The effects of donor-acceptor substitution symmetry on the nonlinear absorption of two-dimensionally-conjugated isomeric chromophores

Aaron D. Slepkov; Jeremiah A. Marsden; Jeremie J. Miller; Laura D. Shirtcliff; Michael M. Haley; Kenji Kamada; Rik R. Tykwinski; Frank A. Hegmann

doi:10.1117/12.617976

29 August 2005 The effects of donor-acceptor substitution symmetry on the nonlinear absorption of two-dimensionally-conjugated isomeric chromophores

Aaron D. Slepkov, Jeremiah A. Marsden, Jeremie J. Miller, Laura D. Shirtcliff, Michael M. Haley, Kenji Kamada, Rik R. Tykwinski, Frank A. Hegmann

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Proceedings Volume 5934, Nonlinear Optical Transmission and Multiphoton Processes in Organics III; 593405 (2005) https://doi.org/10.1117/12.617976
Event: Optics and Photonics 2005, 2005, San Diego, California, United States

Abstract

Differential optical Kerr effect (DOKE) detection is a powerful tool for studying the ultrafast time-resolved dynamics of 3^rd-order nonlinear processes. In this study, DOKE was used to measure the nonlinear absorption properties of tetraethynylphenylene (TEP) solutions in THF using 800 nm, 80 fs laser pulses. These two-dimensional, highly-conjugated chromophores (also known as TPEBs) show high instantaneous two-photon absorption (TPA) for relatively small chromophores. The TPA cross section is strongly dependent on the donor-acceptor geometry in these materials: a quadrupolar, all-donor TEP shows the smallest TPA, with a cross-section of σ⁽²⁾= 90 ± 15 GM. ortho-TEP, for which the donors (and acceptors) are conjugated via the ortho position across the central phenyl ring, is dipolar and displays the largest cross-section, of σ⁽²⁾= 260 ± 30 GM. para-TEP, which is quadrupolar, and meta-TEP, which is dipolar, display similar cross-sections of σ⁽²⁾= 160 ± 10 GM and σ⁽²⁾= 150 ± 10 GM, respectively. In addition to an instantaneous TPA response, these isomers show unique two-photon assisted excited-state absorption (ESA), with the ortho- and meta-TEP displaying a clear 3-10 ps rise to an ESA peak, and subsequent decay. The differences in the nonlinear absorption behaviour of these materials may be partially explained by selection rules and UV-vis spectroscopy. In addition, the polar geometries, coupled to the various in-plane conjugation paths, may further influence their optical nonlinearities. Understanding these trends impacts both the design of materials with desirable nonlinear absorption properties and our understanding of the electronic landscape in functionalized organic materials.

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Aaron D. Slepkov, Jeremiah A. Marsden, Jeremie J. Miller, Laura D. Shirtcliff, Michael M. Haley, Kenji Kamada, Rik R. Tykwinski, and Frank A. Hegmann "The effects of donor-acceptor substitution symmetry on the nonlinear absorption of two-dimensionally-conjugated isomeric chromophores", Proc. SPIE 5934, Nonlinear Optical Transmission and Multiphoton Processes in Organics III, 593405 (29 August 2005); https://doi.org/10.1117/12.617976

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KEYWORDS

Absorption

Nonlinear optics

Laser beam diagnostics

Molecules

Chromophores

Signal processing

Picosecond phenomena

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