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Matteo Mitrano

Publications and source records attributed to Matteo Mitrano.

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Generic character of charge and spin density waves in superconducting cuprates

Understanding the nature of charge density waves (CDW) in cuprate superconductors has been complicated by material specific differences. A striking example is the opposite doping dependence of the CDW ordering wavevector in La-based and Y-based compounds, the two families where charge ordering is strongest and best characterized. Here we report a combined resonant soft X-ray scattering (RSXS) and neutron scattering study of charge and spin density waves in isotopically enriched La$_{1.8-x}$ Eu$_{0.2}$ Sr$_{x}$ CuO$_{4}$ over a range of doping $0.07 \leq x \leq 0.20$. For all dopings studied by RSXS, we find that the CDW amplitude is approximately temperature-independent and develops well above experimentally accessible temperatures. Surprisingly, the CDW ordering wavevector shows a non-monotonic temperature dependence, with a sudden change occurring at temperatures near the SDW onset temperature. We describe this behavior with a Landau-Ginzburg theory for an incommensurate CDW in a metallic system with a finite charge compressibility and CDW-SDW coupling. Our Landau-Ginzburg analysis suggests that the ordering wavevector at high temperatures decreases with increased doping. This behavior is opposite to the trend at low temperatures and highly reminiscent of the doping dependence seen in YBa$_2$ Cu$_3$ O$_{6+δ}$ , suggesting a common origin of the CDW in hole-doped cuprate superconductors.

cond-mat.supr-con

Ultrafast renormalization of the onsite Coulomb repulsion in a cuprate superconductor

Ultrafast lasers are an increasingly important tool to control and stabilize emergent phases in quantum materials. Among a variety of possible excitation protocols, a particularly intriguing route is the direct light-engineering of microscopic electronic parameters, such as the electron hopping and the local Coulomb repulsion (Hubbard $U$). In this work, we use time-resolved x-ray absorption spectroscopy to demonstrate the light-induced renormalization of the Hubbard $U$ in a cuprate superconductor, La$_{1.905}$Ba$_{0.095}$CuO$_4$. We show that intense femtosecond laser pulses induce a substantial redshift of the upper Hubbard band, while leaving the Zhang-Rice singlet energy unaffected. By comparing the experimental data to time-dependent spectra of single- and three-band Hubbard models, we assign this effect to a $\sim140$ meV reduction of the onsite Coulomb repulsion on the copper sites. Our demonstration of a dynamical Hubbard $U$ renormalization in a copper oxide paves the way to a novel strategy for the manipulation of superconductivity, magnetism, as well as to the realization of other long-range-ordered phases in light-driven quantum materials.

cond-mat.str-el

X-Ray Scattering from Light-Driven Spin Fluctuations in a Doped Mott Insulator

Manipulating spin fluctuations with ultrafast laser pulses is a promising route to dynamically control collective phenomena in strongly correlated materials. However, understanding how photoexcited spin degrees of freedom evolve at a microscopic level requires a momentum- and energy-resolved characterization of their nonequilibrium dynamics. Here, we study the photoinduced dynamics of finite-momentum spin excitations in two-dimensional Mott insulators on a square lattice. By calculating the time-resolved resonant inelastic x-ray scattering cross-section, we show that an ultrafast pump above the Mott gap induces a prompt softening of the spin excitation energy, compatible with a transient renormalization of the exchange interaction. While spin fluctuations in a hole-doped system (paramagnons) are well described by Floquet theory, magnons at half filling are found to deviate from this picture. Furthermore, we show that the paramagnon softening is accompanied by an ultrafast suppression of $d$-wave pairing correlations, indicating a link between the transient spin excitation dynamics and superconducting pairing far from equilibrium.

cond-mat.str-el

Reply to arXiv:2103.10268 `Comment on "Crossover of Charge Fluctuations across the Strange Metal Phase Diagram'''

We recently reported [1,2] measurements of the charge density fluctuations in the strange metal cuprate Bi$_{2.1}$Sr$_{1.9}$Ca$_{1.0}$Cu$_{2.0}$O$_{8+x}$ using both reflection M-EELS and transmission EELS with $\leq$10 meV energy resolution. We observed the well-known 1 eV plasmon in this material for momentum $q\lesssim$ 0.12 r.l.u., but found that it does not persist to large $q$. For $q\gtrsim0.12$ r.l.u., we observe a frequency-independent continuum, similar to that observed in early Raman scattering experiments [3,4], that correlates highly with the strange metal phase [2]. In his Comment (arXiv:2103.10268), Joerg Fink claims we do not see the plasmon, and that our results are inconsistent with optics, RIXS, and the author's own transmission EELS measurements with $\sim$100 meV resolution from the early 1990's [5,6]. The author claims we have made a trigonometry error and are measuring a larger momentum than we think. The author asserts that the two-particle excitations of cuprate strange metals are accurately described by weakly interacting band theory in RPA with corrections for conduction band carrier lifetimes and Umklapp effects. Here, we show that the author's Comment is in contradiction with known information from the literature. At $q\lesssim0.12$ r.l.u. we see the same 1 eV plasmon as other techniques. Moreover we compute our momentum correctly, adjusting the sample and detector angles during an energy scan to keep $q$ fixed. The only discrepancy is between our data and the results of Ref. [5] for $q\gtrsim0.12$ r.l.u. where, because of the coarse resolution used, the data had to be corrected for interference from the elastic line. A reexamination of these corrections in early transmission EELS measurements would likely shed light on this discrepancy.

cond-mat.str-el

Search for $Q \sim 0$ order near a forbidden Bragg position in Bi$_{2.1}$Sr$_{1.9}$CaCu$_2$O$_{8+x}$ with resonant soft x-ray scattering

Identifying what broken symmetries are present in the cuprates has become a major area of research. Many authors have reported evidence for so-called "$Q \sim 0$" order that involves broken inversion, mirror, chiral, or time-reversal symmetry that is uniform in space. Not all these observations are well understood and new experimental probes are needed. Here we use resonant soft x-ray scattering (RSXS) to search for $Q \sim 0$ order in Bi$_{2.1}$Sr$_{1.9}$CaCu$_2$O$_{8+x}$ (Bi-2212) by measuring the region of a forbidden Bragg peak, $(0,0,3)$, which is normally extinguished by symmetry but may become allowed on resonance if valence band order is present. Using circularly polarized light, we found that this reflection becomes allowed on the Cu $L_3$ resonance for temperatures $T_c < T < T^\ast$, though remains absent in linear polarization and at other temperatures. This observation suggests the existence of spatially uniform valence band order near the pseudogap temperature. In addition, we observed periodic oscillations in the specular reflectivity from the sample surface that resemble thin film interference fringes, though no known film is present. These fringes are highly resonant, appear in all polarizations, and exhibit a period that depends on the location where the beam strikes the sample surface. We speculate that these fringes arise from interaction between some intrinsic valence band instability and extrinsic structural surface morphologies of the material. Our study supports the existence of some kind of $Q \sim 0$ broken symmetry state in Bi-2212 at intermediate temperatures, and calls for further study using a microfocused beam that could disentangle microscopic effects from macroscopic heterogeneities.

cond-mat.str-el

Multiple charge density waves and superconductivity nucleation at antiphase domain walls in the nematic pnictide Ba$_{1-x}$Sr$_{x}$Ni$_{2}$As$_{2}$

How superconductivity interacts with charge or nematic order is one of the great unresolved issues at the center of research in quantum materials. Ba$_{1-x}$Sr$_{x}$Ni$_{2}$As$_{2}$ (BSNA) is a charge ordered pnictide superconductor recently shown to exhibit a six-fold enhancement of superconductivity due to nematic fluctuations near a quantum phase transition (at $x_c=0.7$). The superconductivity is, however, anomalous, with the resistive transition for $0.4 < x< x_c$ occurring at a higher temperature than the specific heat anomaly. Using x-ray scattering, we discovered a new charge density wave (CDW) in BSNA in this composition range. The CDW is commensurate with a period of two lattice parameters, and is distinct from the two CDWs previously reported in this material. We argue that the anomalous transport behavior arises from heterogeneous superconductivity nucleating at antiphase domain walls in this CDW. We also present new data on the incommensurate CDW, previously identified as being unidirectional, showing that is a rotationally symmetric, "4$Q$" state with $C_4$ symmetry. Our study establishes BSNA as a rare material containing three distinct CDWs, and an exciting testbed for studying coupling between CDW, nematic, and SC orders.

cond-mat.str-el

Extracting correlation effects from Momentum-Resolved Electron Energy Loss Spectroscopy (M-EELS): Synergistic origin of the dispersion kink in Bi$_{2.1}$Sr$_{1.9}$CaCu$_2$O$_{8+x}$

We employ Momentum-Resolved Electron Energy Loss Spectroscopy (M-EELS) on Bi2.1Sr1.9CaCu2O8+x to resolve the issue of the kink feature in the electron dispersion widely observed in the cuprates. To this end, we utilize the GW approximation to relate the density response function measured in in M-EELS to the self-energy, isolating contributions from phonons, electrons, and the momentum dependence of the effective interaction to the decay rates. The phononic contributions, present in the M-EELS spectra due to electron-phonon coupling, lead to kink features in the corresponding single-particle spectra at energies between 40 meV and 80 meV, independent of the doping level. We find that a repulsive interaction constant in momentum space is able to yield the kink attributed to phonons in ARPES. Hence, our analysis of the M-EELS spectra points to local repulsive interactions as a factor that enhances the spectroscopic signatures of electron-phonon coupling in cuprates. We conclude that the strength of the kink feature in cuprates is determined by the combined action of electron-phonon coupling and electron-electron interactions.

cond-mat.supr-con

Probing light-driven quantum materials with ultrafast resonant inelastic X-ray scattering

Ultrafast optical pulses are an increasingly important tool for controlling quantum materials and triggering novel photo-induced phase transitions. Understanding these dynamic phenomena requires a probe sensitive to spin, charge, and orbital degrees of freedom. Time-resolved resonant inelastic X-ray scattering (trRIXS) is an emerging spectroscopic method, which responds to this need by providing unprecedented access to the finite-momentum fluctuation spectrum of photoexcited solids. In this Perspective, we briefly review state-of-the-art trRIXS experiments on condensed matter systems, as well as recent theoretical advances. We then describe future research opportunities in the context of light control of quantum matter.

cond-mat.str-el

Evidence for photoinduced sliding of the charge-order condensate in La$_{1.875}$Ba$_{0.125}$CuO$_4$

We use femtosecond resonant soft x-ray scattering to measure the ultrafast optical melting of charge-order correlations in La$_{1.875}$Ba$_{0.125}$CuO$_4$. By analyzing both the energy-resolved and energy-integrated order parameter dynamics, we find evidence of a short-lived nonequilibrium state, whose features are compatible with a sliding charge density wave coherently set in motion by the pump. This transient state exhibits shifts in both the quasielastic line energy and its wave vector, as expected from a classical Doppler effect. The wave vector change is indeed found to directly follow the pump propagation direction. These results demonstrate the existence of sliding charge order behavior in an unconventional charge density wave system and underscore the power of ultrafast optical excitation as a tool to coherently manipulate electronic condensates.

cond-mat.str-el

Unconventional Charge Density Wave Order in the Pnictide Superconductor Ba(Ni$_{1-x}$Co$_x$)$_2$As$_2$

Ba(Ni$_{1-x}$Co$_x$)$_2$As$_2$ is a structural homologue of the pnictide high temperature superconductor, Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$, in which the Fe atoms are replaced by Ni. Superconductivity is highly suppressed in this system, reaching a maximum $T_c$ = 2.3 K, compared to 24 K in its iron-based cousin, and the origin of this $T_c$ suppression is not known. Using x-ray scattering, we show that Ba(Ni$_{1-x}$Co$_x$)$_2$As$_2$ exhibits a unidirectional charge density wave (CDW) at its triclinic phase transition. The CDW is incommensurate, exhibits a sizable lattice distortion, and is accompanied by the appearance of $α$ Fermi surface pockets in photoemission [B. Zhou et al., Phys. Rev. B 83, 035110 (2011)], suggesting it forms by an unconventional mechanism. Co doping suppresses the CDW, paralleling the behavior of antiferromagnetism in iron-based superconductors. Our study demonstrates that pnictide superconductors can exhibit competing CDW order, which may be the origin of $T_c$ suppression in this system.

cond-mat.str-el

Ultrafast time-resolved x-ray scattering reveals diffusive charge order dynamics in La$_{2-x}$Ba$_x$CuO$_4$

Charge order is universal among high-T$_c$ cuprates but its relevance to superconductivity is not established. It is widely believed that, while static order competes with superconductivity, dynamic order may be favorable and even contribute to Cooper pairing. We use time-resolved resonant soft x-ray scattering to study the collective dynamics of the charge order in the prototypical cuprate, La$_{2-x}$Ba$_x$CuO$_4$. We find that, at energy scales $0.4$ meV $ \lesssim ω\lesssim 2$ meV, the excitations are overdamped and propagate via Brownian-like diffusion. At energy scales below 0.4 meV the charge order exhibits dynamic critical scaling, displaying universal behavior arising from propagation of topological defects. Our study implies that charge order is dynamic, so may participate tangibly in superconductivity.

cond-mat.str-el

Inequivalence of the zero-momentum Limits of Transverse and Longitudinal Dielectric Response in the Cuprates

We address the question of the mismatch between the zero momentum limits of the transverse and longitudinal dielectric functions for a fixed direction of the driving field observed in the cuprates. This question translates to whether or not the order in which the longitudinal and transverse momentum transfers are taken to zero commute. While the two limits commute for both isotropic and anisotropic Drude metals, we argue that a scaleless vertex interaction that depends solely on the angle between scattered electron momenta is sufficient to achieve non-commutativity of the two limits even for a system that is inherently isotropic. We demonstrate this claim for a simple case of the Drude conductivity modified by electron-boson interactions through appropriate vertex corrections, and outline possible consequences of our result to optical and electron energy loss spectroscopy (EELS) measurements close to zero momentum transfer

cond-mat.str-el

Measurement of the dynamic charge response of materials using low-energy, momentum-resolved electron energy-loss spectroscopy (M-EELS)

One of the most fundamental properties of an interacting electron system is its frequency- and wave-vector-dependent density response function, $χ({\bf q},ω)$. The imaginary part, $χ''({\bf q},ω)$, defines the fundamental bosonic charge excitations of the system, exhibiting peaks wherever collective modes are present. $χ$ quantifies the electronic compressibility of a material, its response to external fields, its ability to screen charge, and its tendency to form charge density waves. Unfortunately, there has never been a fully momentum-resolved means to measure $χ({\bf q},ω)$ at the meV energy scale relevant to modern elecronic materials. Here, we demonstrate a way to measure $χ$ with quantitative momentum resolution by applying alignment techniques from x-ray and neutron scattering to surface high-resolution electron energy-loss spectroscopy (HR-EELS). This approach, which we refer to here as "M-EELS," allows direct measurement of $χ''({\bf q},ω)$ with meV resolution while controlling the momentum with an accuracy better than a percent of a typical Brillouin zone. We apply this technique to finite-q excitations in the optimally-doped high temperature superconductor, Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ (Bi2212), which exhibits several phonons potentially relevant to dispersion anomalies observed in ARPES and STM experiments. Our study defines a path to studying the long-sought collective charge modes in quantum materials at the meV scale and with full momentum control.

cond-mat.supr-con

Phonon-pump XUV-photoemission-probe in graphene: evidence for non-adiabatic heating of Dirac carriers by lattice deformation

We modulate the atomic structure of bilayer graphene by driving its lattice at resonance with the in-plane E1u lattice vibration at 6.3um. Using time- and angle-resolved photoemission spectroscopy (tr-ARPES) with extreme ultra-violet (XUV) pulses, we measure the response of the Dirac electrons near the K-point. We observe that lattice modulation causes anomalous carrier dynamics, with the Dirac electrons reaching lower peak temperatures and relaxing at faster rate compared to when the excitation is applied away from the phonon resonance or in monolayer samples. Frozen phonon calculations predict dramatic band structure changes when the E1u vibration is driven, which we use to explain the anomalous dynamics observed in the experiment.

cond-mat.mes-hall

Population Inversion in Monolayer and Bilayer Graphene

The recent demonstration of saturable absorption and negative optical conductivity in the Terahertz range in graphene has opened up new opportunities for optoelectronic applications based on this and other low dimensional materials. Recently, population inversion across the Dirac point has been observed directly by time- and angle-resolved photoemission spectroscopy (tr-ARPES), revealing a relaxation time of only ~ 130 femtoseconds. This severely limits the applicability of single layer graphene to, for example, Terahertz light amplification. Here we use tr-ARPES to demonstrate long-lived population inversion in bilayer graphene. The effect is attributed to the small band gap found in this compound. We propose a microscopic model for these observations and speculate that an enhancement of both the pump photon energy and the pump fluence may further increase this lifetime.

cond-mat.mtrl-sci

Snapshots of non-equilibrium Dirac carrier distributions in graphene

The optical properties of graphene are made unique by the linear band structure and the vanishing density of states at the Dirac point. It has been proposed that even in the absence of a semiconducting bandgap, a relaxation bottleneck at the Dirac point may allow for population inversion and lasing at arbitrarily long wavelengths. Furthermore, efficient carrier multiplication by impact ionization has been discussed in the context of light harvesting applications. However, all these effects are difficult to test quantitatively by measuring the transient optical properties alone, as these only indirectly reflect the energy and momentum dependent carrier distributions. Here, we use time- and angle-resolved photoemission spectroscopy with femtosecond extreme ultra-violet (EUV) pulses at 31.5 eV photon energy to directly probe the non-equilibrium response of Dirac electrons near the K-point of the Brillouin zone. In lightly hole-doped epitaxial graphene samples, we explore excitation in the mid- and near-infrared, both below and above the minimum photon energy for direct interband transitions. While excitation in the mid-infrared results only in heating of the equilibrium carrier distribution, interband excitations give rise to population inversion, suggesting that terahertz lasing may be possible. However, in neither excitation regime do we find indication for carrier multiplication, questioning the applicability of graphene for light harvesting. Time-resolved photoemission spectroscopy in the EUV emerges as the technique of choice to assess the suitability of new materials for optoelectronics, providing quantitatively accurate measurements of non-equilibrium carriers at all energies and wavevectors.

cond-mat.mes-hall

Anisotropic compression in the high pressure regime of pure and Cr-doped vanadium dioxide

We present structural studies of V$_{1-x}$Cr$_x$O$_2$ (pure, 0.7% and 2.5% Cr doped) compounds at room temperature in a diamond anvil cell for pressures up to 20 GPa using synchrotron x-ray powder diffraction. All the samples studied show a persistence of the monoclinic $M_1$ symmetry between 4 and 12 GPa. Above 12 GPa, the monoclinic $M_1$ symmetry changes to isostructural $M_x$ phase (space group $P2_1/c$) with a significant anisotropy in lattice compression of the $b$-$c$ plane of the $M_{1}$ phase. This behavior can be reconciled invoking the pressure induced charge-delocalization.

cond-mat.str-el