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However, in metallic 2D systems, strong free\u2010carrier absorption and shallow optical penetration depth usually suppress the nonlinear response. Realizing pronounced SHG in such highly absorptive materials thus remains a major challenge in nonlinear photonics. In this work, we systematically investigate the SHG response of non\u2010centrosymmetric metallic 3R\u2010TaS\n                    <jats:sub>2<\/jats:sub>\n                    and demonstrate strong broadband SHG across a wide emission wavelength range of 510\u2013705\u00a0nm. By analyzing the wavelength\u2010dependent optical constants and dielectric function, we show that this broadband SHG arises from the combined effects of the non\u2010centrosymmetric crystal structure, a dielectric\u2010like optical response in the visible range, and the absence of sharp resonance features, together with free\u2010carrier\u2010mediated optical damping. Furthermore, substantial SHG enhancement is achieved using a reflective gold substrate, with the enhancement factor increasing from 2.7 to 45.5 as the flake thickness decreases from 123 to 68\u00a0nm. The extracted effective second\u2010order nonlinear susceptibility is comparable to that of MoS\n                    <jats:sub>2<\/jats:sub>\n                    , despite the metallic electronic structure of 3R\u2010TaS\n                    <jats:sub>2<\/jats:sub>\n                    . These results demonstrate that strong, broadband nonlinear optical responses can persist in metallic layered materials and provide new insights into the interplay among metallicity, optical response, and nonlinear light\u2010matter interactions in van der Waals systems.\n                  <\/jats:p>","DOI":"10.1002\/smll.202513532","type":"journal-article","created":{"date-parts":[[2026,8,14]],"date-time":"2026-08-14T14:55:01Z","timestamp":1786719301000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Broadband and Enhanced Second\u2010Harmonic Generation in Metallic 3R\u2010TaS\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-5823-7235","authenticated-orcid":false,"given":"Ruo\u2010Si","family":"Chen","sequence":"first","affiliation":[{"name":"School of Engineering College of Systems and Society Australian National University  Canberra Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuanyu","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Engineering College of Systems and Society Australian National University  Canberra Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiangqi","family":"Liu","sequence":"additional","affiliation":[{"name":"ShanghaiTech Laboratory for Topological Physics ShanghaiTech University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhuoyuan","family":"Lu","sequence":"additional","affiliation":[{"name":"School of Engineering College of Systems and Society Australian National University  Canberra Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuyao","family":"Qiu","sequence":"additional","affiliation":[{"name":"School of Engineering College of Systems and Society Australian National University  Canberra Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Boqing","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Engineering College of Systems and Society Australian National University  Canberra Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tieyu","family":"L\u00fc","sequence":"additional","affiliation":[{"name":"Department of Physics and Institute of Theoretical Physics and Astrophysics Xiamen University  Xiamen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shi\u2010Rui","family":"Zhang","sequence":"additional","affiliation":[{"name":"Research School of Physics Department of Electronic Materials Engineering Australian National University  Canberra Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanfeng","family":"Guo","sequence":"additional","affiliation":[{"name":"ShanghaiTech Laboratory for Topological Physics ShanghaiTech University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6131-3906","authenticated-orcid":false,"given":"Yuerui","family":"Lu","sequence":"additional","affiliation":[{"name":"School of Engineering College of Systems and Society Australian National University  Canberra Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,14]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.68.2153"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.neuroscience.2022.08.003"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.4c03286"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/0022\u20103093(94)90247\u2010X"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.87.161403"},{"key":"e_1_2_8_7_1","first-page":"13061","article-title":"Substrate Interference 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