Mapping molecular orientation and conformation at interfaces by surface nonlinear optics

Zhuang, Xiaowei; Miranda, Paulo B.; Kim, Dongwon; Shen, Y. R.

doi:10.1103/physrevb.59.12632

Cited by 876 publications

(1,532 citation statements)

References 43 publications

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“…The described angular dependences are consistent with the experimental studies in molecular ensembles at interfaces where  angle averaging is likely (Zhuang et al, 1999).…”

Section: Acknowledgmentsupporting

confidence: 88%

“…Under a non-degenerate geometry, when 1  2, the Ppolarization setting of the analyzer would deliver a properly weighted superposition of X and Z projections (Zhuang et al, 1999).…”

Section: Image Reconstruction Protocolmentioning

confidence: 99%

“…In fact, the authors of (Zhuang et al, 1999) employed SSP, SPS and PSS measurement to extract YYZ, YZY and ZYY nonlinearities to address structural properties of pentyl-cyanoterphenyl at the air-water interface. The situation is different for the chiral responses.…”

Section: Acknowledgmentmentioning

confidence: 99%

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Modeling of Infrared–Visible Sum Frequency Generation Microscopy Images of a Giant Liposome

Volkov

Perry

2016

Microsc Microanal

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The article explores the theory of Infrared-Visible Sum Frequency Generation microscopy of phospholipid envelopes with dimensions larger than the wavelength of the nonlinear emission.The main part of the study concerns derivation and accounting for the contributions of effective nonlinear responses specific to sites on the surfaces of a bilayer envelope and their dependence on polarization condition and experimental geometry. The nonlinear responses of sites are mapped onto the image plane according to their emission directions and the numerical aperture of a sampling microscope objective. According to the simulation results, we discuss possible approaches to characterize the shape of the envelope, to extract molecular hyperpolarizabilities, to anticipate possible heterogeneity in envelope composition and anisotropy of the environment proximal to the envelope. The modeling approach offers a promising analytic facility to assist connecting microscopy observations in engineered liposomes, cellular envelopes and sub-cellular 2 organelles of relatively large dimensions to molecular properties and hence to chemistry and structure down to available the spatial resolution.

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“…The described angular dependences are consistent with the experimental studies in molecular ensembles at interfaces where  angle averaging is likely (Zhuang et al, 1999).…”

Section: Acknowledgmentsupporting

confidence: 88%

“…Under a non-degenerate geometry, when 1  2, the Ppolarization setting of the analyzer would deliver a properly weighted superposition of X and Z projections (Zhuang et al, 1999).…”

Section: Image Reconstruction Protocolmentioning

confidence: 99%

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Modeling of Infrared–Visible Sum Frequency Generation Microscopy Images of a Giant Liposome

Volkov

Perry

2016

Microsc Microanal

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“…These polarizations are connected with the laboratory coordinates by nonlinear Fresnel coefficients and appropriate projections. 22,[48][49][50] Figure 2 shows that the main peak is 1738 cm -1 in the SSP polarization spectrum with a weak peak at 1680 cm -1 . In the PPP spectrum, we observed only the peak at 1738 cm -1 .…”

Section: Resultsmentioning

confidence: 99%

Orientational Motions of Vibrational Chromophores in Molecules at the Air/Water Interface with Time-Resolved Sum Frequency Generation

et al. 2008

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The first time-resolved experiments in which interfacial molecules are pumped to excited electronic states and probed by vibrational sum frequency generation (SFG) are reported. This method was used to measure the out-of-plane rotation dynamics, i.e. time dependent changes in the polar angle, of a vibrational chromophore of an interfacial molecule. The chromophore is the carbonyl group, the rotation observed is that of the sCdO bond axis, with respect to the interfacial normal, and the interfacial molecule is coumarin 314 (C314) at the air/water interface. The orientational relaxation time was found to be 220 ( 20 ps, which is much faster than the orientational relaxation time of the permanent dipole moment axis of C314 at the same interface, as obtained from pump-second harmonic probe experiments. Possible effects on the rotation of the sCdO bond axis due to the carbonyl group hydrogen bonding with interfacial water are discussed. From the measured equilibrium orientation of the permanent dipole moment axis and the carbonyl axis, and knowledge of their relative orientation in the molecule, the absolute orientation of C314 at the air/water interface is obtained.

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“…These polarizations are connected with the laboratory coordinates by nonlinear Fresnel coefficients and appropriate projections. [11][12][13] The seven nonzero macroscopic susceptibilities in the laboratory coordinates are obtained from the four polarization combinations.…”

Section: Theoretical Considerationsmentioning

confidence: 99%

Absolute Orientation of Molecules at Interfaces

2006

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A method to determine the absolute orientation of molecules at liquid interfaces by sum frequency generation (SFG) is reported. It is based on measurements of the orientations of two nonparallel vibrationally active chromophores in the molecule of interest combined with a rotation matrix formulation to obtain the absolute molecular orientation. We chose m-tolunitrile, a planar molecule adsorbed to the air/water interface, as a proof-of-method experiment. Quantitative analysis of different polarization sum frequency intensities facilitate unique peak assignments of the methyl and nitrile groups of m-tolunitrile. The SFG analysis of the measurement yields a nitrile group tilting at 53°to the surface normal, and the C 3 axis of the methyl group is almost upright at 23°with respect to the surface normal. Using a rotation matrix formulation, we found that the angle between the surface plane and the m-tolunitrile molecular plane is 70°.

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Mapping molecular orientation and conformation at interfaces by surface nonlinear optics

Cited by 876 publications

References 43 publications

Modeling of Infrared–Visible Sum Frequency Generation Microscopy Images of a Giant Liposome

Modeling of Infrared–Visible Sum Frequency Generation Microscopy Images of a Giant Liposome

Orientational Motions of Vibrational Chromophores in Molecules at the Air/Water Interface with Time-Resolved Sum Frequency Generation

Absolute Orientation of Molecules at Interfaces

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