Symmetry-breaking charge transfer in the excited state of directly linked push-pull porphyrin arrays

Physical Chemistry Chemical Physics : PCCP
Taeyeon KimDongho Kim

Abstract

Herein, we revealed a symmetry-breaking charge transfer (SBCT) process in the excited state of a directly linked push-pull porphyrin dyad (AD) and triad (ADA) via spectroscopic measurements including steady-state absorption and fluorescence, time-resolved fluorescence (TRF), femtosecond transient absorption (fs-TA), and time-resolved infrared (TRIR) measurements. Unprecedented broad fluorescence spectra were observed for porphyrin arrays in polar solvents; these were attributed to the existence of a charge transfer state as evidenced by the TRF measurements. TA measurements also revealed emerging features of a CT state for AD and ADA in polar solvents. These dynamics were also confirmed via TRIR measurements, which provided further information on the solvation and structural relaxation processes of the SBCT process. This is the first observation of an SBCT process in porphyrin arrays, providing fundamental understanding of the strongly coupled porphyrin arrays. Thus, the results of this study reveal the potential of the porphyrin arrays in relevant applications requiring SBCT.

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Citations

Mar 24, 2018·Chemistry : a European Journal·Marika Żyła-KarwowskaMarcin Stępień
Aug 3, 2019·Chemistry : a European Journal·Brunella BardiFrancesca Terenziani
May 18, 2020·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Zoltan SzakacsEric Vauthey
Jul 7, 2020·Physical Chemistry Chemical Physics : PCCP·Xinmiao NiuAndong Xia
Sep 7, 2019·Chemical Communications : Chem Comm·Tongjing WuJianxin Song
Dec 12, 2020·Physical Chemistry Chemical Physics : PCCP·Siin KimHyotcherl Ihee
Apr 21, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Sandeep KumarMuniappan Sankar
Apr 22, 2021·The Journal of Physical Chemistry Letters·Zoltán Szakács, Eric Vauthey
Jul 16, 2021·Journal of the American Chemical Society·Nidhi Kaul, Reiner Lomoth
Aug 10, 2021·Journal of the American Chemical Society·Ebin Sebastian, Mahesh Hariharan
Dec 1, 2017·The Journal of Physical Chemistry Letters·Bogdan DerekaEric Vauthey
Jul 25, 2019·Journal of the American Chemical Society·Yuanyuan GuoAndong Xia

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