Recently, much effort has been devoted to improve the efficiency of organic photovoltaic solar cells based on blends of donors and acceptors molecules in bulk heterojunction architecture. One of the major losses in organic photovoltaic devices has been recombination of polaron pairs at the donor/acceptor domain interfaces. Here, we present a novel method to suppress polaron pair recombination at the donor/acceptor domain interfaces and thus improve the organic photovoltaic solar cell efficiency, by doping the device active layer with spin 1/2 radical galvinoxyl. At an optimal doping level of 3 wt%, the efficiency of a standard poly(3-hexylthiophene)/1-(3-(methoxycarbonyl)propyl)-1-1-phenyl)(6,6)C61 solar cell improves by 18%. A spin-flip mechanism is proposed and supported by magneto-photocurrent measurements, as well as by density functional theory calculations in which polaron pair recombination rate is suppressed by resonant exchange interaction between the spin 1/2 radicals and charged acceptors, which convert the polaron pair spin state from singlet to triplet.
High-speed and high-gain graphene photovoltaic phototransistor gated by a van der Waals heterojunction
School of Integrated Circuits and Microelectronics, State Key Laboratory of Flexible Electronics & School of Flexible Electronics, Northwestern Polytechnical University（西北工业大学集成电路与微纳电子学院、柔性电子技术研究院）；School of Physical Science and Technology, Northwestern Polytechnical University（西北工业大学物理科学与技术学院）
Hybrid Interface States and Spin Polarization at Ferromagnetic Metal-Organic Heterojunctions: Interface Engineering for Efficient Spin Injection in Organic Spintronics
Organic heterojunction solar cells are analyzed within a minimal model that includes the essential physical features of such systems. The dynamical properties of this model, calculated using a master equation approach, account for the qualitative behavior of such systems. The model yields explicit results for current-voltage behavior as well as performance characteristics expressed in terms of the thermodynamic efficiency as well as the power conversion efficiency at maximum power, making it possible to evaluate the optimal setup for this device model.
We report the influence of the AlN interlayer thickness (0-15 nm) on the photovoltaic properties of Al0.37In0.63N on Si heterojunction solar cells deposited by radio frequency sputtering. The poor junction band alignment and the presence of a 2-3 nm thick amorphous layer at the interface mitigates the response in devices fabricated by direct deposition of n-AlInN on p-Si(111). Adding a 4-nm-thick AlN buffer layer improves the AlInN crystalline quality and the interface alignment leading to devices with a conversion efficiency of 1.5% under 1-sun AM1.5G illumination. For thicker buffers the per…
For many years the faith of organic photovoltaics has been linked to the one of fullerene, since fullerene has been considered the electron-acceptor of choice in bulk heterojunctions solar cells. In the last years, the number of molecules that can be very competitive in replacing fullerene has increased significantly. In this work, we study by means of different theoretical methods five molecules that have demonstrated to work effectively as acceptors in organic heterojunctions. We discuss the comparison of simulated absorption spectra with the experimental spectra.
Energetic disorder induced leakage current in organic bulk heterojunction solar cells: comprehending the ultra-high open circuit voltage loss at low temperatures
Recombination losses contribute to reduce $J_{SC}$, $V_{OC}$ and the fill factor of organic solar cells. Recent advances in non-fullerene organic photovoltaics have shown, nonetheless, that efficient charge generation can occur under small energetic driving forces ($ΔE_{DA}$) and low recombination losses. To shed light on this issue, we set up a coarse-grained open quantum mechanical model for investigating the charge generation dynamics subject to various energy loss mechanisms. The influence of energetic driving force, Coulomb interaction, vibrational disorder, geminate recombination, temper…
Absence of Structural Impact of Noble Nanoparticles on P3HT: PCBM Blends for Plasmon Enhanced Bulk-Heterojunction Organic Solar Cells Probed by Synchrotron Grazing Incidence X-Ray Diffraction
In organic bulk heterojunction solar cells, the donor/acceptor interfacial energy offset ($ΔE$) is found to provide the driving force for efficient charge separation which gives rise to high short circuit current density ($J_\mathrm{sc}$), but a high $ΔE$ inevitably undermines the open circuit voltage ($V_\mathrm{oc}$). In this paper, employing the device model method we calculated the steady state current density-voltage ($J-V$) and the $J_\mathrm{sc}-ΔE$ curves under two different charge separation mechanisms to investigate the optimum driving force required for achieving sizable $V_\mathrm{…
Organic Photovoltaic devices (OPVs) are becoming adequately cost and energy efficient to be considered a good investment and it is, therefore, especially important to have a concrete understanding of their operation. We compute energies of charge-transfer (CT) states of the model donor-acceptor lattice system with varying degrees of structural disorder to investigate how fluctuations in the material properties affect electron-hole separation. We also demonstrate how proper statistical treatment of the CT energies recovers experimentally observed "hot" and "cold" exciton dissociation pathways. …
Organic solar cells (OSCs) containing an active layer consisting of a nanostructured blend of a conjugated polymer like poly(3-hexylthiophene) (P3HT) and an electron acceptor molecule have the potential of competing against silicon-based photovoltaic panels. However, this potential is unfulfilled primarily due to interrelated production and stability issues. The generally employed spin coating process for fabricating organic solar cells cannot be scaled up. Recently, He et al., have reported that the gelation of P3HT with [6,6]-phenyl-C61-butyric acid methyl ester (PC60BM) under sub-ambient co…
Linking the highly complex morphology of organic photovoltaic (OPV) thin films to their charge transport properties is critical for achieving high performance material system that serves as a cost-efficient approach for energy harvesting. In this paper, a novel unsupervised feature engineering framework is developed and used to establish reduced-order structure-property linkages for OPV films. This framework takes advantage of digital image processing algorithms to identify the salient material features of OPVs undergoing the charge transport phenomenon. These material states are then used to …
The performance of organic solar cells strongly depends on the bulk heterojunction (BHJ) morphology of the photoactive layer. This BHJ forms during the drying of the wet-deposited solution, because of physical processes such as crystallization and/or liquid liquid phase separation (LLPS). However, the process-structure relationship remains insufficiently understood. In this work, a recently developed, coupled phase field fluid mechanics framework is used to simulate the BHJ formation upon drying. For the first time, this allows to investigate the interplay between all the relevant physical pro…
We investigate nongeminate recombination in organic solar cells based on copper phthalocyanine (CuPc) and C$_{60}$. Two device architectures, the planar heterojunction (PHJ) and the bulk heterojunction (BHJ), are directly compared in view of differences in charge carrier decay dynamics. We apply a combination of transient photovoltage (TPV) experiments, yielding the small perturbation charge carrier lifetime, and charge extraction measurements, providing the charge carrier density. In organic solar cells, charge photogeneration and recombination primarily occur at the donor--acceptor heteroint…
Electron energy-loss spectroscopy (EELS) is a powerful tool for imaging chemical variations at the nanoscale. Here, we investigate a polymer/organic small molecule-blend used as absorber layer in an organic solar cell and employ EELS for distinguishing polymer donor and small molecule acceptor domains in the nanostructured blend based on elemental maps of light elements, such as nitrogen, sulfur or fluorine. Especially for beam sensitive samples, the electron dose needs to be limited, therefore optimized acquisition and data processing strategies are required. We compare data acquired on a pos…
Energy level diagrams in organic electronic devices play a crucial role in device performance and interpretation of device physics. In the case of organic solar cells, it has become routine to estimate the photovoltaic gap of the donor:acceptor blend using the energy values measured on the individual blend components, resulting in a poor agreement with the corresponding open-circuit voltage of the device. To address this issue, we developed a method that allows a direct visualisation of the vertical energetic landscape in the blend, obtained by combining ultraviolet photoemission spectroscopy …
We investigate the mechanical properties of $π$-conjugated polymeric materials composed of regioregular poly(3-hexylthiophene) (P3HT) and fullerene C$_{60}$ using coarse-grained molecular dynamics simulations. Specifically, we perform tensile simulations of P3HT:C$_{60}$ composites with varied degrees of polymerization and C$_{60}$ mass fractions to obtain their stress-strain responses. Decomposition of stress tensor into kinetic energy and virial contributions indicates that the tensile moduli of the pure P3HT samples are greatly dependent on non-bonded interactions and on bonded interactions…
In this article the Wells-Dawson polyoxometalate K6[P2W18O62] is grown as an interfacial layer between indium tin oxide and bulk heterojunction of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM). The structure of the POM layers depends on the thickness and shows a highly anisotropic surface organization. The films have been characterized by atomic force microscopy and X-ray photoelectron spectroscopy (XPS) to gain insight into their macroscopic organization and better understand their electronic properties. Then, they were put at the anodic interface of a P3…
First-principles investigation of organic photovoltaic materials C$_{60}$, C$_{70}$, [C$_{60}$]PCBM, and bis-[C$_{60}$]PCBM using a many-body $G_0W_0$-Lanczos approach
