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While strategies developed for 2D crystals are not directly transferable to 1D systems, we can benefit from them by creating layers formed by interconnected chains. Here, we develop a molecular strategy to illustrate this concept consisting of assembling 1D materials in 2D metal\u2013organic frameworks (MOFs). Crystals of [FeX(pzX)(bpy)] (X = Cl, F; pz = pyrazole; bpy = bipyridine) consist of iron chains along the\n                    <jats:italic>b<\/jats:italic>\n                    \u2010axis, crosslinked via bpy ligands along the\n                    <jats:italic>a<\/jats:italic>\n                    \u2010axis to form 2D layers, stacked along the\n                    <jats:italic>c<\/jats:italic>\n                    \u2010axis via vdW forces. This structural anisotropy manifests itself in highly\u2010anisotropic optical properties, as demonstrated by optical measurements in the visible and terahertz ranges, results which are supported by DFT calculations. Chemical substitution enables the tuning of the optical properties, as exemplified by the photoluminescence of the Cl\u2010derivative, which is quenched for the F\u2010derivative. Thin\u2010layers are obtained by mechanical exfoliation, and their optical properties are further tuned through the fabrication of orthogonally\u2010twisted vdW heterostructures, enabling to effectively switch\u2010off the optical anisotropy. Our work highlights the chemical flexibility of vdW layered MOFs as a platform for designing and manipulating 1D architectures.\n                  <\/jats:p>","DOI":"10.1002\/adma.202517382","type":"journal-article","created":{"date-parts":[[2026,3,28]],"date-time":"2026-03-28T08:46:02Z","timestamp":1774687562000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["One\u2010Dimensional Materials Supported in Two\u2010Dimensional Van der Waals Metal\u2013Organic Frameworks with Optical Anisotropy Switching via Twist\u2010Engineering"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-4524-1735","authenticated-orcid":false,"given":"Eleni C.","family":"Mazarakioti","sequence":"first","affiliation":[{"name":"Instituto de Ciencia Molecular (ICMol) Universitat De Val\u00e8ncia  Paterna 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