Impact of Packing Geometry on Excimer Characteristics and Mobility in Perylene Bisimide Polycrystalline Films.

Efficient exciton transport is essential for high-performance optoelectronics. Considerable efforts have been focused on improving the exciton mobility in organic materials. While it is feasible to improve mobility in organic systems by forming well-ordered stacks, the formation of trap states, particularly the lower-lying states referred to as excimers, remains a significant challenge to enhancing mobility. The mobility of excimer excitons intricately depends on the strength of excitonic coupling in terms of Förster-type diffusive exciton transfer processes. Given that the formation and mobility of excimer excitons are highly sensitive to molecular arrangements (packing geometries), conducting comprehensive investigations into the structure-property relationship in organic systems is crucial. In this study, we prepared three types of polycrystalline films of perylene bisimide (PBI) by varying substituents at the imide and bay positions, which allowed us to tailor the properties of excimer excitons and their mobility based on packing geometries and excitonic coupling strengths. By utilizing femtosecond transient absorption spectroscopy, we observed ultrafast excimer formation in the higher coupling regime, while in the lower coupling regime, the transition from Frenkel to excimer excitons occurs with a time constant of 500 fs. Under high pump-fluence, exciton-exciton annihilation processes occur, indicating the diffusion of excimer excitons. Intriguingly, employing a three-dimensional diffusion model, we derived a diffusion constant that is 3000 times greater in the high coupling regime than in the low coupling regime. To investigate the optoelectronic properties in the form of a bulk system, we fabricated n-type organic field effect transistors and obtained 8000 times higher mobility in the high coupling regime. Furthermore, photocurrent measurements enable us to investigate the charge carrier transport by mobile excimer excitons, suggesting a 230-fold improvement in external quantum efficiency with tightly packing PBI molecules compared to the low coupling regime. These findings not only offer valuable insights into optimizing organic materials for optoelectronic devices but also unveil the intriguing potential of exciton migration within excimers.

Axially Chiral Organic Semiconductors for Visible-Blind UV-Selective Circularly Polarized Light Detection.

Technologies that detect circularly polarized light (CPL), particularly in the UV region, have significant potential for various applications, including bioimaging and optical communication. However, a major challenge in directly sensing CPL arises from the conflicting requirements of planar structures for efficient charge transport and distorted structures for effective interaction with CPL. Here, a novel design of an axially chiral n-type organic semiconductor is presented to surmount the challenge, in which a binaphthyl group results in a high dissymmetry factor at the molecular level, while maintaining excellent electron-transporting characteristics through the naphthalene diimide group. Experimental and computational methods reveal different stacking behaviors in homochiral and heterochiral assemblies, yielding different structures: Nanowires and nanoparticles, respectively. Especially, the homochiral assemblies exhibit effective π-π stacking between naphthalene diimides despite axial chirality. Thus, phototransistors fabricated using enantiomers exhibit a high maximum electron mobility of 0.22 cm2 V-1 s-1 and a detectivity of 3.9 × 1012 Jones, alongside the CPL distinguishing ability with a dissymmetry factor of responsivity of 0.05. Furthermore, the material possesses a wide bandgap, contributing to its excellent visible-blind UV-selective detection. These findings highlight the new strategy for compact CPL detectors, coupled with the demonstration of less-explored n-type and UV region phototransistors.

Organic Mixed Ionic-Electronic Conductors for Bioelectronic Sensors: Materials and Operation Mechanisms.

The field of organic mixed ionic-electronic conductors (OMIECs) has gained significant attention due to their ability to transport both electrons and ions, making them promising candidates for various applications. Initially focused on inorganic materials, the exploration of mixed conduction has expanded to organic materials, especially polymers, owing to their advantages such as solution processability, flexibility, and property tunability. OMIECs, particularly in the form of polymers, possess both electronic and ionic transport functionalities. This review provides an overview of OMIECs in various aspects covering mechanisms of charge transport including electronic transport, ionic transport, and ionic-electronic coupling, as well as conducting/semiconducting conjugated polymers and their applications in organic bioelectronics, including (multi)sensors, neuromorphic devices, and electrochromic devices. OMIECs show promise in organic bioelectronics due to their compatibility with biological systems and the ability to modulate electronic conduction and ionic transport, resembling the principles of biological systems. Organic electrochemical transistors (OECTs) based on OMIECs offer significant potential for bioelectronic applications, responding to external stimuli through modulation of ionic transport. An in-depth review of recent research achievements in organic bioelectronic applications using OMIECs, categorized based on physical and chemical stimuli as well as neuromorphic devices and circuit applications, is presented.

Hierarchically manufactured chiral plasmonic nanostructures with gigantic chirality for polarized emission and information encryption.

Chiral metamaterials have received significant attention due to their strong chiroptical interactions with electromagnetic waves of incident light. However, the fabrication of large-area, hierarchically manufactured chiral plasmonic structures with high dissymmetry factors (g-factors) over a wide spectral range remains the key barrier to practical applications. Here we report a facile yet efficient method to fabricate hierarchical chiral nanostructures over a large area (>11.7 × 11.7 cm2) and with high g-factors (up to 0.07 in the visible region) by imparting extrinsic chirality to nanostructured polymer substrates through the simple exertion of mechanical force. We also demonstrate the application of our approach in the polarized emission of quantum dots and information encryption, including chiral quick response codes and anti-counterfeiting. This study thus paves the way for the rational design and fabrication of large-area chiral nanostructures and for their application in quantum communications and security-enhanced optical communications.

Helical polymers for dissymmetric circularly polarized light imaging.

Control of the spin angular momentum (SAM) carried in a photon provides a technologically attractive element for next-generation quantum networks and spintronics1-5. However, the weak optical activity and inhomogeneity of thin films from chiral molecular crystals result in high noise and uncertainty in SAM detection. Brittleness of thin molecular crystals represents a further problem for device integration and practical realization of chiroptical quantum devices6-10. Despite considerable successes with highly dissymmetric optical materials based on chiral nanostructures11-13, the problem of integration of nanochiral materials with optical device platforms remains acute14-16. Here we report a simple yet powerful method to fabricate chiroptical flexible layers via supramolecular helical ordering of conjugated polymer chains. Their multiscale chirality and optical activity can be varied across the broad spectral range by chiral templating with volatile enantiomers. After template removal, chromophores remain stacked in one-dimensional helical nanofibrils producing a homogeneous chiroptical layer with drastically enhanced polarization-dependent absorbance, leading to well-resolved detection and visualization of SAM. This study provides a direct path to scalable realization of on-chip detection of the spin degree of freedom of photons necessary for encoded quantum information processing and high-resolution polarization imaging.

Ultrasensitive Near-Infrared Circularly Polarized Light Detection Using 3D Perovskite Embedded with Chiral Plasmonic Nanoparticles.

Chiral organic ligand-incorporated low-dimensional metal-halide perovskites have received increasing attention for next-generation photodetectors because of the direct detection capability of circularly polarized light (CPL), which overcomes the requirement for subsidiary optical components in conventional CPL photodetectors. However, most chiral perovskites have been based on low-dimensional structures that confine chiroptical responses to the ultraviolet (UV) or short-wavelength visible region and limit photocurrent due to their wide bandgap and poor charge transport. Here, chiroptical properties of 3D Cs0.05 FA0.5 MA0.45 Pb0.5 Sn0.5 I3 polycrystalline films are achieved by incorporating chiral plasmonic gold nanoparticles (AuNPs) into the mixed PbSn perovskite, without sacrificing its original optoelectronic properties. CPL detectors fabricated using chiral AuNP-embedded perovskite films can operate without external power input; they exhibit remarkable chirality in the near-infrared (NIR) region with a high anisotropy factor of responsivity (gres ) of 0.55, via giant plasmon resonance shift of chiral plasmonic AuNPs. In addition, a CPL detector array fabricated on a plastic substrate demonstrates highly sensitive self-powered NIR detection with superior flexibility and durability.

Boosting the Optoelectronic Properties of Molybdenum Diselenide by Combining Phase Transition Engineering with Organic Cationic Dye Doping.

Two-dimensional layered transition metal dichalcogenides (TMDs) have been investigated intensively as next-generation semiconducting materials. However, conventional TMD-based devices exhibit large contact resistance at the interface between the TMD and the metal electrode because of Fermi level pinning and the Schottky barrier, which results in poor charge injection. Here, we present enhanced charge transport characteristics in molybdenum diselenide (MoSe2) by means of a sequential engineering process called PESOD-2H/1T (i.e., phase transition engineering combined with surface transfer organic cationic dye doping; 2H and 1T represent the trigonal prismatic and octahedral phases, respectively). Substantial improvements are observed in PESOD-processed MoSe2 phototransistors, specifically, an approximately 40 000-fold increase in effective carrier mobility and a 100 000-fold increase in photoresponsivity, compared with the mobility and photoresponsivity of intact MoSe2 phototransistors. Moreover, the PESOD-processed MoSe2 phototransistor on a flexible substrate maintains its optoelectronic properties under tensile stress, with a bending radius of 5 mm.

Effects of the Polarity and Bulkiness of End-Functionalized Side Chains on the Charge Transport of Dicyanovinyl-End-Capped Diketopyrrolopyrrole-Based n-Type Small Molecules.

When designing organic semiconductors, side-chain engineering is as important as modifying the conjugated backbone, which has a significant impact on molecular ordering, morphology, and thus electronic device performance. We have developed three dicyanovinyl-end-capped donor-acceptor diketopyrrolopyrrole-based n-type small molecules (C2C9CN, SiC4CN, and EH4PCN) bearing an identical length of alkyl spacer yet different end-functionalized side chains (i.e., alkyl-, siloxane-, and phosphonate-end pendants). The effects of the end-functionalized side chains on the intrinsic molecular properties, microstructure, and charge transport of the small-molecule series were investigated. In comparison with the alkyl-end side chains, incorporating siloxane-end side chains into the backbone facilitates 2D edge-on oriented high intergrain connectivity/crystallinity and compatibility with the substrate surface, whereas the phosphonate-end analogues have an adverse effect on the film-forming quality due to high polarity. Thereby, an organic field-effect transistor fabricated by SiC4CN shows the best electron mobility up to 1.59 × 10-1 cm2 V-1 s-1 along with a high current on/off ratio >105. This study contributes to our understanding of the role of the end-functionalized side chains (e.g., the effects of polarity and bulkiness of the end groups) for the development of high-performance semiconductors.

A Hippocampus-Inspired Dual-Gated Organic Artificial Synapse for Simultaneous Sensing of a Neurotransmitter and Light.

Organic neuromorphic devices and sensors that mimic the functions of chemical synapses and sensory perception in humans have received much attention for next-generation computing and integrated logic circuits. Despite recent advances, organic artificial synapses capable of detecting both neurotransmitters in liquid environments and light are not reported. Herein, inspired by hippocampal synapses, a dual-gate organic synaptic transistor platform with a photoconductive polymer semiconductor, a ferroelectric insulator of P(VDF-TrFE), and an extended-gate electrode functionalized with boronic acid is developed to simultaneously detect the neurotransmitter dopamine and light. The developed synaptic transistor enables memory consolidation upon repetitive exposure to dopamine and polychromatic light, exhibiting effectively modulated postsynaptic currents. This proof-of-concept hippocampal-synapse-mimetic organic neuromorphic system combining a chemical sensor and a photosensor opens new possibilities for developing low-power organic artificial synaptic multisensors and light-induced memory consolidative artificial synapses, and can also contribute to the development of human-machine interfaces.

Bay-Substitution Effect of Perylene Diimides on Supramolecular Chirality and Optoelectronic Properties of Their Self-Assembled Nanostructures.

One-dimensional (1D) organic chiral supramolecules have received a great deal of attention for their promising applications in chiral recognition systems, chemical sensors, catalysts, and optoelectronics. Compared to modifications at the imide position of a perylene diimide (PDI), few studies have explored bay substitution of chiral PDIs and their self-assemblies into 1D nanomaterials. Herein, we describe the synthesis of three bay-substituted PDIs and explore the effects of bay substitution on supramolecular chirality by examining circular dichroism spectra and the optoelectronic performance of chiral PDI nanomaterials in phototransistors. Among the three fabricated self-assemblies, nanomaterials based on (R)-CN-CPDI-Ph exhibited the highest electron mobility of 0.17 cm2 V-1 s-1, a low threshold voltage of -1 V, and enhanced optoelectronic performance. For example, the photoresponsivity and external quantum efficiency of (R)-CN-CPDI-Ph assemblies were 4-fold higher than those of (R)-2Br-CPDI-Ph and (R)-2F-CPDI-Ph. All three nanomaterials exhibited fast switching speeds compared with previously reported N-substituted PDIs, suggesting that bay substitution can be an effective means of achieving rapid photoswitching. A comprehensive study using density functional theory calculations and crystal analyses revealed that the enhanced optoelectronic performance of (R)-CN-CPDI-Ph nanomaterials is related to the substitution of CN at the bay position of PDI. This minor change provides simultaneous improvements in electron injectability and structural order. Our findings demonstrate that bay substitution can significantly impact the self-assembly, supramolecular chirality, and optoelectronic properties of PDI nanomaterials.

π-Extended perylene diimide double-heterohelicenes as ambipolar organic semiconductors for broadband circularly polarized light detection.

Despite great challenges, the development of new molecular structures with multiple and even conflicting characteristics are eagerly pursued for exploring advanced applications. To develop high-performance chiral organic semiconducting molecules, a distorted π-system is required for strong coupling with circularly polarized light (CPL), whereas planar π-stacking systems are necessary for high charge-carrier mobility. To address this dilemma, in this work, we introduce a skeleton merging approach through distortion of a perylene diimide (PDI) core with four fused heteroaromatics to form an ortho-π-extended PDI double-[7]heterohelicene. PDI double helicene inherits a high dissymmetry factor from the helicene skeleton, and the extended π-planar system concurrently maintains a high level of charge transport properties. In addition, ortho-π-extension of the PDI skeleton brings about near-infrared (NIR) light absorption and ambipolar charge transport abilities, endowing the corresponding organic phototransistors with high photoresponsivity of 450 and 120 mA W-1 in p- and n-type modes respectively, along with a high external quantum efficiency (89%) under NIR light irradiations. Remarkably, these multiple characteristics enable high-performance broadband CPL detections up to NIR spectral region with chiral organic semiconductors.

Fused Aromatic Network with Exceptionally High Carrier Mobility.

Recently, studies of 2D organic layered materials with unique electronic properties have generated considerable interest in the research community. However, the development of organic materials with functional electrical transport properties is still needed. Here, a 2D fused aromatic network (FAN) structure with a C5 N basal plane stoichiometry is designed and synthesized, and thin films are cast from C5 N solution onto silicon dioxide substrates. Then field-effect transistors are fabricated using C5 N thin flakes as the active layer in a bottom-gate top-contact configuration to characterize their electrical properties. The C5 N thin flakes, isolated by polydimethylsiloxane stamping, exhibit ambipolar charge transport and extraordinarily high electron (996 cm2 V-1 s-1 ) and hole (501 cm2 V-1 s-1 ) mobilities, surpassing the performance of most pristine organic materials without doping. These results demonstrate their vast potential for applications in thin-film optoelectronic devices.

Surface-Doped Quasi-2D Chiral Organic Single Crystals for Chiroptical Sensing.

Chiral organic optoelectronics using circularly polarized light (CPL) as the key element in the photonic signal has recently emerged as a next-generation photonic technology. However, it remains challenging to simultaneously achieve high polarization selectivity and superior optoelectronic performance. Supramolecular two-dimensional (2D) chiral organic single crystals may be good candidates for this purpose due to their defect-free nature, molecular diversity, and morphologies. Here, quasi-2D single crystals of chiral perylene diimides with parallelogram and triangle/hexagon morphologies have been selectively fabricated via self-assembly using different cosolvent systems. These materials exhibit amplified circular dichroism (CD) spectral signals, due to their molecular packing modes and supramolecular chirality. Through molecular surface n-doping using hydrazine, chiral single crystals exhibit electron mobility surpassing 1.0 cm2 V-1 s-1, which is one of the highest among chiral organic semiconductors, and excellent optoelectronic functions. Theoretical calculations reveal that the radical anions formed by n-doping increase the electron affinity and/or reduce the energy gap, thus facilitating electron transport. More importantly, the doped organic chiral crystals selectively discriminate CPL handedness with a high anisotropy factor of photoresponsivity (∼0.12). These results demonstrate that surface-doped quasi-2D chiral organic single crystals are highly promising for chiral optoelectronics.

Optoelectronic Property Modulation in Chiral Organic Semiconductor/Polymer Blends.

Organic phototransistors (OPTs) have been widely used in biomedical sensing, optical communications, and imaging. Charge-trapping effect has been utilized as an effective strategy for enhancing their photoresponsivity by effectively decreasing the dark current. The combination of organic semiconductors (OSCs), especially chiral OSCs, with insulating polymers has rarely been carried out for optoelectronic applications. Here, we fabricated OPTs containing both enantiopure and racemic air-stable n-type perylene diimide derivatives, CPDI-CN2-C6, and insulating biopolymer polylactide (PLA) and evaluated their photoresponsive properties. The PLA-blended systems exhibited greatly enhanced optoelectronic performances owing to the intense charge-trapping effect. Interestingly, the racemic system showed 3 times higher electron mobility and 12 times higher specific detectivity (1.3 × 1013 jones) compared with the enantiopure systems due to the more aggregated morphologies and larger grains, indicating that chiral composition can be used as a tuning parameter in optoelectronic devices. Our systematic study provides a feasible and effective method for producing high-performance n-type OPTs under ambient conditions.

Perovskite Granular Wire Photodetectors with Ultrahigh Photodetectivity.

Control over the morphology and crystallinity of metal halide perovskite materials is of key importance to enable high-performance optoelectronics. Here, a simple yet effective template-free self-assembly synthesis of perovskite granular wires with ultrahigh photodetectivity (3.17 × 1015 Jones) is reported. The 1D self-assembly of perovskite grains is driven by differences in the surface interaction energies of the granular facets. The superb photodetecting performance originates from extremely low dark current engendered by energetic barriers featuring unique band-edge modulation along the long axis of wire. Flexible photodetector arrays, fabricated by selectively placing perovskite granular wires onto pre-patterned electrode arrays on a transparent polymer substrate, show independently addressable photonic signal mapping with remarkably high detectivity, photoconductive gain, and responsivity. The "self-assembled nanograin engineering" strategy developed in this study provides a viable method for the development of high-performance perovskite photodetectors and can be extended to other integrated optoelectronic systems.

Understanding of Fluorination Dependence on Electron Mobility and Stability of Naphthalenediimide-Based Polymer Transistors in Environment with 100% Relative Humidity.

A family of copolymers (P(NDIOD-T2Fx)) based on naphthalenediimide (NDI) and 2,2'-bithiophene (T2) units with different amounts of 3,3'-difluoro-2,2'-bithiophene (T2F) decoration were synthesized, characterized, and used in n-type organic field-effect transistors (OFETs). With increasing T2F content in the backbone, we observe increased melting and crystallization transitions, blue-shifted absorptions, and deeper-lying highest occupied molecular orbital (HOMO)/lowest unoccupied molecular orbital (LUMO) levels, together with improved hydrophobicity. The highest electron mobility of 4.48 × 10-1 cm2 V-1 s-1 was obtained for P(NDIOD-T2F0) without a T2F unit, which is attributed to the larger domain grains and crystallites, as well as a more tightly packed and oriented crystalline structure, as evidenced from the morphological study. In contrast, P(NDIOD-T2F100) with the highest T2F content has superior air stability, showing greater than 25% electron mobility retention after 30 days in wet conditions of 100% relative humidity without encapsulation. Even P(NDIOD-T2F100) is able to operate normally after 30 min of immersion in water, which is due to the synergistic contributions from the deep HOMO/LUMO levels and improved hydrophobicity. This study advances our fundamental understanding of how the morphology/crystallinity, device performance, and device stability of n-type copolymers are tuned by incorporating different concentrations of T2F in the backbone, shedding light on an important modification for air- and water-stable n-type materials for future OFET applications.

High-Performance Hybrid Photovoltaics with Efficient Interfacial Contacts between Vertically Aligned ZnO Nanowire Arrays and Organic Semiconductors.

Hybrid photovoltaics (HPVs) incorporating both organic and inorganic semiconducting materials have attracted much attention as next-generation photovoltaics because of their advantage of combining both materials. The hybridization of ZnO nanowires (NWs) and organic semiconductors is expected to be a suitable approach to overcome the limited exciton diffusion length and low electron mobility associated with current organic photovoltaics. The use of ZnO NWs allows researchers to tune nanoscale dimensions more precisely and to achieve rod-to-rod spacing below 10 nm. However, the perfect incorporation of organic semiconductors into densely packed ZnO NW arrays has yet to be achieved. In this study, we report the fabrication of ZnO NW arrays and various organic heterojunction-based HPVs using the feasible and effective vacuum-assisted double coating (VADC) method, achieving full coverage of the organic semiconductors on the compact ZnO NW arrays. The newly proposed VADC method ensures perfect infiltration and full coverage of the organic semiconductors on the densely packed NW arrays. Compared with the conventional single spin-coating process, the use of the VADC method led to 11 and 14% increases in the power conversion efficiency of P3HT:PCBM- and PBDTTT-C-T:PC71BM-based HPVs, respectively. Our studies provide a feasible method for the fabrication of efficient HPVs.

Stretchable and Self-Healable Conductive Hydrogels for Wearable Multimodal Touch Sensors with Thermoresponsive Behavior.

Multifunctional hydrogels with properties including transparency, flexibility, self-healing, and high electrical conductivity have attracted great attention for their potential application to soft electronic devices. The presence of an ionic species can make hydrogels conductive in nature. However, the conductivity of hydrogels is often influenced by temperature, due to the change of the internal nano/microscopic structure when temperature reaches the sol-gel phase transition temperature. In this regard, by introducing a novel surface-capacitive sensor device based on polymers with lower critical solution temperature (LCST) behavior, near-perfect stimulus discriminability of touch and temperature may be realized. Here, we demonstrate a multimodal sensor that can monitor the location of touch points and temperature simultaneously, using poly(N-isopropylacrylamide) (PNIPAAm) in hybrid poly(vinyl alcohol) (PVA) and sodium tetraborate decahydrate cross-linked hydrogels doped with poly(sodium acrylate) (SA) [w/w/w = 5:2.7:1-3]. This multimodal sensor exhibits a response time of 0.3 s and a temperature coefficient of resistance of -0.58% K-1 from 20 to 40 °C. In addition, the LCST behavior of PNIPAAm-incorporated PVA/SA gels is investigated. Incorporation of LCST polymers into high-end hydrogel systems may contribute to the development of temperature-dependent soft electronics that can be applied in smart windows.

Heterochiral Doped Supramolecular Coordination Networks for High-Performance Optoelectronics.

Chiral self-sorting has great potential for constructing new complex structures and determining chirality-dependent properties in multicomponent mixtures. However, it is still of great challenge to achieve high fidelity chiral self-discrimination. Besides, the researches on the coordination polymers or metal-organic frameworks for micro/nanooptoelectronics are still rare due to their low conductivity and difficulty in developing a rapid and simple scale-up synthetic method. Here, heterochiral supramolecular coordination networks (SCNs) were synthesized by the solvothermal reaction of naphthalene diimide enantiomers and cadmium iodide, using the chirality as a synthetic tuning parameter to control the morphologies. Intriguingly, heterochiral micro/nanocrystals exhibited photochromic and photodetecting properties. Furthermore, we also developed a simple and efficient doping method to enhance the conductivity and photoresponsivity of micro/nanocrystals using hydrazine. From experimental and theoretical studies, the mechanism was suggested as follows: the radicals in the singly occupied molecular orbital level of the ligands provide charge carriers that can undergo "through-space" transport between π-π stacked ligands and the electron transfer from adsorbed hydrazine to the SCNs results in reduction of energy gap, leading to increased conductivity. Our findings demonstrate a simple and powerful strategy for implementing coordination networks with redox ligands for micro/nanooptoelectronic applications.

Amplified circularly polarized phosphorescence from co-assemblies of platinum(ii) complexes.

Molecules capable of producing zero-field circularly polarized phosphorescence (CPP) are highly valuable for chiroptoelectronic applications that rely on triplet exciton. However, the paucity of tractable molecular design rules for obtaining CPP emission has inhibited full utilization. We report amplification of CPP by the formation of helical co-assemblies consisting of achiral square planar cycloplatinated complexes and small fractions of homochiral cycloplatinated complexes. The latter has a unique Pfeiffer effect during the formation of superhelical co-assemblies, enabling versatile chiroptical control. Large dissymmetry factors in electronic absorption (g abs, 0.020) and phosphorescence emission (g lum, 0.064) are observed from the co-assemblies. These values are two orders of magnitude improved relative to those of individual molecules. In addition, photoluminescence quantum yields (PLQY) also increase by a factor of ten. Our structural, photophysical, and quantum chemical investigations reveal that the chiroptical amplification is attributable to utilization of both the magnetically allowed electronic transition and asymmetric coupling of excitons. The strategy overcomes the trade-off between g lum and PLQY which has frequently been found for previous molecular emitters of circularly polarized luminescence. It is anticipated that our study will provide new insight into the future research for the exploitation of the full potential of CPP.