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Photoluminescence (PL) spectroscopy has been used to study the defect levels in thin film copper indium diselenide (CuInSe 2 , CIS) which we are developing as the absorber layer for the bottom cell of a monolithically grown perovskite/CuInSe 2 tandem solar cell. Temperature and laser power dependent PL measurements of thin film CIS for two different Cu/In ratios (0.66 and 0.80) have been performed. The CIS film with Cu/In = 0.80 shows a prominent donor-to-acceptor peak (DAP) involving a shallow acceptor of binding energy ∼22 meV, with phonon replica at ∼32 meV spacing. In contrast, PL measurement of CIS film for Cu/In = 0.66 taken at 20 K exhibited an asymmetric and broad PL spectrum with peaks at 0.845 eV and 0.787 eV. Laser intensity dependent PL revealed that the observed peaks 0.845 eV and 0.787 eV shift towards higher energy (aka j-shift) at ∼11.7 meV/decade and ∼ 8 meV/decade with increase in laser intensity respectively. The asymmetric and broad spectrum together with large j-shift suggests that the observed peaks at 0.845 eV and 0.787 eV were related to band-to-tail (BT) and band-to-impurity (BI) transition, respectively. Such a band-tail-related transition originates from the potential fluctuation of defect states at low temperature. The appearance of band related transition in CIS film with Cu/In = 0.66 is the indicator of the presence of large number of charged defect states. 

Spectroscopic ellipsometry (SE) was performed on CuIn Se 2 (CIS) thin films and solar cells with a goal toward optimizing this low bandgap absorber for tandem applications. The CIS thin films and the absorbers in devices were deposited by one-stage thermal co-evaporation on silicon and on Mo-coated soda-lime glass substrates in a deposition system that has yielded CuIn 1-x Ga x Se 2 (CIGS) cells with > 17% efficiency using standard thickness (2.0 μm)x = 0.3 absorbers and > 13% using 0.7 μm low-Ga absorbers. In this study, a mapping capability for CIS Cu stoichiometry y = [Cu]/[In] over the film area was established based on a y-dependent parametric dielectric function (ε 1 , ε 2 ) with bandgap critical point E g decreasing linearly from 1.030 eV for y = 0.7 to 1.016 eV for y = 1.1. In addition, a full set of (ε 1 , ε 2 ) spectra measured for the CIS cell components enables analysis of SE data in terms of an accurate structural model for the device. With this model, spectra in the external quantum efficiency can be predicted, and deviations from this prediction can be attributed to incomplete collection of photogenerated electrons and holes as simulated with a carrier collection profile. 

ABSTRACT Methods of obtaining large grain size and high crystallinity in absorber materials play an important role in fabrication of high-performance methylammonium lead iodide (MAPbI 3 ) perovskite solar cells. Here we study the effect of adding small concentrations of Cd 2+ , Zn 2+ , and Fe 2+ salts to the perovskite precursor solution used in the single-step solution fabrication process. Enhanced grain size and crystallinity in MAPbI 3 films were obtained by using 0.1% of Cd 2+ or Zn 2+ in the precursor solution. Consequently, solar cells constructed with Cd- and Zn-doped perovskite films show a significant improvement in device performance. These results suggest that the process may be an effective and facile method to fabricate high-efficiency perovskite photovoltaic devices.