Characterization and NV Color Center Adjustment of N-S Co-Doped Diamond Crystals in C3H6N6-NiS2 Additive System

doi:10.16553/j.cnki.issn1000-985x.2026.0050

Abstract

Abstract: Doping is an important means to control the NV color center of diamond. In this paper， NiS₂ （S source） and C₃H₆N₆ （N source） with different addition amounts were added to NiMnCo alloy catalyst by temperature gradient method under high temperature and high pressure （temperature 1 281 ℃， pressure 5.6 GPa） to synthesize N-S co-doped diamond single crystal. The optical microscopic analysis of the synthesized samples shows that when the addition amount of NiS₂ （S source） is constant， with the increase of C₃H₆N₆ addition， the color of diamond gradually changes from yellow to yellow-green， and the crystal defects become more. Infrared spectroscopy analysis shows that the increase of C₃H₆N₆ addition will lead to the increase of C-center nitrogen content in diamond samples， and the larger amount of sulfur will promote more nitrogen into diamond. X-ray photoelectron spectroscopy （XPS） shows that both nitrogen and sulfur atoms have successfully entered the diamond lattice. Nitrogen exists in the form of C—N， N＝O and N—N bonds， and sulfur exists in the form of C-S-O， C-SO₂-S-O and C-S sulfides. Raman spectroscopy shows that the increase of C₃H₆N₆ addition will lead to the increase of Raman peak shift of diamond crystal， the increase of internal distortion and the increase of internal stress. Photoluminescence （PL） spectra show that an appropriate amount of nitrogen and sulfur is beneficial for the C-center nitrogen in the diamond lattice to capture the moving holes to form negatively charged NV^-. This study provides a reference for the study of doping regulation of diamond NV color center.

Key words: diamond; NV color center; high temperature and high pressure; crystal defect; vacancy; N-S co-doping

CLC Number:

TQ163

HE Shasha, ZHANG Xiyun, LI Shangsheng, LI Xiaoxiao, HU Qiang, HU Meihua, CHEN Jingjing, GUO Zhenghao, LI Jianlin, LI Li, ZHAO Chunhong, XIAO Hongyu, LI Yong. Characterization and NV Color Center Adjustment of N-S Co-Doped Diamond Crystals in C₃H₆N₆-NiS₂ Additive System[J]. Journal of Synthetic Crystals, 2026, 55(8): 1274-1281.

Figures/Tables 9

Fig.1 Optical microscopic images of diamond synthesized by co-doping with C3H6N6-NiS2

Table 1 Experimental results of diamond synthesized by co-doping with C3H6N6-NiS2

Sample	NiS₂ content/%	C₃H₆N₆ content/%	Color	Inclusion
a	0	0	Yellow	No
b	12	0	Yellow	Little
c	12	0.03	Yellow	No
d	12	0.06	Dull yellow	Many
e	12	0.09	Dull yellow	Many
f	12	0.12	Olivine	Little
g	0	0.09	Green	Little
h	14	0.03	Olivine	Little
i	14	0.06	Olivine	Little
j	14	0.09	Green	Many
k	14	0.12	Black and green	Many

Fig.2 Infrared spectra of diamond synthesized by co-doping with C3H6N6-NiS2

Table 2 CN in diamond synthesized by co-doping with C3H6N6-NiS2

Sample	a	b	c	d	e	f	g	h	i	j
C₃H₆N₆ content/%	0	0	0.03	0.06	0.09	0.12	0.09	0.03	0.06	0.09
NiS₂ content/%	0	12	12	12	12	12	0	14	14	14
C_N/ppm	154	187	217	245	278	695	472	327	353	521

Fig.3 CN in two groups of diamond synthesized by co-doping with different C3H6N6 content

Fig.4 XPS of diamond by co-doping with NiS2（12%） and C3H6N6（0.06%）. （a） C 1s；（b） N 1s；（c） S 2p

Fig.5 Raman spectra of diamond synthesized by co-doping with C3H6N6-NiS2

Table 3 Raman peak positions， FWHM and internal stress of diamond synthesized by co-doping with C3H6N6-NiS2

Sample	Peak position/cm^-1	FWHM/cm^-1	Internal stress/GPa
a	1 332.31	6.20	0.107
b	1 331.80	6.51	0.069
c	1 331.75	5.98	0.086
d	1 331.62	6.34	0.132
e	1 331.47	6.84	0.184
f	1 331.31	6.51	0.239
g	1 331.52	7.08	0.166
h	1 331.56	6.86	0.152
i	1 331.42	6.94	0.201
j	1 331.16	7.35	0.291

Fig.6 PL spectra of diamond synthesized by co-doping with C3H6N6-NiS2

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Characterization and NV Color Center Adjustment of N-S Co-Doped Diamond Crystals in C₃H₆N₆-NiS₂ Additive System

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