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运用激光拉曼光谱研究了450—1050 ℃退火处理对氧化镍中二阶磁振子散射的增强效应, 同时分析了激光功率对氧化镍中二阶磁振子散射的影响. 研究发现, 退火处理可显著增强氧化镍中二阶磁振子散射, 在450—1050 ℃范围内, 退火温度越高, 增强效应越明显, 经过1050 ℃退火处理后二阶磁振子散射增强效应可达两个数量级以上. 该显著增强效应与高温退火处理后氧化镍样品中镍缺陷的显著减少紧密相关, 同时也与镍离子的晶格排列结构紧密相关. 而且高温退火处理还可显著降低激光功率对氧化镍中二阶磁振子散射的影响. 当退火温度较低时, 氧化镍中二阶磁振子散射随激光功率的增加快速减弱并消失, 而经过1050 ℃退火处理后, 氧化镍中二阶磁振子散射在较高激光功率下仍非常显著.Laser Raman spectroscopy is used to study the enhancement effect of two-magnon scattering in nickel oxide through annealing treatment in a temperature range from 450 ℃ to 1050 ℃, and investigate laser heating effect on two-magnon scattering. Our study shows that two-magnon scattering of nickel oxide can be tremendously enhanced with annealing temperature rising. In the temperature range from 450 ℃ to 1050 ℃, the enhancement increases with annealing temperature increasing, and with 1050 ℃ annealing the two-magnon scattering can be enhanced more than two orders of magnitude, also the enhancement of two-magnon scattering is much stronger than that of two-phonon scattering. This tremendous enhancement is correlated not only with the significant decrease of Ni-vacancy by high temperature annealing, but also with the magnetic spin ordering network of Ni ions. The variation of sensitive intensity of two-magnon scattering with the concentration of Ni-vacancy can be used to provide a simple Raman spectroscopy method of quantitatively measuring the Ni-vacancy in nickel oxide. In addition, the annealing treatment can significantly reduce the laser heating effect on two-magnon scatting in nickel oxide power samples. At low annealing temperature, the intensity of two-magnon scattering quickly quenches with increasing laser power. With 1050 ℃ annealing, the laser heating effect on two-magnon scattering is significantly reduced and two-magnon scattering can still have strong intensity at high laser power.
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Keywords:
- two-magnon /
- Raman spectroscopy /
- annealed /
- nickel oxide
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图 1 氧化镍原始样品及经过450, 550, 650, 750, 850, 950和1050 ℃等温度退火处理后的拉曼光谱
Fig. 1. Raman spectra of the original nickel oxide powder and annealed at temperatures of 450, 550, 650, 750, 850, 950, 1050 ℃.
图 2 (a) 归一化2M散射强度与退火温度的关系. 插图为六角锰氧化物中磁振子散射强度与非磁性离子浓度的关系[9]. (b) 2M与2LO散射强度比及归一化2M散射强度的对数与退火温度的关系
Fig. 2. (a) Normalized 2M intensity as a function of annealing temperature. Inset is the magnon scattering intensity as a function of non-magnetic doping concentration in hexagonal manganite[9]. (b) Logarithms of 2M to 2LO intensity ratio and normalized 2M intensity as a function of annealing temperature.
图 3 (a) 850 ℃, (b) 950 ℃, (c) 1050 ℃退火处理氧化镍在0.5, 1, 2, 3, 5, 7 mW等不同激光功率下的拉曼光谱
Fig. 3. Raman spectra of the nickel oxide annealed at (a) 850 ℃, (b) 950 ℃, (c) 1050 ℃ under different laser power of 0.5, 1, 2, 3, 5, 7 mW.
图 4 不同退火温度氧化镍拉曼光谱中(a) 2M和2LO拉曼峰强度对比, 及(b) 2M拉曼峰偏移随激光功率的变化
Fig. 4. Laser power dependence of (a) 2M to 2LO intensity ratio, and (b) 2M Raman shift at different annealing temperatures.
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[1] Dharmaraj N, Prabu P, Nagarajan S, Kim C H, Park J H, Kim H Y 2006 Mater. Sci. Eng. B 128 111
Google Scholar
[2] Chen Z Y, Chen Y Q, Zhang Q K, Tang X Q, Wang D D, Chen Z Q, Mascher P, Wang S J 2017 ECS J. Solid State Sci. Technol. 6 798
Google Scholar
[3] Mishra Sunil K, Subrahmanyam V 2011 Int. J. Mod. Phys. B 25 2507
Google Scholar
[4] Gandhi S, Nagalakshmi N, Baskaran I, Dhanalakshmi V, Gopinathan Nair M R, Anbarasan R 2010 J. Appl. Polym. Sci. 118 1666
Google Scholar
[5] Wang Y, Zhu J, Yang X, Lu L, Wang X 2005 Thermochim. Acta 437 106
Google Scholar
[6] Plashnitsa V V, Gupta V, Miura N 2010 Electrochim. Acta 55 6941
Google Scholar
[7] Chen X B, Kong M H, Choi J Y, Kim H T 2016 J. Phys. D: Appl. Phys. 49 465304
Google Scholar
[8] Chen X B, Guo P C, Huyen N T, Kim S, Yang I S, Wang X Y, Cheong S W 2017 Appl. Phys. Lett. 110 122405
Google Scholar
[9] Nam J Y, Kim S, Nguyen H T M, Chen X B, Choi M S, Lee D, Noh T W, Yang I S 2020 J. Raman Spectrosc. 51 2298
Google Scholar
[10] Gandhi A C, Huang C Y, Yang C C, Chan T S, Cheng C L, Ma Y R, Wu S Y 2011 Nanoscale Res. Lett. 6 485
Google Scholar
[11] Sunny A, Balasubramanian K 2020 J. Phys. Chem. C 124 12636
Google Scholar
[12] Mironova-Ulmane N, Kuzmin A, Sildos I, Puust L, Grabis J 2019 Latv. J. Phys. Tech. Sci. 56 61
Google Scholar
[13] Deshpande M P, Patel K N, Gujarati V P, Patel K, Chaki S H 2016 Adv. Mater. Res. 1141 65
Google Scholar
[14] Lockwood D J, Cottam M G, Baskey J H 1992 J. Magn. Magn. Mater. 104-107 1053
Google Scholar
[15] Duan W J, Lu S H, Wu Z L, Wang Y S 2012 J. Phys. Chem. C 116 26043
Google Scholar
[16] Gandhi A C, Pant J, Pandit S D, Dalimbkar S K, Chan T S, Cheng C L, Ma Y R, Sheng Y W 2013 J. Phys. Chem. C 117 18666
Google Scholar
[17] Lacerda M M, Kargar F, Aytan E, Samnakay R, Debnath B, Li J X, Khitun A, Lake R K, Shi J, Balandin A A 2017 Appl. Phys. Lett. 110 202406
Google Scholar
[18] Baran S, Hoser A, Penc B, Szytula A 2016 Acta Phys. Pol. A 129 35
Google Scholar
[19] Hou H Y, Yang M, Qiu J, Yang Y S, Chen X B 2019 Cryst. 9 357
Google Scholar
[20] Bala N, Singh H K, Verma S, Rath S 2020 Phys. Rev. B 102 024423
Google Scholar
[21] Dietz R E, Parisot G I, Meixner A E 1971 Phys. Rev. B 4 2302
Google Scholar
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