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arXiv:2009.14492 · Nature

A quantum magnetic analogue to the critical point of water

Julio Larrea Jiménez, S. P. G. Crone, Ellen Fogh, Mohamed Zayed, Rolf Lortz, Ekaterina V. Pomjakushina, K. Conder, Andreas Martin Läuchli, Lukas Weber, Stefan Weßel, A. Honecker, Bruce Normand, Christian Rüegg, Philippe Corboz, Henrik Moodysson Rønnow, Frédéric Mila

Published Apr 14, 2021• 129 citations
arXivHTMLPDF

Abstract

Abstract At the familiar liquid-gas phase transition in water, the density jumps discontinuously at atmospheric pressure, but the line of these first-order transitions defined by increasing pressures terminates at the critical point [1], a concept ubiquitous in statistical thermodynamics [2]. In correlated quantum materials, a critical point was predicted [3] and measured [4, 5] terminating the line of Mott metal-insulator transitions, which are also first-order with a discontinuous charge density. In quantum spin systems, continuous quantum phase transitions (QPTs) [6] have been investigated extensively [7-11], but discontinuous QPTs have received less attention. The frustrated quantum antiferromagnet SrCu2(BO3)2 constitutes a near-exact realization of the paradigmatic Shastry-Sutherland model [12-14] and displays exotic phenomena including magnetization plateaux [15], anomalous thermodynamics [16] and discontinuous QPTs [17]. We demonstrate by high-precision specific-heat measurements under pressure and applied magnetic field that, like water, the pressure-temperature phase diagram of SrCu2(BO3)2 has an Ising critical point terminating a first-order transition line, which separates phases with different densities of magnetic particles (triplets). We achieve a quantitative explanation of our data by detailed numerical calculations using newly-developed finite temperature tensor-network methods [16, 18-20]. These results open a new dimension in understanding the thermodynamics of quantum magnetic materials, where the anisotropic spin interactions producing topological properties [21, 22] for spintronic applications drive an increasing focus on first-order QPTs.

DOI
10.1038/s41586-021-03411-8

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Abstract At the familiar liquid-gas phase transition in water, the density jumps discontinuously at atmospheric pressure, but the line of these first-order transitions defined by increasing pressures terminates at the critical point [1], a concept ubiquitous in statistical thermodynamics [2]. In correlated quantum materials, a critical point was predicted [3] and measured [4, 5] terminating the line of Mott metal-insulator transitions, which are also first-order with a discontinuous charge density. In quantum spin systems, continuous quantum phase transitions (QPTs) [6] have been investigated extensively [7-11], but discontinuous QPTs have received less attention. The frustrated quantum antiferromagnet SrCu2(BO3)2 constitutes a near-exact realization of the paradigmatic Shastry-Sutherland model [12-14] and displays exotic phenomena including magnetization plateaux [15], anomalous thermodynamics [16] and discontinuous QPTs [17]. We demonstrate by high-precision specific-heat measurements under pressure and applied magnetic field that, like water, the pressure-temperature phase diagram of SrCu2(BO3)2 has an Ising critical point terminating a first-order transition line, which separates phases with different densities of magnetic particles (triplets). We achieve a quantitative explanation of our data by detailed numerical calculations using newly-developed finite temperature tensor-network methods [16, 18-20]. These results open a new dimension in understanding the thermodynamics of quantum magnetic materials, where the anisotropic spin interactions producing topological properties [21, 22] for spintronic applications drive an increasing focus on first-order QPTs.
Abstract Phase transitions in condensed matter are a source of exotic emergent properties. We study the fully frustrated bilayer Heisenberg antiferromagnet to demonstrate that an applied magnetic field creates a previously unknown emergent criticality. The quantum phase diagram contains four states with distinctly different symmetries, all but one pair separated by first-order transitions. We show by quantum Monte Carlo simulations that the thermal phase diagram is dominated by a wall of discontinuities extending between the dimer-triplet phases and the singlet-containing phases. This wall is terminated at finite temperatures by a critical line, which becomes multicritical where the Berezinskii-Kosterlitz-Thouless (BKT) transition of the dimer-triplet antiferromagnet and the thermal Ising transition of the singlet-triplet crystal phase also terminate. The combination of merging symmetries leads to a 4-state Potts universality not contained in the microscopic Hamiltonian, which we interpret within the Ashkin-Teller model. Our results represent a systematic step in understanding emergent phenomena in quantum magnetic materials, including the “Shastry-Sutherland compound” SrCu2(BO3)2.
Inspired by recent experimental measurements [Guo et al., Phys. Rev. Lett. 124, 206602 (2020PRLTAO0031-900710.1103/PhysRevLett.124.206602); Jiménez et al., Nature (London) 592, 370 (2021)NATUAS0028-083610.1038/s41586-021-03411-8] on frustrated quantum magnet SrCu_{2}(BO_{3})_{2} under combined pressure and magnetic fields, we study the related spin-1/2 Shastry-Sutherland model using state-of-the-art tensor network methods. By calculating thermodynamics, correlations, and susceptibilities, we find, in zero magnetic field, not only a line of first-order dimer-singlet to plaquette-singlet phase transition ending with a critical point, but also signatures of the ordered plaquette-singlet transition with its critical end point terminating on this first-order line. Moreover, we uncover prominent magnetic barocaloric responses, a novel type of quantum correlation induced cooling effect, in the strongly fluctuating supercritical regime. Under finite fields, we identify a quantum phase transition from the plaquette-singlet phase to the spin supersolid phase that breaks simultaneously lattice translational and spin rotational symmetries. The present findings on the Shastry-Sutherland model are accessible in current experiments and would shed new light on the critical and supercritical phenomena in the archetypal frustrated quantum magnet SrCu_{2}(BO_{3})_{2}.
We consider the finite-temperature phase diagram of the S=1/2 frustrated Heisenberg bilayer. Although this two-dimensional system may show magnetic order only at zero temperature, we demonstrate the presence of a line of finite-temperature critical points related to the line of first-order transitions between the dimer-singlet and -triplet regimes. We show by high-precision quantum Monte Carlo simulations, which are sign-free in the fully frustrated limit, that this critical point is in the Ising universality class. At zero temperature, the continuous transition between the ordered bilayer and the dimer-singlet state terminates on the first-order line, giving a quantum critical end point, and we use tensor-network calculations to follow the first-order discontinuities in its vicinity.
Quantum phase transition arises in general as second order phase transition at zero temperature, tuned by a non-thermal parameter such as pressure, doping or a magnetic field. The point in the phase diagram of the material in which different phases meet is called a quantum critical point (QCP). Physics around QCPs are of extensive current interest because the critical quantum fluctuations influence the physical properties in a wide temperature range (quantum criticality), and are believed to be responsible for many emergent physical properties such as non-Fermi liquids and unconventional superconductivity. In this research we explore dynamics and thermodynamics near QCPs via investigating three classes of models, which all have real material correspondence. Specifically first, we study local dynamics in a perturbed quantum critical Ising chain with E8 symmetry, where we show the local dynamical spin susceptibility has a singular dependence on frequency, but differs from the diffusion form. The nuclear magnetic resonance (NMR) relaxation rate at low temperatures depends exponentially on the inverse temperature, whose prefactor we also determine. We propose NMR experiments as a means to further test the applicability of the E8 description for CoNb2O6. Second, we investigate the thermodynamic properties of itinerant ferromagnets near quantum critical points, described by the quantum Landau-Ginzburg theory. We provide a regularized perturbative renormalization group procedure to calculate the free energy. We further carry out numerical calculations on thermodynamic quantities, capturing not only the leading critical behaviors, but also the subleading and nonsingular contributions. We demonstrate various thermodynamic signatures of quantum criticality, including the entropy accumulation effect and the divergence of the specific heat coefficient. A detailed comparison to the recent experimental results on an itinerant ferromagnet Sr3Ru2O7 is also presented. Third, we explore Ising-nematic and magnetic phases and their transitions in iso-electronically doped iron pnictides by carrying out a large-N study of an effective low-energy Ginzburg-Landau model for these systems. We demonstrate that the magnetic and Ising orders transitions are concurrent at zero temperature, and both transitions are weakly first-order, which is consistent with RG-based prediction and experimental observations.
Abstract The 2-dimensional layered oxide material SrCu2(BO3)2, long studied as a realization of the Shastry-Sutherland spin topology, exhibits a range of intriguing physics as a function of both hydrostatic pressure and magnetic field, with a still debated intermediate plaquette phase appearing at approximately 20 kbar and a possible deconfined critical point at higher pressure. Here, we employ a tunnel diode oscillator (TDO) technique to probe the behavior in the combined extreme conditions of high pressure, high magnetic field, and low temperature. We reveal an extensive phase space consisting of multiple magnetic analogs of the elusive supersolid phase and a magnetization plateau. In particular, a 10 × 2 supersolid and a 1/5 plateau, identified by infinite Projected Entangled Pair States (iPEPS) calculations, are found to rely on the presence of both magnetic and non-magnetic particles in the sea of dimer singlets. These states are best understood as descendants of the full-plaquette phase, the leading candidate for the intermediate phase of SrCu2(BO3)2.
The phase diagrams of highly frustrated quantum spin systems can exhibit first-order quantum phase transitions and thermal critical points even in the absence of any long-ranged magnetic order. However, all unbiased numerical techniques for investigating frustrated quantum magnets face significant challenges, and for generic quantum Monte Carlo methods the challenge is the sign problem. Here we report on a general quantum Monte Carlo approach with a loop-update scheme that operates in any basis, and we show that, with an appropriate choice of basis, it allows us to study a frustrated model of coupled spin-1/2 trimers: simulations of the trilayer Heisenberg antiferromagnet in the spin-trimer basis are sign-problem-free when the intertrimer couplings are fully frustrated. This model features a first-order quantum phase transition, from which a line of first-order transitions emerges at finite temperatures and terminates in a thermal critical point. The trimer unit cell hosts an internal degree of freedom that can be controlled to induce an extensive entropy jump at the quantum transition, which alters the shape of the first-order line. We explore the consequences for the thermal properties in the vicinity of the critical point, which include profound changes in the lines of maxima defined by the specific heat. Our findings reveal trimer quantum magnets as fundamental systems capturing in full the complex thermal physics of the strongly frustrated regime.