Methylene Blue Exciton States Steer Nonradiative Relaxation: Ultrafast Spectroscopy of Methylene Blue Dimer

The Journal of Physical Chemistry. B
Jacob C DeanGregory D Scholes

Abstract

The photochemistry and aggregation properties of methylene blue (MB) lead to its popular use in photodynamic therapy. The facile formation of strongly coupled "face-to-face" H-aggregates in concentrated aqueous solution, however, significantly changes its spectroscopic properties and photophysics. The photoinitiated dynamics of the simplest MB aggregate, MB2, was investigated over femtosecond to nanosecond time scales revealing sequential internal conversion events that fully relax the excited population. MB monomer dynamics were analyzed in tandem for a direct comparison. First, ultrafast internal conversion from the electric-dipole allowed upper exciton state to the lower forbidden exciton state was evaluated by use of broadband transient absorption (BBTA) and two-dimensional electronic spectroscopy (2DES) with a time resolution of ∼ 10 fs. Lineshape analysis of MB and MB2 2DES bands at 298 and 77 K show effectively no difference in the diagonal/antidiagonal line width ratio for the dimer, in marked contrast to the distinct reduction of the homogeneous line width for MB. This result is interpreted as ultrafast population relaxation imposing a limitation to the homogeneous line width, instead of pure dephasing as in the case o...Continue Reading

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Citations

Jun 10, 2016·The Journal of Physical Chemistry Letters·Ryan D PensackGregory D Scholes
Dec 20, 2016·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Ana L CostaJ Sérgio Seixas de Melo
Apr 9, 2016·Physical Chemistry Chemical Physics : PCCP·Benjamin W CaplinsDavid A Blank
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Aug 6, 2020·The Journal of Chemical Physics·Tim J ZuehlsdorffChristine M Isborn
Jan 5, 2021·Annual Review of Physical Chemistry·Tim J ZuehlsdorffChristine M Isborn
Apr 27, 2021·The Journal of Physical Chemistry Letters·Jianxin GuanJunrong Zheng
May 4, 2021·Frontiers in Chemistry·Mindy Levine
Apr 24, 2019·The Journal of Physical Chemistry Letters·Jonathan S HuffRyan D Pensack
Dec 13, 2017·Langmuir : the ACS Journal of Surfaces and Colloids·Junxin WangJesse V Jokerst
Aug 19, 2020·The Journal of Physical Chemistry Letters·Michael S ChenThomas E Markland
Apr 16, 2020·The Journal of Physical Chemistry Letters·Luca MorettiMargherita Maiuri
Feb 27, 2018·The Journal of Physical Chemistry. B·Eimer M Tuite, Bengt Nordén
Nov 3, 2021·The Journal of Physical Chemistry. B·Shao-Yu LuLiang Shi

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