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  • Letter

Quantum paramagnetism in the decorated square-kagome antiferromagnet Na6Cu7BiO4(PO4)4Cl3

Nils Niggemann1,2,3,*, Nikita Astrakhantsev4,*, Arnaud Ralko5,3,*, Francesco Ferrari6,3,*, Atanu Maity3, Tobias Müller7, Johannes Richter8,9, Ronny Thomale7,3, Titus Neupert4 et al.

Johannes Reuther1,2,3, Yasir Iqbal3, and Harald O. Jeschke10,3

  • 1Dahlem Center for Complex Quantum Systems and Fachbereich Physik, Freie Universität Berlin, 14195 Berlin, Germany
  • 2Helmholtz-Zentrum Berlin für Materialien und Energie, Hahn-Meitner-Platz 1, 14109 Berlin, Germany
  • 3Department of Physics and Quantum Centre of Excellence for Diamond and Emergent Materials (QuCenDiEM), Indian Institute of Technology Madras, Chennai 600036, India
  • 4Department of Physics, University of Zürich, Winterthurerstrasse 190, CH-8057 Zürich, Switzerland
  • 5Institut Néel, UPR2940, Université Grenoble Alpes, CNRS, Grenoble FR-38042, France
  • 6Institut für Theoretische Physik, Goethe Universität Frankfurt, Max-von-Laue-Straße 1, 60438 Frankfurt am Main, Germany
  • 7Institut für Theoretische Physik und Astrophysik, Julius-Maximilians-Universität Würzburg, Am Hubland, D-97074 Würzburg, Germany
  • 8Institut für Physik, Otto-von-Guericke-Universität Magdeburg, P.O. Box 4120, 39016 Magdeburg, Germany
  • 9Max-Planck-Institut für Physik Komplexer Systeme, Nöthnitzer Straße 38, D-01187 Dresden, Germany
  • 10Research Institute for Interdisciplinary Science, Okayama University, Okayama 700-8530, Japan

  • *These authors contributed equally to this work.

Phys. Rev. B 108, L241117 – Published 19 December, 2023

DOI: https://doi.org/10.1103/PhysRevB.108.L241117

Abstract

The square-kagome lattice Heisenberg antiferromagnet is a highly frustrated Hamiltonian whose material realizations have been scarce. We theoretically investigate the recently synthesized Na6Cu7BiO4(PO)4)4Cl3 where a Cu2+ spin-1/2 square-kagome lattice (with a six site unit cell) is decorated by a seventh magnetic site alternatingly above and below the layers. The material does not show any sign of long-range magnetic order down to 50 mK despite a Curie-Weiss temperature of −212K indicating a quantum paramagnetic phase. Our DFT energy mapping elicits a purely antiferromagnetic Hamiltonian that features longer range exchange interactions beyond the pure square-kagome model and, importantly, we find the seventh site to be strongly coupled to the plane. We combine two variational Monte Carlo approaches, pseudofermion/Majorana functional renormalization group and Schwinger-Boson mean field calculations to show that the complex Hamiltonian of Na6Cu7BiO4(PO)4)4Cl3 still features a nonmagnetic ground state. We explain how the seventh Cu2+ site actually aids the stabilization of the disordered state. We predict static and dynamic spin structure factors to guide future neutron scattering experiments.

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