Search Results (31)

Developing white organic light-emitting diodes (WOLEDs) with high exciton utilization, balanced charge transport, and stable complementary emission remains a challenge for solid-state lighting and display applications. Herein, a triplet reverse intersystem crossing (RISC)-assisted strategy is proposed to enhance triplet exciton harvesting to construct efficient hybrid WOLEDs. The increased RISC channels promote the up-conversion of triplet excitons into radiative singlet excitons, thereby improving the overall exciton utilization efficiency. By further introducing an ultrathin PO-01 layer as an orange orange-emitting component, a hybrid WOLED with a current efficiency of 49.1 cd/A and 34.8 lm/W is realized. Moreover, suppressed efficiency roll-offs and stable spectra are achieved due to balanced charge transport. This work provides a practical route toward high-performance WOLEDs. Full article

Organic light-emitting diodes (OLEDs) have attracted remarkable interest in display and lighting. To effectively address triplet exciton harvesting and enhance external quantum efficiency (EQE), delayed fluorescence AIEgens have gained significant prominence. The primary luminescence mechanism involves the efficient harvesting of triplet excitons via reverse intersystem crossing (RISC) channels, categorized into three types: thermally activated delayed fluorescence (TADF), hybridized local and charge transfer (HLCT), and triplet–triplet annihilation (TTA). In this review, we summarize the recent development of doped and non-doped delayed fluorescent AIEgens-based OLEDs. This review mainly discusses the molecular design strategies and photophysical properties of delayed fluorescent AIEgens and the electroluminescent properties of OLEDs as emitting layers. Finally, the challenges and prospects of delayed fluorescent AIEgens for the fabrication of OLEDs are also briefly discussed. Full article

Thin-film organic solar cells (TFOSCs) are gaining momentum as next-generation photovoltaic technologies due to their lightweight nature, mechanical flexibility, and low cost-effective fabrication. In this pioneering study, we report for the first time the incorporation of cobalt-doped zinc sulfide $(\mathrm{Z}\mathrm{n}\mathrm{S}/\mathrm{C}\mathrm{o})$ nanoparticles (NPs) into a poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl-C61-butyric acid methyl ester (PC61BM) bulk-heterojunction photoactive layer. $\mathrm{Z}\mathrm{n}\mathrm{S}/\mathrm{C}\mathrm{o}$ NPs were successfully synthesized via a wet chemical method and integrated at varying concentrations (1%wt, 3%wt, and 5%wt) to systematically investigate their influence on device performance. The optimal doping concentration of 3%wt yielded a remarkable power conversion efficiency (PCE) of 4.76%, representing a 102% enhancement over the pristine reference device (2.35%) under ambient laboratory conditions. The observed positive trend is attributed to the localized surface plasmon resonance (LSPR) effect and near-field optical enhancement induced by the presence of ZnS/Co NPs in the active layer, thereby increasing light-harvesting capability and exciton dissociation. Comprehensive morphological and optical characterizations using high-resolution scanning electron microscopy (HRSEM), high-resolution transmission electron microscopy (HRTEM), and spectroscopic techniques confirmed uniform nanoparticle dispersion, nanoscale crystallinity, and effective light absorption. These findings highlight the functional role of $\mathrm{Z}\mathrm{n}\mathrm{S}/\mathrm{C}\mathrm{o}$ NPs as dopants in enhancing TFOSC performance, providing valuable insights into optimizing nanoparticle concentration. This work offers a scalable and impactful strategy for advancing high-efficiency, flexible, and wearable organic photovoltaic devices. Full article

The operational stability of organic solar cells critically depends on the excited-state characteristics of electron acceptor materials. Through systematic quantum chemical calculations on four representative acceptors (PCBM, ITIC, Y6, and TBT-26), this study reveals fundamental spectra–stability relationships. Non-fullerene acceptors demonstrate superior light-harvesting with systematically tuned energy levels and significantly lower exciton binding energies (2.05–2.12 eV) compared to PCBM (2.97 eV), facilitating efficient charge separation. Structural dynamics analysis uncovers distinct stability mechanisms: ITIC maintains exceptional structural integrity (anionic RMSD = 0.023, S₁ RMSD = 0.134) with superior bond preservation, ensuring balanced performance–stability. Y6 exhibits substantial structural relaxation in excited states (S₁ RMSD = 0.307, T₁ RMSD = 0.262) despite its low exciton binding energy, indicating significant non-radiative losses. TBT-26 employs selective bond stabilization, preserving acceptor–proximal bonding despite considerable anionic flexibility. These findings establish that optimal molecular design requires both favorable electronic properties and structural preservation in photoactive states, providing crucial guidance for developing efficient and stable organic photovoltaics. Full article

Exciton generation and separation play an important role in the photoelectric properties and the luminescence performance of materials. In order to tailor the defects and grain boundaries and improve the exciton separation and light harvesting of the graphitic carbon nitride (g-C₃N₄) nanosheets, a C₃N₄/bismuth sulfide (Bi₂S₃) nanocomposite was synthesized. The photoelectric properties of the 405, 532, 650, 780, 808, 980 and 1064 nm light sources were studied using Au electrodes and graphite electrodes with 4B and 5B pencil drawings. The results indicate that the C₃N₄/Bi₂S₃ nanocomposite exhibited photocurrent switching behavior in the broadband light spectrum range. It is noted that even with zero bias applied, a good photoelectric signal was still measured. The resulting nanocomposite exhibited good photophysical stability. Physical mechanisms are discussed herein. It is suggested that the interfacial interaction of C₃N₄ and Bi₂S₃ in the nanocomposite creates a strong built-in electric field, which accelerates the separation of excitons. Therefore, as a dynamic process of photoexcitation, fluorescence, the photoelectric effect, and scattering are three main competing processes; the separation of excitons and the extraction of free photogenerated charge can be used as a reference for the fluorescent materials or other photoelectric materials studies as photophysical properties. This study also serves as an important reference for the design, defect and grain boundary modulation or interdisciplinary application of functional nanocomposites, especially for the bandgap modulation and suppression of photogenerated carrier recombination. Full article

Recent advances in electrochemiluminescence (ECL) leveraging thermally activated delayed fluorescence (TADF) have highlighted its potential for near-unity exciton harvesting. However, there are still very limited examples of TADF-ECL emitters. We present a rigid diboron-embedded multiple-resonance TADF emitter, which exhibits blue–green emission at 493 nm with a remarkably narrow bandwidth (FWHM = 22 nm) and minimized singlet-triplet energy gap (ΔE_ST = 0.2 eV), achieving a 67% photoluminescence quantum yield. DFT calculations confirm the short-range charge transfer, enabling narrowband emission. Co-reactant-dependent ECL shows that tripropylamine (TPrA) improves the ECL efficiency from 11% (annihilation) to 51%, while benzoyl peroxide (BPO) yields 1% due to poor radical stabilization. ECL spectra align with photoluminescence, confirming the singlet-state dominance without exciplex interference. TPrA enhances stable radical formation and energy transfer, whereas BPO induces non-radiative losses. These findings establish molecular rigidity and co-reactant selection as pivotal factors in developing high-performance TADF-ECL systems, providing fundamental guidelines for designing organic electrochemiluminescent materials with optimized exciton harvesting efficiency. Full article

Organic solar cells (OSCs) are made from carbon-rich organic compounds with low environmental impacts, unlike the silicon in traditional solar panels. Some of these organic materials can be broken down and reprocessed, enabling the recovery of valuable components. Specifically, the active-layer materials that make up OSCs can be designed with sustainability in mind. However, it is important to note that practical active materials that can be used for the commercialization of OSCs are still an area of research and development due to their low efficiency/stability and processability. Herein, we designed and synthesized three A-D-A’-D-A-type long-conjugated non-fullerene acceptors (NFAs) by incorporating various electron-withdrawing groups into the benzothiadiazole-diindacenodithiophene core. These NFAs, by changing their end-capping groups, exhibit not only distinct physical, optical, and electrochemical properties, but also differences in crystallinity and exciton dissociation. As a result, they exhibited significant differences in photovoltaic performance in PM6 donor-based binary devices. The introduction of small amounts of NFAs as a third component in the PM6:BTP-eC9 blend significantly enhanced its photon harvesting capabilities and influenced its charge transfer dynamics. Finally, we achieved a remarkable power conversion efficiency of nearly 17% by utilizing an eco-friendly solvent. This study provides valuable insights for the development of NFAs in efficient and eco-friendly OSCs. Full article

The Coulomb coupling between transition densities of the pigments in photosynthetic pigment-protein complexes, termed excitonic coupling, is a key factor for the description of optical spectra and energy transfer. A challenging question is the quantification of the screening of the excitonic coupling by the optical polarizability of the environment. We use the equivalence between the sophisticated quantum chemical polarizable continuum (PCM) model and the simple electrostatic Poisson-TrEsp approach to analyze the distance and orientation dependence of the dielectric screening between chlorophylls in photosystem I trimers. On the basis of these calculations we find that the vacuum couplings $V_{mn}^{\left(0\right)}$ and the couplings in the dielectric medium $V_{mn}=f_{mn}{V}_{mn}^{\left(0\right)}$ are related by the empirical screening factor $f_{mn}=0.60+39.6\theta \left(\right|{\kappa }_{mn}|-1.17)exp(-0.56R_{mn}/\AA )$, where ${\kappa }_{mn}$ is the usual orientational factor of the dipole-dipole coupling between the pigments, $R_{mn}$ is the center-to-center distance, and the Heaviside-function $\theta \left(\right|{\kappa }_{mn}|-1.17)$ ensures that the exponential distance dependence only contributes for in-line type dipole geometries. We are confident that the present expression can be applied also to other pigment-protein complexes with chlorophyll or related pigments of similar shape. The variance between the Poisson-TrEsp and the approximate coupling values is found to decrease by a factor of 8 and 3–4 using the present expression, instead of an exponential distance dependent or constant screening factor, respectively, assumed previously in the literature. Full article

A reaction center is a unique biological system that performs the initial charge separation within a Photosystem II (PSII) multiunit enzyme, which eventually drives the catalytic water-splitting in plants and algae. The possible role of quantum coherences coinciding with the energy and charge transfer processes in PSII reaction center is one of the active areas of research. Here, we study these quantum coherences by using a numerically exact method on an excitonic dimer model, including linear vibronic coupling and employing optimal parameters from experimental two-dimensional coherent spectroscopic measurements. This enables us to precisely capture the excitonic interaction between pigments and the dissipation of the energy from electronic and charge-transfer (CT) states to the protein environment. We employ the time nonlocal (TNL) quantum master equation to calculate the population dynamics, which yields numerically reliable results. The calculated results show that, due to the strong dissipation, the lifetime of electronic coherence is too short to have direct participation in the charge transfer processes. However, there are long-lived vibrational coherences present in the system at frequencies close to the excitionic energy gap. These are strongly coupled with the electronic coherences, which makes the detection of the electronic coherences with conventional techniques very challenging. Additionally, we unravel the strong excitonic interaction of radical pair ($P_{D1}$ and $P_{D2}$) in the reaction center, which results in a long-lived electronic coherence of >100 fs, even at room temperature. Our work provide important physical insight to the charge separation process in PSII reaction center, which may be helpful for better understanding of photophysical processes in other natural and artificial light-harvesting systems. Full article

We report on organoboron complexes characterized by very small energy gaps (ΔE_ST) between their singlet and triplet states, which allow for highly efficient harvesting of triplet excitons into singlet states for working as thermally activated delayed fluorescence (TADF) devices. Energy gaps ranging between 0.01 and 0.06 eV with dihedral angles of ca. 90° were registered. The spin–orbit couplings between the lowest excited S₁ and T₁ states yielded reversed intersystem crossing rate constants (K_RISC) of an average of 10⁵ s⁻¹. This setup accomplished radiative decay rates of ca. 10⁶ s⁻¹, indicating highly potent electroluminescent devices, and hence, being suitable for application as organic light-emitting diodes. Full article

Covalent organic frameworks (COFs) have unique features, including intrinsic porosity, crystallinity, and tunability, making them desirable materials for diverse applications ranging from environmental remediation to energy harvesting. Among these applications, COFs are extensively studied for their photocatalytic hydrogen evolution by converting solar energy into clean and renewable fuel via water splitting. COFs have several advantages over conventional inorganic catalysts, such as tunable band structures, high surface areas, and low cost. However, the research in this field is still in the early stages, and COFs still face some challenges, such as low charge carrier mobility, high exciton binding energy, and poor stability. To overcome these challenges, various design strategies relying on a mechanistic approach have been developed to design and modify COFs for enhanced photocatalytic performance. These include extending the π-conjugation, incorporating heteroatoms or metal complexes, and donor–acceptor (D–A) configuration, which ultimately improves the light absorption charge separation of COFs. Additionally, blending COFs with other functional materials, such as inorganic-organic semiconductors, can create synergistic effects to boost photocatalytic activity. In this review, the design aspects of the fabrication of COFs as effective photocatalysts have been reported. Full article

Triplet harvesting processes are essential for enhancing efficiencies of fluorescent organic light-emitting diodes. Besides more conventional thermally activated delayed fluorescence and triplet-triplet annihilation, the hot exciton mechanism has been recently noticed because it helps reduce the efficiency roll-off and improve device stability. Hot exciton materials enable the conversion of triplet excitons to singlet ones via reverse inter-system crossing from high-lying triplet states and thereby the depopulation of long-lived triplet excitons that are prone to chemical and/or efficiency degradation. Although their anti-Kasha characteristics have not been clearly explained, numerous molecules with behaviors assigned to the hot exciton mechanism have been reported. Indeed, the related developments appear to have just passed the stage of infancy now, and there will likely be more roles that computational elucidations can play. With this perspective in mind, we review some selected experimental studies on the mechanism and the related designs and then on computational studies. On the computational side, we examine what has been found and what is still missing with regard to properly understanding this interesting mechanism. We further discuss potential future points of computational interests toward aiming for eventually presenting in silico design guides. Full article

Frenkel excitons are responsible for the transport of light energy in many molecular systems. Coherent electron dynamics govern the initial stage of Frenkel-exciton transfer. Capability to follow coherent exciton dynamics in real time will help to reveal their actual contribution to the efficiency of light-harvesting. Attosecond X-ray pulses are the tool with the necessary temporal resolution to resolve pure electronic processes with atomic sensitivity. We describe how attosecond X-ray pulses can probe coherent electronic processes during Frenkel-exciton transport in molecular aggregates. We analyze time-resolved absorption cross section taking broad spectral bandwidth of an attosecond pulse into account. We demonstrate that attosecond X-ray absorption spectra can reveal delocalization degree of coherent exciton transfer dynamics. Full article

Surface morphologies, light harvesting abilities, crystal structures, and excitonic properties of the formamiminium lead triiodide (FAPbI₃) based alloy perovskite thin films were investigated by using the scanning electron microscopic images, absorbance spectra, X-ray diffraction patterns, photoluminescence (PL) spectra and time-resolved PL decaying curves. Our experimental results show that the fresh Cs_xFA_1−xPbI₃, Rb_xFA_1−xPbI₃, and FAPb(SCN_xI_1−x)₃ alloy thin films are a pure α-phase perovskite crystal, a α-phase: δ-phase mixed perovskite crystal, and a PbI₂ crystal/α-phase: δ-phase mixed perovskite crystal at room temperatures, respectively. Among the three FAPbI₃ based alloy perovskite solar cells, the Cs_xFA_1−xPbI₃ solar cells have the better photovoltaic responses. It is noted that the high photocurrent density is mainly due to the formation of cube-like surface morphology and the long carrier lifetime of 368 ns when the Cs_xFA_1−xPbI₃ alloy perovskite thin film is used as the light-absorbing layer. Our findings provide the relation between the properties of the FAPbI₃ based alloy perovskite thin films and the photovoltaic responses of the resultant solar cells. Full article

Thermally activated delayed fluorescence (TADF) materials, which can harvest all excitons and emit light without the use of noble metals, are an appealing class of functional materials emerging as next-generation organic electroluminescent materials. Triplet excitons can be upconverted to the singlet state with the aid of ambient thermal energy under the reverse inter-system crossing owing to the small singlet–triplet splitting energy (ΔE_ST). This results from a specific molecular design consisting of minimal overlap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital, due to the spatial separation of the electron-donating and electron-releasing part. When a well-designed device structure is applied, high-performance blue-emitting TADF organic light-emitting diodes can be realized with an appropriate molecular design. Unlike the previous literature that has reviewed general blue-emitting TADF materials, in this paper, we focus on materials other than pure organic molecules with twist D-π-A structures, including multi-resonance TADF, through-space charge transfer TADF, and metal-TADF materials. Cutting-edge molecules with extremely small and even negative ΔE_ST values are also introduced as candidates for next-generation TADF materials. In addition, OLED structures used to exploit the merits of the abovementioned TADF emitters are also described in this review. Full article