Measuring and Controlling the Electronic Structure of PbS QDs
Matthew Beard a, Craig Perkins a, Jianbing Zhang a, Jao van de Lagemaat a, Joseph Luther a, Elisa Miller a, Daniel Kroupa a, Ryan Crisp a, Antoine Kahn b, Philip Schulz b
a NREL, 16253 Denver West Parkway, Golden, 80401, United States
b Department of Electrical Engineering, Princeton University, Department of Electrical Engineering, Princeton University, Princeton, NJ 08544, United States
c Chemical and Biosciences Department, University of Colorado, Boulder, University of Colorado, Chemical and Biosciences Department, Boulder, Colorado 80309, United States
d Department of Physics, Colorado School of Mines, Department of Physics, Colorado School of Mines, Golden, CO 80401, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe September Meeting 2015 (NFM15)
Santiago de Compostela, Spain, 2015 September 6th - 15th
Oral, Elisa Miller, presentation 046
Publication date: 8th June 2015

Quantum Dot (QD) solar cells are an active area of photovoltaics (PVs) research due to their potential to be competitive devices in the PV market.  Tuning the band alignment of PbS QD solar cells enhances solar cell efficiencies; therefore, it is important to correctly quantify the valence band maximum (VBM) and conduction band minimum (CBM).  The PV community typically relies on X-ray and ultraviolet photoelectron spectroscopy (XPS and UPS) measurements for the QD band energies. These XPS/UPS measurements are used to directly measure the VBM and indirectly determine the CBM. For size-selected PbS QDs, previous photoelectron spectroscopy reports have determined that the VBM is independent of the PbS QD size and, therefore, only the CBM is dependent on the QD size. We show with a comprehensive XPS/UPS study on size-selected PbS QDs that the previous results are incorrectly interpreted and that both the VBM and CBM energies are dependent on the PbS QD size. This is shown through a combination of UPS/XPS, inverse photoelectron spectroscopy (IPES) measurements, effective mass approximation, GW calculations, and other experimental techniques. With this knowledge, we show that XPS VB measurements can still be used to study the effects of surface treatments. We show that the Fermi level to VB position can be controlled with different surface treatments, such as TBAI, MPA, PbI2, and Na2S, to make the PbS QD thin films more n- or p-type; however, we do not assign absolute energies to the VBM or CBM through these measurements.



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