Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling

Abraham, Baxter; Nieto-Pescador, Jesus; Gundlach, Lars

doi:10.1021/acs.jpclett.6b01439

Title: Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling

Abstract

Cyclic tetrapyrroles are the active core of compounds with crucial roles in living systems, such as hemoglobin and chlorophyll, and in technology as photocatalysts and light absorbers for solar energy conversion. Zinc-tetraphenylporphyrin (Zn-TPP) is a prototypical cyclic tetrapyrrole that has been intensely studied in past decades. Because of its importance for photochemical processes the optical properties are of particular interest, and, accordingly, numerous studies have focused on light absorption and excited-state dynamics of Zn-TPP. Relaxation after photoexcitation in the Soret band involves internal conversion that is preceded by an ultrafast process. This relaxation process has been observed by several groups. Until now, it has not been established if it involves a higher lying ”dark” state or vibrational relaxation in the excited S₂ state. Here we combine high time resolution electronic and vibrational spectroscopy to show that this process constitutes vibrational relaxation in the anharmonic ₂ potential.

Authors:

Abraham, Baxter ^[1]; Nieto-Pescador, Jesus ^[2]; Gundlach, Lars ^[1]

Univ. of Delaware, Newark, DE (United States). Dept. of Chemistry and Biochemistry
Univ. of Delaware, Newark, DE (United States). Dept. of Physics and Astronomy

Publication Date:: Tue Aug 02 00:00:00 EDT 2016

Research Org.:: Univ. of Delaware, Newark, DE (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1345807

Grant/Contract Number:: SC0016288

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry Letters

Additional Journal Information:: Journal Volume: 7; Journal Issue: 16; Journal ID: ISSN 1948-7185

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 14 SOLAR ENERGY

Citation Formats


                    Abraham, Baxter, Nieto-Pescador, Jesus, and Gundlach, Lars. Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling.  United States: N. p., 2016. 
Web.  doi:10.1021/acs.jpclett.6b01439.

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                    Abraham, Baxter, Nieto-Pescador, Jesus, & Gundlach, Lars. Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling.  United States.  https://doi.org/10.1021/acs.jpclett.6b01439

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                    Abraham, Baxter, Nieto-Pescador, Jesus, and Gundlach, Lars. Tue .  
"Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling".  United States.  https://doi.org/10.1021/acs.jpclett.6b01439.  https://www.osti.gov/servlets/purl/1345807.

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@article{osti_1345807,

  title        = {Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling},

  author       = {Abraham, Baxter and Nieto-Pescador, Jesus and Gundlach, Lars},

  abstractNote = {Cyclic tetrapyrroles are the active core of compounds with crucial roles in living systems, such as hemoglobin and chlorophyll, and in technology as photocatalysts and light absorbers for solar energy conversion. Zinc-tetraphenylporphyrin (Zn-TPP) is a prototypical cyclic tetrapyrrole that has been intensely studied in past decades. Because of its importance for photochemical processes the optical properties are of particular interest, and, accordingly, numerous studies have focused on light absorption and excited-state dynamics of Zn-TPP. Relaxation after photoexcitation in the Soret band involves internal conversion that is preceded by an ultrafast process. This relaxation process has been observed by several groups. Until now, it has not been established if it involves a higher lying ”dark” state or vibrational relaxation in the excited S2 state. Here we combine high time resolution electronic and vibrational spectroscopy to show that this process constitutes vibrational relaxation in the anharmonic 2 potential.},

  doi          = {10.1021/acs.jpclett.6b01439},

  journal      = {Journal of Physical Chemistry Letters},

  number       = 16,

  volume       = 7,

  place        = {United States},

  year         = {Tue Aug 02 00:00:00 EDT 2016},

  month        = {Tue Aug 02 00:00:00 EDT 2016}

}

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Photophysical processes in electronic states of zinc tetraphenyl porphyrin accessed on one- and two-photon excitation in the soret region
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Works referencing / citing this record:

Ultrafast photochemistry of free-base porphyrin: a theoretical investigation of B → Q internal conversion mediated by dark states
journal, January 2018

Falahati, Konstantin; Hamerla, Carsten; Huix-Rotllant, Miquel
Physical Chemistry Chemical Physics, Vol. 20, Issue 18
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Title: Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling

Abstract

Citation Formats

A Chlorin-Based Nanoscale Metal–Organic Framework for Photodynamic Therapy of Colon Cancers journal, June 2015

Porphyrin Cosensitization for a Photovoltaic Efficiency of 11.5%: A Record for Non-Ruthenium Solar Cells Based on Iodine Electrolyte journal, October 2015

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Kinetics of disaggregation of a non-covalent zinc tetraphenylporphyrin dimer in solution journal, May 2003

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Kinetics of disaggregation of a non-covalent zinc tetraphenylporphyrin dimer in solution
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Metalloporphyrin structure and dynamics from resonance raman spectroscopy
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