arXiv subjects

Benjamin A. Frandsen

Publications and source records attributed to Benjamin A. Frandsen.

53 records · Page 3Linked to original sources

arXiv2019

Robust block magnetism in the spin ladder compound BaFe$_2$Se$_3$ under hydrostatic pressure

The majority of the iron-based superconductors (FeSCs) exhibit a two-dimensional square lattice structure. Recent reports of pressure-induced superconductivity in the spin-ladder system, BaFe$_2$X$_3$ (X =S,Se), introduce a quasi-one-dimensional prototype and an insulating parent compound to the FeSCs. Here we report X-ray, neutron diffraction and muon spin relaxation experiments on BaFe$_2$Se$_3$ under hydrostatic pressure to investigate its magnetic and structural properties across the pressure-temperature phase diagram. A structural phase transition was identified at a pressure of 3.7(3) GPa. Neutron diffraction measurements at 6.8(3) GPa and 120 K show that the block magnetism persists even at these high pressures. A steady increase and then fast drop of the magnetic transition temperature $T\rm_N$ and greatly reduced moment above the pressure $P_s$ indicate potentially rich and competing phases close to the superconducting phase in this ladder system.

cond-mat.supr-con↗

arXiv2019

Hidden spin-orbital order in the Kitaev hyperhoneycomb $β$-Li$_2$IrO$_3$

We report the existence of a phase transition at high temperature in the 3D Kitaev candidate material, $β$-Li$_2$IrO$_3$. We show that the transition is bulk, intrinsic and orders a tiny magnetic moment with a spatially anisotropic saturation moment. We show that even though this transition is global, it does not freeze the local Ir moments, which order at much lower temperatures into an incommensurate state. Rather, the ordered moment has an orbital origin that is coupled to spin correlations, likely of a Kitaev origin. The separate ordering of spin-correlated orbital moments and of local Ir moments reveals a novel way in which magnetic frustration in Kitaev systems can lead to coexisting magnetic states.

cond-mat.str-el↗

arXiv2019

Quantitative characterization of short-range orthorhombic fluctuations in FeSe through pair distribution function analysis

Neutron and x-ray total scattering measurements have been performed on powder samples of the iron chalcogenide superconductor FeSe. Using pair distribution function (PDF) analysis of the total scattering data to investigate short-range atomic correlations, we establish the existence of an instantaneous, local orthorhombic structural distortion attributable to nematic fluctuations that persists well into the high-temperature tetragonal phase, at least up to 300 K and likely to significantly higher temperatures. This short-range orthorhombic distortion is correlated over a length scale of about 1 nm at 300 K and grows to several nm as the temperature is lowered toward the long-range structural transition temperature. In the low-temperature nematic state, the local instantaneous structure exhibits an enhanced orthorhombic distortion relative to the average structure with a typical relaxation length of 3 nm. The quantitative characterization of these orthorhombic fluctuations sheds light on nematicity in this canonical iron-based superconductor.

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arXiv2019

Incommensurate magnetism near quantum criticality in CeNiAsO

Two phase transitions in the tetragonal strongly correlated electron system CeNiAsO were probed by neutron scattering and zero field muon spin rotation. For $T <T_{N1}$ = 8.7(3) K, a second order phase transition yields an incommensurate spin density wave with wave vector $\textbf{k} = (0.44(4), 0, 0)$. For $T < T_{N2}$ = 7.6(3) K, we find co-planar commensurate order with a moment of $0.37(5)~μ_B$, reduced to $30 \%$ of the saturation moment of the $|\pm\frac{1}{2}\rangle$ Kramers doublet ground state, which we establish by inelastic neutron scattering. Muon spin rotation in $\rm CeNiAs_{1-x}P_xO$ shows the commensurate order only exists for x $\le$ 0.1 so the transition at $x_c$ = 0.4(1) is from an incommensurate longitudinal spin density wave to a paramagnetic Fermi liquid.

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arXiv2018

Widespread orthorhombic fluctuations in the (Sr,Na)Fe$_2$As$_2$ family of superconductors

We report comprehensive pair distribution function measurements of the hole-doped iron-based superconductor system Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$. Structural refinements performed as a function of temperature and length scale reveal orthorhombic distortions of the instantaneous local structure across a large region of the phase diagram possessing average tetragonal symmetry, indicative of fluctuating nematicity. These nematic fluctuations are present up to high doping levels ($x \gtrsim 0.48$, near optimal superconductivity) and high temperatures (above room temperature for $x = 0$, decreasing to 150 K for $x = 0.48$), with a typical length scale of 1-3 nm. This work highlights the ubiquity of nematic fluctuations in a representative iron-based superconductor and provides important details about the evolution of these fluctuations across the phase diagram.

cond-mat.supr-con↗

arXiv2018

Gradual Enhancement of Stripe-Type Antiferromagnetism in Spin Ladder Material BaFe$_2$S$_3$ Under Pressure

We report pressure-dependent neutron diffraction and muon spin relaxation/rotation measurements combined with first-principles calculations to investigate the structural, magnetic, and electronic properties of BaFe$_2$S$_3$ under pressure. The experimental results reveal a gradual enhancement of the stripe-type ordering temperature with increasing pressure up to 2.6 GPa and no observable change in the size of the ordered moment. The ab initio calculations suggest that the magnetism is highly sensitive to the Fe-S bond lengths and angles, clarifying discrepancies with previously published results. In contrast to our experimental observations, the calculations predict a monotonic reduction of the ordered moment with pressure. We suggest that the robustness of the stripe-type antiferromagnetism is due to strong electron correlations not fully considered in the calculations.

cond-mat.supr-con↗

arXiv2018

Disentangling superconducting and magnetic orders in NaFe_1-xNi_xAs using muon spin rotation

Muon spin rotation and relaxation studies have been performed on a "111" family of iron-based superconductors NaFe_1-xNi_xAs. Static magnetic order was characterized by obtaining the temperature and doping dependences of the local ordered magnetic moment size and the volume fraction of the magnetically ordered regions. For x = 0 and 0.4 %, a transition to a nearly-homogeneous long range magnetically ordered state is observed, while for higher x than 0.4 % magnetic order becomes more disordered and is completely suppressed for x = 1.5 %. The magnetic volume fraction continuously decreases with increasing x. The combination of magnetic and superconducting volumes implies that a spatially-overlapping coexistence of magnetism and superconductivity spans a large region of the T-x phase diagram for NaFe_1-xNi_xAs . A strong reduction of both the ordered moment size and the volume fraction is observed below the superconducting T_C for x = 0.6, 1.0, and 1.3 %, in contrast to other iron pnictides in which one of these two parameters exhibits a reduction below TC, but not both. The suppression of magnetic order is further enhanced with increased Ni doping, leading to a reentrant non-magnetic state below T_C for x = 1.3 %. The reentrant behavior indicates an interplay between antiferromagnetism and superconductivity involving competition for the same electrons. These observations are consistent with the sign-changing s-wave superconducting state, which is expected to appear on the verge of microscopic coexistence and phase separation with magnetism. We also present a universal linear relationship between the local ordered moment size and the antiferromagnetic ordering temperature TN across a variety of iron-based superconductors. We argue that this linear relationship is consistent with an itinerant-electron approach, in which Fermi surface nesting drives antiferromagnetic ordering.

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arXiv2017

Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$ with magnetic pair distribution function analysis

We present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$, which belong to a class of recently discovered pyrochlore compounds based on transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 Å, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space.

cond-mat.str-el↗

arXiv2017

Ba(Zn,Co)2As2: a II-II-V Diluted Ferromagnetic Semiconductor with N-type Carriers

Diluted ferromagnetic semiconductors (DMSs) that combine the properties of semiconductors with ferromagnetism have potential application in spin-sensitive electronics (spintronics) devices. The search for DMS materials exploded after the observation of ferromagnetic ordering in III-V (Ga,Mn)As films. Recently, a series of DMS compounds isostructural to iron-based superconductors have been reported. Among them, the highest Curie temperature $T_C$ of 230 K has been achieved in (Ba,K)(Zn,Mn)$_2$As$_2$. However, most DMSs, including (Ga,Mn)As, are p-type, i.e., the carriers that mediate ferromagnetism are holes. For practical applications, DMS with n-type carriers are also advantageous. Here we report the successful synthesis of a II-II-V diluted ferromagnetic semiconductor with n-type carriers, Ba(Zn,Co)$_2$As$_2$. Magnetization measurements show that the ferromagnetic transition occurs up to $T_{C} \sim$ 45 K. Hall effect and Seebeck effect measurements jointly confirm that the dominant carriers are electrons. Through muon spin relaxation ($μ$SR), a volume sensitive magnetic probe, we have also confirmed that the ferromagnetism in Ba(Zn,Co)$_2$As$_2$ is intrinsic and the internal field is static.

cond-mat.mtrl-sci↗

arXiv2017

Local orthorhombicity in the magnetic $C_4$ phase of the hole-doped iron-arsenide superconductor Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$

We report temperature-dependent pair distribution function measurements of Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$, an iron-based superconductor system that contains a magnetic phase with reentrant tetragonal symmetry, known as the magnetic $C_4$ phase. Quantitative refinements indicate that the instantaneous local structure in the $C_4$ phase is comprised of fluctuating orthorhombic regions with a length scale of $\sim$2 nm, despite the tetragonal symmetry of the average static structure. Additionally, local orthorhombic fluctuations exist on a similar length scale at temperatures well into the paramagnetic tetragonal phase. These results highlight the exceptionally large nematic susceptibility of iron-based superconductors and have significant implications for the magnetic $C_4$ phase and the neighboring $C_2$ and superconducting phases.

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arXiv2017

Emergent phases in iron pnictides: Double-Q antiferromagnetism, charge order and enhanced nematic correlations

Electron correlations produce a rich phase diagram in the iron pnictides. Earlier theoretical studies on the correlation effect demonstrated how quantum fluctuations weaken and concurrently suppress a $C_2$-symmetric single-Q antiferromagnetic order and a nematic order. Here we examine the emergent phases near the quantum phase transition. For a $C_4$-symmetric collinear double-Q antiferromagnetic order, we show that it is accompanied by both a charge order and an enhanced nematic susceptibility. Our results provide understanding for several intriguing recent experiments in hole-doped iron arsenides, and bring out common physics that underlies the different magnetic phases of various iron-based superconductors.

cond-mat.supr-con↗

arXiv2017

Uniaxial pressure effect on the magnetic ordered moment and transition temperatures in BaFe$_{2-x}T_x$As$_2$ ($T=$Co, Ni)

We use neutron diffraction and muon spin relaxation to study the effect of in-plane uniaxial pressure on the antiferromagnetic (AF) orthorhombic phase in BaFe$_2$As$_2$ and its Co- and Ni-substituted members near optimal superconductivity. In the low temperature AF ordered state, uniaxial pressure necessary to detwin the orthorhombic crystals also increases the magnetic ordered moment, reaching an 11$\%$ increase under 40 MPa for BaFe$_{1.9}$Co$_{0.1}$As$_2$, and a 15$\%$ increase for BaFe$_{1.915}$Ni$_{0.085}$As$_2$. We also observe an increase of the AF ordering temperature ($T_N$) of about 0.25 K/MPa in all compounds, consistent with density functional theory calculations that reveal better Fermi surface nesting for itinerant electrons under uniaxial pressure. The doping dependence of the magnetic ordered moment is captured by combining dynamical mean field theory with density functional theory, suggesting that the pressure-induced moment increase near optimal superconductivity is closely related to quantum fluctuations and the nearby electronic nematic phase.

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arXiv2016

Local atomic and magnetic structure of dilute magnetic semiconductor (Ba,K)(Zn,Mn)$_2$As$_2$

We have studied the atomic and magnetic structure of the dilute ferromagnetic semiconductor system (Ba,K)(Zn,Mn)$_2$As$_2$ through atomic and magnetic pair distribution function analysis of temperature-dependent x-ray and neutron total scattering data. We detected a change in curvature of the temperature-dependent unit cell volume of the average tetragonal crystallographic structure at a temperature coinciding with the onset of ferromagnetic order. We also observed the existence of a well-defined local orthorhombic structure on a short length scale of $\lesssim 5$ Å, resulting in a rather asymmetrical local environment of the Mn and As ions. Finally, the magnetic PDF revealed ferromagnetic alignment of Mn spins along the crystallographic $c$-axis, with robust nearest-neighbor ferromagnetic correlations that exist even above the ferromagnetic ordering temperature. We discuss these results in the context of other experiments and theoretical studies on this system.

cond-mat.str-el↗

arXiv2016

Verification of Anderson superexchange in MnO via magnetic pair distribution function analysis and \textit{ab initio} theory

We present temperature-dependent atomic and magnetic pair distribution function (PDF) analysis of neutron total scattering measurements of antiferromagnetic MnO, an archetypal strongly correlated transition-metal oxide. The known antiferromagnetic ground-state structure fits the low-temperature data closely with refined parameters that agree with conventional techniques, confirming the reliability of the newly developed magnetic PDF method. The measurements performed in the paramagnetic phase reveal significant short-range magnetic correlations on a $\sim$1~nm length scale that differ substantially from the low-temperature long-range spin arrangement. \textit{Ab initio} calculations using a self-interaction-corrected local spin density approximation of density functional theory predict magnetic interactions dominated by Anderson superexchange and reproduce the measured short-range magnetic correlations to a high degree of accuracy. Further calculations simulating an additional contribution from a direct exchange interaction show much worse agreement with the data. The Anderson superexchange model for MnO is thus verified by experiment and confirmed by \textit{ab initio} theory.

cond-mat.str-el↗

arXiv2016

Volume-wise destruction of the antiferromagnetic Mott insulating state through quantum tuning

Metal-to-insulator transitions (MITs) are a dramatic manifestation of strong electron correlations in solids1. The insulating phase can often be suppressed by quantum tuning, i.e. varying a nonthermal parameter such as chemical composi- tion or pressure, resulting in a zero-temperature quantum phase transition (QPT) to a metallic state driven by quantum fluctuations, in contrast to conventional phase transitions driven by thermal fluctuations. Theories of exotic phenomena known to occur near the Mott QPT such as quantum criticality and high-temperature superconductivity often assume a second-order QPT, but direct experimental evidence for either first- or second-order behavior at the magnetic QPT associated with the Mott transition has been scarce and further masked by the superconducting phase in unconventional superconductors. Most measurements of QPTs have been performed by volume-integrated probes, such as neutron scattering, magnetization, and transport, in which discontinuous behavior, phase separation, and spatially inhomogeneous responses are averaged and smeared out, leading at times to misidentification as continuous second-order transitions. Here, we demonstrate through muon spin relaxation/rotation (MuSR) experiments on two archetypal Mott insulating systems, composition-tuned RENiO3 (RE=rare earth element) and pressured-tuned V2O3, that the QPT from antiferromagnetic insulator to paramagnetic metal is first-order: the magnetically ordered volume fraction decreases to zero at the QPT, resulting in a broad region of intrinsic phase separation, while the ordered magnetic moment retains its full value across the phase diagram until it is suddenly destroyed at the QPT. These findings call for further investigation into the role of inelastic soft modes and the nature of dynamic spin and charge fluctuations underlying the transition.

cond-mat.str-el↗

arXiv2015

Magnetic structure determination from the magnetic pair distribution function (mPDF): ground state of MnO

An experimental determination of the magnetic pair distribution function (mPDF) defined in an earlier paper (Frandsen, Yang, and Billinge. (2014) Acta Crystallogr. A, 70(1), 3-11) is presented for the first time. The mPDF was determined from neutron powder diffraction data from a reactor and a neutron time-of-flight total scattering source on a powder sample of the antiferromagnetic oxide MnO. A description of the data treatment that allowed the measured mPDF to be extracted and then modelled is provided and utilized to investigate the low-temperature structure of MnO. Atomic and magnetic co-refinements support the scenario of a locally monoclinic ground-state atomic structure, despite the average structure being rhombohedral, with the magnetic PDF analysis successfully recovering the known antiferromagnetic spin configuration. The total scattering data suggest a preference for the spin axis to lie along the pseudocubic [10$\bar{1}$] direction. Finally, $r$-dependent PDF refinements indicate that the local monoclinic structure tends toward the average rhombohedral $R\overline{3}m$ symmetry over a length scale of approximately 100~Å.

cond-mat.mtrl-sci↗

arXiv2014

Intra-unit-cell nematic charge order in the titanium-oxypnictide family of superconductors

Understanding the role played by broken symmetry states such as charge, spin, and orbital orders in the mechanism of emergent properties such as high-temperature superconductivity (HTSC) is a major current topic in materials research. That the order may be within one unit cell, such as nematic, was only recently considered theoretically, but its observation in the iron-pnictide and doped cuprate superconductors places it at the forefront of current research. Here we show that the recently discovered BaTi$_2$Sb$_2$O superconductor and its "parent" compound BaTi$_2$As$_2$O form a symmetry-breaking nematic ground state that can be naturally explained as an intra-unit-cell charge order with $d$-wave symmetry, pointing to the ubiquity of the phenomenon. These findings, together with the key structural features in these materials being intermediate between the cuprate and iron-pnictide HTSC materials, render the titanium oxypnictides an important new material system to understand the nature of nematic order and its relationship to superconductivity.

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