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Spatial distribution of triplet excitons near the organic semiconductor interface is clarified. The result indicates that 90% of the triplet excitons are confined to less than 10 nm from the interface, where photoelectric conversion and charge recombination occur.

Li@PCBM was synthesized. It exists in a monomer-dimer equilibrium in solution but as a monomer in the PCBM matrix. The fully dispersed Li@PCBM served as an n-dopant for the surrounding empty PCBM, raising the Fermi level by 0.13 eV.

The single relaxation time (SRT) and the revised matrix (RM) lattice Boltzmann models are compared for simulations of three dimensional forced isotropic turbulence with resolutions of 1283 and 2563, respectively. Guo et al.[1] forcing technique with the same forcing parameters and conditions is used to investigate the ability and stability of the two models for simulations of forced turbulence. Some new aspects and results have been confirmed such as the superiority of the MRT model to simulate forced turbulence in comparison with the SRT model. To overcome the stability shortage problem of the lattice Boltzmann models, it is proposed to apply the Courant-Friedichs-Lewy condition (CFL) [2] by multiplying the velocity input with the CFL coefficient which is less than unity and by dividing the output velocity data by the same CFL coeffi-cent. The initial velocity field is chosen as u(x, 0) = 0 and the force is injected at low wave-numbers with a fixed forcing amplitude of 10−4 for all cases. The single relaxation time is set to τ = 0.503 in all SRT simulations. Results show that the obtained turbulent velocity fields yield universal characteristics as proven in previous theoretical, experimental and numerical studies. The Taylor Reynolds number for the simulations are found as : Rλ(SRT) = 62 and Rλ(M RT) = 65 for the resolution of 1283 and Rλ(SRT) = 107 and Rλ(M RT) = 82 for the case of 2563, respectively. To test the weak incompressibility for the SRT model in comparison to the MRT model, the probability distribution function (PDF) of the density ρ is depicted and it is found that ρ is almost unity at all timesteps for the MRT case, while a clear disturbance about unity is observed for the SRT case. Time variation’s statistics such as the Taylor Reynolds number Rλ, the Taylor microscale λ, the Kolmogrov microscale η and energy spectra are calculated and depicted for all cases. One of the disadvantages of the MRT case is the simulations time which is found about twice the SRT simulations time, where about 80 hours are needed for simulating 12000 timesteps in the 2563 case in comparison to 42 hours for the SRT model using the same hardware resources.

Among the three primary colors, blue emission in organic light-emitting diodes (OLEDs) are highly important but very difficult to develop. OLEDs have already been commercialized; however, blue OLEDs have the problem of requiring a high applied voltage due to the high-energy of blue emission. Herein, an ultralow voltage turn-on at 1.47 V for blue emission with a peak wavelength at 462 nm (2.68 eV) is demonstrated in an OLED device. This OLED reaches 100 cd/m2, which is equivalent to the luminance of a typical commercial display, at 1.97 V. Blue emission from the OLED is achieved by the selective excitation of the low-energy triplet states at a low applied voltage by using the charge transfer (CT) state as a precursor and the triplet-triplet annihilation, which forms one emissive singlet from two triplet excitons. We found that the essential component for efficient blue emission is a smaller energy difference between the CT state and triplet exciton, accelerating the energy transfer between the two states and achieving the optimal performance by avoiding direct decay from the CT state to the ground state. Our study demonstrates that the developed OLED allows for a much longer operation lifetime than that from a typical blue phosphorescent OLED because the blue emission originates from a stable low-energy triplet exciton that avoids degrading the constituent materials.

The energy of photons, that is, the wavelength of light, can be upgraded through interactions with materials in a process called photon upconversion1. Although upconversion in organic solids is important for various applications, such as photovoltaics and bioimaging, conventional upconversion systems, based on intersystem crossing (ISC), suffer from low efficiency2–6. Here we report a novel upconversion system with heterojunctions of organic semiconductors. The upconversion occurs through charge separation and recombination, which mediate charge transfer states at the interface. This process can efficiently convert the incident photons to triplets without relying on ISC, which is typically facilitated by the heavy-atom effect1. As a result, a solid-state upconversion system is achieved with an external efficiency that is two orders of magnitude higher than those demonstrated by conventional systems6. Using this result, efficient upconversion, from near-infrared to visible light, can be realized on flexible organic thin films under a weak light-emitting-diode-induced excitation, observable by naked eyes. Highly efficient upconversion of light by organic semiconductor heterojunction interfaces is demonstrated. This process is enabled by charge separation- and recombination-mediated charge transfer states at the interface.

Single-crystalline organic semiconductors exhibiting band transport have opened new possibilities for the utilization of efficient charge carrier conduction in organic electronic devices. The epitaxial growth of molecular materials is a promising route for the realization of well-crystallized organic semiconductor p–n junctions for optoelectronic applications enhanced by the improved charge carrier mobility. In this study, the formation of a high-quality crystalline interface upon “quasi-homoepitaxial” growth of bis(trifluoromethyl)dimethylrubrene (fmRub) on the single-crystal surface of rubrene was revealed by using out-of-plane and grazing-incidence X-ray diffraction techniques. Ultraviolet photoelectron spectroscopy results indicated abrupt electronic energy levels and the occurrence of band bending across this quasi-homoepitaxial interface. This study verifies that the minimization of the lattice mismatch enhances the crystalline qualities at the heterojunctions even for van der Waals molecular condensates, potentially opening an untested route for the realization of high-mobility organic semiconductor optoelectronics.

Curved perylene diimides fused with seven-membered rings have been synthesized using a regioselective bay-functionalization method and Pd-catalyzed intramolecular C-H/C-Br coupling reaction. X-Ray analysis and temperature-dependent NMR spectroscopy revealed the curved molecular structure with a certain degree of conformational flexibility. The curved and expanded π-conjugation altered the electronic properties while retaining the intrinsic properties of the parent perylene diimide. Despite the absence of solubilizing N-substituents, the curved perylene diimides showed sufficient solubility for application in solution-processed organic photovoltaic devices. The devices showed superior performance with a power conversion efficiency of up to 2.76% due to suppressed charge recombination. Our detailed investigations suggest that the introduction of a curved structure enables the removal of the bulky N-substituents, which is an effective way to achieve a thin-film morphology suitable for photoelectric conversion.

Dinaphtho[2,3-b:2',3'-f]thieno[3,2-b]thiophene (DNTT) is a p-type organic semiconductor that exhibits high charge-carrier mobility and atmospheric stability. Although it has been proposed that the ...

Polymer-blend solar cells (all-PSCs) based on a copolymer of naphthodithiophene diimide and bithiophene (PNDTI-BT-DT) as a near-infrared absorber as well as an electron acceptor were fabricated in combination with PTB7 as an electron donor. Notably, the external quantum efficiency spectra of the all-PSCs demonstrated photoresponse up to 900 nm with the efficiency of 25% at 800 nm, which is much higher than that for the previously reported all-PSCs. Power conversion efficiency as high as 2.59% was achieved under the irradiation of simulated solar light (AM1.5, 100 mW/cm2). Both PNDTI-BT-DT and PTB7 formed a crystalline structure in the blend films similar to in the pristine films, leading to the efficient charge generation contributed from both polymers.

The development of an efficient synthetic protocol for multiply bay-functionalized perylenes and application of these products to photovoltaics are reported. Tetrabenzyl 1-(4-tert-butylphenoxy)perylene-3,4,9,10-tetracarboxylate underwent a regioselective bromination at the 7-position followed by a further bromination at the 12-position to provide a 7,12-dibromide in high 84% yield. This compound was transformed into a tetrasubstituted C2h -symmetric dibromide by a controlled monoetherification and a final bromination. The synthetic versatility of the new brominated precursors was demonstrated by their application to cross-coupling reactions, cyanation, and derivatization to the corresponding perylene diimide (PDI). Owing to the high solubility and the raised LUMO level, the obtained tetrasubstituted PDI showed significant advantages as an acceptor material for photovoltaic applications, exhibiting a remarkably high open-circuit voltage (VOC ) reaching 1.00 V. The observed high VOC could be understood by reduction of energy offset for charge separation and non-radiative recombination loss.

The influence of N-substituents on the photovoltaic properties of singly bay-linked perylene diimides (diPDIs) was systematically investigated to understand the aromatic-aliphatic balance, which is beneficial for achieving high device performance in organic photovoltaic (OPV) systems. The synthesis of various N-substituted diPDIs was successfully achieved using a newly developed one-step procedure, resulting in sufficiently high yields. Detailed investigations of seven variants of diPDIs demonstrated that the primary alkyl substituents, particularly the 2-ethylhexyl group, induce the self-organized growth of thin films with high crystallinity. This is beneficial for enhancing the device performance of bulk heterojunction (BHJ) systems. The results presented herein reveal the important roles of alkyl side chains as hydrophobic solubilizing auxiliaries or primary determinants in the control of the active layer nanomorphology. This offers a valuable guideline that is essential for developing high-performance organic semiconductor materials for future practical applications.

A two dimensional partial differential equation scheme that uses a second-order hyperbolic diffusion equation for image denoising is developed to a three dimensional model for filtering isotropic turbulence. The mathematical derivation of the model is introduced and a consistent finite difference numerical approximation scheme is proposed. The model is tested against the velocity fields of isotropic turbulence that are simulated by solving the lattice Boltzmann(LB) and the Navier–Stokes(NS) equations, respectively. The D3Q15 LB model and the Fourier spectral method are used to solve the LB equation and the Navier–Stokes vorticity equation at grid points of 2563, respectively. Also the filtering method with the choice of the same filtering parameters is applied against a synthetic turbulent field with the same number of points. The high rotation vortex identification method Q is used to visualize the total, coherent and incoherent fields in all cases of the study. Despite the different nature of the LB and NS direct numerical simulations and the synthetic turbulence, all input parameters for the hyperbolic filtering model are chosen the same in all cases. Comparisons between the LB and NS filtered energy spectra, coherent vortices, incoherent regions, skewness, flatness and the fourth order moments are also considered. The same features are calculated for the non-filtered and filtered synthetic turbulent fields. It is shown that the coherent part preserves all statistical features of turbulence. However, the isotropy is the only feature that has been preserved for the incoherent part and other statistical features are divergent in all cases of the study.

In this study, attempts to suppress numerical viscosity in incompressible smoothed particle hydrodynamics (SPH) computations are reported. Two-dimensional computations are performed for inviscid and viscous flows to evaluate the effects of numerical viscosity suppression. The first approach is to reduce numerical viscosity at the wall by considering only the wall-normal components of the forces between fluid particles and wall particles. The second approach is to reduce numerical viscosity within the flow field by employing elliptic kernel functions whose major axes are aligned with the local mean flow direction. It is found that special treatment of the wall radically reduces the numerical wall friction. Using an elliptic kernel function is found to work reasonably well in reducing numerical viscosity.

Numerical simulations of the liquid flow scattering from rotary atomizers are performed using an incompressible smoothed particle hydrodynamics (SPH) method. The influence of grooves at the edges of the atomizers on the formation of ligaments and droplets is investigated changing the numbers and shapes of the grooves. As a result, it is found that small droplets are likely to be generated when the number of grooves is large and the depth of grooves is deep. It is also found that the grooves work more effectively in bell-cup atomizers than in disk type atomizers. Keywords: Smoothed particle hydrodynamics (SPH), Rotary atomizer, Grooves, Droplet

Formation of pn homojunction in a single semiconductor material through doping is key for photocurrent generation in inorganic solar cells (SCs). In contrast, a donor/acceptor heterojunction is generally utilized in organic SCs in order to split coulombically bound exciton forming in organic semiconductors. Here, an organic pn homojunction SC showing high internal quantum efficiency of about 30% is reported. pn Homojunction was created by co-deposition of p or n type dopants and an organic semiconductor. An increase of the photocurrent density by more than 8 times, from the undoped device to pn homojunction device with 5% doping, was observed. The increase of photocurrent due to charge separation was assisted by the built-in potential near the pn homojunction interface that was controlled by doping concentration. The result demonstrated that the pn homojunction interface in a single organic semiconductor layer formed by doping can achieve efficient charge separation and provide a suitable alternative to the donor/acceptor interface that has been considered necessary for photoconversion in organic SCs.

Blended junctions are indispensable for organic solar cells; however, the fabrication of electron and hole transport routes in blended cells remains quite challenging. Herein, a lateral alternating multilayered junction using a high-mobility organic semiconductor is proposed and demonstrated. A total of 93% of the photogenerated electrons and holes are laterally collected over a long distance (0.14 mm). The exciton-collection efficiency reaches 75% in a lateral alternating multilayered junction with a layer thickness of 10 nm. A lateral organic alternating multilayered junction that completely collects both excitons and carriers can be an alternative blended junction for organic solar cells.

Doped rubrene single-crystal photovoltaic cells were fabricated. Whole photocurrent generated in the pn-homojunction with the macroscopic area of 2 mm × 1 mm was confirmed to be collected through the p-doped homoepitaxial layer. A single-crystal substrate collected excitons to the pn-homojunction with the collection efficiency reaching 46%, owing to the long exciton diffusion length of 2.7 μm.

Energy of photons, i.e. the wavelength of light, can be upgraded through interactions with materials—a process called photon upconversion (UC). Although UC in organic solids is important for various applications, such as in photovoltaics and bioimaging, conventional UC systems, based on intersystem crossing (ISC), suffer from low efficiency. Herein, we report a novel UC mechanism at heterojunctions of organic semiconductors in bilayer structures. The UC occurs by triplet formation during the charge separation and recombination through dynamic exciton: charge transfer (CT) state at the interface. This can efficiently convert the incident photons to triplets without relying on the ISC, whose rate is typically accelerated by the heavy-atom effect. As a result, a solid-state UC system is achieved with an external efficiency of two orders of magnitude higher than those of the conventional systems. Using this result, efficient UC, from near-infrared to visible light, cab be realized on flexible organic thin films under a weak light-emitting diode-induced excitation, observable by naked eyes. Reference: S. Izawa and M. Hiramoto, Nat. Photon., DOI: org/10.1038/s41566-021-00904-w.

Charge transfer (CT) state is a key intermediate to understand recombination processes in organic solar cells (OSCs). In this study, we measured the recombination emission from the CT state under different applied voltages in OSCs and a photocurrent density flowing on the circuit simultaneously. We proposed a “photoluminescence (PL)–voltage (V) plot” that is the voltage dependence of PL intensity of the CT state. The PL–V plot includes information only from the CT state recombination at the donor/acceptor interface and is complementary to the “current density (J)–V plot” that is the most important information for evaluating OSCs. The results demonstrated that the fill factor (FF) of the PL–V plot is higher than that of the J–V plot, predicting the ideal FF of the device. Our result demonstrated that the simultaneous measurement of photocurrent and recombination emission could be a strong tool for evaluating photoconversion characteristics in OSCs.

Reducing operating voltage is the remaining frontier for organic light-emitting diodes (OLEDs) because their quantum efficiency (QE) of electroluminescence has been already maximized. Herein, we report an efficient OLED in which a blight emission equivalent to a luminance of a display is achieved by only a 1.5 V battery. The OLED is based on upconversion (UC) emission utilizing triplet-triplet annihilation occurring near donor/acceptor (D/A) interface. We found that a character of a charge transfer state that is key intermediate for the UC emission could be controlled by D/A interfacial interaction. As a result, parasitic loss processes for UC were greatly suppressed from over 90% to about 10%, and two order of magnitude higher QE than the previous UC-OLED was achieved. Our result demonstrated that the efficient UC could be realized by the management of the energy transfer steps at the D/A interface and utilizing UC emission can be one of the possible candidate for efficient OLED with extremely low driving voltage.

In the field of organic solar cells, lateral junction is a new concept. Moreover, the photovoltaic behavior is firstly observed for surprising long organic lateral junctions reaching 1.8 cm and the new operation mechanism dominated by trap-assisted recombination is proposed.

In the field of organic solar cells, lateral junction is a new concept. Moreover, the photovoltaic behavior is firstly observed for surprising long organic lateral junctions reaching 1.8 cm and the new operation mechanism dominated by trap-assisted recombination is proposed.

An experimental study is performed to investigate the flow structures near the edges of rotating disks with different edge shapes. By changing the rotational speed, the Reynolds number is changed from 277 to 356. It is found that the fluid motion near the sharp edge differs depending on whether a rotating shaft is at the disk surface. A flow developing on the flat side of the disk surface changes its direction toward the curved outer surface on the shaft side, and the flow goes straight outward, leaving the disk on the flat side. The existence of the supporting shaft increases the radial velocity of the flow while decreasing the azimuthal velocity. The effects of the edge shape of the disk on the flow fields are also investigated by changing the shape of the disk edges. Rounded and chamfered edges have no noticeable effect on the azimuthal velocity on the curved outer surface, whereas changing the edge shape enhanced the velocity in the disk-thickness direction. In the FFT analyses of the azimuthal velocity measured at the edge of the curved outer surface when the disk edge is rounded, an increase in power across a range of frequencies is observed. Only in the chamfered edge disk case, a peak in the spectrum of the velocity that corresponds to a wavenumber which appears in the transitional boundary layers is observed.

This study numerically investigates an early stage of nonlinear interaction for the better understanding of the onset of nonlinear behaviors. Two-dimensional shear flow is chosen as a canonical flow. When two disturbances of different wavenumbers satisfying no resonance condition are initially given, new components appear one after another while the original disturbances grow. The vorticity budget analysis shows that the beat of the two exciting modes plays an essential role in forming the sum and difference nonlinear components, namely the secondary modes. For the nonlinear interaction mechanism, the high vorticity around the center of the shear layer is locally transported in the transverse direction at specific streamwise sections where the amplitude of the vertical velocity fluctuation becomes relatively larger compared to other sections. The distance between these specific sections corresponds to the wavelength of the beat. The vertically dispersed vorticity will then be convected in the horizontal directions by the mean flow. As a result, several regions of concentrated vorticity appear which eventually develop into vortices. The amplification mechanism is found to be the same for both the primary and secondary modes, though the secondary modes arise from the additional perturbation deriving from the initial perturbation.

Organic solar cells (OSCs) based on blends of electron donor (D) and acceptor (A) semiconducting materials now have a power conversion efficiency exceeding 17%, and 100% internal quantum efficiency of free charge generation has already been realized. Therefore, reducing the energy loss in the open-circuit voltage (VOC) is critically important for further enhancing the efficiency of OSCs. In this chapter, the background and recent findings concerning VOC in OSCs are reviewed, beginning with an explanation of the photoconversion mechanism in OSCs in relation to VOC. Following this, the empirical understanding of VOC is outlined, and the models used for explaining the determination of VOC in OSCs are described. In the next section, recent progress for increasing VOC in OSCs by modifying the D/A interface is summarized. The topics discussed are energy-level alignment, doping, the pn homojunction, energy-level control at the monolayer scale, crystallinity, and functionalization of acceptor molecules. Finally, ways in which the VOC in OSCs can be maximized are proposed with a view to the future.

Perylene has had a tremendous impact in the history of material research for the molecular semiconductors. Among numerous derivatives of this polyaromatic hydrocarbon, perylene diimide (PDI) represents a promising class of organic materials envisioned as non-fullerene acceptors (NFAs) for the practical organic photovoltaic (OPV) applications due to their enhanced photo- and thermal stability and remarkably high electron affinity, some of which realize band-like transport properties. The present review guides some of the representative achievements in the development of rationally designed PDI systems, highlighting synthetic methodologies based on bay-functionalization strategies for creating well-designed molecular nanostructures and structure-performance relationship of perylene-based small molecular acceptors (SMAs) for the photovoltaic outcomes.