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This perspective identifies future technological directions for solar photovoltaics and examines potential limits to terawatt-scale PV deployment.

Quantum dot photovoltaics (QDPV) offer the potential for low-cost solar cells. To develop strategies for continued improvement in QDPVs, a better understanding of the factors that limit their performance is essential. Here, we study carrier recombination processes that limit the power conversion efficiency of PbS QDPVs. We demonstrate the presence of radiative sub-bandgap states and sub-bandgap state filling in operating devices by using photoluminescence (PL) and electroluminescence (EL) spectroscopy. These sub-bandgap states are most likely the origin of the high open-circuit-voltage (VOC) deficit and relatively limited carrier collection that have thus far been observed in QDPVs. Combining these results with our perspectives on recent progress in QDPV, we conclude that eliminating sub-bandgap states in PbS QD films has the potential to show a greater gain than may be attainable by optimization of interfaces between QDs and other materials. We suggest possible future directions that could guide the design of high-performance QDPVs.

Bismuth‐based compounds have recently gained increasing attention as potentially nontoxic and defect‐tolerant solar absorbers. However, many of the new materials recently investigated show limited photovoltaic performance. Herein, one such compound is explored in detail through theory and experiment: bismuth oxyiodide (BiOI). BiOI thin films are grown by chemical vapor transport and found to maintain the same tetragonal phase in ambient air for at least 197 d. The computations suggest BiOI to be tolerant to antisite and vacancy defects. All‐inorganic solar cells (ITO|NiOx|BiOI|ZnO|Al) with negligible hysteresis and up to 80% external quantum efficiency under select monochromatic excitation are demonstrated. The short‐circuit current densities and power conversion efficiencies under AM 1.5G illumination are nearly double those of previously reported BiOI solar cells, as well as other bismuth halide and chalcohalide photovoltaics recently explored by many groups. Through a detailed loss analysis using optical characterization, photoemission spectroscopy, and device modeling, direction for future improvements in efficiency is provided. This work demonstrates that BiOI, previously considered to be a poor photocatalyst, is promising for photovoltaics.

Vertical arrays of ZnO nanowires can decouple light absorption from carrier collection in PbS quantum dot solar cells and increase power conversion efficiencies by 35%. The resulting ordered bulk heterojunction devices achieve short-circuit current densities in excess of 20 mA cm(-2) and efficiencies of up to 4.9%.

Growth of semiconducting nanostructures on graphene would open up opportunities for the development of flexible optoelectronic devices, but challenges remain in preserving the structural and electrical properties of graphene during this process. We demonstrate growth of highly uniform and well-aligned ZnO nanowire arrays on graphene by modifying the graphene surface with conductive polymer interlayers. On the basis of this structure, we then demonstrate graphene cathode-based hybrid solar cells using two different photoactive materials, PbS quantum dots and the conjugated polymer P3HT, with AM 1.5G power conversion efficiencies of 4.2% and 0.5%, respectively, approaching the performance of ITO-based devices with similar architectures. Our method preserves beneficial properties of graphene and demonstrates that it can serve as a viable replacement for ITO in various photovoltaic device configurations.

Thin films of colloidal quantum dots (QDs) are promising solar photovoltaic (PV) absorbers in spite of their disordered nature. Disordered PV materials face a power conversion efficiency limit lower than the ideal Shockley–Queisser bound because of increased radiative recombination through band-tail states. However, investigations of band tailing in QD solar cells have been largely restricted to indirect measurements, leaving their ultimate efficiency in question. Here we use photothermal deflection spectroscopy (PDS) to robustly characterize the absorption edge of lead sulfide (PbS) QD films for different bandgaps, ligands, and processing conditions used in leading devices. We also present a comprehensive overview of band tailing in many commercial and emerging PV technologiesincluding c-Si, GaAs, a-Si:H, CdTe, CIGS, and perovskitesthen calculate detailed-balance efficiency limits incorporating Urbach band tailing for each technology. Our PDS measurements on PbS QDs show sharp exponential band tails, with Urbach energies of 22 ± 1 meV for iodide-treated films and 24 ± 1 meV for ethanedithiol-treated films, comparable to those of polycrystalline CdTe and CIGS films. From these results, we calculate a maximum efficiency of 31%, close to the ideal limit without band tailing. This finding suggests that disorder does not constrain the long-term potential of QD solar cells.

Any new solar photovoltaic (PV) technology must reach low production costs to compete with today's marketleading crystalline silicon and commercial thin-film PV technologies. Colloidal quantum dots (QDs) could open up new applications by enabling lightweight and flexible PV modules. However, the cost of synthesizing nanocrystals at the large scale needed for PV module production has not previously been investigated. Based on our experience with commercial QD scale-up, we develop a Monte Carlo model to analyze the cost of synthesizing lead sulfide and metal halide perovskite QDs using 8 different reported synthetic methods. We also analyze the cost of solution-phase ligand exchange for preparing deposition-ready PbS QD inks, as well as the manufacturing cost for roll-to-roll solution-processed PV modules using these materials. We find that present QD synthesis costs are prohibitively high for PV applications, with median costs of 11 to 59 $ per g for PbS QDs (0.15 to 0.84 $ per W for a 20% efficient cell) and 73 $ per g for CsPbI 3 QDs (0.74 $ per W). QD ink preparation adds 6.3 $ per g (0.09 $ per W). In total, QD materials contribute up to 55% of the total module cost, making even roll-to-roll-processed QDPV modules significantly more expensive than silicon PV modules. These results suggest that the development of new low-cost synthetic methods is critically important for the commercial relevance of QD photovoltaics. Using our cost model, we identify strategies for reducing synthetic cost and propose a cost target of 5 $ per g to move QD solar cells closer to commercial viability. Broader contextColloidal quantum dots (QDs) have been widely investigated as an avenue toward ultra-low-cost solar photovoltaics (PV), alongside organics and metal halide perovskites. It is often implicitly assumed-and explicitly stated-that QD-based PV technologies can reach low cost because they employ low-cost, abundant elements and low-temperature, high-throughput manufacturing processes. However, this argument holds true only if QDs can be synthesized at low cost-materials dictate the module cost floor. Here we report the first detailed analysis of the cost of large-scale QD synthesis for PV applications. Our Monte Carlo approach constitutes a complete cost modeling framework for QD photovoltaics, from raw precursors to finished modules. We find that QD synthesis is prohibitively expensive today, highlighting the importance of synthetic cost for the commercial viability of QD solar technologies and guiding further research toward promising synthetic directions.