TY - JOUR
T1 - Surface-Area-Dependent Electron Transfer between Isoenergetic 2D Quantum Wells and a Molecular Acceptor
AU - Diroll, Benjamin T.
AU - Fedin, Igor
AU - Darancet, Pierre
AU - Talapin, Dmitri V.
AU - Schaller, Richard D.
N1 - Funding Information:
This work was performed in part at the Center for Nanoscale Materials, a US Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility under Contract No. DEAC02- 06CH11357.
Publisher Copyright:
© 2016 American Chemical Society.
PY - 2016/9/7
Y1 - 2016/9/7
N2 - We report measurements of electron transfer rates for four isoenergetic donor-acceptor pairs comprising a molecular electron acceptor, methylviologen (MV), and morphology-controlled colloidal semiconductor nanoparticles of CdSe. The four nanoparticles include a spherical quantum dot (QD) and three differing lateral areas of 4-monolayer-thick nanoplatelets (NPLs), each with a 2.42 eV energy gap. As such, the measurements, performed via ultrafast photoluminescence, relate the dependence of charge transfer rate on the spatial extent of the initial electron-hole pair wave function explicitly, which we show for the first time to be related to surface area in this regime that is intermediate between homogeneous and heterogeneous charge transfer as well as 2D to 0D electron transfer. The observed nonlinear dependence of rate with surface area is attributed to exciton delocalization within each structure, which we show via temperature-dependent absorption measurements remains constant.
AB - We report measurements of electron transfer rates for four isoenergetic donor-acceptor pairs comprising a molecular electron acceptor, methylviologen (MV), and morphology-controlled colloidal semiconductor nanoparticles of CdSe. The four nanoparticles include a spherical quantum dot (QD) and three differing lateral areas of 4-monolayer-thick nanoplatelets (NPLs), each with a 2.42 eV energy gap. As such, the measurements, performed via ultrafast photoluminescence, relate the dependence of charge transfer rate on the spatial extent of the initial electron-hole pair wave function explicitly, which we show for the first time to be related to surface area in this regime that is intermediate between homogeneous and heterogeneous charge transfer as well as 2D to 0D electron transfer. The observed nonlinear dependence of rate with surface area is attributed to exciton delocalization within each structure, which we show via temperature-dependent absorption measurements remains constant.
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U2 - 10.1021/jacs.6b06572
DO - 10.1021/jacs.6b06572
M3 - Article
C2 - 27518932
AN - SCOPUS:84986201023
VL - 138
SP - 11109
EP - 11112
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 35
ER -