Xiaobo Shang

( RRRR )-diPDI-CyPh was designed and synthesized with favorable g _abs and preferred MM conformation. Its annealed thin films enabled dual-wavelength CPL detection ( g _ph = −0.31 at 455 nm and 0.22 at 530 nm) and multidimensional optical encryption.

Chiral small‐molecule organic semiconductors are attractive for circularly polarized light (CPL) detection owing to their tunable functionality and versatile processability. However, their intrinsic trade‐off between large dissymmetry factor and high carrier mobility ( μ ) hinders the application for high‐performance CPL detection. To overcome this issue, the chiral induction combined with the ring‐fusion strategy is employed to rationally construct a new n‐type chiral nanographene imide ( S )‐Cy‐FT‐FPDI. In the monomeric state, ( S )‐Cy‐FT‐FPDI exhibited distinct circular dichroism (CD) signals, with the maximum absorption dissymmetry factor ( g _abs ) reaching −2.16 × 10 ⁻³ . The ( S )‐Cy‐FT‐FPDI annealed thin films presented dual‐wavelength CPL responses at 455 and 595 nm, with photocurrent dissymmetry factors ( g _ph ) of 0.22 and 0.53, respectively, while delivering high μ of 0.57 cm ² V ⁻¹ s ⁻¹ , successfully balancing the favorable electrical performance and excellent chiroptical property. Remarkably, the achieved μ and g _ph outperform most of the previously reported chiral organic small‐molecule counterparts. Then, we have successfully demonstrated the high‐fidelity encoding and encryption based on ( S )‐Cy‐FT‐FPDI annealed thin films. Our work provides a feasible molecular design strategy for chiral organic small molecules with concurrent high g _ph and μ , balancing the dissymmetry factor‐mobility trade‐off towards high‐performance CPL detection.

Chiral small‐molecule organic semiconductors are attractive for circularly polarized light (CPL) detection owing to their tunable functionality and versatile processability. However, their intrinsic trade‐off between large dissymmetry factor and high carrier mobility ( μ ) hinders the application for high‐performance CPL detection. To overcome this issue, the chiral induction combined with the ring‐fusion strategy is employed to rationally construct a new n‐type chiral nanographene imide ( S )‐Cy‐FT‐FPDI. In the monomeric state, ( S )‐Cy‐FT‐FPDI exhibited distinct circular dichroism (CD) signals, with the maximum absorption dissymmetry factor ( g _abs ) reaching −2.16 × 10 ⁻³ . The ( S )‐Cy‐FT‐FPDI annealed thin films presented dual‐wavelength CPL responses at 455 and 595 nm, with photocurrent dissymmetry factors ( g _ph ) of 0.22 and 0.53, respectively, while delivering high μ of 0.57 cm ² V ⁻¹ s ⁻¹ , successfully balancing the favorable electrical performance and excellent chiroptical property. Remarkably, the achieved μ and g _ph outperform most of the previously reported chiral organic small‐molecule counterparts. Then, we have successfully demonstrated the high‐fidelity encoding and encryption based on ( S )‐Cy‐FT‐FPDI annealed thin films. Our work provides a feasible molecular design strategy for chiral organic small molecules with concurrent high g _ph and μ , balancing the dissymmetry factor‐mobility trade‐off towards high‐performance CPL detection.

Reliable recognition of complex scenes remains challenging because physically distinct objects can exhibit similar appearances in conventional intensity images, while dynamically changing environments require continuous temporal information processing. Although circularly polarized light (CPL) provides an additional optical dimension for distinguishing surface reflection properties, integrating efficient polarization perception with multi‐timescale synaptic plasticity in a single material platform remains difficult because these functionalities require fundamentally different carrier dynamics. Here, we demonstrate that donor–acceptor composition engineering in chiral bulk‐heterojunction diodes enables programmable carrier dynamics across multiple timescales. By regulating the balance between carrier transport and trapping, the devices evolve from volatile through quasi‐nonvolatile to nonvolatile synaptic plasticity while preserving efficient CPL photodetection. The optimized composition delivers a photocurrent dissymmetry factor of −0.026, whereas complementary volatile and nonvolatile devices enable cooperative temporal information processing. As a proof of concept, a polarization neuromorphic vision system combining RGB–CPL multidimensional perception and multi‐timescale memory improves static recognition accuracy by 15% and dynamic recognition accuracy by up to 12% compared with conventional systems. This work establishes donor–acceptor composition engineering as a strategy for coordinating optical perception and temporal computation, opening opportunities for polarization‐aware neuromorphic vision and intelligent optoelectronics.

Ultraviolet circularly polarized light (UV‐CPL) has significant applications in chiral optoelectronics however its sensitive detection is hindered by the challenge of designing wide‐bandgap chiral organic semiconductors. Herein, we synthesized two diastereomeric benzo[ ghi ]perylenetriimides (( S,S,S )/( S,S,R )‐BPTI‐Ph) and assembled them into ordered microwire arrays. ( S,S,S )‐BPTI‐Ph microwire arrays show higher absorption dissymmetry factor ( g _abs = 2.3 × 10 ⁻³ ) than ( S,S,R )‐BPTI‐Ph microwire arrays ( g _abs = 1.3 × 10 ⁻³ ) at 365 nm. Theoretical calculations revealed this enhancement originates from the optimized angle between electric and magnetic transition dipole moments. The organic phototransistors based on ( S,S,S )‐BPTI‐Ph microwire arrays achieved high photocurrent dissymmetry factor ( g _ph = 0.46), which was higher than that of ( S,S,R )‐BPTI‐Ph ( g _ph = 0.16), representing one of the highest values among the reported UV‐CPL detectors. Furthermore, a 50 × 50 pixel high‐resolution UV‐CPL star pattern imaging was demonstrated based on the favorable CPL detecting properties of ( S,S,S )‐BPTI‐Ph microwire arrays. This work provides a rational design strategy for chiral organic materials with high‐performance UV‐CPL detection via diastereomeric effect.

Chiral perylene diimides (PDIs) are promising candidates for circularly polarized light (CPL) detection due to their intrinsic chirality, outstanding photothermal stability and tunable molecular structures. However, the photocurrent dissymmetry factor ( g _ph ) of CPL photodetectors based on chiral PDIs remains relatively low, limiting their applications in advanced chiral optoelectronics. In this work, two constitutional isomers of PDIs, ( S,S )‐BPTI‐ L ‐Ile and ( S,S )‐BPTI‐ L ‐Leu, were synthesized and self‐assembled into microcrystal arrays. ( S,S )‐BPTI‐ L ‐Ile microcrystal arrays had 7.1 × 10 ⁻³ absorption dissymmetry factor ( g _abs ), 2.4 times that of ( S,S )‐BPTI‐ L ‐Leu microcrystal arrays ( g _abs = 2.9 × 10 ⁻³ ). Theoretical calculations indicated that this difference originated from the distinct angle between the electric and magnetic transition dipole moments in the two microcrystal arrays. Meanwhile, the corresponding ( S,S )‐BPTI‐ L ‐Ile microcrystal arrays achieved record‐high g _ph of 0.84 among chiral PDIs, which is consistent with higher spin polarization of 61%, nearly twice that of the ( S,S )‐BPTI‐ L ‐Leu microcrystal arrays (31%). Benefiting from its outstanding CPL detection capability and intrinsic device‐to‐device variability, ( S,S )‐BPTI‐ L ‐Ile microcrystal arrays were further applied to construct physical unclonable functions (PUFs) for secure information encryption. This work demonstrates the crucial role of constitutional isomers in regulating molecular packing, enhancing the detection capability of CPL, and highlights their potential for information security applications.

Circularly polarized light (CPL) photodetectors are of great interest for applications in polarization imaging, information encryption, and optical communication. Chiral organic small molecules have emerged as attractive active materials due to their structural tunability, well‐defined intrinsic chirality, and solution processability. However, in most chiral organic small molecule systems, molecular‐scale effects and optical selection rules lead to mismatch in magnitude and spatial orientation between the magnetic and electric transition dipole moments, resulting in low absorption dissymmetry factors ( g _abs ) and poor compatibility between chiroptical response and charge transport. This review summarizes the recent progress in chiral organic small molecules for CPL detection from the perspective of group theory. By comparing the representative chiral point groups such as C ₁ , C _n , and D _n , we elucidate how point group symmetry imposes constraints on the relative arrangement of transition dipole moments, thereby governing the molecular g _abs . In particular, the D ₂ point group can enforce both electric and magnetic transition dipole alignment along the principal molecular axes, yielding an optimal orientation (0° or 180°) and thus enabling the high g _abs . Recent advances in chiral organic small molecules D ₂ point group demonstrate their potential to simultaneously achieve strong chiroptical responses and efficient charge transport, offering a clear structural guideline for the rational design of high‐performance CPL photodetectors based on chiral organic small molecules. image

Chiral π‐conjugated organic small molecules, due to their intrinsic chirality, well‐defined molecular structures and ease of modification, are promising for circularly polarized light (CPL) detection. However, their practical application is hindered by low absorption dissymmetry factor ( g _abs ), arising from imbalanced electric and magnetic transition dipole moments ( µ and m ). Here, a template‐free method using chiral memory effect was reported to fabricate helical supramolecules with high g _abs . Two chiral dinaphthocoronene tetraimides enantiomer pairs were synthesized: ( R )‐PDI‐( R )‐NI‐Ph/( S )‐PDI‐( S )‐NI‐Ph and ( S )‐PDI‐( R )‐NI‐Ph/( R )‐PDI‐( S )‐NI‐Ph. After annealing films at 350°C to remove chiral pendants, ( R )‐PDI‐( R )‐NI/( S )‐PDI‐( S )‐NI films showed much higher | g _abs | (0.08) than the other set (0.01), with helical assemblies formed via chiral memory effect. Notably, large‐area arrays of ( R )‐PDI‐( R )‐NI films enabled CPL imaging, and a bionic artificial visual system was constructed with this film as “retina” and an artificial neural network as “neural center” for reliable CPL discrimination, offering a scalable strategy for high‐performance chiral optoelectronics.

Continuous, smooth chiral polymer films fabricated by a kinetically controlled dip-coating method achieve high-performance circularly polarized light detection, demonstrating binary logic information encoding and decoding.