Covalent Linking Greatly Enhances Photoinduced Electron Transfer in Fullerene-Quantum Dot Nanocomposites: Time-Domain Ab Initio Study

Vitaly V. Chaban, Victor Prezhdo, Oleg Prezhdo

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

Resumé

Nonadiabatic molecular dynamics combined with time-domain density functional theory are used to study electron transfer (ET) from a CdSe quantum dot (QD) to the C-60 fullerene, occurring in several types of hybrid organic/inorganic nanocomposites. By unveiling the time dependence of the ET process, we show that covalent bonding between the QD and C-60 is particularly important to ensure ultrafast transmission of the excited electron from the QD photon-harvester to the C-60 electron acceptor. Despite the close proximity of the donor and acceptor species provided by direct van der Waals contact, it leads to a notably weaker QD-C-60 interaction than a lengthy molecular bridge. We show that the ET rate in a nonbonded mixture of QDs and C-60 can be enhanced by doping. The photoinduced ET is promoted primarily by mid- and low-frequency vibrations. The study establishes the basic design principles for enhancing photoinduced charge separation in nanoscale light harvesting materials.
OriginalsprogEngelsk
TidsskriftThe Journal of Physical Chemistry Letters
Vol/bind4
Udgave nummer1
Sider (fra-til)1-6
ISSN1948-7185
DOI
StatusUdgivet - 2013

Fingeraftryk

Fullerenes
Semiconductor quantum dots
Nanocomposites
Electrons
Harvesters
Density functional theory
Molecular dynamics
Photons
Doping (additives)

Citer dette

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abstract = "Nonadiabatic molecular dynamics combined with time-domain density functional theory are used to study electron transfer (ET) from a CdSe quantum dot (QD) to the C-60 fullerene, occurring in several types of hybrid organic/inorganic nanocomposites. By unveiling the time dependence of the ET process, we show that covalent bonding between the QD and C-60 is particularly important to ensure ultrafast transmission of the excited electron from the QD photon-harvester to the C-60 electron acceptor. Despite the close proximity of the donor and acceptor species provided by direct van der Waals contact, it leads to a notably weaker QD-C-60 interaction than a lengthy molecular bridge. We show that the ET rate in a nonbonded mixture of QDs and C-60 can be enhanced by doping. The photoinduced ET is promoted primarily by mid- and low-frequency vibrations. The study establishes the basic design principles for enhancing photoinduced charge separation in nanoscale light harvesting materials.",
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Covalent Linking Greatly Enhances Photoinduced Electron Transfer in Fullerene-Quantum Dot Nanocomposites: Time-Domain Ab Initio Study. / Chaban, Vitaly V. ; Prezhdo, Victor ; Prezhdo, Oleg.

I: The Journal of Physical Chemistry Letters, Bind 4, Nr. 1, 2013, s. 1-6.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

TY - JOUR

T1 - Covalent Linking Greatly Enhances Photoinduced Electron Transfer in Fullerene-Quantum Dot Nanocomposites: Time-Domain Ab Initio Study

AU - Chaban, Vitaly V.

AU - Prezhdo, Victor

AU - Prezhdo, Oleg

PY - 2013

Y1 - 2013

N2 - Nonadiabatic molecular dynamics combined with time-domain density functional theory are used to study electron transfer (ET) from a CdSe quantum dot (QD) to the C-60 fullerene, occurring in several types of hybrid organic/inorganic nanocomposites. By unveiling the time dependence of the ET process, we show that covalent bonding between the QD and C-60 is particularly important to ensure ultrafast transmission of the excited electron from the QD photon-harvester to the C-60 electron acceptor. Despite the close proximity of the donor and acceptor species provided by direct van der Waals contact, it leads to a notably weaker QD-C-60 interaction than a lengthy molecular bridge. We show that the ET rate in a nonbonded mixture of QDs and C-60 can be enhanced by doping. The photoinduced ET is promoted primarily by mid- and low-frequency vibrations. The study establishes the basic design principles for enhancing photoinduced charge separation in nanoscale light harvesting materials.

AB - Nonadiabatic molecular dynamics combined with time-domain density functional theory are used to study electron transfer (ET) from a CdSe quantum dot (QD) to the C-60 fullerene, occurring in several types of hybrid organic/inorganic nanocomposites. By unveiling the time dependence of the ET process, we show that covalent bonding between the QD and C-60 is particularly important to ensure ultrafast transmission of the excited electron from the QD photon-harvester to the C-60 electron acceptor. Despite the close proximity of the donor and acceptor species provided by direct van der Waals contact, it leads to a notably weaker QD-C-60 interaction than a lengthy molecular bridge. We show that the ET rate in a nonbonded mixture of QDs and C-60 can be enhanced by doping. The photoinduced ET is promoted primarily by mid- and low-frequency vibrations. The study establishes the basic design principles for enhancing photoinduced charge separation in nanoscale light harvesting materials.

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