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Here, we present the comprehensive relativistic electronic structure investigation of a heavy molecular anion FrF\u2212, which is anticipated to be a promising candidate for laser cooling and for studies of conjugation and parity violation. Using high-level two-component configuration\u2013interaction methods, we carried out a detailed investigation of the cooling cycle mechanism of the FrF\u2212 molecular anion and evaluated the key parameters\u2014effective electric field (Eeff), hyperfine constant (A\u2016), electron\u2013nucleon scalar\u2013pseudoscalar constant (WP,T), and nuclear quadrupole moment constant (WM). By quantitatively disentangling the contributions from basis-set hierarchy, electron correlation, spin\u2013orbit coupling, and quantum electrodynamics effects, we provide a transparent and reliable uncertainty analysis for each constant. Our results reveal that FrF\u2212 exhibits a remarkably large intrinsic sensitivity to the eEDM, rivaling leading neutral and cationic candidates. These findings establish ultracold molecular anions as a powerful and previously untapped platform for next-generation symmetry tests and precision measurement science.<\/jats:p>","DOI":"10.1063\/5.0321267","type":"journal-article","created":{"date-parts":[[2026,5,5]],"date-time":"2026-05-05T11:35:17Z","timestamp":1777980917000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Ultracold heavy molecular anions as enhanced probes of\n                    <i>CP<\/i>\n                    violation"],"prefix":"10.1063","volume":"164","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2214-9610","authenticated-orcid":false,"given":"Huagang","family":"Xiao","sequence":"first","affiliation":[{"name":"Institute of Atomic and Molecular Physics, Sichuan University 1 , Chengdu 610065,","place":["China"]},{"name":"College of Physics, Chengdu University of Technology 2 , Chengdu 610059,","place":["China"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-4471-5992","authenticated-orcid":false,"given":"Qin","family":"Fan","sequence":"additional","affiliation":[{"name":"Institute of Atomic and Molecular Physics, Sichuan University 1 , Chengdu 610065,","place":["China"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-8342-2522","authenticated-orcid":false,"given":"Xin","family":"Zhou","sequence":"additional","affiliation":[{"name":"Institute of Atomic and Molecular Physics, Sichuan University 1 , Chengdu 610065,","place":["China"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4065-3802","authenticated-orcid":false,"given":"Tao","family":"Gao","sequence":"additional","affiliation":[{"name":"Institute of Atomic and Molecular Physics, Sichuan University 1 , Chengdu 610065,","place":["China"]}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"317","published-online":{"date-parts":[[2026,5,5]]},"reference":[{"key":"2026050507351265100_c1","doi-asserted-by":"publisher","first-page":"279","DOI":"10.1016\/j.physrep.2004.08.031","volume":"405","year":"2005","journal-title":"Phys. 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