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Abhisek Bandyopadhyay

Publications and source records attributed to Abhisek Bandyopadhyay.

12 recordsLinked to original sources

Regulating oxygen content and superconductivity in La$_3$Ni$_2$O$_{7+δ}$

The synthesis of high-quality Ruddlesden-Popper (RP) nickelates remains challenging due to variations in oxygen content and the prevalence of intergrown RP phases. Precisely controlling the stoichiometry and characterizing the resulting physical properties are essential for understanding the mechanism of high-$T_c$ superconductivity in these materials. In this work, we synthesize a series of La$_3$Ni$_2$O$_{7+δ}$ samples with systematically controlled oxygen content and perform comprehensive structural and compositional analyses. Precise oxygen tuning enables us to tailor the microstructure, yielding a pure bilayer phase, a mixture of bilayer and hybrid single-layer-bilayer phases, and a predominantly bilayer phase containing trilayer intergrowths. High-pressure transport measurements reveal distinct superconducting transitions with contrasting $T_c$ values, corresponding to the bilayer phase, the hybrid phase, and trilayer inclusions. Notably, we find that oxygen content not only governs the phase purity$-$i.e., the presence of intergrowth phases$-$but also directly modulates the upper critical field ($H_{c2}$) of the bilayer superconductivity. By establishing a phase diagram of $T_c$ and $H_{c2}$ as functions of oxygen content in La$_3$Ni$_2$O$_{7+δ}$, this work advances synthetic control and provides new insights into the superconducting mechanism of RP nickelates.

cond-mat.supr-con↗

Emergent Dynamic Magnetic Ground State in a Mixed 3d/5d Heavy Fermion System CaCu3Ir4O12

Quantum-disordered magnetic ground states are challenging to identify in three-dimensional (3D) oxides, where strong exchange pathways typically favour long-range magnetic order or spin freezing. The quadruple perovskite $\mathrm{CaCu_3Ir_4O_{12}}$, crystallizing in the cubic $Im\bar{3}$ structure, provides a 3D lattice where $\mathrm{Cu^{2+}}$ $3d$ moments are coupled to an extended Ir $5d$ network, offering a rare platform for probing quantum-disordered magnetism in a mixed $3d/5d$ electron system. Here, we combine bulk probes, including DC and AC magnetic susceptibility, and heat capacity measurements (down to $50~\mathrm{mK}$), along with the local microscopic probe muon spin relaxation ($μ$SR) (down to $40~\mathrm{mK}$), to investigate the true magnetic ground state of $\mathrm{CaCu_3Ir_4O_{12}}$. Despite strong antiferromagnetic interactions ($θ_{\mathrm{W}} \sim -200~\mathrm{K}$, with an applied-field dependence), no signature of long-range magnetic ordering or spin freezing is detected down to the lowest measured temperatures. Furthermore, our in-depth zero-field (ZF) and longitudinal-field (LF) $μ$SR characterizations confirm strong quantum spin fluctuations and the truly dynamic nature of the local moments down to $40~\mathrm{mK}$. These results establish $\mathrm{CaCu_3Ir_4O_{12}}$ as a promising 3D quantum-disordered magnet and a well-characterized platform for exploring fluctuation-dominated states in correlated $3d/5d$ oxides.

cond-mat.str-el↗

Unveiling the magnetic ground states in the iridate double perovskite Pr(2-x)SrxMgIrO6 (x = 0 and 0.5) series

We report here the results of a detailed magnetic, thermodynamic, and neutron powder diffraction (NPD) studies carried out on the double perovskite iridates Pr(2-x)SrxMgIrO6 (x = 0 and 0.5). Temperature dependent bulk DC susceptibility data clearly reveals a sharp antiferromagnetic (AFM) transition at 14.5 K in Pr2MgIrO6(x = 0). Next, a weaker signature of an AFM transition at a lower temperature (6 K) is observed in x = 0.5 i.e., Pr1.5Sr0.5MgIrO6 (PSMIO1505). The observed magnetic transitions are further corroborated by the presence of anomalies around the same temperatures in our T-dependent specific heat results. The charge states of both Pr and Ir cations have been confirmed to be the expected ones (3+ for Pr in both the compounds, while Ir is in a pure 4+ state for x = 0 and in a mixed 4+/5+ state for x = 0.5) from the core-level x-ray photoemission spectroscopy (XPS) measurements. Using neutron powder diffraction (NPD) the magnetic ground states and the magnetic moment values were determined for both compounds. Both the Pr- and Ir-sites undergo AFM ordering below the respective transition temperatures, designated by the propagation vector k = ( 1/2 , 0, 1/2 ), in both the compounds.

cond-mat.str-el↗

Quantum spin liquid ground state in a rare-earth triangular antiferromagnet SmTa$_7$O$_{19}$

The rare-earth-based geometrically frustrated triangular magnets have attracted considerable attention due to the intricate interplay between strong spin-orbit coupling and the crystal electric field (CEF), which often leads to effective spin-1/2 degrees of freedom and therefore promotes strong quantum fluctuations at low temperatures, thus offering an excellent route to stabilize a quantum spin liquid (QSL) ground state. We have investigated the ground state magnetic properties of a polycrystalline sample of $\text{SmTa}_7\text{O}_{19}$ which we propose to have a gapless QSL ground state by employing powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), DC and AC-magnetic susceptibility, $M$ vs. $H$ isotherm, specific heat, and muon spin rotation/relaxation measurements ($μ$SR) down to 30 mK. The combined structural and electronic studies reveal the formation of an edge-sharing equilateral triangular lattice of Sm$^{3+}$ ions in $ab$ plane. The DC, AC magnetic susceptibility, and heat capacity measurements reveal that $\text{SmTa}_7\text{O}_{19}$ does not exhibit any long-range magnetic ordering transition down to 50 mK. The zero-field (ZF)-$μ$SR study strongly refutes the long-range magnetically ordered ground state and/or any partial spin-freezing down to at least 30 mK. The ZF-muon-spin relaxation rate is weakly temperature dependent between 50 and 20 K, rapidly increases below $\sim$20 K and saturates at low temperatures between 2 K and 30 mK, which has been attributed to a characteristic signature of QSL systems. Further, our longitudinal-field (LF)-$μ$SR measurements at 0.1 K reveal a dynamic nature of the magnetic ground state. In addition, our high-field specific heat data suggest a gapless nature of spin excitations in this compound.

cond-mat.str-el↗

Novel quantum spin liquid ground state in the trimer rhodate Ba$_4$NbRh$_3$O$_{12}$

Frustrated magnets offer a plethora of exotic magnetic ground states, including quantum spin liquids (QSLs), in which enhanced quantum fluctuations prevent a long-range magnetic ordering of the strongly correlated spins down to lowest temperature. Here we have investigated the trimer based mixed valence hexagonal rhodate Ba$_4$NbRh$_3$O$_{12}$ using a combination of dc and ac magnetization, electrical resistivity, specific heat, and muon spin rotation/relaxation ($μ$SR) measurements. Despite the substantial antiferromagnetic exchange interactions, as evident from the Weiss temperature ($θ_{\mathrm{W}}\sim -35$ to -45 K), among the Rh-local moments, neither long-range magnetic ordering nor spin-freezing is observed down to at least 50 mK, in ac-susceptibility, specific heat and ZF-$μ$SR measurements (down to 0.26 K). We ascribe the absence of any magnetic transition to enhanced quantum fluctuations as a result of geometrical frustration arising out of the edge-sharing equilateral Rh-triangular network in the structure. Our longitudinal-field $μ$SR result evidences persistent spin fluctuations down to 0.26~K, thus stabilizing a dynamic QSL ground state in Ba$_4$NbRh$_3$O$_{12}$. Furthermore, the magnetic specific heat ($C_{\mathrm{m}}$) data at low-$T$ reveal a significant $T$-linear contribution plus a quadratic $T$-dependence. A $T$-linear behavior is evocative of gapless spin excitations, while the $T^2$-term of $C_{\mathrm{m}}$ may indicate the Dirac QSL phenomenology of the spinon excitations with a linear dispersion.

cond-mat.str-el↗

The interplay between structural, magnetic and electronic states in the pyrochlore iridate Eu2Ir2O7

We address the concomitant metal-insulator transition (MIT) and antiferromagnetic ordering in the novel pyrochlore iridate Eu2Ir2O7 by combining x-ray absorption spectroscopy, x-ray and neutron diffractions and density functional theory (DFT) based calculations. The temperature dependent powder x-ray diffraction clearly rules out any change in the lattice symmetry below the MIT, nevertheless a clear anomaly in the Ir-O-Ir bond angle and Ir-O bond length is evident at the onset of MIT. From the x-ray absorption near edge structure (XANES) spectroscopic study of Ir-L3 and L2 edges, the effective spin-orbit coupling is found to be intermediate, at least quite far from the strong atomic spin-orbit coupling limit. Powder neutron diffraction measurement is in line with an all-in-all-out magnetic structure of the Ir-tetrahedra in this compound, which is quite common among rare-earth pyrochlore iridates. The sharp change in the Ir-O-Ir bond angle around the MIT possibly arises from the exchange striction mechanism, which favors an enhanced electron correlation via weakening of Ir-Ir orbital overlap and an insulating phase below TMI . The theoretical calculations indicate an insulating state for shorter bond angle validating the experimental observation. Our DFT calculations show a possibility of intriguing topological phase below a critical value of the Ir-O distance, which is shorter than the experimentally observed bond length. Therefore, a topological state may be realized in bulk Eu2Ir2O7 sample if the Ir-O bond length can be reduced by the application of sufficient external pressure.

cond-mat.str-el↗

Sr$_3$LiIrO$_6$: a potential quantum spin liquid candidate in the one dimensional $d^4$ iridate family

Spin-orbit coupling (SOC) offers a large variety of novel and extraordinary magnetic and electronic properties in otherwise `ordinary pool' of heavy ion oxides. Here we present a detailed study on an apparently isolated hexagonal 2$H$ spin-chain $d^4$ iridate Sr$_3$LiIrO$_6$ (SLIO) with geometric frustration. Our structural studies clearly reveal perfect Li-Ir chemical order in this compound. Our combined experimental and {\it ab-initio} electronic structure investigations establish a magnetic ground state with finite Ir$^{5+}$ magnetic moments in this compound, contrary to the anticipated nonmagnetic $J$=0 state. Furthermore, the dc magnetic susceptibility ($χ$), heat capacity ($C_p$) and spin-polarized density functional theory (DFT) studies unravel that despite having noticeable antiferromagnetic correlation among the Ir$^{5+}$ local moments, this SLIO system evades any kind of magnetic ordering down to at least 2 K due to geometrical frustration, arising from the comparable interchain Ir-O-O-Ir superexchange interaction strengths, hence promoting SLIO as a potential quantum spin liquid candidate.

cond-mat.str-el↗

Failure to achieve the $J_{eff}$~=~0 state even in nearly isolated Ir$^{5+}$ in Sr$_3$NaIrO$_6$: are iridates enough for realizing true $j$-$j$ coupling?

Spin-orbit coupling (SOC) often gives rise to interesting electronic and magnetic phases in an otherwise ordinary pool of paramagnetic heavy metal oxides. In presence of strong SOC, assumed to be working in $j$-$j$ coupling regime, 5$d^4$ iridates are generally speculated to possess a nonmagnetic $J_{eff}$~=~0 singlet ground state, which invariably gets masked due to different solid-state effects (e.g. hopping). Here, we try to probe the trueness of the atomic SOC-based proposal in an apparently 1-dimensional system, Sr$_3$NaIrO$_6$, possessing a 2$H$ hexagonal structure with well separated Ir$^{5+}$ (5$d^4$) ions. But all the detailed experimental as well as theoretical characterizations reveal that the ground state of Sr$_3$NaIrO$_6$ is not nonmagnetic, rather accommodating a significantly high effective magnetic moment on Ir$^{5+}$ ion. However our combined dc susceptibility ($χ$), ${}^{23}$Na nuclear magnetic resonance (NMR), muon-spin-relaxation/rotation ($μ$SR) and heat capacity ($C_p$) measurements clearly refute any sign of spin-freezing or ordered magnetism among the Ir$^{5+}$ moments due to geometrical exchange frustration, while in-depth zero-field (ZF) and longitudinal field (LF) $μ$SR investigations strongly point towards inhomogeneous quantum spin-orbital liquid (QSOL)-like ground state. In addition, the linear temperature dependence of both the NMR spin-lattice relaxation rate and the magnetic heat capacity at low temperatures suggest low-lying gapless spin excitations in the QSOL phase of this material. Finally, we conclude that the effective SOC realised in $d^4$ iridates are unlikely to offer a ground state which will be consistent with a purely atomic $j$-$j$ coupling description.

cond-mat.str-el↗

A Colossal Electroresistance response, accompanied by metal-insulator transition, in a mixed-valent vanadate

Colossal electroresistance (CER) in manganites, i.e., a large change in electrical resistance under the influence of either an applied electric field or an applied electric current, has often been described as complimentary to the colossal magnetoresistance (CMR) effect. Mixed valent vanadates with active t2g and empty eg orbitals, unlike manganites, have not naturally been discussed in this context, as double exchange based CMR is not realizable in them. However, presence of coupled spin and orbital degrees of freedom, metal-insulator transition (MIT) accompanied by orbital order-disorder transition, etc., anyway make the vanadates an exciting group of materials. Here we probe a Fe-doped hollandite lead vanadate PbFe1.75V4.25O11 (PFVO), which exhibits a clear MIT as a function of temperature. Most importantly, a giant fall in the resistivity, indicative of a CER, as well as a systematic shift in the MIT towards higher temperature are observed as a function of applied electric current. Detailed structural, magnetic, thermodynamic and transport studies point towards a complex interplay between orbital order/disorder effect, MIT and double exchange in this system.

cond-mat.str-el↗

Evolution of electronic and magnetic properties in a series of iridate double perovskites Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1.0)

Spin-orbit coupling (SOC) plays a crucial role in magnetic and electronic properties of 5$d$ iridates. In this paper we have experimentally investigated the structural and physical properties of a series of Ir-based double perovskite compounds Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1; hereafter abbreviated as PMIO, PSMIO1505, and PSMIO). Interestingly, these compounds have recently been proposed to undergo a transition from the spin-orbit-coupled Mott insulating phase at $x$ = 0 to the elusive half-metallic antiferromagnetic (HMAFM) state with Sr doping at $x$ = 1. However, our detailed magnetic and electrical measurements refute any kind of HMAFM possibility in either of the doped samples. In addition, we establish that within these Pr$_{2-x}$Sr$_x$MgIrO$_6$ double perovskites, changes in Ir-oxidation states (4+ for PMIO to 5+ for PSMIO via mixed 4+/5+ for PSMIO1505) lead to markedly different magnetic behaviors. While SOC on Ir is at the root of the observed insulating behaviors for all three samples, the correlated magnetic properties of these three compounds develop entirely due to the contribution from local Ir moments. Additionally, the magnetic Pr$^{3+}$ (4$f^2$) ions, instead of showing any kind of ordering, only contribute to the total paramagnetic moment. It is seen that the PrSrMgIrO$_6$ sample does not order down to 2 K despite antiferromagnetic interactions. But, the $d^5$ iridate Pr$_2$MgIrO$_6$ shows a sharp antiferromagnetic (AFM) transition at around 14 K, and in the mixed valent Pr$_{1.5}$Sr$_{0.5}$MgIrO$_6$ sample the AFM transition is shifted to a much lower temperature ($\sim$ 6 K) due to weakening of the AFM exchange.

cond-mat.str-el↗

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↗

Development of half metallicity within mixed magnetic phase of Cu$_{1-x}$Co$_x$MnSb alloy

Cubic Half-Heusler Cu$_{1-x}$Co$_x$MnSb (0 $\leq$ $x$ $\leq$ 0.1) compounds have been investigated both experimentally and theoretically for their magnetic, transport and electronic properties in search of possible half metallic antiferromagnetism. The systems (Cu,Co)MnSb are of particular interest as the end member alloys CuMnSb and CoMnSb are semi metallic (SM) antiferromagnetic (AFM) and half metallic (HM) ferromagnetic (FM), respectively. Clearly, Co-doping at the Cu-site of CuMnSb introduces changes in the carrier concentration at the Fermi level that may lead to half-metallic ground state but there remains a persistent controversy whether the AFM to FM transition occurs simultaneously. Our experimental results reveal that the AFM to FM magnetic transition occurs through a percolation mechanism where Co-substitution gradually suppresses the AFM phase and forces FM polarization around every dopant cobalt. As a result a mixed magnetic phase is realized within this composition range while a nearly HM band structure is developed already at the 10% Co-doping. Absence of T$^2$ dependence in the resistivity variation at low T-region serves as an indirect proof of opening up an energy gap at the Fermi surface in one of the spin channels. This is further corroborated by the ab-initio electronic structure calculations that suggests a nearly ferromagnetic half-metallic ground state is stabilized by Sb-p holes produced upon Co doping.

cond-mat.str-el↗