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However, the fundamental role of interlayer interactions in modifying the overall nonlinear optical susceptibilities remains elusive. In this paper, we report anisotropic enhancement of second-harmonic generation (SHG) from a WS2\/ReSe2 heterobilayer, where the individual composite layers possess distinctive crystal phases. We investigate polarization-resolved response and twist-angle dependence in SHG and reveal that band alignment alone is insufficient to explain the observed anisotropy in the modified SHG response. Spectral shifts in excitonic features highlight band renormalization, supporting the role of hybridization between the two layers. Furthermore, SHG enhancement is highly anisotropic and can even be suppressed in some orientations, suggesting possible intensity-borrowing mechanisms within the heterostructure. Our work demonstrates the ability to tune both the intensity and polarization dependence of nonlinear optical responses with van der Waals stacking of distinctive crystal phases.<\/jats:p>","DOI":"10.1063\/5.0313933","type":"journal-article","created":{"date-parts":[[2026,3,9]],"date-time":"2026-03-09T12:35:52Z","timestamp":1773059752000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Enhanced second-harmonic generation from WS2\/ReSe2 heterostructure"],"prefix":"10.1063","volume":"164","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3564-0000","authenticated-orcid":false,"given":"Kanchan","family":"Shaikh","sequence":"first","affiliation":[{"name":"Department of Chemistry, University of Michigan 1 , Ann Arbor, Michigan 48109,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-4215-4787","authenticated-orcid":false,"given":"Taejun","family":"Yoo","sequence":"additional","affiliation":[{"name":"Department of Chemistry, University of Michigan 1 , Ann Arbor, Michigan 48109,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-0431-6347","authenticated-orcid":false,"given":"Zeyuan","family":"Zhu","sequence":"additional","affiliation":[{"name":"Department of Chemistry, University of Michigan 1 , Ann Arbor, Michigan 48109,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8192-3960","authenticated-orcid":false,"given":"Qiuyang","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Physics, University of Michigan 2 , Ann Arbor, Michigan 48109,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9604-984X","authenticated-orcid":false,"given":"Amalya C.","family":"Johnson","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Stanford University 3 , Stanford, California 94305,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0629-3230","authenticated-orcid":false,"given":"Hui","family":"Deng","sequence":"additional","affiliation":[{"name":"Department of Physics, University of Michigan 2 , Ann Arbor, Michigan 48109,","place":["USA"]},{"name":"Department of Electrical Engineering and Computer Science, University of Michigan 4 , Ann Arbor, Michigan 48109,","place":["USA"]},{"name":"Quantum Research Institute, University of Michigan 5 , Ann Arbor, Michigan 48109,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1467-8328","authenticated-orcid":false,"given":"Fang","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Stanford University 6 , Stanford, California 94305,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4391-1328","authenticated-orcid":false,"given":"Yuki","family":"Kobayashi","sequence":"additional","affiliation":[{"name":"Department of Chemistry, University of Michigan 1 , Ann Arbor, Michigan 48109,","place":["USA"]},{"name":"Quantum Research Institute, University of Michigan 5 , Ann Arbor, Michigan 48109,","place":["USA"]}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"317","published-online":{"date-parts":[[2026,3,9]]},"reference":[{"key":"2026030908354660900_c1","doi-asserted-by":"publisher","first-page":"419","DOI":"10.1038\/nature12385","volume":"499","year":"2013","journal-title":"Nature"},{"key":"2026030908354660900_c2","doi-asserted-by":"publisher","first-page":"58","DOI":"10.1038\/s43586-022-00139-1","volume":"2","year":"2022","journal-title":"Nat. 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