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Third‐Order Nonlinear Optical Modulation in MoS<sub>2</sub> Nanosheets in the Presence of CdSe and CdSe/V<sub>2</sub>O<sub>5</sub> Quantum Dots

Srinivasa Rao KondaGPL Photonics Laboratory State Key Laboratory of Luminescence Science and Technology Changchun Institute of Optics Fine Mechanics and Physics Chinese Academy of Sciences Changchun Jilin 130033 ChinaPuspendu BarikMaterials Science and Engineering Program, College of Arts and Sciences, American University of Sharjah, Sharjah, UAESubhash C. SinghThe Institute of Optics University of Rochester Rochester NY 14627 USAMottamchetty VenkateshGPL Photonics Laboratory State Key Laboratory of Luminescence Science and Technology Changchun Institute of Optics Fine Mechanics and Physics Chinese Academy of Sciences Changchun Jilin 130033 ChinaAmit SrivasthavaDepartment of Physics TDPG College VBS Purvanchal University Jaunpur 222001 IndiaR. A. GaneevInstitute of Fundamental and Applied Research TIIAME National Research University Tashkent 100000 UzbekistanS. Venugopal RaoSchool of Physics &amp; DIA‐CoE (formerly ACRHEM) University of Hyderabad Hyderabad Telangana 500046 IndiaChunlei GuoThe Institute of Optics University of Rochester Rochester NY 14627 USAWei LiGPL Photonics Laboratory, State Key Laboratory of Luminescence Science and Technology, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun, Jilin, 130033 China

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Abstract Embedding semiconductor quantum dots (QDs) into a 2D transition metal dichalcogenide (TMDCs) can significantly modulate the electronic charge transfer and, hence, the nonlinear optical (NLO) properties of the TMDCs. However, the influence of strong interactions within 2D nanostructure‐QDs composites on their third‐order NLO responses has not been explored thus far. The third‐order NLO characteristics of few‐layered MoS 2 nanosheets embedded with CdSe and CdSe/V 2 O 5 QDs are studied using 35‐fs pulses at 400 and 800 nm excitations. It is observed that an alteration of the third‐order NLO properties in MoS 2 occurs in the presence of QDs. Notably, the MoS 2 ‐QDs hybrid system exhibits a significant modulation in third‐order nonlinearities, with a substantial multi‐fold increase in the figure of merit in the presence of core CdSe QDs and suppression with passivated CdSe/V 2 O 5 QDs. These findings strongly indicate that QD‐based hybrid systems with charge transfer channels probably enhance carrier mobility and enable tunable electron transfer dynamics, which can emerge as a viable strategy for tailoring third‐order NLO properties in TMDCs, positioning these hybrid materials as promising candidates for optoelectronic applications.

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