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Nature Communications

Double dome structure of the Bose–Einstein condensation in diluted S = 3/2 quantum magnets

Yoshito Watanabe, Atsushi Miyake, Masaki Gen, Yuta Mizukami, Kenichiro Hashimoto, T. Shibauchi, Akihiko Ikeda, Masashi Tokunaga, Takashi Kurumaji, Y. Tokunaga, T. Arima

Published Mar 10, 2023• 5 citations
Publisher

Abstract

Abstract Bose–Einstein condensation (BEC) in quantum magnets, where bosonic spin excitations condense into ordered ground states, is a realization of BEC in a thermodynamic limit. Although previous magnetic BEC studies have focused on magnets with small spins of S ≤ 1, larger spin systems potentially possess richer physics because of the multiple excitations on a single site level. Here, we show the evolution of the magnetic phase diagram of S = 3/2 quantum magnet Ba2CoGe2O7 when the averaged interaction J is controlled by a dilution of magnetic sites. By partial substitution of Co with nonmagnetic Zn, the magnetic order dome transforms into a double dome structure, which can be explained by three kinds of magnetic BECs with distinct excitations. Furthermore, we show the importance of the randomness effects induced by the quenched disorder: we discuss the relevance of geometrical percolation and Bose/Mott glass physics near the BEC quantum critical point.

DOI
10.1038/s41467-023-36725-4

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arXiv:cond-mat/0203052•Physical Review A•May 29, 2002•163 citations
Abstract Bose–Einstein condensation (BEC) in quantum magnets, where bosonic spin excitations condense into ordered ground states, is a realization of BEC in a thermodynamic limit. Although previous magnetic BEC studies have focused on magnets with small spins of S ≤ 1, larger spin systems potentially possess richer physics because of the multiple excitations on a single site level. Here, we show the evolution of the magnetic phase diagram of S = 3/2 quantum magnet Ba2CoGe2O7 when the averaged interaction J is controlled by a dilution of magnetic sites. By partial substitution of Co with nonmagnetic Zn, the magnetic order dome transforms into a double dome structure, which can be explained by three kinds of magnetic BECs with distinct excitations. Furthermore, we show the importance of the randomness effects induced by the quenched disorder: we discuss the relevance of geometrical percolation and Bose/Mott glass physics near the BEC quantum critical point.
The recent experimental advances in the field of quantum spin materials have led to well-controlled systems which can be used in order to simulate complex quantum models in a clean fashion. Here we discuss how fascinating effects normally known from bosonic systems such as the Bose-Einstein condensation can be investigated with the help of such materials. We discuss as an example how a crossover between an effectively one-dimensional geometry described by a Luttinger liquid to a three-dimensional Bose-Einstein condensation can be induced. Additionally, we point out how more complex phases as the Bose-glass phase could be realized in these quantum magnets. Introduction Although it can seem paradoxical, the quantum magnetic states found in insulators offer an interesting route to study Bose-Einstein condensation (BEC) and more generally phenomena related to itinerant, interacting bosonic systems. In many materials, the repulsion between the electrons causes the ground state to be a Mott insulator with one electron localized per site. In such a case, the charge degrees of freedom are completely locked by large charge gaps (usually of the order of tens of electron volts). However, one can study the fascinating physics of the spin degrees of freedom. As was shown a long time ago, the localized spins are coupled by a so-called superexchange which may be ferro- or antiferromagnetic. The properties of the exchange coupling between the spins depend mainly on the underlying atomic structure of the material. The resulting physics is extremely rich and such materials can have a host of phases ranging from ordered magnetic phases to so-called spin-liquid phases in which spin–spin correlations decay extremely fast with distance. The field of research concerning these materials, dubbed quantum magnetism, is thus an extremely active field in its own right [1]. Additionally, one can exploit the formal mapping that exists between spin operators and bosonic ones, as will be described in the next section, to connect the magnetic materials to itinerant bosonic systems with interactions between the bosons. This opens the way to use such quantum spin systems as quantum simulators. A quantum simulator means that the experimental system can be employed in order to “solve” in a controlled way a problem/Hamiltonian known from a different less controlled physical realization, e.g., inspired by fundamental many-body physics, quantum information or computational applications.
We numerically investigate the phase diagram of two-dimensional site-diluted coupled dimer systems in an external magnetic field. We show that this phase diagram is characterized by the presence of an extended Bose glass, not accessible to mean-field approximation, and stemming from the localization of two distinct species of bosonic quasiparticles appearing in the ground state. On the one hand, nonmagnetic impurities doped into the dimer-singlet phase of a weakly coupled dimer system are known to free up local magnetic moments. The deviations of these local moments from full polarization along the field can be mapped onto a gas of bosonic quasiparticles, which undergo condensation in zero and very weak magnetic fields, corresponding to transverse long-range antiferromagnetic order. An increasing magnetic field lowers the density of such quasiparticles to a critical value at which a quantum phase transition occurs, corresponding to the quasiparticle localization on clusters of local magnets (dimers, trimers, etc.) and to the onset of a Bose glass. Strong finite-size quantum fluctuations hinder further depletion of quasiparticles from such clusters, and thus lead to the appearance of pseudoplateaus in the magnetization curve of the system. On the other hand, site dilution hinders the field-induced Bose-Einstein condensation of triplet quasiparticles on the intact dimers, and it introduces instead a Bose glass of triplets. A thorough numerical investigation of the phase diagram for a planar system of coupled dimers shows that the two above-mentioned Bose glass phases are continuously connected, and they overlap in a finite region of parameter space, thus featuring a two-species Bose glass. The quantum phase transition from Bose glass to magnetically ordered phases in two dimensions is marked by novel universal exponents ($z\ensuremath{\approx}2$, $\ensuremath{\beta}\ensuremath{\approx}0.9$, and $\ensuremath{\nu}\ensuremath{\approx}1$). Hence we conclude that doped quantum antiferromagnets in a field represent an ideal setting for the study of fundamental dirty-boson physics.
This article reviews experimental and theoretical work on Bose-Einstein condensation in quantum magnets. These magnets are natural realizations of gases of interacting bosons whose relevant parameters such as dimensionality, lattice geometry, amount of disorder, nature of the interactions, and particle concentration can vary widely between different compounds. The particle concentration can be easily tuned by applying an external magnetic field which plays the role of a chemical potential. This rich spectrum of realizations offers a unique possibility for studying the different physical behaviors that emerge in interacting Bose gases from the interplay between their relevant parameters. The plethora of other bosonic phases that can emerge in quantum magnets, of which the Bose-Einstein condensate is the most basic ground state, is reviewed. The compounds discussed in this review have been intensively studied in the last two decades and have led to important contributions in the area of quantum magnetism. In spite of their apparent simplicity, these systems often exhibit surprising behaviors. The possibility of using controlled theoretical approaches has triggered the discovery of unusual effects induced by frustration, dimensionality, or disorder.
It is investigated theoretically that magnetized Bose-Einstein condensation (BEC) with the internal (spin) degrees of freedom exhibits a rich variety of phase transitions, depending on the sign of the interaction in the spin channel. In the antiferromagnetic interaction case there exist always double BEC transitions from single component BEC to multiple component BEC. In the ferromagnetic case BEC becomes always unstable at a lower temperature, leading to a phase separation. The detailed phase diagram for the temperature vs the polarization, the spatial spin structure, the distribution of non-condensates and the excitation spectrum are examined for the harmonically trapped systems.
The field-induced antiferromagnetic ordering in systems of weakly coupled S = 1/2 dimers at zero temperature can be described as a Bose-Einstein condensation of triplet quasiparticles (singlet quasiholes) in the ground state. For the case of a Heisenberg bilayer, it is here shown how the above picture is altered in the presence of site dilution of the magnetic lattice. Geometric randomness leads to quantum localization of the quasiparticles or quasiholes and to an extended Bose-glass phase in a realistic disordered model. This localization phenomenon drives the system towards a quantum-disordered phase well before the classical geometric percolation threshold is reached.
The ground states of Bose-Einstein condensates (BECs) of spin-2 bosons are classified into three distinct phases (ferromagnetic, ``antiferromagnetic,'' and cyclic) depending on the s-wave scattering lengths of binary collisions for total-spin 0, 2, and 4 channels. Many-body spin correlations and magnetic response of the condensate in each of these phases are studied in a mesoscopic regime, while low-lying excitation spectra are investigated in the thermodynamic regime. In the mesoscopic regime, where the system is so tightly confined that the spatial degrees of freedom are frozen, the exact, many-body ground state for each phase is found to be expressed in terms of the creation operators of pair or trio bosons having spin correlations. These pairwise and trio-wise units are shown to bring about some unique features of spin-2 BECs such as a huge jump in magnetization from minimum to maximum possible values and the robustness of the minimum-magnetization state against an applied magnetic field. In the thermodynamic regime, where the system is spatially uniform, low-lying excitation spectra in the presence of magnetic field are obtained analytically using the Bogoliubov approximation. In the ferromagnetic phase, the excitation spectrum consists of one Goldstone mode and four single-particle modes. In the antiferromagnetic phase, where spin-singlet ``pairs'' undergo Bose-Einstein condensation, the spectrum consists of two Goldstone modes and three massive ones, all of which become massless when magnetic field vanishes. In the cyclic phase, where boson ``trios'' condense into a spin-singlet state, the spectrum is characterized by two Goldstone modes, one single-particle mode having a magnetic-field-independent energy gap, and a gapless single-particle mode that becomes massless in the absence of magnetic field.