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In order to overcome the problem of crystal growth and the toxicity of BeO raw materials in KBe<jats:sub>2<\/jats:sub>BO<jats:sub>3<\/jats:sub>F<jats:sub>2<\/jats:sub> (KBBF), the only applicable DUV NLO crystal so far, we substitute Be<jats:sup>2+<\/jats:sup> cations with Zn<jats:sup>2+<\/jats:sup> in the KBBF structure and modify the halogen anions, by which three new Zn\u2010containing KBBF\u2010like compounds, CsZn<jats:sub>2<\/jats:sub>BO<jats:sub>3<\/jats:sub>X<jats:sub>2<\/jats:sub> (X<jats:sub>2<\/jats:sub>=F<jats:sub>2<\/jats:sub>, Cl<jats:sub>2<\/jats:sub>, and FCl), have been successfully synthesized. They all exhibit excellent NLO properties, including improved SHG responses (2.8\u20133.5\u00d7KDP) and short UV cut\u2010off edges (&lt;190\u2005nm). In comparison with KBBF, CsZn<jats:sub>2<\/jats:sub>BO<jats:sub>3<\/jats:sub>X<jats:sub>2<\/jats:sub> (X<jats:sub>2<\/jats:sub>=F<jats:sub>2<\/jats:sub>, Cl<jats:sub>2<\/jats:sub>, and FCl) are all chemically benign and have better growth habits, so they are all promising as DUV NLO crystals. Further study on structure\u2013property relationships indicates that the mixing of halogen anions is a feasible strategy to enhance the SHG responses of the KBBF family.<\/jats:p>","DOI":"10.1002\/anie.202008346","type":"journal-article","created":{"date-parts":[[2020,7,17]],"date-time":"2020-07-17T14:46:44Z","timestamp":1594997204000},"page":"19006-19010","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":143,"title":["CsZn<sub>2<\/sub>BO<sub>3<\/sub>X<sub>2<\/sub> (X<sub>2<\/sub>=F<sub>2<\/sub>, Cl<sub>2<\/sub>, and FCl): A Series of Beryllium\u2010Free Deep\u2010Ultraviolet Nonlinear\u2010Optical Crystals with Excellent Properties"],"prefix":"10.1002","volume":"59","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3973-4020","authenticated-orcid":false,"given":"Jinjie","family":"Zhou","sequence":"first","affiliation":[{"name":"Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystal Tianjin University of Technology  Tianjin 300384 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Youquan","family":"Liu","sequence":"additional","affiliation":[{"name":"Beijing Center for Crystal R&amp;D Key Lab of Functional Crystals and Laser Technology of Chinese Academy of Sciences Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing 100190 P. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhanggui","family":"Hu","sequence":"additional","affiliation":[{"name":"Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystal Tianjin University of Technology  Tianjin 300384 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiyang","family":"Wang","sequence":"additional","affiliation":[{"name":"Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystal Tianjin University of Technology  Tianjin 300384 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yicheng","family":"Wu","sequence":"additional","affiliation":[{"name":"Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystal Tianjin University of Technology  Tianjin 300384 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2020,8,24]]},"reference":[{"key":"e_1_2_2_1_1","unstructured":"\u00a0"},{"key":"e_1_2_2_2_2","doi-asserted-by":"publisher","DOI":"10.1016\/S1359-0286(96)80085-4"},{"key":"e_1_2_2_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/(SICI)1521-4095(199809)10:13<979::AID-ADMA979>3.0.CO;2-N"},{"key":"e_1_2_2_4_2","doi-asserted-by":"publisher","DOI":"10.1016\/S0927-796X(00)00025-5"},{"key":"e_1_2_2_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/9783527646388"},{"key":"e_1_2_2_6_1","first-page":"235","volume":"28","author":"Chen C. 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