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P. G. Freeman

Publications and source records attributed to P. G. Freeman.

At least 19 recordsLinked to original sources

Autonomous Diffractometry Enabled by Visual Reinforcement Learning

Automation underpins progress across scientific and industrial disciplines. Yet, automating tasks requiring interpretation of abstract visual information remain challenging. For example, crystal alignment strongly relies on humans with the ability to comprehend diffraction patterns. Here we introduce an autonomous system that aligns single crystals without access to crystallography and diffraction theory. Using a model-free reinforcement learning framework, an agent learns to identify and navigate towards high-symmetry orientations directly from Laue diffraction patterns. Despite the absence of human supervision, the agent develops human-like strategies to achieve time-efficient alignment across different crystal symmetry classes. With this, we provide a computational framework for intelligent diffractometers. As such, our approach advances the development of automated experimental workflows in materials science.

cs.LG

Stability of charge-stripe ordered La2-xSrxNiO4+delta at one third doping

The stability of charge ordered phases is doping dependent, with different materials having particularly stable ordered phases. In the half filled charge ordered phases of the cuprates this occurs at one eighth doping, whereas in charge-stripe ordered La2-xSrxNiO4+delta there is enhanced stability at one third doping. In this paper we discuss the known details of the charge-stripe order in La2-xSrxNiO4+delta, and how these properties lead to the one third doping stability.

cond-mat.str-el

Damped spin excitations in a doped cuprate superconductor with orbital hybridization

A resonant inelastic x-ray scattering (RIXS) study of overdamped spin-excitations in slightly underdoped La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) with $x=0.12$ and $0.145$ is presented. Three high-symmetry directions have been investigated: (1) the antinodal $(0,0)\rightarrow (1/2,0)$, (2) the nodal $(0,0)\rightarrow (1/4,1/4)$ and (3) the zone boundary direction $(1/2,0)\rightarrow (1/4,1/4)$ connecting these two. The overdamped excitations exhibit strong dispersions along (1) and (3), whereas a much more modest dispersion is found along (2). This is in strong contrast to the undoped compound La$_{2}$CuO$_4$ (LCO) for which the strongest dispersions are found along (1) and (2). The $t-t^{\prime}-t^{\prime\prime}-U$ Hubbard model used to explain the excitation spectrum of LCO predicts $-$ for constant $U/t$ $-$ that the dispersion along (3) scales with $(t^{\prime}/t)^2$. However, the diagonal hopping $t^{\prime}$ extracted on LSCO using single-band models is low ($t^{\prime}/t\sim-0.16$) and decreasing with doping. We therefore invoked a two-orbital ($d_{x^2-y^2}$ and $d_{z^2}$) model which implies that $t^{\prime}$ is enhanced. This effect acts to enhance the zone-boundary dispersion within the Hubbard model. We thus conclude that hybridization of $d_{x^2-y^2}$ and $d_{z^2}$ states has a significant impact on the zone-boundary dispersion in LSCO.

cond-mat.supr-con

Magnetic excitations of the charge stripe electrons below half doping in La(2-x)Sr(x)NiO4, x = 0.45 and x = 0.4

The low energy magnetic excitation spectrum of charge stripe ordered La(2-x)Sr(x)NiO4, x = 0.4 and x = 0.45 samples were studied by neutron scattering. Two excitation modes are observed in both materials, one from the ordered magnetic moments, and a second mode consistent with pseudo-one-dimensional antiferromagnetic excitations of the charge stripe electrons (q-1D). The dispersion of the q-1D excitation follows the same relation as in x = 1/3 composition, with even spectral weight in the two counter-propagating branches of the x = 0.4 sample, however in the $x = 0.45$ sample only one dispersion branch has any measurable spectral weight. The evolution of the q-1D excitations on doping to the checkerboard charge ordered phase is discussed.

cond-mat.str-el

Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$(M = Ir, Rh): A family of 5\textit{\textcolor{black}{d}}/4\textit{\textcolor{black}{d}}-based, diluted quantum spin liquids

We report the structural and magnetic properties of the 4}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Rh) based and 5}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Ir) based systems Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$ (nominally $x$ = 0.5, 1). The studied compositions were found to crystallize in a hexagonal structure with the centrosymmetric space group }$P6_{3}/mmc$.\textcolor{black}{{} The structures comprise of A$_{2}$O$_{9}$ polyhedra (with the A site (possibly) statistically occupied by M and Ti) in which pairs of transition metal ions are stacked along the crystallographic }\textit{\textcolor{black}{c}}\textcolor{black}{-axis. These pairs form triangular bilayers in the $ab$-plane. The magnetic Rh and Ir ions occupy these bilayers, diluted by Ti ions even for $x$ = 1. These bilayers are separated by a triangular layer which is dominantly occupied by Ti ions. From magnetization measurements we infer strong antiferromagnetic couplings for all of the materials but the absence of any spin-freezing or spin-ordering down to 2~K. Further, specific heat measurements down to 0.35~K show no sign of a phase transition for any of the compounds. Based on these thermodynamic measurements we propose the emergence of a quantum spin liquid ground state for Ba$_{3}$Rh$_{0.5}$Ti$_{2.5}$O$_{9}$, and Ba$_{3}$Ir$_{0.5}$Ti$_{2.5}$O$_{9}$, in addition to the already reported Ba$_{3}$IrTi$_{2}$O$_{9}$. }

cond-mat.str-el

Direct evidence for charge stripes in a layered cobalt oxide

Recent experiments indicate that static stripe-like charge order is generic to the hole-doped copper oxide superconductors and competes with superconductivity. Here we show that a similar type of charge order is present in La$_{5/3}$Sr$_{1/3}$CoO$_4$, an insulating analogue of the copper oxide superconductors containing cobalt in place of copper. The stripe phase we have detected is accompanied by short-range, quasi-one-dimensional, antiferromagnetic order, and provides a natural explanation for the distinctive hourglass shape of the magnetic spectrum previously observed in neutron scattering measurements of La$_{5/3}$Sr$_{1/3}$CoO$_4$ and many hole-doped copper oxide superconductors. The results establish a solid empirical basis for theories of the hourglass spectrum built on short-range, quasi-static, stripe correlations.

cond-mat.str-el

Sc_{2}Ga_{2}CuO_{7}: A possible Quantum spin liquid near the percolation threshold

Sc$_{2}$Ga$_{2}$CuO$_{7}$ (SGCO) crystallizes in a hexagonal structure (space group: $P$$6$$_{3}/mmc$),\textcolor{black}{{} which can be seen as an alternating stacking of single and double triangular layers. Combining neutron, x-ray, and resonant x-ray diffraction we establish that the single triangular layers are mainly populated by non-magnetic Ga$^{3+}$ ions (85\% Ga and 15\% Cu), while the bi-layers have comparable population of Cu$^{2+}$ and Ga$^{3+}$} ions \textcolor{black}{(43\% Cu and 57\% Ga)}. Our susceptibility measurements in the temperature range 1.8 - 400 K give no indication of any spin-freezing or magnetic long-range order (LRO). We infer an effective paramagnetic moment $μ_{eff}=1.79\pm0.09$ $μ_{B}$ and a Curie-Weiss temperature $θ_{CW}$ of about $-44$ K, suggesting antiferromagnetic interactions between the Cu$^{2+}$($S=1/2$) ions. Low-temperature neutron powder diffraction data showed no evidence for LRO down to 1.5 K. In our specific heat data as well, no anomalies were found down to 0.35 K, in the field range 0-140 kOe.\textcolor{black}{{} The magnetic specific heat, $C_{m}$, exhibits a broad maximum at around 2.5 K followed by a nearly power law $C$$_{m}$$\propto$ $T$$^α$ behavior at lower temperatures, with $α$ increasing from }0.3\textcolor{black}{{} to} 1.9\textcolor{black}{{} as a function of field for fields upto 90 kOe and then remaining at 1.9 for fields upto 140 kOe. Our results point to a disordered ground state in SGCO. }

cond-mat.str-el

Magnetic phase diagram of La$_{2-x}$Sr$_{x}$CoO$_{4}$ revised using muon-spin relaxation

We report the results of a muon-spin relaxation ($μ$SR) investigation of La$_{2-x}$Sr$_{x}$CoO$_{4}$, an antiferromagnetic insulating series which has been shown to support charge ordered and magnetic stripe phases and an hourglass magnetic excitation spectrum. We present a revised magnetic phase diagram, which shows that the suppression of the magnetic ordering temperature is highly sensitive to small concentrations of holes. Distinct behavior within an intermediate $x$ range ($0.2 \leq x \lesssim 0.6$) suggests that the putative stripe ordered phase extends to lower $x$ than previously thought. Further charge doping ($0.67 \leq x \leq 0.9$) prevents magnetic ordering for $T \gtrsim 1.5~{\rm K}$

cond-mat.str-el

Jahn-Teller versus quantum effects in the spin-orbital material LuVO3

We report on combined neutron and resonant x-ray scattering results, identifying the nature of the spin-orbital ground state and magnetic excitations in LuVO3 as driven by the orbital parameter. In particular, we distinguish between models based on orbital Peierls dimerization, taken as a signature of quantum effects in orbitals, and Jahn-Teller distortions, in favor of the latter. In order to solve this long-standing puzzle, polarized neutron beams were employed as a prerequisite in order to solve details of the magnetic structure, which allowed quantitative intensity-analysis of extended magnetic excitation data sets. The results of this detailed study enabled us to draw definite conclusions about classical vs quantum behavior of orbitals in this system and to discard the previous claims about quantum effects dominating the orbital physics of LuVO3 and similar systems.

cond-mat.str-el

CAMEA ESS - The Continuous Angle Multi-Energy Analysis Indirect Geometry Spectrometer for the European Spallation Source

The CAMEA ESS neutron spectrometer is designed to achieve a high detection efficiency in the horizontal scattering plane, and to maximize the use of the long pulse European Spallation Source. It is an indirect geometry time-of-flight spectrometer that uses crystal analysers to determine the final energy of neutrons scattered from the sample. Unlike other indirect gemeotry spectrometers CAMEA will use ten concentric arcs of analysers to analyse scattered neutrons at ten different final energies, which can be increased to 30 final energies by use of prismatic analysis. In this report we will outline the CAMEA instrument concept, the large performance gain, and the potential scientific advancements that can be made with this instrument.

physics.ins-det

Stripe disorder and dynamics in the hole-doped antiferromagnetic insulator La5/3Sr1/3CoO4

We report on an investigation into the dynamics of the stripe phase of La5/3Sr1/3CoO4, a material recently shown to have an hour-glass magnetic excitation spectrum. A combination of magnetic susceptibility, muon-spin relaxation and nuclear magnetic resonance measurements strongly suggest that the physics is determined by a disordered configuration of charge and spin stripes whose frustrated magnetic degrees of freedom are strongly dynamic at high temperature and which freeze out in a glassy manner as the temperature is lowered. Our results broadly confirm a recent theoretical prediction, but show that the charge quenching remains incomplete well below the charge ordering temperature and reveal, in detail, the manner in which the magnetic degrees of freedom are frozen.

cond-mat.str-el

Development of the Magnetic Excitations of Charge-Stripe Ordered La(2-x)Sr(x)NiO(4) on Doping Towards Checkerboard Charge Order

The magnetic excitation spectrums of charge stripe ordered La(2-x)Sr(x)NiO(4) x = 0.45 and x = 0.4 were studied by inelastic neutron scattering. We found the magnetic excitation spectrum of x = 0.45 from the ordered Ni^2+ S = 1 spins to match that of checkerboard charge ordered La(1.5)Sr(0.5)NiO(4). The distinctive asymmetry in the magnetic excitations above 40 meV was observed for both doping levels, but an additional ferromagnetic mode was observed in x = 0.45 and not in the x = 0.4. We discuss the origin of crossover in the excitation spectrum between x = 0.45 and x = 0.4 with respect to discommensurations in the charge stripe structure.

cond-mat.str-el

Zn-induced spin dynamics in overdoped La$_{2-x}$Sr$_x$Cu$_{1-y}$Zn$_y$O$_4$

Spin fluctuations and the local spin susceptibility in isovalently Zn-substituted La$_{2-x}$Sr$_{x}$Cu$_{1-y}$Zn$_y$O$_4$ ($x=0.25$, $y\approx0.01$) are measured via inelastic neutron scattering techniques. As Zn$^{2+}$ is substituted onto the Cu$^{2+}$-sites, an anomalous enhancement of the local spin susceptibility $χ^{\prime\prime}(ω)$ appears due to the emergence of a commensurate antiferromagnetic excitation centered at wave vector \textbf{Q}$=(π, π, 0)$ that coexists with the known incommensurate SDW excitations at \textbf{Q}$_{HK}=(π\pmδ,π), (π,π\pmδ)$. Our results support a picture of Zn-induced antiferromagnetic (AF) fluctuations appearing through a local staggered polarization of Cu$^{2+}$-spins, and the simultaneous suppression of T$_c$ as AF fluctuations are slowed in proximity to Zn-impurities suggests the continued importance of high energy AF fluctuations at the far overdoped edge of superconductivity in the cuprates.

cond-mat.supr-con

Evidence of Magnetic Correlations Among the Charge Stripe Electrons of Charge-Stripe Ordered La2NiO4.11

The magnetic excitations of charge-stripe ordered La2NiO4.11 where investigated using polarized- and unpolarized-neutron scattering to determine the magnetic excitations of the charge stripe electrons. We observed a magnetic excitation mode consistent with the gapped quasi-one-dimensional antiferromagnetic correlations of the charge stripe electrons previously observed in La(2-x)Sr(x)NiO(4) x = 1/3 and x = 0.275.

cond-mat.str-el

Spin anisotropy of the resonance in superconducting FeSe0.5Te0.5

We have used polarized-neutron inelastic scattering to resolve the spin fluctuations in superconducting FeSe0.5Te0.5 into components parallel and perpendicular to the layers. A spin resonance at an energy of 6.5 meV is observed to develop below T_c in both fluctuation components. The resonance peak is anisotropic, with the in-plane component slightly larger than the out-of-plane component. Away from the resonance peak the magnetic fluctuations are isotropic in the energy range studied. The results are consistent with a dominant singlet pairing state with s^{\pm} symmetry, with a possible minority component of different symmetry.

cond-mat.supr-con

Hour-glass magnetic spectrum in an insulating, hole-doped antiferromagnet

Superconductivity in layered copper-oxide compounds emerges when charge carriers are added to antiferromagnetically-ordered CuO2 layers. The carriers destroy the antiferromagnetic order, but strong spin fluctuations persist throughout the superconducting phase and are intimately linked to super-conductivity. Neutron scattering measurements of spin fluctuations in hole-doped copper oxides have revealed an unusual `hour-glass' feature in the momentum-resolved magnetic spectrum, present in a wide range of superconducting and non-superconducting materials. There is no widely-accepted explanation for this feature. One possibility is that it derives from a pattern of alternating spin and charge stripes, an idea supported by measurements on stripe-ordered La1.875Ba0.125CuO4. However, many copper oxides without stripe order also exhibit an hour-glass spectrum$. Here we report the observation of an hour-glass magnetic spectrum in a hole-doped antiferromagnet from outside the family of superconducting copper oxides. Our system has stripe correlations and is an insulator, which means its magnetic dynamics can conclusively be ascribed to stripes. The results provide compelling evidence that the hour-glass spectrum in the copper-oxide superconductors arises from fluctuating stripes.

cond-mat.str-el

Low energy, quasi-one-dimensional, spin dynamics in charge-ordered La(2-x)Sr(x)NiO(4)

The low energy spin excitations of La(2-x)Sr(x)NiO(4), x = 0.275 and 1/3, have been investigated by unpolarized- and polarized-inelastic neutron scattering from single crystals. A pattern of magnetic diffuse scattering is observed in both compositions, and is consistent with quasi-one-dimensional AFM spin correlations along the charge stripes. Analysis of the energy lineshape for x = 1/3 indicates that the diffuse scattering is inelastic with a characteristic energy of 1.40 +/- 0.07 meV. There is no discernible difference between the diffuse scattering from x = 0.275 and x = 1/3, suggesting that it is an intrinsic property of the charge stripes.

cond-mat.str-el

Anisotropic Neutron Spin Resonance in Superconducting BaFe$_{1.9}$Ni$_{0.1}$As$_2$

We use polarized inelastic neutron scattering to show that the neutron spin resonance below $T_c$ in superconducting BaFe$_{1.9}$Ni$_{0.1}$As$_2$ ($T_c=20$ K) is purely magnetic in origin. Our analysis further reveals that the resonance peak near 7~meV only occurs for the planar response. This challenges the common perception that the spin resonance in the pnictides is an isotropic triplet excited state of the singlet Cooper pairs, as our results imply that only the $S_{001}=\pm1$ components of the triplet are involved.

cond-mat.supr-con