Čermák Petr, Schneidewind Astrid, Liu Benqiong, Koza Michael Marek, Franz Christian, Schönmann Rudolf, Sobolev Oleg, Pfleiderer Christian
Faculty of Mathematics and Physics, Department of Condensed Matter Physics, Charles University, 121 16 Praha, Czech Republic;
Forschungszentrum Jülich GmbH, Jülich Centre for Neutron Science at Heinz Maier-Leibnitz Zentrum, 85748 Garching, Germany.
Proc Natl Acad Sci U S A. 2019 Apr 2;116(14):6695-6700. doi: 10.1073/pnas.1819664116. Epub 2019 Mar 20.
Nearly a century of research has established the Born-Oppenheimer approximation as a cornerstone of condensed-matter systems, stating that the motion of the atomic nuclei and electrons may be treated separately. Interactions beyond the Born-Oppenheimer approximation are at the heart of magneto-elastic functionalities and instabilities. We report comprehensive neutron spectroscopy and ab initio phonon calculations of the coupling between phonons, CEF-split localized 4f electron states, and conduction electrons in the paramagnetic regime of [Formula: see text], an archetypal Kondo lattice compound. We identify two distinct magneto-elastic hybrid excitations that form even though all coupling constants are small. First, we find a CEF-phonon bound state reminiscent of the vibronic bound state (VBS) observed in other materials. However, in contrast to an abundance of optical phonons, so far believed to be essential for a VBS, the VBS in [Formula: see text] arises from a comparatively low density of states of acoustic phonons. Second, we find a pronounced anticrossing of the CEF excitations with acoustic phonons at zero magnetic field not observed before. Remarkably, both magneto-elastic excitations are well developed despite considerable damping of the CEFs that arises dominantly by the conduction electrons. Taking together the weak coupling with the simultaneous existence of a distinct VBS and anticrossing in the same material in the presence of damping suggests strongly that similarly well-developed magneto-elastic hybrid excitations must be abundant in a wide range of materials. In turn, our study of the excitation spectra of [Formula: see text] identifies a tractable point of reference in the search for magneto-elastic functionalities and instabilities.
近一个世纪的研究已将玻恩-奥本海默近似确立为凝聚态系统的基石,该近似表明原子核和电子的运动可以分开处理。超出玻恩-奥本海默近似的相互作用是磁弹性功能和不稳定性的核心。我们报告了对[化学式:见原文](一种典型的近藤晶格化合物)顺磁态下声子、晶体场效应(CEF)分裂的局域4f电子态和传导电子之间耦合的综合中子光谱学研究和从头算声子计算。我们识别出两种不同的磁弹性混合激发,尽管所有耦合常数都很小,但它们依然形成。首先,我们发现一种CEF-声子束缚态,类似于在其他材料中观察到的振动电子束缚态(VBS)。然而,与大量被认为对VBS至关重要的光学声子不同,[化学式:见原文]中的VBS源于声子态密度相对较低。其次,我们发现了在零磁场下CEF激发与声子之间明显的反交叉现象,这是之前未观察到的。值得注意的是,尽管CEF主要由于传导电子而受到相当大的阻尼,但这两种磁弹性激发都发展得很好。在存在阻尼的情况下,同一材料中弱耦合与独特VBS和反交叉现象的同时存在强烈表明,类似发展良好的磁弹性混合激发在广泛的材料中必定大量存在。反过来,我们对[化学式:见原文]激发光谱的研究确定了一个易于处理的参考点,用于寻找磁弹性功能和不稳定性。