Sixty Years of Surface-Specific Spectroscopy

Geiger, Franz M.; Hartland, Gregory V.

doi:10.1021/acs.jpcb.2c05020

Cited by 5 publications

(3 citation statements)

References 55 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…A common theme in determining the vibrational spectroscopy of water is unraveling site-specific interactions in water clusters, namely in characterizing the free and bound O–H stretches. Using linear spectroscopy, such as FTIR and Raman, can reveal essential information about hydrogen bond strengths and the local environment of water through the OH stretching mode frequency; however, these spectra often suffer from spectral congestion and band broadening. , Beyond purely vibrational spectroscopy, vibrational SFG has recently been used in visualizing the extent of interfacial water and probing water–surface interactions. ,, This technique improves upon pure IR measurements by distinct electronic excitations that suggest molecular locality and directionality in addition to characteristic vibrational modes. A special case of SFG is Second Harmonic Generation (SHG) spectra where the visible and IR excitation frequencies are identical; recent studies emphasizing second order nonlinear susceptibility measured in SHG have diminished some issues researchers have experienced in modeling more distinct features in charged interfaces and water–silica interfaces, − including acceptor–donor, acceptor–donor–donor (ADD), acceptor–acceptor–donor (AAD), as the main examples .…”

Section: Resultsmentioning

confidence: 99%

The Local Vibrational Mode Theory and Its Place in the Vibrational Spectroscopy Arena

et al. 2022

View full text Add to dashboard Cite

This Feature Article starts highlighting some recent experimental and theoretical advances in the field of IR and Raman spectroscopy, giving a taste of the breadth and dynamics of this striving field. The local mode theory is then reviewed, showing how local vibrational modes are derived from fundamental normal modes. New features are introduced that add to current theoretical efforts: (i) a unique measure of bond strength based on local mode force constants ranging from bonding in single molecules in different environments to bonding in periodic systems and crystals and (ii) a new way to interpret vibrational spectra by pinpointing and probing interactions between particular bond stretching contributions to the normal modes. All of this represents a means to work around the very nature of normal modes, namely that the vibrational motions in polyatomic molecules are delocalized. Three current focus points of the local mode analysis are reported, demonstrating how the local mode analysis extracts important information hidden in vibrational spectroscopy data supporting current experiments: (i) metal−ligand bonding in heme proteins, such as myoglobin and neuroglobin; (ii) disentanglement of DNA normal modes; and (iii) hydrogen bonding in water clusters and ice. Finally, the use of the local mode analysis by other research groups is summarized. Our vision is that in the future local mode analysis will be routinely applied by the community and that this Feature Article serves as an incubator for future collaborations between experiment and theory.

show abstract

Section: Resultsmentioning

confidence: 99%

The Local Vibrational Mode Theory and Its Place in the Vibrational Spectroscopy Arena

et al. 2022

View full text Add to dashboard Cite

show abstract

“…Strong electric elds have been reported by indirect measurements, 25 and one of the challenges is clearly to measure these eld strengths more directly, for instance, using nonlinear optical approaches. 26 In various environmental, biological, and technological contexts, water interfaces with charged surfaces. Fundamental questions remain about water and aqueous electrolyte solutions at charged interfaces.…”

mentioning

confidence: 99%

“…Strong electric fields have been reported by indirect measurements, 25 and one of the challenges is clearly to measure these field strengths more directly, for instance, using nonlinear optical approaches. 26 …”

mentioning

confidence: 99%