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Title: Third-order nonlinear optical properties of sulfur-rich compounds

Abstract

The molecular third-order optical nonlinearity {gamma}{sub R} (second hyperpolarizability or nonlinear refractive index) was measured for a series of sulfur-rich molecules: sulfur (S{sub 8}), carbon-sulfur compounds, and metal thiolate clusters. Z-scan techniques (pulse width 27 ps, wavelength 527 nm) were used to measure these properties in solution by comparing the solution to the pure solvent. The authors approach is an efficient way to evaluate a number of different compounds and to quickly direct synthetic strategies for improved nonlinear and linear optical properties. The optical nonlinearities were evaluated in terms of figures of merit {vert{underscore}bar}W{vert{underscore}bar}/I{sub 0} and [T]{sup {minus}1}, where {vert{underscore}bar}W{vert{underscore}bar}/I{sub 0} is the ratio of nonlinear refraction to linear absorption and [T]{sup {minus}1} is the ratio of nonlinear refraction to nonlinear absorption. Among the carbon-sulfur compounds, C{sub 6}S{sub 8}O{sub 2} had the largest figures of merit: {vert{underscore}bar}W{vert{underscore}bar}/I{sub 0} = 4.3 x 10{sup {minus}13} m{sup 2} W{sup {minus}1} and [T]{sup {minus}1} > 5. The metal thiolate cluster with the largest second hyperpolarizability was [Zn{sub 10}S{sub 4}(SPh){sub 16}]{sup 4{minus}} ({gamma}{sub R} = {minus}7.8 x 10{sup {minus}56} C m{sup 4} V{sup {minus}3}, {minus}6.3 x 10{sup {minus}31} esu). This cluster exhibited no measurable linear or nonlinear absorption, so the figures of merit were effectivelymore » infinite. Previous work on the second hyperpolarizability of sulfur-rich compounds examined species that were hampered by substantial linear absorption coefficients. The present work shows that high figures of merit can be achieved without significant linear or nonlinear absorption.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Univ. of Illinois, Urbana, IL (US)
Sponsoring Org.:
USDOE; National Science Foundation (NSF); US Department of the Air Force; US Department of the Army
OSTI Identifier:
20000067
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory
Additional Journal Information:
Journal Volume: 103; Journal Issue: 35; Other Information: PBD: 2 Sep 1999; Journal ID: ISSN 1089-5639
Country of Publication:
United States
Language:
English
Subject:
40 CHEMISTRY; NONLINEAR OPTICS; REFRACTIVE INDEX; SULFUR COMPOUNDS; SULFIDES; AROMATICS; ORGANIC SULFUR COMPOUNDS; METALS

Citation Formats

Breitzer, J.G., Dlott, D.D., Iwaki, L.K., Kirkpatrick, S.M., and Rauchfuss, T.B. Third-order nonlinear optical properties of sulfur-rich compounds. United States: N. p., 1999. Web. doi:10.1021/jp990137f.
Breitzer, J.G., Dlott, D.D., Iwaki, L.K., Kirkpatrick, S.M., & Rauchfuss, T.B. Third-order nonlinear optical properties of sulfur-rich compounds. United States. doi:10.1021/jp990137f.
Breitzer, J.G., Dlott, D.D., Iwaki, L.K., Kirkpatrick, S.M., and Rauchfuss, T.B. Thu . "Third-order nonlinear optical properties of sulfur-rich compounds". United States. doi:10.1021/jp990137f.
@article{osti_20000067,
title = {Third-order nonlinear optical properties of sulfur-rich compounds},
author = {Breitzer, J.G. and Dlott, D.D. and Iwaki, L.K. and Kirkpatrick, S.M. and Rauchfuss, T.B.},
abstractNote = {The molecular third-order optical nonlinearity {gamma}{sub R} (second hyperpolarizability or nonlinear refractive index) was measured for a series of sulfur-rich molecules: sulfur (S{sub 8}), carbon-sulfur compounds, and metal thiolate clusters. Z-scan techniques (pulse width 27 ps, wavelength 527 nm) were used to measure these properties in solution by comparing the solution to the pure solvent. The authors approach is an efficient way to evaluate a number of different compounds and to quickly direct synthetic strategies for improved nonlinear and linear optical properties. The optical nonlinearities were evaluated in terms of figures of merit {vert{underscore}bar}W{vert{underscore}bar}/I{sub 0} and [T]{sup {minus}1}, where {vert{underscore}bar}W{vert{underscore}bar}/I{sub 0} is the ratio of nonlinear refraction to linear absorption and [T]{sup {minus}1} is the ratio of nonlinear refraction to nonlinear absorption. Among the carbon-sulfur compounds, C{sub 6}S{sub 8}O{sub 2} had the largest figures of merit: {vert{underscore}bar}W{vert{underscore}bar}/I{sub 0} = 4.3 x 10{sup {minus}13} m{sup 2} W{sup {minus}1} and [T]{sup {minus}1} > 5. The metal thiolate cluster with the largest second hyperpolarizability was [Zn{sub 10}S{sub 4}(SPh){sub 16}]{sup 4{minus}} ({gamma}{sub R} = {minus}7.8 x 10{sup {minus}56} C m{sup 4} V{sup {minus}3}, {minus}6.3 x 10{sup {minus}31} esu). This cluster exhibited no measurable linear or nonlinear absorption, so the figures of merit were effectively infinite. Previous work on the second hyperpolarizability of sulfur-rich compounds examined species that were hampered by substantial linear absorption coefficients. The present work shows that high figures of merit can be achieved without significant linear or nonlinear absorption.},
doi = {10.1021/jp990137f},
journal = {Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory},
issn = {1089-5639},
number = 35,
volume = 103,
place = {United States},
year = {1999},
month = {9}
}