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The Duel of Magnetic Interactions and Structural Instabilities: Itinerant Frustration in the Triangular Lattice Compound LiCrSe2
KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.ORCID iD: 0000-0003-4441-8882
KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.ORCID iD: 0000-0001-8879-7875
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

The recent synthesis of the chromium selenide compound LiCrSe2 constitutes a valuable addition to the ensemble of two-dimensional triangular lattice antiferromagnets (2D-TLA). In this work we present the very first comprehensive study of the combined low temperature nuclear and magnetic structure established in this material. Details on the connection between Li-ion dynamics and structural changes are also presented along with a direct link between atomic structure and spin order via a strong magnetoelastic coupling. LiCrSe2 was found to undergo a first order structural transition from a trigonal crystal system with space group P3¯m1 to a monoclinic one with space group C2/m at Ts=30~K. Such restructuring of the lattice is accompanied by a magnetic transition at TN=30~K, with the formation of a complex spin arrangement for the Cr3+ moments. Refinement of the magnetic structure with neutron diffraction data and complementary muon spin rotation analysis reveal the presence of two incommensurate magnetic domains with a up-up-down-down arrangement of the spins with ferromagnetic (FM) double chains coupled antiferromagnetically (AFM). In addition to this unusual arrangement, the spin axial vector is modulated both in direction and modulus, resulting in a spin density wave-like order with periodic suppression of the Cr moment along the chains. This behavior is believed to appear as a result of strong competition between direct exchange AFM and superexchange FM couplings established between both nearest neighbor and next nearest neighbor Cr3+ ions. We finally conjecture that the resulting magnetic order is stabilized via subtle vacancy/charge order within the Li layers, potentially causing a mix of two different magnetic phases within the sample.

National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:kth:diva-321697DOI: 10.48550/arXiv.2211.06864OAI: oai:DiVA.org:kth-321697DiVA, id: diva2:1712361
Note

Published in Communications Materials DOI: 10.1038/s43246-023-00407-x

QC 20221129

Available from: 2022-11-21 Created: 2022-11-21 Last updated: 2024-02-05Bibliographically approved
In thesis
1. A Comprehensive Experimental Approach to Multifunctional Quantum Materials and their Physical Properties: Geometry and Physics in Condensed Matter
Open this publication in new window or tab >>A Comprehensive Experimental Approach to Multifunctional Quantum Materials and their Physical Properties: Geometry and Physics in Condensed Matter
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis ranges within the vast framework of experimental condensed matter physics. Several different systems, and physical phenomena, are presented here from a structuralist standpoint. In fact, we show how, in solid condensed matter, the underlying arrangement of atoms, the symmetry of their structure, and their mutual interactions, underpin the form and the nature of their collective emergent properties. Our effort in this work was focused on unveiling complex magnetic ground states in newly synthesized materials, as well as in the clarification of unconventional symmetry breaking phenomena in highly debated systems. In all cases, we could understand the physics of such systems only when we elucidated the details, and temperature dependent evolution, of their structures.

About the choice of target materials for our investigations, our starting point has not only been fundamental condensed matter physics, but also forward looking towards a sustainable future. Here we considered both the development of energy efficient spintronics and quantum computing, as well as the need for efficient conversion and storage of clean energy. Therefore, this project is concerned with the advanced characterization of novel ”multifunctional” materials, that constitute a unique playground for fundamental scientific research, but also lend themselves to potential novel technical applications. Such materials might indeed display high temperature dynamical properties, which make them suitable for rechargeable batteries and heat conduction applications. At the same time, they are also strongly correlated electron systems at lower temperatures, and their fundamental magnetic and electronic properties are relevant for the development of quantum devices. To explore these properties, extensive experimental studies using large-scale research facilities were employed. In this project, several unique and powerful state-of-the-art high-resolution neutron scattering, X-ray scattering, and muon spin rotation techniques were used.

Place, publisher, year, edition, pages
Stockholm: Kungliga Tekniska högskolan, 2022. p. 137
Series
TRITA-SCI-FOU ; 2022:58
Keywords
quantum materials, neutron, muon, X-ray, symmetry, phase transitions
National Category
Condensed Matter Physics
Research subject
Physics, Material and Nano Physics
Identifiers
urn:nbn:se:kth:diva-321992 (URN)978-91-8040-420-4 (ISBN)
Public defence
2022-12-19, (Room 4204), Hannes Alfvéns väg 12, vån. 4, Alba Nova, KTH, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2022-11-28 Created: 2022-11-28 Last updated: 2023-12-07Bibliographically approved

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Nocerino, ElisabettaForslund, Ola KenjiMatsubara, NamiMånsson, Martin

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