arXiv subjects

F. J. Litterst

Publications and source records attributed to F. J. Litterst.

At least 19 recordsLinked to original sources

arXiv2026

Competing Ordering Modes in the Distorted Quantum Kagome Material Clinoatacamite Cu$_2$Cl(OH)$_3$

We have studied the magnetic properties of clinoatacamite Cu$_2$Cl(OH)$_3$, the parent compound of the quantum spin liquid candidate herbertsmithite and a longstanding puzzle among frustrated quantum magnets. As we reveal using density-functional theory, clinoatacamite belongs to the class of distorted kagome antiferromagnets with the kagome plane being embedded into a low-symmetry crystal structure. By means of thermodynamic measurements, muon spin rotation/relaxation as well as neutron diffraction on single crystals, we find in zero magnetic field complex behavior below $T_\mathrm{I}$ = 18.1 K which unfolds in three temperature regions I-III. We propose this complexity in multicritical clinoatacamite to arise from the competition of antiferromagnetic ordering modes from the underconstrained manifold of modes, which can lead to a metamagnetic texture in zero field.

cond-mat.str-el↗

arXiv2023

Near coincidence of metal-insulator transition and quantum critical fluctuations: Electronic ground state and magnetic order in Fe$_{1-x}$Co$_{x}$Si

We present a detailed study of the electronic and magnetic ground state properties of Fe$_{1-x}$Co$_{x}$Si using a combination of macroscopic and microscopic experimental techniques. From these experiments we quantitatively characterize the metal-insulator transition and magnetic/non-magnetic quantum phase transition occurring at low doping levels in Fe$_{1-x}$Co$_{x}$Si. From our study, we find a surprising closeness of the critical composition of the metal-insulator transition at $x_{\mathrm{MIT}} = 0.014$ and the quantum phase transition at $x_{\mathrm{LRO}} \sim 0.024-0.031$. It suggests that these effects are cooperative and depend on each other.

cond-mat.str-el↗

arXiv2022

Muon spin rotation and relaxation study on Nb$_{1-y}$Fe$_{2+y}$

We present a detailed study of the magnetic properties of weakly ferromagnetic/quantum critical Nb$_{1-y}$Fe$_{2+y}$ using muon spin rotation and relaxation ($μ$SR). By means of an angular dependent study of the muon spin rotation signal in applied magnetic fields on a single crystal in the paramagnetic state we establish the muon stopping site in the crystallographic lattice of NbFe$_2$. With this knowledge we develop models to describe the muon spin rotation and relaxation signals in the weakly ferromagnetic, spin density wave and quantum critical phases of Nb$_{1-y}$Fe$_{2+y}$ and fit the corresponding experimental data. In particular, we quantify the $μ$SR response for quantum critical behavior in Nb$_{1.0117}$Fe$_{1.9883}$ and extract the influence of residual weak structural disorder. From our analysis, Nb$_{1-y}$Fe$_{2+y}$ emerges to be uniquely suited to study quantum criticality close to weak itinerant ferromagnetic order.

cond-mat.str-el↗

arXiv2020

The effect of structural and magnetic disorder on the 3$d$-5$d$ exchange interactions of La$_{2-x}$Ca$_{x}$CoIrO$_{6}$

The delicate balance between spin-orbit coupling, Coulomb repulsion and crystalline electric field interactions observed in Ir-based oxides is usually manifested as exotic magnetic behavior. Here we investigate the evolution of the exchange coupling between Co and Ir for partial La substitution by Ca in La$_{2}$CoIrO$_6$. A great advantage of the use of Ca$^{2+}$ as replacement for La$^{3+}$ is the similarity of its ionic radii. Thus, the observed magnetic changes can more easily be associated to electronic variations. A thorough investigation of the structural, electronic and magnetic properties of the La$_{2-x}$Ca$_{x}$CoIrO$_6$ system was carried out by means of synchrotron x-ray powder diffraction, muon spin rotation and relaxation ($μ$SR), AC and DC magnetization, XAS, XMCD, Raman spectroscopy, electrical resistivity and dielectric permittivity. Our XAS results show that up to 25% of Ca substitution at the La site results in the emergence of Co$^{3+}$, possibly in high spin state, while the introduction of larger amount of Ca leads to the increase of Ir valence. The competing magnetic interactions resulting from the mixed valences lead to a coexistence of a magnetically ordered and an emerging spin glass (SG) state for the doped samples. Our $μ$SR results indicate that for La$_{2}$CoIrO$_6$ a nearly constant fraction of a paramagnetic (PM) phase persists down to low temperature, possibly related to the presence of a small amount of Ir$^{3+}$ and to the anti-site disorder at Co/Ir sites. For the doped compounds the PM phase freezes below 30 K, but there is still some dynamics associated with the SG. The dielectric data obtained for the parent compound and the one with 25% of Ca-doping indicate a possible magnetodielectric effect, which is discussed in terms of the electron hopping between the TM ions, the anti-site disorder and the distorted crystalline structure.

cond-mat.mtrl-sci↗

arXiv2019

The zero-field-cooled exchange bias effect in phase-segregated La$_{2-x}$A$_{x}$CoMnO$_{6-δ}$ (A = Ba, Ca, Sr; x = 0, 0.5)

In the zero-field-cooled exchange bias (ZEB) effect the unidirectional magnetic anisotropy is set at low temperatures even when the system is cooled in the absence of external magnetic field. La$_{1.5}$Sr$_{0.5}$CoMnO$_{6}$ stands out as presenting the largest ZEB reported so far, while for La$_{1.5}$Ca$_{0.5}$CoMnO$_{6}$ the exchange bias field ($H_{EB}$) is one order of magnitude smaller. Here we show that La$_{1.5}$Ba$_{0.5}$CoMnO$_{6}$ also exhibits a pronounced shift of its magnetic hysteresis loop, with intermediate $H_{EB}$ value in respect to Ca- and Sr-doped samples. In order to figure out the microscopic mechanisms responsible for this phenomena, these compounds were investigated by means of synchrotron X-ray powder diffraction, Raman spectroscopy, muon spin rotation and relaxation, AC and DC magnetization, X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). The parent compound La$_{2}$CoMnO$_{6}$ was also studied for comparison, as a reference of a non-ZEB material. Our results show that the Ba-, Ca- and Sr-doped samples present a small amount of phase segregation, and that the ZEB effect is strongly correlated to the system's structure. We also observed that mixed valence states Co$^{2+}$/Co$^{3+}$ and Mn$^{4+}$/Mn$^{3+}$ are already present at the La$_{2}$CoMnO$_{6}$ parent compound, and that Ba$^{2+}$/Ca$^{2+}$/Sr$^{2+}$ partial substitution at La$^{3+}$ site leads to a large increase of Co average valence, with a subtle augmentation of Mn formal valence. Estimates of the Co and Mn valences from the $L$-edge XAS indicate the presence of oxygen vacancies in all samples (0.05$\leq δ\leq$0.1). Our XMCD results show a great decrease of Co moment for the doped compounds, and indicate that the shift of the hysteresis curves for these samples is related to uncompensated antiferromagnetic coupling between Co and Mn.

cond-mat.mtrl-sci↗

arXiv2018

Tuning the $S = 1/2$ square-lattice antiferromagnet Sr$_2$Cu(Te$_{1-x}$W$_x$)O$_6$ from Néel order to quantum disorder to columnar order

The spin-1/2 square-lattice Heisenberg model is predicted to have a quantum disordered ground state when magnetic frustration is maximized by competing nearest-neighbor $J_1$ and next-nearest-neighbor $J_2$ interactions ($J_2/J_1 \approx 0.5$). The double perovskites Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are isostructural spin-1/2 square-lattice antiferromagnets with Néel ($J_1$ dominates) and columnar ($J_2$ dominates) magnetic order, respectively. Here we characterize the full isostructural solid solution series Sr$_2$Cu(Te$_{1-x}$W$_x$)O$_6$ ($0 \leq x \leq 1$) tunable from Néel order to quantum disorder to columnar order. A spin-liquid-like ground state was previously observed for the $x$ = 0.5 phase, but we show that the magnetic order is suppressed below 1.5 K in a much wider region of $x \approx$ 0.1-0.6. This coincides with significant $T$-linear terms in the low-temperature specific heat. However, density functional theory calculations predict most of the materials are not in the highly frustrated $J_2/J_1 \approx 0.5$ region square-lattice Heisenberg model. Thus, a combination of both magnetic frustration and quenched disorder is the likely origin of the spin-liquid-like state in $x$ = 0.5.

cond-mat.str-el↗

arXiv2018

Spin-liquid-like state in a spin-1/2 square-lattice antiferromagnet perovskite induced by $d^{10}$-$d^0$ cation mixing

A quantum spin liquid state has long been predicted to arise in spin-1/2 Heisenberg square-lattice antiferromagnets at the boundary region between Néel (nearest-neighbor interaction dominates) and columnar (next-nearest-neighbor dominates) antiferromagnetic order. However, there are no known compounds in this region. Here we use $d^{10}$-$d^0$ cation mixing to tune the magnetic interactions on the square lattice while simultaneously introducing disorder. We find spin-liquid-like behavior in the double perovskite Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$, where the isostructural end phases Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are Néel and columnar type antiferromagnets, respectively. We show that magnetism in Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$ is entirely dynamic down to 19 mK. Additionally, we observe at low temperatures for Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$, similar to several spin liquid candidates, a plateau in muon spin relaxation rate and a strong $T$-linear dependence in specific heat. Our observations for Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$ highlight the role of disorder in addition to magnetic frustration in spin liquid physics.

cond-mat.str-el↗

arXiv2017

Magnetic order of intermetallic FeGa$_{3-y}$Ge$_y$ studied by $μ$SR and $^{57}$Fe Mössbauer spectroscopy

Temperature dependent magnetization, muon spin rotation and $^{57}$Fe Mössbauer spectroscopy experiments performed on crystals of intermetallic FeGa$_{3-y}$Ge$_{y}$ ($y=0.11,0.14,0.17,0.22,0.27$, $0.29,0.32$) are reported. Whereas at $y=0.11$ even a sensitive magnetic microprobe such as $μ$SR does not detect magnetism, all other samples display weak ferromagnetism with a magnetic moment of up to 0.22 $μ_B$ per Fe atom. As a function of doping and of temperature a crossover from short range to long range magnetic order is observed, characterized by a broadly distributed spontaneous internal field. However, the $y=0.14$ and $y=0.17$ remain in the short range ordered state down to the lowest investigated temperature. The transition from short range to long range order appears to be accompanied by a change of the character of the spin fluctuations, which exhibit spin wave excitations signature in the LRO part of the phase diagram. Mössbauer spectroscopy for $y=0.27$ and 0.32 indicates that the internal field lies in the plane perpendicular to the crystallographic $c$ axis. The field distribution and its evolution with doping suggest that the details of the Fe magnetic moment formation and the consequent magnetic state are determined not only by the dopant concentration but also by the way the replacement of the Ga atoms surrounding the Fe is accomplished.

cond-mat.str-el↗

arXiv2015

The magnetic ground state properties of non-centrosymmetric CePt$_3$B$_{1-x}$Si$_x$

We present a study of the alloying series of the non-centrosymmetric $f$-electron intermetallic CePt$_3$B$_{1-x}$Si$_x$ by means of muon spin rotation and relaxation measurements. In addition, we include a high pressure magnetization investigation of the stoichiometric parent compound CePt$_3$B. From our data we establish the nature of the magnetic ground state properties of the series, derive the ordered magnetic moment as function of stoichiometry and gain insight into the evolution of the symmetry of the ordered magnetic state with $x$. We thus can verify the notion that the behavior of the sample series can essentially be understood within the framework of the Doniach phase diagram. Further, our findings raise the issue of the role the Dzyaloshinskii-Moriya magnetic interaction plays in correlated electron materials, and its effect on magnetic fluctuations in such materials.

cond-mat.str-el↗

arXiv2014

Magnetic short and long range order in PbFe$_{1/2}$Ta$_{1/2}$O$_{3}$

PbFe$_{1/2}$Ta$_{1/2}$O$_{3}$ (PFT) belongs to the family of PbB$'_{x}$B$"_{1-x}$O$_{3}$ which have inherent chemical disorder at the B-site. Due to this disorder, a complex magnetic phase diagram is expected in the material. In this paper, we report experimental results of magnetic properties in PFT through macroscopic characterization, neutron scattering and Mössbauer spectroscopy techniques. With these results we show for the first time that PbFe$_{1/2}$Ta$_{1/2}$O$_{3}$ behaves very similar to PbFe$_{1/2}$Nb$_{1/2}$O$_{3}$, i.e, it undergoes AF transition at 153 K and has a spinglass transition at 10 K, below which the antiferromagnetism coexists with spinglass. We suggest that the mechanism which is responsible for such a non-trivial ground state can be explained by a speromagnet-like spin arrangement similar to the one proposed for PbFe$_{1/2}$Nb$_{1/2}$O$_{3}$.

cond-mat.str-el↗

arXiv2013

Microscopic Coexistence of Antiferromagnetic and Spin-Glass States

The disordered antiferromagnet \pfn (\pfns) is investigated in a wide temperature range by combining Mössbauer spectroscopy and neutron diffraction experiments. It is demonstrated that the magnetic ground state is a {\it microscopic} coexistence of antiferromagnetic and a spin-glass orders. This speromagnet-like phase features frozen-in short-range fluctuations of the Fe$^{3+}$ magnetic moments that are transverse to the long-range ordered antiferromagnetic spin component.

cond-mat.str-el↗

arXiv2010

Magnetoelastic and structural properties of azurite Cu3(CO3)2(OH)2 from neutron scattering and muon spin rotation

Azurite, Cu3(CO3)2(OH)2, has been considered an ideal example of a one-dimensional (1D) diamond chain antiferromagnet. Early studies of this material imply the presence of an ordered antiferromagnetic phase below $T_N \sim 1.9$ K while magnetization measurements have revealed a 1/3 magnetization plateau. Until now, no corroborating neutron scattering results have been published to confirm the ordered magnetic moment structure. We present recent neutron diffraction results which reveal the presence of commensurate magnetic order in azurite which coexists with significant magnetoelastic strain. The latter of these effects may indicate the presence of spin frustration in zero applied magnetic field. Muon spin rotation, $μ$SR, reveals an onset of short-range order below 3K and confirms long-range order below $T_N$.

cond-mat.stat-mech↗

arXiv2010

Low frequency spin dynamics in the quantum magnet copper pyrazine dinitrate

The S=1/2 antiferromagnetic Heisenberg chain exhibits a magnetic field driven quantum critical point. We study the low frequency spin dynamics in copper pyrazine dinitrate (CuPzN), a realization of this model system of quantum magnetism, by means of $^{13}$C-NMR spectroscopy. Measurements of the nuclear spin-lattice relaxation rate $T_1^{-1}$ in the vicinity of the saturation field are compared with quantum Monte Carlo calculations of the dynamic structure factor. Both show a strong divergence of low energy excitations at temperatures in the quantum regime. The analysis of the anisotropic $T_1^{-1}$-rates and frequency shifts allows one to disentangle the contributions from transverse and longitudinal spin fluctuations for a selective study and to determine the transfer of delocalized spin moments from copper to the neighboring nitrogen atoms.

cond-mat.str-el↗

arXiv2009

Field-induced coupled superconductivity and spin density wave order in the Heavy Fermion compound CeCoIn5

The high field superconducting state in CeCoIn5 has been studied by transverse field muon spin rotation measurements with an applied field parallel to the crystallographic c-axis close to the upper critical field Hc2 = 4.97 T. At magnetic fields >= 4.8 T the muon Knight shift is enhanced and the superconducting transition changes from second order towards first order as predicted for Pauli-limited superconductors. The field and temperature dependence of the transverse muon spin relaxation rate sigma reveal paramagnetic spin fluctuations in the field regime from 2 T < H < 4.8 T. In the normal state close to Hc2 correlated spin fluctuations as described by the self consistent renormalization theory are observed. The results support the formation of a mode-coupled superconducting and antiferromagnetically ordered phase in CeCoIn5 for H directed parallel to the c-axis.

cond-mat.str-el↗

arXiv2009

Quantum critical dynamics of a S = 1/2 antiferromagnetic Heisenberg chain studied by 13C-NMR spectroscopy

We present a 13C-NMR study of the magnetic field driven transition to complete polarization of the S=1/2 antiferromagnetic Heisenberg chain system copper pyrazine dinitrate Cu(C_4H_4N_2)(NO_3)_2 (CuPzN). The static local magnetization as well as the low-frequency spin dynamics, probed via the nuclear spin-lattice relaxation rate 1/T_1, were explored from the low to the high field limit and at temperatures from the quantum regime (k_B T << J) up to the classical regime (k_B T >> J). The experimental data show very good agreement with quantum Monte Carlo calculations over the complete range of parameters investigated. Close to the critical field, as derived from static experiments, a pronounced maximum in 1/T_1 is found which we interpret as the finite-temperature manifestation of a diverging density of zero-energy magnetic excitations at the field-driven quantum critical point.

cond-mat.str-el↗

arXiv2009

Electronic properties of LaOFFeAs in the normal state probed by NMR/NQR

We report 139La, 57Fe and 75As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements on powders of the new LaO1-xFxFeAs superconductor for x = 0 and x = 0.1 at temperatures up to 480 K, and compare our measured NQR spectra with local density approximation (LDA) calculations. For all three nuclei in the x = 0.1 material, it is found that the local Knight shift increases monotonically with an increase in temperature, and scales with the macroscopic susceptibility, suggesting a single magnetic degree of freedom. Surprisingly, the spin lattice relaxation rates for all nuclei also scale with one another, despite the fact that the form factors for each site sample different regions of q-space. This result suggests a lack of any q-space structure in the dynamical spin susceptibility that might be expected in the presence of antiferromagnetic correlations. Rather, our results are more compatible with simple quasi-particle scattering. Furthermore, we find that the increase in the electric field gradient at the As cannot be accounted for by LDA calculations, suggesting that structural changes, in particular the position of the As in the unit cell, dominate the NQR response.

cond-mat.supr-con↗

arXiv2009

The electronic phase diagram of the LaO1-xFxFeAs superconductor

The competition of magnetic order and superconductivity is a key element in the physics of all unconventional superconductors, e.g. in high-transition-temperature cuprates 1, heavy fermions 2 and organic superconductors3. Here superconductivity is often found close to a quantum critical point where long-range antiferromagnetic order is gradually suppressed as a function of a control parameter, e.g. charge carrier doping or pressure. It is believed that dynamic spin fluctuations associated with this quantum critical behaviour are crucial for the mechanism of superconductivity. Recently high-temperature superconductivity has been discovered in iron-pnictides providing a new class of unconventional superconductors4,5,6. Similar to other unconventional superconductors the parent compounds of the pnictides exhibit a magnetic ground state7,8 and superconductivity is induced upon charge carrier doping. In this Letter the structural and electronic phase diagram is investigated by means of x-ray scattering, MuSR and Moessbauer spectroscopy on the series LaO1-xFxFeAs. We find a discontinuous first-order-like change of the Neel temperature, the superconducting transition temperature and of the respective order parameters. Our results strongly question the relevance of quantum critical behaviour in ironpnictides and prove a strong coupling of the structural orthorhombic distortion and the magnetic order both disappearing at the phase boundary to the superconducting state.

cond-mat.supr-con↗

arXiv2008

Commensurate Spin Density Wave in LaOFeAs: A Local Probe Study

We present a detailed study on the magnetic order in the undoped mother compound LaOFeAs of the recently discovered Fe-based superconductor LaO$_{1-x}$F$_x$FeAs. In particular, we present local probe measurements of the magnetic properties of LaOFeAs by means of $^{57}$Fe Mössbauer spectroscopy and muon spin relaxation in zero external field along with magnetization and resistivity studies. These experiments prove a commensurate static magnetic order with a strongly reduced ordered moment of 0.25(5) $μ_B$ at the iron site below T_N = 138 K, well separated from a structural phase transition at T_N = 156 K. The temperature dependence of the sublattice magnetization is determined and compared to theory. Using a four-band spin density wave model both, the size of the order parameter and the quick saturation below T_N are reproduced.

cond-mat.supr-con↗