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Magneto-luminescent molecules have significant applications in data storage and quantum computing. However, design of these bi-functional molecules coupled with magnetic behavior and photoluminescence is still challenging. In this work, we report a metallofullerene DyErScN@Ⅰh-C80 exhibiting single-molecule magnet (SMM) behavior and near-infrared emission. For DyErScN@Ⅰh-C80, two functional lanthanide metal ions of Dy3+ (SMM function) and Er3+ (luminescent function) are integrated inside a fullerene cage using a trimetallic nitride template, and its structure has been unambiguously characterized by single-crystal X-ray diffraction. Magnetic measurements revealed that DyErScN@Ⅰh-C80 behaves as a SMM with a blocking temperature up to 9 K resulting from the intramolecular magnetic interaction between Dy3+ and Er3+ ions. Moreover, DyErScN@Ⅰh-C80 exhibits temperature-dependent near-infrared emission around 1.5 µm with multiple splitting peaks from Er3+, which arises from the influence of Dy3+ ion. This study provides a new strategy to synthesize new magneto-luminescent molecule materials.
Ardavan, A.; Rival, O.; Morton, J. J. L.; Blundell, S. J.; Tyryshkin, A. M.; Timco, G. A.; Winpenny, R. E. P. Will spin-relaxation times in molecular magnets permit quantum information processing? Phys. Rev. Lett. 2007, 98, 057201.
Bogani, L.; Wernsdorfer, W. Molecular spintronics using single-molecule magnets. Nat. Mater. 2008, 7, 179-186.
Aromí, G.; Aguilà, D.; Gamez, P.; Luis, F.; Roubeau, O. Design of magnetic coordination complexes for quantum computing. Chem. Soc. Rev. 2012, 41, 537-546.
Liu, Y. X.; Wang, D. S.; Shi, J. X.; Peng, Q.; Li, Y. D. Magnetic tuning of upconversion luminescence in lanthanide-doped bifunctional nanocrystals. Angew. Chem., Int. Ed. 2013, 52, 4366-4369.
Zhou, N.; Xu, B.; Gan, L.; Zhang, J. P.; Han, J. B.; Zhai, T. Y. Narrowband spectrally selective near-infrared photodetector based on up-conversion nanoparticles used in a 2D hybrid device. J. Mater. Chem. C 2017, 5, 1591-1595.
Bazalova, O.; Kvicalova, M.; Valkova, T.; Slaby, P.; Bartos, P.; Netusil, R.; Tomanova, K.; Braeunig, P.; Lee, H. J.; Sauman, I. et al. Cryptochrome 2 mediates directional magnetoreception in cockroaches. Proc. Natl. Acad. Sci. USA 2016, 113, 1660-1665.
Maeda, K.; Henbest, K. B.; Cintolesi, F.; Kuprov, I.; Rodgers, C. T.; Liddell, P. A.; Gust, D.; Timmel, C. R.; Hore, P. J. Chemical compass model of avian magnetoreception. Nature 2008, 453, 387-390.
Long, J.; Guari, Y.; Ferreira, R. A. S.; Carlos, L. D.; Larionova, J. Recent advances in luminescent lanthanide based single-molecule magnets. Coord. Chem. Rev. 2018, 363, 57-70.
Bi, Y.; Chen, C.; Zhao, Y. F.; Zhang, Y. Q.; Jiang, S. D.; Wang, B. W.; Han, J. B.; Sun, J. L.; Bian, Z. Q.; Wang, Z. M. et al. Thermostability and photoluminescence of dy(Ⅲ) single-molecule magnets under a magnetic field. Chem. Sci. 2016, 7, 5020-5031.
Jia, J. H.; Li, Q. W.; Chen, Y. C.; Liu, J. L.; Tong, M. L. Luminescent single-molecule magnets based on lanthanides: Design strategies, recent advances and magneto-luminescent studies. Coord. Chem. Rev. 2019, 378, 365-381.
Wang, Z. Y.; Izumi, N.; Nakanishi, Y.; Koyama, T.; Sugai, T.; Tange, M.; Okazaki, T.; Shinohara, H. Near-infrared photoluminescence properties of endohedral mono- and dithulium metallofullerenes. ACS Nano 2016, 10, 4282-4287.
Kodama, T.; Ohnishi, M.; Park, W.; Shiga, T.; Park, J.; Shimada, T.; Shinohara, H.; Shiomi, J.; Goodson, K. E. Modulation of thermal and thermoelectric transport in individual carbon nanotubes by fullerene encapsulation. Nat. Mater. 2017, 16, 892-897.
Liu, F. P.; Krylov, D. S.; Spree, L.; Avdoshenko, S. M.; Samoylova, N. A.; Rosenkranz, M.; Kostanyan, A.; Greber, T.; Wolter, A. U. B.; Büchner, B. et al. Single molecule magnet with an unpaired electron trapped between two lanthanide ions inside a fullerene. Nat. Commun. 2017, 8, 16098.
Westerström, R.; Dreiser, J.; Piamonteze, C.; Muntwiler, M.; Weyeneth, S.; Brune, H.; Rusponi, S.; Nolting, F.; Popov, A.; Yang, S. F. et al. An endohedral single-molecule magnet with long relaxation times: DySc2N@C80. J. Am. Chem. Soc. 2012, 134, 9840-9843.
Krylov, D. S.; Liu, F.; Avdoshenko, S. M.; Spree, L.; Weise, B.; Waske, A.; Wolter, A. U. B.; Büchner, B.; Popov, A. A. Record-high thermal barrier of the relaxation of magnetization in the nitride clusterfullerene Dy2ScN@C80-Ⅰh. Chem. Commun. 2017, 53, 7901-7904.
Rincón-García, L.; Ismael, A. K.; Evangeli, C.; Grace, I.; Rubio-Bollinger, G.; Porfyrakis, K.; Agraït, N.; Lambert, C. J. Molecular design and control of fullerene-based bi-thermoelectric materials. Nat. Mater. 2016, 15, 289-293.
Wu, B.; Wang, T. S.; Feng, Y. Q.; Zhang, Z. X.; Jiang, L.; Wang, C. R. Molecular magnetic switch for a metallofullerene. Nat. Commun. 2015, 6, 6468.
Ito, Y.; Okazaki, T.; Okubo, S.; Akachi, M.; Ohno, Y.; Mizutani, T.; Nakamura, T.; Kitaura, R.; Sugai, T.; Shinohara, H. Enhanced 1520 nm photoluminescence from Er3+ ions in di-erbium-carbide metallofullerenes (Er2C2)@C82 (isomers Ⅰ, Ⅱ, and Ⅲ). ACS Nano 2007, 1, 456-462.
Macfarlane, R. M.; Bethune, D. S.; Stevenson, S.; Dorn, H. C. Fluorescence spectroscopy and emission lifetimes of Er3+ in ErxSc3−xN@C80 (x = 1-3). Chem. Phys. Lett. 2001, 343, 229-234.
Olmstead, M. M.; de Bettencourt-Dias, A.; Duchamp, J. C.; Stevenson, S.; Dorn, H. C.; Balch, A. L. Isolation and crystallographic characterization of ErSc2N@C80: An endohedral fullerene which crystallizes with remarkable internal order. J. Am. Chem. Soc. 2000, 122, 12220-12226.
Westerström, R.; Dreiser, J.; Piamonteze, C.; Muntwiler, M.; Weyeneth, S.; Krämer, K.; Liu, S. X.; Decurtins, S.; Popov, A.; Yang, S. F. et al. Tunneling, remanence, and frustration in dysprosium-based endohedral single-molecule magnets. Phys. Rev. B 2014, 89, 060406.
Dreiser, J.; Westerström, R.; Zhang, Y.; Popov, A. A.; Dunsch, L.; Krämer, K.; Liu, S. X.; Decurtins, S.; Greber, T. The metallofullerene field-induced single-ion magnet HoSc2N@C80. Chem. -〞Eur. J. 2014, 20, 13536-13540.
Chen, Y. C.; Liu, J. L.; Ungur, L.; Liu, J.; Li, Q. W.; Wang, L. F.; Ni, Z. P.; Chibotaru, L. F.; Chen, X. M.; Tong, M. L. Symmetry-supported magnetic blocking at 20 K in pentagonal bipyramidal Dy(Ⅲ) single-ion magnets. J. Am. Chem. Soc. 2016, 138, 2829-2837.
Aquilante, F.; Autschbach, J.; Carlson, R. K.; Chibotaru, L. F.; Delcey, M. G.; De Vico, L.; Fdez. Galván, I.; Ferré, N.; Frutos, L. M.; Gagliardi, L. et al. MOLCAS 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table. J. Comput. Chem. 2016, 37, 506-541.
Lines, M. E. Orbital angular momentum in the theory of paramagnetic clusters. J. Chem. Phys. 1971, 55, 2977-2984.
Ungur, L.; van den Heuvel, W.; Chibotaru, L. F. Ab initio investigation of the non-collinear magnetic structure and the lowest magnetic excitations in dysprosium triangles. New J. Chem. 2009, 33, 1224-1230.
Chibotaru, L. F.; Ungur, L.; Soncini, A. The origin of nonmagnetic kramers doublets in the ground state of dysprosium triangles: Evidence for a toroidal magnetic moment. Angew. Chem., Int. Ed. 2008, 47, 4126-4129.
Chibotaru, L. F.; Ungur, L.; Aronica, C.; Elmoll, H.; Pilet, G.; Luneau, D. Structure, magnetism, and theoretical study of a mixed-valence Co3ⅡCo4Ⅲ heptanuclear wheel: Lack of SMM behavior despite negative magnetic anisotropy. J. Am. Chem. Soc. 2008, 130, 12445-12455.
Dantelle, G.; Tiwari, A.; Rahman, R.; Plant, S. R.; Porfyrakis, K.; Mortier, M.; Taylor, R. A.; Briggs, G. A. D. Optical properties of Er3+ in fullerenes and in β-PbF2 single-crystals. Opt. Mater. 2009, 32, 251-256.
Wybourne, B. G. Spectroscopic Properties of Rare Earths; Interscience Publishers: New York, 1965.
Wybourne, B. G.; Smentek, L. Optical Spectroscopy of Lanthanides: Magnetic and Hyperfine Interactions; CRC Press: Boca Raton, 2007.
Jones, M. A. G.; Morton, J. J. L.; Taylor, R. A.; Ardavan, A.; Briggs, G. A. D. PL, magneto-PL and PLE of the trimetallic nitride template fullerene Er3N@C80. Phys. Status Solidi B 2006, 243, 3037-3041.
Tiwari, A.; Dantelle, G.; Porfyrakis, K.; Ardavan, A.; Briggs, G. A. D. Temperature-dependent photoluminescence study of ErSc2N@C80 and Er2ScN@C80 fullerenes. Phys. Status Solidi B 2008, 245, 1998-2001.
Jones, M. A. G.; Taylor, R. A.; Ardavan, A.; Porfyrakis, K.; Briggs, G. A. D. Direct optical excitation of a fullerene-incarcerated metal ion. Chem. Phys. Lett. 2006, 428, 303-306.
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