arXiv subjects

Martin Greven

Publications and source records attributed to Martin Greven.

At least 37 records · Page 2Linked to original sources

arXiv2020

Anisotropic Time-Domain Electronic Response in Cuprates

Superconductivity in the cuprates is characterized by spatial inhomogeneity and an anisotropic electronic gap of d-wave symmetry. The aim of this work is to understand how this anisotropy affects the non-equilibrium electronic response of high-Tc superconductors. We compare the nodal and antinodal non-equilibrium response to photo-excitations with photon energy comparable to the superconducting gap and polarization along the Cu-Cu axis of the sample. The data are supported by an effective d-wave BCS model indicating that the observed enhancement of the superconducting transient signal mostly involves an increase of pair coherence in the antinodal region, which is not induced at the node.

cond-mat.supr-con↗

arXiv2020

Electronic Structure and Small Hole Polarons in YTiO3

As a prototypical Mott insulator with ferromagnetic ordering, YTiO3 (YTO) is of great interest in the study of strong electron correlation effects and orbital ordering. Here we report the first molecular beam epitaxy (MBE) growth of YTO films, combined with theoretical and experimental characterization of the electronic structure and charge transport properties. The obstacles of YTO MBE growth are discussed and potential routes to overcome them are proposed. DC transport and Seebeck measurements on thin films and bulk single crystals identify p-type Arrhenius transport behavior, with an activation energy of ~ 0.17 eV in thin films, consistent with the energy barrier for small hole polaron migration from hybrid density functional theory (DFT) calculations. Hard X-ray photoelectron spectroscopy measurements (HAXPES) show the lower Hubbard band (LHB) at 1.1 eV below the Fermi level, whereas a Mott-Hubbard band gap of ~1.5 eV is determined from photoluminescence (PL) measurements. These findings provide critical insight into the electronic band structure of YTO and related materials.

cond-mat.mtrl-sci↗

arXiv2020

Post-growth annealing effects on charge and spin excitations in Nd$_{2-x}$Ce$_x$CuO$_4$

We report a Cu K- and L$_3$-edge resonant inelastic x-ray scattering study of charge and spin excitations of bulk Nd$_{2-x}$Ce$_x$CuO$_4$, with focus on post-growth annealing effects. For the parent compound Nd$_2$CuO$_4$ ($x = 0$), a clear charge-transfer gap is observed in the as-grown state, whereas the charge excitation spectra indicate that electrons are doped in the annealed state. This is consistent with the observation that annealed thin-film and polycrystalline samples of RE$_2$CuO$_4$ (RE = rare earth) can become metallic and superconducting at sufficiently high electron concentrations without Ce doping. For $x = 0.16$, a Ce concentration for which it is known that oxygen reduction destroys long-range antiferromagnetic order and induces superconductivity, we find that the high-energy spin excitations of non-superconducting as-grown and superconducting annealed crystals are nearly identical. This finding is in stark contrast to the significant changes in the low-energy spin excitations previously observed via neutron scattering.

cond-mat.supr-con↗

arXiv2019

Soft X-ray Absorption Spectroscopy and Magnetic Circular Dichroism as Operando Probes of Complex Oxide Electrolyte Gate Transistors

Electrolyte-based transistors utilizing ionic liquids/gels have been highly successful in the study of charge-density-controlled phenomena, particularly in oxides. Experimental probes beyond transport have played a significant role, despite challenges to their application in electric double-layer transistors. Here, we demonstrate application of synchrotron soft X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) as operando probes of the charge state and magnetism in ion-gel-gated ferromagnetic perovskite films. Electrochemical response via oxygen vacancies at positive gate bias in LaAlO$_3$(001)/La$_{0.5}$Sr$_{0.5}$CoO$_{3-δ}$ is used as a test case. XAS/XMCD measurements of 4-25 unit-cell-thick films first probe the evolution of hole doping (from the O K-edge pre-peak) and ferromagnetism (at the Co L-edges), to establish a baseline. Operando soft XAS/XMCD of electrolyte-gated films is then demonstrated, using optimized spin-coated gels with thickness $\sim$1 $μ$m, and specific composition. Application of gate voltages up to +4 V is shown to dramatically suppress the O $K$-edge XAS pre-peak intensity and Co $L$-edge XMCD, thus enabling the Co valence and ferromagnetism to be tracked upon gate-induced reduction. Soft XAS and XMCD, with appropriate electrolyte design, are thus established as viable for the operando characterization of electrolyte-gated oxides.

cond-mat.mtrl-sci↗

arXiv2019

Doping-dependent phonon anomaly and charge-order phenomena in the HgBa$_{2}$CuO$_{4+δ}$ and HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$

Using resonant X-ray diffraction and Raman spectroscopy, we study charge correlations and lattice dynamics in two model cuprates, HgBa$_{2}$CuO$_{4+δ}$ and HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$. We observe a maximum of the characteristic charge order temperature around the same hole concentration ($p \approx 0.09$) in both compounds, and concomitant pronounced anomalies in the lattice dynamics that involve the motion of atoms in and/or adjacent to the CuO$_2$ layers. These anomalies are already present at room temperature, and therefore precede the formation of the static charge correlations, and we attribute them to an instability of the CuO$_2$ layers. Our finding implies that the charge order in the cuprates is an emergent phenomenon, driven by a fundamental variation in both lattice and electronic properties as a function of doping.

cond-mat.supr-con↗

arXiv2018

Universal superconducting precursor in perovskite-based oxides

A pivotal challenge posed by unconventional superconductors is to unravel how superconductivity emerges upon cooling from the generally complex normal state. Some of the most prominent unconventional superconductors are oxides: strontium titanate, strontium ruthenate, and the cuprates exhibit greatly different superconducting transition temperatures $T_c$, and although their respective superconducting pairing mechanisms remain unknown, they are thought to differ as well. Here we use nonlinear magnetic response, a probe that is uniquely sensitive to the superconducting precursor, to uncover remarkable universal behavior in these three distinct classes of superconductors. We find unusual exponential temperature dependence of the diamagnetic response above the transition temperature $T_c$, with a characteristic temperature scale that strongly varies with $T_c$. We correlate this scale with the sensitivity of $T_c$ to local stress, and show that it is influenced by intentionally-induced structural disorder. The universal behavior is therefore caused by intrinsic, self-organized structural inhomogeneity, inherent to the oxides perovskite-based structure. The prevalence of such inhomogeneity has far-reaching implications for the interpretation of electronic properties of perovskite-related oxides in general.

cond-mat.supr-con↗

arXiv2018

Signatures of enhanced superconducting phase coherence through MID-IR excitation in optimally doped Y-Bi2212

Optimally doped cuprate superconductors are characterized by the presence of superconducting fluctuations in a relatively large temperature region above the critical transition temperature. We reveal here that the effect of thermal disorder, which decreases the condensate phase coherence at equilibrium, can be dynamically contrasted by photoexcitation with ultrashort mid-infrared pulses. In particular, our findings reveal that light pulses with photon energy comparable to the amplitude of the superconducting gap and polarized in plane along the copper-copper direction [110] can dynamically enhance the optical response which is associated to the onset of superconductivity. We propose that this effect could be rationalized by an effective d-wave BCS model, which reveals that mid-infrared pulses result in a transient increase of the phase coherence.

cond-mat.str-el↗

arXiv2018

Growth and characterization of HgBa2CaCu2O6+d and HgBa2Ca2Cu3O8+d crystals

We report the successful synthesis of single-crystalline cuprate superconductors HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$ and HgBa$_{2}$Ca$_{2}$Cu$_{3}$O$_{8+δ}$. These compounds are well-known for their high optimal superconducting critical temperatures of $T_\mathrm{c}$ = 128 K and 134 K at ambient pressure, respectively, and for their challenging synthesis. Using a conventional quartz-tube encapsulation method and a two-layer encapsulation method that utilizes custom-built high-pressure furnaces, we are able to grow single crystals with linear dimensions up to several millimeters parallel to the CuO$_2$ planes. Extended post-growth anneals are shown to lead to sharp superconducting transitions, indicative of high macroscopic homogeneity. X-ray diffraction and polarized Raman spectroscopy are identified as viable methods to resolve the seemingly unavoidable inter-growth of the two compounds. Our work helps to remove obstacles toward the study of these model cuprate systems with experimental probes that require sizable high-quality crystals.

cond-mat.supr-con↗

arXiv2018

Decomposition of La2-xSrxCuO4 into Several La2O3 Phases at Elevated Temperatures in Ultra-High Vacuum inside a Transmission Electron Microscope

We report the decomposition of La2-xSrxCuO4 into La2O3 and Cu nanoparticles in ultra-high vacuum, observed by in-situ heating experiments in a transmission electron microscope (TEM). The analysis of electron diffraction data reveals that the phase decomposition process starts at about 150 °C and is considerably expedited in the temperature range of 350-450 °C. Two major resultant solid phases are identified as metallic Cu and La2O3 by electron diffraction, simulation, and electron energy-loss spectroscopy (EELS) analyses. With the aid of calculations, La2O3 phases are further identified to be derivatives of a fluorite structure - fluorite, pyrochlore, and (distorted) bixbyite - characterized by different oxygen-vacancy order. Additionally, the bulk plasmon energy and the fine structures of the O K and La M4,5 EELS edges are reported for these structures, along with simulated O K X-ray absorption near-edge structure. The resultant Cu nanoparticles and La2O3 phases remain unchanged after cooling to room temperature.

cond-mat.mtrl-sci↗

arXiv2018

Orientation of the intra-unit-cell magnetic moment in the high-Tc superconductor HgBa2CuO$_{4+δ}$

Polarized-neutron diffraction experiments (PND) have revealed that the pseudogap state of the cuprates exhibits unusual intra-unit-cell (IUC) magnetism. At a qualitative level, the data indicate a moment direction that is neither perpendicular nor parallel to the CuO2 layers, yet an accurate measurement of a structurally simple compound has been lacking. Here we report PND results with unprecedented accuracy for the IUC magnetic order in the simple-tetragonal single-CuO$_2$-layer compound HgBa2CuO$_{4+δ}$. At the transition temperature, we find evidence for magnetic critical scattering. Deep in the ordered state, we determine the moment direction to be 70° $\pm$ 10° away from the normal to the CuO$_2$ layers, which rules out both purely planar loop currents and high-symmetry Dirac multipoles, the two most prominent theoretical proposals for the microscopic origin of the IUC magnetism. However, the data are consistent with Dirac multipoles of lower symmetry or, alternatively, with a particular configuration of loop currents that flow on the faces of the CuO$_6$ octahedra.

cond-mat.supr-con↗

arXiv2017

Dynamics of correlation-frozen antinodal quasiparticles in superconducting cuprates

Many puzzling properties of high-$T_c$ superconducting (HTSC) copper oxides have deep roots in the nature of the antinodal quasiparticles, the elementary excitations with wavevector parallel to the Cu-O bonds. These electronic states are most affected by the onset of antiferromagnetic correlations and charge instabilities and they host the maximum of the anisotropic superconducting gap and pseudogap. In this work, we use time-resolved extreme-ultra-violet (EUV) photoemission with proper photon energy (18 eV) and time-resolution (50 fs) to disclose the ultrafast dynamics of the antinodal states in a prototypical HTSC cuprate. After photoinducing a non-thermal charge redistribution within the Cu and O orbitals, we reveal a dramatic momentum-space differentiation of the transient electron dynamics. While the nodal quasi-particle distribution is heated up as in a conventional metal, new quasiparticle states transiently emerge at the antinodes, similarly to what is expected for a photoexcited Mott insulator, where the frozen charges can be released by an impulsive excitation. This transient antinodal metallicity is mapped into the dynamics of the O-2$p$ bands thus directly demonstrating the intertwining between the low- and high-energy scales that is typical of correlated materials. Our results suggest that the correlation-driven freezing of the electrons moving along the Cu-O bonds, analogous to the Mott localization mechanism, constitutes the starting point for any model of high-$T_c$ superconductivity and other exotic phases of HTSC cuprates.

cond-mat.str-el↗

arXiv2017

Emergence of superconductivity in the cuprates via a universal percolation process

A pivotal step toward understanding unconventional superconductors would be to decipher how superconductivity emerges from the unusual normal state upon cooling. In the cuprates, traces of superconducting pairing appear above the macroscopic transition temperature $T_c$, yet extensive investigation has led to disparate conclusions. The main difficulty has been the separation of superconducting contributions from complex normal state behaviour. Here we avoid this problem by measuring the nonlinear conductivity, an observable that is zero in the normal state. We uncover for several representative cuprates that the nonlinear conductivity vanishes exponentially above $T_c$, both with temperature and magnetic field, and exhibits temperature-scaling characterized by a nearly universal scale $T_0$. Attempts to model the response with the frequently evoked Ginzburg-Landau theory are unsuccessful. Instead, our findings are captured by a simple percolation model that can also explain other properties of the cuprates. We thus resolve a long-standing conundrum by showing that the emergence of superconductivity in the cuprates is dominated by their inherent inhomogeneity.

cond-mat.supr-con↗

arXiv2017

Percolative nature of the dc paraconductivity in the cuprate superconductors

We present an investigation of the planar direct-current (dc) paraconductivity of the model cuprate material HgBa$_2$CuO$_{4+δ}$ in the underdoped part of the phase diagram. The simple quadratic temperature-dependence of the Fermi-liquid normal-state resistivity enables us to extract the paraconductivity above the macroscopic $T_c$ with great accuracy. The paraconductivity exhibits unusual exponential temperature dependence, with a characteristic temperature scale that is distinct from $T_c$. In the entire temperature range where it is discernable, the paraconductivity is quantitatively explained by a simple superconducting percolation model, which implies that underlying gap disorder dominates the emergence of superconductivity.

cond-mat.supr-con↗

arXiv2015

Electronic spin susceptibilities and superconductivity in HgBa$_{2}$CuO$_{4+δ}$ from nuclear magnetic resonance

Nuclear magnetic resonance (NMR) experiments on single crystals of HgBa$_{2}$CuO$_{4+δ}$ are presented that identify two distinct temperature-dependent spin susceptibilities: one is due to a spin component that is temperature-dependent above the critical temperature for superconductivity ($T_{\rm c}$) and reflects pseudogap behavior; the other is Fermi-liquid-like in that it is temperature independent above $T_{\rm c}$ and vanishes rapidly below $T_{\rm c}$. In addition, we demonstrate the existence of a third, hitherto undetected spin susceptibility: it is temperature independent at higher temperatures, vanishes at lower temperatures (below $T_0\neq T_{\rm c}$), and changes sign near optimal doping. This susceptibility either arises from the coupling between the two spin components, or it could be given by a distinct third spin component.

cond-mat.supr-con↗

arXiv2014

Photo-enhanced antinodal conductivity in the pseudogap state of high Tc cuprates

A major challenge in understanding the cuprate superconductors is to clarify the nature of the fundamental electronic correlations that lead to the pseudogap phenomenon. Here we use ultrashort light pulses to prepare a non-thermal distribution of excitations and capture novel properties that are hidden at equilibrium. Using a broadband (0.5-2 eV) probe we are able to track the dynamics of the dielectric function, unveiling an anomalous decrease of the scattering rate of the charge carriers in a pseudogap-like region of the temperature ($T$) and hole-doping ($p$) phase diagram. In this region, delimited by a well-defined $T^*_{neq}(p)$ line, the photo-excitation process triggers the evolution of antinodal excitations from gapped (localized) to delocalized quasi-particles characterized by a longer lifetime. The novel concept of photo-enhanced antinodal conductivity is naturally explained within the single-band Hubbard model, in which the short-range Coulomb repulsion leads to a k-space differentiation between "nodal" quasiparticles and antinodal excitations.

cond-mat.str-el↗

arXiv2013

The Strain Derivatives of $T_c$ in HgBa$_2$CuO$_{4+δ}$: CuO$_2$ Plane Alone is Not Enough

The strain derivatives of $T_c$ along the $a$ and $c$ axes have been determined for HgBa$_2$CuO$_{4+δ}$ (Hg1201), the simplest monolayer cuprate with the highest $T_c$ of all monolayer cuprates ($T_c$ = 97 K at optimal doping). The underdoped compound with the initial $T_c$ of 65 K has been studied as a function of pressure up to 20 GPa by magnetic susceptibility and X-ray diffraction (XRD). The observed linear increase in $T_c$ with pressure is the same as previously been found for the optimally-doped compound. The above results have enabled the investigation of the origins of the significantly different $T_c$ values of optimally doped Hg1201 and the well-studied compound La$_{2-x}$Sr$_{x}$CuO$_{4}$ (LSCO), the latter value of $T_c$ = 40 K being only about 40% of the former. Hg1201 can have almost identical CuO$_6$ octahedra as LSCO if specifically strained. When the apical and in-plane CuO$_2$ distances are the same for the two compounds, a large discrepancy in their $T_c$ remains. Differences in crystal structures and interactions involving the Hg-O charge reservoir layers of Hg1201 may be responsible for the different $T_c$ values exhibited by the two compounds.

cond-mat.supr-con↗

arXiv2013

Universal quantum oscillations in the underdoped cuprate superconductors

The metallic state of the underdoped high-Tc cuprates has remained an enigma: How may seemingly disconnected Fermi surface segments, observed in zero magnetic field as a result of the opening of a partial gap (the pseudogap), possess conventional quasiparticle properties? How do the small Fermi-surface pockets evidenced by the observation of quantum oscillations (QO) emerge as superconductivity is suppressed in high magnetic fields? Such QO, discovered in underdoped YBa2Cu3O6.5 (Y123) and YBa2Cu4O8 (Y124), signify the existence of a conventional Fermi surface (FS). However, due to the complexity of the crystal structures of Y123 and Y124 (CuO2 double-layers, CuO chains, low structural symmetry), it has remained unclear if the QO are specific to this particular family of cuprates. Numerous theoretical proposals have been put forward to explain the route toward QO, including materials-specific scenarios involving CuO chains and scenarios involving the quintessential CuO2 planes. Here we report the observation of QO in underdoped HgBa2CuO4+δ (Hg1201), a model cuprate superconductor with individual CuO2 layers, high tetragonal symmetry, and no CuO chains. This observation proves that QO are a universal property of the underdoped CuO2 planes, and it opens the door to quantitative future studies of the metallic state and of the Fermi-surface reconstruction phenomenon in this structurally simplest cuprate.

cond-mat.supr-con↗

arXiv2013

In search for the pairing glue in cuprates by non-equilibrium optical spectroscopy

In strongly correlated materials the electronic and optical properties are significantly affected by the coupling of fermionic quasiparticles to different degrees of freedom, such as lattice vibrations and bosonic excitations of electronic origin. Broadband ultrafast spectroscopy is emerging as the premier technique to unravel the subtle interplay between quasiparticles and electronic or phononic collective excitations, by their different characteristic timescales and spectral responses. By investigating the femtosecond dynamics of the optical properties of Y-Bi2212 crystals over the 0.5-2 eV energy range, we disentangle the electronic and phononic contributions to the generalized electron-boson Eliashberg function, showing that the spectral distribution of the electronic excitations, such as spin fluctuations and current loops, and the strength of their interaction with quasiparticles can account for the high critical temperature of the superconducting phase transition. Finally, we discuss how the use of this technique can be extended to the underdoped region of the phase diagram of cuprates, in which a pseudogap in the quasiparticle density of states opens. The microscopic modeling of the interaction of ultrashort light pulses with unconventional superconductors will be one of the key challenges of the next-years materials science, eventually leading to the full understanding of the role of the electronic correlations in controlling the dynamics on the femtosecond timescale.

cond-mat.supr-con↗