高通量制备的SmxPr1–xFeO3晶体中反铁磁自旋模式和晶体场跃迁的太赫兹光谱

方雨青; 金钻明; 陈海洋; 阮舜逸; 李炬赓; 曹世勋; 彭滟; 马国宏; 朱亦鸣

doi:10.7498/aps.69.20200732

摘要

太赫兹辐射已经成为研究稀土铁氧化物(RFeO₃)的远红外响应和电子自旋特性的有效手段. 本文研究了高通量制备的稀土共掺杂Sm_xPr_1–xFeO₃单晶在零磁场下的反铁磁自旋模式(qAFM)和稀土离子的晶体场跃迁. 利用透射型太赫兹时域光谱, 实验测得Sm_0.2Pr_0.8FeO₃和Sm_0.4Pr_0.6FeO₃单晶的qAFM共振频率位于PrFeO₃单晶和SmFeO₃单晶的qAFM共振频率(分别为0.57和0.42 THz)的连线上. Sm_xPr_1–xFeO₃的qAFM模式频率随Sm³⁺离子掺杂浓度的增大而增大. 实验结果表明, Sm_0.4Pr_0.6FeO₃在160 K左右发生温度诱导的自旋重取向相变. 当晶体温度低于80 K, 晶体场效应导致Sm_0.2Pr_0.8FeO₃的吸收谱在0.5 THz附近出现宽带吸收峰. 目前的研究结果表明, 太赫兹光谱数据有助于检测高通量制备稀土铁氧体的晶体质量和稀土元素含量, 并将提高稀土掺杂对材料物性调控的分析能力.

关键词:

Abstract

Terahertz (THz) transient has become an effective method to study the optical and electronic spin characteristics of the rare earth orthoferrites RFeO₃. High-throughput grown crystal sample is sliced at different locations, then the continuously tunable rare earth elements co-doped single crystal Sm_xPr_1–xFeO₃ is studied with antiferromagnetic spin mode (qAFM) and crystal field transitions of rare earth ions under zero magnetic fields. Using THz time-domain spectroscopy, the qAFM resonance frequencies of Sm_0.2Pr_0.8FeO₃ and Sm_0.4Pr_0.6FeO₃ single crystals are located on the connection line of the qAFM frequencies of PrFeO₃ (0.57 THz) and SmFeO₃ (0.42 THz), therefore the frequency of qAFM increases linearly with doping concentration of Sm³⁺ ion increasing. The Sm_0.4Pr_0.6FeO₃ crystal undergoes a temperature-induced spin reorientation phase transition at about 160 K. When the crystal temperature is lower than 80 K, a wide band absorption peak of about 0.5 THz appears in the absorption spectrum of Sm_0.2Pr_0.8FeO₃ due to the crystal field effect. Our results show that THz spectral data not only allow us to monitor the quality of rare earth orthoferrite crystals prepared by high throughput and analyze the rare earth elements of the sample, but also improve the ability to analyze the physical properties of the co-doped RFeO₃.

Keywords:

作者及机构信息

1.
上海理工大学, 太赫兹技术创新研究院, 上海市现代光学系统重点实验室, 光学仪器与系统教育部工程中心,太赫兹光谱与影像技术协同创新中心, 上海　200093

2.
上海大学理学院, 上海　200444

3.
上海科技大学-上海光机所超强超快联合实验室, 上海　201210

4.
同济大学上海智能科学与技术研究院, 上海　200092

通信作者: 金钻明, physics_jzm@usst.edu.cn ; 马国宏, ghma@staff.shu.edu.cn ; 朱亦鸣, ymzhu@usst.edu.cn

基金项目: 国家自然科学基金(批准号: 61975110, 11674213, 61735010, 11604202)、111项目(批准号: D18014)、上海市科委国际联合实验室项目(批准号: 17590750300)、上海市科委重点项目(批准号: YDZX20193100004960)、上海市青年科技启明星计划(批准号: 18QA1401700)、上海市教育委员会和上海市教育发展基金会“晨光计划”(批准号: 16CG45)和上海高校青年东方学者计划(批准号: QD2015020)资助的课题

Authors and contacts

1.
Terahertz Technology Innovation Research Institute, Shanghai Key Lab of Modern Optical System, and Engineering Research Center of Optical Instrument and System (Ministry of Education), Terahertz Spectrum and Imaging Cooperative Innovation Center, University of Shanghai for Science and Technology, Shanghai 200093, China

2.
Department of Physics, Shanghai University, Shanghai 200444, China

3.
STU & SIOM Joint Laboratory for Superintense Lasers and the Applications, Shanghai 201210, China

4.
Shanghai Institute of Intelligent Science and Technology, Tongji University, Shanghai 200092, China

Corresponding author: Jin Zuan-Ming, physics_jzm@usst.edu.cn ; Ma Guo-Hong, ghma@staff.shu.edu.cn ; Zhu Yi-Ming, ymzhu@usst.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 61975110, 11674213, 61735010, 11604202), the 111 Project (Grant No. D18014), the International Joint Lab Program of the Science and Technology Commission Shanghai Municipality, China (Grant No. 17590750300), the Key Project of the Science and Technology Commission Shanghai Municipality, China (Grant No. YDZX20193100004960), the Shanghai Rising-Star Program of the Science and Technology Commission of Shanghai Municipality, China (Grant No. 18QA1401700), the Chenguang Project of Shanghai Educational Development Foundation, China (Grant No. 16CG45), and the Young Eastern Scholar Project of Shanghai Municipal Education Commission, China (Grant No. QD2015020)

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参考文献

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施引文献

图 1 (a)高通量制备准连续成分单晶Sm_xPr_1–xFeO₃示意图; (b) SmFeO₃, PrFeO₃ 和Sm_0.2Pr_0.8FeO₃单晶的晶体结构图

Fig. 1. (a) Experimental schematic of quasi-continuous phase formation in the high-throughput grown Sm_xPr_1–xFeO₃ (x = 0, 0.4, 0.7, 0.9, 1.0); (b) the crystallography structure of the single crystal SmFeO₃, PrFeO₃, and Sm_0.2Pr_0.8FeO₃.

下载: 全尺寸图片幻灯片

图 2 (a) THz-TDS实验装置示意图; (b) b切Sm_0.2Pr_0.8FeO₃单晶(红色); (c) Sm_0.4Pr_0.6FeO₃单晶(蓝色) 300 K时的太赫兹时域透射谱, 此时H_THz//c; 插图分别表示振荡部分(40—60 ps)的傅里叶变换光谱及其洛伦兹拟合(虚线)

Fig. 2. (a) Experimental setup diagram of THz-TDS. The THz time-domain waveforms transmitted through the b-cut (b) Sm_0.2Pr_0.8FeO₃ and (c) Sm_0.4Pr_0.6FeO₃ crystal at 300 K and the insets indicate the spectrum of oscillating parts obtained by Fourier transform of the waveform, which is fitted with a Lorentzian contour (dotted line).

下载: 全尺寸图片幻灯片

图 3 室温下Sm_xPr_1–xFeO₃单晶的qAFM自旋共振频率与Sm³⁺离子含量的关系, 其中插图表示qAFM模式的振动

Fig. 3. Summarized frequencies of the qAFM resonances at several Sm³⁺ ion contents at room temperature and the insets indicate the vibration of the qAFM.

下载: 全尺寸图片幻灯片

图 4 b切Sm_0.4Pr_0.6FeO₃单晶qAFM模式的共振频率和振幅随温度的关系; 插图表示Fe³⁺离子亚晶格的磁结构: 低温相(Г₂)、中间相(Г₄)、高温相(Г₂₄)

Fig. 4. The frequencies and amplitudes of the qAFM resonances of b-cut Sm_0.4 Pr_0.6FeO₃ crystal. Inset shows the magnetic structure of RFeO₃ in the low-temperature(Г₂), intermediate(Г₄), and high temperature(Г₂₄)phases.

下载: 全尺寸图片幻灯片

图 5 (a) Sm_0.2Pr_0.8FeO₃单晶温度依赖的太赫兹时域谱, 为了表达更为清楚, 不同温度的时域光谱在纵轴方向做了等间距的平移; 40, 80和300 K时Sm_0.2Pr_0.8FeO₃单晶的(b)折射率和(c)吸收系数, 插图为Pr³⁺离子基态在晶体场中能级劈裂示意图

Fig. 5. (a) The temperature dependent THz waveforms transmitted through the Sm_0.2Pr_0.8FeO₃ single crystal; (b) refractive indices and (c) absorption spectra of Sm_0.2Pr_0.8FeO₃ at 40, 80, and 300 K. The inset in (c) shows the energy level splitting of Pr³⁺ ion in the ground state crystal field.

下载: 全尺寸图片幻灯片

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[2]	Jungwirth T, Marti X, Wadley P, Wunderlich J 2016 Nat. Nanotech. 11 231 Google Scholar
[3]	Mikhaylovskiy R V, Hendry E, Secchi A, et al. 2015 Nat. Commun. 6 8190 Google Scholar
[4]	Kurihara T, Watanabe H, Nakajima M, Karube S, Oto K, Otani Y, Suemoto T 2018 Phys. Rev. Lett. 120 107202 Google Scholar
[5]	Baierl S, Hohenleutner M, Kampfrath T, Zvezdin A K, Kimel A V, Huber R, Mikhaylovskiy R V 2016 Nat. Photon. 10 715 Google Scholar
[6]	Nova T F, Cartella A, Cantaluppi A, et al. 2017 Nat. Phys. 13 132 Google Scholar
[7]	Pierce R D, Wolfe R, Van Uitert L G 1969 J. Appl. Phys. 40 1241 Google Scholar
[8]	Jiang J, Song G, Wang D, Jin Z, Tian Z, Lin X, Han J, Ma G, Cao S, Cheng Z 2016 J. Phys.: Condens. Matter 28 116002 Google Scholar
[9]	Yamaguchi K, Kurihara T, Minami Y, Nakajima M, Suemoto T 2013 Phys. Rev. Lett. 110 137204 Google Scholar
[10]	Liu X, Jin Z, Zhang S, et al. 2018 J. Phys. D: Appl. Phys. 51 024001 Google Scholar
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高通量制备的Sm_xPr_1–xFeO₃晶体中反铁磁自旋模式和晶体场跃迁的太赫兹光谱