4.5 Review

Sum frequency generation vibrational spectroscopy (SFG-VS) for complex molecular surfaces and interfaces: Spectral lineshape measurement and analysis plus some controversial issues

Journal

PROGRESS IN SURFACE SCIENCE
Volume 91, Issue 4, Pages 155-182

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.progsurf.2016.10.001

Keywords

Sum-frequency generation vibrational spectroscopy; Surface selectivity; Surface nonlinear spectroscopy; Surfaces and interfaces; Molecular orientation; Dipole contribution; Phase-resolved SFG-VS; Chiral SFG-VS; Vibrational spectral lineshape; Bloch dynamics model

Funding

  1. Materials Synthesis and Simulation Across Scales (MS3) Initiative through the LDRD program at Pacific Northwest National Laboratory (PNNL)
  2. Department of Energy (DOE) [DE-AC05-76RL01830]
  3. DOE's Office of Biological and Environmental Research (BER)

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Sum-frequency generation vibrational spectroscopy (SFG-VS) was first developed in the 1980s and it has been proven a uniquely sensitive and surface/interface selective spectroscopic probe for characterization of the structure, conformation and dynamics of molecular surfaces and interfaces. In recent years, there have been many progresses in the development of methodology and instrumentation in the SFG-VS toolbox that have significantly broadened the application to complex molecular surfaces and interfaces. In this review, after presenting a unified view on the theory and methodology focusing on the SFG-VS spectral lineshape, as well as the new opportunities in SFG-VS applications with such developments, some of the controversial issues that have been puzzling the community are discussed. The aim of this review is to present to the researchers and students interested in molecular surfaces and interfacial sciences up-to-date perspectives complementary to the existing textbooks and reviews on SFG-VS. (C) 2016 Elsevier Ltd. All rights reserved.

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