Laboratory for Ultrafast Microscopy and Electron Scattering, Institute of Condensed-Matter Physics, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland.
Proc Natl Acad Sci U S A. 2012 Apr 10;109(15):5603-8. doi: 10.1073/pnas.1117028109. Epub 2012 Mar 26.
The effect of dimensionality on materials properties has become strikingly evident with the recent discovery of graphene. Charge ordering phenomena can be induced in one dimension by periodic distortions of a material's crystal structure, termed Peierls ordering transition. Charge-density waves can also be induced in solids by strong coulomb repulsion between carriers, and at the extreme limit, Wigner predicted that crystallization itself can be induced in an electrons gas in free space close to the absolute zero of temperature. Similar phenomena are observed also in higher dimensions, but the microscopic description of the corresponding phase transition is often controversial, and remains an open field of research for fundamental physics. Here, we photoinduce the melting of the charge ordering in a complex three-dimensional solid and monitor the consequent charge redistribution by probing the optical response over a broad spectral range with ultrashort laser pulses. Although the photoinduced electronic temperature far exceeds the critical value, the charge-density wave is preserved until the lattice is sufficiently distorted to induce the phase transition. Combining this result with ab initio electronic structure calculations, we identified the Peierls origin of multiple charge-density waves in a three-dimensional system for the first time.
随着最近对石墨烯的发现,维度对材料性能的影响变得非常明显。通过周期性地扭曲材料的晶体结构,可以在一维中诱导电荷有序现象,这被称为 Peierls 有序转变。通过载流子之间的强烈库仑斥力,也可以在固体中诱导电荷密度波,并且在极限情况下,Wigner 预测在接近温度绝对零度的自由空间中的电子气中可以诱导出结晶本身。类似的现象也在更高维度中观察到,但对应相转变的微观描述通常存在争议,并且仍然是基础物理研究的一个开放领域。在这里,我们用光诱导复杂三维固体中的电荷有序熔融,并通过用超短激光脉冲在宽光谱范围内探测光学响应来监测随后的电荷重新分布。尽管光诱导的电子温度远远超过了临界值,但电荷密度波一直保持到晶格被充分扭曲以诱导相变。将这一结果与从头算电子结构计算相结合,我们首次在三维系统中确定了多个电荷密度波的 Peierls 起源。