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
1. [1]
  Qianqian Liu , Xing Du , Wanfei Li , Wei-Lin Dai , Bo Liu . Synergistic Effects of Internal Electric and Dipole Fields in SnNb₂O₆/Nitrogen-Enriched C₃N₅ S-Scheme Heterojunction for Boosting Photocatalytic Performance. Acta Physico-Chimica Sinica, 2024, 40(10): 2311016-. doi: 10.3866/PKU.WHXB202311016
2. [2]
  Zhuoming Liang , Ming Chen , Zhiwen Zheng , Kai Chen . Multidimensional Studies on Ketone-Enol Tautomerism of 1,3-Diketones By ¹H NMR. University Chemistry, 2024, 39(7): 361-367. doi: 10.3866/PKU.DXHX202311029
3. [3]
  Donghui PAN , Yuping XU , Xinyu WANG , Lizhen WANG , Junjie YAN , Dongjian SHI , Min YANG , Mingqing CHEN . Preparation and in vivo tracing of ⁶⁸Ga-labeled PM_2.5 mimetic particles for positron emission tomography imaging. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 669-676. doi: 10.11862/CJIC.20230468
4. [4]
  Xue Xin , Qiming Qu , Islam E. Khalil , Yuting Huang , Mo Wei , Jie Chen , Weina Zhang , Fengwei Huo , Wenjing Liu . Hetero-phase zirconia encapsulated with Au nanoparticles for boosting electrocatalytic nitrogen reduction. Chinese Chemical Letters, 2024, 35(5): 108654-. doi: 10.1016/j.cclet.2023.108654
5. [5]
  Guorong Li , Yijing Wu , Chao Zhong , Yixin Yang , Zian Lin . Predesigned covalent organic framework with sulfur coordination: Anchoring Au nanoparticles for sensitive colorimetric detection of Hg(Ⅱ). Chinese Chemical Letters, 2024, 35(5): 108904-. doi: 10.1016/j.cclet.2023.108904
6. [6]
  Huihui LIU , Baichuan ZHAO , Chuanhui WANG , Zhi WANG , Congyun ZHANG . Green synthesis of MIL-101/Au composite particles and their sensitivity to Raman detection of thiram. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 2021-2030. doi: 10.11862/CJIC.20240059
7. [7]
  Peng ZHOU , Xiao CAI , Qingxiang MA , Xu LIU . Effects of Cu doping on the structure and optical properties of Au₁₁(dppf)₄Cl₂ nanocluster. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1254-1260. doi: 10.11862/CJIC.20240047
8. [8]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028
9. [9]
  Bing LIU , Huang ZHANG , Hongliang HAN , Changwen HU , Yinglei ZHANG . Visible light degradation of methylene blue from water by triangle Au@TiO₂ mesoporous catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 941-952. doi: 10.11862/CJIC.20230398
10. [10]
  Gengchen Guo , Tianyu Zhao , Ruichang Sun , Mingzhe Song , Hongyu Liu , Sen Wang , Jingwen Li , Jingbin Zeng . Au-Fe₃O₄ dumbbell-like nanoparticles based lateral flow immunoassay for colorimetric and photothermal dual-mode detection of SARS-CoV-2 spike protein. Chinese Chemical Letters, 2024, 35(6): 109198-. doi: 10.1016/j.cclet.2023.109198
11. [11]
  Liang MA , Honghua ZHANG , Weilu ZHENG , Aoqi YOU , Zhiyong OUYANG , Junjiang CAO . Construction of highly ordered ZIF-8/Au nanocomposite structure arrays and application of surface-enhanced Raman spectroscopy. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1743-1754. doi: 10.11862/CJIC.20240075
12. [12]
  Yunting Shang , Yue Dai , Jianxin Zhang , Nan Zhu , Yan Su . Something about RGO (Reduced Graphene Oxide). University Chemistry, 2024, 39(9): 273-278. doi: 10.3866/PKU.DXHX202306050
13. [13]
  Zhihuan XU , Qing KANG , Yuzhen LONG , Qian YUAN , Cidong LIU , Xin LI , Genghuai TANG , Yuqing LIAO . Effect of graphene oxide concentration on the electrochemical properties of reduced graphene oxide/ZnS. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1329-1336. doi: 10.11862/CJIC.20230447
14. [14]
  Hao Wu , Zhen Liu , Dachang Bai . ¹H NMR Spectrum of Amide Compounds. University Chemistry, 2024, 39(3): 231-238. doi: 10.3866/PKU.DXHX202309020
15. [15]
  Tengjiao Wang , Tian Cheng , Rongjun Liu , Zeyi Wang , Yuxuan Qiao , An Wang , Peng Li . Conductive Hydrogel-based Flexible Electronic System: Innovative Experimental Design in Flexible Electronics. University Chemistry, 2024, 39(4): 286-295. doi: 10.3866/PKU.DXHX202309094
16. [16]
  Zhuo WANG , Junshan ZHANG , Shaoyan YANG , Lingyan ZHOU , Yedi LI , Yuanpei LAN . Preparation and photocatalytic performance of CeO₂-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1708-1718. doi: 10.11862/CJIC.20240067
17. [17]
  Zhenlin Zhou , Siyuan Chen , Yi Liu , Chengguo Hu , Faqiong Zhao . A New Program of Voltammetry Experiment Teaching Based on Laser-Scribed Graphene Electrode. University Chemistry, 2024, 39(2): 358-370. doi: 10.3866/PKU.DXHX202308049
18. [18]
  Rui Gao , Ying Zhou , Yifan Hu , Siyuan Chen , Shouhong Xu , Qianfu Luo , Wenqing Zhang . Design, Synthesis and Performance Experiment of Novel Photoswitchable Hybrid Tetraarylethenes. University Chemistry, 2024, 39(5): 125-133. doi: 10.3866/PKU.DXHX202310050
19. [19]
  Jinkang Jin , Yidian Sheng , Ping Lu , Zhan Lu . Introducing a Website for Learning Nuclear Magnetic Resonance (NMR) Spectrum Analysis. University Chemistry, 2024, 39(11): 388-396. doi: 10.12461/PKU.DXHX202403054
20. [20]
  Jing SU , Bingrong LI , Yiyan BAI , Wenjuan JI , Haiying YANG , Zhefeng Fan . Highly sensitive electrochemical dopamine sensor based on a highly stable In-based metal-organic framework with amino-enriched pores. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1337-1346. doi: 10.11862/CJIC.20230414

Get Citation

PDF

XML

Metrics

PDF Downloads(12)
Abstract views(529)
HTML views(97)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

Metrics

通讯作者: 陈斌, bchen63@163.com

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