arXiv subjects

Alex Hallett

Publications and source records attributed to Alex Hallett.

4 recordsLinked to original sources

arXiv2026

Chirality in BaTiOCu$_4$(PO$_4$)$_4$

We present a first principles study of the ferrochiral phase transition in chiral BaTiOCu$_4$(PO$_4$)$_4$, which has been shown using X-ray diffraction to proceed via the antiferroaxial rotation of antipolar structural units. We analyze the atomic-site electric and magnetic multipole moments to identify connections between these multipoles and chirality and corroborate the previous experimental interpretation. We show that antiferroically ordered atomic-site electric toroidal dipole moments act as an order parameter for the antiferroaxial rotations, and that the overall chiral order is parameterized by the composite order of the antipolar electric dipole and electric toroidal dipole moments. Finally, we evaluate the suitability of various proposed order parameters for chirality, show that some can be excluded and suggest the most promising directions for future exploration.

cond-mat.mtrl-sci↗

arXiv2024

Effects of doping on polar order in SrTiO$_{3}$ from first-principles modeling

SrTiO$_{3}$ is an incipient ferroelectric and an exceptionally dilute superconductor with a dome-like dependence on carrier concentration. Stabilization of a polar phase through chemical substitution or strain significantly enhances the superconducting critical temperature, suggesting a possible connection between the polar instability and unconventional Cooper pairing. To investigate the effects of doping on the polar order in SrTiO$_{3}$, we develop a simplified free energy model which includes only the degrees of freedom necessary to capture the relevant physics of a doped, biaxially compressively strained system. We simulate the polar and antiferrodistortive thermal phase transitions using Monte Carlo methods for different doping levels and comment on the doping dependence of the transition temperatures and the formation of polar nanodomains. In addition, the temperature-dependent phonon spectral function is calculated using Langevin simulations to investigate the lattice dynamics of the doped system. We also examine the effects of doping on the electronic structure within the polar phase, including the density of states and band splitting. Finally, we compute the polarization dependence of the Rashba parameter and the doping dependence of the Midgal ratio, and place our results in the broader context of proposed pairing mechanisms.

cond-mat.supr-con↗

arXiv2023

Combinatorial exploration of quantum spin liquid candidates in the herbertsmithite material family

Geometric frustration of magnetic ions can lead to a quantum spin liquid ground state where long range magnetic order is avoided despite strong exchange interactions. The physical realization of quantum spin liquids comprises a major unresolved area of contemporary materials science. One prominent magnetically-frustrated structure is the kagome lattice. The naturally occurring minerals herbertsmithite [ZnCu$_3$(OH)$_6$Cl$_2$] and Zn-substituted barlowite [ZnCu$_3$(OH)$_6$BrF] both feature perfect kagome layers of spin-$1/2$ copper ions and display experimental signatures consistent with a quantum spin liquid state at low temperatures. To investigate other possible candidates within this material family, we perform a systematic first-principles combinatorial exploration of structurally related compounds [$A$Cu$_3$(OH)$_6B_2$ and $A$Cu$_3$(OH)$_6BC$] by substituting non-magnetic divalent cations ($A$) and halide anions ($B$, $C$). After optimizing such structures using density functional theory, we compare various structural and thermodynamic parameters to determine which compounds are most likely to favor a quantum spin liquid state. Convex hull calculations using binary compounds are performed to determine feasibility of synthesis. We also estimate the likelihood of interlayer substitutional disorder and spontaneous distortions of the kagome layers. After considering all of these factors as a whole, we select several promising candidate materials that we believe deserve further attention.

cond-mat.str-el↗

arXiv2022

Modeling polar order in compressively strained SrTiO$_{3}$

Strontium titanate is an incipient ferroelectric in which superconductivity emerges at exceptionally low doping levels. Remarkably, stabilizing the polar phase through strain or chemical substitution has been shown to significantly enhance the superconducting critical temperature, and the polar instability plays a pivotal role in the majority of proposed superconducting pairing mechanisms. A rigorous understanding of ferroelectricity is therefore essential to elucidate the electron pairing mechanism in this material. To investigate the nature of the polar order in strontium titanate, we develop a simplified free energy model that only includes the degrees of freedom necessary to capture the relevant physics in a biaxially compressively strained system. Our model is able to calculate the energies of large, disordered systems with near DFT-level accuracy. We simulate the ferroelectric and antiferrodistortive phase transitions using the Monte Carlo method and discuss the coupling between various order parameters. Finally, we assess the character of the polar transition, which we find to be neither strictly displacive nor order-disorder.

cond-mat.mtrl-sci↗