Monolithic integrated thin film tandem solar cells consisting of a high bandgap perovskite top cell and a low bandgap thin film bottom cell are expected to reach higher power conversion efficiencies (PCEs) with lower manufacturing cost and environmental impacts than the market-dominant crystalline silicon photovoltaics. There have been several demonstrations of 4-terminal and 2-terminal perovskite tandem devices with CuInGaSe2 (CIGS) or CuInSe2 (CIS) and, similar to the other tandem structures, the optimization of this device relies on optimal choice for the perovskite bandgap and thickness. Therefore, further advancement will be enabled by tuning the perovskite absorber to maximize the photocurrent limited by the current match condition. Here, we systematically study the optical absorption and transmission of perovskite thin films with varying absorber band gap. Based on these results, we model the photocurrent generations in both perovskite and CIS subcells and estimate the performances of projected tandem devices by considering the ideally functioning perovskite and CIS device. Our results show that for perovskite layers with 500 nm thickness the optimal bandgap is around 1.6 eV. With these configurations, PCEs above 20% could be achieved by monolithically integrated perovskite/CIS tandem solar cells. Also by modelling the absorption at every layer we calculate the quantum efficiency at each subcell in addition to tracking optical losses.

Photoluminescence (PL) spectroscopy has been used to study the defect levels in thin film copper indium diselenide (CuInSe2, CIS) which we are developing as the absorber layer for the bottom cell of a monolithically grown perovskite/CuInSe2 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.