Comparative Raman study of Ruddlesden-Popper nickelates and the monolayer-trilayer polymorph

Fuente: arXiv
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Autores principales: Sundaramurthy, Vignesh, Suthar, Abhi, Puphal, Pascal, Le, Congcong, Gu, Yuhao, Yilmaz, Hasan, Sosa-Lizama, Pablo, van Aken, Peter A., Suyolcu, Y. Eren, Isobe, Masahiko, Schnyder, Andreas P., Wu, Xianxin, Minola, Matteo, Keimer, Bernhard, Hepting, Matthias
Formato: Preprint
Publicado: 2025
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author Sundaramurthy, Vignesh
Suthar, Abhi
Puphal, Pascal
Le, Congcong
Gu, Yuhao
Yilmaz, Hasan
Sosa-Lizama, Pablo
van Aken, Peter A.
Suyolcu, Y. Eren
Isobe, Masahiko
Schnyder, Andreas P.
Wu, Xianxin
Minola, Matteo
Keimer, Bernhard
Hepting, Matthias
author_facet Sundaramurthy, Vignesh
Suthar, Abhi
Puphal, Pascal
Le, Congcong
Gu, Yuhao
Yilmaz, Hasan
Sosa-Lizama, Pablo
van Aken, Peter A.
Suyolcu, Y. Eren
Isobe, Masahiko
Schnyder, Andreas P.
Wu, Xianxin
Minola, Matteo
Keimer, Bernhard
Hepting, Matthias
contents Ruddlesden-Popper (RP) nickelates have attracted intense interest following the discovery of superconductivity in several members of the series, including bilayer (BL) La$_3$Ni$_2$O$_7$, trilayer (TL) La$_4$Ni$_3$O$_{10}$, and structural polymorphs composed of monolayer-bilayer or monolayer-trilayer (ML-TL) units. However, an inherent propensity of the RP series to form intergrown phases during single-crystal synthesis, together with spatial variations in oxygen stoichiometry, has complicated the determination of their intrinsic material properties. As a consequence, conflicting reports have emerged on both their electronic phase transitions and lattice dynamics. In this work, we perform a comparative study of the phononic and electronic Raman responses of high-quality ML-TL single crystals and contrast them with those of other RP nickelates, using samples with optimized oxygen content. We establish several Raman spectral features that enable unambiguous phase identification across the series. Moreover, we uncover characteristics in the phononic and electronic Raman response of ML-TL that are not reflected in the pure ML and TL compounds. We attribute these differences to a distinctive electronic structure arising from self-doping and confinement effects induced by the ML unit within the ML-TL lattice architecture.
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publishDate 2025
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spellingShingle Comparative Raman study of Ruddlesden-Popper nickelates and the monolayer-trilayer polymorph
Sundaramurthy, Vignesh
Suthar, Abhi
Puphal, Pascal
Le, Congcong
Gu, Yuhao
Yilmaz, Hasan
Sosa-Lizama, Pablo
van Aken, Peter A.
Suyolcu, Y. Eren
Isobe, Masahiko
Schnyder, Andreas P.
Wu, Xianxin
Minola, Matteo
Keimer, Bernhard
Hepting, Matthias
Strongly Correlated Electrons
Superconductivity
Ruddlesden-Popper (RP) nickelates have attracted intense interest following the discovery of superconductivity in several members of the series, including bilayer (BL) La$_3$Ni$_2$O$_7$, trilayer (TL) La$_4$Ni$_3$O$_{10}$, and structural polymorphs composed of monolayer-bilayer or monolayer-trilayer (ML-TL) units. However, an inherent propensity of the RP series to form intergrown phases during single-crystal synthesis, together with spatial variations in oxygen stoichiometry, has complicated the determination of their intrinsic material properties. As a consequence, conflicting reports have emerged on both their electronic phase transitions and lattice dynamics. In this work, we perform a comparative study of the phononic and electronic Raman responses of high-quality ML-TL single crystals and contrast them with those of other RP nickelates, using samples with optimized oxygen content. We establish several Raman spectral features that enable unambiguous phase identification across the series. Moreover, we uncover characteristics in the phononic and electronic Raman response of ML-TL that are not reflected in the pure ML and TL compounds. We attribute these differences to a distinctive electronic structure arising from self-doping and confinement effects induced by the ML unit within the ML-TL lattice architecture.
title Comparative Raman study of Ruddlesden-Popper nickelates and the monolayer-trilayer polymorph
topic Strongly Correlated Electrons
Superconductivity
url https://arxiv.org/abs/2512.17583