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Leveraging the symmetry tunability of van der Waals materials, we address this limitation via electrostatic control of the Hamiltonian. By employing an ion-gel top gate to exert a strong out-of-plane displacement field, we effectively break the inversion symmetry of bilayer graphene and unlock its latent \u03c7(2) nonlinearity. We demonstrate a giant, actively tunable SHG response with a nonlinear susceptibility \u03c7(2) \u223c 300 pm\/V in the communication band, exceeding that of monolayer MoS2 by over an order of magnitude, whereas the signal remains undetectable under conventional SiO2 back-gating. Polarization-resolved measurements confirm a symmetry reduction to the C3v point group, while thickness-dependent studies establish a generalized framework for nonlinear optics in centrosymmetric stacks. Our work positions electrostatic symmetry control as a general approach for activating and controlling nonlinear responses in 2D materials, with potential applications in actively tunable integrated photonics and quantum light sources.<\/jats:p>","DOI":"10.1021\/acsnano.6c07601","type":"journal-article","created":{"date-parts":[[2026,7,13]],"date-time":"2026-07-13T16:42:03Z","timestamp":1783960923000},"page":"20849-20856","source":"Crossref","is-referenced-by-count":0,"title":["Giant and Actively\nTunable Second-Harmonic Generation\nin Bilayer Graphene"],"prefix":"10.1021","volume":"20","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1989-4767","authenticated-orcid":true,"given":"Mingwen","family":"Zhang","sequence":"first","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710129"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1704-4144","authenticated-orcid":true,"given":"Yi","family":"Zhang","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710129"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoyu","family":"Wang","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nannan","family":"Han","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Luojun","family":"Du","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7386-5185","authenticated-orcid":true,"given":"Xiaoqing","family":"Chen","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710129"]},{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianlin","family":"Zhao","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710129"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2469-5807","authenticated-orcid":true,"given":"Xuetao","family":"Gan","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi\u2019an, China, 710129"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,13]]},"reference":[{"key":"2026072810082777900_cit1","doi-asserted-by":"publisher","first-page":"118","DOI":"10.1103\/PhysRevLett.7.118","article-title":"Generation\nof Optical Harmonics","volume":"7","author":"Franken","year":"1961","journal-title":"Phys. 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