Citation: ZHAO Yeliang, WANG Bing. Effect of Substrate on the Electron Spin Resonance Spectra of N@C₆₀ Molecules[J]. Acta Physico-Chimica Sinica, ;2018, 34(12): 1312-1320. doi: 10.3866/PKU.WHXB201803011 shu

Effect of Substrate on the Electron Spin Resonance Spectra of N@C₆₀ Molecules

ZHAO Yeliang ,
WANG Bing ^,

Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, P. R. China

Corresponding author: WANG Bing, bwang@ustc.edu.cn
Received Date: 23 January 2018
Revised Date: 27 February 2018
Accepted Date: 27 February 2018
Available Online: 1 December 2018
Fund Project: The project was supported by the National Key Research and Development Program of China (2016YFA0200603)the National Key Research and Development Program of China 2016YFA0200603

The controlled coupling of spin centers is essential in the construction of molecular spin-based quantum information processing architectures. A major challenge is to induce the requisite coupling between two adjacent spins, while protecting them from neighboring spins and other environmental interactions. Owing to their native spin properties, endohedral fullerenes are attractive for use as elements in quantum information processing architectures. N@C₆₀ is an endohedral fullerene molecule with a highly reactive nitrogen atom at the center of the carbon cage. The endohedral nitrogen is atomic and not covalently bound to the cage atoms; therefore, the nitrogen atom is chemically inert toward the outer environment. Owing to its remarkably long electron-spin lifetimes and sharp resonances, N@C₆₀ has exceptional properties for quantum computing. The thermal stability and molecular structure of N@C₆₀ make it a useful embodiment of a quantum bit — a fundamental element for a quantum computer. Several future quantum computer architectures based on N@C₆₀ have been proposed, one of which is a two-dimensional, quantum-bit array on specific substrates. However, a challenging yet important task is to understand the effect of various substrates on the spin properties of the endohedral fullerene, since the interaction between the endohedral fullerene and the substrate may largely affect the spin characters of the endohedral N atom. The fabrication of an endohedral fullerene molecular array on substrates is also a challenge because high-temperature methods such as evaporation will cause decomposition of N@C₆₀. Here we report our investigation on the electron spin resonance (ESR) of N@C₆₀ molecules on various substrates such as Au(111), Si(111), and SiO₂. In this study, N@C₆₀ was prepared using the ion implantation method, and enrichment was performed using a multistep and recycling high-performance liquid chromatography (HPLC) system with a Cosmosil Buckyprep column. N@C₆₀ molecular films on Au(111) substrates were prepared at room temperature. In addition, scanning tunneling microscope (STM) topography of the N@C₆₀/C₆₀ monolayer on Au(111) was obtained at a sample temperature of 5 K in ultra high vacuum (UHV). We found that the ESR signal of the N@C₆₀ molecules decreases rapidly and disappeared approximately 360 min after the deposition of N@C₆₀ on Au(111). In comparison, the ESR signal was maintained for a longer time on the Si(111) and SiO₂ substrates. We propose that coupling between the Au(111) substrate and the endohedral N atoms quenches the ESR signal of the endohedral N atom, while the Si(111) and SiO₂ substrates have a smaller effect on the ESR signal. This result offers useful information for the design of basic quantum computer architectures.
- Au(111),
- Endohedral fullerene,
- Scanning tunneling microscopy,
- Electron spin Resonance,
- Decohence,
- Dipolar coupling
1. [1]
  Chaur, M. N.; Athans, A. J.; Echegoyen, L. Tetrahedron 2008, 64, 11387. doi: 10.1016/j.tet.2008.08.060 doi: 10.1016/j.tet.2008.08.060
2. [2]
  Stevenson, S.; Rice, G.; Glass, T.; Harich, K.; Cromer, F.; Jordan, M. R.; Craft, J.; Hadju, E.; Bible, R.; Olmstead, M. M.; et al. Nature 1999, 401, 55. doi: 10.1038/43415 doi: 10.1038/43415
3. [3]
  Wang, C. R.; Kai, T.; Tomiyama, T.; Yoshida, T.; Kobayashi, Y.; Nishibori, E.; Takata, M.; Sakata, M.; Shinohara, H. Angew. Chem. Int. Ed. 2001, 40, 397. doi: 10.1002/1521-3773(20010119)40:2<397::AID-ANIE397>3.0.CO;2-3 doi: 10.1002/1521-3773(20010119)40:2<397::AID-ANIE397>3.0.CO;2-3
4. [4]
  Chai, Y.; Guo, T.; Jin, C.; Haufler, R. E.; Chibante, L. P. F.; Fure, J.; Wang, L.; Alford, J. M.; Smalley, R. E. J. Phys. Chem. 1991, 95, 7564. doi: 10.1021/j100173a002 doi: 10.1021/j100173a002
5. [5]
  Yamada, M.; Akasaka, T.; Nagase, S. Acc. Chem. Res. 2010, 43 (1), 92. doi: 10.1021/ar900140n doi: 10.1021/ar900140n
6. [6]
  Sun, B.; Li, M.; Luo, H.; Shi, Z.; Gu, Z. Electrochim. Acta 2002, 47, 3545. doi: 10.1016/S0013-4686(02)00355-9 doi: 10.1016/S0013-4686(02)00355-9
7. [7]
  Liu, X. S.; Lei, D.; Gan, L. H. Acta Phys. -Chim. Sin. 2016, 32, 929. doi: 10.3866/PKU.WHXB201601221
8. [8]
  Sun, D. Y.; Liu, Z. Y.; Guo, X. H.; Xu, W. G.; Ji, Y. P.; Liu, S. Y. Acta Phys. -Chim. Sin. 1996, 12, 1110. doi: 10.3866/PKU.WHXB19961213
9. [9]
  Sun, D. Y.; Liu, Z. Y.; Guo, X. H.; Xu, W. G.; Ji, Y. P.; Liu, S. Y. Acta Phys. -Chim. Sin. 1996, 12, 873. doi: 10.3866/PKU.WHXB19961003
10. [10]
  Alvarez, M. M.; Gillan, E. G.; Holczer, K.; Kaner, R. B.; Min, K. S.; Whetten, R. L. J. Phys. Chem. 1991, 95, 10561. doi: 10.1021/j100179a014 doi: 10.1021/j100179a014
11. [11]
  Stevenson, S.; Mackey, M. A.; Stuart, M. A.; Phillips, J. P.; Easterling, M. L.; Chancellor, C. J.; Olmstead, M. M.; Balch, A. L. J. Am. Chem. Soc. 2008, 130, 11844. doi: 10.1021/ja803679u doi: 10.1021/ja803679u
12. [12]
  Saunders, M.; Jiménez-Vázquez, H. A.; Cross, R. J.; Poreda, R. J.; Science 1993, 259, 1428. doi: 10.1126/science.259.5100.1428 doi: 10.1126/science.259.5100.1428
13. [13]
  Saunders, M.; Cross, R. J.; Jiménez-Vázquez, H. A.; Shimshi, R.; Khong, A. Science 1996, 271, 1693. doi: 10.1126/science.271.5256.1693 doi: 10.1126/science.271.5256.1693
14. [14]
  Saunders, M.; Jiménez-Vázquez, H. A.; Cross, R. J.; Mroczkowski, S.; Freedberg, D. I.; Anet, F. A. L. Nature 1994, 367, 256. doi: 10.1038/367256a0 doi: 10.1038/367256a0
15. [15]
  Murphy, T. A.; Pawlik, Th; Weidinger, A.; Höhne, M.; Alcala, R.; Spaeth, J. M. Phys. Rev. Lett. 1996, 77, 1075. doi: 10.1103/PhysRevLett.77.1075 doi: 10.1103/PhysRevLett.77.1075
16. [16]
  Weidinger, A.; Waiblinger, M.; Pietzak, B.; Murphy, T. A. Appl. Phys. A 1998, 66, 287. doi: 10.1007/s003390050668 doi: 10.1007/s003390050668
17. [17]
  Dietel, E.; Hirsch, A.; Pietzak, B.; Waiblinger, M.; Lips, K.; Weidinger, A.; Gruss, A.; Dinse, K. J. Am. Chem. Soc. 1999, 121, 2432. doi: 10.1021/ja983812s doi: 10.1021/ja983812s
18. [18]
  Greer, J. C. Chem. Phys. Lett. 2000, 326, 567. doi: 10.1016/S0009-2614(00)00839-3 doi: 10.1016/S0009-2614(00)00839-3
19. [19]
  Harneit, W. Phys. Rev. A 2000, 65, 032322. doi: 10.1103/PhysRevA.65.032322 doi: 10.1103/PhysRevA.65.032322
20. [20]
  Pietzak, B.; Waiblinger, M.; Murphy, T. A.; Weidinger, A.; Höhne, M.; Dietel, E.; Hirsch, A. Chem. Phys. Lett. 1997, 279, 259. doi: 10.1016/S0009-2614(97)01100-7 doi: 10.1016/S0009-2614(97)01100-7
21. [21]
  Goedde, B.; Waiblinger, M.; Jakes, P.; Weiden, N.; Dinse, K.; Weidinger, A. Chem. Phys. Lett. 2001, 334, 12. doi: 10.1016/S0009-2614(00)01406-8 doi: 10.1016/S0009-2614(00)01406-8
22. [22]
  Wakahara, T.; Matsunaga, Y.; Katayama, A.; Maeda, Y.; Kako, M.; Akasaka, T.; Okamura, M.; Kato, T.; Choe, Y.; Kobayashi, K.; et al. Chem. Commun. 2003, 23, 2940. doi: 10.1039/B309470G doi: 10.1039/B309470G
23. [23]
  Liu, G.; Khlobystov, A. N.; Ardavan, A.; Briggs, G. A. D.; Porfyrakis, K. Chem. Phys. Lett. 2011, 508, 187. doi: 10.1016/j.cplett.2011.04.039 doi: 10.1016/j.cplett.2011.04.039
24. [24]
  Farrington, B. J.; Jevric, M.; Rance, G. A.; Ardavan, A.; Khlobystov, A. N.; Briggs, G. A. D.; Porfyrakis, K. Angew. Chem. Int. Ed. 2012, 51, 3587. doi: 10.1002/anie.201107490 doi: 10.1002/anie.201107490
25. [25]
  Liu, G.; Khlobystov, A. N.; Charalambidis, G.; Coutsolelos, A. G.; Briggs, G. A. D.; Porfyrakis, K. J. Am. Chem. Soc. 2012, 134, 1938. doi: 10.1021/ja209763u doi: 10.1021/ja209763u
26. [26]
  Liu, G.; Gimenez-Lopez, M.; Jevric, M.; Khlobystov, A. N.; Briggs, G. A. D.; Porfyrakis, K. J. Phys. Chem. B 2013, 117, 5925. doi: 10.1021/jp401582j doi: 10.1021/jp401582j
27. [27]
  Plant, S. R.; Jevric, M.; Morton, J. J. L.; Ardavan, A.; Khlobystov, A. N.; Briggs, G. A. D.; Porfyrakis, K. Chem. Sci. 2013, 4, 2971. doi: 10.1039/c3sc50395j doi: 10.1039/c3sc50395j
28. [28]
  Zhou, S.; Rasovic, I.; Briggs, G. A. D.; Porfyrakis, K. Chem. Commun. 2015, 51, 7096. doi: 10.1039/c5cc01459j doi: 10.1039/c5cc01459j
29. [29]
  Benjamin, S. C.; Ardavan, A.; Briggs, G. A. D.; Britz, D. A.; Gunlycke, D.; Jefferson, J.; Jones, M. A. G.; Leigh, D. F.; Lovett, B. W.; Khlobystov, A. N.; et al. J. Phys.: Condens. Matter 2006, 18, 867. doi: 10.1088/0953-8984/18/21/S12 doi: 10.1088/0953-8984/18/21/S12
30. [30]
  Waiblinger, M.; Lips, K.; Harneit, W.; Weidinger, A.; Dietel, E.; Hirsch, A. Phys. Rev. B 2001, 64, 159901. doi: 10.1103/PhysRevB.64.159901 doi: 10.1103/PhysRevB.64.159901
31. [31]
  Mauser, H.; Hirsch, A.; van Eikema Hommes, N. J. R.; Clark, T.; Pietzak, B.; Weidinger, A.; Dunsch, L. Angew. Chem. Int. Ed. 1997, 36, 2835. doi: 10.1002/anie.199728351 doi: 10.1002/anie.199728351
32. [32]
  Song, X.; Ma, Y.; Wang, C.; Luo, Y. Chem. Phys. Lett. 2011, 517, 199. doi: 10.1016/j.cplett.2011.10.045 doi: 10.1016/j.cplett.2011.10.045
33. [33]
  Jakes, P; Dinse, K; Meyer, C.; Harneit, W.; Weidinger, A. Phys. Chem. Chem. Phys. 2003, 5, 4080. doi: 10.1039/B308284A doi: 10.1039/B308284A
34. [34]
  Waiblinger, M.; Goedde, B.; Lips, K.; Harneit, W.; Jakes, P.; Weidinger, A.; Dinse, K. AIP Conf. Proc. 2000, 544, 195. doi: 10.1063/1.1342498 doi: 10.1063/1.1342498
35. [35]
  Warner, M.; Din, S.; Tupitsyn, I. S.; Morley, G. W.; Stoneham, A. M.; Gardener, J. A.; Wu, Z.; Fisher, A. J.; Heutz, S.; Kay, C. W. M.; et al. Nature 2013, 503, 504. doi: 10.1038/nature12597 doi: 10.1038/nature12597
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Effect of Substrate on the Electron Spin Resonance Spectra of N@C₆₀ Molecules