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arXiv 2202.03315cond-mat.mtrl-sci
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(TaSe $_4$)$_2$ I的价态和芯能级激发超快动力学

Ultrafast dynamics in (TaSe$_4$)$_2$I triggered by valence and core-level excitation

Wibke Bronsch, Manuel Tuniz, Giuseppe Crupi, Michela De Col, Denny Puntel, Davide Soranzio, Alessandro Giammarino, Michele Perlangeli, Helmuth Berger, Dario De … 展开作者

Wibke Bronsch, Manuel Tuniz, Giuseppe Crupi, Michela De Col, Denny Puntel, Davide Soranzio, Alessandro Giammarino, Michele Perlangeli, Helmuth Berger, Dario De Angelis, Danny Fainozzi, Ettore Paltanin, Stefano Pelli Cresi, Gabor Kurdi, Laura Foglia, Riccardo Mincigrucci, Fulvio Parmigiani, Filippo Bencivenga, Federico Cilento

摘要:

在这项工作中,我们研究了范式准一维材料(TaSe $_4$)$_2$ I的平衡动力学,当冷却到室温以下时,即在T $_{\rm{CDW}} $ = 263 K时,该材料表现出向无公度CDW相的转变。我们利用光学激光和自由电子激光(FEL)为基础的时间分辨光谱,以研究的正常状态和CDW阶段的选择性激发的效果,通过探测的近红外/可见光的光学性质沿和垂直于CDW的方向,其中系统是金属和绝缘,分别。在绝缘子系统的情况下,由47 eV和119 eV的超短X射线自由电子激光脉冲激发芯能级引起的反射率瞬变类似于仅激发化合物的价带时记录的反射率瞬变-由1.55 eV的近红外脉冲。相反,金属子系统显示依赖于光激发能量的弛豫动力学。此外,CDW振幅模式的激发仅针对低光子能量的激发而被记录。这一事实表明,光与有序态物质的耦合主要是在价带中直接注入离域载流子时实现的,而不是在芯能级中注入局域激发。在补充方面,桌面实验使我们能够证明准单向性质的CDW阶段(TaSe $_4$)$_2$ I,其指纹沿其$c$轴检测。我们的研究结果提供了新的见解的对称性的有序相的(TaSe $_4$)$_2$ I扰动的选择性激发,并提出了一种新的方法的基础上互补的桌面和自由电子激光光谱的复杂材料的研究。

英文摘要:

In this work, we study the out-of-equilibrium dynamics of the paradigmatic quasi-one-dimensional material (TaSe$_4$)$_2$I, that exhibits a transition into an incommensurate CDW phase when cooled just below room temperature, namely at T$_{\rm{CDW}} $= 263 K. We make use of both optical laser and free-electron laser (FEL) based time-resolved spectroscopies in order to study the effect of a selective excitation on the normal-state and on the CDW phases, by probing the near-infrared/visible optical properties both along and perpendicularly to the direction of the CDW, where the system is metallic and insulating, respectively. Excitation of the core-levels by ultrashort X-ray FEL pulses at 47 eV and 119 eV induces reflectivity transients resembling those recorded when only exciting the valence band of the compound - by near-infrared pulses at 1.55 eV - in the case of the insulating sub-system. Conversely, the metallic sub-system displays a relaxation dynamics which depends on the energy of photo-excitation. Moreover, excitation of the CDW amplitude mode is recorded only for excitation at low-photon-energy. This fact suggests that the coupling of light to ordered states of matter can predominantly be achieved when directly injecting delocalized carriers in the valence band, rather than localized excitations in the core levels. On a complementary side, table-top experiments allow us to prove the quasi-unidirectional nature of the CDW phase in (TaSe$_4$)$_2$I, whose fingerprints are detected along its $c$-axis only. Our results provide new insights on the symmetry of the ordered phase of (TaSe$_4$)$_2$I perturbed by a selective excitation, and suggest a novel approach based on complementary table-top and FEL spectroscopies for the study of complex materials.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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