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DOE OSTI · 2484177

Towards non-blinking and photostable perovskite quantum dots

Mi, Chenjia [University of Oklahoma, Norman, OK (United States); The University of Oklahoma] (ORCID:000000032169864X)·Gee, Gavin C. [University of Oklahoma, Norman, OK (United States)]·Lander, Chance W. [University of Oklahoma, Norman, OK (United States)] (ORCID:0000000288193905)·Shin, Donghoon [Northwestern University, Evanston, IL (United States)] (ORCID:000000025017547X)·Atteberry, Matthew L. [University of Oklahoma, Norman, OK (United States)]·Akhmedov, Novruz G. [University of Oklahoma, Norman, OK (United States)]·Hidayatova, Lamia [University of Oklahoma, Norman, OK (United States)]·DiCenso, Jesse D. [University of Oklahoma, Norman, OK (United States)]·Yip, Wai Tak [University of Oklahoma, Norman, OK (United States)]·Chen, Bin [Northwestern University, Evanston, IL (United States)] (ORCID:0000000221067664)·Shao, Yihan [University of Oklahoma, Norman, OK (United States)] (ORCID:000000019337341X)·Dong, Yitong [University of Oklahoma, Norman, OK (United States)] (ORCID:0000000270693725)
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Abstract

Surface defect-induced photoluminescence blinking and photodarkening are ubiquitous in lead halide perovskite quantum dots. Despite efforts to stabilize the surface by chemically engineering ligand binding moieties, blinking accompanied by photodegradation still poses barriers to implementing perovskite quantum dots in quantum emitters. To date, ligand tail engineering in the solid state has rarely been explored for perovskite quantum dots. We posit that attractive intermolecular interactions between low-steric ligand tails, such as π-π stacking, can promote the formation of a nearly epitaxial ligand layer that significantly reduces the quantum dot surface energy. Here, we show that single CsPbBr 3 quantum dots covered by stacked phenethylammonium ligands exhibit nearly non-blinking single photon emission with high purity (~98%) and extraordinary photostability (12 hours continuous operation and saturated excitations), allowing the determination of size-dependent exciton radiative rates and emission line widths of CsPbBr 3 quantum dots at the single particle level.

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36 MATERIALS SCIENCE37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY77 NANOSCIENCE AND NANOTECHNOLOGYExcited statesQuantum dots

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Mi, Chenjia [University of Oklahoma, Norman, OK (United States); The University of Oklahoma] (ORCID:000000032169864X), Gee, Gavin C. [University of Oklahoma, Norman, OK (United States)], Lander, Chance W. [University of Oklahoma, Norman, OK (United States)] (ORCID:0000000288193905), Shin, Donghoon [Northwestern University, Evanston, IL (United States)] (ORCID:000000025017547X), Atteberry, Matthew L. [University of Oklahoma, Norman, OK (United States)], Akhmedov, Novruz G. [University of Oklahoma, Norman, OK (United States)], Hidayatova, Lamia [University of Oklahoma, Norman, OK (United States)], DiCenso, Jesse D. [University of Oklahoma, Norman, OK (United States)], Yip, Wai Tak [University of Oklahoma, Norman, OK (United States)], Chen, Bin [Northwestern University, Evanston, IL (United States)] (ORCID:0000000221067664), Shao, Yihan [University of Oklahoma, Norman, OK (United States)] (ORCID:000000019337341X), Dong, Yitong [University of Oklahoma, Norman, OK (United States)] (ORCID:0000000270693725). 2025-01-02. Towards non-blinking and photostable perovskite quantum dots. https://doi.org/10.1038/s41467-024-55619-7

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The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

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