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Herein, the simultaneous detection of second\u2010harmonic generation (SHG) and third\u2010harmonic generation (THG) optical responses in a recently discovered 2D in\u2010plane ferroelectric material, NbOI\n                    <jats:sub>2<\/jats:sub>\n                    is reported, as well as the giant modulation of SHG and THG in NbOI\n                    <jats:sub>2<\/jats:sub>\n                    by integrating with atomically thin MoS\n                    <jats:sub>2<\/jats:sub>\n                    . Both experimental and theoretical results show that NbOI\n                    <jats:sub>2<\/jats:sub>\n                    , ranging from few\u2010layer to thick\u2010layer dimensions, exhibits robust SHG and THG responses with pronounced dependence on excitation polarization and wavelength. This behavior is attributed to the anisotropic band structure and excitonic resonance effects in NbOI\n                    <jats:sub>2<\/jats:sub>\n                    . By interfacing a few\u2010layer NbOI\n                    <jats:sub>2<\/jats:sub>\n                    with a monolayer MoS\n                    <jats:sub>2<\/jats:sub>\n                    , the amplitude and polarization of both SHG and THG signals are effectively modulated, which can be further tailored by excitation wavelength and twist angle. The nonlinear optical control in MoS\n                    <jats:sub>2<\/jats:sub>\n                    \/NbOI\n                    <jats:sub>2<\/jats:sub>\n                    heterostructures is correlated with polar symmetry coupling, which is well modeled via nonlinear electromagnetic theory. This study thus provides a new material platform based on van der Waals ferroelectric heterostructures for dynamic control of nonlinear light intensity and polarization, paving the path for developing advanced nonlinear photonic nanodevices.\n                  <\/jats:p>","DOI":"10.1002\/smll.202513034","type":"journal-article","created":{"date-parts":[[2025,11,29]],"date-time":"2025-11-29T19:00:52Z","timestamp":1764442852000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Giant Modulation of Second and Third Harmonic Generations in in\u2010Plane Ferroelectric NbOI\n                    <sub>2<\/sub>\n                    via MoS\n                    <sub>2<\/sub>\n                    Atomic Layers"],"prefix":"10.1002","volume":"22","author":[{"given":"Jiabin","family":"Liu","sequence":"first","affiliation":[{"name":"School of Optoelectronic Engineering and Instrumentation Science Dalian University of Technology  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