Klein Julian, Pingault Benjamin, Florian Matthias, Heißenbüttel Marie-Christin, Steinhoff Alexander, Song Zhigang, Torres Kierstin, Dirnberger Florian, Curtis Jonathan B, Weile Mads, Penn Aubrey, Deilmann Thorsten, Dana Rami, Bushati Rezlind, Quan Jiamin, Luxa Jan, Sofer Zdeněk, Alù Andrea, Menon Vinod M, Wurstbauer Ursula, Rohlfing Michael, Narang Prineha, Lončar Marko, Ross Frances M
Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States.
ACS Nano. 2023 Mar 28;17(6):5316-5328. doi: 10.1021/acsnano.2c07316. Epub 2023 Mar 16.
Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for the study of fundamental interactions and excitations, such as Tomonaga-Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly for magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D material embedded in a magnetically ordered environment. The strong 1D electronic character originates from the Cr-S chains and the combination of weak interlayer hybridization and anisotropy in effective mass and dielectric screening, with an effective electron mass ratio of / ∼ 50. This extreme anisotropy experimentally manifests in strong electron-phonon and exciton-phonon interactions, a Peierls-like structural instability, and a Fano resonance from a van Hove singularity of similar strength to that of metallic carbon nanotubes. Moreover, because of the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D-correlated many-body physics in the presence of magnetic order.
在展现出相互竞争的电子和磁序的一维(1D)系统中的关联量子现象,对于研究诸如汤川-卢廷格液体、拓扑序以及具有与它们高维对应物中预期的准粒子完全不同性质的缺陷等基本相互作用和激发而言,具有浓厚的研究兴趣。然而,纯净的一维电子系统在实验上很难实现,特别是对于磁有序系统。在此,我们表明范德华层状磁性半导体CrSBr的行为类似于嵌入磁有序环境中的准一维材料。其强烈的一维电子特性源于Cr-S链以及层间弱杂化与有效质量和介电屏蔽中的各向异性的结合,有效电子质量比约为50。这种极端各向异性在实验上表现为强电子-声子和激子-声子相互作用、类皮尔斯结构不稳定性以及来自与金属碳纳米管强度相似的范霍夫奇点的法诺共振。此外,由于维度降低和层间耦合,CrSBr拥有具有高结合能和振子强度的光谱窄(1 meV)激子,这些激子继承了一维特性。总体而言,CrSBr最好被理解为一堆弱杂化的单层,并且似乎是在磁有序存在的情况下研究奇异激子和一维关联多体物理的实验上有吸引力的候选材料。