An SHG Magic Angle:  Dependence of Second Harmonic Generation Orientation Measurements on the Width of the Orientation Distribution

Simpson, Garth J.; Rowlen, Kathy L.

doi:10.1021/ja983683f

Cited by 157 publications

(182 citation statements)

References 19 publications

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“…Different from the d-function model, the recovered ratio of local frame tensor elements approach an asymptotic value of 3 as the tilt-angle distribution approaches a broad disordered limit. Conceptually, the asymptotic value of 3 is explained by the weak order limit, where c ð2Þ l;zzz yc ð2Þ l;zxx þ c ð2Þ l;xxz þ c ð2Þ l;xzx (56). The independence of the previously reported values from the ONIOM calculations on the distribution width can be understood based on this same asymptotic behavior.…”

Section: Discussion Of the Triple-helix Distribution With Respect To mentioning

confidence: 63%

Imaging the Nonlinear Susceptibility Tensor of Collagen by Nonlinear Optical Stokes Ellipsometry

Dow

DeWalt

Sullivan

et al. 2016

Biophysical Journal

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Nonlinear optical Stokes ellipsometric (NOSE) microscopy was demonstrated for the analysis of collagen-rich biological tissues. NOSE is based on polarization-dependent second harmonic generation imaging. NOSE was used to access the molecular-level distribution of collagen fibril orientation relative to the local fiber axis at every position within the field of view. Fibril tilt-angle distribution was investigated by combining the NOSE measurements with ab initio calculations of the predicted molecular nonlinear optical response of a single collagen triple helix. The results were compared with results obtained previously by scanning electron microscopy, nuclear magnetic resonance imaging, and electron tomography. These results were enabled by first measuring the laboratory-frame Jones nonlinear susceptibility tensor, then extending to the local-frame tensor through pixel-by-pixel corrections based on local orientation.

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Section: Discussion Of the Triple-helix Distribution With Respect To mentioning

confidence: 63%

Imaging the Nonlinear Susceptibility Tensor of Collagen by Nonlinear Optical Stokes Ellipsometry

Dow

DeWalt

Sullivan

et al. 2016

Biophysical Journal

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“…70 Therefore, it may come from a relatively broad orientational distribution. Indeed, because there are different kinds of non-straddle-type water molecule at the interface region, as clearly indicated by the broad vibrational spectra between 3100cm −1 and 3500cm −1 in SFG-VS studies, 26,65,66,67,68 a relatively broad orientational distribution for the non-straddle-type hydrogen-bonded water molecule is generally expected.…”

Section: Water Molecule Orientation At Neat Air/water Interfacementioning

confidence: 99%

Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution

Zhang

Dong

et al. 2005

The Journal of Chemical Physics

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It has been generally accepted that there are significant quadrupolar and bulk contributions to the second harmonic generation (SHG) reflected from the neat air/water interface, as well as common liquid interfaces. Because there has been no general methodology to determine the quadrupolar and bulk contributions to the SHG signal from a liquid interface, this conclusion was reached based on the following two experimental phenomena. Namely, the broken of the macroscopic Kleinman symmetry, and the significant temperature dependence of the SHG signal from the neat air/water interface. However, because sum frequency generation vibrational spectroscopy (SFG-VS) measurement of the neat air/water interface observed no apparent temperature dependence, the temperature dependence in the SHG measurement has been reexamined and proven to be an experimental artifact. Here we present a complete microscopic analysis of the susceptibility tensors of the air/water interface, and show that dipolar contribution alone can be used to address the issue of broken of the macroscopic Kleinman symmetry at the neat air/water interface. Using this analysis, the orientation of the water molecules at the interface can be obtained, and it is consistent with the measurement from SFG-VS. Therefore, the key rationales to conclude significantly quadrupolar and bulk contributions to the SHG signal of the neat air/water interface can no longer be considered as valid as before. This new understanding of the air/water interface can shed light on our understanding of the nonlinear optical responses from other molecular interfaces as well.

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“…The light was plane-polarized before the surfactant solution using a Glan-Thomson prism (extinction ratio 10 −6 , Type K, Steeg & Reuter). The plane of polarization was rotated 39 • from vertical polarization, where the SHG apparent molecular tilt angle is independent of the true distribution mean [25]. Spectral purity of the incoming light was assured by use of an IR cut-off filter (BG39, Schott) in conjunction with a narrow-band interference filter (532 BP, LOT-Oriel).…”

Section: Shg Experimentsmentioning

confidence: 99%

A study of kinetic molecular exchange processes in the medium frequency range by surface SHG on an oscillating bubble

Örtegren

Wantke

Motschmann

et al. 2004

Journal of Colloid and Interface Science

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The dilatational properties of fluid surfaces and interfaces have been comprehensively investigated in recent years. For example, an improved oscillating bubble device provided experimental results that allow for critical testing of established surface models, such as the Lucassen/van den Tempel (LvdT) model. The comparison of the LvdT model with the oscillating bubble experiments demonstrates a mismatch between the model parameters. For example, near the CMC or the limit of solubility the calculated parameters of surfactant solutions become unrealistically large. The deviation can be explained by the introduction of more detailed surface models, in particular by the modification of the effective thickness of the surface layer, its internal structure and the molecular exchange processes between these structures. For the verification of such processes an experimental setup was realized which allows for an independent determination of the instantaneous adsorption state at the surface of an oscillating bubble inside a surfactant solution. The setup utilizes the Second Harmonic Generation (SHG)-effect at the air-solution interface generated by the light of a pulsed LASER. The set-up is described in detail, and the results of a first experimental series are presented and discussed in this paper. As system, aqueous solutions of the fluortenside F381 were used.  2004 Elsevier Inc. All rights reserved.

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An SHG Magic Angle: Dependence of Second Harmonic Generation Orientation Measurements on the Width of the Orientation Distribution

Cited by 157 publications

References 19 publications

Imaging the Nonlinear Susceptibility Tensor of Collagen by Nonlinear Optical Stokes Ellipsometry

Imaging the Nonlinear Susceptibility Tensor of Collagen by Nonlinear Optical Stokes Ellipsometry

Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution

A study of kinetic molecular exchange processes in the medium frequency range by surface SHG on an oscillating bubble

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