1. Mixed-valence state in the dilute-impurity regime of La-substituted SmB6.
- Author
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Zonno, M., Michiardi, M., Boschini, F., Levy, G., Volckaert, K., Curcio, D., Bianchi, M., Rosa, P. F. S., Fisk, Z., Hofmann, Ph., Elfimov, I. S., Green, R. J., Sawatzky, G. A., and Damascelli, A.
- Subjects
VALENCE fluctuations ,PHOTOELECTRON spectroscopy ,X-ray absorption ,X-ray spectroscopy ,INTEGERS - Abstract
Homogeneous mixed-valence (MV) behaviour is one of the most intriguing phenomena of f-electron systems. Despite extensive efforts, a fundamental aspect which remains unsettled is the experimental determination of the limiting cases for which MV emerges. Here we address this question for SmB
6 , a prototypical MV system characterized by two nearly-degenerate Sm2+ and Sm3+ configurations. By combining angle-resolved photoemission spectroscopy (ARPES) and x-ray absorption spectroscopy (XAS), we track the evolution of the mean Sm valence, vSm , in the Smx La1−x B6 series. Upon substitution of Sm ions with trivalent La, we observe a linear decrease of valence fluctuations to an almost complete suppression at x = 0.2, with vSm ~ 2; surprisingly, by further reducing x, a re-entrant increase of vSm develops, approaching the value of vimp ~ 2.35 in the dilute-impurity limit. Such behaviour departs from a monotonic evolution of vSm across the whole series, as well as from the expectation of its convergence to an integer value for x → 0. Our ARPES and XAS results, complemented by a phenomenological model, demonstrate an unconventional evolution of the MV character in the Smx La1−x B6 series, paving the way to further theoretical and experimental considerations on the concept of MV itself, and its influence on the macroscopic properties of rare-earth compounds in the dilute-to-intermediate impurity regime. This study reveals a non-monotonic evolution of the mixed-valence character in the Smx La1−x B6 series, with near-complete suppression of valence fluctuations in the intermediate substitution regime, followed by a re-emergent mixed-valence behavior in the dilute-impurity limit. [ABSTRACT FROM AUTHOR]- Published
- 2024
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