Charge Transfer from Quantum-Confined 0D, 1D, and 2D Nanocrystals
Not Available
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Engineering topics
Zhu, Haiming
Publications and source records attributed to Zhu, Haiming.
On the role of asymmetric molecular geometry in high-performance organic solar cells
Although asymmetric molecular design has been widely demonstrated effective for organic photovoltaics (OPVs), the correlation between asymmetric molecular geometry and their optoelectronic properties is still unclear. To access this issue, we have designed and synthesized several symmetric-asymmetric non-fullerene acceptors (NFAs) pairs with identical physical and optoelectronic properties. Interestingly, we found that the asymmetric NFAs universally exhibited increased open-circuit voltage compared to their symmetric counterparts, due to the reduced non-radiative charge recombination. From our molecular-dynamic simulations, the asymmetric NFA naturally exhibits more diverse molecular interaction patterns at the donor (D):acceptor (A) interface as compared to the symmetric ones, as well as higher D:A interfacial charge-transfer state energy. Moreover, it is observed that the asymmetric structure can effectively suppress triplet state formation. These advantages enable a best efficiency of 18.80%, which is one of the champion results among binary OPVs. Therefore, this work unambiguously demonstrates the unique advantage of asymmetric molecular geometry, unveils the underlying mechanism, and highlights the manipulation of D:A interface as an important consideration for future molecular design.
14 SOLAR ENERGY↗
All-polymer organic solar cells with nano-to-micron hierarchical morphology and large light receiving angle
Distributed photovoltaics in living environment harvest the sunlight in different incident angles throughout the day. The development of planer solar cells with large light-receiving angle can reduce the requirements in installation form factor and is therefore urgently required. Here, thin film organic photovoltaics with nano-sized phase separation integrated in micro-sized surface topology is demonstrated as an ideal solution to proposed applications. All-polymer solar cells, by means of a newly developed sequential processing, show large magnitude hierarchical morphology with facilitated exciton-to-carrier conversion. The nano fibrilar donor-acceptor network and micron-scale optical field trapping structure in combination contributes to an efficiency of 19.06% (certified 18.59%), which is the highest value to date for all-polymer solar cells. Furthermore, the micron-sized surface topology also contributes to a large light-receiving angle. A 30% improvement of power gain is achieved for the hierarchical morphology comparing to the flat-morphology devices. These inspiring results show that all-polymer solar cell with hierarchical features are particularly suitable for the commercial applications of distributed photovoltaics due to its low installation requirement.
14 SOLAR ENERGY↗
Near-infrared absorbing acceptor with suppressed triplet exciton generation enabling high performance tandem organic solar cells
Reducing the energy loss of sub-cells is critical for high performance tandem organic solar cells, while it is limited by the severe non-radiative voltage loss via the formation of non-emissive triplet excitons. Herein, we develop an ultra-narrow bandgap acceptor BTPSeV-4F through replacement of terminal thiophene by selenophene in the central fused ring of BTPSV-4F, for constructing efficient tandem organic solar cells. The selenophene substitution further decrease the optical bandgap of BTPSV-4F to 1.17 eV and suppress the formation of triplet exciton in the BTPSV-4F-based devices. The organic solar cells with BTPSeV-4F as acceptor demonstrate a higher power conversion efficiency of 14.2% with a record high short-circuit current density of 30.1 mA cm –2 and low energy loss of 0.55 eV benefitted from the low non-radiative energy loss due to the suppression of triplet exciton formation. We also develop a high-performance medium bandgap acceptor O1-Br for front cells. By integrating the PM6:O1-Br based front cells with the PTB7-Th:BTPSeV-4F based rear cells, the tandem organic solar cell demonstrates a power conversion efficiency of 19%. The results indicate that the suppression of triplet excitons formation in the near-infrared-absorbing acceptor by molecular design is an effective way to improve the photovoltaic performance of the tandem organic solar cells.
14 SOLAR ENERGY↗
Reconfiguring band-edge states and charge distribution of organic semiconductor–incorporated 2D perovskites via pressure gating
Two-dimensional (2D) semiconductor heterostructures are key building blocks for many electronic and optoelectronic devices. Reconfiguring the band-edge states and modulating their interplay with charge carriers at the interface in a continuous manner have long been sought yet are challenging. Here, using organic semiconductor–incorporated 2D halide perovskites as the model system, we realize the manipulation of band-edge states and charge distribution via mechanical—rather than chemical or thermal—regulation. Compression induces band-alignment switching and charge redistribution due to the different pressure responses of organic and inorganic building blocks, giving controllable emission properties of 2D perovskites. We propose and demonstrate a “pressure gating” strategy that enables the control of multiple emission states within a single material. We also reveal that band-alignment transition at the organic-inorganic interface is intrinsically not well resolved at room temperature owing to the thermally activated transfer and shuffling of band-edge carriers. This work provides important fundamental insights into the energetics and carrier dynamics of hybrid semiconductor heterostructures.
42 ENGINEERING↗
Design Rules of the Mixing Phase and Impacts on Device Performance in High-Efficiency Organic Photovoltaics
In nonfullerene acceptor- (NFA-) based solar cells, the exciton splitting takes place at both domain interface and donor/acceptor mixture, which brings in the state of mixing phase into focus. The energetics and morphology are key parameters dictating the charge generation, diffusion, and recombination. It is revealed that tailoringthe electronic properties of the mixing region by doping with larger-bandgap components could reduce the density of state but elevate the filling state level, leading to improved open-circuit voltage ( V OC ) and reduced recombination. The monomolecular and bimolecular recombinations are shown to be intercorrelated, which show a Gaussian-like relationship with V OC and linear relationship with short-circuit current density ( J SC ) and fill factor (FF). The kinetics of hole transfer and exciton diffusion scale with J SC similarly, indicating the carrier generation in mixing region and crystalline domain are equally important. From the morphology perspective, the crystalline order could contribute to V OC improvement, and the fibrillar structure strongly affects the FF. These observations highlight the importance of the mixing region and its connection with crystalline domains and point out the design rules to optimize the mixing phase structure, which is an effective approach to further improve device performance.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Spontaneous carrier generation and low recombination in high-efficiency non-fullerene solar cells
The current research reveals the unique photo physical properties and carrier generation mechanisms of high efficiency non-fullerene acceptor-based organic photovoltaic blends. The analysis of device performance, morphology, and photo physics reveals that the interface carrier generation cannot support the device's current output. It is seen that primary photon excitons can dissociate into charge carriers in Y6, which displays a time scale of ∼0.3 ps with polaron yields above 28% in neat and blended thin films. This characteristic in combination with a large exciton diffusion length enables high morphology tolerance in Y6-overloaded blends. The carrier generation process is also combined with recombination studies. The recombination rate quantified by flux-dependent transient absorption measurements yields less than 5% total recombination and nearly 0% geminate recombination. Furthermore, these results define the advantages of the Y6 non-fullerene acceptor (NFA) and reveal the fundamental importance of developing new NFA materials with superior photo physical properties.
14 SOLAR ENERGY↗
Versatile Sequential Casting Processing for Highly Efficient and Stable Binary Organic Photovoltaics
Forming an ideal bulk heterojunction (BHJ) morphology is a critical issue governing the photon to electron process in organic solar cells (OSCs). Complementary to the widely-used blend casting (BC) method for BHJ construction, sequential casting (SC) can also enable similar or even better morphology and device performance for OSCs. Here, BC and SC methods on three representative donor:acceptor (D:A) blends are utilized, that is, PM6:PC 71 BM, PM6:IT-4F and PM6:L8-BO. Higher power conversion efficiencies (PCEs) in all cases by taking advantage of beneficial morphology from SC processing are achieved, and a champion PCE of 18.86% (certified as 18.44%) based on the PM6:L8-BO blend is reached, representing the record value among binary OSCs. The observations on phase separation and vertical distribution inspire the proposal of the swelling–intercalation phase-separation model to interpret the morphology evolution during SC processing. Further, the vertical phase segregation is found to deliver an improvement of device performance via affecting the charge transport and collection processes, as evidenced by the D:A-ratio-dependent photovoltaic properties. Besides, OSCs based on SC processing show advantages on device photostability and upscale fabrication. Finally, this work demonstrates the versatility and efficacy of the SC method for BHJ-based OSCs.
14 SOLAR ENERGY↗
Slot-Die-Coated Organic Solar Cells Optimized through Multistep Crystallization Kinetics
Not provided.
Energy & Fuels↗
Compromising Charge Generation and Recombination with Asymmetric Molecule for High-Performance Binary Organic Photovoltaics with Over 18% Certified Efficiency
Balancing the charge generation and recombination constitutes a major challenge to break the current limit of organic photovoltaics (OPVs). Here, to address this issue, an asymmetric non-fullerene acceptor, namely the AC9, is developed and high-performance OPV with a champion efficiency of 18.43% (18.1% certified) is demonstrated. This represents the record value among binary OPVs. Comprehensive analysis on exciton dissociation, charge collection, carrier transport, and recombination has been carried out, unveiling that the improved device performance of asymmetric AC9-based OPVs is originated from a better compromise between charge generation and non-radiative charge recombination, compared with the corresponding symmetric ones. This work provides a high-performing molecule and paves the way for high-performance OPVs through asymmetric molecular design.
36 MATERIALS SCIENCE↗
Correlating Electronic Structure and Device Physics with Mixing Region Morphology in High-Efficiency Organic Solar Cells
The donor/acceptor interaction in non-fullerene organic photovoltaics leads to the mixing domain that dictates the morphology and electronic structure of the blended thin film. Initiative effort is paid to understand how these domain properties affect the device performances on high-efficiency PM6:Y6 blends. Different fullerenes acceptors are used to manipulate the feature of mixing domain. It is seen that a tight packing in the mixing region is critical, which could effectively enhance the hole transfer and lead to the enlarged and narrow electron density of state (DOS). As a result, short-circuit current (J SC ) and fill factor (FF) are improved. The distribution of DOS and energy levels strongly influences open-circuit voltage (V OC ). The raised filling state of electron Fermi level is seen to be key in determining device V OC . Energy disorder is found to be a key factor to energy loss, which is highly correlated with the intermolecular distance in the mixing region. A 17.53% efficiency is obtained for optimized ternary devices, which is the highest value for similar systems. The current results indicate that a delicate optimization of the mixing domain property is an effective route to improve the V OC , J SC , and FF simultaneously, which provides new guidelines for morphology control toward high-performance organic solar cells.
36 MATERIALS SCIENCE↗
Mechanism study on organic ternary photovoltaics with 18.3% certified efficiency: from molecule to device
Our work presents a study on the working mechanism of ternary organic photovoltaic devices based on non-fullerene acceptors, focusing on the composition-dependent optoelectronic property variations in blend films and devices.
Chemistry↗