Prediction of Fluorooxoborates with Colossal Second Harmonic Generation (SHG) Coefficients and Extremely Wide Band Gaps: Towards Modulating Properties by Tuning the BO3/BO3F Ratio in Layers
Fluorooxoborates have inspired investigations of deep‐ultraviolet (DUV) nonlinear optical (NLO) materials that can meet the multiple criteria. Herein, five stable structures with the composition of BaB2O3F2 (I–V) are discovered using the ab initio evolutionary algorithm. Among them, BaB2O3F2‐I has b...
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| Vydáno v: | Angewandte Chemie International Edition Ročník 58; číslo 34; s. 11726 - 11730 |
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| Vydání: | International ed. in English |
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| ISSN: | 1433-7851, 1521-3773 |
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| Abstract | Fluorooxoborates have inspired investigations of deep‐ultraviolet (DUV) nonlinear optical (NLO) materials that can meet the multiple criteria. Herein, five stable structures with the composition of BaB2O3F2 (I–V) are discovered using the ab initio evolutionary algorithm. Among them, BaB2O3F2‐I has been synthesized experimentally and confirms the reliability of the method. All of the predicted structures possess extremely wide band gaps (8.1–9.0 eV). Moreover, four new structures exhibit giant second harmonic generation (SHG) coefficients (>3×KDP, d36=0.39 pm V−1). A novel type of the [BOF] layer with BO3:BO3F ratio of [1:1] is found in BaB2O3F2‐II and BaB2O3F2‐III. While BaB2O3F2‐IV and BaB2O3F2‐V are solely composed of the BO3F group and have colossal SHG coefficients (ca. 4×KDP). It gives the direct evidence that the BO3F group could generate strong SHG effect. Most importantly, the influences of BO3:BO3F ratio and their number density on band gap, birefringence and SHG effects are investigated.
Fluorooxoborates have inspired investigations of deep‐ultraviolet (DUV) nonlinear optical (NLO) materials. Five stable structures with the composition of BaB2O3F2 (I–V) are discovered using the ab initio evolutionary algorithm. Among them, BaB2O3F2‐I is known and confirms the reliability of the method. It shows that BO3F groups can give large band gaps and strong second harmonic generation (SHG) responses. |
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| AbstractList | Fluorooxoborates have inspired investigations of deep‐ultraviolet (DUV) nonlinear optical (NLO) materials that can meet the multiple criteria. Herein, five stable structures with the composition of BaB2O3F2 (I–V) are discovered using the ab initio evolutionary algorithm. Among them, BaB2O3F2‐I has been synthesized experimentally and confirms the reliability of the method. All of the predicted structures possess extremely wide band gaps (8.1–9.0 eV). Moreover, four new structures exhibit giant second harmonic generation (SHG) coefficients (>3×KDP, d36=0.39 pm V−1). A novel type of the [BOF] layer with BO3:BO3F ratio of [1:1] is found in BaB2O3F2‐II and BaB2O3F2‐III. While BaB2O3F2‐IV and BaB2O3F2‐V are solely composed of the BO3F group and have colossal SHG coefficients (ca. 4×KDP). It gives the direct evidence that the BO3F group could generate strong SHG effect. Most importantly, the influences of BO3:BO3F ratio and their number density on band gap, birefringence and SHG effects are investigated. Fluorooxoborates have inspired investigations of deep‐ultraviolet (DUV) nonlinear optical (NLO) materials that can meet the multiple criteria. Herein, five stable structures with the composition of BaB2O3F2 (I–V) are discovered using the ab initio evolutionary algorithm. Among them, BaB2O3F2‐I has been synthesized experimentally and confirms the reliability of the method. All of the predicted structures possess extremely wide band gaps (8.1–9.0 eV). Moreover, four new structures exhibit giant second harmonic generation (SHG) coefficients (>3×KDP, d36=0.39 pm V−1). A novel type of the [BOF] layer with BO3:BO3F ratio of [1:1] is found in BaB2O3F2‐II and BaB2O3F2‐III. While BaB2O3F2‐IV and BaB2O3F2‐V are solely composed of the BO3F group and have colossal SHG coefficients (ca. 4×KDP). It gives the direct evidence that the BO3F group could generate strong SHG effect. Most importantly, the influences of BO3:BO3F ratio and their number density on band gap, birefringence and SHG effects are investigated. Fluorooxoborates have inspired investigations of deep‐ultraviolet (DUV) nonlinear optical (NLO) materials. Five stable structures with the composition of BaB2O3F2 (I–V) are discovered using the ab initio evolutionary algorithm. Among them, BaB2O3F2‐I is known and confirms the reliability of the method. It shows that BO3F groups can give large band gaps and strong second harmonic generation (SHG) responses. |
| Author | Zhang, Bingbing Xie, Congwei Tikhonov, Evgenii Yang, Zhihua Pan, Shilie |
| Author_xml | – sequence: 1 givenname: Bingbing surname: Zhang fullname: Zhang, Bingbing organization: Xinjiang Key Laboratory of Electronic Information Materials and Devices – sequence: 2 givenname: Evgenii surname: Tikhonov fullname: Tikhonov, Evgenii organization: Xinjiang Key Laboratory of Electronic Information Materials and Devices – sequence: 3 givenname: Congwei surname: Xie fullname: Xie, Congwei organization: Northwestern Polytechnical University – sequence: 4 givenname: Zhihua orcidid: 0000-0001-9214-3612 surname: Yang fullname: Yang, Zhihua email: zhyang@ms.xjb.ac.cn organization: Xinjiang Key Laboratory of Electronic Information Materials and Devices – sequence: 5 givenname: Shilie orcidid: 0000-0003-4521-4507 surname: Pan fullname: Pan, Shilie email: slpan@ms.xjb.ac.cn organization: Xinjiang Key Laboratory of Electronic Information Materials and Devices |
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| SubjectTerms | ab initio evolutionary algorithm Birefringence Coefficients deep-ultraviolet Energy gap Evolutionary algorithms fluorooxoborates Multiple criterion nonlinear optical materials Predictions Second harmonic generation |
| Title | Prediction of Fluorooxoborates with Colossal Second Harmonic Generation (SHG) Coefficients and Extremely Wide Band Gaps: Towards Modulating Properties by Tuning the BO3/BO3F Ratio in Layers |
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