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Herein, we report a new ammonium-based mixed-halide halogenometallate, [BTMA]2CdBr2I2, that crystallizes in the polar P21 space group and exhibits coupled ferroelectric and piezoelectric responses. The noncentrosymmetric nature of the structure is confirmed by its pronounced second harmonic generation (SHG) activity. Bulk ferroelectricity is evidenced by a well-saturated, rectangular polarization\u2013electric field (P\u2013E) hysteresis loop with a polarization of 4.43 \u03bcC cm\u20132, while piezoresponse force microscopy (PFM) directly visualizes switchable ferroelectric domains, confirming intrinsic polarization at the microscale. Beyond these fundamental properties, we further demonstrate device-level functionality by integrating [BTMA]2CdBr2I2 into flexible thermoplastic polyurethane (TPU) composites. The optimized 10 wt % composite delivers a high piezoelectric nanogenerator output voltage of 15.9 V, a power density of 10.24 \u03bcW cm\u20132, and an output work efficiency (OWE) of 23.7%. These results not only establish mixed halide engineering as a viable strategy to access polar molecular materials but also position halogenometallate-based hybrids as promising candidates for flexible, high-performance energy harvesting technologies.<\/jats:p>","DOI":"10.1021\/acs.inorgchem.6c02484","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T21:01:32Z","timestamp":1787259692000},"page":"19811-19820","source":"Crossref","is-referenced-by-count":0,"title":["Halide Substitution\nDriven Symmetry Breaking in a\nFerroelectric Mixed-Halide Halogenometallate for Piezoelectric Energy\nHarvesting"],"prefix":"10.1021","volume":"65","author":[{"given":"Ashlesha S.","family":"Goswami","sequence":"first","affiliation":[{"name":"Indian Institute of Science Education and Research, Pune , , Dr. Homi Bhabha Road , ,","place":["Pune, India, 411008"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0191-6849","authenticated-orcid":true,"given":"Nilotpal","family":"Deka","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research, Pune , , Dr. Homi Bhabha Road , ,","place":["Pune, India, 411008"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vinayak B.","family":"Gadagin","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research, Pune , , Dr. Homi Bhabha Road , ,","place":["Pune, India, 411008"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6117-6876","authenticated-orcid":true,"given":"Jan K.","family":"Zare\u0328ba","sequence":"additional","affiliation":[{"name":"Wroc\u0142aw University of Science and Technology , , ,","place":["Wroc\u0142aw, Poland, 50-370"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5933-4414","authenticated-orcid":true,"given":"Ramamoorthy","family":"Boomishankar","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research, Pune , , Dr. Homi Bhabha Road , ,","place":["Pune, India, 411008"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,20]]},"reference":[{"key":"2026090222504780300_cit1","doi-asserted-by":"publisher","first-page":"214663","DOI":"10.1016\/j.ccr.2022.214663","article-title":"Recent advances in ferroelectric\nmetal complexes","volume":"469","author":"Sekine","year":"2022","journal-title":"Coord. 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