The key role of solvation dynamics in intramolecular electron transfer: time-resolved photophysics of crystal violet lactone

The Journal of Physical Chemistry. a
Uli SchmidhammerJerzy Karpiuk

Abstract

The intramolecular electron-transfer reaction in crystal violet lactone in polar aprotic solvents is studied with femtosecond transient absorption spectroscopy. The initially excited charge transfer state (1)CT A is rapidly converted into a highly polar charge transfer state (1)CT B. This ultrafast electron transfer is seen as a solvent-dependent dual fluorescence in steady-state spectra. We find that the electron-transfer process can be followed by a change from a double-peaked transient absorption spectrum to a single-peak one in the low picosecond range. The transient absorption kinetic curves are multiexponential, and the fitted time constants are solvent dependent but do not reproduce the known solvation times. For 6-dimethylaminophthalide, the optically active constituent of crystal violet lactone, only a small temporal evolution of the spectra is found. To explain these findings, we present a model that invokes a time-dependent electron-transfer rate. The rate is determined by the instantaneous separation of the two charge-transfer states. Because of their differing dipole moments, they are dynamically lowered to a different extent by the solvation. When they temporarily become isoenergetic, equal forward and backward tr...Continue Reading

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Citations

Oct 22, 2008·Physical Chemistry Chemical Physics : PCCP·Uwe MegerleStefan Lochbrunner
Jan 10, 2013·Annual Review of Physical Chemistry·Arnulf RosspeintnerEric Vauthey
Sep 9, 2015·Physical Chemistry Chemical Physics : PCCP·Patrick KölleEberhard Riedle
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Sep 14, 2010·The Journal of Physical Chemistry. a·Xiang Li, Mark Maroncelli
Apr 23, 2013·The Journal of Physical Chemistry. a·M JózefowiczJ R Heldt
May 4, 2011·The Journal of Physical Chemistry. B·Xiang LiMark Maroncelli
Apr 20, 2017·Physical Chemistry Chemical Physics : PCCP·Malgorzata BaydaBronislaw Marciniak
Jun 10, 2010·Physical Chemistry Chemical Physics : PCCP·Jerzy KarpiukJacek Nowacki
Dec 3, 2016·Journal of Fluorescence·Marek PietrzakJanina R Heldt
Aug 6, 2010·The Journal of Physical Chemistry. B·Manoj KumbhakarHaridas Pal
Jul 20, 2018·The Journal of Physical Chemistry. a·Nikolaos LiarosJohn T Fourkas

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