Magnetic excitations in Nd𝑛+1⁢ Ni𝑛⁢ O3⁢𝑛+1 Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering

TenHuisen, Sophia F. R.; Pan, Grace A.; Song, Qi; Baykusheva, Denitsa R.; Segedin, Dan Ferenc; Goodge, Berit H.; Paik, Hanjong; Pelliciari, Jonathan; Bisogni, Valentina; Gu, Yanhong; Agrestini, Stefano; Nag, Abhishek; García-Fernández, Mirian; Zhou, Ke-Jin; Kourkoutis, Lena F.; Brooks, Charles M.; Mundy, Julia A.; Dean, Mark P. M.; Mitrano, Matteo

doi:10.1103/physrevb.111.165145

Magnetic excitations in Nd_𝑛+1⁢ Ni_𝑛⁢ O_3⁢𝑛+1 Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering

Journal Article · Tue Apr 22 00:00:00 EDT 2025 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.111.165145· OSTI ID:2568104

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Harvard Univ., Cambridge, MA (United States)
Harvard Univ., Cambridge, MA (United States); Institute of Science and Technology Austria (ISTA), Klosterneuburg (Austria)
Cornell Univ., Ithaca, NY (United States)
Cornell University
National Synchrotron Light Source II; Brookhaven National Laboratory
Harwell Science and Innovation Campus, Didcot (United Kingdom). Diamond Light Source, Ltd.
Brookhaven National Laboratory (BNL), Upton, NY (United States)

Magnetic interactions are thought to play a key role in the properties of many unconventional superconductors, including cuprates, iron pnictides, and square-planar nickelates. Superconductivity was also recently observed in the bilayer and trilayer Ruddlesden-Popper nickelates, the electronic structure of which is expected to differ from that of cuprates and square-planar nickelates. Here we study how electronic structure and magnetic interactions evolve with the number of layers, 𝑛, in thin film Ruddlesden-Popper nickelates Nd_𝑛+1⁢Ni_𝑛⁢O_3⁢𝑛+1 with 𝑛 = 1,3, and 5 using resonant inelastic x-ray scattering (RIXS). The RIXS spectra are consistent with a high-spin |3⁢𝑑⁸⁢ $$\underline{𝐿}$$⟩ electronic configuration, resembling that of La_2−𝑥⁢Sr_𝑥⁢NiO₄ and the parent perovskite, NdNiO₃. The magnetic excitations soften to lower energy in the structurally self-doped, higher-𝑛 films. In conclusion, our observations confirm that structural tuning is an effective route for altering electronic properties, such as magnetic superexchange, in this prominent family of materials.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS)

Grant/Contract Number:: SC0012704; SC0014664; SC0021925

OSTI ID:: 2568104

Alternate ID(s):: OSTI ID: 2561500

Report Number(s):: BNL--228205-2025-JAAM

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 16 Vol. 111; ISSN 2469-9950; ISSN 2469-9969

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Magnetic excitations in Nd𝑛+1⁢ Ni𝑛⁢ O3⁢𝑛+1 Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering

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Magnetic excitations in Nd_𝑛+1⁢ Ni_𝑛⁢ O_3⁢𝑛+1 Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering