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Nonlinear optical responses in two-dimensional (2D) materials can build free-space optical neuromorphic computing systems. Ensuring the high performance and the tunability of the system is essential to encode diverse functions. However, common strategies, including the integration of external electrode arrays or photonic structures with 2D materials, and barely patterned 2D materials, exhibit a contradiction between performance and tunability. Because the unique band dispersions of 2D materials can provide hidden paths to boost nonlinear responses independently, here we introduced a new free-space optical computing concept within a bare molybdenum disulfide array. This system can preserve high modulation performance with fast speed, low energy consumption, and high signal-to-noise ratio. Due to the freedom from the restrictions of fixed photonic structures, the tunability is also enhanced through the synergistic encodings of the 2D cells and the excitation pulses. The computing mechanism of transition from two-photon absorption to synergistic excited states absorption intrinsically improved the modulation capability of nonlinear optical responses, revealed from the relative transmittance modulated by a pump-probe-control strategy. Optical artificial neural network (ANN) and digital processing were demonstrated, revealing the feasibility of the free-space optical computing based on bare 2D materials toward neuromorphic applications.
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http://dx.doi.org/10.1038/s41467-024-54776-z | DOI Listing |
J Am Chem Soc
September 2025
Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States.
Understanding how molecular aggregation influences nonlinear optical properties is essential for advancing organic fluorophores in imaging, sensing, and photonic applications. However, the relationship between the molecular aggregation and the magnitude of nonlinear two-photon absorption cross-section remains underexplored. Here, we systematically investigate the aggregation-dependent two-photon absorption properties of the fluorophore TPAPhCN by tuning the degree of aggregation.
View Article and Find Full Text PDFJ Org Chem
September 2025
School of Chemical and Biopharmaceutical Sciences, Technological University Dublin, City Campus, Grangegorman, Dublin D07 EWV4, Ireland.
A series of unsymmetrically substituted BODIPY dyes featuring fused benzo- or naphtho-fragments on one pyrrolic unit were synthesized from the corresponding pyrrolic precursors. The synthetic route was optimized using a modular approach based on the condensation of formylpyrroles with alkylpyrroles, enabling the identification of precursor combinations that minimize byproduct formation and improve preparative yields. The resulting benzo- and naphtho-fused BODIPYs display intense fluorescence in the red region, with emission maxima spanning 590-680 nm and fluorescence quantum yields ranging from 0.
View Article and Find Full Text PDFJ Am Chem Soc
September 2025
Center for Nanochemistry, Beijing Science and Engineering Center for Nanocarbons, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.
Incorporating atomically thin two-dimensional (2D) materials with optical fibers expands their potential for optoelectronic applications. Recent advancements in chemical vapor deposition have enabled the batch production of these hybrid fibers, paving the way for practical implementation. However, their functionality remains constrained by the integration of a single 2D material, restricting their versatile performance.
View Article and Find Full Text PDFChaos
September 2025
Lomonosov Moscow State University, Faculty of Physics, Moscow 119992, Russia.
Soliton propagation of laser radiation in various nonlinear media is of great importance because of its numerous applications. Active periodic structures with parity-time symmetry provide the possibility for the solitons generation due to the balance of energy gain and loss. In the present paper, we derive an approximate analytical soliton solution to a model of two-color laser radiation propagation in an active periodic structure.
View Article and Find Full Text PDFChem Sci
September 2025
State Key Laboratory of Crystal Materials, Tianjin Key Laboratory of Functional Crystal Materials, Institute of Functional Crystals, Tianjin University of Technology Tianjin 300384 China
Nonlinear optical (NLO) crystals capable of expanding the spectral region of solid-state are of great importance for many high-tech applications, yet their rational structure design remains a great challenge because of the conflicting property requirements among second harmonic generation (SHG) response, ultraviolet (UV) cut-off edge, and birefringence. Herein, based on the chemical disubstitution of the classic NLO crystal SrBeBO (SBBO), , substituting [BO] triangles with larger π-conjugated [BO] groups and substituting high-toxic [BeO] tetrahedra with environment-friendly [AlO] tetrahedra, a new high-performance aluminoborate NLO crystal, BaAlBO, has been successfully designed and synthesized. The theoretical calculations and optical property measurements indicate that BaAlBO exhibits not only the largest SHG response among the reported aluminoborates (2.
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