Thermal Fluctuations on Förster Resonance Energy Transfer in Dyadic Solar Cell Sensitizers: A Combined Ab Initio Molecular Dynamics and TDDFT Investigation

Rodrigo A. Urzúa-Leiva, Sergio Rampino, Ramiro Arratia-Perez, Edoardo Mosconi, Mariachiara Pastore, Filippo De Angelis

Resultado de la investigación: Article

4 Citas (Scopus)

Resumen

Förster resonance energy transfer (FRET) is a key process in dyadic dye-sensitized solar cells (DSSCs) where an "antenna" donor has the role of collecting photons and redirecting the captured energy to an adsorbed-dye acceptor unit. Despite its popularity in, e.g., biology, where FRET rates are used to derive structural information on fairly complex systems, relatively few studies have appeared in the DSSCs field. These were based, to the best of our knowledge, either on a static modeling of FRET or on the so called isotropic regime assuming an isotropic motion of the donor/acceptor units and uncorrelated donor/acceptor relative distance and orientation. In this paper we carry out a combined Car-Parrinello molecular dynamics and TDDFT investigation to unravel the impact of thermal fluctuations on FRET in two dyadic carbazole-phenothiazine dye sensitizers. Both isolated and full-packed adsorption conditions are considered, mimicking the dye adsorption topology on TiO2. Results are discussed in relation to the above mentioned models and rationalized in terms of the structural differences of the considered dyes. We find a considerable difference between the FRET rates calculated at zero temperature and the results obtained by including thermal fluctuations, highlighting an important role of the latter in determining FRET rates in dyadic donor-acceptor dye-sensitized solar cells.

Idioma originalEnglish
Páginas (desde-hasta)16490-16499
Número de páginas10
PublicaciónJournal of Physical Chemistry C
Volumen119
N.º29
DOI
EstadoPublished - 23 jul 2015

Huella dactilar

dyadics
Energy transfer
Molecular dynamics
Solar cells
solar cells
dyes
energy transfer
molecular dynamics
Coloring Agents
Dyes
Adsorption
phenothiazines
adsorption
carbazoles
Hot Temperature
Large scale systems
complex systems
biology
Railroad cars
Photons

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

Citar esto

Urzúa-Leiva, Rodrigo A. ; Rampino, Sergio ; Arratia-Perez, Ramiro ; Mosconi, Edoardo ; Pastore, Mariachiara ; Angelis, Filippo De. / Thermal Fluctuations on Förster Resonance Energy Transfer in Dyadic Solar Cell Sensitizers : A Combined Ab Initio Molecular Dynamics and TDDFT Investigation. En: Journal of Physical Chemistry C. 2015 ; Vol. 119, N.º 29. pp. 16490-16499.
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abstract = "F{\"o}rster resonance energy transfer (FRET) is a key process in dyadic dye-sensitized solar cells (DSSCs) where an {"}antenna{"} donor has the role of collecting photons and redirecting the captured energy to an adsorbed-dye acceptor unit. Despite its popularity in, e.g., biology, where FRET rates are used to derive structural information on fairly complex systems, relatively few studies have appeared in the DSSCs field. These were based, to the best of our knowledge, either on a static modeling of FRET or on the so called isotropic regime assuming an isotropic motion of the donor/acceptor units and uncorrelated donor/acceptor relative distance and orientation. In this paper we carry out a combined Car-Parrinello molecular dynamics and TDDFT investigation to unravel the impact of thermal fluctuations on FRET in two dyadic carbazole-phenothiazine dye sensitizers. Both isolated and full-packed adsorption conditions are considered, mimicking the dye adsorption topology on TiO2. Results are discussed in relation to the above mentioned models and rationalized in terms of the structural differences of the considered dyes. We find a considerable difference between the FRET rates calculated at zero temperature and the results obtained by including thermal fluctuations, highlighting an important role of the latter in determining FRET rates in dyadic donor-acceptor dye-sensitized solar cells.",
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Thermal Fluctuations on Förster Resonance Energy Transfer in Dyadic Solar Cell Sensitizers : A Combined Ab Initio Molecular Dynamics and TDDFT Investigation. / Urzúa-Leiva, Rodrigo A.; Rampino, Sergio; Arratia-Perez, Ramiro; Mosconi, Edoardo; Pastore, Mariachiara; Angelis, Filippo De.

En: Journal of Physical Chemistry C, Vol. 119, N.º 29, 23.07.2015, p. 16490-16499.

Resultado de la investigación: Article

TY - JOUR

T1 - Thermal Fluctuations on Förster Resonance Energy Transfer in Dyadic Solar Cell Sensitizers

T2 - A Combined Ab Initio Molecular Dynamics and TDDFT Investigation

AU - Urzúa-Leiva, Rodrigo A.

AU - Rampino, Sergio

AU - Arratia-Perez, Ramiro

AU - Mosconi, Edoardo

AU - Pastore, Mariachiara

AU - Angelis, Filippo De

PY - 2015/7/23

Y1 - 2015/7/23

N2 - Förster resonance energy transfer (FRET) is a key process in dyadic dye-sensitized solar cells (DSSCs) where an "antenna" donor has the role of collecting photons and redirecting the captured energy to an adsorbed-dye acceptor unit. Despite its popularity in, e.g., biology, where FRET rates are used to derive structural information on fairly complex systems, relatively few studies have appeared in the DSSCs field. These were based, to the best of our knowledge, either on a static modeling of FRET or on the so called isotropic regime assuming an isotropic motion of the donor/acceptor units and uncorrelated donor/acceptor relative distance and orientation. In this paper we carry out a combined Car-Parrinello molecular dynamics and TDDFT investigation to unravel the impact of thermal fluctuations on FRET in two dyadic carbazole-phenothiazine dye sensitizers. Both isolated and full-packed adsorption conditions are considered, mimicking the dye adsorption topology on TiO2. Results are discussed in relation to the above mentioned models and rationalized in terms of the structural differences of the considered dyes. We find a considerable difference between the FRET rates calculated at zero temperature and the results obtained by including thermal fluctuations, highlighting an important role of the latter in determining FRET rates in dyadic donor-acceptor dye-sensitized solar cells.

AB - Förster resonance energy transfer (FRET) is a key process in dyadic dye-sensitized solar cells (DSSCs) where an "antenna" donor has the role of collecting photons and redirecting the captured energy to an adsorbed-dye acceptor unit. Despite its popularity in, e.g., biology, where FRET rates are used to derive structural information on fairly complex systems, relatively few studies have appeared in the DSSCs field. These were based, to the best of our knowledge, either on a static modeling of FRET or on the so called isotropic regime assuming an isotropic motion of the donor/acceptor units and uncorrelated donor/acceptor relative distance and orientation. In this paper we carry out a combined Car-Parrinello molecular dynamics and TDDFT investigation to unravel the impact of thermal fluctuations on FRET in two dyadic carbazole-phenothiazine dye sensitizers. Both isolated and full-packed adsorption conditions are considered, mimicking the dye adsorption topology on TiO2. Results are discussed in relation to the above mentioned models and rationalized in terms of the structural differences of the considered dyes. We find a considerable difference between the FRET rates calculated at zero temperature and the results obtained by including thermal fluctuations, highlighting an important role of the latter in determining FRET rates in dyadic donor-acceptor dye-sensitized solar cells.

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