Skip to main content

Utilizing Coupled-Oscillator Photophysics to Elaborate Chromophores with Exceptional Molecular Hyperpolarizabilities

Publication ,  Journal Article
Uyeda, HT; Miloradovic, I; Zhao, Y; Wostyn, K; Asselbergsh, I; Clays, K; Persoons, A; Therien, MJ
Published in: Proceedings of SPIE - The International Society for Optical Engineering
January 1, 2003

The syntheses and electrooptic properties of a family of nonlinear optical chromophores are described. Typically, these species feature an ethyne-elaborated, highly polarizable porphyrinic component, and metal polypyridyl complexes that serve as integral donor and acceptor elements. The frequency dependence of the dynamic hyperpolarizability of a wide-range of these chromophores, that vary widely with respect to their electronic structure, was determined from hyper-Rayleigh light scattering (HRS) measurements carried out at fundamental incident irradiation wavelengths (λinc) of 830, 1064, and 1300 nm. These data show that: (i) Coupled oscillator photophysics and metal-mediated cross-coupling can be exploited to elaborate high βλ supermolecules that exhibit significant excited-state electronic communication between their respective pigment building blocks; (ii) High-stability metal polypyridyl compounds constitute an attractive alternative to electron releasing dialkyl- and diarylamino groups, the most commonly used donor moieties in a wide-range of established NLO dyes, and long-recognized to be the moiety that often limits the thermal stability of such compounds; (iii) This design strategy clearly enables ready elaboration of extraordinarily large βλ chromophores at telecommunication-relevant wavelengths; and (iv) Multiple charge-transfer (CT) transitions within a single chromophore can be designed to have transition dipole moments of the same or opposite sign; because the sign of the resonance enhancement factor is frequency dependent, appropriate engineering of the relative contributions of these CT states at a given wavelength provides a new means to regulate the magnitude of dynamic hyperpolarizabilities.

Duke Scholars

Published In

Proceedings of SPIE - The International Society for Optical Engineering

DOI

ISSN

0277-786X

Publication Date

January 1, 2003

Volume

5212

Start / End Page

117 / 121

Related Subject Headings

  • 5102 Atomic, molecular and optical physics
  • 4009 Electronics, sensors and digital hardware
  • 4006 Communications engineering
 

Citation

APA
Chicago
ICMJE
MLA
NLM
Uyeda, H. T., Miloradovic, I., Zhao, Y., Wostyn, K., Asselbergsh, I., Clays, K., … Therien, M. J. (2003). Utilizing Coupled-Oscillator Photophysics to Elaborate Chromophores with Exceptional Molecular Hyperpolarizabilities. Proceedings of SPIE - The International Society for Optical Engineering, 5212, 117–121. https://doi.org/10.1117/12.508261
Uyeda, H. T., I. Miloradovic, Y. Zhao, K. Wostyn, I. Asselbergsh, K. Clays, A. Persoons, and M. J. Therien. “Utilizing Coupled-Oscillator Photophysics to Elaborate Chromophores with Exceptional Molecular Hyperpolarizabilities.” Proceedings of SPIE - The International Society for Optical Engineering 5212 (January 1, 2003): 117–21. https://doi.org/10.1117/12.508261.
Uyeda HT, Miloradovic I, Zhao Y, Wostyn K, Asselbergsh I, Clays K, et al. Utilizing Coupled-Oscillator Photophysics to Elaborate Chromophores with Exceptional Molecular Hyperpolarizabilities. Proceedings of SPIE - The International Society for Optical Engineering. 2003 Jan 1;5212:117–21.
Uyeda, H. T., et al. “Utilizing Coupled-Oscillator Photophysics to Elaborate Chromophores with Exceptional Molecular Hyperpolarizabilities.” Proceedings of SPIE - The International Society for Optical Engineering, vol. 5212, Jan. 2003, pp. 117–21. Scopus, doi:10.1117/12.508261.
Uyeda HT, Miloradovic I, Zhao Y, Wostyn K, Asselbergsh I, Clays K, Persoons A, Therien MJ. Utilizing Coupled-Oscillator Photophysics to Elaborate Chromophores with Exceptional Molecular Hyperpolarizabilities. Proceedings of SPIE - The International Society for Optical Engineering. 2003 Jan 1;5212:117–121.

Published In

Proceedings of SPIE - The International Society for Optical Engineering

DOI

ISSN

0277-786X

Publication Date

January 1, 2003

Volume

5212

Start / End Page

117 / 121

Related Subject Headings

  • 5102 Atomic, molecular and optical physics
  • 4009 Electronics, sensors and digital hardware
  • 4006 Communications engineering