Disrupted Attosecond Charge Carrier Delocalization at a Hybrid Organic/Inorganic Semiconductor Interface.
Despite significant interest in hybrid organic/inorganic semiconductor interfaces, little is known regarding the fate of charge carriers at metal oxide interfaces, particularly on ultrafast time scales. Using core-hole clock spectroscopy, we investigate the ultrafast charge carrier dynamics of conductive ZnO films at a hybrid interface with an organic semiconductor. The adsorption of C60 on the ZnO surface strongly suppresses the ultrafast carrier delocalization and increases the charge carrier residence time from 400 attoseconds to nearly 30 fs. Here, we show that a new hybridized interfacial density of states with substantial molecular character is formed, fundamentally altering the observed carrier dynamics. The remarkable change in the dynamics sheds light on the fate of carriers at hybrid organic/inorganic semiconductor interfaces relevant to organic optoelectronics and provides for the first time an atomistic picture of the electronically perturbed near-interface region of a metal oxide.
†Department of Chemistry and Biochemistry, University of Arizona, 1306 E. University Boulevard, Tucson, Arizona 85721, United States.
David A
DA
Racke
†Department of Chemistry and Biochemistry, University of Arizona, 1306 E. University Boulevard, Tucson, Arizona 85721, United States.
Leah L
LL
Kelly
‡School of Mechanical Engineering and Center for Organic Photonics and Electronics, Georgia Institute of Technology, 901 Atlantic Drive, Atlanta, Georgia 30332, United States.
Hyungchul
H
Kim
§National Renewable Energy Laboratory, National Center for Photovoltaics, 15013 Denver West Parkway, Golden, Colorado 80401, United States.
Philip
P
Schulz
§National Renewable Energy Laboratory, National Center for Photovoltaics, 15013 Denver West Parkway, Golden, Colorado 80401, United States.
Ajaya
A
Sigdel
§National Renewable Energy Laboratory, National Center for Photovoltaics, 15013 Denver West Parkway, Golden, Colorado 80401, United States.
Joseph J
JJ
Berry
‡School of Mechanical Engineering and Center for Organic Photonics and Electronics, Georgia Institute of Technology, 901 Atlantic Drive, Atlanta, Georgia 30332, United States.
Samuel
S
Graham
∥SLAC National Accelerator Laboratory, Stanford Synchrotron Radiation Lightsource, 2575 Sand Hill Road, MS 99, Menlo Park, California 94025, United States.
Dennis
D
Nordlund
†Department of Chemistry and Biochemistry, University of Arizona, 1306 E. University Boulevard, Tucson, Arizona 85721, United States.|⊥Department of Physics, University of Arizona, 1118 E. Fourth Street, Tucson, Arizona 85721, United States.
Oliver L A
OL
Monti
charge localization; core−hole clock; semiconductor; thin films