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We present a method for designing spectrally- selective optoelectronic films with a finite absorption bandwidth. We demonstrate the process by designing a film composed of lead sulfide colloidal quantum dots (PbS-CQDs). Designs incorporate the patterning of absorbing PbS-CQD films into photonic crystal- like slabs which couple incident light into leaky modes within the plane of the absorbing films, modulating the absorption spectrum. Computational times required to calculate optical spectra are drastically decreased by implementing the Fourier Modal Method. Furthermore, a supervised machine-learning-based inverse design methodology is presented which allows tailoring of the PbS-CQD film optical properties for use in a variety of photovoltaic applications, such as tandem cells in which spectral tailoring can enable current-matching flexibility. 

Lead Sulfide (PbS) colloidal quantum dots (CQDs) are promising materials for flexible and wearable photovoltaic devices and technologies due to their low cost, solution processibility and bandgap tunability with quantum dot size. However, PbS CQD solar cells have limitations on performance efficiency due to charge transport losses in the CQD layers and hole transport layer (HTL). This study pursues two promising techniques in parallel to address these challenges. Solution-phase annealing of the absorbing PbS-PbX2 (X = Br, I) layer can reduce charge transport losses by removing oleic acid and parasitic hydroxyl ligands. Additionally, optoelectronic simulations are used to show that HTL performance can be improved by the addition of a 2D transition metal dichalcogenide (TMD) layer to the PbS CQD-based HTL. We use solution-phase exfoliation to produce and incorporate 2D WSe2 nanoflakes into the HTL. We report a power conversion efficiency (PCE) increase of up to 3.4% for the solution-phase-annealed devices and up to 1% for the 2D WSe2 HTL augmented devices. A combination of these two techniques should result in high-performing PbS CQD solar cells, paving the way for further advancements in flexible photovoltaics.