaces.Nature communications · 2017Article
- Watching Proteins Wiggle: Mapping Structures with Two-Dimensional Infrared Spectroscopy.Chemical reviews · 2017Review
- Molecule-specific interactions of diatomic adsorbates at metal-liquid interfaces.Structural dynamics (Melville, N.Y.) · 2017Article
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4 authors.
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Abstract
In the last ten years, two-dimensional infrared spectroscopy has become an important technique for studying molecular structures and dynamics. We report the implementation of heterodyne detected two-dimensional sum-frequency generation (HD 2D SFG) spectroscopy, which is the analog of 2D infrared (2D IR) spectroscopy, but is selective to noncentrosymmetric systems such as interfaces. We implement the technique using mid-IR pulse shaping, which enables rapid scanning, phase cycling, and automatic phasing. Absorptive spectra are obtained, that have the highest frequency resolution possible, from which we extract the rephasing and nonrephasing signals that are sometimes preferred. Using this technique, we measure the vibrational mode of CO adsorbed on a polycrystalline Pt surface. The 2D spectrum reveals a significant inhomogenous contribution to the spectral line shape, which is quantified by simulations. This observation indicates that the surface conformation and environment of CO molecules is more complicated than the simple "atop" configuration assumed in previous work. Our method can be straightforwardly incorporated into many existing SFG spectrometers. The technique enables one to quantify inhomogeneity, vibrational couplings, spectral diffusion, chemical exchange, and many other properties analogous to 2D IR spectroscopy, but specifically for interfaces.
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