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Electron and energy transfer in a porphyrin-oxoporphyrinogen-fullerene triad, ZnP-OxP-C
Ist Teil von
Physical chemistry chemical physics : PCCP, 2020-07, Vol.22 (25), p.14356-14363
Erscheinungsjahr
2020
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
A multichromophoric triad,
ZnP-OxP-C
60
containing porphyrin (
ZnTPP
hereafter
ZnP
), oxoporphyrinogen (
OxP
) and fullerene (
C
60
) has been synthesized to probe the intramolecular dynamics of its electron and energy transfer in relation to the presence of the closely linked electron deficient
OxP-C
60
'special pair', constructed as a mimic of the naturally occurring photosynthetic antenna-reaction center. The DFT optimized structure of the triad reveals the relative spatial remoteness of the
ZnP
entity with proximal
OxP
/
C
60
entities. Free-energetics of different energy and electron transfer events were estimated using spectral, computational and electrochemical studies, according to the Rehm-Weller approach. Femtosecond transient absorption spectral studies revealed energy transfer from
1
ZnP*
to
OxP
to yield
ZnP-
1
OxP*-C
60
, and electron transfer to yield
ZnP&z.rad;
+
-OxP-C
60
&z.rad;
−
and/or
ZnP-OxP&z.rad;
+
-C
60
&z.rad;
−
charge seperated states. That is, the
ZnP
entity in the triad operates as both antenna and electron donor to generate relatively long-lived charge separated states thus mimicking the early photoevents of natural photosynthesis.
Competitive energy and electron transfer in a newly synthesized supramolecular triad composed of zinc porphyrin, oxoporphyrinogen and C
60
has been demonstrated using ultrafast pump-probe spectroscopy.
Sprache
Englisch
Identifikatoren
ISSN: 1463-9076
eISSN: 1463-9084
DOI: 10.1039/d0cp02696d
Titel-ID: cdi_rsc_primary_d0cp02696d
Format
–
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