Anomalous Correlation between Thermal Conductivity and Elastic Modulus in Two-Dimensional Hybrid Metal Halide Perovskites.

Device-level implementation of soft materials for energy conversion and thermal management demands a comprehensive understanding of their thermal conductivity and elastic modulus to mitigate thermo-mechanical challenges and ensure long-term stability. Thermal conductivity and elastic modulus are usually positively correlated in soft materials, such as amorphous macromolecules, which poses a challenge to discover materials that are either soft and thermally conductive or hard and thermally insulative. Here, we show anomalous correlations of thermal conductivity and elastic modulus in two-dimensional (2D) hybrid organic-inorganic perovskites (HOIP) by engineering the molecular interactions between organic cations. By replacing conventional alkyl-alkyl and aryl-aryl type organic interactions with mixed alkyl-aryl interactions, we observe an enhancement in elastic modulus with a reduction in thermal conductivity. This anomalous dependence provides a route to engineer thermal conductivity and elastic modulus independently and a guideline to search for better thermal management materials. Further, introducing chirality into the organic cation induces a molecular packing that leads to the same thermal conductivity and elastic modulus regardless of the composition across all half-chiral 2D HOIPs. This finding provides substantial leeway for further investigations in chiral 2D HOIPs to tune optoelectronic properties without compromising thermal and mechanical stability.

Optimized Incorporation of Furan into Diketopyrrolopyrrole-Based Conjugated Polymers for Organic Field-Effect Transistors.

Flexible electronics have received considerable attention in the past decades due to their promising application in rollable display screens, wearable devices, implantable devices, and other electronic applications. In particular, conjugated polymers are favored for flexible electronics due to their mechanical flexibility and potential for solution-processed fabrication techniques, such as blade-coating, roll-to-roll printing, and high-throughput printing allowing for high-performance transistor devices. Thiophene is the prevailing conjugated unit to construct these conjugated polymers due to its favorable electronic properties. On the other hand, furans are among the few conjugated moieties that are easily derived from bio renewable resources. To promote sustainability, we selectively introduced furan into the conjugated backbone of a high-mobility polymer scaffold and systematically studied the effect on the microstructure and charge transport. We show that partially and selectively replacing thiophene units with furan can yield nearly comparable performance compared to the all-thiophene polymer. This strategy offers an improvement in the sustainability of the polymer by incorporating bio-sourced furan without sacrificing the high-performance characteristics. Meanwhile, polymers with incorrect or complete furan incorporation show reduced mobilities. This work serves to develop coherent structure-morphology-performance relationships; such knowledge will establish guidelines for the future development of sustainable, furan-based conjugated materials.

The role of interfacial donor-acceptor percolation in efficient and stable all-polymer solar cells.

Polymerization of Y6-type acceptor molecules leads to bulk-heterojunction organic solar cells with both high power-conversion efficiency and device stability, but the underlying mechanism remains unclear. Here we show that the exciton recombination dynamics of polymerized Y6-type acceptors (Y6-PAs) strongly depends on the degree of aggregation. While the fast exciton recombination rate in aggregated Y6-PA competes with electron-hole separation at the donor-acceptor (D-A) interface, the much-suppressed exciton recombination rate in dispersed Y6-PA is sufficient to allow efficient free charge generation. Indeed, our experimental results and theoretical simulations reveal that Y6-PAs have larger miscibility with the donor polymer than Y6-type small molecular acceptors, leading to D-A percolation that effectively prevents the formation of Y6-PA aggregates at the interface. Besides enabling high charge generation efficiency, the interfacial D-A percolation also improves the thermodynamic stability of the blend morphology, as evident by the reduced device "burn-in" loss upon solar illumination.

Precise synthesis and photovoltaic properties of giant molecule acceptors.

Series of giant molecule acceptors DY, TY and QY with two, three and four small molecule acceptor subunits are synthesized by a stepwise synthetic method and used for systematically investigating the influence of subunit numbers on the structure-property relationship from small molecule acceptor YDT to giant molecule acceptors and to polymerized small molecule acceptor PY-IT. Among these acceptors-based devices, the TY-based film shows proper donor/acceptor phase separation, higher charge transfer state yield and longer charge transfer state lifetime. Combining with the highest electron mobility, more efficient exciton dissociation and lower charge carrier recombination properties, the TY-based device exhibits the highest power conversion efficiency of 16.32%. These results indicate that the subunit number in these acceptors has significant influence on their photovoltaic properties. This stepwise synthetic method of giant molecule acceptors will be beneficial to diversify their structures and promote their applications in high-efficiency and stable organic solar cells.

Auxiliary sequential deposition enables 19%-efficiency organic solar cells processed from halogen-free solvents.

High-efficiency organic solar cells are often achieved using toxic halogenated solvents and additives that are constrained in organic solar cells industry. Therefore, it is important to develop materials or processing methods that enabled highly efficient organic solar cells processed by halogen free solvents. In this paper, we report an innovative processing method named auxiliary sequential deposition that enables 19%-efficiency organic solar cells processed by halogen free solvents. Our auxiliary sequential deposition method is different from the conventional blend casting or sequential deposition methods in that it involves an additional casting of dithieno[3,2-b:2',3'-d]thiophene between the sequential depositions of the donor (D18-Cl) and acceptor (L8-BO) layers. The auxiliary sequential deposition method enables dramatic performance enhancement from 15% to over 18% compared to the blend casting and sequential deposition methods. Furthermore, by incorporating a branched-chain-engineered acceptor called L8-BO-X, device performance can be boosted to over 19% due to increased intermolecular packing, representing top-tier values for green-solvent processed organic solar cells. Comprehensive morphological and time-resolved characterizations reveal that the superior blend morphology achieved through the auxiliary sequential deposition method promotes charge generation while simultaneously suppressing charge recombination. This research underscores the potential of the auxiliary sequential deposition method for fabricating highly efficient organic solar cells using environmentally friendly solvents.

Additive-free molecular acceptor organic solar cells processed from a biorenewable solvent approaching 15% efficiency.

We report on the use of molecular acceptors (MAs) and donor polymers processed with a biomass-derived solvent (2-methyltetrahydrofuran, 2-MeTHF) to facilitate bulk heterojunction (BHJ) organic photovoltaics (OPVs) with power conversion efficiency (PCE) approaching 15%. Our approach makes use of two newly designed donor polymers with an opened ring unit in their structures along with three molecular acceptors (MAs) where the backbone and sidechain were engineered to enhance the processability of BHJ OPVs using 2-MeTHF, as evaluated by an analysis of donor-acceptor (D-A) miscibility and interaction parameters. To understand the differences in the PCE values that ranged from 9-15% as a function of composition, the surface, bulk, and interfacial BHJ morphologies were characterized at different length scales using atomic force microscopy, grazing-incidence wide-angle X-ray scattering, resonant soft X-ray scattering, X-ray photoelectron spectroscopy, and 2D solid-state nuclear magnetic resonance spectroscopy. Our results indicate that the favorable D-A intermixing that occurs in the best performing BHJ film with an average domain size of ∼25 nm, high domain purity, uniform distribution and enhanced local packing interactions - facilitates charge generation and extraction while limiting the trap-assisted recombination process in the device, leading to high effective mobility and good performance.

Study of Glass Formation and Crystallization Kinetics in a 2D Metal Halide Perovskite Using Ultrafast Calorimetry.

While crystalline 2D metal halide perovskites (MHPs) represent a well-celebrated semiconductor class, supporting applications in the fields of photovoltaics, emitters, and sensors, the recent discovery of glass formation in an MHP opens many new opportunities associated with reversible glass-crystalline switching, with each state offering distinct optoelectronic properties. However, the previously reported [S-(-)-1-(1-naphthyl)ethylammonium]2PbBr4 perovskite is a strong glass former with sluggish glass-crystal transformation time scales, pointing to a need for glassy MHPs with a broader range of compositions and crystallization kinetics. Herein we report glass formation for low-melting-temperature 1-MeHa2PbI4 (1-MeHa = 1-methyl-hexylammonium) using ultrafast calorimetry, thereby extending the range of MHP glass formation across a broader range of organic (fused ring to branched aliphatic) and halide (bromide to iodide) compositions. The importance of a slight loss of organic and hydrogen iodide components from the MHP in stabilizing the glassy state is elucidated. Furthermore, the underlying kinetics of glass-crystal transformation, including activation energies, crystal growth rate, Angell plot, and fragility index, is studied using a combination of kinetic, thermodynamic, and rheological modeling techniques. An inferred fast crystal growth rate of 0.21 m/s for 1-MeHa2PbI4 shows promise toward suitability in extended application spaces, for example, in metamaterials, nonvolatile memory, and optical and neuromorphic computing devices.

Introducing a Phenyl End Group in the Inner Side Chains of A-DA'D-A Acceptors Enables High-Efficiency Organic Solar Cells Processed with Nonhalogenated Solvent.

Power conversion efficiency (PCE) of organic solar cells (OSCs) processed by nonhalogenated solvents is unsatisfactory due to the unfavorable morphology. Herein, two new small molecule acceptors (SMAs) Y6-Ph and L8-Ph are synthesized by introducing a phenyl end group in the inner side chains of the SMAs of Y6 and L8-BO, respectively, for overcoming the excessive aggregation of SMAs in the long-time film forming processed by nonhalogenated solvents. First, the effect of the film forming time on the aggregation property and photovoltaic performance of Y6, L8-BO, Y6-Ph, and L8-Ph is studied by using the commonly used solvents: chloroform (CF) (rapid film forming process) and chlorobenzene (CB) (slow film forming process). It is found that Y6- and L8-BO-based OSCs exhibit a dramatic drop in PCE from CF- to CB-processed devices owing to the large phase separation, while the Y6-Ph and L8-Ph based OSCs show obviously increased PCEs Furthermore, L8-Ph-based OSCs processed by nonhalogenated solvent o-xylene (o-XY) achieved a high PCE of 18.40% with an FF of 80.11%. The results indicate that introducing a phenyl end group in the inner side chains is an effective strategy to modulate the morphology and improve the photovoltaic performance of the OSCs processed by nonhalogenated solvents.

Unveiling re-entrant phase behavior and crystalline-amorphous interactions in semi-conducting polymer:small molecule blends.

It has been reported recently that conjugated polymer:small molecule systems might exhibit complex, re-entrant phase behavior with hourglass or closed-loop miscibility gaps due to an 'apparent' lower critical solution temperature branch. However, the study did not firmly establish if the observations were reflecting equilibrium or not. To assure that the observed shapes of the binodals via a mixing experiment represent local near-equilibrium conditions that capture complex molecular interactions or equation-of-state effects, we present here the liquidus and the binodal for the exact same systems, i.e., PTB7-Th:PC61BM, PffBT4T-C9C13:PC71BM and PTB7-Th:EH-IDTBR, with the liquidus measured via a demixing experiment with long annealing time of days to weeks. We observe that the binodal displayed consistent trends with the liquidus, revealing an underlying thermodynamic and not microstructural or kinetic cause behind the complex phase behavior. Our results highlight the need for a novel, sufficiently complex physical model for understanding these non-trivial phase diagrams of semi-conducting materials. We also discover that the composition difference (Δϕ) between liquidus and binodal reflects the crystalline-amorphous interaction, exhibiting a linear relationship with the binodal composition (ϕb,polymer), i.e., Δϕ increases as χaa decreases. This possibly provides a new approach for obtaining the crystalline-amorphous interaction parameter χca(T) beyond the commonly used melting point depression method, which estimates χca near the melting temperature Tm of the crystalline component. The capability of obtaining χca(T) over a more extended temperature range may encourage more extensive studies and facilitate the understanding of χca in general, but particularly for all the novel non-fullerene acceptors that are able to crystallize.

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.

Emergent molecular traits of lettuce and tomato grown under wavelength-selective solar cells.

The integration of semi-transparent organic solar cells (ST-OSCs) in greenhouses offers new agrivoltaic opportunities to meet the growing demands for sustainable food production. The tailored absorption/transmission spectra of ST-OSCs impacts the power generated as well as crop growth, development and responses to the biotic and abiotic environments. To characterize crop responses to ST-OSCs, we grew lettuce and tomato, traditional greenhouse crops, under three ST-OSC filters that create different light spectra. Lettuce yield and early tomato development are not negatively affected by the modified light environment. Our genomic analysis reveals that lettuce production exhibits beneficial traits involving nutrient content and nitrogen utilization while select ST-OSCs impact regulation of flowering initiation in tomato. These results suggest that ST-OSCs integrated into greenhouses are not only a promising technology for energy-neutral, sustainable and climate-change protected crop production, but can deliver benefits beyond energy considerations.

Control of Host-Matrix Morphology Enables Efficient Deep-Blue Organic Light-Emitting Devices.

Mixing a sterically bulky, electron-transporting host material into a conventional single host-guest emissive layer is demonstrated to suppress phase separation of the host matrix while increasing the efficiency and operational lifetime of deep-blue phosphorescent organic light-emitting diodes (PHOLEDs) with chromaticity coordinates of (0.14, 0.15). The bulky host enables homogenous mixing of the molecules comprising the emissive layer while suppressing single host aggregation; a significant loss channel of nonradiative recombination. By controlling the amorphous phase of the host-matrix morphology, the mixed-host device achieves a significant reduction in nonradiative exciton decay, resulting in 120 ± 6% increase in external quantum efficiency relative to an analogous, single-host device. In contrast to single host PHOLEDs where electrons are transported by the host and holes by the dopants, both charge carriers are conducted by the mixed host, reducing the probability of exciton annihilation, thereby doubling of the deep-blue PHOLED operational lifetime. These findings demonstrate that the host matrix morphology affects almost every aspect of PHOLED performance.

Relating reorganization energies, exciton diffusion length and non-radiative recombination to the room temperature UV-vis absorption spectra of NF-SMA.

Understanding excited-state reorganization energies, exciton diffusion lengths and non-radiative (NR) recombination, and the overall optoelectronic responses of nonfullerene small molecule acceptors (NF-SMAs) is important in order to rationally design new materials with controlled properties. While the effects of structural modifications on the optical gaps and electron affinities of NF-SMAs have been studied extensively, analyses of their absorption spectra that carefully characterize electronic and vibrational contributions that allow comparisons of reorganization energies and their implications for exciton diffusion lengths and NR recombination have yet to be reported. Here, we study the room temperature absorption spectra of three structural classes of NF-SMAs in dilute solutions through multiparameter Franck Condon (MFC) analyses and density functional theory (DFT) calculations. We show that the absorption spectra of these NF-SMAs can be categorized based on molecular structure-spectra correlation. The absorption spectra of curved, Y6-like structures can be described using an MFC model with two electronic transitions and two effective vibrational modes. The results of MFC/DFT analyses reveal that Y6 exhibits the smallest intra-molecular reorganization energy among the materials studied. Linear ITIC-like molecular structures reveal larger reorganization energies and reduced conformational uniformity compared to Y6. Meanwhile structures such as IDTBR and IEICO, which have an extra π-conjugated moiety between the donor and acceptor moieties, have large excited-state reorganization energies and low degrees of conformational uniformity. Since the intra-molecular reorganization energy is correlated with exciton diffusion length and nonradiative voltage losses (ΔVnr), our results highlight the power of RT absorption spectroscopy and DFT calculations as simple tools to designing improved OSCs materials with small reorganization energies, small ΔVnr, large exciton diffusion length and low energetic disorder (due to a strongly dominant conformation).

Small-Molecule Acceptor with Unsymmetric Substituents and Fused Rings for High-Performance Organic Solar Cells with Enhanced Mobility and Reduced Energy Losses.

A new unsymmetric small-molecule acceptor (SMA) BTPOSe-4F was designed by unsymmetric structure modification to Y6 with an alkyl upper side chain replaced by an alkoxy side chain and a sulfur atom in its central fused ring replaced by a selenium atom, for the application as an acceptor to fabricate organic solar cells (OSCs). BTPOSe-4F exhibits a higher lowest unoccupied molecular orbital (LUMO) energy level, a reduced nonradiation energy loss, and better charge extraction properties in its binary OSCs with a higher Voc of 0.886. Furthermore, the ternary OSCs with the addition of PC71BM demonstrated a higher power conversion efficiency (PCE) of 17.33% with Voc of 0.890 V. This work reveals that the unsymmetric modification strategy can further give impetus to the photovoltaic performance promotion of OSCs for Y6-series SMAs.

Importance of Electric-Field-Independent Mobilities in Thick-Film Organic Solar Cells.

In organic solar cells (OSCs), a thick active layer usually yields a higher photocurrent with broader optical absorption than a thin active layer. In fact, a ∼300 nm thick active layer is more compatible with large-area processing methods and theoretically should be a better spot for efficiency optimization. However, the bottleneck of developing high-efficiency thick-film OSCs is the loss in fill factor (FF). The origin of the FF loss is not clearly understood, and there a direct method to identify photoactive materials for high-efficiency thick-film OSCs is lacking. Here, we demonstrate that the mobility field-dependent coefficient is an important parameter directly determining the FF loss in thick-film OSCs. Simulation results based on the drift-diffusion model reveal that a mobility field-dependent coefficient smaller than 10-3 (V/cm)-1/2 is required to maintain a good FF in thick-film devices. To confirm our simulation results, we studied the performance of two ternary bulk heterojunction (BHJ) blends, PTQ10:N3:PC71BM and PM6:N3:PC71BM. We found that the PTQ10 blend film has weaker field-dependent mobilities, giving rise to a more balanced electron-hole transport at low fields. While both the PM6 blend and PTQ10 blend yield good performance in thin-film devices (∼100 nm), only the PTQ10 blend can retain a FF = 74% with an active layer thickness of up to 300 nm. Combining the benefits of a higher JSC in thick-film devices, we achieved a PCE of 16.8% in a 300 nm thick PTQ10:N3:PC71BM OSC. Such a high FF in the thick-film PTQ10 blend is also consistent with the observation of lower charge recombination from light-intensity-dependent measurements and lower energetic disorder observed in photothermal deflection spectroscopy.

A Top-Down Strategy to Engineer ActiveLayer Morphology for Highly Efficient and Stable All-Polymer Solar Cells.

A major challenge hindering the further development of all-polymer solar cells (all-PSCs) employing polymerized small-molecule acceptors is the relatively low fill factor (FF) due to the difficulty in controlling the active-layer morphology. The issues typically arise from oversized phase separation resulting from the thermodynamically unfavorable mixing between two macromolecular species, and disordered molecular orientation/packing of highly anisotropic polymer chains. Herein, a facile top-down controlling strategy to engineer the morphology of all-polymer blends is developed by leveraging the layer-by-layer (LBL) deposition. Optimal intermixing of polymer components can be achieved in the two-step process by tuning the bottom-layer polymer swelling during top-layer deposition. Consequently, both the molecular orientation/packing of the bottom layer and the molecular ordering of the top layer can be optimized with a suitable top-layer processing solvent. A favorable morphology with gradient vertical composition distribution for efficient charge transport and extraction is therefore realized, affording a high all-PSC efficiency of 17.0% with a FF of 76.1%. The derived devices also possess excellent long-term thermal stability and can retain >90% of their initial efficiencies after being annealed at 65 °C for 1300 h. These results validate the distinct advantages of employing an LBL processing protocol to fabricate high-performance all-PSCs.

Achieving 19% Power Conversion Efficiency in Planar-Mixed Heterojunction Organic Solar Cells Using a Pseudosymmetric Electron Acceptor.

A record power conversion efficiency (PCE) of over 19% is realized in planar-mixed heterojunction (PMHJ) organic solar cells (OSCs) by adopting the asymmetric selenium substitution strategy in making a pseudosymmetric electron acceptor, BS3TSe-4F. The combined molecular asymmetry with more polarizable selenium substitution increases the dielectric constant of the D18/BS3TSe-4F blend, helping lower the exciton binding energy. On the other hand, dimer packing in BS3TSe-4F is facilitated to enable free charge generation, helping more efficient exciton dissociation and lowering the radiative recombination loss (ΔE2 ) of OSCs. As a result, PMHJ OSCs based on D18/BS3TSe-4F achieve a PCE of 18.48%. By incorporating another mid-bandgap acceptor Y6-O into D18/BS3TSe-4F to form a ternary PMHJ, a higher open-circuit voltage (VOC ) can be achieved to realize an impressive PCE of 19.03%. The findings of using pseudosymmetric electron acceptors in enhancing device efficiency provides an effective way to develop highly efficient acceptor materials for OSCs.

16.52% Efficiency All-Polymer Solar Cells with High Tolerance of the Photoactive Layer Thickness.

All-polymer solar cells (all-PSCs) have drawn growing attention and achieved tremendous progress recently, but their power conversion efficiency (PCE) still lags behind small-molecule-acceptor (SMA)-based PSCs due to the relative difficulty on morphology control of polymer photoactive blends. Here, low-cost PTQ10 is introduced as a second polymer donor (a third component) into the PM6:PY-IT blend to finely tune the energy-level matching and microscopic morphology of the polymer blend photoactive layer. The addition of PTQ10 decreases the π-π stacking distance, and increases the π-π stacking coherence length and the ordered face-on molecular packing orientation, which improves the charge separation and transport in the photoactive layer. Moreover, the deeper highest occupied molecular orbital energy level of the PTQ10 polymer donor than PM6 leads to higher open-circuit voltage of the ternary all-PSCs. As a result, a PCE of 16.52% is achieved for ternary all-PSCs, which is one of the highest PCEs for all-PSCs. In addition, the ternary devices exhibit a high tolerance of the photoactive layer thickness with high PCEs of 15.27% and 13.91% at photoactive layer thickness of ≈205 and ≈306 nm, respectively, which are the highest PCEs so far for all-PSCs with a thick photoactive layer.

Semi-paracrystallinity in semi-conducting polymers.

Precise determination of structural organization of semi-conducting polymers is of paramount importance for the further development of these materials in organic electronic technologies. Yet, prior characterization of some of the best-performing materials for transistor and photovoltaic applications, which are based on polymers with rigid backbones, often resulted in conundrums in which X-ray scattering and microscopy yielded seemingly contradicting results. Here we solve the paradox by introducing a new structural model, i.e., semi-paracrystalline organization. The model establishes that the microstructure of these materials relies on a dense array of small paracrystalline domains embedded in a more disordered matrix. Thus, the overall structural order relies on two parameters: the novel concept of degree of paracrystallinity (i.e., paracrystalline volume/mass fraction, introduced here for the first time) and the lattice distortion parameter of paracrystalline domains (g-parameter from X-ray scattering). Structural parameters of the model are correlated with long-range charge carrier transport, revealing that charge transport in semi-paracrystalline materials is particularly sensitive to the interconnection of paracrystalline domains.

High Miscibility Compatible with Ordered Molecular Packing Enables an Excellent Efficiency of 16.2% in All-Small-Molecule Organic Solar Cells.

In all-small-molecule organic solar cells (ASM-OSCs), a high short-circuit current (Jsc ) usually needs a small phase separation, while a high fill factor (FF) is generally realized in a highly ordered packing system. However, small domain and ordered packing always conflicted each other in ASM-OSCs, leading to a mutually restricted Jsc and FF. In this study, alleviation of the previous dilemma by the strategy of obtaining simultaneous good miscibility and ordered packing through modulating homo- and heteromolecular interactions is proposed. By moving the alkyl-thiolation side chains from the para- to the meta-position in the small-molecule donor, the surface tension and molecular planarity are synchronously enhanced, resulting in compatible properties of good miscibility with acceptor BTP-eC9 and strong self-assembly ability. As a result, an optimized morphology with multi-length-scale domains and highly ordered packing is realized. The device exhibits a long carrier lifetime (39.8 µs) and fast charge collection (15.5 ns). A record efficiency of 16.2% with a high FF of 75.6% and a Jsc of 25.4 mA cm-2 in the ASM-OSCs is obtained. These results demonstrate that the strategy of simultaneously obtaining good miscibility with high crystallinity could be an efficient photovoltaic material design principle for high-performance ASM-OSCs.