arXiv subjects

A. Nag

Publications and source records attributed to A. Nag.

17 recordsLinked to original sources

arXiv2022

Signature of quantum criticality in cuprates by charge density fluctuations

The universality of the strange metal phase in many quantum materials is often attributed to the presence of a quantum critical point (QCP), a zero-temperature phase transition ruled by quantum fluctuations. In cuprates, where superconductivity hinders direct QCP observation, indirect evidence comes from the identification of fluctuations compatible with the strange metal phase. Here we show that the recently discovered charge density fluctuations (CDF) possess the right properties to be associated to a quantum phase transition. Using resonant x-ray scattering, we studied the CDF in two families of cuprate superconductors across a wide doping range (up to $p$=0.22). At $p^*\approx$0.19, the putative QCP, the CDF intensity peaks, and the characteristic energy $\Delta$ is minimum, marking a wedge-shaped region in the phase diagram indicative of a quantum critical behavior, albeit with anomalies. These findings strengthen the role of charge order in explaining strange metal phenomenology and provide insights into high-temperature superconductivity.

cond-mat.supr-con↗

arXiv2022

Gapped collective charge excitations and interlayer hopping in cuprate superconductors

We use resonant inelastic x-ray scattering (RIXS) to probe the propagation of plasmons in the electron-doped cuprate superconductor Sr$_{0.9}$La$_{0.1}$CuO$_2$ (SLCO). We detect a plasmon gap of $\sim$~120 meV at the two-dimensional Brillouin zone center, indicating that low-energy plasmons in SLCO are not strictly acoustic. The plasmon dispersion, including the gap, is accurately captured by layered $t$-$J$-$V$ model calculations. A similar analysis performed on recent RIXS data from other cuprates suggests that the plasmon gap is generic and its size is related to the magnitude of the interlayer hopping $t_z$. Our work signifies the three-dimensionality of the charge dynamics in layered cuprates and provides a new method to determine $t_z$.

cond-mat.str-el↗

arXiv2022

Probing electron-phonon interactions away from the Fermi level with resonant inelastic x-ray scattering

Interactions between electrons and lattice vibrations are responsible for a wide range of material properties and applications. Recently, there has been considerable interest in the development of resonant inelastic x-ray scattering (RIXS) as a tool for measuring electron-phonon (e-ph) interactions. Here, we demonstrate the ability of RIXS to probe the interaction between phonons and specific electronic states both near to, and away from, the Fermi level. We performed carbon $K$-edge RIXS measurements on graphite, tuning the incident x-ray energy to separately probe the interactions of the $π^*$ and $σ^*$ electronic states. Our high-resolution data reveals detailed structure in the multi-phonon RIXS features that directly encodes the momentum dependence of the e-ph interaction strength. We develop a Green's-function method to model this structure, which naturally accounts for the phonon and interaction-strength dispersions, as well as the mixing of phonon momenta in the intermediate state. This model shows that the differences between the spectra can be fully explained by contrasting trends of the e-ph interaction through the Brillouin zone, being concentrated at the $Γ$ and $K$ points for the $π^*$ states, while being significant at all momenta for the $σ^*$ states. Our results advance the interpretation of phonon excitations in RIXS, and extend its applicability as a probe of e-ph interactions to a new range of out-of-equilibrium situations.

cond-mat.str-el↗

arXiv2021

Quadrupolar magnetic excitations in an isotropic spin-1 antiferromagnet

The microscopic origins of emergent behaviours in condensed matter systems are encoded in their excitations. In ordinary magnetic materials, single spin-flips give rise to collective dipolar magnetic excitations called magnons. Likewise, multiple spin-flips can give rise to multipolar magnetic excitations in magnetic materials with spin $\mathbf{S} \boldsymbol{\ge} \mathbf{1}$. Unfortunately, since most experimental probes are governed by dipolar selection rules, collective multipolar excitations have generally remained elusive. For instance, only dipolar magnetic excitations have been observed in isotropic $\mathbf{S}\boldsymbol{=}\mathbf{1}$ Haldane spin systems. Here, we unveil a hidden quadrupolar constituent of the spin dynamics in antiferromagnetic $\mathbf{S}\boldsymbol{=}\mathbf{1}$ Haldane chain material Y$_\mathbf{2}$BaNiO$_\mathbf{5}$ using Ni $\mathbf{L_3}$-edge resonant inelastic x-ray scattering. Our results demonstrate that pure quadrupolar magnetic excitations can be probed without direct interactions with dipolar excitations or anisotropic perturbations. Originating from on-site double spin-flip processes, the quadrupolar magnetic excitations in Y$_\mathbf{2}$BaNiO$_\mathbf{5}$ show a remarkable dual nature of collective dispersion. While one component propagates as non-interacting entities, the other behaves as a bound quadrupolar magnetic wave. This result highlights the rich and largely unexplored physics of higher-order magnetic excitations.

cond-mat.str-el↗

arXiv2021

Magnetic excitations in infinite-layer nickelates

The discovery of superconductivity in infinite-layer nickelates brings us tantalizingly close to a new material class that mirrors the cuprate superconductors. Here, we report on magnetic excitations in these nickelates, measured using resonant inelastic x-ray scattering (RIXS) at the Ni L3-edge, to shed light on the material complexity and microscopic physics. Undoped NdNiO2 possesses a branch of dispersive excitations with a bandwidth of approximately 200 meV, reminiscent of strongly-coupled, antiferromagnetically aligned spins on a square lattice, despite a lack of evidence for long range magnetic order. The significant damping of these modes indicates the importance of coupling to rare-earth itinerant electrons. Upon doping, the spectral weight and energy decrease slightly, while the modes become overdamped. Our results highlight the role of Mottness in infinite-layer nickelates.

cond-mat.supr-con↗

arXiv2021

Strong Superexchange in a $d^{9-δ}$ Nickelate Revealed by Resonant Inelastic X-Ray Scattering

The discovery of superconductivity in a $d^{9-δ}$ nickelate has inspired disparate theoretical perspectives regarding the essential physics of this class of materials. A key issue is the magnitude of the magnetic superexchange, which relates to whether cuprate-like high-temperature nickelate superconductivity could be realized. We address this question using Ni L-edge and O K-edge spectroscopy of the reduced trilayer nickelate $d^{9-1/3}$ La4Ni3O8 and associated theoretical modeling. A magnon energy scale of ~80 meV resulting from a nearest-neighbor magnetic exchange of $J = 69(4)4$ meV is observed, proving that $d^{9-δ}$ nickelates can host a large superexchange. This value, along with that of the Ni-O hybridization estimated from our O K-edge data, implies that trilayer nickelates represent an intermediate case between the infinite-layer nickelates and the cuprates, and suggests that they represent a promising route towards higher-temperature nickelate superconductivity.

cond-mat.supr-con↗

arXiv2020

Charge Order Lock-in by Electron-Phonon Coupling in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$

We report an ultrahigh resolution resonant inelastic x-ray scattering (RIXS) study of the in-plane bond-stretching phonon mode in stripe-ordered cuprate La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. Phonon softening and lifetime shortening are found around the charge ordering wave vector. In addition to these self-energy effects, the electron-phonon coupling is probed by its proportionality to the RIXS cross section. We find an enhancement of the electron-phonon coupling around the charge-stripe ordering wave vector upon cooling into the low-temperature tetragonal structure phase. These results suggest that in addition to electronic correlations, electron-phonon coupling contributes significantly to the emergence of long-range charge-stripe order in cuprates.

cond-mat.supr-con↗

arXiv2020

Orbital and Spin Character of Doped Carriers in Infinite-Layer Nickelates

The recent discovery of superconductivity in Nd$_{1-x}$Sr$_{x}$NiO$_2$ has drawn significant attention in the field. A key open question regards the evolution of the electronic structure with respect to hole doping. Here, we exploit x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) to probe the doping dependent electronic structure of the NiO$_2$ planes. Upon doping, a higher energy feature in Ni $L_3$ edge XAS develops in addition to the main absorption peak. By comparing our data to atomic multiplet calculations including $D_{4h}$ crystal field, the doping induced feature is consistent with a $d^8$ spin singlet state, in which doped holes reside in the $d_{x^2-y^2}$ orbitals, similar to doped single band Hubbard models. This is further supported by orbital excitations observed in RIXS spectra, which soften upon doping, corroborating with Fermi level shift associated with increasing holes in the $d_{x^2-y^2}$ orbital.

cond-mat.str-el↗

arXiv2020

Evolution of spin excitations from bulk to monolayer FeSe

The discovery of enhanced superconductivity (SC) in FeSe films grown on SrTiO3 (FeSe/STO) has revitalized the field of Fe-based superconductors. In the ultrathin limit, the superconducting transition temperature Tc is increased by almost an order of magnitude, raising new questions on the pairing mechanism. As in other unconventional superconductors, antiferromagnetic spin fluctuations have been proposed as a candidate to mediate SC in this system. Thus, it is essential to study the evolution of the spin dynamics of FeSe in the ultrathin limit to elucidate their relationship with superconductivity. Here, we investigate and compare the spin excitations in bulk and monolayer FeSe grown on STO using high-resolution resonant inelastic x-ray scattering (RIXS) and quantum Monte Carlo (QMC) calculations. Despite the absence of long-range magnetic order, bulk FeSe displays dispersive magnetic excitations reminiscent of other Fe-pnictides. Conversely, the spin excitations in FeSe/STO are gapped, dispersionless, and significantly hardened relative to the bulk counterpart. By comparing our RIXS results with simulations of a bilayer Hubbard model, we connect the evolution of the spin excitations to the Fermiology of the two systems. The present study reveals a remarkable reconfiguration of spin excitations in FeSe/STO, which is essential to understand the role of spin fluctuations in the pairing mechanism.

cond-mat.str-el↗

arXiv2020

Dynamical spin susceptibility in La2CuO4 studied by resonant inelastic x-ray scattering

Resonant inelastic X-ray scattering (RIXS) is a powerful probe of elementary excitations in solids. It is now widely applied to study magnetic excitations. However, its complex cross-section means that RIXS has been more difficult to interpret than inelastic neutron scattering (INS). Here we report high-resolution RIXS measurements of magnetic excitations of La2CuO4, the antiferromagnetic parent of one system of high-temperature superconductors. At high energies (~2 eV), the RIXS spectra show angular-dependent dd orbital excitations which are found to be in good agreement with single-site multiplet calculations. At lower energies (<0.3 eV), we show that the wavevector-dependent RIXS intensities are proportional to the product of the single-ion spin-flip cross section and the dynamical susceptibility of the spin-wave excitations. When the spin-flip crosssection is dividing out, the RIXS magnon intensities show a remarkable resemblance to INS data. Our results show that RIXS is a quantitative probe the dynamical spin susceptibility in cuprate and therefore should be used for quantitative investigation of other correlated electron materials.

cond-mat.str-el↗

arXiv2020

Spectroscopic Evidence for Charge Order Melting via Quantum Fluctuations in a Cuprate

Copper-oxide high TC superconductors possess a number of exotic orders co-existing with or proximal to superconductivity, whose quantum fluctuations may account for the unusual behaviors of the normal state, even affecting superconductivity. Yet, spectroscopic evidence about such quantum fluctuations remains elusive. Here, we reveal spectroscopic fingerprints for such fluctuations associated with a charge order (CO) in nearly optimally-doped Bi2Sr2CaCu2O8+d, using resonant inelastic x-ray scattering (RIXS). In the superconducting state, while the quasi-elastic CO signal decreases with temperature, the interplay between CO fluctuations and bond-stretching phonons in the form of a Fano-like interference paradoxically increases, incompatible with expectations for competing orders. Invoking general principles, we argue that this behavior reflects the properties of a dissipative system near an order-disorder quantum critical point, where the dissipation varies with the opening of the pseudogap and superconducting gap at low temperatures, leading to the proliferation of quantum critical fluctuations which melt CO.

cond-mat.supr-con↗

arXiv2020

Nature of the charge-density wave excitations in cuprates

The discovery of charge-density wave (CDW)-related effects in the resonant inelastic x-ray scattering (RIXS) spectra of cuprates holds the tantalizing promise of clarifying the interactions that stabilize the electronic order. Here, we report a comprehensive RIXS study of La2-xSrxCuO4 (LSCO) finding that CDW effects persist up to a remarkably high doping level of x = 0.21 before disappearing at x = 0.25. The inelastic excitation spectra remain essentially unchanged with doping despite crossing a topological transition in the Fermi surface. This indicates that the spectra contain little or no direct coupling to electronic excitations near the Fermi surface, rather they are dominated by the resonant cross-section for phonons and CDW-induced phonon-softening. We interpret our results in terms of a CDW that is generated by strong correlations and a phonon response that is driven by the CDW-induced modification of the lattice.

cond-mat.supr-con↗

arXiv2019

Anisotropic damping of the spin fluctuations in doped La2-xSrxCuO4 studied by resonant inelastic x-ray scattering

We report high-resolution resonant inelastic x-ray scattering (RIXS) measurements of the collective spin fluctuations in three compositions of the superconducting cuprate system La2-xSrxCuO4. We have mapped out the excitations throughout much of the 2-D (h,k) Brillouin zone. The spin fluctuations in La2-xSrxCuO4 are found to be fairly well-described by a damped harmonic oscillator model, thus our data allows us to determine the full wavevector dependence of the damping parameter. This parameter increases with doping and is largest along the (h, h) line, where it is peaked near (0.2,0.2). We have used a new procedure to determine the absolute wavevector-dependent susceptibility for the doped compositions La2-xSrxCuO4 (x=0.12,0.16) by normalising our data to La2CuO4 measurements made with inelastic neutron scattering (INS). We find that the evolution with doping of the intensity of high-energy excitations measured by RIXS and INS is consistent. For the doped compositions, the wavevector-dependent susceptibility is much larger at (1/4,1/4) than at (1/2,0). It increases rapidly along the (h,h) line towards the antiferromagnetic wavevector of the parent compound (1/2,1/2). Thus, the strongest magnetic excitations, and those predicted to favour superconductive pairing, occur towards the (1/2,1/2) position as observed by INS.

cond-mat.supr-con↗

arXiv2019

High-resolution resonant inelastic x-ray scattering study of the electron-phonon coupling in honeycomb $α$-Li$_2$IrO$_3$

The excitations in honeycomb $α$-Li$_2$IrO$_3$ have been investigated with high-resolution resonant inelastic x-ray scattering (RIXS) at the O K edge. The low-energy response is dominated by a fully resolved ladder of excitations, which we interpret as being due to multi-phonon processes in the presence of strong electron-phonon coupling (EPC). At higher energies, the orbital excitations are shown to be dressed by phonons. The high quality of the data permits a quantitative test of the analytical model for the RIXS cross-section, which has been proposed to describe EPC in transition metal oxides (TMOs). We find that the magnitude of the EPC is comparable to that found for a range of 3d TMOs. This indicates that EPC may be of equal importance in determining the phenomenology displayed by corresponding 5d based systems.

cond-mat.str-el↗

arXiv2019

Electronic structure of the parent compound of superconducting infinite-layer nickelates

The search for oxide materials with physical properties similar to the cuprate high Tc superconductors, but based on alternative transition metals such as nickel, has grown and evolved over time. The recent discovery of superconductivity in doped infinite-layer nickelates RNiO2 (R = rare-earth element) further strengthens these efforts.With a crystal structure similar to the infinite-layer cuprates - transition metal oxide layers separated by a rare-earth spacer layer - formal valence counting suggests that these materials have monovalent Ni1+ cations with the same 3d electron count as Cu2+ in the cuprates. Here, we use x-ray spectroscopy in concert with density functional theory to show that the electronic structure of RNiO2 (R = La, Nd), while similar to the cuprates, includes significant distinctions. Unlike cuprates with insulating spacer layers between the CuO2 planes, the rare-earth spacer layer in the infinite-layer nickelate supports a weakly-interacting three-dimensional 5d metallic state. This three-dimensional metallic state hybridizes with a quasi-two-dimensional, strongly correlated state with 3dx2-y2 symmetry in the NiO2 layers. Thus, the infinite-layer nickelate can be regarded as a sibling of the rare earth intermetallics, well-known for heavy Fermion behavior, where the NiO2 correlated layers play an analogous role to the 4f states in rare-earth heavy Fermion compounds. This unique Kondo- or Anderson-lattice-like "oxide-intermetallic" replaces the Mott insulator as the reference state from which superconductivity emerges upon doping.

cond-mat.supr-con↗

arXiv2019

Hopping induced ground-state magnetism in 6H perovskite iridates

Investigation of elementary excitations has advanced our understanding of many-body physics governing most physical properties of matter. Recently spin-orbit excitons have drawn much attention, whose condensates near phase transitions exhibit Higgs mode oscillations, a long-sought physical phenomenon [Nat. Phys. {\bf 13}, 633 (2017)]. These critical transition points resulting from competing spin-orbit coupling (SOC), local crystalline symmetry and exchange interactions, are not obvious in Iridium based materials, where SOC prevails in general. Here, we present results of resonant inelastic x-ray scattering on a spin-orbital liquid Ba$_3$ZnIr$_2$O$_9$ and three other 6H-hexagonal perovskite iridates which show magnetism, contrary to non-magnetic singlet ground state expected due to strong SOC. Our results show that substantial hopping between closely placed Ir$^{5+}$ ions within Ir$_2$O$_9$ dimers in these 6H-iridates, modifies spin-orbit coupled states and reduces spin-orbit excitation energies. Here, we are forced to use at least a two-site model, to match the excitation spectrum going in line with the strong intra-dimer hopping. Apart from SOC, low energy physics of iridates is thus critically dependent on hopping, and may not be ignored even for systems having moderate hopping, where the excitation spectra can be explained using an atomic model. SOC which is generally found to be 0.4-0.5~eV in iridates, is scaled in effect down to $\sim$0.26~eV for the 6H-systems, sustaining the hope to achieve quantum criticality by tuning Ir-Ir separation.

cond-mat.str-el↗

arXiv2010

A novel technique for image steganography based on Block-DCT and Huffman Encoding

Image steganography is the art of hiding information into a cover image. This paper presents a novel technique for Image steganography based on Block-DCT, where DCT is used to transform original image (cover image) blocks from spatial domain to frequency domain. Firstly a gray level image of size M x N is divided into no joint 8 x 8 blocks and a two dimensional Discrete Cosine Transform (2-d DCT) is performed on each of the P = MN / 64 blocks. Then Huffman encoding is also performed on the secret messages/images before embedding and each bit of Huffman code of secret message/image is embedded in the frequency domain by altering the least significant bit of each of the DCT coefficients of cover image blocks. The experimental results show that the algorithm has a high capacity and a good invisibility. Moreover PSNR of cover image with stego-image shows the better results in comparison with other existing steganography approaches. Furthermore, satisfactory security is maintained since the secret message/image cannot be extracted without knowing decoding rules and Huffman table.

cs.MM↗