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Photoinduced Charge Shift in Li+-Doped Giant Nested Fullerenes

Cite this: J. Phys. Chem. C 2019, 123, 27, 16525–16532
Publication Date (Web):June 18, 2019
https://doi.org/10.1021/acs.jpcc.9b02354
Copyright © 2019 American Chemical Society
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Abstract

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Over the last years, carbon nano-onions (CNOs) have been in focus in material science research. Their red-shifted absorption allows utilizing CNOs as promising photosensitizers. We report here a systematic study of excited state properties of six double-layered Li+-doped fullerenes of Ih symmetry: [[email protected]60@C240]+, [[email protected]60@C540]+, [[email protected]60@C960]+, [[email protected]240@C540]+, [[email protected]240@C960]+, and [[email protected]540@C960]+. On the basis of time-dependent density functional theory calculations, we show that the long-wave absorption by the Li+-doped species leads to charge transfer (CT) between the inner and the outer shells unlike their neutral double-layered precursors. The CT energy depends strongly on the size of the concentric fullerenes and it can easily be tuned by varying both the encapsulated metal ion and the size of the shells. Two types of low-lying excited states are identified: (1) capacitor-like structures, as Li+@C60–@C240+, with alternating positive and negative charges, and (2) states, where the positive charge is delocalized over the outer shell, as in [email protected]240@C540+. We suggest a simple expression to estimate the energy difference of these excited states and to predict the type of the lowest CT state in nested fullerenes. The effect of nature of the encapsulated ion on the CT state energies is considered. The highest occupied molecular orbital–lowest unoccupied molecular orbital transition energy is found to vary significantly when going from [[email protected]60@C240]+ to [[email protected]540@C960]+.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.9b02354.

  • Methods description; formation energy of the CNOs, the interaction energies between the CNOs layers, and the superadditivity energies; comparison of electronic properties calculated by semiempirical methods and TDA/DFT; vertical IP and vertical EA values for fullerenes; HOMO–LUMO gap in the CNOs; electronic properties of triplet excited states of [[email protected]60@C240]+; calculated absorption spectra for C60@C240 and [[email protected]60@C240]+; and frontier molecular orbitals for [[email protected]240@C540]+ and [[email protected]240@C540]+ (PDF)

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Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

Cited By

This article is cited by 10 publications.

  1. A. J. Stasyuk, O. A. Stasyuk, M. Solà, A. A. Voityuk. Electron Transfer in a Li+-Doped Zn-Porphyrin–[10]CPP⊃Fullerene Junction and Charge-Separated Bands with Opposite Response to Polar Environments. The Journal of Physical Chemistry B 2020, 124 (41) , 9095-9102. https://doi.org/10.1021/acs.jpcb.0c05204
  2. Jesús Antonio Luque-Urrutia, Thalía Ortiz-García, Miquel Solà, Albert Poater. Green Energy by Hydrogen Production from Water Splitting, Water Oxidation Catalysis and Acceptorless Dehydrogenative Coupling. Inorganics 2023, 11 (2) , 88. https://doi.org/10.3390/inorganics11020088
  3. O. A. Stasyuk, A. J. Stasyuk, M. Solà, A. A. Voityuk. Photoinduced electron transfer in host–guest complexes of double nanohoops. Journal of Nanostructure in Chemistry 2022, 46 https://doi.org/10.1007/s40097-022-00518-w
  4. Simon Zank, Jesús M. Fernández‐García, Anton J. Stasyuk, Alexander A. Voityuk, Marcel Krug, Miquel Solà, Dirk M. Guldi, Nazario Martín. Initiating Electron Transfer in Doubly Curved Nanographene Upon Supramolecular Complexation of C 60. Angewandte Chemie 2022, 134 (7) https://doi.org/10.1002/ange.202112834
  5. Simon Zank, Jesús M. Fernández‐García, Anton J. Stasyuk, Alexander A. Voityuk, Marcel Krug, Miquel Solà, Dirk M. Guldi, Nazario Martín. Initiating Electron Transfer in Doubly Curved Nanographene Upon Supramolecular Complexation of C 60. Angewandte Chemie International Edition 2022, 61 (7) https://doi.org/10.1002/anie.202112834
  6. A. J. Stasyuk, O. A. Stasyuk, M. Solà, A. A. Voityuk. Photoinduced electron transfer in mechanically interlocked suit[3]ane systems. Journal of Materials Chemistry C 2021, 9 (30) , 9436-9445. https://doi.org/10.1039/D1TC01673C
  7. Olga A. Stasyuk, Anton J. Stasyuk, Miquel Solà, Alexander A. Voityuk. [10]CPP‐Based Inclusion Complexes of Charged Fulleropyrrolidines. Effect of the Charge Location on the Photoinduced Electron Transfer. Chemistry – A European Journal 2021, 27 (34) , 8737-8744. https://doi.org/10.1002/chem.202005516
  8. Alireza Aghajamali, Amir Karton. Comparative Study of Carbon Force Fields for the Simulation of Carbon Onions. Australian Journal of Chemistry 2021, 74 (10) , 709-714. https://doi.org/10.1071/CH21172
  9. Jesús Antonio Luque‐Urrutia, Albert Poater, Miquel Solà. Do Carbon Nano‐onions Behave as Nanoscopic Faraday Cages? A Comparison of the Reactivity of C 60 , C 240 , C 60 @C 240 , Li + @C 60 , Li + @C 240 , and Li + @C 60 @C 240. Chemistry – A European Journal 2020, 26 (4) , 804-808. https://doi.org/10.1002/chem.201904650
  10. Anton J. Stasyuk, Olga A. Stasyuk, Miquel Solà, Alexander A. Voityuk. Hypsochromic solvent shift of the charge separation band in ionic donor–acceptor Li + @C 60 ⊂[10]CPP. Chemical Communications 2019, 55 (75) , 11195-11198. https://doi.org/10.1039/C9CC05787K

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