Asymmetric phase diagram and dimensional crossover in a system of spin-1/2 dimers under applied hydrostatic pressure

TL;DR

This study explores how applying pressure to a spin-1/2 dimer system causes a dimensional crossover and introduces a new quantum critical point, revealing complex magnetic phase behavior influenced by pressure-induced structural changes.

Contribution

It provides the first detailed analysis of pressure effects on the magnetic phase diagram and quantum criticality in a quasi-two-dimensional spin-1/2 dimer material.

Findings

Emergence of a new phase above the upper field transition at high pressure

Identification of a zero-field quantum critical point at 15.7 kbar

Pressure induces a dimensional crossover driven by interdimer interactions

Abstract

We present the magnetic and structural properties of [Cu(pyrazine)$_{0.5}$(glycine)]ClO$_4$ under applied pressure. As previously reported, at ambient pressure this material consists of quasi-two-dimensional layers of weakly coupled antiferromagnetic dimers which undergo Bose-Einstein condensation of triplet excitations between two magnetic field-induced quantum critical points (QCPs). The molecular building blocks from which the compound is constructed give rise to exchange strengths that are considerably lower than those found in other $S = 1/2$ dimer materials, which allows us to determine the pressure evolution of the entire field-temperature magnetic phase diagram using radio-frequency magnetometry. We find that a distinct phase emerges above the upper field-induced transition at elevated pressures and also show that an additional QCP is induced at zero-field at a critical pressure of $p_{\rm c} = 15.7(5)$ kbar. Pressure-dependent single-crystal X-ray diffraction and density functional theory calculations indicate that this QCP arises primarily from a dimensional crossover driven by an increase in the interdimer interactions between the planes. While the effect of quantum fluctuations on the lower field-induced transition is enhanced with applied pressure, quantum Monte Carlo calculations suggest that this alone cannot explain an unconventional asymmetry that develops in the phase diagram.