Comparative Raman study of Ruddlesden-Popper nickelates and the monolayer-trilayer polymorph
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| Autores principales: | , , , , , , , , , , , , , , |
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| Formato: | Preprint |
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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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2512_17583 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| 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 |