arXiv subjects

Abhishek Nag

Publications and source records attributed to Abhishek Nag.

35 records · Page 2Linked to original sources

arXiv2022

Novel magnetic excitations beyond the single- and double-magnons

Conventional wisdom suggests that one photon that carries one unit of angular momentum can change the spin angular momentum of a magnetic system with one unit (delta Ms = +-1) at most. This would imply that a two-photon scattering process can manipulate the spin angular momentum of the magnetic system with a maximum of two units. Here we examine the fundamental limit of the photon-driven transport of angular momentum by studying the magnon spectrum of α-Fe2O3 using resonant inelastic x-ray scattering. We discovered a cascade of higher-rank magnons carrying double, triple, quadruple, and quintuple the spin angular momentum of a single-magnon. Guided by theoretical calculations, we reveal how a two-photons scattering process can create exotic higher-rank magnons and the relevance of these quasiparticles for magnon-based applications.

cond-mat.str-el↗

arXiv2022

Charge Transfer and $dd$ excitations in AgF$_{2}$

Charge transfer (CT) insulators are the parent phase of a large group of today's unconventional high-temperature superconductors. Here we study experimentally and theoretically the interband excitations of the CT insulator silver fluoride AgF$_2$, which has been proposed as an excellent analogue of oxocuprates. Optical conductivity and resonant inelastic X-ray scattering (RIXS) on AgF$_2$ polycrystalline sample show a close similarity with that measured on undoped La$_2$CuO$_4$. While the former shows a CT gap $\sim$3.4 eV, larger than in the cuprate, $dd$ excitations are nearly at the same energy in the two materials. DFT and exact diagonalization cluster computations of the multiplet spectra show that AgF$_2$ is more covalent than the cuprate, in spite of the larger fundamental gap. Furthermore, we show that AgF$_2$ is at the verge of a charge transfer instability. The overall resemblance of our data on AgF$_2$ to those published previously on La$_2$CuO$_4$ suggests that the underlying CT insulator physics is the same, while AgF$_2$ could also benefit from a proximity to a charge density wave phase as in BaBiO$_3$. Therefore, our work provides a compelling support to the future use of fluoroargentates for materials' engineering of novel high-temperature superconductors.

cond-mat.supr-con↗

arXiv2021

Multiferroic-enabled magnetic exciton in 2D quantum entangled van der Waals antiferromagnet NiI2

Matter-light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, we report that the broken inversion symmetry of multiferroicity can act as an external knob enabling the magnetic exciton in van der Waals antiferromagnet NiI2. We further discover that this magnetic exciton arises from a transition between Zhang-Rice-triplet and Zhang-Rice-singlet's fundamentally quantum entangled states. This quantum entanglement produces an ultra-sharp optical exciton peak at 1.384 eV with a 5 meV linewidth. Our work demonstrates that NiI2 is two-dimensional magnetically ordered with an intrinsically quantum entangled ground state.

cond-mat.str-el↗

arXiv2021

A Broken Translational Symmetry State in an Infinite-Layer Nickelate

A defining signature of strongly correlated electronic systems is the existence of competing phases with similar ground state energies, resulting in a rich phase diagram. While in the recently discovered nickelate superconductors, a high antiferromagnetic exchange energy has been reported, which implies the existence of strong electronic correlations, signatures of competing phases have not yet been observed. Here, we uncover a charge order (CO) in infinite-layer nickelates La1-xSrxNiO2 using resonant x-ray scattering across the Ni L-edge. In the parent compound, the CO arranges along the Ni-O bond direction with an incommensurate wave vector (0.344+/-0.002, 0) r.l.u., distinct from the stripe order in other nickelates which propagates along a direction 45 degree to the Ni-O bond. The CO resonance profile indicates that CO originates from the Ni 3d states and induces a parasitic charge modulation of La electrons. Upon doping, the CO diminishes and the ordering wave vector shifts toward a commensurate value of 1/3 r.l.u., indicating that the CO likely arises from strong correlation effects and not from Fermi surface nesting.

cond-mat.supr-con↗

arXiv2021

Doping-dependence of the electron-phonon coupling in two families of bilayer superconducting cuprates

While electron-phonon coupling (EPC) is crucial for Cooper pairing in conventional superconductors, its role in high-$T_c$ superconducting cuprates is debated. Using resonant inelastic x-ray scattering at the oxygen $K$-edge, we studied the EPC in Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (Bi2212) and Nd$_{1+x}$Ba$_{2-x}$Cu$_3$O$_{7-δ}$ (NBCO) at different doping levels ranging from heavily underdoped ($p =0.07$) to overdoped ($p=0.21$). We analyze the data with a localized Lang-Firsov model that allows for the coherent excitations of two phonon modes. While electronic band dispersion effects are non-negligible, we are able to perform a study of the relative values of EPC matrix elements in these cuprate families. In the case of NBCO, the choice of the excitation energy allows us to disentangle modes related to the CuO$_3$ chains and the CuO$_2$ planes. Combining the results from the two families, we find the EPC strength decreases with doping at $\mathbf{q_\parallel}=(-0.25, 0)$ r.l.u., but has a non-monotonic trend as a function of doping at smaller momenta. This behavior is attributed to the screening effect of charge carriers. We also find that the phonon intensity is enhanced in the vicinity of the charge-density-wave (CDW) excitations while the extracted EPC strength appears to be less sensitive to their proximity. By performing a comparative study of two cuprate families, we are able to identify general trends in the EPC for the cuprates and provide experimental input to theories invoking a synergistic role for this interaction in $d$-wave pairing.

cond-mat.supr-con↗

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

Evolution of the electronic structure in Ta$_2$NiSe$_5$ across the structural transition revealed by resonant inelastic x-ray scattering

We utilized high-energy-resolution resonant inelastic X-ray scattering (RIXS) at both the Ta and Ni $L_3$-edges to map out element-specific particle-hole excitations in Ta$_2$NiSe$_5$ across the phase transition. Our results reveal a momentum dependent gap-like feature in the low energy spectrum, which agrees well with the band gap in element-specific joint density of states calculations based on ab initio estimates of the electronic structure in both the low temperature monoclinic and the high temperature orthorhombic structure. Below $T_c$, the RIXS energy-momentum map shows a minimal gap at the Brillouin zone center ($\sim$ 0.16 eV), confirming that Ta$_2$NiSe$_5$ possesses a direct band gap in its low temperature ground state. However, inside the gap, no signature of anticipated collective modes with an energy scale comparable to the gap size can be identified. Upon increasing the temperature to above $T_c$, whereas the gap at the zone center closes, the RIXS map at finite momenta still possesses the gross features of the low temperature map, suggesting a substantial mixing between the Ta and Ni orbits in the conduction and valence bands, which does not change substantially across the phase transition. Our experimental observations and comparison to the theoretical calculations lend further support that the phase transition and the corresponding gap opening in Ta$_2$NiSe$_5$ is largely structural by nature with possible minor contribution from the putative exciton condensate.

cond-mat.str-el↗

arXiv2021

Unraveling the orbital physics in a canonical orbital system KCuF$_3$

We explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system KCuF$_3$. Using the Cu $L_3$-edge resonant inelastic X-ray scattering we show that the non-dispersive high-energy peaks result from the Cu$^{2+}$ $dd$ orbital excitations. These high-energy modes show good agreement with the {\it ab-initio} quantum chemistry calculation based on a single cluster, indicating that the $dd$ excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Mueller Ansatz calculations. The localized $dd$ excitations and the observation of the strongly dispersive magnetic excitations suggest that orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong {\it local} Jahn-Teller effect in KCuF$_3$, which predominantly drives orbital ordering.

cond-mat.str-el↗

arXiv2020

Detection of Acoustic Plasmons in Hole-Doped Lanthanum and Bismuth Cuprate Superconductors Using Resonant Inelastic X-Ray Scattering

High Tc superconductors show a rich variety of phases associated with their charge degrees of freedom. Valence charges can give rise to charge ordering or acoustic plasmons in these layered cuprate superconductors. While charge ordering has been observed for both hole- and electron-doped cuprates, acoustic plasmons have only been found in electron-doped materials. Here, we use resonant inelastic X-ray scattering (RIXS) to observe the presence of acoustic plasmons in two families of hole-doped cuprate superconductors [La2-xSrxCuO4 (LSCO) and Bi2Sr1.6La0.4CuO6+d (Bi2201)], crucially completing the picture. Interestingly, in contrast to the quasi-static charge ordering which manifests at both Cu and O sites, the observed acoustic plasmons are predominantly associated with the O sites, revealing a unique dichotomy in the behaviour of valence charges in hole-doped cuprates.

cond-mat.str-el↗

arXiv2020

Paramagnons and high-temperature superconductivity in mercury-based cuprates

We present a comparative study of magnetic excitations in the first two Ruddlesden-Popper members of the Hg-family of high-temperature superconducting cuprates, which are chemically nearly identical and have the highest critical temperature ($T_\mathrm{c}$) among all cuprate families. Our inelastic photon scattering experiments reveal that the two compounds' paramagnon spectra are nearly identical apart from an energy scale factor of $\sim130\%$ that matches the ratio of $T_\mathrm{c}$'s, as expected in magnetic Cooper pairing theories. By relating our observations to other cuprates, we infer that the strength of magnetic interactions determines how high $T_\mathrm{c}$ can reach. Our finding can be viewed as a magnetic analogue of the isotope effect, thus firmly supporting models of magnetically mediated high-temperature superconductivity.

cond-mat.supr-con↗

arXiv2020

Multi-orbital charge density wave excitations and concomitant phonon anomalies in Bi$_2$Sr$_2$LaCuO$_{6+δ}$

Charge density waves (CDWs) are ubiquitous in under-doped cuprate superconductors. As a modulation of the valence electron density, CDWs in hole-doped cuprates possess both Cu-3d and O-2p orbital character owing to the strong hybridization of these orbitals near the Fermi level. Here, we investigate under-doped Bi$_2$Sr$_{1.4}$La$_{0.6}$CuO$_{6+δ}$ using resonant inelastic X-ray scattering (RIXS) and find that a short-range CDW exists at both Cu and O sublattices in the copper-oxide (CuO2) planes with a comparable periodicity and correlation length. Furthermore, we uncover bond-stretching and bond-buckling phonon anomalies concomitant to the CDWs. Comparing to slightly over-doped Bi$_2$Sr$_{1.8}$La$_{0.2}$CuO$_{6+δ}$, where neither CDWs nor phonon anomalies appear, we highlight that a sharp intensity anomaly is induced in the proximity of the CDW wavevector (QCDW) for the bond-buckling phonon, in concert with the diffused intensity enhancement of the bond-stretching phonon at wavevectors much greater than QCDW. Our results provide a comprehensive picture of the quasi-static CDWs, their dispersive excitations, and associated electron-phonon anomalies, which are key for understanding the competing electronic instabilities in cuprates.

cond-mat.str-el↗

arXiv2020

Crystalline and magnetic structure of Ba2CuO3+δ investigated by x-ray absorption spectroscopy and resonant inelastic x-ray scattering

Motivated by the recent synthesis of Ba$_2$CuO$_{3+δ}$ (BCO), a high temperature superconducting cuprate with putative $d_{3z^2-r^2}$ ground state symmetry, we investigated its electronic structure by means of Cu $L_3$ x-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) at the Cu $L_3$ edge on a polycrystalline sample. We show that the XAS profile of BCO is characterised by two peaks associated to inequivalent Cu sites, and that its RIXS response features a single, sharp peak associated to crystal-field excitations. We argue that these observations are only partially compatible with the previously proposed crystal structure of BCO. Based on our spectroscopic results and on previously published powder diffraction measurements, we propose a crystalline structure characterized by two inequivalent Cu sites located at alternated planes along the $c$ axis: nominally trivalent Cu(1) belonging to very short Cu-O chains, and divalent Cu(2) in the oxygen deficient CuO$_ {1.5}$ planes. We also analyze the low-energy region of the RIXS spectra to estimate the magnitude of the magnetic interactions in BCO and find that in-plane nearest neighbor superexchange exceeds 120~meV, similarly to that of other layered cuprates. Although these results do not support the pure $d_{3z^2-r^2}$ ground state scenario, they hint at a significant departure from the common quasi-2D electronic structure of superconducting cuprates of pure $d_{x^2-y^2}$ symmetry.

cond-mat.mtrl-sci↗

arXiv2019

Magnetic ground state of distorted 6H perovskite Ba$_3$CdIr$_2$O$_9$

Perovskite iridates of 6H hexagonal structure present a plethora of possibilities in terms of the variety of ground states resulting from a competition between spin-orbit coupling (SOC), hopping, noncubic crystal field ($Δ_{CFE}^{NC}$) and superexchange energy scales within the Ir$_2$O$_9$ dimers. Here we have investigated one such compound Ba$_3$CdIr$_2$O$_9$ by x-ray diffraction, dc magnetic susceptibility($χ$), heat capacity($C_p$) and also ${}^{113}$Cd nuclear magnetic resonance (NMR) spectroscopy. We have established that the magnetic ground state has a small but finite magnetic moment on Ir$^{5+}$ in this system, which likely arises from intradimer Ir-Ir hopping and local crystal distortions. Our heat capacity, NMR, and dc magnetic susceptibility measurements further rule out any kind of magnetic long-/short-range ordering among the Ir moments down to at least 2K. In addition, the magnetic heat capacity data shows linear temperature dependence at low temperatures under applied high fields ($>$ 30 kOe), suggesting gapless spin-density of states in the compound.

cond-mat.str-el↗

arXiv2018

Origin of magnetic moments and presence of a resonating valence bond state in Ba$_2$YIrO$_6$

While it was speculated that 5$d^4$ systems would possess non-magnetic $J$~=~0 ground state due to strong Spin-Orbit Coupling (SOC), all such systems have invariably shown presence of magnetic moments so far. A puzzling case is that of Ba$_2$YIrO$_6$, which in spite of having a perfectly cubic structure with largely separated Ir$^{5+}$ ($d^4$) ions, has consistently shown presence of weak magnetic moments. Moreover, we clearly show from Muon Spin Relaxation ($μ$SR) measurements that a change in the magnetic environment of the implanted muons in Ba$_2$YIrO$_6$ occurs as temperature is lowered below 10~K. This observation becomes counterintuitive, as the estimated value of SOC obtained by fitting the RIXS spectrum of Ba$_2$YIrO$_6$ with an atomic $j-j$ model is found to be as high as 0.39~eV, meaning that the system within this model is neither expected to possess moments nor exhibit temperature dependent magnetic response. Therefore we argue that the atomic $j-j$ coupling description is not sufficient to explain the ground state of such systems, where despite having strong SOC, presence of hopping triggers delocalisation of holes, resulting in spontaneous generation of magnetic moments. Our theoretical calculations further indicate that these moments favour formation of spin-orbital singlets in the case of Ba$_2$YIrO$_6$, which is manifested in $μ$SR experiments measured down to 60~mK.

cond-mat.mtrl-sci↗

arXiv2015

Spin-orbital liquid state assisted by singlet-triplet excitation in $J~=~0$ ground state of Ba$_3$ZnIr$_2$O$_9$

Strong spin-orbit coupling (SOC) effects of heavy $d$-orbital elements have long been neglected in describing the ground states of their compounds thereby overlooking a variety of fascinating and yet unexplored magnetic and electronic states, until recently. The spin-orbit entangled electrons in such compounds can get stabilized into unusual spin-orbit multiplet $J$-states which warrants severe investigations. Here we show using detailed magnetic and thermodynamic studies and theoretical calculations the ground state of Ba$_3$ZnIr$_2$O$_9$, a 6$H$ hexagonal perovskite is a close realisation of the elusive $J$~=~0 state. However, we find that local Ir moments are spontaneously generated due to the comparable energy scales of the singlet-triplet splitting driven by SOC and the superexchange interaction mediated by strong intra-dimer hopping. While the Ir ions within the structural Ir$_2$O$_9$ dimer prefers to form a spin-orbit singlet state (SOS) with no resultant moment, substantial interdimer exchange interactions from a frustrated lattice ensure quantum fluctuations till the lowest measured temperatures and stabilize a spin-orbital liquid phase.

cond-mat.str-el↗

arXiv2012

Giant texturing effect in multiferroic MnWO$_4$ polycrystals

Different methods of texturing polycrystalline materials are developed over years to use/probe anisotropic material properties with relative ease, where complicated and expensive single crystal growth processes could be avoided. In this paper, particle morphology assisted texturing in multiferroic MnWO$_4$ has been discussed. Detailed powder x-ray diffraction vis-a-vis scanning electron microscopic studies on differently annealed and processed samples have been employed to probe the giant texturing effect in powdered MnWO$_4$. A quantitative measure of the texturing has been carried out by means of Rietveld analysis technique. Qualitative presentation of magnetic and dielectric data on textured pellet demonstrated the development of clear anisotropic physical properties in polycrystalline pellets. Finally, we established that the highly anisotropic plate like particles are formed due to easy cleavage of the significantly large crystalline grains.

cond-mat.mtrl-sci↗

arXiv2012

LaSrVMoO$_6$: A case study for $A$-site covalency-driven local cationic order in double perovskites

An unusual atomic scale chemical fluctuation in LaSrVMoO$_6$, in terms of narrow patches of La,V and Sr,Mo-rich phases, has been probed in detail to understand the origin of such a chemical state. Exhaustive tuning of the equilibrium synthesis parameters showed that the extent of phase separation can never be melted down below an unit cell dimension making it impossible to achieve the conventional $B$-site ordered structure, which establishes that the observed `inhomogeneous' patch-like structure with minimum dimension of few angstroms is a reality in LaSrVMoO$_6$. Therefore, another type of local chemical order, hitherto unknown in double perovskites, gets introduced here. X-ray diffraction, electron microscopy elemental mapping, magnetic, and various spectroscopic studies have been carried out on samples, synthesized under different conditions. These experimental results in conjunction with {\it ab-initio} electronic structure calculation revealed that it is the energy stability, gained by typical La-O covalency as in LaVO$_3$, that leads to the preferential La,V and Sr,Mo ionic proximity, and the consequent patchy structure.

cond-mat.mtrl-sci↗