Combined IR-Raman vs vibrational sum-frequency heterospectral correlation spectroscopy

Roy, Sandra; Beutier, Clémentine; Hore, Dennis K.

doi:10.1016/j.molstruc.2018.01.072

Cited by 13 publications

(17 citation statements)

References 35 publications

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“…18,30,31 Overall, these spectra indicate that salts influence the appearance of the VSFG signal from BSA at the interface. We note the VSFG signal probes interfacial BSA only, and not the bulk BSA due to the electric field induced χ (3) term, [32][33][34][35][36][37][38][39][40][41][42][43] because of the large ionic strength (I=0.71 mol/L) used in this study.…”

Section: Resultsmentioning

confidence: 86%

Salting Up of Proteins at the Air/Water Interface

Shrestha

Luo

et al. 2019

Langmuir

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Vibrational sum frequency generation (VSFG) spectroscopy and surface pressure measurements are used to investigate the adsorption of a globular protein, bovine serum albumin (BSA), at the air/water interface with and without the presence of salts. We find at low (2 to 5 ppm) protein concentrations, which is relevant to environmental conditions, both VSFG and surface pressure measurements of BSA behave drastically different than at higher concentrations. Instead of emerging to the surface immediately, as observed at 1000 ppm, protein adsorption kinetics is on the order of tens of minutes at lower concentrations. Most importantly, salts strongly enhance the presence of BSA at the interface. This "salting up" effect differs from the well-known "salting out" effect as it occurs at protein concentrations wellbelow where "salting out" occurs. The dependence on salt concentration suggests this effect relates to a large extent electrostatic interactions and volume exclusion. Additionally, results from other proteins and the pH dependence of the kinetics indicate that salting up depends on the flexibility of proteins. This initial report demonstrates "salting up" as a new type of salt-driven interfacial phenomenon, which is worthy of continued investigation given the importance of salts in biological and environmental aqueous systems.

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Section: Resultsmentioning

confidence: 86%

Salting Up of Proteins at the Air/Water Interface

Shrestha

Luo

et al. 2019

Langmuir

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“…It is not a coincidence if the polarizability is involved in the Raman process. As a 3rd order non-linear process, Raman spectroscopy is driven by [63,68,69]:…”

Section: Raman Spectroscopymentioning

confidence: 99%

A Unified Mathematical Formalism for First to Third Order Dielectric Response of Matter: Application to Surface-Specific Two-Colour Vibrational Optical Spectroscopy

Humbert

Noblet

2021

Symmetry

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To take advantage of the singular properties of matter, as well as to characterize it, we need to interact with it. The role of optical spectroscopies is to enable us to demonstrate the existence of physical objects by observing their response to light excitation. The ability of spectroscopy to reveal the structure and properties of matter then relies on mathematical functions called optical (or dielectric) response functions. Technically, these are tensor Green’s functions, and not scalar functions. The complexity of this tensor formalism sometimes leads to confusion within some articles and books. Here, we do clarify this formalism by introducing the physical foundations of linear and non-linear spectroscopies as simple and rigorous as possible. We dwell on both the mathematical and experimental aspects, examining extinction, infrared, Raman and sum-frequency generation spectroscopies. In this review, we thus give a personal presentation with the aim of offering the reader a coherent vision of linear and non-linear optics, and to remove the ambiguities that we have encountered in reference books and articles.

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“…We have recently illustrated the utility of generating a bulk vibrational spectrum where each resonance is described by an oscillator strength that is the product of the IR transition dipole moment and the Raman transition polarizability. 38 Such spectra, although never realized in any experiment, are particularly useful for comparison with SFG spectra. This is because the vibrational hyperpolarizability may be expressed as the product of these two quantities.…”

Section: Composite Ir-raman Spectramentioning

confidence: 99%

“…In Ref. 38, we describe the detailed procedure for generating these spectra from the experimental Im{χ (1) } and Im{χ (3) } spectra to produce a spectrum with oscillator strength ∂α/∂Q ∂µ/∂Q , rather than ∂α/∂Q • ∂µ/∂Q . Here, ∂α/∂Q is the polarizability derivative with respect to the normal mode coordinate, and ∂µ/∂Q is the corresponding dipole moment derivative, both evaluated at the equilibrium geometry.…”

Section: Composite Ir-raman Spectramentioning

confidence: 99%

“…The homospectral correlation is generally more featurerich when applied to SFG data, as both the orientation and population of molecules at the surface contribute to the intensity of the vibrational modes. 38,[62][63][64] For example, a particular mode may have a strong IR transition dipole moment and Raman transition polarizability, but that part of the molecule may be oriented close to the plane of the surface, significantly reducing its intensity in the case of our C ∞v symmetry. The orientation and symmetry consideration is the dominant contribution to the SFG, as even molecules with strong IR and Raman transitions are SFG-silent in the bulk solution phase.…”

Section: Surface Homospectral Correlationmentioning

confidence: 99%

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Adsorption of heptane–toluene binary mixtures on a hydrophobic polymer surface

Ramsay

Beutier

McGarvey

et al. 2019

The Journal of Chemical Physics

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Paper published as part of the special topic on Nonlinear Spectroscopy and Interfacial Structure and Dynamics Note: This article is part of the Special Topic "Nonlinear Spectroscopy and Interfacial Structure and Dynamics" in J. Chem. Phys. ARTICLES YOU MAY BE INTERESTED IN Water structure at the interface of alcohol monolayers as determined by molecular dynamics simulations and computational vibrational sum-frequency generation spectroscopy

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Combined IR-Raman vs vibrational sum-frequency heterospectral correlation spectroscopy

Cited by 13 publications

References 35 publications

Salting Up of Proteins at the Air/Water Interface

Salting Up of Proteins at the Air/Water Interface

A Unified Mathematical Formalism for First to Third Order Dielectric Response of Matter: Application to Surface-Specific Two-Colour Vibrational Optical Spectroscopy

Adsorption of heptane–toluene binary mixtures on a hydrophobic polymer surface

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