arXiv subjects

Daniel Phelan

Publications and source records attributed to Daniel Phelan.

13 recordsLinked to original sources

arXiv2026

Model-free Analysis of Scattering and Imaging Data with Escort-Weighted Shannon Entropy and Divergence Matrices

We demonstrate a model-free data analysis framework that leverages escort-weighted Shannon Entropy and several divergence matrices to detect phase transitions in scattering and imaging datasets. By establishing a connection between physical entropy and informational entropy, this approach provides a sensitive method for identifying phase transitions without an explicit physical model or order parameter. We further show that pairwise divergence matrices, including Kullback-Leibler divergence, Jeffrey Divergence, Jensen-Shannon Divergence and antisymmetric Kullback-Leibler divergence, provide more comprehensive measures of statistical changes than scalar entropy alone. Our approach successfully detects the onset of both long- and short-range order in neutron and X-ray scattering data, as well as a non-trivial phase transition in magnetic skyrmion lattices observed through Lorentz-transition electron microscopy. These results establish a framework for automated, model-free analysis of experimental data with broad applications in materials science and condensed matter physics.

cond-mat.mtrl-sci↗

arXiv2025

Insulating ground state and 2-k magnetic structure of candidate Weyl Hydrogen atom K$_2$Mn$_3$(AsO$_4$)$_3$

The ideal Weyl 'Hydrogen-atom' semi-metal exhibits only a single pair of Weyl nodes and no other trivial states at the Fermi energy. Such a material would be a panacea in the study of Weyl quasi particles allowing direct unambiguous observation of their topological properties. The alluaudite-like K$_2$Mn$_3$(AsO$_4$)$_3$ compound was recently proposed as such a material. Here we use comprehensive experimental work and first principle calculations to assess this prediction. We find K$_2$Mn$_3$(AsO$_4$)$_3$ crystallizes in the $C2/c$ symmetry with a quasi-1D Mn sublattice, growing as small needle-like crystals. Bulk properties measurements reveal magnetic transitions at $\approx$ 8 and $\approx$ 4 K which neutron scattering experiments show correspond to two distinct magnetic orders, first a partially ordered ferrimagnetic $\mathbf{k_1}$= (0, 0, 0) structure at 8 K and a second transition of $\mathbf{k_2}$= (1, 0, 0) at 4 K to a fully ordered state. Below the second transition, both ordering vectors are necessary to describe the complex magnetic structure with modulated spin magnitudes. Both of the best-fit magnetic structures in this work are found to break the symmetry necessary for the generation of the Weyl nodes, though one of the magnetic structures allowed by $\mathbf{k_1}$ does preserve this symmetry. However, the crystals are optically transparent and ellipsometry measurements reveal a large band-gap, undermining expectations of semi-metallic behavior. Density functional theory calculations predict an insulating antiferromagnetic ground state, in contrast to previous reports, and suggest potential frustration on the magnetic sublattice. Given the wide tunability of the alluaudite structure we consider ways to push the system closer to semi-metallic state.

cond-mat.str-el↗

arXiv2025

The 6H-Perovskite Dimer Lattice with Antiferromagnetic Interactions: Ba$_3$ARu$_2$O$_9$

We investigate the magnetic behavior of the 6H-perovskite dimer lattice Ba$_3$Zn$_{1-x}$Ca$_x$Ru$_2$O$_9$ using analytical theory, density functional theory, inelastic neutron scattering, and modeling of historical magnetization and neutron-scattering data. A dimer mean-field theory built upon classical Luttinger-Tisza analysis generates a phase diagram revealing a transition from a nonmagnetic singlet to a finite-moment ground state as interdimer couplings increase. A (generalized) linear spin-wave theory captures multiplet mixing, excitation gap closing, and fluctuation-induced moment suppression. Density functional theory on select compounds and neutron spectroscopy on dilute Ba$_3$Zn(Ru$_{1-x}$Sb$_x$)$_2$O$_9$ confirm the exchange hierarchy, enabling quantification of previously published experiments within this framework. Our results identify three mechanisms for magnetic moment suppression: quantum fluctuations, ligand hybridization, and nonmagnetic-singlet/magnetic-multiplet mixing.

cond-mat.str-el↗

arXiv2025

Lattice-charge coupling in a trilayer nickelate with intertwined density wave order

Intertwined charge and spin correlations are ubiquitous in a wide range of transition metal oxides and are often perceived as intimately related to unconventional superconductivity. Theoretically envisioned as driven by strong electronic correlations, the intertwined order is usually found to be strongly coupled to the lattice as signaled by pronounced phonon softening. Recently, both charge/spin density waves (CDW/SDW) and superconductivity have been discovered in several Ruddlesden-Popper (RP) nickelates, in particular trilayer nickelates RE4Ni3O10 (RE=Pr, La). The nature of the intertwined order and the role of lattice-charge coupling are at the heart of the debate about these materials. Using inelastic X-ray scattering, we mapped the phonon dispersions in RE4Ni3O10 and found no evidence of phonon softening near the CDW wavevector over a wide temperature range. Calculations of the electronic susceptibility revealed a peak at the observed SDW ordering vector but not at the CDW wavevector. The absence of phonon softening is in sharp contrast to that in canonical oxide materials, notably cuprates. Our experimental and theoretical findings highlight the crucial role of the spin degree of freedom and establish a foundation for understanding the interplay between superconductivity and density-wave transitions in RP nickelate superconductors and beyond.

cond-mat.str-el↗

arXiv2024

Non-equilibrium dynamics in geometrically frustrated spin glass Bi$_2$Fe$_3$GaO$_9$ with a Cairo lattice

We have explored the relaxation process of the spin glass phase in Bi$_2$Fe$_3$GaO$_9$, a geometrically frustrated magnet with a unique structure consisting of pentagonal building blocks known as the Cairo lattice. Using dc magnetization measurements on single crystals, we estimate the relaxation time across various temperatures and fields. Our results indicate that the relaxation time of Bi$_2$Fe$_3$GaO$_9$ follows the Arrhenius law as a function of temperature but remains relatively constant as the applied magnetic field varies. Further, through a carefully designed protocol, we observe significant rejuvenation and memory effects. Remarkably, the memory effects in Bi$_2$Fe$_3$GaO$_9$ are found to be more similar to those observed in classical spin glasses rather than in spin jamming systems, both in terms of the magnitude of the memory effect and the value of the exponent that describes the relaxation behavior. Our findings suggest that Bi$_2$Fe$_3$GaO$_9$ provides an excellent platform for investigating the time-dependent evolution of underlying magnetism using neutron scattering, paving the way for future research.

cond-mat.dis-nn↗

arXiv2023

Local atomic and magnetic structure of multiferroic (Sr,Ba)(Mn,Ti)O$_3$

We present a detailed study of the local atomic and magnetic structure of the type-I multiferroic perovskite system (Sr,Ba)(Mn,Ti)O$_3$ using x-ray and neutron pair distribution function (PDF) analysis, polarized neutron scattering, and muon spin relaxation ($\mu$SR) techniques. The atomic PDF analysis reveals widespread nanoscale tetragonal distortions of the crystal structure even in the paraelectric phase with average cubic symmetry, corresponding to incipient ferroelectricity in the local structure. Magnetic PDF analysis, polarized neutron scattering, and $\mu$SR likewise confirm the presence of short-range antiferromagnetic correlations in the paramagnetic state, which grow in magnitude as the temperature approaches the magnetic transition. We show that these short-range magnetic correlations coincide with a reduction of the tetragonal (i.e. ferroelectric) distortion in the average structure, suggesting that short-range magnetism can play an important role in magnetoelectric and/or magnetostructural phenomena even without genuine long-range magnetic order. The reduction of the tetragonal distortion scales linearly with the local magnetic order parameter, pointing to spontaneous linear magnetoelectric coupling in this system. These findings provide greater insight into the multiferroic properties of (Sr,Ba)(Mn,Ti)O$_3$ and demonstrate the importance of investigating the local atomic and magnetic structure to gain a deeper understanding of the intertwined degrees of freedom in multiferroics.

cond-mat.str-el↗

arXiv2022

Thermal Hysteresis Behavior of Skyrmion Lattices in the van der Waals Ferromagnet Fe3GeTe2

Understanding the physics of phase transitions in two-dimensional (2D) systems underpins the research in diverse fields including statistical mechanics, quantum systems, nanomagnetism, and soft condensed matter. However, many fundamental aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions, which are non-trivial chiral spin structures, can be considered as quasi-particles that form two-dimensional lattices. Here we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. Our quantitative analysis explains this behavior based on the energy landscape of skyrmions and demonstrates the potential to control the lattice order in 2D phase transitions.

cond-mat.mtrl-sci↗

arXiv2022

Competing Charge/Spin-Stripe and Correlated Metal Phases in Trilayer Nickelates (Pr$_{1-x}$La$_x$)$_4$Ni$_3$O$_8$

Low-valent nickelates R$_{n+1}$Ni$_n$O$_{2n+2}$ (R = rare earth) containing Ni$^{1+}$ (d$^{9}$) with a quasi-two-dimensional (quasi-2D) square planar coordination geometry possess structural and electronic properties that are similar to those of high-Tc cuprates, including superconductivity itself in the doped infinite layer ($n = \infty$) RNiO$_2$ system. Within this R$_{n+1}$Ni$_n$O$_{2n+2}$ nickelate family, the crystallographic isomorphs Pr$_4$Ni$_3$O$_8$ and La$_4$Ni$_3$O$_8$ exhibit singularly different ground states: Pr$_4$Ni$_3$O$_8$ is metallic and La$_4$Ni$_3$O$_8$ is a charge- and spin-stripe ordered insulator. To explore and understand the ground state evolution from metallic Pr$_4$Ni$_3$O$_8$ to stripe-ordered La$_4$Ni$_3$O$_8$ in the R$_4$Ni$_3$O$_8$ family, we have grown a series of isovalent-substituted single crystals (Pr$_{1-x}$La$_x$)$_4$Ni$_3$O$_8$. Combining thermodynamic, transport, magnetic, and synchrotron X-ray single crystal diffraction measurements, we reveal a transition between metallic and stripe-insulator phase regions, with a putative quantum phase transition at x = 0.4. We propose two possible models for (Pr$_{1-x}$La$_x$)$_4$Ni$_3$O$_8$: an electronically inhomogeneous system that could serve as a candidate for exploring quantum Griffiths phase physics and a homogeneous system with a putative quantum critical point at the phase boundary.

cond-mat.str-el↗

arXiv2021

The essential role of magnetic frustration in the phase diagrams of doped cobaltites

Doped perovskite cobaltites (e.g., La$_{1-x}$Sr$_x$CoO$_3$) have been extensively studied for their spin-state physics, electronic inhomogeneity, and insulator-metal transitions. Ferromagnetically-interacting spin-state polarons emerge at low $x$ in the phase diagram of these compounds, eventually yielding long-range ferromagnetism. The onset of long-range ferromagnetism ($x \approx 0.18$) is substantially delayed relative to polaron percolation ($x \approx 0.05$), however, generating a troubling inconsistency. Here, Monte-Carlo simulations of a disordered classical spin model are used to establish that previously ignored magnetic frustration is responsible for this effect, enabling faithful reproduction of the magnetic phase diagram.

cond-mat.str-el↗

arXiv2021

Harnessing Interpretable and Unsupervised Machine Learning to Address Big Data from Modern X-ray Diffraction

The information content of crystalline materials becomes astronomical when collective electronic behavior and their fluctuations are taken into account. In the past decade, improvements in source brightness and detector technology at modern x-ray facilities have allowed a dramatically increased fraction of this information to be captured. Now, the primary challenge is to understand and discover scientific principles from big data sets when a comprehensive analysis is beyond human reach. We report the development of a novel unsupervised machine learning approach, XRD Temperature Clustering (X-TEC), that can automatically extract charge density wave (CDW) order parameters and detect intra-unit cell (IUC) ordering and its fluctuations from a series of high-volume X-ray diffraction (XRD) measurements taken at multiple temperatures. We apply X-TEC to XRD data on a quasi-skutterudite family of materials, (Ca$_x$Sr$_{1-x}$)$_3$Rh$_4$Sn$_{13}$, where a quantum critical point arising from charge order is observed as a function of Ca concentration. We further apply X-TEC to XRD data on the pyrochlore metal, Cd$_2$Re$_2$O$_7$, to investigate its two much debated structural phase transitions and uncover the Goldstone mode accompanying them. We demonstrate how unprecedented atomic scale knowledge can be gained when human researchers connect the X-TEC results to physical principles. Specifically, we extract from the X-TEC-revealed selection rule that the Cd and Re displacements are approximately equal in amplitude, but out of phase. This discovery reveals a previously unknown involvement of $5d^2$ Re, supporting the idea of an electronic origin to the structural order. Our approach can radically transform XRD experiments by allowing in-operando data analysis and enabling researchers to refine experiments by discovering interesting regions of phase space on-the-fly.

cond-mat.str-el↗

arXiv2019

High pO2 Floating Zone Crystal Growth of the Perovskite Nickelate PrNiO3

Single crystals of PrNiO3 were grown under an oxygen pressure of 295 bar using a unique high-pressure optical-image floating zone furnace. The crystals, with volume in excess of 1 mm3, were characterized structurally using single crystal and powder X-ray diffraction. Resistivity, specific heat, and magnetic susceptibility were measured, all of which evidenced an abrupt, first order metal-insulator transition (MIT) at ~130 K, in agreement with previous literature reports on polycrystalline specimens. Temperature-dependent single crystal diffraction was performed to investigate changes through the MIT. Our study demonstrates the opportunity space for high fugacity, reactive environments for single crystal growth specifically of perovskite nickelates but more generally to correlated electron oxides.

cond-mat.mtrl-sci↗

arXiv2017

Nonlinear Pauli Susceptibilities in Sr$_3$Ru$_2$O$_7$ and Universal Features of Itinerant Metamagnetism

We report, for the first time, measurements of the third order, $χ_3$ and fifth order, $χ_5$, susceptibilities in an itinerant oxide metamagnet, Sr$_3$Ru$_2$O$_7$ for magnetic fields both parallel and perpendicular to the c-axis. These susceptibilities exhibit maxima in their temperature dependence such that $T_1 \approx 2T_3 \approx 4T_5$ where the $T_i$ are the position in temperature where a peak in the $i$-th order susceptibility occurs. These features taken together with the scaling of the critical field with the temperature $T_1$ observed in a diverse variety of itinerant metamagnets find a natural explanation in a single band model with one Van Hove singularity (VHS) and onsite repulsion $U$. The separation of the VHS from the Fermi energy $Δ$, sets a single energy scale, which is the primary driver for the observed features of itinerant metamagnetism at low temperatures.

cond-mat.str-el↗

arXiv2009

Pressure-Induced Effects on the Structure of the FeSe Superconductor

A polycrystalline sample of FeSe, which adopts the tetragonal PbO-type structure (P4/nmm) at room temperature, has been prepared using solid state reaction. We have investigated pressure-induced structural changes in tetragonal FeSe at varying hydrostatic pressures up to 0.6 GPa in the orthorhombic (T = 50 K) and tetragonal (T = 190 K) phases using high resolution neutron powder diffraction. We report that the structure is quite compressible with a Bulk modulus around 31 GPa to 33 GPa and that the pressure response is anisotropic with a larger compressibility along the c-axis. Key bond angles of the SeFe4 pyramids and FeSe4 tetrahedra are also determined as a function of pressure.

cond-mat.supr-con↗