{"title":"Ce3+掺杂调制(1R,2R)-DACHGeI4的非线性光学性质","authors":"Jing Huang, , , Hualin Bi, , , Huitao Zhang, , , Jia Zhou, , , Jialin Zhang, , , Huanbo Wang, , and , Jun Wang*, ","doi":"10.1021/acs.jpclett.5c02690","DOIUrl":null,"url":null,"abstract":"<p >Chiral perovskites exhibit great potential in polarization optics and spintronics due to their excellent structural and electronic properties. This study uses (1<i>R</i>,2<i>R</i>)-DACH as the organic component to synthesize a novel 2D germanium-based chiral perovskite single crystal, (1<i>R</i>,2<i>R</i>)-DACHGeI<sub>4</sub> (where (1<i>R</i>,2<i>R</i>)-DACH is (1<i>R</i>,2<i>R</i>)-(−)-1,2-cyclohexanediamine). To address the impact of lattice defects in germanium-based perovskites on optical properties, a rare-earth Ce<sup>3+</sup> doping compensation strategy is adopted. Experiments show Ce<sup>3+</sup> doping enhances photoluminescence quantum yield and fluorescence lifetime, regulates spintronic states, replaces partial Ge<sup>2+</sup> to cause lattice distortion, changes the crystal space group from chiral <i>P</i>2<sub>1</sub>2<sub>1</sub>2 to nonchiral <i>Pba</i>2, and destroys the chiral structure. DFT calculations confirm these experimental results. This work provides a new approach to improving the nonlinear optical properties of 2D germanium-based perovskites and deepens the understanding of the intrinsic relationship between chiral perovskite structures and spintronic states.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 39","pages":"10273–10281"},"PeriodicalIF":4.6000,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Modulating Nonlinear Optical Properties of (1R,2R)-DACHGeI4 through Ce3+ Doping\",\"authors\":\"Jing Huang, , , Hualin Bi, , , Huitao Zhang, , , Jia Zhou, , , Jialin Zhang, , , Huanbo Wang, , and , Jun Wang*, \",\"doi\":\"10.1021/acs.jpclett.5c02690\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Chiral perovskites exhibit great potential in polarization optics and spintronics due to their excellent structural and electronic properties. This study uses (1<i>R</i>,2<i>R</i>)-DACH as the organic component to synthesize a novel 2D germanium-based chiral perovskite single crystal, (1<i>R</i>,2<i>R</i>)-DACHGeI<sub>4</sub> (where (1<i>R</i>,2<i>R</i>)-DACH is (1<i>R</i>,2<i>R</i>)-(−)-1,2-cyclohexanediamine). To address the impact of lattice defects in germanium-based perovskites on optical properties, a rare-earth Ce<sup>3+</sup> doping compensation strategy is adopted. Experiments show Ce<sup>3+</sup> doping enhances photoluminescence quantum yield and fluorescence lifetime, regulates spintronic states, replaces partial Ge<sup>2+</sup> to cause lattice distortion, changes the crystal space group from chiral <i>P</i>2<sub>1</sub>2<sub>1</sub>2 to nonchiral <i>Pba</i>2, and destroys the chiral structure. DFT calculations confirm these experimental results. This work provides a new approach to improving the nonlinear optical properties of 2D germanium-based perovskites and deepens the understanding of the intrinsic relationship between chiral perovskite structures and spintronic states.</p>\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"16 39\",\"pages\":\"10273–10281\"},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2025-09-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpclett.5c02690\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpclett.5c02690","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Modulating Nonlinear Optical Properties of (1R,2R)-DACHGeI4 through Ce3+ Doping
Chiral perovskites exhibit great potential in polarization optics and spintronics due to their excellent structural and electronic properties. This study uses (1R,2R)-DACH as the organic component to synthesize a novel 2D germanium-based chiral perovskite single crystal, (1R,2R)-DACHGeI4 (where (1R,2R)-DACH is (1R,2R)-(−)-1,2-cyclohexanediamine). To address the impact of lattice defects in germanium-based perovskites on optical properties, a rare-earth Ce3+ doping compensation strategy is adopted. Experiments show Ce3+ doping enhances photoluminescence quantum yield and fluorescence lifetime, regulates spintronic states, replaces partial Ge2+ to cause lattice distortion, changes the crystal space group from chiral P21212 to nonchiral Pba2, and destroys the chiral structure. DFT calculations confirm these experimental results. This work provides a new approach to improving the nonlinear optical properties of 2D germanium-based perovskites and deepens the understanding of the intrinsic relationship between chiral perovskite structures and spintronic states.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.