论文标题

超快动力学(tase $ _4 $)$ _ 2 $ i由Valence触发和核心级别的激发

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

论文作者

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

论文摘要

在这项工作中,我们研究了范式的Quasi One维材料(tase $ _4 $)$ _ 2 $ i的平衡外动力学,该材料在冷却低于室温的情况下会过渡到不兑现的CDW相位,即在T $ _ {\ rmm {cdw} $ {cdw} $ = 263; las = 263 K.我们均可使用基于激光(FEL)的时间分辨光谱镜,以研究选择性激发对正常状态和CDW阶段的影响,通过探测近红外/可见光的光学特性,并沿着CDW的方向沿CDW的方向持续,并在系统中分别是金属和绝缘的。在47 eV处的超舒放X射线脉冲对核心水平的激发,而119 eV引起了反射率瞬变,类似于记录的脉冲,而仅激发了该化合物的价带(在1.55 eV时)的近红外脉冲,而在绝缘子系统的情况下。相反,金属子系统显示出一个取决于光启动能量的松弛动力学。此外,仅记录CDW振幅模式的激发仅用于低光能的激发。这一事实表明,当直接在价带中直接注入离域载体时,可以主要实现光与物质有序状态的耦合,而不是核心水平的局部激发。在互补的一面,桌面实验使我们能够证明CDW阶段(tase $ _4 $)$ _ 2 $ i的准单向性质,其指纹仅沿其$ c $轴(仅检测到)。我们的结果为(Tase $ _4 $)$ _ 2 $ i受到选择性激发的扰动的(Tase $ _4 $)$ _ 2 $ i的对称性提供了新的见解,并提出了一种基于互补的桌面和FEL光谱的新方法,以研究复杂材料。

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.

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