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Herein, based on the unique two\u2010dimensional layered structure in KBe<jats:sub>2<\/jats:sub>BO<jats:sub>3<\/jats:sub>F<jats:sub>2<\/jats:sub> (KBBF), two new compounds, Sn<jats:sub>2<\/jats:sub>PO<jats:sub>4<\/jats:sub>I and Sn<jats:sub>2<\/jats:sub>BO<jats:sub>3<\/jats:sub>I, were designed and synthesized successfully, maintaining the layer structural feature and enhancing the optical anisotropy of crystals. In particular, the birefringence of Sn<jats:sub>2<\/jats:sub>PO<jats:sub>4<\/jats:sub>I is larger than or equal to 0.664 @546\u2005nm, which is largest among the reported borates and phosphates, even surpassing commercial birefringent crystals YVO<jats:sub>4<\/jats:sub> and TiO<jats:sub>2<\/jats:sub>. This work indicates that a breakthrough in birefringence of inorganic compound was achieved. Also, it provides a guiding idea for exploring large birefringence materials in the future.<\/jats:p>","DOI":"10.1002\/anie.202111604","type":"journal-article","created":{"date-parts":[[2021,9,15]],"date-time":"2021-09-15T08:18:04Z","timestamp":1631693884000},"page":"24901-24904","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":215,"title":["Sn<sub>2<\/sub>PO<sub>4<\/sub>I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non \u03c0\u2010Conjugated Phosphate"],"prefix":"10.1002","volume":"60","author":[{"given":"Jingyu","family":"Guo","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics &amp; Chemistry of CAS Xinjiang Key Laboratory of Electronic Information Materials and Devices  40-1 South Beijing Road Urumqi 830011 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Abudukadi","family":"Tudi","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics &amp; Chemistry of CAS Xinjiang Key Laboratory of Electronic Information Materials and Devices  40-1 South Beijing Road Urumqi 830011 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shujuan","family":"Han","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics &amp; Chemistry of CAS Xinjiang Key Laboratory of Electronic Information Materials and Devices  40-1 South Beijing Road Urumqi 830011 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhihua","family":"Yang","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics &amp; Chemistry of CAS Xinjiang Key Laboratory of Electronic Information Materials and Devices  40-1 South Beijing Road Urumqi 830011 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4521-4507","authenticated-orcid":false,"given":"Shilie","family":"Pan","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics &amp; Chemistry of CAS Xinjiang Key Laboratory of Electronic Information Materials and Devices  40-1 South Beijing Road Urumqi 830011 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2021,10,20]]},"reference":[{"key":"e_1_2_2_1_1","doi-asserted-by":"publisher","DOI":"10.1117\/1.3483597"},{"key":"e_1_2_2_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.6b00452"},{"key":"e_1_2_2_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201913974"},{"key":"e_1_2_2_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201913974"},{"key":"e_1_2_2_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5b11712"},{"key":"e_1_2_2_5_1","doi-asserted-by":"publisher","DOI":"10.1117\/3.626141"},{"key":"e_1_2_2_6_1","volume-title":"Polarized Light","author":"Goldstein D. 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