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J. Sannigrahi

Publications and source records attributed to J. Sannigrahi.

15 recordsLinked to original sources

Microscopic investigation of spin dynamics in the single-chain magnet Sr4Mn2CoO9

One-dimensional single-chain magnets offer a unique platform for studying the interplay of crystal-field effects, exchange interactions, and lattice dynamics. Here, we investigate spin excitations in Sr4Mn2CoO9 using inelastic neutron scattering (INS) and theoretical modelling. INS reveals two low-energy magnetic excitations at 4 and 7 meV from Mn-Co-Mn spin chains, alongside higher-energy crystal-electric-field (CEF) excitations from two crystallographically inequivalent Co2+ sites. Interestingly, these spin excitations persist at room temperature, demonstrating dynamic magnetic correlations in the absence of long-range order. Furthermore, the crystal-field modelling, based on Stevens operator formalism, reproduces well the CEF spectra, establishing Ising-like Kramers ground-state doublets with strong uniaxial magnetic anisotropy for both Co2+ ions. In addition, the spin wave simulation using SpinW reproduces the spin excitation spectrum and reveals microscopic exchange interactions in two non-interacting Mn-Co-Mn spin chains. Finally, machine-learning lattice-dynamics calculations confirm the phonon spectrum and spin-phonon coupling. By projecting the exchange Hamiltonian onto CEF ground-state doublets, we estimate exchange-induced splittings matching the observed excitations. Thus, our results elucidate low-energy spin dynamics arising from combined crystal-field anisotropy and exchange interactions, with the persistent low-energy excitation providing a microscopic pathway for thermally activated spin relaxation. Furthermore, this work delivers a unified microscopic understanding of the interplay between crystal-field effects, magnetic exchange, and lattice dynamics in Sr4Mn2CoO9, advancing insights into spin dynamics in low-dimensional transition-metal oxides.

cond-mat.mtrl-sci↗

Interplay between trimer structure and magnetic ground state in Ba5Ru3O12 probed by Neutron and muSR techniques

We report a detailed inelastic neutron scattering (INS) and muon spin relaxation (muSR) investigation of a trimer Ruthenate Ba5Ru3O12 system, which undergoes long-range antiferromagnetic ordering at TN = 60 K. The INS reveals two distinct spin wave excitations below TN: one at 5.6 meV and the other at 10-15 meV. By accompanying the INS spectra based on a linear spin wave theory using SpinW software and machine learning force fields (MLFFs), we show that Ba5Ru3O12 exhibits spin frustration due to competing exchange interactions between neighboring and next-neighboring Ru-moments, exchange anisotropy, and strong spin-orbit coupling, which yields a non-collinear spin structure, in contrast to other ruthenate trimers in this series. Interestingly, these magnetic excitations do not completely vanish even at high temperatures above TN, evidencing short-range magnetic correlations in this trimer system. This is further supported by muSR spectroscopy, which exhibits a gradual drop in the initial asymmetry around the magnetic phase transition and is further verified through maximum entropy analysis. The results of muSR spectroscopy indicate a dynamic nature of magnetic order, attributed to local magnetic anisotropy within the trimer as a result of local structural distortion and different hybridization, consistent with canted spin-structure. We predict the ground state of Ru3O12-isolated trimer through theoretical calculations, which agree with the experimentally observed spin excitation

cond-mat.str-el↗

Role of crystal field ground state in the classical spin-liquid behavior of a quasi-one dimensional spin-chain system Sr3NiPtO6

The spin-chain compound Sr3NiPtO6 is known to have a nonmagnetic ground state. We have investigated the nature of ground state of Sr3NiPtO6 using magnetic susceptibility $χ(T)$, heat capacity $C_{\rm p}(T)$, muon spin relaxation ($μ$SR) and inelastic neutron scattering (INS) measurements. The $χ(T)$ and $C_{\rm p}(T)$ do not exhibit any pronounced anomaly that can be associated with a phase transition to a magnetically ordered state. Our $μ$SR data confirm the absence of long-range magnetic ordering down to 0.04 K. Furthermore, the muon spin relaxation rate increases below 20 K and exhibits temperature independent behavior at low temperature, very similar to that observed in a quantum spin-liquid system. The INS data show a large excitation near 8~meV, and the analysis of the INS data reveals a singlet CEF ground state with a first excited CEF doublet state at $Δ_{\rm CEF}$ = 7.7 meV. The estimated CEF parameters reveal a strong planar anisotropy in the calculated $χ(T)$, consistent with the reported behavior of the $χ(T)$ of single crystal Sr3NiPtO6. We propose that the nonmagnetic singlet ground state and a large $Δ_{\rm CEF}$ (much larger than the exchange interaction $\mathcal{J}_{\rm ex}$) are responsible for the absence of long-range magnetic ordering and can mimic a classical spin-liquid behavior in this quasi-1D spin chain system Sr3NiPtO6. The classical spin-liquid ground state observed in Sr3NiPtO6 is due to the single-ion property, which is different from the quantum spin-liquid ground state observed in geometrically frustrated systems, where two-ion exchanges play an important role.

cond-mat.str-el↗

Nodeless time-reversal symmetry breaking in the centrosymmetric superconductor Sc$_5$Co$_4$Si$_{10}$ probed by muon-spin spectroscopy

We investigate the superconducting properties of Sc$_{5}$Co$_{4}$Si$_{10}$ using low-temperature resistivity, magnetization, heat capacity, and muon-spin rotation and relaxation ($μ$SR) measurements. We find that Sc$_{5}$Co$_{4}$Si$_{10}$ {exhibits type-II} superconductivity with a superconducting transition temperature $T_\mathrm{C}= 3.5 (1)$\,K. The temperature dependence of the superfluid density obtained from transverse-field $μ$SR spectra is best modeled using an isotropic Bardeen-Cooper-Schrieffer type $s$-wave gap symmetry with $2Δ/k_\mathrm{B}T_\mathrm{C} = 2.84(2)$. However, the zero-field muon-spin relaxation asymmetry reveals the appearance of a spontaneous magnetic field below $T_\mathrm{C}$, indicating that time-reversal symmetry (TRS) is broken in the superconducting state. Although this behavior is commonly associated with non-unitary or mixed singlet-triplet pairing, our group-theoretical analysis of the Ginzburg-Landau free energy alongside density functional theory calculations indicates that unconventional mechanisms are pretty unlikely. Therefore, we have hypothesized that TRS breaking may occur via a conventional electron-phonon process.

cond-mat.supr-con↗

A crossover from Kondo semiconductor to metallic antiferromagnet with $5d$-electron doping in CeFe$_2$Al$_{10}$

We report a systematic study of the $5d$-electron-doped system Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($0 \leq x \leq 0.15$). With increasing $x$, the orthorhombic $b$~axis decreases slightly while accompanying changes in $a$ and $c$ leave the unit cell volume almost unchanged. Inelastic neutron scattering, along with thermal and transport measurements, reveal that for the Kondo semiconductor CeFe$_2$Al$_{10}$, the low-temperature energy gap which is proposed to be a consequence of strong $c \mhyphen f$ hybridization, is suppressed by a small amount of Ir substitution for Fe, and that the system adopts a metallic ground state with an increase in the density of states at the Fermi level. The charge or transport gap collapses (at $x=$~0.04) faster than the spin gap with Ir substitution. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements demonstrate that the system undergoes long-range antiferromagnetic order below a Néel temperature, $T_{\mathrm{N}}$, of 3.1(2)~K for $x = 0.15$. The ordered moment is estimated to be smaller than 0.07(1)~$μ_\mathrm{B}$/Ce although the trivalent state of Ce is confirmed by Ce L$_3$-edge x-ray absorption near edge spectroscopy. It is suggested that the $c \mhyphen f$ hybridization gap, which plays an important role in the unusually high ordering temperatures observed in Ce$T_2$Al$_{10}$ ($T$ = Ru and Os), may not be necessary for the onset of magnetic order with a low $T_{\mathrm{N}}$ seen here in Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$.

cond-mat.str-el↗

Robustness of helical magnetic structure under external pressure in Fe-doped MnNiGe alloy

We have investigated the detailed magnetic structure of a Fe-doped MnNiGe alloy of nominal composition MnNi$_{0.75}$Fe$_{0.25}$Ge by ambient and high pressure (6 kbar) neutron powder diffraction study. The alloy undergoes a martensitic phase transition between 230 K and 275 K. The low-temperature martensite phase orders antiferromagnetically with helical modulation of Mn-spins. At 1.5 K, the incommensurate propagation vector $\bf k$ is found to be (0.1790(1),0,0), and it remains almost unchanged with temperature under ambient condition. The Application of external pressure ($P$) reduces the martensitic transition temperature and results in a significant change in the incommensurate magnetic propagation vector. At 10 K, with 6 kbar of external pressure, the incommensurate magnetic structure of the alloy stabilizes with $\bf k$ = (0.1569(1),0,0). Interestingly, the strong temperature dependence of $\bf k$ in the presence of external $P$ has also been observed.

cond-mat.mtrl-sci↗

Commensurate to incommensurate magnetic phase transition in Honeycomb-lattice pyrovanadate Mn2V2O7

We have synthesized single crystalline sample of Mn$_2$V$_2$O$_7$ using floating zone technique and investigated the ground state using magnetic susceptibility, heat capacity and neutron diffraction. Our magnetic susceptibility and heat capacity reveal two successive magnetic transitions at $T_{N1} =$ 19 K and $T_{N2} =$ 11.8 K indicating two distinct magnetically ordered phases. The single crystal neutron diffraction study shows that in the temperature ($T$) range 11.8 K $\le T \le$ 19 K the magnetic structure is commensurate with propagation vector $k_1 = (0, 0.5, 0)$, while upon lowering temperature below $T_{N2} =$ 11.8 K an incommensurate magnetic order emerges with $k_2 = (0.38, 0.48, 0.5)$ and the magnetic structure can be represented by cycloidal modulation of the Mn spin in $ac-$plane. We are reporting this commensurate to incommensurate transition for the first time. We discuss the role of the magnetic exchange interactions and spin-orbital coupling on the stability of the observed magnetic phase transitions.

cond-mat.str-el↗

First order valence transition: Neutron diffraction, inelastic neutron scattering and x-ray absorption investigations on the double perovskite Ba2PrRu0.9Ir0.1O6

Bulk studies have revealed a first-order valence phase transition in Ba$_2$PrRu$_{1-x}$Ir$_x$O$_6$ ($0.10 \le x \le 0.25$), which is absent in the parent compounds with $x = 0$ (Pr$^{3+}$) and $x =1$ (Pr$^{4+}$), which exhibit antiferromagnetic order with transition temperatures $T_{\rm N} = 120$ and 72 K, respectively. In the present study, we have used magnetization, heat capacity, neutron diffraction, inelastic neutron scattering and x-ray absorption measurements to investigate the nature of the Pr ion in $x =0.1$. The magnetic susceptibility and heat capacity of $x =0.1$ show a clear sign of the first order valence phase transition below 175 K, where the Pr valence changes from 3+ to 4+. Neutron diffraction analysis reveals that $x =0.1$ crystallizes in a monoclinic structure with space group $P2_1/n$ at 300 K, but below 175 K two phases coexist, the monoclinic having the Pr ion in a 3+ valence state and a cubic one ($Fm\overline{3}m$) having the Pr ion in a 4+ valence state. Clear evidence of an antiferromagnetic ordering of the Pr and Ru moments is found in the monoclinic phase of the $x = 0.1$ compound below 110 K in the neutron diffraction measurements. Meanwhile the cubic phase remains paramagnetic down to 2 K, a temperature below which heat capacity and susceptibility measurements reveal a ferromagnetic ordering. High energy inelastic neutron scattering data reveal well-defined high-energy magnetic excitations near 264 meV at temperatures below the valence transition. The high energy excitations are assigned to the Pr$^{4+}$ ions in the cubic phase and the low energy excitations to the Pr$^{3+}$ ions in the monoclinic phase. Further direct evidence of the Pr valence transition has been obtained from the x-ray absorption spectroscopy.

cond-mat.str-el↗

Magnetic states of Ni-Mn-Sn based shape memory alloy: a combined muon spin relaxation and neutron diffraction study

The fascinating multiple magnetic states observed in the Ni-Mn-Sn based metamagnetic shape memory alloy are addressed through a combined muon spin relaxation (muSR) and neutron powder diffraction studies. The material used in the present investigation is an off-stoichiometric alloy of nominal composition, Ni[2.04]Mn[1.4]Sn[0.56]. This prototypical alloy, similar to other members in the Ni-Mn-Sn series, orders ferromagnetically below T[CA] (= 320 K), and undergoes martensitic type structural transition at T[MS] (= 290 K), which is associated with the sudden loss of magnetization. The sample regains its magnetization below another magnetic transition at T[CM] = 260 K. Eventually, the composition shows a step-like anomaly at T[B] = 120 K, which is found to coincide with the blocking temperature of exchange bias effect observed in the alloy. In our study, the initial asymmetry A_[10] ) of the $μ$SR data falls rapidly below T[CA], indicating the onset of bulk magnetic order. A[10] regains its full asymmetry value below T[MS] suggesting the collapse of the ferromagnetic order into a fully disordered paramagnetic state. Below the second magnetic transition at T[CM], asymmetry drops again, confirming the re-entrance of a long range ordered state. Interestingly, A[10] increases sluggishly below T[B], indicating that the system attains a disordered/glassy magnetic phase below T[B], which is responsible for the exchange bias and frequency dispersion in the ac susceptibility data as previously reported. The neutron powder diffraction data do not show any magnetic superlattice reflections, ruling out the possibility of a long range antiferromagnetic state at low temperatures. The ground state is likely to be comprised of a concentrated metallic spin-glass in the backdrop of an ordered ferromagnetic state.

cond-mat.str-el↗

Magnetoelastic coupling and ferromagnetic-type in-gap spin excitations in multiferroic $α$-Cu$_2$V$_2$O$_7$

We investigate magnetoelectric coupling and low-energy magnetic excitations in multiferroic $α$-Cu$_2$V$_2$O$_7$ by detailed thermal expansion, magnetostriction, specific heat and magnetization measurements in magnetic fields up to 15~T and by high-field/high-frequency electron spin resonance studies. Our data show negative thermal expansion in the temperature range $\leq 200$~K under study. Well-developed anomalies associated with the onset of multiferroic order (canted antiferromagnetism with a significant magnetic moment and ferroelectricity) imply pronounced coupling to the structure. We detect anomalous entropy changes in the temperature regime up to $\sim 80$~K which significantly exceed the spin entropy. Failure of Grüneisen scaling further confirms that several dominant ordering phenomena are concomitantly driving the multiferroic order. By applying external magnetic fields, anomalies in the thermal expansion and in the magnetization are separated. Noteworthy, the data clearly imply the development of a canted magnetic moment at temperatures above the structural anomaly. Low-field magnetostriction supports the scenario of exchange-striction driven multiferroicity. We observe low-energy magnetic excitations well below the antiferromagnetic gap, i.e., a ferromagnetic-type resonance branch associated with the canted magnetic moment arising from Dzyaloshinsii-Moriya interactions. The anisotropy parameter $\tilde{D}=1.6(1)$~meV indicates a sizeable ratio of DM- and isotropic magnetic exchange.

cond-mat.str-el↗

Observation of non-Fermi liquid behavior in hole doped Eu2Ir2O7

The Weyl semimetallic compound Eu2Ir2O7 along with its hole doped derivatives (which is achieved by substituting trivalent Eu by divalent Sr) are investigated through transport, magnetic and calorimetric studies. The metal-insulator transition (MIT) temperature is found to get substantially reduced with hole doping and for 10% Sr doping the composition is metallic down to temperature as low as 5 K. These doped compounds are found to violate the Mott-Ioffe-Regel condition for minimum electrical conductivity and show distinct signature of non-Fermi liquid behavior at low temperature. The MIT in the doped compounds does not correlate with the magnetic transition point and Anderson-Mott type disorder induced localization may be attributed to the ground state insulating phase. The observed non-Fermi liquid behavior can be understood on the basis of disorder induced distribution of spin orbit coupling parameter which is markedly different in case of Ir4+ and Ir5+ ions.

cond-mat.str-el↗

Spin wave excitations in the pyrovanadate alpha-Cu2V2O7

The pyrovanadate alpha-Cu2V2O7 belongs to the orthorhombic (Fdd2) class of crystals with noncentrosymmetric crystal structure. Recently, the compound has been identified to be a magnetic multiferroic with a substantial electric polarization below the magnetic transition temperature TC = 35 K. Here we report the results of our inelastic neutron scattering (INS) studies on a polycrystalline sample of alpha-Cu2V2O7. Our INS data clearly show the existence of dispersive spin wave excitations below TC with a zone-boundary energy of 11 meV at 5 K.We have analyzed the data using linear spin wave theory, which shows good agreement between the experiment and calculation. The analysis is consistent with the third nearest neighbor exchange interaction playing a dominant role in the magnetism of the material.

cond-mat.str-el↗

Exchange striction induced giant ferroelectric polarization in copper based multiferroic material $α$-Cu$_2$V$_2$O$_7$

We report $α$-Cu$_2$V$_2$O$_7$ to be an improper multiferroic with the simultaneous development of electric polarization and magnetization below $T_C$ = 35 K. The observed spontaneous polarization of magnitude 0.55 $μ$Ccm$^{-2}$ is highest among the copper based improper multiferroic materials. Our study demonstrates sizable amount of magneto-electric coupling below $T_C$ even with a low magnetic field. The theoretical calculations based on density functional theory (DFT) indicate magnetism in $α$-Cu$_2$V$_2$O$_7$ is a consequence of {\em ferro-orbital} ordering driven by polar lattice distortion due to the unique pyramidal (CuO$_{5}$) environment of Cu. The spin orbit coupling (SOC) further stabilize orbital ordering and is crucial for magnetism. The calculations indicate that the origin of the giant ferroelectric polarization is primarily due to the symmetric exchange-striction mechanism and is corroborated by temperature dependent X-ray studies.

cond-mat.str-el↗

Two dimensional magnetic correlation in the unconventional corrugated layered oxides (Ba,Sr)$_4$Mn$_3$O$_{10}$

Both Ba$_4$Mn$_3$O$_{10}$ and Sr$_4$Mn$_3$O$_{10}$ crystallize in an orthorhombic crystal structure consisting of corrugated layers containing Mn$_3$O$_{12}$ polydedra. The thermal variation of magnetic susceptibility of the compositions consists of a broad hump like feature indicating the presence of low dimensional magnetic correlation. We have systematically investigated the magnetic data of these compounds and found that the experimental results match quite well with the two dimensional Heisenberg model of spin-spin interaction. The two dimensional nature of the magnetic spin-spin interaction is supported by the low temperature heat capacity data of Ba$_4$Mn$_3$O$_{10}$. Interestingly, both the samples show dielectric anomaly near the magnetic ordering temperature indicating multiferroic behavior.

cond-mat.str-el↗

Magnetic and electric properties of CaMn7O12 based multiferroic compounds: effect of electron doping

The mixed-valent multiferroic compound CaMn7O12 is studied for its magnetic and electric properties. The compound undergoes magnetic ordering below 90 K with a helimagnetic structure followed by a low temperature magnetic anomaly observed around 43 K. The present study shows that the magnetic anomaly at 43 K is associated with thermal hysteresis indicating first order nature of the transition. The compound also shows field-cooled magnetic memory and relaxation below 43 K, although no zero-field-cooled memory is present. Clear magnetic hysteresis loop is present in the magnetization versus field measurements signifying the presence of some ferromagnetic clusters in the system. We doped trivalent La at the cite of divalent Ca expecting to enhance the fraction of Mn$^{3+}$ ions. The La doped samples show reduced magnetization, although the temperatures associated with the magnetic anomalies remain almost unaltered. Interestingly, the spontaneous electrical polarization below 90 K increases drastically on La substitution. We propose that the ground state of the pure as well as the La doped compositions contain isolated superparamagnetic like clusters, which can give rise to metastability in the form of field-cooled memory and relaxation. The ground state is not certainly spin glass type as it is evident from the absence of zero-field-cooled memory and frequency shift in the ac suceptibility measurements.

cond-mat.str-el↗