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Artificial systems for sequential chirality transmission/amplification and energy relay are perpetual topics that entail learning from nature. However, engineering chiral light-harvesting supramolecular systems remains a challenge. Here, we developed new chiral light-harvesting systems with a sequential Förster resonance energy transfer process where a designed blue-violet-emitting BINOL (1,1'-Bi-2-naphthol) compound, BINOL-di-octadecylamide (BDA), functions as an initiator of chirality and light absorbance, a new green-emitting hexagonal tetraphenylethene-based macrocycle (TPEM) with aggregation-induced emission serves as a conveyor, and Nile red (NiR) or/and a near-infrared dye, tetraphenylethene (TPE)-based benzoselenodiazole (TPESe), are the terminal acceptors. Benefiting from the close contact and large optical overlap between donors and acceptors at each level, triad and tetrad relaying systems sequentially and efficiently furnish chirality transmission/amplification and energy transfer along the cascaded line BDA-TPEM-NiR (or/and TPESe), leading to bright customized-color circularly polarized luminescence (CPL) and bright white-light-emitting CPL (CIE coordinates: 0.33, 0.34) with an amplified dissymmetry factor () of 3.5 × 10 over a wide wavelength range. This work provides a new direction for the construction of chiral light-harvesting systems for a broad range of applications in chiroptical physics and chemistry.
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http://dx.doi.org/10.1021/jacs.1c12767 | DOI Listing |
ACS Omega
August 2025
Graduate School of Engineering, Chiba University, 1-33 Yayoi-cho, Inage-ku, Chiba 263-8522, Japan.
The optical vortex laser-induced forward transfer (OV-LIFT) technique enables the direct print of well-aligned dots with high spatial resolution and high positional accuracy. In this work, we demonstrate the direct printing of a 2-dimensional biomaterial (cyanobacteria cells) dot array using the OV-LIFT technique. The number of bacteria and size of the printed dots were controlled by simply adjusting the thickness of the donor film and the numerical aperture (NA) of focusing optics.
View Article and Find Full Text PDFNat Commun
July 2025
State Key Laboratory of Precision and Intelligent Chemistry, Department of Polymer Science and Engineering, University of Science and Technology of China, Hefei, Anhui, China.
The simultaneous transfer of chirality and energy is essential in biological systems, serving as a key inspiration for developing artificial analogs. Traditional methods, such as doping donor-acceptor chromophores into chiral gels or films, exhibit low chirality transfer efficiency due to inadequate stereo-communication. Here we present a bio-inspired strategy modeled on the chlorosomes of green bacteria.
View Article and Find Full Text PDFNanoscale
April 2025
State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai 200433, China.
Photonic crystals with advanced, unique and well-defined functional nanostructures demonstrate exquisite controllable modulation in light harvesting and emission for unrivalled optical performance. Herein, through ingeniously integrating aggregation-induced emission (AIE) luminogens and chiral helical media into ordered periodic structures, the resulting optically active photonic crystal films exhibit an enhanced photoluminescence (PL) characteristic (increased to 2.2 times the original value) and distinctive emerging circular dichroism (CD) responses near the photonic bandgap (PBG) of the photonic crystal.
View Article and Find Full Text PDFAcc Chem Res
April 2025
State Key Laboratory of Petroleum Molecular & Process Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Shanghai Frontiers Science Center of Molecule Intelligent Syntheses, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, P.
ConspectusFluorescence by small molecular dyes is renowned for its real-time, dynamic, and noninvasive nature. It has become indispensable across scientific domains, including information storage, optoelectronic materials, biosensing, and both diagnosing and treating diseases. Despite their widespread use, these molecular dyes suffer from several limitations due to the sensitivity of their photophysical properties to environmental factors, such as concentration, solvent composition, and polarity.
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February 2025
Beijing National Laboratory of Molecular Sciences and CAS Key Laboratory of Colloid, Interface and Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, North First Street 2, Zhongguancun, Beijing, 100190, China.
Precise organization of organic molecules into homochiral double-helix remains a challenge due to the difficulty in controlling both self-assembly process and chirality transfer across length scales. Here, we report that a type of bisnaphthalene bisurea molecule could assemble into chirality-controlled nanoscale double-helices by a supramolecular rosette-intermediated hierarchical self-assembly mechanism. A solvent-mixing self-assembly protocol is adopted to direct bisnaphthalene bisurea cyclization into chiral discrete rosettes through cooperative intramolecular and intermolecular hydrogen bonds.
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