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Showing papers by "Alex K.-Y. Jen published in 2020"


Journal ArticleDOI
TL;DR: A rationally designed bifunctional molecule, piperazinium iodide (PI), containing both R2NH and R2 NH2+ groups on the same six-membered ring, behaving both as an electron donor and an electron acceptor to react with different surface-terminating ends on perovskite films is reported.
Abstract: Passivating surface and bulk defects of perovskite films has been proven to be an effective way to minimize nonradiative recombination losses in perovskite solar cells (PVSCs). The lattice interference and perturbation of atomic periodicity at the perovskite surfaces often significantly affect the material properties and device efficiencies. By tailoring the terminal groups on the perovskite surface and modifying the surface chemical environment, the defects can be reduced to enhance the photovoltaic performance and stability of derived PVSCs. Here, we report a rationally designed bifunctional molecule, piperazinium iodide (PI), containing both R2NH and R2NH2+ groups on the same six-membered ring, behaving both as an electron donor and an electron acceptor to react with different surface-terminating ends on perovskite films. The resulting perovskite films after defect passivation show released surface residual stress, suppressed nonradiative recombination loss, and more n-type characteristics for sufficient energy transfer. Consequently, charge recombination is significantly suppressed to result in a high open-circuit voltage (VOC) of 1.17 V and a reduced VOC loss of 0.33 V. A very high power conversion efficiency (PCE) of 23.37% (with 22.75% certified) could be achieved, which is the highest value reported for inverted PVSCs. Our work reveals a very effective way of using rationally designed bifunctional molecules to simultaneously enhance the device performance and stability.

336 citations


Journal ArticleDOI
TL;DR: The studies reveal that the nitrile (C-N) groups on the small molecule effectively reduce the trap density of the perovskite film and thus significantly suppresses the non-radiative recombination in the derived PVSC by passivating the Pb-exposed surface, resulting in an improved open-circuit voltage from 1.10 V to 1.16”V after passivation.
Abstract: All-inorganic perovskite solar cells (PVSCs) have drawn increasing attention because of their outstanding thermal stability. However, their performance is still inferior than the typical organic-inorganic counterparts, especially for the devices with p-i-n configuration. Herein, we successfully employ a Lewis base small molecule to passivate the inorganic perovskite film, and its derived PVSCs achieved a champion efficiency of 16.1% and a certificated efficiency of 15.6% with improved photostability, representing the most efficient inverted all-inorganic PVSCs to date. Our studies reveal that the nitrile (C-N) groups on the small molecule effectively reduce the trap density of the perovskite film and thus significantly suppresses the non-radiative recombination in the derived PVSC by passivating the Pb-exposed surface, resulting in an improved open-circuit voltage from 1.10 V to 1.16 V after passivation. This work provides an insight in the design of functional interlayers for improving efficiencies and stability of all-inorganic PVSCs. There has been a hot competition to optimize the device performance for all-inorganic perovskite solar cells. Here Wang et al. employ a Lewis base molecule to suppresses the non-radiative recombination in the inverted device and achieve a champion efficiency of 16.1%.

307 citations


Journal ArticleDOI
TL;DR: Chlorine-functionalized graphdiyne (GCl) is successfully applied as a multifunctional solid additive to fine-tune the morphology and improve device efficiency as well as reproductivity for the first time and confirms the efficacy of GCl to enhance device performance.
Abstract: Morphology tuning of the blend film in organic solar cells (OSCs) is a key approach to improve device efficiencies. Among various strategies, solid additive is proposed as a simple and new way to enable morphology tuning. However, there exist few solid additives reported to meet such expectations. Herein, chlorine-functionalized graphdiyne (GCl) is successfully applied as a multifunctional solid additive to fine-tune the morphology and improve device efficiency as well as reproductivity for the first time. Compared with 15.6% efficiency for control devices, a record high efficiency of 17.3% with the certified one of 17.1% is obtained along with the simultaneous increase of short-circuit current (Jsc ) and fill factor (FF), displaying the state-of-the-art binary organic solar cells at present. The redshift of the film absorption, enhanced crystallinity, prominent phase separation, improved mobility, and decreased charge recombination synergistically account for the increase of Jsc and FF after introducing GCl into the blend film. Moreover, the addition of GCl dramatically reduces batch-to-batch variations benefiting mass production owing to the nonvolatile property of GCl. All these results confirm the efficacy of GCl to enhance device performance, demonstrating a promising application of GCl as a multifunctional solid additive in the field of OSCs.

302 citations


Journal ArticleDOI
17 Jun 2020-Joule
TL;DR: In this paper, a large alkylammonium interlayer (LAI) was employed to reduce the energy loss occurred between transport layers and perovskite, which can simultaneously suppress the non-radiative energy losses at both top and bottom interfaces.

220 citations


Journal ArticleDOI
TL;DR: The face-to-face π-core interaction induced by benzo[2,1,3]thiadiazole S-N containing moieties plays a significant role in governing the molecular geometries and unique packing of Y6 and CH1007 to ensure their superior charge-transporting properties.
Abstract: Understanding the molecular structure and self-assembly of thiadiazole-derived non-fullerene acceptors (NFAs) is very critical for elucidating the origin of their extraordinary charge generation an...

212 citations


Journal ArticleDOI
TL;DR: A thiol-functionalized 2D conjugated metal–organic framework as an electron-extraction layer at the perovskite/cathode interface enables the realization of highly stable perovSKite solar cells with minimized lead ion leakage.
Abstract: Despite the notable progress in perovskite solar cells, maintaining long-term operational stability and minimizing potentially leaked lead (Pb2+) ions are two challenges that are yet to be resolved. Here we address these issues using a thiol-functionalized 2D conjugated metal–organic framework as an electron-extraction layer at the perovskite/cathode interface. The resultant devices exhibit high power conversion efficiency (22.02%) along with a substantially improved long-term operational stability. The perovskite solar cell modified with a metal–organic framework could retain more than 90% of its initial efficiency under accelerated testing conditions, that is continuous light irradiation at maximum power point tracking for 1,000 h at 85 °C. More importantly, the functionalized metal–organic framework could capture most of the Pb2+ leaked from the degraded perovskite solar cells by forming water-insoluble solids. Therefore, this method that simultaneously tackles the operational stability and lead contamination issues in perovskite solar cells could greatly improve the feasibility of large-scale deployment of perovskite photovoltaic technology. Two-dimensional conjugated metal–organic frameworks used as an electron-extraction layer enable the realization of highly stable perovskite solar cells with minimized lead ion leakage.

203 citations


Journal ArticleDOI
TL;DR: In this article, the authors show that incorporating a third component with lower miscibility and higher lowest unoccupied molecular orbital (LUMO) level into the state-of-the-art PM6:Y6 system can significantly enhance the performance of devices.
Abstract: It is widely known that the miscibility between donor and acceptor is a crucial factor that affects the morphology and thus device performance of nonfullerene organic solar cells (OSCs). In this Letter, we show that incorporating a third component with lower miscibility and higher lowest unoccupied molecular orbital (LUMO) level into the state-of-the-art PM6:Y6 system can significantly enhance the performance of devices. The best results of the ternary devices are achieved by adding a small molecular acceptor named ITCPTC (similar to 5% w/w), which significantly improves the power conversion efficiency (PCE) of the host system from 16.44% to 17.42%. The higher LUMO of the third component increases the open-circuit voltage (V-oc), while the low miscibility enlarges the domains and leads to improved short-circuit current density (J(sc)) and fill factor (FF). The efficacy of this strategy is supported by using other nonfullerene third components including an asymmetric small molecule (N7IT) and a polymer acceptor (PF2-DTC), which play the same role as ITCPTC and boost the PCEs to 16.96% and 17.04%, respectively. Our approach can be potentially applied to a wide range of OSC material systems and should facilitate the development of the OSC field.

176 citations


Journal ArticleDOI
TL;DR: Recent progress in the rational design, morphology, dynamics, and multi-functional applications starting from 2015 will be highlighted to deepen understanding of the structure-property relationship.
Abstract: With developments in materials, thin-film processing, fine-tuning of morphology, and optimization of device fabrication, the performance of organic solar cells (OSCs) has improved markedly in recent years Designing low-bandgap materials has been a focus in order to maximize solar energy conversion However, there are only a few successful low-bandgap donor materials developed with near-infrared (NIR) absorption that are well matched to the existing efficient acceptors Porphyrin has shown great potential as a useful building block for constructing low-bandgap donor materials due to its large conjugated plane and strong absorption Porphyrin-based donor materials have been shown to contribute to many record-high device efficiencies in small molecule, tandem, ternary, flexible, and OSC/perovskite hybrid solar cells Specifically, non-fullerene small-molecule solar cells have recently shown a high power conversion efficiency of 12% using low-bandgap porphyrin All these have validated the great potential of porphyrin derivatives as effective donor materials and made DPPEZnP-TRs a family of best low-bandgap donor materials in the OSC field so far Here, recent progress in the rational design, morphology, dynamics, and multi-functional applications starting from 2015 will be highlighted to deepen understanding of the structure-property relationship Finally, some future directions of porphyrin-based OSCs are presented

133 citations


Journal ArticleDOI
14 Oct 2020-Joule
TL;DR: In this paper, the authors used 4TIC as the additional non-fullerene acceptor (NFA) to construct ternary organic solar cells (SM-OSCs) with high power conversion efficiency (PCE) of 15.88%.

133 citations


Journal ArticleDOI
TL;DR: A Pb-S bonding approach is developed to synthesize water-resistant perovskite@silica nanodots that are capable of emitting and lasing in aqueous environments for long periods.
Abstract: Owing to their large absorption cross-sections and high photoluminescence quantum yields, lead halide perovskite quantum dots (PQDs) are regarded as a promising candidate for various optoelectronics applications. However, easy degradation of PQDs in water and in a humid environment is a critical hindrance for applications. Here we develop a Pb-S bonding approach to synthesize water-resistant perovskite@silica nanodots keeping their emission in water for over six weeks. A two-photon whispering-gallery mode laser device made of these ultra-stable nanodots retain 80% of its initial emission quantum yield when immersed in water for 13 h, and a two-photon random laser based on the perovskite@silica nanodots powder could still operate after the nanodots were dispersed in water for up to 15 days. Our synthetic approach opens up an entirely new avenue for utilizing PQDs in aqueous environment, which will significantly broaden their applications not only in optoelectronics but also in bioimaging and biosensing. Lead halide perovskite quantum dots (PQDs) promise applications in optoelectronics but are limited by sensitivity to wet environments. Here the authors develop a Pb-S bonding approach to synthesize PQDs@silica nanodots that are capable of emitting and lasing in aqueous environments for long periods.

111 citations


Journal ArticleDOI
TL;DR: In this article, the authors highlight the recent significant progress made in organic second-and third-order nonlinear optical materials for high-speed information processing in addressing the challenges of reduced energy consumption and enhanced speed and bandwidth.
Abstract: Organic nonlinear optical (NLO) materials are very important for high-speed information processing in addressing the challenges of reduced energy consumption and enhanced speed and bandwidth. In particular, organic second-order NLO materials are very promising for meeting the combined requirements of ultra-low energy and ultra-high bandwidth in electro-optic (EO) modulation, while organic third-order NLO materials have good potential for applications in ultra-speed all-optical signal processing (AOSP). This review highlights the recent significant progress made in organic second- and third-order NLO materials. For second-order NLO materials, the recent advances in the efficient and cost-effective synthesis of dipolar polyene chromophores and thin-film engineering for efficient electric field poling are summarized. The applications and prospects of these high-performance EO materials are also discussed. For third-order NLO materials, we discuss the molecular design strategies of cyanine dyes for AOSP applications, particularly focusing on anionic tricyanofuran (TCF)-based cyanines. We aim to provide a better understanding of the structure–property relationships for cyanine-based AOSP materials. Finally, a summary and outlook for advancing high-performance organic NLO materials are provided.





Journal ArticleDOI
TL;DR: In this paper, a simple strategy by applying phenethylammonium halides to reduce the energy loss and suppress the phase segregation of wide-bandgap perovskite solar cells is developed.



Journal ArticleDOI
TL;DR: PPE2 is found to improve the quality of perovskite films cast on top with larger grain sizes and more oriented crystallization, and rational understanding of the reasons why two isomeric polymer HTMs with almost identical photophysical properties, hole‐transporting ability, and surface wettability deliver so distinctly different device performance under similar device fabrication conditions is manifested.
Abstract: Currently, there are only very few dopant-free polymer hole-transporting materials (HTMs) that can enable perovskite solar cells (PVSCs) to demonstrate a high power conversion efficiency (PCE) of greater than 20%. To address this need, a simple and efficient way is developed to synthesize novel crossconjugated polymers as high performance dopant-free HTMs to endow PVSCs with a high PCE of 21.3%, which is among the highest values reported for single-junction inverted PVSCs. More importantly, rational understanding of the reasons why two isomeric polymer HTMs (PPE1 and PPE2) with almost identical photophysical properties, hole-transporting ability, and surface wettability deliver so distinctly different device performance under similar device fabrication conditions is manifested. PPE2 is found to improve the quality of perovskite films cast on top with larger grain sizes and more oriented crystallization. These results help unveil the new HTM design rules to influence the perovskite growth/crystallization for improving the performance of inverted PVSCs.

Journal ArticleDOI
TL;DR: In this article, the effect of a thin organic bulk-heterojunction interlayer on improving the photovoltaic performance of lead sulfide (PbS) colloidal quantum dot (CQD) solar cells was demonstrated.
Abstract: We have successfully demonstrated the effect of a thin organic bulk-heterojunction (BHJ) interlayer on improving the photovoltaic performance of lead sulfide (PbS) colloidal quantum dot (CQD) solar...



Journal ArticleDOI
12 May 2020-ACS Nano
TL;DR: This work presents a spectrally selective electrode (SSE) by imitating the integrating strategy of beetle cuticle for achieving narrow bandpass ST-OSCs with high efficiency and long-term stability, and indicates the application potential of SSEs in light-emitting diodes, lasers, and photodetectors.
Abstract: The visual aesthetic that involves color, brightness, and glossiness is of great importance for building integrated photovoltaics. Semitransparent organic solar cells (ST-OSCs) are thus considered as the most promising candidate due to their superiority in transparency and efficiency. However, the realization of high color purity with narrow bandpass transmitted light usually causes the severely suppressed transparency in ST-OSCs. Herein, we present a spectrally selective electrode (SSE) by imitating the integrating strategy of beetle cuticle for achieving narrow bandpass ST-OSCs with high efficiency and long-term stability. The proposed SSE allows for efficient light-selective passage, leading to tunable narrow bandpass transmitted light from violet to red. An optimized power conversion efficiency of 15.07% is achieved for colorful ST-OSCs, which exhibit color purity close to 100% and a peak transmittance approaching 30%. Long-term stability is also improved for ST-OSCs made with this SSE due to the light-rejecting and the moisture-blocking abilities. The realization of bright and colorful ST-OSCs also indicates the application potential of SSEs in light-emitting diodes, lasers, and photodetectors.


Journal ArticleDOI
27 Apr 2020
TL;DR: In this article, the authors present a platform for electro-optic photon conversion based on silicon-organic hybrid photonics, which combines high quality factor microwave and optical resonators with an electrooptic polymer cladding to perform microwave-to-optical photon conversion from 6.7 GHz to 193 THz.
Abstract: Low-loss fiber optic links have the potential to connect superconducting quantum processors together over long distances to form large scale quantum networks. A key component of these future networks is a quantum transducer that coherently and bidirectionally converts photons from microwave frequencies to optical frequencies. We present a platform for electro-optic photon conversion based on silicon-organic hybrid photonics. Our device combines high quality factor microwave and optical resonators with an electro-optic polymer cladding to perform microwave-to-optical photon conversion from 6.7 GHz to 193 THz (1558 nm). The device achieves an electro-optic coupling rate of 590 Hz in a millikelvin dilution refrigerator environment. We use an optical heterodyne measurement technique to demonstrate the single-sideband nature of the conversion with a selectivity of approximately 10 dB. We analyze the effects of stray light in our device and suggest ways in which this can be mitigated. Finally, we present initial results on high-impedance spiral resonators designed to increase the electro-optic coupling.

Journal ArticleDOI
TL;DR: In this article, three new small molecules based on the benzo [1,2-b:4,5-b]dithiophene (BDT) fused central core with different side-chains were designed and synthesized to investigate the side-chain effect on the properties of nonfullerene acceptors.

Journal ArticleDOI
TL;DR: Comprehensive spectroscopic as well as computational approaches were executed, providing a correlation for the emission efficiencies versus energy gaps between the metal-to-ligand charge transfer (MLCT)/ππ* emitting excited state and upper lying metal-centered dd quenching state.
Abstract: A series of charge-neutral bis-tridentate Ir(III) complexes (1, 3, and 4) were prepared via employing three distinctive tridentate prochelates, that is, (pzptBphFO)H2, [(phpyim)H2·(PF6)], and [(pim...

Journal ArticleDOI
TL;DR: In this article, the dipole moment of the terminals has been revealed as an important factor and its working mechanism has been thoroughly investigated by systematically studying six ternary OSCs.
Abstract: Fused-ring electron acceptor (FREA) based ternary organic solar cells (OSCs) have made significant progress and attracted considerable attention due to their simple device architecture and broad absorption range in devices. There are three key parameters that need to be fine-tuned in ternary OSCs including absorption, energy level and morphology in order to realize high efficiencies. Herein, a series of FREAs with diverse electron-rich cores or electron-deficient terminals are developed and rationally combined to achieve high performance ternary OSCs. The dipole moment of FREAs’ terminals has been unveiled as an important factor and its working mechanism has been thoroughly investigated by systematically studying six ternary OSCs. These ternary blends all exhibit complementary absorption and cascade energy levels, which can facilitate efficient light-harvesting and charge transfer. Additionally, the morphological effects on ternary OSCs are eliminated through comparative studies while demonstrating distinctively different performance. The preliminary results show that compatible dipole moment between two FREAs is critical in ternary blends. Specifically, the performance of the ternary system with two FREAs having quite different dipole moment terminals is worse compared to that with similar terminal dipole moments. The pair with larger difference in the dipole moment will also negatively impact device performance. This interesting phenomenon is likely due to the fact that very different dipole moments of terminals in FREAs can significantly decrease the electron mobility as well as induce unbalanced hole/electron transport. Consequently, it results in increased charge recombination and reduced charge collection efficiency. This finding demonstrates that the dipole moment of FREAs should be taken into account in designing ternary OSCs.

Journal ArticleDOI
TL;DR: In this paper, a single-crystal X-ray diffraction study was conducted on complex Cz6 in an attempt to provide an unambiguous structural proof, which confirmed the dominance of azole-pyridine-carbazole cyclometalate in controlling the emission energy gap, while the carbene pincer was less influential on the detected emission peak wavelength.
Abstract: Both monoanionic dicarbene pincer chelate and dianionic azole-pyridine-carbazole cyclometalate were successfully employed in the preparation of respective bis-tridentate Ir(III) metal complexes (Cz6–9) in moderate yields. Tuning of emission to blue was achieved by the addition of dual methoxy substituents at the carbazole cyclometalate, as well as the introduction of either methoxy or dimethylamino group at the central pyridinyl fragment of the azole-pyridine-carbazole cyclometalate. Single-crystal X-ray diffraction study was conducted on complex Cz6 in an attempt to provide an unambiguous structural proof. Photophysical properties were next measured in degassed CH2Cl2 solution at RT, giving structureless emission with peak maximum spanning 460–508 nm and photoluminescence quantum yield of 22–87%. A TD-DFT calculation confirmed the dominance of azole-pyridine-carbazole cyclometalate in controlling the emission energy gap, while the carbene pincer was less influential on the detected emission peak wavelength, i.e. acted as an ancillary. Importantly, the experimentally detected radiative lifetime (e.g. 2.78–17.18 μs) showed a clear correlation to the calculated metal-to-ligand charge transfer percentage of the electronic transitions (10.8–7.5%). Organic light-emitting diode devices gave turn-on voltages of 4.3 and 4.3 V, maximum EQE = 16.3 and 12.2%, power efficiencies of 17.6 and 10.4 lm W−1 and with CIEx,y coordinates of (0.16, 0.26) and (0.16, 0.20) for Cz6 and 7 at 15 wt%, confirming their potential as blue dopants for phosphorescent organic light-emitting diodes.

Journal ArticleDOI
TL;DR: An efficient post-functionalization protocol of the Mitsunobu reaction between a commercial reactive polymer of poly(4-vinylphenol) and 9-(2-hydroxylethyl)-N,N, N,N-tetrakis(4methoxyphenyl)-9H-carbazole-2,7-diamine is reported to synthesize a novel side-chain polymer (PVP-CZ) with a high density of hole transporting moieties.