Two-Photon-Induced versus One-Photon-Induced Isomerization Dynamics of a Bistable Azobenzene Derivative in Solution

The Journal of Physical Chemistry. B
J MorenoS A Kovalenko

Abstract

We report on a bistable azobenzene derivative with sufficiently high 2-photon absorption to induce its photochemical isomerization and measurable excited state dynamics. Broadband transient absorption spectra were recorded and compared upon 1-photon (331 nm) and 2-photon (640 nm) excitation of the S0 → S2 transition. The spectra are different at early (t ∼ 1 ps) and late (t ∼ 100 ps) time but show similar photoisomerization behavior on a 10 ps time scale. With 2-photon excitation, strong population transfer S2 → Sn occurs due to resonance absorption of a third pump photon. Subsequent internal conversion Sn → S1 results in a very hot S1 population causing extra-broadening of the transient spectra. The resonance pump absorption is common with nonlinear excitation and should be taken into account when considering photochemical applications. The 2-photon excitation cross-section σ((2)) at 640 nm was measured to be 7 GM for the specific tetra-ortho-fluorinated azobenzene derivative and 1 GM for unsubstituted parent azobenzene. The direct 2-photon induced trans-to-cis isomerization, described herein, provides an unprecedented potential for spatially addressing P-type (bistable) azobenzene photoswitches in 3D.

References

Jan 1, 1985·Proceedings of the National Academy of Sciences of the United States of America·R S Liu, A E Asato
Jan 21, 2006·Angewandte Chemie·Anzar KhanStefan Hecht
Nov 26, 2009·The Journal of Physical Chemistry. a·Marcus BöckmannDominik Marx
May 10, 2011·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Yi FuJoseph R Lakowicz
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Nov 5, 2014·The Journal of Physical Chemistry. B·Amanda L HoukChristopher G Elles

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Citations

Aug 20, 2016·Chemical Communications : Chem Comm·Robert J Mart, Rudolf K Allemann
Aug 4, 2018·Angewandte Chemie·Stefan PasslickGraham C R Ellis-Davies
Sep 27, 2018·Journal of the American Chemical Society·Baihao ShaoIvan Aprahamian
Oct 7, 2017·Journal of the American Chemical Society·Ilya N IoffeSergey A Kovalenko
Jun 28, 2019·The Journal of Physical Chemistry. a·Dragos Lucian IsacMariana Pinteală
Aug 31, 2021·Journal of the American Chemical Society·Hosung KiJeongho Kim

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