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Nonlinear Optical Methods for Characterization of Molecular Structure and Surface Chemistry

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Abstract

The principles, strengths and limitations of several nonlinear optical (NLO) methods for characterizing biological systems are reviewed. NLO methods encompass a wide range of approaches that can be used for real-time, in-situ characterization of biological systems, typically in a label-free mode. Multiphoton excitation fluorescence (MPEF) is widely used for high-quality imaging based on electronic transitions, but lacks interface specificity. Second harmonic generation (SHG) is a parametric process that has all the virtues of the two-photon version of MPEF, yielding a signal at twice the frequency of the excitation light, which provides interface specificity. Both SHG and MPEF can provide images with high structural contrast, but they typically lack molecular or chemical specificity. Other NLO methods such as coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS) can provide high-sensitivity imaging with chemical information since Raman active vibrations are probed. However, CARS and SRS lack interface and surface specificity. A NLO method that provides both interface/surface specificity as well as molecular specificity is vibrational sum frequency generation (SFG) spectroscopy. Vibration modes that are both Raman and IR active are probed in the SFG process, providing the molecular specificity. SFG, like SHG, is a parametric process, which provides the interface and surface specificity. SFG is typically done in the reflection mode from planar samples. This has yielded rich and detailed information about the molecular structure of biomaterial interfaces and biomolecules interacting with their surfaces. However, 2-D systems have limitations for understanding the interactions of biomolecules and interfaces in the 3-D biological environment. The recent advances made in instrumentation and analysis methods for sum frequency scattering (SFS) now present the opportunity for SFS to be used to directly study biological solutions. By detecting the scattering at angles away from the phase-matched direction even centrosymmetric structures that are isotropic (e.g., spherical nanoparticles functionalized with self-assembled monolayers or biomolecules) can be probed. Often a combination of multiple NLO methods or a combination of a NLO method with other spectroscopic methods is required to obtain a full understanding of the molecular structure and surface chemistry of biomaterials and the biomolecules that interact with them. Using the right combination methods provides a powerful approach for characterizing biological materials.

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Figure 1b is reproduced with permission from Ref. [53], copyright 2002 National Academy of Sciences

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Reproduced with permission from Ref. [64], copyright 2015 John Wiley and Sons

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b is reproduced with permission from Ref. [8], copyright 2008 American Association for the Advancement of Science

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Reproduced with permission from Ref. [79], copyright 2015 American Chemical Society

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Fig. 7

Reproduced with permission from Ref. [101], copyright 2003 American Chemical Society

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Reproduced with permission from Ref. [106], copyright 2013 American Chemical Society

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Reproduced with permission from Ref. [115], copyright 2009 American Institute of Physics Publishing

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Reproduced with permission from Ref. [168], copyright 2010 American Institute of Physics

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Reproduced with permission from Ref. [174], copyright 2017 Nature Publishing Group

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Acknowledgements

The authors gratefully acknowledge the support of NIH grant EB-002027 during the preparation of this manuscript as well as both NIH grant EB-002027 and NSF grant CBET-1125791 for some of the results described in it. We also thank our colleagues for many stimulating discussions about non-linear optical spectroscopy and microscopy over the years, especially Professor Gabor A. Somorjai for his leadership in developing and showing the impact of vibration SFG for obtaining detailed molecular information about surfaces and interfaces.

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  1. Departments of Bioengineering & Chemical Engineering, National ESCA & Surface Analysis Center for Biomedical Problems, Molecular Engineering & Sciences Institute, University of Washington, Seattle, WA, 98195-1653, USA

    Patrik K. Johansson, Lars Schmüser & David G. Castner

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Johansson, P.K., Schmüser, L. & Castner, D.G. Nonlinear Optical Methods for Characterization of Molecular Structure and Surface Chemistry. Top Catal 61, 1101–1124 (2018). https://doi.org/10.1007/s11244-018-0924-3

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