论文标题
Kramer Doublets,Phonons,Crystal Field激发及其在ND2ZNIRO中的耦合
Kramer doublets, phonons, crystal-field excitations and their coupling in Nd2ZnIrO6
论文作者
论文摘要
我们报告了在温度范围为4-330 K的单晶石ND2ZNIRO6的单个晶体上的全面拉曼碎片测量值,并且跨越20 cm-1至5500 cm-1的宽光谱范围。该论文着重于涉及稀有地球ND3+离子的KRAMERS双线的晶格振动和电子过渡,并具有局部C1位点对称性。这些准粒子激发的温度演变使我们能够确定ND2ZNIRO6晶格和电子自由度之间的复杂耦合。通过重新规范化声子的自能参数,即峰频率和线宽度,可以观察到声子和晶体场激发之间的强耦合。对于大多数观察到的一阶声子,声子频率显示出突然的硬化和线宽度的狭窄。我们观察到了基态最低的KRAMERS双线(4I9/2)的多数,即在低温下(低于〜100 K)的Kramers脱落性提升,归因于ND-ND/IR交换相互作用,以及与自由度的杂物耦合。观察到的分裂为〜2-3 MEV,与估计值一致。我们还观察到大量的高能量模式,总计46,归因于4f3水平的ND3+耦合到反射在其异常温度演化中的声子之间的相结构过渡。
We report comprehensive Raman-scattering measurements on a single crystal of double-perovskite Nd2ZnIrO6 in temperature range of 4-330 K, and spanning a broad spectral range from 20 cm-1 to 5500 cm-1. The paper focuses on lattice vibrations and electronic transitions involving Kramers doublets of the rare-earth Nd3+ ion with local C1 site symmetry. Temperature evolution of these quasi-particle excitations have allowed us to ascertain the intricate coupling between lattice and electronic degrees of freedom in Nd2ZnIrO6. Strong coupling between phonons and crystal-field excitation is observed via renormalization of the self-energy parameter of the phonons i.e. peak frequency and line-width. The phonon frequency shows abrupt hardening and line-width narrowing below ~ 100 K for the majority of the observed first-order phonons. We observed splitting of the lowest Kramers doublets of ground state (4I9/2) multiplets i.e. lifting of the Kramers degeneracy, prominently at low-temperature (below ~ 100 K), attributed to the Nd-Nd/Ir exchange interactions and the intricate coupling with the lattice degrees of freedom. The observed splitting is of the order of ~ 2-3 meV and is consistent with the estimated value. We also observed a large number of high-energy modes, 46 in total, attributed to the intra-configurational transitions between 4f3 levels of Nd3+ coupled to the phonons reflected in their anomalous temperature evolution.