arXiv subjects

Anna E. Böhmer

Publications and source records attributed to Anna E. Böhmer.

At least 19 recordsLinked to original sources

arXiv2026

Synthetic control over marcasite-pyrite polymorph formation in the Fe1-xCoxSe2 series

Transition-metal dichalcogenides of the pyrite-marcasite family are model systems of crystal chemistry. A few of these show polymorphism. The theoretical ground state of CoSe2 is marcasite, but the material is typically synthesized in the pyrite structure. Polymorphism has been observed in nanoparticles and synthetic control of the polymorphs of CoSe2 has not been achieved. We have synthesized material libraries of the Fe1-xCoxSe2 series by combining combinatorial deposition and ex-situ selenization. The approach allows to efficiently explore substitution ranges and crystal structures that form for different synthesis conditions. We find that higher levels of Co content x within the marcasite structure are possible when synthesizing at low temperatures. At a synthesis temperature of only 250° C, we have successfully synthesized marcasite CoSe2 as the majority phase. Density functional theory simulations reveal that the two isomorphs of CoSe2 are extremely close in energy and that the orthorhombic phase is the energetic ground state. Our experimental and theoretical data show that the marcasite structure is the equilibrium phase of Fe1-xCoxSe2 in the entire composition range.

cond-mat.mtrl-sci↗

arXiv2021

Edwards-Anderson parameter and local Ising-nematicity in FeSe revealed via NMR spectral broadening

The NMR spectrum of FeSe shows a dramatic broadening on cooling towards the bulk nematic phase at $T_s=90$ K, due to the formation of a quasi-static, short-range-ordered nematic domain structure. However, a quantitative understanding of the NMR broadening and its relationship to the nematic susceptibility is still lacking. Here, we show that the temperature and pressure dependence of the broadening is in quantitative agreement with the mean-field Edwards-Anderson parameter of an Ising-nematic model in the presence of random-field disorder introduced by non-magnetic impurities. Furthermore, these results reconcile the interpretation of NMR and Raman spectroscopy data in FeSe under pressure.

cond-mat.str-el↗

arXiv2021

Multi-Atom Quasiparticle Scattering Interference for Superconductor Energy-Gap Symmetry Determination

Complete theoretical understanding of the most complex superconductors requires a detailed knowledge of the symmetry of the superconducting energy-gap $Δ_\mathbf{k}^α$, for all momenta $\mathbf{k}$ on the Fermi surface of every band $α$. While there are a variety of techniques for determining $|Δ_\mathbf{k}^α|$, no general method existed to measure the signed values of $Δ_\mathbf{k}^α$. Recently, however, a new technique based on phase-resolved visualization of superconducting quasiparticle interference (QPI) patterns centered on a single non-magnetic impurity atom, was introduced. In principle, energy-resolved and phase-resolved Fourier analysis of these images identifies wavevectors connecting all k-space regions where $Δ_\mathbf{k}^α$ has the same or opposite sign. But use of a single isolated impurity atom, from whose precise location the spatial phase of the scattering interference pattern must be measured is technically difficult. Here we introduce a generalization of this approach for use with multiple impurity atoms, and demonstrate its validity by comparing the $Δ_\mathbf{k}^α$ it generates to the $Δ_\mathbf{k}^α$ determined from single-atom scattering in FeSe where $s_{\pm}$ energy-gap symmetry is established. Finally, to exemplify utility, we use the multi-atom technique on LiFeAs and find scattering interference between the hole-like and electron-like pockets as predicted for $Δ_\mathbf{k}^α$ of opposite sign.

cond-mat.supr-con↗

arXiv2020

Evolution of nematic fluctuations in CaK(Fe$_{1-x}$Ni$_{x}$)$_{4}$As$_{4}$ with spin-vortex crystal magnetic order

The CaK(Fe$_{1-x}$Ni$_{x}$)$_{4}$As$_{4}$ superconductors resemble the archetypal 122-type iron-based materials but have a crystal structure with distinctly lower symmetry. This family hosts one of the few examples of the so-called spin-vortex crystal magnetic order, a non-collinear magnetic configuration that preserves tetragonal symmetry, in contrast to the orthorhombic collinear stripe-type magnetic configuration common to the 122-type systems. Thus, nematic order is completely absent from its phase diagram. To investigate the evolution of nematic fluctuations in such a case, we present elastoresistance and elastic modulus measurements in CaK(Fe$_{1-x}$Ni$_{x}$)$_{4}$As$_{4}$ ($x = 0-0.05$) combined with phenomenological modeling and density functional theory. We find clear experimental signatures of considerable nematic fluctuations, including softening of the Young's modulus $Y_{[110]}$ and a Curie-Weiss type divergence of the B2g elastoresistance coefficient in CaK(Fe$_{0.951}$Ni$_{0.049}$)$_4$As$_4$. Overall, nematic fluctuations within this series bear strong similarities to the hole-doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ series, including a substitution-induced sign change. Our theoretical analysis addresses the effect of the specific crystal symmetry of the 1144-type structure in determining its magnetic ground state and on the nematic fluctuations.

cond-mat.supr-con↗

arXiv2019

Bulk superconductivity and role of fluctuations in the iron-based superconductor FeSe at high pressures

The iron-based superconductor FeSe offers a unique possibility to study the interplay of superconductivity with purely nematic as well magnetic-nematic order by pressure (p) tuning. By measuring specific heat under p up to 2.36GPa, we study the multiple phases in FeSe using a thermodynamic probe. We conclude that superconductivity is bulk across the entire p range and competes with magnetism. Our analysis suggests that superconducting and magnetic fluctuations exist over a wide temperature range above the respective bulk transition temperatures, whenever magnetism is present. These observations highlight similarities between FeSe and underdoped cuprate superconductors where fluctuations play a crucial role.

cond-mat.supr-con↗

arXiv2018

Imaging Orbital-selective Quasiparticles in the Hund's Metal State of FeSe

Strong electronic correlations, emerging from the parent Mott insulator phase, are key to copper-based high temperature superconductivity (HTS). By contrast, the parent phase of iron-based HTS is never a correlated insulator. But this distinction may be deceptive because Fe has five active d-orbitals while Cu has only one. In theory, such orbital multiplicity can generate a Hund's Metal state, in which alignment of the Fe spins suppresses inter-orbital fluctuations producing orbitally selective strong correlations. The spectral weights $Z_m$ of quasiparticles associated with different Fe orbitals m should then be radically different. Here we use quasiparticle scattering interference resolved by orbital content to explore these predictions in FeSe. Signatures of strong, orbitally selective differences of quasiparticle $Z_m$ appear on all detectable bands over a wide energy range. Further, the quasiparticle interference amplitudes reveal that $Z_{xy}<Z_{xz}<<Z_{yz}$, consistent with earlier orbital-selective Cooper pairing studies. Thus, orbital-selective strong correlations dominate the parent state of iron-based HTS in FeSe.

cond-mat.str-el↗

arXiv2018

Subdominant $d$-wave interaction in superconducting CaKFe$_4$As$_2$?

We report inelastic light scattering results on the stoichiometric and fully ordered superconductor CaKFe$_4$As$_2$ as a function of temperature and light polarization. In the energy range between 10 and 315 cm$^{-1}$ (1.24 and 39.1 meV) we observe the particle-hole continuum above and below the superconducting transition temperature $T_c$ and 7 of the 8 Raman active phonons. The main focus is placed on the analysis of the electronic excitations. Below $T_c$ all three symmetries projected with in-plane polarizations display a redistribution of spectral weight characteristic for superconductivity. The energies of the pair-breaking peaks in $A_{1g}$ and $B_{2g}$ symmetry are in approximate agreement with the results from photoemission studies. In $B_{1g}$ symmetry the difference between normal and superconducting state is most pronounced, and the feature is shifted downwards with respect to those in $A_{1g}$ and $B_{2g}$ symmetry. The maximum peaking at 134 cm$^{-1}$ (16.6 meV) has a substructure on the high-energy side. We interpret the peak at 134 cm$^{-1}$ in terms of a collective Bardasis-Schrieffer (BS) mode and the substructure as a remainder of the pair-breaking feature on the electron bands. There is a very weak peak at 50 cm$^{-1}$ (6.2 meV) which is tentatively assigned to another BS mode.

cond-mat.supr-con↗

arXiv2018

Distinct pressure evolution of coupled nematic and magnetic order in FeSe

FeSe, despite being the structurally simplest compound in the family of iron-based superconductors, shows an astoundingly rich interplay of physical phenomena including nematicity and pressure-induced magnetism. Here, we present a microscopic study of these two phenomena by high-energy x-ray diffraction and time-domain Mössbauer spectroscopy on FeSe single crystals over a wide temperature and pressure range. The topology of the pressure-temperature phase diagram is a surprisingly close parallel to the well-known doping-temperature phase diagram of BaFe2As2 generated through partial Fe/Co and Ba/Na substitution. In FeSe with pressure p as a control parameter, the magneto-structural ground state can be tuned from "pure" nematic - paramagnetic with an orthorhombic lattice distortion - through a strongly coupled magnetically ordered and orthorhombic state to a magnetically ordered state without an orthorhombic lattice distortion. The magnetic hyperfine field increases monotonically over a wide pressure range. However, the orthorhombic distortion initially decreases under increasing pressure, but is stabilized by cooperative coupling to the pressure-induced magnetic order. Close to the reported maximum of the superconducting critical temperature Tc (occuring at p = 6.8 GPa), the orthorhombic distortion suddenly disappears and FeSe remains tetragonal down to the lowest temperature measured. Analysis of the structural and magnetic order parameters suggests an independent origin of the structural and magnetic ordering phenomena, and their cooperative coupling leads to the similarity with the canonical phase diagram of iron pnictides.

cond-mat.supr-con↗

arXiv2017

Pseudogap Behavior of the Nuclear Spin-lattice Relaxation Rate in FeSe Probed by $^{77}$Se-NMR

We conducted $^{77}$Se-nuclear magnetic resonance studies of the iron-based superconductor FeSe in magnetic fields of 0.6 to 19 T to investigate the superconducting and normal-state properties. The nuclear spin-lattice relaxation rate divided by the temperature $(T_1T)^{-1}$ increases below the structural transition temperature $T_\mathrm{s}$ but starts to be suppressed below $T^*$, well above the superconducting transition temperature $T_\mathrm{c}(H)$, resulting in a broad maximum of $(T_1T)^{-1}$ at $T_\mathrm{p}(H)$. This is similar to the pseudogap behavior in optimally doped cuprate superconductors. Because $T^*$ and $T_\mathrm{p}(H)$ decrease in the same manner as $T_\mathrm{c}(H)$ with increasing $H$, the pseudogap behavior in FeSe is ascribed to superconducting fluctuations, which presumably originate from the theoretically predicted preformed pair above $T_\mathrm{c}(H)$.

cond-mat.supr-con↗

arXiv2017

Nematicity, magnetism and superconductivity in FeSe

Iron-based superconductors are well known for their complex interplay between structure, magnetism and superconductivity. FeSe offers a particularly fascinating example. This material has been intensely discussed because of its extended nematic phase, whose relationship with magnetism is not obvious. Superconductivity in FeSe is highly tunable, with the superconducting transition temperature, $T_\mathrm{c}$, ranging from 8 K in bulk single crystals at ambient pressure to almost 40 K under pressure or in intercalated systems, and to even higher temperatures in thin films. In this topical review, we present an overview of nematicity, magnetism and superconductivity, and discuss the interplay of these phases in FeSe. We focus on bulk FeSe and the effects of physical pressure and chemical substitutions as tuning parameters. The experimental results are discussed in the context of the well-studied iron-pnictide superconductors and interpretations from theoretical approaches are presented.

cond-mat.supr-con↗

arXiv2017

Direct visualization of phase separation between superconducting and nematic domains in Co-doped CaFe2As2 close to a first order phase transition

We show that biaxial strain induces alternating tetragonal superconducting and orthorhombic nematic domains in Co substituted CaFe2As2. We use Atomic Force, Magnetic Force and Scanning Tunneling Microscopy (AFM, MFM and STM) to identify the domains and characterize their properties, finding in particular that tetragonal superconducting domains are very elongated, more than several tens of micron long and about 30 nm wide, have the same Tc than unstrained samples and hold vortices in a magnetic field. Thus, biaxial strain produces a phase separated state, where each phase is equivalent to what is found at either side of the first order phase transition between antiferromagnetic orthorhombic and superconducting tetragonal phases found in unstrained samples when changing Co concentration. Having such alternating superconducting domains separated by normal conducting domains with sizes of order of the coherence length opens opportunities to build Josephson junction networks or vortex pinning arrays and suggests that first order quantum phase transitions lead to nanometric size phase separation under the influence of strain.

cond-mat.supr-con↗

arXiv2017

Dynamic Elastoresistivity Evidence for Slow Nematic Fluctuations in BaFe$_2$As$_2$

An instrumentation problem with the signal acquisition at high frequencies was discovered and we no longer believe that the experimental data presented in the manuscript, showing a frequency enhancement of the elastoresistivity, are correct. After correcting the problem, the elastoresistivity data is frequency independent in the range investigated. Therefore, the authors have withdrawn this submission. We would like to thank Alex Hristov, Johanna Palmstrom, Josh Straquadine and Ian Fisher (Stanford) for the kind discussions and assistance we received which helped us identify these problems.

cond-mat.str-el↗

arXiv2017

Growth and characterization of BaZnGa

We report the growth, structure and characterization of BaZnGa, identifying it as the sole known ternary compound in the Ba-Zn-Ga system. Single crystals of BaZnGa can be grown out of excess Ba-Zn and adopt a tI36 structure type. There are three unique Ba sites and three M\,=\,Zn/Ga sites. Using DFT calculations we can argue that whereas one of these three M sites is probably solely occupied by Ga, the other two M sites, most likely, have mixed Zn/Ga occupancy. Temperature dependent resistivity and magnetization measurements suggest that BaZnGa is a poor metal with no electronic or magnetic phase transitions between 2\,K and 300\,K.

cond-mat.mtrl-sci↗

arXiv2017

Discovery of Orbital-Selective Cooper Pairing in FeSe

The superconductor FeSe is of intense interest thanks to its unusual non-magnetic nematic state and potential for high temperature superconductivity. But its Cooper pairing mechanism has not been determined. Here we use Bogoliubov quasiparticle interference imaging to determine the Fermi surface geometry of the bands surrounding the $Γ= (0,0)$ and $X=(π/ a_{Fe}, 0)$ points of FeSe, and to measure the corresponding superconducting energy gaps. We show that both gaps are extremely anisotropic but nodeless, and exhibit gap maxima oriented orthogonally in momentum space. Moreover, by implementing a novel technique we demonstrate that these gaps have opposite sign with respect to each other. This complex gap configuration reveals the existence of orbital-selective Cooper pairing which, in FeSe, is based preferentially on electrons from the $d_{yz}$ orbitals of the iron atoms.

cond-mat.supr-con↗

arXiv2017

Dome of magnetic order inside the nematic phase of sulfur-substituted FeSe under pressure

The pressure dependence of the structural, magnetic and superconducting transitions and of the superconducting upper critical field were studied in sulfur-substituted Fe(Se$_{1-x}$S$_{x}$). Resistance measurements were performed on single crystals with three substitution levels ($x$=0.043, 0.096, 0.12) under hydrostatic pressures up to 1.8 GPa and in magnetic fields up to 9 T, and compared to data on pure FeSe. Our results illustrate the effects of chemical and physical pressure on Fe(Se$_{1-x}$S$_{x}$). On increasing sulfur content, magnetic order in the low-pressure range is strongly suppressed to a small dome-like region in the phase diagrams. However, $T_s$ is much less suppressed by sulfur substitution and $T_c$ of Fe(Se$_{1-x}$S$_{x}$) exhibits similar non-monotonic pressure dependence with a local maximum and a local minimum present in the low pressure range for all $x$. The local maximum in $T_c$ coincides with the emergence of the magnetic order above $T_c$. At this pressure the slope of the upper critical field decreases abruptly. The minimum of $T_c$ correlates with a broad maximum of the upper critical field slope normalized by $T_c$.

cond-mat.supr-con↗

arXiv2016

Fermi surface reconstruction in FeSe under high pressure

We report Shubnikov-de Haas (SdH) oscillation measurements on FeSe under high pressure up to $P$ = 16.1 kbar. We find a sudden change in SdH oscillations at the onset of the pressure-induced antiferromagnetism at $P$ $\sim$ 8 kbar. We argue that this change can be attributed to a reconstruction of the Fermi surface by the antiferromagnetic order. The negative d$T_c$/d$P$ observed in a range between $P$ $\sim$ 8 and 12 kbar may be explained by the reduction in the density of states due to the reconstruction. The ratio of the transition temperature to the effective Fermi energy remains high under high pressure: $k_BT_c/E_F$ $\sim$ 0.1 even at $P$ = 16.1 kbar.

cond-mat.supr-con↗

arXiv2016

Non-monotonic pressure evolution of the upper critical field in superconducting FeSe

The pressure dependence of the upper critical field, $H_\textrm{c2,c}$, of single crystalline FeSe was studied using measurements of the inter-plane resistivity, $ρ_{\textrm{c}}$ in magnetic fields parallel to tetragonal $c$-axis. $H_\textrm{c2,c}(T)$ curves obtained under hydrostatic pressures up to $1.56$ GPa, the range over which the superconducting transition temperature, $T_\textrm{c}$, of FeSe exhibits a non-monotonic dependence with local maximum at $p_1\approx$ 0.8 GPa and local minimum at $p_2\approx$ 1.2 GPa. The slope of the upper critical field at $T_\textrm{c}$, $\left(\textrm{d}H_\text{c2,c}/\textrm{d}T\right)_{T_\textrm{c}}$, also exhibits a non-monotonic pressure dependence with distinct changes at $p_1$ and $p_2$. For $p p_2$ the slope is in good quantitative agreement with a single band, orbital Helfand-Werthamer theory with Fermi velocities determined from Shubnikov-de Haas measurements. This finding indicates that Fermi surface changes are responsible for the local minimum of $T_\textrm{c}(p)$ at $p_2\approx$ 1.2 GPa.

cond-mat.supr-con↗

arXiv2016

Magnetization and transport properties of single crystalline RPd${_2}$P${_2}$ (R=Y, La-Nd, Sm-Ho, Yb)

Single crystals of RPd${_2}$P${_2}$ (R=Y, La-Nd, Sm-Ho, Yb) were grown out of a high temperature solution rich in Pd and P and characterized by room-temperature powder X-ray diffraction, anisotropic temperature- and field-dependent magnetization and temperature-dependent in-plane resistivity measurements. In this series, YPd${_2}$P${_2}$ and LaPd${_2}$P${_2}$ and YbPd${_2}$P${_2}$ (with Yb$^{+2}$) are non local-moment bearing, whereas CePd${_2}$P${_2}$ and PrPd${_2}$P${_2}$ order at low temperature with a ferromagnetic component along the crystallographic c-axis. The rest of the series manifest low temperature antiferromagnetic ordering. EuPd${_2}$P${_2}$ has Eu$^{+2}$ ions and both EuPd${_2}$P${_2}$ and GdPd${_2}$P${_2}$ have isotropic paramagnetic susceptibilities consistent with $L = 0$ and $J=S=\frac{7}{2}$ and exhibit multiple magnetic transitions. For R=Eu-Dy, there are multiple, $T>1.8$ K transitions in zero applied magnetic field and for R=Nd, Eu, Gd, Tb, and Dy there are clear metamagnetic transitions at T=2.0 K for $H<55$ kOe. Strong anisotropies arising mostly from crystal electric field (CEF) effects were observed for most magnetic rare earths with $L\neq 0$. The experimentally estimated CEF parameters B$^2_0$ were calculated from the anisotropic paramagnetic $θ_{ab}$ and $ θ_{c}$ values and compared to theoretical trends across the rare earth series. The ordering temperatures as well as the polycrystalline averaged paramagnetic Curie-Weiss temperature, $θ_{ave}$, were extracted from magnetization and resistivity measurements, and compared to the de-Gennes factor.

cond-mat.str-el↗