Wang Zhao, Jiazheng Zhou, Linan Wang, Wenqi Jin, Yingying Kong, Yu Chu and Junjie Li
{"title":"Pb6Ba3Si2S8I10:一种具有准二维结构和宽带隙的新型硫卤化物","authors":"Wang Zhao, Jiazheng Zhou, Linan Wang, Wenqi Jin, Yingying Kong, Yu Chu and Junjie Li","doi":"10.1039/D4DT02315C","DOIUrl":null,"url":null,"abstract":"<p >Pb-based chalcogenides display abundant structural diversity and distinguished properties. Based on a mixed anion and dimensional reduction combined strategy, a wide band gap Pb-based thiohalide, Pb<small><sub>6</sub></small>Ba<small><sub>3</sub></small>Si<small><sub>2</sub></small>S<small><sub>8</sub></small>I<small><sub>10</sub></small>, has been rationally designed and synthesized experimentally by the flux method. The compound crystallizes in the <em>R</em><img><em>c</em> space group with cell parameters <em>a</em> = 9.7925(2) Å, <em>b</em> = 9.7925(2) Å, and <em>c</em> = 70.628(3) Å and is composed of [SiS<small><sub>4</sub></small>] tetrahedra and unprecedented [PbI<small><sub>5</sub></small>S<small><sub>2</sub></small>] polyhedral units, resulting in a unique quasi-two-dimensional structure, which enriches the chemical and structural diversity of Pb-based thiohalides. The experimental band gap of Pb<small><sub>6</sub></small>Ba<small><sub>3</sub></small>Si<small><sub>2</sub></small>S<small><sub>8</sub></small>I<small><sub>10</sub></small> was determined to be 2.80 eV. Based on statistical analyses and to the best of our knowledge, it is the largest experimental optical band gap among the known Pb-based thiohalides. The results demonstrate the feasibility of using highly electropositive Ba atoms to regulate the dimensions of the structural framework of thiohalides and give new insights into the structure and property modifications of thiohalides by the mixed anion and dimensional reduction combined strategy.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":null,"pages":null},"PeriodicalIF":4.3000,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Pb6Ba3Si2S8I10: a new thiohalide with a quasi-two-dimensional structure and wide band gap†\",\"authors\":\"Wang Zhao, Jiazheng Zhou, Linan Wang, Wenqi Jin, Yingying Kong, Yu Chu and Junjie Li\",\"doi\":\"10.1039/D4DT02315C\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Pb-based chalcogenides display abundant structural diversity and distinguished properties. Based on a mixed anion and dimensional reduction combined strategy, a wide band gap Pb-based thiohalide, Pb<small><sub>6</sub></small>Ba<small><sub>3</sub></small>Si<small><sub>2</sub></small>S<small><sub>8</sub></small>I<small><sub>10</sub></small>, has been rationally designed and synthesized experimentally by the flux method. The compound crystallizes in the <em>R</em><img><em>c</em> space group with cell parameters <em>a</em> = 9.7925(2) Å, <em>b</em> = 9.7925(2) Å, and <em>c</em> = 70.628(3) Å and is composed of [SiS<small><sub>4</sub></small>] tetrahedra and unprecedented [PbI<small><sub>5</sub></small>S<small><sub>2</sub></small>] polyhedral units, resulting in a unique quasi-two-dimensional structure, which enriches the chemical and structural diversity of Pb-based thiohalides. The experimental band gap of Pb<small><sub>6</sub></small>Ba<small><sub>3</sub></small>Si<small><sub>2</sub></small>S<small><sub>8</sub></small>I<small><sub>10</sub></small> was determined to be 2.80 eV. Based on statistical analyses and to the best of our knowledge, it is the largest experimental optical band gap among the known Pb-based thiohalides. The results demonstrate the feasibility of using highly electropositive Ba atoms to regulate the dimensions of the structural framework of thiohalides and give new insights into the structure and property modifications of thiohalides by the mixed anion and dimensional reduction combined strategy.</p>\",\"PeriodicalId\":3,\"journal\":{\"name\":\"ACS Applied Electronic Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2024-09-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Electronic Materials\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/dt/d4dt02315c\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ELECTRICAL & ELECTRONIC\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Electronic Materials","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/dt/d4dt02315c","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ELECTRICAL & ELECTRONIC","Score":null,"Total":0}
Pb6Ba3Si2S8I10: a new thiohalide with a quasi-two-dimensional structure and wide band gap†
Pb-based chalcogenides display abundant structural diversity and distinguished properties. Based on a mixed anion and dimensional reduction combined strategy, a wide band gap Pb-based thiohalide, Pb6Ba3Si2S8I10, has been rationally designed and synthesized experimentally by the flux method. The compound crystallizes in the Rc space group with cell parameters a = 9.7925(2) Å, b = 9.7925(2) Å, and c = 70.628(3) Å and is composed of [SiS4] tetrahedra and unprecedented [PbI5S2] polyhedral units, resulting in a unique quasi-two-dimensional structure, which enriches the chemical and structural diversity of Pb-based thiohalides. The experimental band gap of Pb6Ba3Si2S8I10 was determined to be 2.80 eV. Based on statistical analyses and to the best of our knowledge, it is the largest experimental optical band gap among the known Pb-based thiohalides. The results demonstrate the feasibility of using highly electropositive Ba atoms to regulate the dimensions of the structural framework of thiohalides and give new insights into the structure and property modifications of thiohalides by the mixed anion and dimensional reduction combined strategy.