Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 93
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
Nat Commun ; 12(1): 1772, 2021 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-33741966

RESUMO

A critical bottleneck for improving the performance of organic solar cells (OSC) is minimising non-radiative losses in the interfacial charge-transfer (CT) state via the formation of hybrid energetic states. This requires small energetic offsets often detrimental for high external quantum efficiency (EQE). Here, we obtain OSC with both non-radiative voltage losses (0.24 V) and photocurrent losses (EQE > 80%) simultaneously minimised. The interfacial CT states separate into free carriers with ≈40-ps time constant. We combine device and spectroscopic data to model the thermodynamics of charge separation and extraction, revealing that the relatively high performance of the devices arises from an optimal adjustment of the CT state energy, which determines how the available overall driving force is efficiently used to maximize both exciton splitting and charge separation. The model proposed is universal for donor:acceptor (D:A) with low driving forces and predicts which D:A will benefit from a morphology optimization for highly efficient OSC.

2.
Nat Commun ; 12(1): 178, 2021 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-33420010

RESUMO

Tandem organic solar cells are based on the device structure monolithically connecting two solar cells to broaden overall absorption spectrum and utilize the photon energy more efficiently. Herein, we demonstrate a simple strategy of inserting a double bond between the central core and end groups of the small molecule acceptor Y6 to extend its conjugation length and absorption range. As a result, a new narrow bandgap acceptor BTPV-4F was synthesized with an optical bandgap of 1.21 eV. The single-junction devices based on BTPV-4F as acceptor achieved a power conversion efficiency of over 13.4% with a high short-circuit current density of 28.9 mA cm-2. With adopting BTPV-4F as the rear cell acceptor material, the resulting tandem devices reached a high power conversion efficiency of over 16.4% with good photostability. The results indicate that BTPV-4F is an efficient infrared-absorbing narrow bandgap acceptor and has great potential to be applied into tandem organic solar cells.

3.
Artigo em Inglês | MEDLINE | ID: mdl-33270428

RESUMO

We investigate the photovoltaic characteristics of organic solar cells (OSCs) for two distinctly different nanostructures, by comparing the charge carrier dynamics for bilayer- and bulk-heterojunction OSCs. Most interestingly, both architectures exhibit fairly similar power conversion efficiencies (PCEs), reflecting a comparable critical domain size for charge generation and charge recombination. Although this is, at first hand, surprising, a detailed analysis points out the similarity between these two concepts. A bulk-heterojunction architecture arranges the charge generating domains in a 3D ensemble across the whole bulk, while bilayer architectures arrange the specific domains on top of each other, rather than sharp bilayers. Specifically, for the polymer PBDB-T-2F, we find that the enhanced charge generation in a bulk composite is partially compensated by reduced recombination in the bilayer architecture, when nonfullerene acceptors (NFAs) are used instead of a fullerene acceptor. Overall, we demonstrate that bilayer-heterojunction OSCs with NFAs can reach competitive PCEs compared to the corresponding bulk-heterojunction OSCs because of reduced nonradiative open-circuit voltage losses, and suppressed trap-assisted recombination, as a result of a vertically separated donor-to-acceptor nanostructure. In contrast, the bilayer-heterojunction OSCs with the fullerene acceptor exhibited poor photovoltaic characteristics compared to the corresponding bulk devices because of highly aggregated acceptor molecules on top of the polymer donor. Although free carrier generation is reduced in a in a bilayer-heterojunction, because of reduced donor/acceptor interfaces and a limited exciton diffusion length, more favorable transport pathways for unipolar charge collection can partially compensate the aforementioned disadvantages. We propose that the unique properties of NFAs may open a technical venue for the bilayer-heterojunction as a great and easy alternative to the bulk heterojunction.

4.
Nat Commun ; 11(1): 6328, 2020 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-33303755

RESUMO

Light-induced halide segregation limits the bandgap tunability of mixed-halide perovskites for tandem photovoltaics. Here we report that light-induced halide segregation is strain-activated in MAPb(I1-xBrx)3 with Br concentration below approximately 50%, while it is intrinsic for Br concentration over approximately 50%. Free-standing single crystals of CH3NH3Pb(I0.65Br0.35)3 (35%Br) do not show halide segregation until uniaxial pressure is applied. Besides, 35%Br single crystals grown on lattice-mismatched substrates (e.g. single-crystal CaF2) show inhomogeneous segregation due to heterogenous strain distribution. Through scanning probe microscopy, the above findings are successfully translated to polycrystalline thin films. For 35%Br thin films, halide segregation selectively occurs at grain boundaries due to localized strain at the boundaries; yet for 65%Br films, halide segregation occurs in the whole layer. We close by demonstrating that only the strain-activated halide segregation (35%Br/45%Br thin films) could be suppressed if the strain is properly released via additives (e.g. KI) or ideal substrates (e.g. SiO2).

5.
ACS Nano ; 2020 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-33231422

RESUMO

Silver nanowire (AgNW) networks show excellent optical, electrical, and mechanical properties, which make them ideal candidates for transparent electrodes in flexible and stretchable devices. Various coating strategies and testing setups have been developed to further improve their stretchability and to evaluate their performance. Still, a comprehensive microscopic understanding of the relationship between mechanical and electrical failure is missing. In this work, the fundamental deformation modes of five-fold twinned AgNWs in anisotropic networks are studied by large-scale SEM straining tests that are directly correlated with corresponding changes in the resistance. A pronounced effect of the network anisotropy on the electrical performance is observed, which manifests itself in a one order of magnitude lower increase in resistance for networks strained perpendicular to the preferred wire orientation. Using a scale-bridging microscopy approach spanning from NW networks to single NWs to atomic-scale defects, we were able to identify three fundamental deformation modes of NWs, which together can explain this behavior: (i) correlated tensile fracture of NWs, (ii) kink formation due to compression of NWs in transverse direction, and (iii) NW bending caused by the interaction of NWs in the strained network. A key observation is the extreme deformability of AgNWs in compression. Considering HRTEM and MD simulations, this behavior can be attributed to specific defect processes in the five-fold twinned NW structure leading to the formation of NW kinks with grain boundaries combined with V-shaped surface reconstructions, both counteracting NW fracture. The detailed insights from this microscopic study can further improve fabrication and design strategies for transparent NW network electrodes.

6.
Nat Commun ; 11(1): 6005, 2020 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-33243982

RESUMO

In non-fullerene organic solar cells, the long-range structure ordering induced by end-group π-π stacking of fused-ring non-fullerene acceptors is considered as the critical factor in realizing efficient charge transport and high power conversion efficiency. Here, we demonstrate that side-chain engineering of non-fullerene acceptors could drive the fused-ring backbone assembly from a π-π stacking mode to an intermixed packing mode, and to a non-stacking mode to refine its solid-state properties. Different from the above-mentioned understanding, we find that close atom contacts in a non-stacking mode can form efficient charge transport pathway through close side atom interactions. The intermixed solid-state packing motif in active layers could enable organic solar cells with superior efficiency and reduced non-radiative recombination loss compared with devices based on molecules with the classic end-group π-π stacking mode. Our observations open a new avenue in material design that endows better photovoltaic performance.

7.
Adv Mater ; : e2002973, 2020 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-32790202

RESUMO

The performance and industrial viability of organic photovoltaics are strongly influenced by the functionality and stability of interface layers. Many of the interface materials most commonly used in the lab are limited in their operational stability or their materials cost and are frequently not transferred toward large-scale production and industrial applications. In this work, an advanced aqueous-solution-processed cathode interface layer is demonstrated based on cost-effective organosilica nanodots (OSiNDs) synthesized via a simple one-step hydrothermal reaction. Compared to the interface layers optimized for inverted organic solar cells (i-OSCs), the OSiNDs cathode interlayer shows improved charge carrier extraction and excellent operational stability for various model photoactive systems, achieving a remarkably high power conversion efficiency up to 17.15%. More importantly, the OSiNDs' interlayer is extremely stable under thermal stress or photoillumination (UV and AM 1.5G) and undergoes no photochemical reaction with the photoactive materials used. As a result, the operational stability of inverted OSCs under continuous 1 sun illumination (AM 1.5G, 100 mW cm-2 ) is significantly improved by replacing the commonly used ZnO interlayer with OSiND-based interfaces.

8.
Nat Commun ; 11(1): 3943, 2020 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-32770068

RESUMO

A major challenge for organic solar cell (OSC) research is how to minimize the tradeoff between voltage loss and charge generation. In early 2019, we reported a non-fullerene acceptor (named Y6) that can simultaneously achieve high external quantum efficiency and low voltage loss for OSC. Here, we use a combination of experimental and theoretical modeling to reveal the structure-property-performance relationships of this state-of-the-art OSC system. We find that the distinctive π-π molecular packing of Y6 not only exists in molecular single crystals but also in thin films. Importantly, such molecular packing leads to (i) the formation of delocalized and emissive excitons that enable small non-radiative voltage loss, and (ii) delocalization of electron wavefunctions at donor/acceptor interfaces that significantly reduces the Coulomb attraction between interfacial electron-hole pairs. These properties are critical in enabling highly efficient charge generation in OSC systems with negligible donor-acceptor energy offset.

9.
Adv Mater ; 32(26): e2000571, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32449209

RESUMO

Almost all highly efficient perovskite solar cells (PVSCs) with power conversion efficiencies (PCEs) of greater than 22% currently contain the thermally unstable methylammonium (MA) molecule. MA-free perovskites are an intrinsically more stable optoelectronic material for use in solar cells but compromise the performance of PVSCs with relatively large energy loss. Here, the open-circuit voltage (Voc ) deficit is circumvented by the incorporation of ß-guanidinopropionic acid (ß-GUA) molecules into an MA-free bulk perovskite, which facilitates the formation of quasi-2D structure with face-on orientation. The 2D/3D hybrid perovskites embed at the grain boundaries of the 3D bulk perovskites and are distributed through half the thickness of the film, which effectively passivates defects and minimizes energy loss of the PVSCs through reduced charge recombination rates and enhanced charge extraction efficiencies. A PCE of 22.2% (certified efficiency of 21.5%) is achieved and the operational stability of the MA-free PVSCs is improved.

10.
Front Chem ; 8: 302, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32426324

RESUMO

All-polymer solar cells (all-PSCs) composed of polymer donors and acceptors have attracted widespread attention in recent years. However, the broad and efficient photon utilization of polymer:polymer blend films remains challenging. In our previous work, we developed NOE10, a linear oligoethylene oxide (OE) side-chain modified naphthalene diimide (NDI)-based polymer acceptor which exhibited a power conversion efficiency (PCE) of 8.1% when blended with a wide-bandgap polymer donor PBDT-TAZ. Herein, we report a ternary all-PSC strategy of incorporating a state-of-the-art narrow bandgap polymer (PTB7-Th) into the PBDT-TAZ:NOE10 binary system, which enables 8.5% PCEs within a broad ternary polymer ratio. We further demonstrate that, compared to the binary system, the improved photovoltaic performance of ternary all-PSCs benefits from the combined effect of enhanced photon absorption, more efficient charge generation, and balanced charge transport. Meanwhile, similar to the binary system, the ternary all-PSC also shows excellent thermal stability, maintaining 98% initial PCE after aging for 300 h at 65°C. This work demonstrates that the introduction of a narrow-bandgap polymer as a third photoactive component into ternary all-PSCs is an effective strategy to realize highly efficient and stable all-PSCs.

11.
Nano Lett ; 20(5): 3090-3097, 2020 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-32283026

RESUMO

Despite the intense research on photovoltaic lead halide perovskites, reported optical properties as basic as the absorption onset and the optical band gap vary significantly. To unambiguously answer the question whether the discrepancies are a result of differences between bulk and "near-surface" material, we perform two nonlinear spectroscopies with drastically different information depths on single crystals of the prototypical (CH3NH3)PbI3 methylammonium lead iodide. Two-photon absorption, detected via the resulting generation of carriers and photocurrents (2PI-PC), probes the interband transitions with an information depth in the millimeter range relevant for bulk (single-crystal) material. In contrast, the transient magneto-optical Kerr effect (trMOKE) measured in a reflection geometry determines the excitonic transition energies in the region near (hundreds of nm) the surface which also determine the optical properties in typical thin films. To identify differences between structural phases, we sweep the sample temperature across the orthorhombic-tetragonal phase transition temperature. In the application-relevant room-temperature tetragonal phase (at 170 K), we find a bulk band gap of 1.55 ± 0.01 eV, whereas in the near-surface region excitonic transitions occur at 1.59 ± 0.01 eV. The latter value is consistent with previous reflectance measurements by other groups and considerably higher than the bulk band gap. The small band gap of the bulk material explains the extended infrared absorption of crystalline perovskite solar cells, the low-energy bands which carry optically driven spin-polarized currents, and the narrow bandwidth of crystalline perovskite photodetectors making use of the spectral filtering at the surface.

12.
Phys Chem Chem Phys ; 22(12): 6638-6652, 2020 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-32159553

RESUMO

The performance of solution-processed solar cells strongly depends on the geometrical structure and roughness of the photovoltaic layers formed during film drying. During the drying process, the interplay of crystallization and liquid-liquid demixing leads to structure formation on the nano- and microscale and to the final rough film. In order to better understand how the film structure can be improved by process engineering, we aim at theoretically investigating these systems by means of phase-field simulations. We introduce an evaporation model based on the Cahn-Hilliard equation for the evolution of the fluid concentrations coupled to the Allen-Cahn equation for the liquid-vapour phase transformation. We demonstrate its ability to match the experimentally measured drying kinetics and study the impact of the parameters of our model. Furthermore, the evaporation of solvent blends and solvent-vapour annealing are investigated. The dry film roughness emerges naturally from our set of equations, as illustrated through preliminary simulations of spinodal decomposition and film drying on structured substrates.

13.
Adv Mater ; 32(14): e1907801, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32049386

RESUMO

Fundamental advances to increase the efficiency as well as stability of organic photovoltaics (OPVs) are achieved by designing ternary blends, which represents a clear trend toward multicomponent active layer blends. The development of high-throughput and autonomous experimentation methods is reported for the effective optimization of multicomponent polymer blends for OPVs. A method for automated film formation enabling the fabrication of up to 6048 films per day is introduced. Equipping this automated experimentation platform with a Bayesian optimization, a self-driving laboratory is constructed that autonomously evaluates measurements to design and execute the next experiments. To demonstrate the potential of these methods, a 4D parameter space of quaternary OPV blends is mapped and optimized for photostability. While with conventional approaches, roughly 100 mg of material would be necessary, the robot-based platform can screen 2000 combinations with less than 10 mg, and machine-learning-enabled autonomous experimentation identifies stable compositions with less than 1 mg.

14.
Adv Mater ; 32(16): e1908305, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32108389

RESUMO

As the power conversion efficiency (PCE) of organic solar cells (OSCs) has surpassed the 17% baseline, the long-term stability of highly efficient OSCs is essential for the practical application of this photovoltaic technology. Here, the photostability and possible degradation mechanisms of three state-of-the-art polymer donors with a commonly used nonfullerene acceptor (NFA), IT-4F, are investigated. The active-layer materials show excellent intrinsic photostability. The initial morphology, in particular the mixed region, causes degradation predominantly in the fill factor (FF) under illumination. Electron traps are formed due to the reorganization of polymers and diffusion-limited aggregation of NFAs to assemble small isolated acceptor domains under illumination. These electron traps lead to losses mainly in FF, which is in contradistinction to the degradation mechanisms observed for fullerene-based OSCs. Control of the composition of NFAs close to the thermodynamic equilibrium limit while keeping adequate electron percolation and improving the initial polymer and NFA ordering are of the essence to stabilize the FF in NFA-based solar cells, which may be the key tactics to develop next-generation OSCs with high efficiency as well as excellent stability.

15.
ACS Appl Mater Interfaces ; 11(42): 39018-39025, 2019 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-31576735

RESUMO

Controllably manipulating the spectral response of broadband-absorbing semiconductors is crucial for developing wavelength-selective optoelectronic devices. In this article, we report for the first time, the bias-dependent spectral responses for a metal-halide perovskite photodiode. Tunable external quantum efficiencies in the short- and long-wavelength regimes, and the full spectral range (ca. 300-800 nm) are observed when the device is operated under short-circuit, and forward and reverse bias conditions, respectively. This observation is understood by the interplay of wavelength-dependent penetration depth and barrier formation within the photodiode device stack. The general applicability of this concept is confirmed by a systematic study on a series of mixed-halide perovskite devices. These results suggest that the proposed concept allows as a promising platform and should inspire further exploration of multispectral responsive optoelectronic devices.

16.
Adv Sci (Weinh) ; 6(17): 1901067, 2019 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-31508290

RESUMO

Metal halide perovskite solar cells (PSCs) have raised considerable scientific interest due to their high cost-efficiency potential for photovoltaic solar energy conversion. As PSCs already are meeting the efficiency requirements for renewable power generation, more attention is given to further technological barriers as environmental stability and reliability. However, the most major obstacle limiting commercialization of PSCs is the lack of a reliable and scalable process for thin film production. Here, a generic crystallization strategy that allows the controlled growth of highly qualitative perovskite films via a one-step blade coating is reported. Through rational ink formulation in combination with a facile vacuum-assisted precrystallization strategy, it is possible to produce dense and uniform perovskite films with high crystallinity on large areas. The universal application of the method is demonstrated at the hand of three typical perovskite compositions with different band gaps. P-i-n perovskite solar cells show fill factors up to 80%, underpinning the statement of the importance of controlling crystallization dynamics. The methodology provides important progress toward the realization of cost-effective large-area perovskite solar cells for practical applications.

17.
Nat Commun ; 10(1): 4100, 2019 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-31506443

RESUMO

Naphthalenediimide-based n-type polymeric semiconductors are extensively used for constructing high-performance all-polymer solar cells (all-PSCs). For such all-polymer systems, charge recombination can be reduced by using thinner active layers, yet suffering insufficient near-infrared light harvesting from the polymeric acceptor. Conversely, increasing the layer thickness overcomes the light harvesting issue, but at the cost of severe charge recombination effects. Here we demonstrate that to manage light propagation within all-PSCs, a thick bulk-heterojunction film of approximately 350 nm is needed to effectively enhance photo-harvesting in the near-infrared region. To overcome the severe charge recombination in such a thick film, a non-halogenic additive is used to induce a well-ordered micro-structure that inherently suppresses recombination loss. The combined strategies of light management and delicate morphology optimization lead to a promising efficiency over 10% for thick-film all-PSCs with active area of 1 cm2, showing great promise for future large-scale production and application of all-PSCs.

18.
J Am Chem Soc ; 141(31): 12322-12328, 2019 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-31310113

RESUMO

Effective, solution-processable designs of interfacial electron-transporting layers (ETLs) or hole-blocking layers are promising tools in modern electronic devices, e.g., to improve the performance, cost, and stability of perovskite-based solar cells. Herein, we introduce a facile synthetic route of thiazole-modified carbon nitride with 1.5 nm thick nanosheets which can be processed to a homogeneous, metal-free ETL for inverted perovskite solar cells. We show that thiazole-modified carbon nitride enables electronic interface enhancement via suppression of charge recombination, achieving 1.09 V in Voc and a rise to 20.17 mA/cm2 in Jsc. Hence, this report presents the successful implementation of a carbon-nitride-based structure to boost charge extraction from the perovskite absorber toward the electron transport layer in p-i-n devices.

19.
ACS Appl Mater Interfaces ; 11(32): 28851-28857, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31314481

RESUMO

Metal halide perovskite semiconductors have the potential to enable low-cost, flexible, and efficient solar cells for a wide range of applications. Physical vapor deposition by co-evaporation of precursors is a method that results in very smooth and pinhole-free perovskite thin films and allows excellent control over film thickness and composition. However, for a deposition method to become industrially scalable, reproducible process control and high device yields are essential. Unfortunately, to date, the control and reproducibility of evaporating organic precursors such as methylammonium iodide (MAI) have proved extremely challenging. We show that the established method of controlling the evaporation rate of MAI with quartz microbalances (QMBs) is critically sensitive to the concentration of the impurities MAH2PO3 and MAH2PO2 that are usually present in MAI after synthesis. Therefore, controlling the deposition rate of MAI with QMBs is unreliable since the concentration of such impurities typically varies from one batch of MAI to another and even during the course of a deposition. However once reliable control of MAI deposition is achieved, we find that the presence of precursor impurities during perovskite deposition does not degrade the solar cell performance. Our results indicate that as long as precursor deposition rates are well controlled, physical vapor deposition will allow high solar cell device yields even if the purity of precursors changes from one run to another.

20.
ACS Appl Mater Interfaces ; 11(20): 18555-18563, 2019 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-31046222

RESUMO

Worldwide research efforts have been devoted to organic photovoltaics in the hope of a large-scale commercial application in the near future. To meet the industrial production requirements, organic photovoltaics that can reach power conversion efficiency (PCE) of over 10% along with promising operational device stability are of utmost interest. In the study, we take PCE11:PCBM as a model system, which can achieve over 11% PCE when processed from nonhalogen solvents, to deeply investigate the morphology-performance-stability correlation. We demonstrate that four batches of PCE11 with varying crystalline properties can achieve similar high performance in combination with PCBM. Careful device optimization is necessary in each case to properly address the requirements for the quite distinct microstructures. The bulk-heterojunction (BHJ) microstructure is comprehensively investigated as a function of the macromolecular weight and crystallinity. It is demonstrated that small differences in morphology significantly affect the kinetics and thermodynamic equilibrium of the BHJ microstructure as well as the photostability and thermal stability of the PCE11:PCBM solar cells.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA
...