Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics

Wheeler, Lance M.; Sanehira, Erin M.; Marshall, Ashley R.; Schulz, Philip; Suri, Mokshin; Anderson, Nicholas C.; Christians, Jeffrey A.; Nordlund, Dennis; Sokaras, Dimosthenis; Kröll, Thomas; Harvey, Steven P.; Berry, Joseph J.; Lin, Lih Y.; Luther, Joseph M.

doi:10.1021/jacs.8b04984

Cited by 324 publications

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“…[39][40][41][42][43][44][45] The change from bulk to nanoscale endows materials new advantages in engineering discrete energy levels, solution processing, and composition management. Quite recently, all-inorganic perovskite nanocrystals or QDs with CsPbX 3 stoichiometry quickly emerged and attracted wide attention in optoelectronic devices due to their flexible composition adjustment, size tunability, high tolerance to defects, and greatly improved phase stability.…”

mentioning

confidence: 99%

“…[39][40][41][42][43][44][45] The change from bulk to nanoscale endows materials new advantages in engineering discrete energy levels, solution processing, and composition management. [43] Extensive previous work on PbS QDs has demonstrated that surface ligands can modulate the peculiarity of QDs in terms of dispersibility in solution, electron coupling between QDs in film and density of trap states, as well as stability. [40] In addition, a formamidinium iodide (FAI) treatment on CsPbI 3 QD films was developed, which can double the carrier mobility in the film, enabling increased photocurrent, and led to a record certified QD solar cell efficiency of 13.4%.…”

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confidence: 99%

“…The CsAc-treated cells show enhanced efficiency and narrower PCE distribution compared to the control cells, confirming the improved reproducibility of QD solar cells. [43] Therefore, the removal of long organic ligands could decrease the distance between individual QDs and could further enhance electron coupling. The underlying reasons for the improvement will be discussed in the following section.…”

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confidence: 99%

“…It is worth noting that the enhanced average PCE (from 11.96% to 13.67%) is mainly attributed to the improved J SC (from 13.23 to 14.66 mA cm −2 ) and FF (from 0.733 to 0.750) in the CsAc-treated cells. [43] To assess whether CsAc post-treatment would induce the grain growth of CsPbI 3 QDs, the morphology of QD films w/wo treatment was then investigated. The external quantum efficiency (EQE) curves in Figure 1d reveal that the best CsAc-treated cell exhibits higher EQE values between 350 and 700 nm than that of the control cell.…”

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14.1% CsPbI₃ Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

Ling

Zhou

Yuan

et al. 2019

Advanced Energy Materials

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During the past decade, inorganic CQDs, namely the lead chalcogenides (e.g., PbS), have attracted tremendous attention in solution-processed solar cells. Due to the great efforts on CQDs synthesis modification, [7][8][9] surface passivation, [10][11][12] and device fabrication optimization, [13][14][15][16] PbS QD solar cells continue to progress at an extraordinary rate, improving overall efficiencies by ≈1% per year and currently have a certified power conversion efficiency (PCE) exceeding 12%. [17] Meanwhile, the past decade has witnessed unprecedented success of organicinorganic hybrid perovskites in PV applications, with the reported PCE of perovskite solar cells exceeding 23%. [18][19][20][21][22][23][24][25][26][27][28] However, the challenging stability issues of these hybrid perovskites further motivate the research of all-inorganic perovskites (CsPbX 3 , X = Cl − , Br − , I − or mixed halides) without any volatile organic components. [29][30][31][32][33][34][35][36][37][38] Among these all-inorganic perovskite materials, α-CsPbI 3 exhibits an ideal optical bandgap (E g ) of 1.73 eV for PV applications. However, the nonphotoactive orthorhombic phase (E g = 2.82 eV) is more thermodynamically preferred at low temperature. [29] Therefore, the perovskite phase of CsPbI 3 usually requires complex annealing processes at high temperature to achieve satisfactory film quality. As mentioned above, QD technology offers colloidal synthesis of conventional bulk materials, which Surface manipulation of quantum dots (QDs) has been extensively reported to be crucial to their performance when applied into optoelectronic devices, especially for photovoltaic devices. In this work, an efficient surface passivation method for emerging CsPbI 3 perovskite QDs using a variety of inorganic cesium salts (cesium acetate (CsAc), cesium idodide (CsI), cesium carbonate (Cs 2 CO 3 ), and cesium nitrate (CsNO 3 )) is reported. The Cs-salts post-treatment can not only fill the vacancy at the CsPbI 3 perovskite surface but also improve electron coupling between CsPbI 3 QDs. As a result, the free carrier lifetime, diffusion length, and mobility of QD film are simultaneously improved, which are beneficial for fabricating high-quality conductive QD films for efficient solar cell devices. After optimizing the post-treatment process, the short-circuit current density and fill factor are significantly enhanced, delivering an impressive efficiency of 14.10% for CsPbI 3 QD solar cells. In addition, the Cs-salt-treated CsPbI 3 QD devices exhibit improved stability against moisture due to the improved surface environment of these QDs. These findings will provide insight into the design of high-performance and low-trap-states perovskite QD films with desirable optoelectronic properties. Perovskite Quantum DotsThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.Solution-processed colloidal quantum dots (CQDs) are promising candidates for the next generation photovoltaics (PVs) due to the excellent tuna...

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mentioning

confidence: 99%

“…[39][40][41][42][43][44][45] The change from bulk to nanoscale endows materials new advantages in engineering discrete energy levels, solution processing, and composition management. [43] Extensive previous work on PbS QDs has demonstrated that surface ligands can modulate the peculiarity of QDs in terms of dispersibility in solution, electron coupling between QDs in film and density of trap states, as well as stability. [40] In addition, a formamidinium iodide (FAI) treatment on CsPbI 3 QD films was developed, which can double the carrier mobility in the film, enabling increased photocurrent, and led to a record certified QD solar cell efficiency of 13.4%.…”

mentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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14.1% CsPbI₃ Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

Ling

Zhou

Yuan

et al. 2019

Advanced Energy Materials

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“…Abdruck mit Genehmigung. [109] Copyright 2018, American Chemical Society. b) Chemische Struktur von mGR und CsPbI 3 -QDs und deren Quervernetzungsmechanismus;schematische Darstellung des Ladungstransportprozesses und des Stabilisierungsmechanismus fürdie filmbasierten mGR/CsPbI 3 -PSCs.…”

Section: Angewandte Chemieunclassified

Anorganische CsPbX₃‐Perowskit‐Solarzellen: Fortschritte und Perspektiven

et al. 2019

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+ + ]D ie Autoren haben zu gleichen Teilen zu dieser Arbeit beigetragen. Die Identifikationsnummern (ORCID) der Autoren sind unter https://doi.org/10.1002/ange.201901081 zu finden.Perowskite auf Halogenidbasis haben sicha ufgrund ihrer hervorragenden optoelektronischen Eigenschaften zu einem der wichtigsten Themen in der Photovoltaik-Forschung entwickelt. Insbesondere wurden bei organisch-anorganischen Perowskit-Solarzellen (PSCs) rasche Fortschritte beim Wirkungsgrad (PCE, power conversion efficiency) erreicht, mit einem derzeitigen Rekordwert von 23.7 %PCE. Die an sichinstabile Beschaffenheit dieser Materialien, insbesondere gegenüber Feuchtigkeit und Wärme,stellt jedoch ein Problem bezüglichihrer Langzeitstabilitätd ar.Der Ersatz der fragilen organischen Gruppe durch robustere anorganische Cs + -Kationen ergibt Caesiumbleihalogenide CsPbX 3 (X = Halogenid), die thermischv iel stabiler und meist auchs tabiler gegen andere Faktoren sind. Seit dem ersten Bericht im Jahr 2015 ist der PCE von CsPbX 3 -basierten PSCs von 2.9 %bis auf heute 17.1 %m it deutlichv erbesserter Stabilitätg estiegen. In diesem Aufsatz sollen die bisherigen Ergebnisse auf dem Gebiet zusammenfasst und Lçsungen fürE ntwicklungsengpässe vorgeschlagen werden.

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Nucleation and Growth of Colloidal Semiconductor Nanoparticles

Enright

Ritchhart

Cossairt

2020

Encyclopedia of Inorganic and Bioinorganic Chemistry

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Solution‐phase syntheses of semiconductor nanoparticles provide a versatile and scalable approach to obtain nanomaterials with desirable structure and function. The most common mechanism invoked to explain the nucleation and growth of colloidal semiconductor nanocrystals is the LaMer model, an extension of classical nucleation theory. This model is widely used to conceptualize the conversion of molecular precursors into nanoparticles, and is characterized by three stages: monomer buildup, nucleation, and particle growth. Each of these stages represents a fundamental aspect of nanoparticle synthesis, and each has been widely studied over the past several decades. One of the core successes of this model has been the prediction of the “burst nucleation” method, which has enabled the synthesis of monodisperse nanoparticles in many material systems. Increasingly, however, it has become apparent that many chemical systems do not follow classical nucleation theory, but rather grow via nonclassical cluster‐mediated or aggregative growth processes. Regardless of the nucleation mechanism, highly monodisperse semiconductor nanoparticles can be obtained through kinetic size focusing or digestive ripening. Kinetic size focusing occurs during the nanoparticle growth phase when monomer concentration is high and smaller particles grow faster than their larger counterparts, enabling the smaller particles to “catch up” in size to give a more monodisperse ensemble. Digestive ripening, on the other hand, is a postsynthetic strategy where additional ligand is provided to the system to etch larger particles and redistribute monomer to smaller particles to get a more uniform sample. Beyond the synthesis of spherical colloidal nanoparticles, procedures can be modified to achieve a range of anisotropic structures including 1D nanorods and 2D nanosheets. Seeded and templated growth strategies can lend additional synthetic flexibility to more easily access a range of complex architectures. Continued innovation in synthetic methods and mechanistic understanding will pave the way for technological translation and lasting impact across applications from biological imaging to catalysis and many other next‐generation technologies.

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Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics

Cited by 324 publications

References 47 publications

14.1% CsPbI₃ Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

14.1% CsPbI₃ Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

Anorganische CsPbX₃‐Perowskit‐Solarzellen: Fortschritte und Perspektiven

Nucleation and Growth of Colloidal Semiconductor Nanoparticles

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Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics

Cited by 324 publications

References 47 publications

14.1% CsPbI3 Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

14.1% CsPbI3 Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

Anorganische CsPbX3‐Perowskit‐Solarzellen: Fortschritte und Perspektiven

Nucleation and Growth of Colloidal Semiconductor Nanoparticles

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14.1% CsPbI₃ Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

14.1% CsPbI₃ Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

Anorganische CsPbX₃‐Perowskit‐Solarzellen: Fortschritte und Perspektiven