New Tools for Surface Second-Harmonic Generation

Simpson, Garth J.

doi:10.1366/0003702011951245

Cited by 26 publications

(35 citation statements)

References 202 publications

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“…Although SFG has been predicted and observed in the bulk from chiral solutions, the intensity of the nonlinear field attributed to chiral interactions was typically four to six orders of magnitude weaker than for analogous SHG measurements of oriented chiral surface systems. 27,[29][30][31] The relative values of all nonzero elements of the complex ␤ (2) tensor can be determined by summing together the contributions from all the excited states and projection onto the internal molecular coordinates: 11,36 ␤ i jk…”

Section: Theorymentioning

confidence: 99%

“…3,5 In the limiting cases in which only one or two elements of the ␤ (2) tensor are significant, the measured nonlinearity of the surface film ͑described by the (2) tensor͒ can be used to interpret parameters related to molecular orientation using fairly simple expressions. [1][2][3][4][5][6][7][9][10][11] In contrast, chromophores of low symmetry generally have unique nonzero values for all 18 independent elements of the ␤ (2) tensor for second harmonic generation and all 27 for sum frequency generation ͑SFG͒. This striking increase in the number of contributing elements of the ␤ (2) tensor has restricted meaningful extraction of orientation information in systems of low symmetry, including chiral films.…”

Section: Introductionmentioning

confidence: 99%

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Molecular and surface hyperpolarizability of oriented chromophores of low symmetry

2002

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In chromophores of low symmetry, including chiral species, modeling calculations generally do not produce the most convenient set of coordinates for evaluating the molecular second order nonlinear polarizability tensor ␤ (2) . By referencing the internal coordinate axes with respect to a single, dominant transition, the number of significant electric-dipole allowed ␤ (2) tensor elements can be reduced from 18 in second harmonic generation ͑SHG͒ to at most 3, with the complete removal of all chiral elements. This coordinate transformation reduces the complexity of SHG measurements of oriented chiral systems to a level consistent with chromophores of significantly higher symmetry and provides a straightforward approach for extracting orientation information from polarization measurements.

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Section: Theorymentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Molecular and surface hyperpolarizability of oriented chromophores of low symmetry

2002

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“…IR (28)(29)(30)(31)(32), Raman (33)(34)(35)(36)(37)(38)(39), second-harmonic generation (SHG) (40)(41)(42)(43)(44)(45), and SFG (18,(46)(47)(48)(49)(50)(51)(52)(53)(54)(55) spectroscopy have all been developed into quantitative techniques for structural determination using polarized light. Many studies have explored the surface specificity of SHG/SFG (18,19,45,(56)(57)(58), but there have been only a few reports that discuss the technique in comparison to IR and Raman approaches for the same molecules (43,(59)(60)(61)(62)(63).…”

Section: Introductionmentioning

confidence: 99%

IR Absorption, Raman Scattering, and IR-Vis Sum-Frequency Generation Spectroscopy as Quantitative Probes of Surface Structure

Hung

Stege

Hore

2014

Applied Spectroscopy Reviews

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Vibrational spectroscopy is a valuable quantitative tool for the determination of structure at surfaces. Various techniques may be applicable and useful, depending on what is available, the transparency of the substrates, the need for in situ probes, and the degree of interfacial specificity required. We examine and compare signals in infrared absorption, Raman scattering, and vibrational sum-frequency generation spectroscopy to the underlying molecular response. In all of these experiments, varying the beam polarizations enables the orientation of specific chemical functional groups to be determined. However, the sensitivity of each technique is directly connected to the manner in which the molecular response manifests itself in the measured signal. Starting with simple distributions of a single vibrational mode, leading up to multiple vibrational bands in more complex orientation distributions, we compare these three techniques in terms of their sensitivity to features of the molecular orientation distribution. This review is aimed at guiding planned experiments when multiple techniques are available for surface structural analysis.

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“…Understanding the way a reactant is adsorbed on a catalysts surface could help to design a more specific catalyst for a given reaction. Second Harmonic Generation (SHG) has proved to be a powerful technique to study equilibrium and dynamic process at interfaces [1][2][3] . A special feature of this technique is that it is electric dipole forbidden in centrosymmetric media [4][5][6] .…”

Section: Introductionmentioning

confidence: 99%

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mentioning

confidence: 99%

Concentration dependence of surface nonlinear susceptibility of vanadyl-porphyrin at silica surfaces

Echevarria

Gutiérrez

Sosa

et al. 2001

Linear and Nonlinear Optics of Organic Materials

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Resonant molecular optical second harmonic generation (SHG) has been obtained from [2,3,7,8,12, 13, 17, vanadyl, (OEP)V=O, adsorbed on the hypotenuse face of a glass prism. Rotational intensity patterns are showed by plotting the second harmonic intensity as a function of the incident polarization angle of the fundamental wave, at a fixed angle of incidence. Evaluation of these patterns by Fourier analysis allowed the determination of the second order susceptibilities components of the adsorbed layers. Assuming a delta distribution function, the mean orientation angles from normal to the surface plane, were obtained for different solution concentrations. Our results indicate an abrupt change in the angle for two concentration ranges.

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New Tools for Surface Second-Harmonic Generation

Cited by 26 publications

References 202 publications

Molecular and surface hyperpolarizability of oriented chromophores of low symmetry

Molecular and surface hyperpolarizability of oriented chromophores of low symmetry

IR Absorption, Raman Scattering, and IR-Vis Sum-Frequency Generation Spectroscopy as Quantitative Probes of Surface Structure

Concentration dependence of surface nonlinear susceptibility of vanadyl-porphyrin at silica surfaces

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