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@PHDTHESIS{Costantini:453801,
author = {Costantini, Roberto},
othercontributors = {Morgante, Alberto},
title = {{E}xciton {D}ynamics in {M}olecular {H}eterojunctions},
school = {Universita degli Studi di Trieste},
type = {Dissertation},
reportid = {PUBDB-2021-00192},
pages = {87},
year = {2020},
note = {Dissertation, Universita degli Studi di Trieste, 2020},
abstract = {In recent years, the need for a more sustainable economic
development contributed to the increasing interest in
renewable energy sources. With encouraging trends on power
conversion efficiencies and manufacturing costs,
photovoltaics is expected to be the workhorse for the
production of green energy in the future. Silicon is
currently the dominant photovoltaic technology but, in the
past decade, novel solutions based on organic semiconductors
became attractive for their potential of overcoming the
Shockley-Queisser limit and offering unmatched efficiencies
by exploiting singlet fission. The latter is an exciton
multiplication process in which, for a certain class of
materials, a singlet exciton splits into two triplet
excitons, thus potentially doubling the charge carriers.
Significant work is still necessary to fully benefit of
singlet fission in photovoltaics; in particular, a higher
degree of control over exciton transport and dissociation
mechanisms at hetero-organic interfaces is required for
efficiently harvesting triplet excitons. To the aim of
better understanding such processes, at the ANCHOR-SUNDYN
endstation of the ALOISA beamline at Elettra we developed an
experimental setup for time-resolved X-ray spectroscopies,
in which the exciton dynamics in organic films can be
characterized by X-ray photoemission and absorption
spectroscopies with a 100 ps resolution. Here, we can
combine time-resolved measurements with standard X-ray and
UV spectroscopies for a more detailed analysis of the
samples.We apply this approach to donor/acceptor interfaces,
the prototypical architectures of organic photovoltaic
devices; we investigate triplet excited states in pentacene
by means of time-resolved X-ray absorption, which displays a
pump-induced feature with a 0.3±0.2 ns lifetime below the
LUMO resonance, that we associated to molecules in the
triplet state. On the picosecond time scale, measurements
performed at the FLASH free-electron laser reveal a
photoelectron response that we deem related to the triplet
exciton dissociation at the interface with the underlying
C60 film. A similar effect is also observed in pump-probe
photoemission spectra of tetracene / copper phthalocyanine
interfaces. On this second system, we tuned the pump
wavelength to selectively excite the two materials and
examined the different behavior of the photogenerated
excitons; the presence of a transient field in the
microsecond time scale suggests that triplet excitons are
involved in the charge transfer that occurs from tetracene
to copper phthalocyanine, in agreement with previous
studies. The results presented here demonstrate that
time-resolved X-ray spectroscopies can provide valuable
information for the characterization of exciton dynamics in
hetero-organic interfaces.},
cin = {DOOR ; HAS-User},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {6G2 - FLASH (POF3-622)},
pid = {G:(DE-HGF)POF3-6G2},
experiment = {EXP:(DE-H253)F-PG2-20150101},
typ = {PUB:(DE-HGF)11},
doi = {10.3204/PUBDB-2021-00192},
url = {https://bib-pubdb1.desy.de/record/453801},
}