Second-Order Nonlinear Optical Response of Electron Donor–Acceptor Hybrids Formed between Corannulene and Metallofullerenes
A charge transfer (CT) complex was formed between C20H10 and Li+@C60 in the ground state by the concave–convex π–π CT interaction. Herein, the structures, binding interactions, electronic absorption spectra, and first hyperpolarizabilities of a series of Li+ and Li atom in contact with C60 have been...
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| Published in | Journal of physical chemistry. C Vol. 119; no. 44; pp. 24965 - 24975 |
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| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
05.11.2015
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1932-7447 1932-7455 1932-7455 |
| DOI | 10.1021/acs.jpcc.5b06870 |
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| Abstract | A charge transfer (CT) complex was formed between C20H10 and Li+@C60 in the ground state by the concave–convex π–π CT interaction. Herein, the structures, binding interactions, electronic absorption spectra, and first hyperpolarizabilities of a series of Li+ and Li atom in contact with C60 have been explored with density functional theory methods. It is found that independent of the doping position, doping Li atom can significantly narrow the wide gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) (E gap = 2.82 eV) of the pure C20H10/C60 in the range of 0.86–0.99 eV. Among them, the Li-doped outer isomer C20H10/LiC60 can exhibit the intriguing n-type characteristic, where a high energy level containing the excess electron is introduced as the new HOMO orbital in the original gap of C20H10/C60. Furthermore, the diffuse excess electron also brings C20H10/C60 the considerable first hyperpolarizability, which is 3.53 × 10–29 esu. When Li+ and Li were encapsulated into the C60 cage, inner complexes C20H10/Li+@C60 and C20H10/Li@C60 of enhanced static first hyperpolarizabilities (5.39 and 2.13 × 10–29 esu, respectively) are also delivered due to that encapsulated Li+@C60 and Li@C60 show enhanced electron acceptability as compared to pristine C60, leading to more obvious intermolecular CT transitions. From a certain point of view, such systems can be considered as high-performance NLO materials that combine the basic characteristics of a classical donor–acceptor superstructure and systems with cations and easily polarizable excess electrons. |
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| AbstractList | A charge transfer (CT) complex was formed between C₂₀H₁₀ and Li⁺@C₆₀ in the ground state by the concave–convex π–π CT interaction. Herein, the structures, binding interactions, electronic absorption spectra, and first hyperpolarizabilities of a series of Li⁺ and Li atom in contact with C₆₀ have been explored with density functional theory methods. It is found that independent of the doping position, doping Li atom can significantly narrow the wide gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) (Egₐₚ = 2.82 eV) of the pure C₂₀H₁₀/C₆₀ in the range of 0.86–0.99 eV. Among them, the Li-doped outer isomer C₂₀H₁₀/LiC₆₀ can exhibit the intriguing n-type characteristic, where a high energy level containing the excess electron is introduced as the new HOMO orbital in the original gap of C₂₀H₁₀/C₆₀. Furthermore, the diffuse excess electron also brings C₂₀H₁₀/C₆₀ the considerable first hyperpolarizability, which is 3.53 × 10–²⁹ esu. When Li⁺ and Li were encapsulated into the C₆₀ cage, inner complexes C₂₀H₁₀/Li⁺@C₆₀ and C₂₀H₁₀/Li@C₆₀ of enhanced static first hyperpolarizabilities (5.39 and 2.13 × 10–²⁹ esu, respectively) are also delivered due to that encapsulated Li⁺@C₆₀ and Li@C₆₀ show enhanced electron acceptability as compared to pristine C₆₀, leading to more obvious intermolecular CT transitions. From a certain point of view, such systems can be considered as high-performance NLO materials that combine the basic characteristics of a classical donor–acceptor superstructure and systems with cations and easily polarizable excess electrons. A charge transfer (CT) complex was formed between C20H10 and Li+@C60 in the ground state by the concave–convex π–π CT interaction. Herein, the structures, binding interactions, electronic absorption spectra, and first hyperpolarizabilities of a series of Li+ and Li atom in contact with C60 have been explored with density functional theory methods. It is found that independent of the doping position, doping Li atom can significantly narrow the wide gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) (E gap = 2.82 eV) of the pure C20H10/C60 in the range of 0.86–0.99 eV. Among them, the Li-doped outer isomer C20H10/LiC60 can exhibit the intriguing n-type characteristic, where a high energy level containing the excess electron is introduced as the new HOMO orbital in the original gap of C20H10/C60. Furthermore, the diffuse excess electron also brings C20H10/C60 the considerable first hyperpolarizability, which is 3.53 × 10–29 esu. When Li+ and Li were encapsulated into the C60 cage, inner complexes C20H10/Li+@C60 and C20H10/Li@C60 of enhanced static first hyperpolarizabilities (5.39 and 2.13 × 10–29 esu, respectively) are also delivered due to that encapsulated Li+@C60 and Li@C60 show enhanced electron acceptability as compared to pristine C60, leading to more obvious intermolecular CT transitions. From a certain point of view, such systems can be considered as high-performance NLO materials that combine the basic characteristics of a classical donor–acceptor superstructure and systems with cations and easily polarizable excess electrons. |
| Author | Qiu, Yong-Qing Lu, Hui-Zhe Wang, Li Wang, Wen-Yong |
| AuthorAffiliation | China Agricultural University Institute of Functional Material Chemistry, Faculty of Chemistry Northeast Normal University Department of Applied Chemistry |
| AuthorAffiliation_xml | – name: Department of Applied Chemistry – name: China Agricultural University – name: Northeast Normal University – name: Institute of Functional Material Chemistry, Faculty of Chemistry |
| Author_xml | – sequence: 1 givenname: Li surname: Wang fullname: Wang, Li – sequence: 2 givenname: Wen-Yong surname: Wang fullname: Wang, Wen-Yong – sequence: 3 givenname: Yong-Qing surname: Qiu fullname: Qiu, Yong-Qing email: qiuyq466@nenu.edu.cn – sequence: 4 givenname: Hui-Zhe surname: Lu fullname: Lu, Hui-Zhe email: luhz2008@yahoo.com.cn |
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| Title | Second-Order Nonlinear Optical Response of Electron Donor–Acceptor Hybrids Formed between Corannulene and Metallofullerenes |
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