Chromophore orientations in a nonlinear optical azopolymer diffraction grating

Even and odd order parameters from far-field Raman and near-field second harmonic generation microscopies

F. Lagugné-Labarthet, C. Sourisseau, Richard D Schaller, R. J. Saykally, P. Rochon

Research output: Contribution to journalArticle

33 Citations (Scopus)

Abstract

A diffraction grating with a large diffraction efficiency (η = 25% on the first order) was inscribed on an azobenzene-containing polymer thin film, electrically poled, and characterized using spatially resolved Raman confocal microscopy and near-field scanning optical microscopy (NSOM) coupled with second-order nonlinear optical measurements. Linear (Raman) and nonlinear (second harmonic generation or SHG) polarized microscopic measurements were performed on a grating with ∼ 1.4 μm periodicity, revealing the molecular orientations in various regions of the sinusoidal relief surface. The most probable distribution functions f(θ) of the chromophore orientations were derived using the two first even parity Legendre polynomials 〈P 2〉 and 〈P 4〉 together with the two odd order parameters 〈P 1〉 and 〈P 3〉, as determined by Raman and SHG, respectively. These distribution functions show that the poling treatment is quite efficient and also emphasize the importance of determining both couples of the order parameters in such a surface-modulated optical element. In particular, new information is provided about the formation mechanism of the additional surface modulations of half periodicity that are revealed by the SHG-NSOM data but are not detected in the far-field Raman scattering measurements.

Original languageEnglish
Pages (from-to)17059-17068
Number of pages10
JournalJournal of Physical Chemistry B
Volume108
Issue number44
DOIs
Publication statusPublished - Nov 4 2004

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Diffraction gratings
Chromophores
Harmonic generation
gratings (spectra)
chromophores
Near field scanning optical microscopy
far fields
harmonic generations
near fields
Microscopic examination
microscopy
Distribution functions
periodic variations
distribution functions
Azobenzene
scanning
Diffraction efficiency
Legendre functions
Molecular orientation
Confocal microscopy

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Chromophore orientations in a nonlinear optical azopolymer diffraction grating : Even and odd order parameters from far-field Raman and near-field second harmonic generation microscopies. / Lagugné-Labarthet, F.; Sourisseau, C.; Schaller, Richard D; Saykally, R. J.; Rochon, P.

In: Journal of Physical Chemistry B, Vol. 108, No. 44, 04.11.2004, p. 17059-17068.

Research output: Contribution to journalArticle

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