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arXiv 2102.07912cond-mat.str-elcond-mat.mtrl-sci
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激子绝缘体Ta $_2$ Ni(Se $_{1-x}$ S $_x$)$_5$的晶格动力学

Lattice dynamics of the excitonic insulator Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$

Mai Ye, Pavel A. Volkov, Himanshu Lohani, Irena Feldman, Minsung Kim, Amit Kanigel, Girsh Blumberg

摘要:

最近,我们采用电子偏振分辨拉曼光谱来揭示Ta 2NiSe 5的强相关激子绝缘体(EI)性质,Volkov等人[arXiv:2007.07344],并且还表明对于Ta $_2$ Ni(Se $_{1-x}$ S $_x$)$_5$合金,临界激子波动随着硫浓度x而减小,从而暴露出协作晶格不稳定性,该不稳定性在大x时接管,Volkov等人[arXiv:2104.07032]。在这里,我们专注于这个EI家庭的晶格动力学。我们确定了所有的拉曼活性光学声子的完全对称和交流四极对称,并研究它们随温度和硫浓度的演变。我们证明了选择规则的变化,在温度低于正交单斜相转变在Tc(x),这是相关的EI相。我们发现,Tc(x)单调下降,从328 K的Ta 2NiSe 5到120 K的Ta 2NiS 5和晶格畸变的幅度也随着硫浓度x减小。当x < 0.7时,两个最低频率的B2 g声子模在高温下表现出强烈的非对称线型,这是由于Fano干涉与半金属态中存在的宽激子连续谱的缘故。在扩展的Fano模型的框架内,我们发展了激子-声子相互作用激发线型的定量描述,使我们能够导出内禀声子参数,并确定激子-声子相互作用强度,它影响转变温度Tc(x)。我们还观察到签名的声学模式散射的结构域壁低于Tc形成的协助。基于我们的研究结果,我们还提出了一个一致的解释,在时间分辨泵浦探测实验中观察到的振荡的起源。

英文摘要:

Recently, we employed electronic polarization-resolved Raman spectroscopy to reveal the strongly correlated excitonic insulator (EI) nature of Ta2NiSe5, Volkov et al. [arXiv:2007.07344], and also showed that for Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$ alloys the critical excitonic fluctuations diminish with sulfur concentration x exposing a cooperating lattice instability that takes over for large x, Volkov et al. [arXiv:2104.07032]. Here we focus on the lattice dynamics of this EI family. We identify all Raman-active optical phonons of fully symmetric and ac-quadrupole-like symmetries and study their evolution with temperature and sulfur concentration. We demonstrate the change of selection rules at temperatures below the orthorhombic-to-monoclinic transition at Tc(x) that is related to the EI phase. We find that Tc(x) decrease monotonically from 328 K for Ta2NiSe5 to 120 K for Ta2NiS5 and that the magnitude of lattice distortion also decreases with the sulfur concentration x. For x < 0.7, the two lowest-frequency B2g phonon modes show strongly asymmetric lineshapes at high temperatures due to Fano interference with the broad excitonic continuum present in a semimetallic state. Within the framework of extended Fano model, we develop a quantitative description of the interacting exciton-phonon excitation lineshape, enabling us to derive the intrinsic phonon parameters and determine the exciton-phonon interaction strength, that affects the transition temperature Tc(x). We also observe signatures of the acoustic mode scattered assisted by the structural domain walls formed below Tc. Based on our results, we additionally present a consistent interpretation of the origin of oscillations observed in time-resolved pump-probe experiments.

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