高压下层状钙钛矿Sr2Ta2O7陶瓷中晶格动力学与相变的拉曼散射研究

钱超; 亓文明; MATTURSUNAbliz; 胡清扬; 王元元; 董洪亮; 陈斌

doi:10.11858/gywlxb.20251269

高压下层状钙钛矿Sr₂Ta₂O₇陶瓷中晶格动力学与相变的拉曼散射研究

doi: 10.11858/gywlxb.20251269

钱超^{1, 2,},
亓文明^{2, 3,*, ,},
MATTURSUNAbliz⁴,
胡清扬²,
王元元^1,*, ,,
董洪亮^2,*, ,,
陈斌^2,*, ,

1.
上海第二工业大学能源与材料学院, 上海　201209
2.
北京高压科学研究中心, 上海　201203
3.
山东理工大学物理与光电工程学院, 山东淄博　255000
4.
华东师范大学极性材料与器件教育部重点实验室, 上海　200062

基金项目: 国家自然科学基金（42150101）；国家重点研发计划（2021YFA0718900）

详细信息

作者简介:
钱　超（1998－），男，硕士研究生，主要从事高压钙钛矿材料结构与性能研究. E-mail：chao.qian@hpstar.ac.cn

通讯作者:
亓文明（1993－），男，博士，主要从事高压下凝聚态物理、光学与地球物理研究.E-mail：wenming.hp@outlook.com

王元元（1983－），女，博士，教授，主要从事微纳尺度载流子输运性质研究.E-mail：wangyuanyuan@sspu.edu.cn

董洪亮（1983－），男，博士，副研究员，主要从事高压等极端条件下材料的合成、结构、物性以及服役行为研究. E-mail：hongliang.dong@hpstar.ac.cn

陈　斌（1968－），男，博士，研究员，主要从事高压物理研究. E-mail：chenbin@hpstar.ac.cn

中图分类号: O521.2
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出版历程
- 收稿日期: 2025-11-27
- 修回日期: 2025-12-25
- 网络出版日期: 2026-01-01
- 刊出日期: 2026-10-22

Raman Scattering Study of Lattice Dynamics and Phase Transitions in Layered Perovskite Sr₂Ta₂O₇ Ceramics under High Pressure

QIAN Chao^{1, 2
,},
QI Wenming^{2, 3,*
, ,},
MATTURSUN Abliz⁴,
HU Qingyang²,
WANG Yuanyuan^{1,*
, ,},
DONG Hongliang^{2,*
, ,},
CHEN Bin^{2,*
, ,}

1.
School of Energy and Materials, Shanghai Polytechnic University, Shanghai 201209, China
2.
Center for High Pressure Science and Technology Advanced Research, Shanghai 201203, China
3.
School of Physics and Optoelectronic Engineering, Shandong University of Technology, Zibo 255000, Shandong, China
4.
Key Laboratory of Polar Materials and Devices, Ministry of Education, East China Normal University, Shanghai 200062, China

摘要

摘要: 锶钽酸盐Sr₂Ta₂O₇是一种空间群为正交Cmcm相的陶瓷，凭借其在多铁性材料领域的潜在应用前景，已成为近年来的研究热点。然而，静水压力对其复杂晶格结构的调控机制及相变行为尚未明确，在一定程度上限制了对该材料“结构-性能”关系的深入理解。利用原位高压拉曼光谱技术，系统研究了高达30 GPa压力范围内正交Cmcm相Sr₂Ta₂O₇的晶格动力学响应特性，这是迄今报道的该材料体系的最高压力研究。结果表明：当压力达到5 GPa时，材料的拉曼振动模式出现显著变化，该现象源于对称性破缺引发的相变，对应从公度相到非公度相的转变；随着压力进一步升高至20 GPa，材料可能发生第2次相变，该相变过程为与晶格无序化密切相关的一级相变，但高压相的具体晶体结构仍有待进一步研究。拉曼光谱分析结果显示，该高压相的结构畸变可能遵循正交→单斜的转变路径。
- 高压 /
- 钙钛矿 /
- 相变 /
- 拉曼光谱
Abstract: The strontium tantalate Sr₂Ta₂O₇ is a ceramic with an orthogonal Cmcm space group. Due to its potential applications in the field of multiferroics, it has become a research hotspot in recent years. However, the regulatory mechanism and phase transition behavior of hydrostatic pressure on its complex lattice structure remain unclear, which, to some extent, limits the in-depth understanding of the “structure-property” relationship of this material. This study systematically investigates the lattice dynamic response characteristics of orthogonal Cmcm Sr₂Ta₂O₇ under high pressure up to 30 GPa by using in-situ high-pressure Raman spectroscopy, marking the highest pressure on this system to date. The results manifest that when the pressure reaches 5 GPa, significant changes occur in the Raman vibrational modes of the material. This phenomenon is attributed to a commensurate-to-incommensurate structural transition induced by symmetry breaking, consistent with previous research findings on Sr₂Ta₂O₇. As the pressure further increasing to 20 GPa, a second phase transition may occur, which is identified as a first-order phase transition closely related to lattice disordering. However, the specific crystal structure of this high-pressure phase remains to be further confirmed in future studies. The Raman spectroscopy analysis suggests that the structural distortion of this high-pressure phase may follow a transformation pathway from orthogonal to monoclinic.
- high-pressure /
- perovskite /
- phase transition /
- Raman spectroscopy

HTML全文

图 1 (a) 常压下正交相Sr₂Ta₂O₇陶瓷的拉曼光谱（黑色空心圆圈为观测数据，绿色实线为各分峰拟合结果，红色实线为拟合峰叠加之和），(b) 高压下 Sr₂Ta₂O₇样品的光学显微镜照片和(c) Sr₂Ta₂O₇的晶体结构

Figure 1. (a) Raman spectrum of orthorhombic Sr₂Ta₂O₇ ceramic under ambient conditions (The observed data is represented by black hollow circles. The green solid lines represent the individual fitting peaks. The red solid line represents the sum fitting peak.); (b) typical microscope image of Sr₂Ta₂O₇ under high pressure; (c) crystal structure of Sr₂Ta₂O₇

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图 2 高压下的晶格振动外模：(a) 0～8.4 GPa压力区间Sr₂Ta₂O₇在低频区（25～200 cm⁻¹）的拉曼光谱，(b) 9.8～30 GPa压力区间Sr₂Ta₂O₇在低频区（25～200 cm⁻¹）的拉曼光谱

Figure 2. Lattice vibrational external modes under high pressure: (a) Raman spectra of Sr₂Ta₂O₇ in low-frequency (25−200 cm⁻¹) region between 0 and 8.4 GPa; (b) Raman spectra of Sr₂Ta₂O₇ in low-frequency (25−200 cm⁻¹) region between 9.8 and 30 GPa

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图 3 高压下的TaO₆八面体内模：(a) 0～8.4 GPa压力区间Sr₂Ta₂O₇在中频区（200～400 cm⁻¹）的拉曼光谱，(b) 9.8～30 GPa压力区间Sr₂Ta₂O₇在中频区（200～400 cm⁻¹）的拉曼光谱，(c) 0～30 GPa压力区间Sr₂Ta₂O₇在高频区（550～1000 cm⁻¹）的拉曼光谱

Figure 3. TaO₆ octahedral internal modes under high pressure: (a) Raman spectra of Sr₂Ta₂O₇ in medium-frequency (200−400 cm⁻¹) region between 0 and 8.4 GPa; (b) Raman spectra of Sr₂Ta₂O₇ in medium-frequency (200−400 cm⁻¹) region between 9.8 and 30 GPa; (c) Raman spectra of Sr₂Ta₂O₇ in high-frequency (550−1000 cm⁻¹) region between 0 and 30 GPa

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图 4 Sr₂Ta₂O₇拉曼活性模频移在(a) 低频区和(b) 高频区随压力的变化关系，(c) Sr₂Ta₂O₇晶格外模与八面体内模的Grüneisen参数，(d) Sr₂Ta₂O₇特征峰拉曼位移与半高宽随压力的变化趋势

Figure 4. Pressure dependence of the shifts of Raman active modes for Sr₂Ta₂O₇ in (a) low frequency and (b) high frequency; (c) mode Grüneisen parameters of lattice external modes and octahedral modes in Sr₂Ta₂O₇; (d) pressure dependence of the Raman shift and the full width at half maximum in the symbolic peak of Sr₂Ta₂O₇

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表 1 Cmcm相中各拉曼模的零压频率、一阶压力导数及模式Grüneisen参数

Table 1. Raman frequencies at 0 GPa, first derivatives of pressure of each Raman modes and mode Grüneisen parameters in Cmcm phase

Lattice modes	ω₀/cm⁻¹	dω/dp	γ	Octahedral modes	ω₀/cm⁻¹	dω/dp	γ
$ {A}_{\text{g}} $	60.8	0.45	0.75	$ {B}_{\text{3g}} $	212.4	1.80	0.86
$ {B}_{\text{1g}} $	71.5	4.20	5.99	$ {B}_{\text{1g}} $	252.4	−0.40	−0.16
$ {A}_{\text{g}} $	88.4	3.39	3.91	$ {B}_{\text{2g}} $	280.3	3.34	1.21
$ {A}_{\text{g}} $	99.2	3.68	3.78	$ {B}_{\text{3g}} $	288.3	4.70	1.66
$ {A}_{\text{g}} $	122.1	2.53	2.11	$ {A}_{\text{g}} $	304.0	3.15	1.056
$ {B}_{\text{1g}} $	135.6	2.44	1.84	$ {A}_{\text{g}} $	326.0	5.22	1.63
$ {B}_{\text{1g}} $	141.3	2.98	2.15	$ {B}_{\text{2g}} $	355.5	3.54	1.015
				$ {B}_{\text{1g}} $	578.3	4.93	0.87
				$ {B}_{\text{3g}} $	630.0	9.54	1.54
				$ {A}_{\text{g}} $	838.9	4.53	0.55
				$ {A}_{\text{g}} $	880.1	0.42	0.0486

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