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High Efficiency Colloidal Quantum Dot Photovoltaics via Robust Self-Assembled Monolayers
김기환,F. Pelayo Garcia de Arquer,윤영진,Xinzheng Lan,Mengxia Liu,Oleksandr Voznyy,Zhenyu Yang,Fengjia Fan,Alexander H. Ip,Pongsakorn Kanjanaboos,Sjoerd Hoogland,김진영,Edward H. Sargent 한국고분자학회 2016 한국고분자학회 학술대회 연구논문 초록집 Vol.41 No.1
High-Efficiency Colloidal Quantum Dot Photovoltaics via Robust Self-Assembled Monolayers
Kim, Gi-Hwan,Garcí,a de Arquer, F. Pelayo,Yoon, Yung Jin,Lan, Xinzheng,Liu, Mengxia,Voznyy, Oleksandr,Yang, Zhenyu,Fan, Fengjia,Ip, Alexander H.,Kanjanaboos, Pongsakorn,Hoogland, Sjoerd,Kim, Jin American Chemical Society 2015 NANO LETTERS Vol.15 No.11
Metal-Organic Frameworks Mediate Cu Coordination for Selective CO<sub>2</sub> Electroreduction
Nam, Dae-Hyun,Bushuyev, Oleksandr S.,Li, Jun,De Luna, Phil,Seifitokaldani, Ali,Dinh, Cao-Thang,Garcí,a de Arquer, F. Pelayo,Wang, Yuhang,Liang, Zhiqin,Proppe, Andrew H.,Tan, Chih Shan,Todorovic& American Chemical Society 2018 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.140 No.36
<P>The electrochemical carbon dioxide reduction reaction (CO<SUB>2</SUB>RR) produces diverse chemical species. Cu clusters with a judiciously controlled surface coordination number (CN) provide active sites that simultaneously optimize selectivity, activity, and efficiency for CO<SUB>2</SUB>RR. Here we report a strategy involving metal-organic framework (MOF)-regulated Cu cluster formation that shifts CO<SUB>2</SUB> electroreduction toward multiple-carbon product generation. Specifically, we promoted undercoordinated sites during the formation of Cu clusters by controlling the structure of the Cu dimer, the precursor for Cu clusters. We distorted the symmetric paddle-wheel Cu dimer secondary building block of HKUST-1 to an asymmetric motif by separating adjacent benzene tricarboxylate moieties using thermal treatment. By varying materials processing conditions, we modulated the asymmetric local atomic structure, oxidation state and bonding strain of Cu dimers. Using electron paramagnetic resonance (EPR) and in situ X-ray absorption spectroscopy (XAS) experiments, we observed the formation of Cu clusters with low CN from distorted Cu dimers in HKUST-1 during CO<SUB>2</SUB> electroreduction. These exhibited 45% C<SUB>2</SUB>H<SUB>4</SUB> faradaic efficiency (FE), a record for MOF-derived Cu cluster catalysts. A structure-activity relationship was established wherein the tuning of the Cu-Cu CN in Cu clusters determines the CO<SUB>2</SUB>RR selectivity.</P> [FIG OMISSION]</BR>
Acid-Assisted Ligand Exchange Enhances Coupling in Colloidal Quantum Dot Solids
Jo, Jea Woong,Choi, Jongmin,Garcí,a de Arquer, F. Pelayo,Seifitokaldani, Ali,Sun, Bin,Kim, Younghoon,Ahn, Hyungju,Fan, James,Quintero-Bermudez, Rafael,Kim, Junghwan,Choi, Min-Jae,Baek, Se-Woong American Chemical Society 2018 NANO LETTERS Vol.18 No.7
<P>Colloidal quantum dots (CQDs) are promising solution-processed infrared-absorbing materials for optoelectronics. In these applications, it is crucial to replace the electrically insulating ligands used in synthesis to form strongly coupled quantum dot solids. Recently, solution-phase ligand-exchange strategies have been reported that minimize the density of defects and the polydispersity of CQDs; however, we find herein that the new ligands exhibit insufficient chemical reactivity to remove original oleic acid ligands completely. This leads to low CQD packing and correspondingly low electronic performance. Here we report an acid-assisted solution-phase ligand-exchange strategy that, by enabling efficient removal of the original ligands, enables the synthesis of densified CQD arrays. Our use of hydroiodic acid simultaneously facilitates high CQD packing via proton donation and CQD passivation through iodine. We demonstrate highly packed CQD films with a 2.5 times increased carrier mobility compared with prior exchanges. The resulting devices achieve the highest infrared photon-to-electron conversion efficiencies (>50%) reported in the spectral range of 0.8 to 1.1 eV.</P> [FIG OMISSION]</BR>
Tailoring the Energy Landscape in Quasi-2D Halide Perovskites Enables Efficient Green-Light Emission
Quan, Li Na,Zhao, Yongbiao,Garcí,a de Arquer, F. Pelayo,Sabatini, Randy,Walters, Grant,Voznyy, Oleksandr,Comin, Riccardo,Li, Yiying,Fan, James Z.,Tan, Hairen,Pan, Jun,Yuan, Mingjian,Bakr, Osman American Chemical Society 2017 NANO LETTERS Vol.17 No.6
<P>Organo-metal halide perovskites are a promising platform for optoelectronic applications in view of their excellent charge-transport and bandgap tunability. However, their low photoluminescence quantum efficiencies, especially in low-excitation regimes, limit their efficiency for light emission. Consequently, perovskite light-emitting devices are operated under high injection, a regime under which the materials have so far been unstable. Here we show that, by concentrating photoexcited states into a small subpopulation of radiative domains, one can achieve a high quantum yield, even at low excitation intensities. We tailor the composition of quasi-2D perovskites to direct the energy transfer into the lowest-bandgap minority phase and to do so faster than it is lost to nonradiative centers. The new material exhibits 60% photoluminescence quantum yield at excitation intensities as low as 1.8 mW/cm(2), yielding a ratio of quantum yield to excitation intensity of 0.3 cm(2)/mW; this represents a decrease of 2 orders of magnitude in the excitation power required to reach high efficiency compared with the best prior reports. Using this strategy, we report light-emitting diodes with external quantum efficiencies of 7.4% and a high luminescence of 8400 cd/m(2).</P>
A Novel DPP Based Polymer HTL for PbS CQD-SCs
천형진,김홍일,백세웅,류승언,이승진,최민재,최경원,Margherita Biondi,Sjoerd Hoogland,F. Pelayo Garcia de Arquer,권순기,박태호,Edward H. Sargent,김윤희 한국고분자학회 2021 한국고분자학회 학술대회 연구논문 초록집 Vol.46 No.1
DPP-based polymers are widely used in organic photovoltaics (OPV) and organic field-effect transistors (OFET) as the p-type materials. DPP with bithiophene (π-bridge) has already been proven to have excellent charge transport properties owing to an attractive S···O electrostatic interaction that induces π–π stacking. Therefore, we were performed Stille coupling reaction to combine these D–A building blocks to form the desired HTL. PD2FCT-29DPP (D1–A1–D1–A2) is a D–A alternating copolymer from the DPP (A2) and CPDT (D1) with fluorinated BT (A1). PD2FCT-29DPP-based devices achieve an FF of 70.0% and a PCE of 14.0%.