arXiv subjects

A. Revcolevschi

Publications and source records attributed to A. Revcolevschi.

At least 19 recordsLinked to original sources

arXiv2021

Unraveling higher-order corrections in the spin dynamics of RIXS spectra

Resonant inelastic x-ray scattering (RIXS) is an evolving tool for investigating spin dynamics of strongly correlated materials, which complements inelastic neutron scattering. Both techniques have found that non-spin-conserving (NSC) excitations in quasi-1D isotropic quantum antiferromagnets are confined to the two-spinon phase space. Outside this phase space, only spin-conserving (SC) four-spinon excitations have been detected using O $K$-edge RIXS. Here, we investigate SrCuO$_2$ and find four-spinon excitations outside the two-spinon phase space at both O $K$- and Cu $L_3$-edges. Using the Kramers-Heisenberg formalism, we demonstrate that the four-spinon excitations arise from both SC and NSC processes at Cu $L_3$-edge. We show that these new excitations only appear in the second-order terms of the ultra-fast core-hole lifetime expansion and arise from long-range spin fluctuations. These results thus open a new window to the spin dynamics of quantum magnets.

cond-mat.str-el↗

arXiv2021

Probing the interplay between lattice dynamics and short-range magnetic correlations in CuGeO3 with femtosecond RIXS

Investigations of magnetically ordered phases on the femtosecond timescale have provided significant insights into the influence of charge and lattice degrees of freedom on the magnetic sub-system. However, short-range magnetic correlations occurring in the absence of long-range order, for example in spin-frustrated systems, are inaccessible to many ultrafast techniques. Here, we show how time-resolved resonant inelastic X-ray scattering (trRIXS) is capable of probing such short-ranged magnetic dynamics in a charge-transfer insulator through the detection of a Zhang-Rice singlet exciton. Utilizing trRIXS measurements at the O K-edge, and in combination with model calculations, we probe the short-range spin-correlations in the frustrated spin chain material CuGeO3 following photo-excitation, revealing a strong coupling between the local lattice and spin sub-systems.

cond-mat.str-el↗

arXiv2018

Direct observation of multi-spinon excitations outside of the two-spinon continuum in the antiferromagnetic spin chain cuprate Sr2CuO3

One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying emergent phenomena such as quasiparticle fractionalization and quantum criticality. The antiferromagnetic Heisenberg chain of spins-1/2 is an important reference system; its elementary excitations are spin-1/2 quasiparticles called spinons that are always created in pairs. However, while inelastic neutron scattering (INS) experiments routinely observe the excitation continuum associated with two-spinon states, the presence of more complex dynamics associated with four-spinon states has only been inferred from comparison with theory. Here, we show that resonant inelastic x-ray scattering (RIXS) is capable of accessing the four-spinon excitations directly, in a spectroscopic region separated from the two-spinon continuum. Our results provide the first direct measurement of four-spinon excitations, which is made possible by the fundamentally different correlation functions probed by RIXS compared to INS. This advance holds great promise as a tool in the search for novel quantum states, in particular quantum spin liquids.

cond-mat.str-el↗

arXiv2017

Spin pseudogap in the $S=\frac{1}{2}$ chain material Sr$_2$CuO$_3$ with impurities

The low energy magnetic excitation spectrum of the Heisenberg antiferromagnetic $S = 1/2$ chain system Sr$_2$CuO$_3$ with Ni- and Ca-impurities is studied by neutron spectroscopy. In all cases, a defect-induced spectral pseudogap is observed and shown to scale proportionately to the number of scattering centers in the spin chains.

cond-mat.str-el↗

arXiv2016

Magnetic ordering in the ultra-pure site-diluted spin chain materials SrCu$_{1-x}$Ni$_x$O$_2$

Muon spin rotation technique is used to study magnetic ordering in ultra-pure samples of SrCu$_{1-x}$Ni$_x$O$_2$, an archetypical $S=1/2$ antiferromagnetic Heisenberg chain system with a small amount of $S=1$ defects. The ordered state in the parent compound is shown to be highly homogeneous, contrary to previous report [M. Matsuda et al., Phys. Rev. B \textbf{55}, R11953 (1997)]. Even minute amount of Ni impurities result in inhomogeneous order and a decrease of the transition temperature. At as little as $0.5$~\% Ni concentration, magnetic ordering is entirely suppressed. The results are compared to previous theoretical studies of weakly coupled spin chains with site-defects.

cond-mat.str-el↗

arXiv2016

Nematicity in stripe ordered cuprates probed via resonant x-ray scattering

In underdoped cuprate superconductors, a rich competition occurs between superconductivity and charge density wave (CDW) order. Whether rotational symmetry breaking (nematicity) occurs intrinsically and generically or as a consequence of other orders is under debate. Here we employ resonant x-ray scattering in stripe-ordered (La,M)_2CuO_4 to probe the relationship between electronic nematicity of the Cu 3d orbitals, structure of the (La,M)_2O_2 layers, and CDW order. We find distinct temperature dependences for the structure of the (La,M)_2O_2 layers and the electronic nematicity of the CuO_2 planes, with only the latter being enhanced by the onset of CDW order. These results identify electronic nematicity as an order parameter that is distinct from a purely structural order parameter in underdoped striped cuprates.

cond-mat.supr-con↗

arXiv2014

Inhomogeneous ordering in weakly coupled Heisenberg $S=1/2$ chains with random bonds

Long range magnetic ordering in the quasi-one-dimensional random-bond antiferromagnet BaCu$_2$(Si$_{1-x}$Ge$_{x}$)$_2$O$_7$ is studied in $μ$SR experiments as a function of disorder strength. Compared to the disorder-free parent materials, the saturation ordered moment is found to be considerably reduced. Moreover, even in weakly disordered species, the magnetically ordered state is shown to be highly inhomogeneous. The results are interpreted in terms of weakly coupled random spin chains, governed by the ``infinite randomness`` fixed point.

cond-mat.str-el↗

arXiv2014

Amorphous ferromagnetism and re-entrant magnetic glassiness in Sm$_{2}$Mo$_{2}$O$_{7}$: new insights into the electronic phase diagram of pyrochlore molybdates

We discuss the magnetic properties of a Sm$_{2}$Mo$_{2}$O$_{7}$ single crystal as investigated by means of different experimental techniques. In the literature, a conventional itinerant ferromagnetic state is reported for the Mo$^{4+}$ sublattice below $\sim 78$ K. However, our results of dc magnetometry, muon spin spectroscopy ($μ^{+}$SR) and high-harmonics magnetic ac susceptibility unambiguously evidence highly disordered conditions in this phase, in spite of the crystalline and chemical order. This disordered magnetic state shares several common features with amorphous ferromagnetic alloys. This scenario for Sm$_{2}$Mo$_{2}$O$_{7}$ is supported by the anomalously high values of the critical exponents, as mainly deduced by a scaling analysis of our dc magnetization data and confirmed by the other techniques. Moreover, $μ^{+}$SR detects a significant static magnetic disorder at the microscopic scale. At the same time, the critical divergence of the third-harmonic component of the ac magnetic susceptibility around $\sim 78$ K leads to additional evidence towards the glassy nature of this magnetic phase. Finally, the longitudinal relaxation of $μ^{+}$ spin polarization (also supported by results of ac susceptibility) evidences re-entrant glassy features similar to amorphous ferromagnets.

cond-mat.str-el↗

arXiv2014

Macroscopic Quantum Coherence of the Spin Triplet in the Spin-Ladder Compound Sr14Cu24O41

We report the direct observation by inelastic neutron scattering experiments of a spin triplet of magnetic excitations in the response associated with the ladders in the composite cuprate Sr14Cu24O41. This appears as a peak at q_{Q1D}=πand energy Δ_1=32.5 meV, and we conjecture that all the triplets making up this conspicuous peak have the same phase and therefore interpret it as the signature of the occurrence of quantum coherence along the ladder direction between entangled spin pairs. From the comparison with previous neutron and x-ray data, we conclude that the temperature evolution of this mode is driven by the crystallization of holes into a charge density wave in the ladder sublattice

cond-mat.str-el↗

arXiv2014

Magnetisation of hole-doped CuO2 spin chains in Sr14-xCaxCu24O41

We report on magnetisation measurements of Sr14-xCaxCu24O41, with 0 <= x <= 12, in magnetic fields up to 16 T. The low temperature magnetic response of the CuO2 spin chains changes strongly upon doping. For x = 0, the ground state with nearly independent dimers is confirmed. Reduction of the number of holes in the chains through Ca-doping leads to an additional contribution to the magnetisation, which depends linearly on the magnetic field. Remarkably, the slope of this linear contribution increases with the Ca content. We argue that antiferromagnetic spin chains do not account for this behaviour but that the hole dynamics might be involved.

cond-mat.str-el↗

arXiv2014

Spin Gap in the Single Spin-1/2 Chain Cuprate Sr$_{1.9}$Ca$_{0.1}$CuO$_3$

We report $^{63}$Cu nuclear magnetic resonance and muon spin rotation measurements on the S=1/2 antiferromagnetic Heisenberg spin chain compound Sr$_{1.9}$Ca$_{0.1}$CuO$_3$. An exponentially decreasing spin-lattice relaxation rate 1/T$_1$ indicates the opening of a spin gap. This behavior is very similar to what has been observed for the cognate zigzag spin chain compound Sr$_{0.9}$Ca$_{0.1}$CuO$_2$, and confirms that the occurrence of a spin gap upon Ca doping is independent of the interchain exchange coupling $J'$. Our results therefore generally prove the appearance of a spin gap in an antiferromagnetic Heisenberg spin chain induced by a local bond disorder of the intrachain exchange coupling $J$. A low temperature upturn of 1/T$_1$ evidences growing magnetic correlations. However, zero field muon spin rotation measurements down to 1.5 K confirm the absence of magnetic order in this compound which is most likely suppressed by the opening of the spin gap.

cond-mat.str-el↗

arXiv2014

Bond disorder and spinon heat transport in the $S=\tfrac{1}{2}$ Heisenberg spin chain compound Sr$_2$CuO$_3$: from clean to dirty limits

We investigate the effect of disorder on the heat transport properties of the $S=\tfrac{1}{2}$ Heisenberg chain compound Sr$_2$CuO$_3$ upon chemically substituting Sr by increasing concentrations of Ca. As Ca occupies sites outside but near the Cu-O-Cu spin chains, bond disorder, i.e. a spatial variation of the exchange interaction $J$, is expected to be realized in these chains. We observe that the magnetic heat conductivity ($κ_{\mathrm{mag}}$) due to spinons propagating in the chains is gradually but strongly suppressed with increasing amount of Ca, where the doping dependence can be understood in terms of increased scattering of spinons due to Ca-induced disorder. This is also reflected in the spinon mean free path which can be separated in a doping independent but temperature dependent scattering length due to spinon-phonon scattering, and a temperature independent but doping dependent spinon-defect scattering length. The latter spans from very large ($>$ 1300 lattice spacings) to very short ($\sim$ 12 lattice spacings) and scales with the average distance between two neighboring Ca atoms. Thus, the Ca-induced disorder acts as an effective defect within the spin chain, and the doping scheme allows to cover the whole doping regime between the clean and the dirty limits. Interestingly, at maximum impurity level we observe, in Ca-doped Sr$_2$CuO$_3$, an almost linear increase of $κ_{\mathrm{mag}}$ at temperatures above 100 K which reflects the intrinsic low temperature behavior of heat transport in a Heisenberg spin chain. These findings are quite different from that observed for the Ca-doped double spin chain compound, SrCuO$_2$, where the effect of Ca seems to saturate already at intermediate doping levels.

cond-mat.str-el↗

arXiv2013

Structural transitions in a doped lanthanum cuprate

139La NMR and relaxation measurements have been performed on La{1.8-x}Eu{0.2}Sr{x}CuO{4} (x = 0.13 and 0.2) single crystals. The temperature dependence of the 139La NMR spectra in all the structural phases (HTT -> LTO -> LTT) reveals the non-vanishing tilt angle of the CuO6 octahedra in the HTT phase, opposed to the case of La{2-x}Sr{x}CuO{4} where the tilt angle disappears immediately above the transition. Since 139La relaxation data provide evidence of the thermodynamic critical fluctuations associated with the structural phase transitions, HTT -> LTO and LTO -> LTT, we conclude that the structural transitions in Eu-doped La{2-x}Sr{x}CuO{4} should be of the order-disorder type rather than of the displacive type observed in La{2-x}Sr{x}CuO{4}. The change of the nature of the structural transitions caused by doping Eu appears to be consistent with the LTO -> LTT transition that is absent in La{2-x}Sr{x}CuO{4}.

cond-mat.str-el↗

arXiv2012

Low temperature ballistic spin transport in the S=1/2 antiferromagnetic Heisenberg chain compound SrCuO2

We report zero and longitudinal magnetic field muon spin relaxation measurements of the spin S=1/2 antiferromagnetic Heisenberg chain material SrCuO2. We find that in a weak applied magnetic field B the spin-lattice relaxation rate follows a power law B^n with n=-0.9(3). This result is temperature independent for 5K < T < 300 K. Within conformal field theory and using the Müller ansatz we conclude ballistic spin transport in SrCuO2.

cond-mat.str-el↗

arXiv2012

Dimensional crossover of spin chains in a transverse staggered field: an NMR study

Heisenberg spin-1/2 chain materials are known to substantially alter their static and dynamic properties when experiencing an effective transverse staggered field originating from the varying local environment of the individual spins. We present a temperature-, angular- and field-dependent 29Si NMR study of the model compound BaCu2Si2O7. The experimental data are interpreted in terms of the divergent low-temperature transverse susceptibility, predicted by theory for spin chains in coexisting longitudinal and transverse staggered fields. Our analysis first employs a finite-temperature "Density Matrix Renormalization Group" (DMRG) study of the relevant one-dimensional Hamiltonian. Next we compare our numerical with the presently known analytical results. With an analysis based on crystal symmetries we show how the anisotropic contribution to the sample magnetization is experimentally accessible even below the ordering temperature, in spite of its competition with the collinear order parameter of the antiferromagnetic phase. The modification of static and dynamic properties of the system due to the presence of a local transverse staggered field (LTSF) acting on the one-dimensional spin array are argued to cause the unusual spin reorientation transitions observed in BaCu2Si2O7. On the basis of a Ginzburg-Landau type analysis, we discuss aspects of competing spin structures in the presence of magnetic order and the enhanced transverse susceptibility.

cond-mat.str-el↗

arXiv2012

Spin-Orbital Separation in the quasi 1D Mott-insulator Sr2CuO3

As an elementary particle the electron carries spin \hbar/2 and charge e. When binding to the atomic nucleus it also acquires an angular momentum quantum number corresponding to the quantized atomic orbital it occupies (e.g., s, p or d). Even if electrons in solids form bands and delocalize from the nuclei, in Mott insulators they retain their three fundamental quantum numbers: spin, charge and orbital[1]. The hallmark of one-dimensional (1D) physics is a breaking up of the elementary electron into its separate degrees of freedom[2]. The separation of the electron into independent quasi-particles that carry either spin (spinons) or charge (holons) was first observed fifteen years ago[3]. Using Resonant Inelastic X-ray Scattering on the 1D Mott-insulator Sr2CuO3 we now observe also the orbital degree of freedom separating. We resolve an orbiton liberating itself from spinons and propagating through the lattice as a distinct quasi-particle with a substantial dispersion of ~0.2 eV.

cond-mat.str-el↗

arXiv2012

Electronic confinement and ordering instabilities in colossal magnetoresistive bilayer manganites

We present angle-resolved photoemission studies of (La1-zPrz)2-2xSr1+2xMn2O7 with x=0.4 and z=0.1,0.2 and 0.4 along with density functional theory calculations and x-ray scattering data. Our results show that the bilayer splitting in the ferromagnetic metallic phase of these materials is small, if not completely absent. The charge carriers are therefore confined to a single MnO2-layer, which in turn results in a strongly nested Fermi surface. In addition to this, the spectral function also displays clear signatures of an electronic ordering instability well below the Fermi level. The increase of the corresponding interaction strength with z and its magnitude of ~400 meV make the coupling to a bare phonon highly unlikely. Instead we conclude that fluctuating order, involving electronic and lattice degrees of freedom, cause the observed renormalisation of the spectral features.

cond-mat.str-el↗

arXiv2012

Spinon heat transport and spin-phonon interaction in the antiferromagnetic spin-1/2 Heisenberg chain cuprates Sr2CuO3 and SrCuO2

We have investigated the thermal conductivity κ_mag of high-purity single crystals of the spin chain compound Sr2CuO3 which is considered an excellent realization of the one-dimensional spin-1/2 antiferromagnetic Heisenberg model. We find that the spinon heat conductivity κ_mag is strongly enhanced as compared to previous results obtained on samples with lower chemical purity. The analysis of κ_mag allows to compute the spinon mean free path l_mag as a function of temperature. At low-temperature we find l_mag\sim0.5\mum, corresponding to more than 1200 chain unit cells. Upon increasing the temperature, the mean free path decreases strongly and approaches an exponential decay ~1/T*exp(T*/T) which is characteristic for umklapp processes with the energy scale k_B T*. Based on Matthiesen's rule we decompose l_mag into a temperature-independent spinon-defect scattering length l0 and a temperature dependent spinon-phonon scattering length l_sp(T). By comparing l_mag(T) of Sr2CuO3 with that of SrCuO2, we show that the spin-phonon interaction, as expressed by l_sp is practically the same in both systems. The comparison of the empirically derived l_sp with model calculations for the spin-phonon interaction of the one-dimensional spin-1/2 XY model yields reasonable agreement with the experimental data.

cond-mat.str-el↗