The process of photon upconversion promises importance for many optoelectronic applications, as it can result in higher efficiencies and more effective photon management. Upconversion via triplet−triplet annihilation (TTA) occurs at low incident powers and at high efficiencies, requirements for integration into existing optoelectronic devices. Semiconductor nanocrystals are a diverse class of triplet sensitizers with advantages over traditional molecular sensitizers such as energetic tunability and minimal energy loss during the triplet sensitization process. In this Perspective, we review current progress in semiconductor nanocrystal triplet sensitization, specifically focusing on the nanocrystal, the ligand shell which surrounds the nanocrystal, and progress in solid-state sensitization. Finally, we discuss potential areas of improvement which could result in more efficient upconversion systems sensitized by semiconductor nanocrystals. Specifically, we focus on the development of solid-state TTA upconversion systems, elucidation of the energy transfer mechanisms from nanocrystal to transmitter ligand which underpin the upconversion process and propose novel configurations of nanocrystal-sensitized systems.

Photon upconversion, particularly via triplet-triplet annihilation (TTA), could prove beneficial in expanding the efficiencies and overall impacts of optoelectronic devices across a multitude of technologies. The recent development of bulk metal halide perovskites as triplet sensitizers is one potential step toward the industrialization of upconversion-enabled devices. Here, we investigate the impact of varying additions of bromide into a lead iodide perovskite thin film on the TTA upconversion process in the annihilator molecule rubrene. We find an interplay between the bromide content and the overall device efficiency. In particular, a higher bromide content results in higher internal upconversion efficiencies, enabled by more efficient charge extraction at the interface, likely due to a more favorable band alignment. However, the external upconversion efficiency decreases, as the absorption cross section in the near infrared is reduced. The highest upconversion performance is found in our study for a bromide content of 5%. This result can be traced back to a high absorption cross section in the near infrared and higher photoluminescence quantum yield in comparison to the iodide-only perovskite, as well as an increased driving force for charge transfer.

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Metal halide perovskite materials have recently upended the field of photovoltaics and are aiming to make waves across a multitude of other fields and applications. Recently, perovskite nanocrystals have been synthesized and are rapidly outpacing traditional semiconductor nanocrystals in application driven fields due to their inherent defect tolerance and facile tunability, resulting in high photoluminescent quantum yields and efficient devices. Future improvements to perovskite nanocrystals toward device driven applications must come at the perovskite surface. The last half decade has resulted in considerable progress in tailoring the perovskite nanocrystal/ligand surface toward maximizing the optoelectronic performance. Here, we review the current progress and discuss how further improvements could be made to further improve this bright class of materials.

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