Effect of native carbon vacancies on evolution of defects in ZrC1-x under He ion irradiation and annealing

doi:10.1016/j.jmst.2022.01.004

Abstract

Abstract:

The dynamic study of radiation-induced defects with annealing is critical for the material design for next-generation nuclear energy systems. The native vacancy could affect the development of defects, which lacks study. In the present work, the as-hot pressed ZrC_1-_x (x=0, 0.15, 0.3) ceramics which comprised crystallites of a few microns in size with different amounts of carbon vacancies were irradiated by 540 keV He²⁺ ions at room temperature with a fluence of 1 × 10¹⁷/cm². The radiation-induced lattice expansion was found to be a common phenomenon in a sequence of ZrC_0.85≥ZrC_1.0>ZrC_0.7. Both X-ray and electron diffractions confirmed maintenance of structural integrity without amorphization after irradiation. Inside the irradiated region, only “black-dot” type defects, i.e., clusters of point defects were observed while no helium-induced cavities, cracks, or extended dislocations were detected. The as-irradiated ZrC_1-_x were then annealed at different high temperatures. Upon annealing at 800 °C, very tiny helium-induced cavities were found to be generated and the crystal lattice recovered to a great extent, especially for the sub-stoichiometric samples. While annealed at 1500 °C, all the samples almost fully recovered the crystal lattices close to those of as-hot pressed ones. Meanwhile, large cavities and extended dislocations were generated. With increasing amount of native carbon vacancies, the size of cavities increased while the length and density of extended dislocations decreased. Inverse changes of lattice parameters during irradiation and annealing processes have been interpreted by the kinetics of defects. Finally, the correlation between native vacancies and damage behavior is discussed.

Key words: Native carbon vacancies, Zirconium carbide, He ions irradiation, Helium bubbles, Dislocations

Weichao Bao, Xin-Gang Wang, Ying Lu, Ji-Xuan Liu, Shikuan Sun, Guo-Jun Zhang, Fangfang Xu. Effect of native carbon vacancies on evolution of defects in ZrC_1-_x under He ion irradiation and annealing[J]. J. Mater. Sci. Technol., 2022, 119: 87-97.

Figures/Tables 15

Fig. 1. The damage in dpa and He ions range for the implantation fluence of 1 × 1017/cm2 at 540 keV in ZrC1-x (x=0, 0.15, 0.3) which were calculated by SRIM with the mode of ‘Kinchin-Pease’.

Fig. 2. BSE images of as-hot pressed ZrC1.0 (a), ZrC0.85 (b) and ZrC0.7 (c), respectively.

Fig. 3. (a) GIXRD patterns of as-hot pressed, as-irradiated and as-annealed ZrC1-x (x=0, 0.15, 0.3) with a glancing angle of 2°; (b) Changing of crystal lattices of ZrC1-x (x=0, 0.15, 0.3) via irradiation and post-annealing with respect to lattice parameter a (left) and ∆a/a (right).

Fig. 4. Cross-sectional TEM images of as-irradiated ZrC1.0, ZrC0.85 and ZrC0.7 samples. (a-c) BF images; (d-f) SAD patterns of the damaged area marked by a yellow circle in (a-c); (g-i) BF images of the damaged area near the irradiated/non-irradiated interface.

Fig. 5. Cross-sectional TEM images of 800 °C-annealed ZrC1.0, ZrC0.85 and ZrC0.7. (a-c) BF images; (d-f) and (g-i) BF under-focused and over-focused images, respectively, of the damaged area close to the interface as marked by dashed blue squares in (a-c). (de-focus ± ～300 nm).

Fig. 6. Cross-sectional TEM images of 800 °C-annealed ZrC0.7. (a, b) BF under-focused and over-focused images, respectively, of the damaged area close to the interface. (de-focus ± ～1 µm).

Fig. 7. Cross-sectional TEM images of 1500 °C-annealed ZrC1.0, ZrC0.85 and ZrC0.7. (a, e, i) HAADF images at low magnification; (b, f, j) SAD patterns of the area outlined by green dashed circles in (a, e, i); (e, g, h) and (I, k, l) magnified HAADF and ADF images, respectively, showing cavities and extended dislocations near the interface between irradiated and non-irradiated area.

Fig. 8. Two-beam BF images of 1500 °C-annealed ZrC1.0 (a), ZrC0.85 (b) and ZrC0.7 (c), respectively, by using the (2¯00) reflection.

Table 1. Features of dislocations in 1500 °C-annealed ZrC1.0, ZrC0.85, and ZrC0.7.

Samples	Layered No.	Depth range	Features of dislocations
ZrC_1.0	1	0-630 nm	High density of small dislocation loops with a diameter of <20 nm; sporadic dislocations with a length of 50-150 nm (marked by the yellow dashed circle in Fig. 7(a)).
	2	630-1080 nm	Sparse long dislocations with a length of 150-400 nm; few dislocations with a diameter of <20 nm.
	3	1080-1330 nm	Severely damaged areas where individual defects can hardly be discernible.
ZrC_0.85	1	0-750 nm	Sporadic dislocations with a length of 50-100 nm (marked by the yellow dashed circle in Fig. 7(b)), and tiny dislocation loops with a diameter of ∼5 nm whose density became higher near the bottom of this layer.
	2	750-1100 nm	Sparse long dislocations with a length of 50-150 nm.
	3	1100-1280 nm	Dense short dislocations with a length of <50 nm along with dislocation loops of increased diameters (<20 nm).
ZrC_0.7	1	0-750 nm	No dislocations or loops at all.
ZrC_0.7	2	750-1400 nm	Dense small dislocation loops with a diameter of <20 nm; sporadic dislocations with a length of 50-150 nm (marked by the yellow dash circle in Fig. 7(c)).

Fig. 9. Cross-sectional TEM images of as-annealed ZrC1.0, ZrC0.85 and ZrC0.7. (a-c) and (d-f) BF under-focused images of 800 °C- and 1500 °C-annealed samples around the interface, respectively. (de-focus ± ～1 µm)

Fig. 10. Schematic drawing of different types of defects. (The He-Vacancy and vacancy clusters involve more atoms or vacancies, not only the numbers in the graphic.)

Table 2. Defect formation energies and migration barriers.

Empty Cell	C vacancy	C interstitial		Zr vacancy		Zr interstitial
Formation energy^a	0.93 eV	3.56 eV		7.19 eV		10.36 eV
Migration barriers^b	4.41 eV	0.27 eV		5.44 eV		4.41 eV
Empty Cell	He@C vacancy		He@Zr vacancy		He interstitial
Formation energy^c	0.80 eV		0.70 eV		4.22 eV
Migration barriers^c	2.85 eV		4.20 eV		0.7-0.8 eV
Empty Cell	C Frenkel pairs		Zr Frenkel pairs		Schottky defect
Formation energy^c	4.54 eV		17.69 eV		8.14 eV

Fig. 11. Cross-sectional TEM images of 1500 °C-annealed ZrC0.85 and ZrC0.7. (a, b) BF under-focused and over-focused images, respectively, of the unirradiated area in ZrC0.85; (c, d) BF under-focused and over-focused images, respectively, of the unirradiated area in ZrC0.7. (de-focus ± 300 nm)

Fig. 12. (a-c) BF under-focused images of 1500 °C-annealed ZrC1.0 at different areas; (d, e) BF under-focused images of 1500 ˚C-annealed ZrC0.85 and ZrC0.7, respectively. (deviation parameter s » 0, de-focus ± ～1 µm)

Fig. 13. Mechanism of annealing induced generation of extended dislocations with decoration of helium bubbles. (a) “black-dot” defects and He atoms inside the as-irradiated sample; (b) Growth of dislocations with He atoms moving around; (c) Growth of helium bubbles with removal of matrix atoms; (d) Movement of displaced matrix atoms driven by local stress; (e) Extended dislocations with decoration of helium bubbles.

References 51

[1]	G.S. Was, Fundamentals of Radiation Materials Science: Metals and Alloys, Springer, Berlin, 2007.
[2]	M.J. Zheng, I. Szlufarska, D. Morgan, J. Nucl. Mater. 471 (2016) 214-219. DOI URL
[3]	J.X. Xue, G.J. Zhang, L.P. Guo, H.B. Zhang, X.G. Wang, J. Zou, S.M. Peng, X.G. Long, J. Eur. Ceram. Soc. 34 (2014) 633-639. DOI URL
[4]	H.W. Hugosson, U. Jansson, B. Johansson, O. Eriksson, Chem. Phys. Lett. 333 (2001) 444-450. DOI URL
[5]	X.G. Wang, W.M. Guo, Y.M. Kan, G.J. Zhang, P.L. Wang, J. Eur. Ceram. Soc. 31 (2011) 1103-1111. DOI URL
[6]	Y. Katoh, G. Vasudevamurthy, T. Nozawa, L.L. Snead, J. Nucl. Mater. 441 (2013) 718-742. DOI URL
[7]	Z.J. Yu, X. Lv, S.Y. Lai, L. Yang, W.J. Lei, X.G. Luan, R. Riedel, J. Adv. Ceram. 8 (2019) 112-120. DOI URL
[8]	G.H. Reynolds, J. Nucl. Mater. 62 (1976) 9-16. DOI URL
[9]	K. Minato, T. Ogawa, K. Fukuda, H. Sekino, I. Kitagawa, N. Mita, J. Nucl. Mater. 249 (1995) 142-149. DOI URL
[10]	R.V. Sara, J. Am. Ceram. Soc. 48 (2010) 243-247. DOI URL
[11]	L.L. Snead, Y. Katoh, S. Kondo, J. Nucl. Mater. 399 (2010) 200-207. DOI URL
[12]	R.E. Bullock, J. Nucl. Mater. 125 (1984) 304-319. DOI URL
[13]	X. Wang, C. Xu, S. Hu, H. Zhang, X. Zhou, S. Peng, J. Nucl. Mater. 521 (2019) 146-154. DOI URL
[14]	M. Jiang, H.Y. Xiao, H.B. Zhang, S.M. Peng, C.H. Xu, Z.J. Liu, X.T. Zu, Acta Mater 110 (2016) 192-199. DOI URL
[15]	S. Pellegrino, L. Thomé, A. Debelle, S. Miro, P. Trocellier, Nucl. Instrum. Methods Phys. Res. 327 (2014) 103-107. DOI URL
[16]	S. Pellegrino, L. Thomé, A. Debelle, S. Miro, P. Trocellier, Nucl. Instrum. Methods Phys. Res. 307 (2013) 294-298. DOI URL
[17]	W.C. Bao, J.X. Liu, X.G. Wang, H.B. Zhang, J.X. Xue, S.K. Sun, F.F. Xu, J.M. Xue, G.J. Zhang, Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms 434 (2018) 23-28. DOI URL
[18]	S. Pellegrino, J.P. Crocombette, A. Debelle, T. Jourdan, P. Trocellier, L. Thome, Acta Mater 102 (2016) 79-87. DOI URL
[19]	D. Gosset, M. Dolle, D. Simeone, G. Baldinozzi, L. Thome, Nucl. Instrum. Meth- ods Phys. Res. Sect. B-Beam Interact. Mater. Atoms 266 (2008) 2801-2805.
[20]	J. Gan, M.K. Meyer, R.C. Birtcher, T.R. Allen, J. Astm Int. 3 (2006) 12376. DOI URL
[21]	C. Ulmer, Ph.D. Thesis, The Pennsylvania State University, 2014.
[22]	C.J. Ulmer, A.T. Motta, M.A. Kirk, J. Nucl. Mater. 466 (2015) 606-614. DOI URL
[23]	A. Motta, K. Sridharan, D. Morgan, I. Szlufarska, Understanding the Irradia- tion Behavior of Zirconium Carbide, Office of Scientific & Technical Information Technical Reports, No. 10-679, 2013.
[24]	J. Gan, Y. Yang, C. Dickson, T. Allen, J. Nucl. Mater. 389 (2009) 317-325. DOI URL
[25]	Y. Yang, Clayton A. Dickerson, H. Swoboda, B. Miller, Todd R. Allen, J. Nucl. Mater. 378 (2008) 341-348. DOI URL
[26]	S. Agarwal, A. Bhattacharya, P. Trocellier, S.J. Zinkle, Acta Mater 163 (2019) 14-27. DOI URL
[27]	Y. Huang, B.R. Maier, T.R. Allen, Nucl. Eng. Des. 277 (2014) 55-63. DOI URL
[28]	Y. Yang, W.Y. Lo, C. Dickerson, T.R. Allen, J. Nucl. Mater. 454 (2014) 130-135. DOI URL
[29]	B.X. Wei, Y.J. Wang, H.B. Zhang, D. Wang, S.M. Peng, Y. Zhou, Mater. Lett. 228 (2018) 254-257. DOI URL
[30]	B.X. Wei, D. Wang, Y.J. Wang, H.B. Zhang, Materials 12 (2019) 3768. DOI URL
[31]	X.G. Wang, G.J. Zhang, J.X. Xue, Y. Tang, X. Huang, C.M. Xu, P.L. Wang, J. Am. Ceram. Soc. 96 (2013) 32-36. DOI URL
[32]	X.G. Wang, J.X. Liu, Y.M. Kan, G.J. Zhang, J. Eur. Ceram. Soc. 32 (2012) 1795-1802. DOI URL
[33]	W. Bao, S. Robertson, J.X. Liu, G.J. Zhang, F.F. Xu, H.Z. Wu, J. Eur. Ceram. Soc. 38 (2018) 4373-4383. DOI URL
[34]	J. Ziegler, J.P. Biersack, M.D. Ziegler, The Stopping and Range of Ions in Matter, fifth ed., Springer, Berlin, 2008.
[35]	W. Bao, S. Robertson, J.W. Zhao, J.X. Liu, H. Wu, G.J. Zhang, F. Xu, J. Mater. Sci. Technol. 72 (2021) 223-230. DOI URL
[36]	V. Krsjak, J. Degmova, S. Sojak, V. Slugen, J. Nucl. Mater. 499 (2018) 38-46. DOI URL
[37]	S. Agarwal, P. Trocellier, Y. Serruys, S. Vaubaillon, S. Miro, Nucl. Instrum. Meth- ods Phys. Res. Sect. B-Beam Interact. Mater. Atoms 327 (2014) 117-120.
[38]	G. Busker, M.A. van Huis, R.W. Grimes, A. van Veen, Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms 171 (2000) 528-536. DOI URL
[39]	W. Beeré, G.L. Reynolds, Acta Metall 20 (1972) 845-848. DOI URL
[40]	H. Trinkaus, B.N. Singh, J. Nucl. Mater. 323 (2003) 229-242. DOI URL
[41]	R.D.S. Yadava, J. Nucl. Mater. 98 (1981) 47-62. DOI URL
[42]	Y. Zhang, B. Liu, J. Wang, J. Wang, Acta Mater 111 (2016) 232-241. DOI URL
[43]	S. Kim, I. Szlufarska, D. Morgan, J. Appl. Phys. 107 (2010) 053521. DOI URL
[44]	M.J. Zheng, I. Szlufarska, D. Morgan, J. Nucl. Mater. 457 (2015) 343-351. DOI URL
[45]	X. Yang, Y. Lu, P. Zhang, J. Nucl. Mater. 465 (2015) 161-166. DOI URL
[46]	Y. Zhang, B. Liu, J. Wang, Sci. Rep. 5 (2016) 18098. DOI URL
[47]	T. Yang, C.A. Taylor, S. Kong, C. Wang, Y. Zhang, X. Huang, J. Xue, S. Yan, Y. Wang, J. Nucl. Mater. 443 (2013) 40-48. DOI URL
[48]	J. Chen, P. Jung, H. Trinkaus, Phys. Rev. Lett. 82 (1999) 2709-2712. DOI URL
[49]	J. Chen, P. Jung, H. Trinkaus, Phys. Rev. B 61 (20 0 0) 12923-12932. DOI URL
[50]	N. Takada, M. Misawa, A. Tomiyama, S. Hosokawa, J. Nucl. Sci. Technol. 38 (2001) 330-341. DOI URL
[51]	X.Y. Yang, Y. Lu, P. Zhang, J. Appl. Phys. 117 (2015) 5.