Yang, LanBoukhvalov, Danil W.Li, HuiLi, WenboDai, ShengHumphrey, Mark G.Zhang, ChiHuang, Zhipeng2025-05-232025-05-23ORCID:/0000-0002-4433-6783/work/184100635http://www.scopus.com/inward/record.url?scp=85208409463&partnerID=8YFLogxKhttps://hdl.handle.net/1885/733752690Simultaneously optimizing nonlinear absorption coefficient and modulation depth is a considerable challenge for nonlinear optical materials. Here we present an effective solution through constructing PbS2-based inorganic-organic superlattice. PbS2/Cn superlattice particles are synthesized, where n (4, 6, and 8) denotes the number of carbon atoms in the organic component. First-principles simulations indicate the formation of covalent bonds and van der Waals interaction between PbS2 unit and interlayer organic molecules. All samples exhibit strong nonlinear absorption under femtosecond laser excitation with a wavelength range between 515 nm and 900 nm, and the nonlinear absorption coefficient increases with interlayer distance. The optimized sample, PbS2/C8, demonstrates outstanding nonlinear absorption and substantial modulation depth under 800 nm (the third-order nonlinear absorption coefficient βeff, 10449 ± 609 cm GW−1; modulation depth, 39.1%) and 900 nm (the fifth-order nonlinear absorption coefficient γeff, 6465 ± 68 cm3 GW−2; modulation depth, 88.1%), which exhibits saturable absorption under 515 nm (βeff, -4932 ± 818 cm GW−1; modulation depth, 48.1%). It exhibits a small optical limiting threshold of 1.23 mJ cm−2. These performances surpass those of typical single-/few-layer metal chalcogenides. Structural and spectral analyses elucidate that the remarkable optical nonlinearity can be attributed to quantum confinement in the inorganic layer and the dielectric enhancement of the superlattice.Z.H. acknowledges the support from the National Natural Science Foundation of China (Nos. 62275197 and 51772214), the Natural Science Foundation of Shanghai (23ZR1465700), the National Youth Talent Support Program of China (No. W03070073), and the Fundamental Research Funds for the Central Universities. C.Z. acknowledges support from the National Natural Science Foundation of China (No. 51432006), the Ministry of Education of China for the Changjiang Innovation Research Team (No. IRT14R23), the Ministry of Education and the State Administration of Foreign Experts Affairs for the 111 Project (No. B13025), and the Innovation Program of Shanghai Municipal Education Commission. D.W.B. acknowledges support from the Jiangsu Innovative and Entrepreneurial Talents Project and the Ministry of Science and Education of the Russian Federation (Project FEUZ-2023-0013). S.D. thanks the National Natural Science Foundation of China (22376062), the Science and Technology Commission of Shanghai Municipality (22ZR1415700), and the Fundamental Research Funds for the Central Universities. Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at East China University of Science and Technology. M.G.H. thanks the Australian Research Council (DP170100411). Z.H. acknowledges the support from the National Natural Science Foundation of China (Nos. 62275197 and 51772214), the Natural Science Foundation of Shanghai (23ZR1465700), the National Youth Talent Support Program of China (No. W03070073), and the Fundamental Research Funds for the Central Universities. C.Z. acknowledges support from the National Natural Science Foundation of China (No. 51432006), the Ministry of Education of China for the Changjiang Innovation Research Team (No. IRT14R23), the Ministry of Education and the State Administration of Foreign Experts Affairs for the 111 Project (No. B13025), and the Innovation Program of Shanghai Municipal Education Commission. D.W.B. acknowledges support from the Jiangsu Innovative and Entrepreneurial Talents Project and the Ministry of Science and Education of the Russian Federation (Project FEUZ\u20102023\u20100013). S.D. thanks the National Natural Science Foundation of China (22376062), the Science and Technology Commission of Shanghai Municipality (22ZR1415700), and the Fundamental Research Funds for the Central Universities. Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at East China University of Science and Technology. M.G.H. thanks the Australian Research Council (DP170100411).enPublisher Copyright: © 2024 Wiley-VCH GmbH.dielectric confinementlead sulfidenonlinear opticalquantum confinementsuperlattices2024-12-2010.1002/adom.20240145385208409463