Maklar J, Windsor Y W, Nicholson C W, Puppin M, Walmsley P, Esposito V, Porer M, Rittmann J, Leuenberger D, Kubli M, Savoini M, Abreu E, Johnson S L, Beaud P, Ingold G, Staub U, Fisher I R, Ernstorfer R, Wolf M, Rettig L
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Berlin, Germany.
Department of Physics and Fribourg Center for Nanomaterials, University of Fribourg, Fribourg, Switzerland.
Nat Commun. 2021 May 3;12(1):2499. doi: 10.1038/s41467-021-22778-w.
The interaction of many-body systems with intense light pulses may lead to novel emergent phenomena far from equilibrium. Recent discoveries, such as the optical enhancement of the critical temperature in certain superconductors and the photo-stabilization of hidden phases, have turned this field into an important research frontier. Here, we demonstrate nonthermal charge-density-wave (CDW) order at electronic temperatures far greater than the thermodynamic transition temperature. Using time- and angle-resolved photoemission spectroscopy and time-resolved X-ray diffraction, we investigate the electronic and structural order parameters of an ultrafast photoinduced CDW-to-metal transition. Tracking the dynamical CDW recovery as a function of electronic temperature reveals a behaviour markedly different from equilibrium, which we attribute to the suppression of lattice fluctuations in the transient nonthermal phonon distribution. A complete description of the system's coherent and incoherent order-parameter dynamics is given by a time-dependent Ginzburg-Landau framework, providing access to the transient potential energy surfaces.
多体系统与强光脉冲的相互作用可能会导致远离平衡态的新型涌现现象。近期的一些发现,比如某些超导体中临界温度的光学增强以及隐藏相的光稳定化,已使该领域成为一个重要的研究前沿。在此,我们展示了在远高于热力学转变温度的电子温度下的非热电荷密度波(CDW)序。利用时间和角度分辨光电子能谱以及时间分辨X射线衍射,我们研究了超快光诱导的CDW到金属转变的电子和结构序参量。追踪作为电子温度函数的动态CDW恢复过程,揭示出一种与平衡态明显不同的行为,我们将其归因于瞬态非热声子分布中晶格涨落的抑制。通过一个含时金兹堡 - 朗道框架给出了系统相干和非相干序参量动力学的完整描述,从而能够获取瞬态势能面。