arXiv subjects

Sitaram Ramakrishnan

Publications and source records attributed to Sitaram Ramakrishnan.

At least 19 recordsLinked to original sources

arXiv2026

Pressure-Driven Structural Transitions without a Displacive Charge-Density Wave in La$_2$SmNi$_2$O$_7$

We investigated the structural properties of bilayer nickelate La$_2$SmNi$_2$O$_7$ as a function of pressure and temperature. At ambient conditions, we show that the material crystallizes as a monoclinic superstructure distinct from the one previously reported and close to the pseudo-orthorhombic structure of pristine La$_3$Ni$_2$O$_7$. No signatures of satellite reflections associated with charge density wave (CDW) ordering are detected at low temperature. Upon compression, a sequence of pressure-induced structural transitions from monoclinic to orthorhombic 15 GPa and then tetragonal 21 GPa symmetry is observed. Within the superconducting dome, the quality of the X-ray diffraction data enables structural refinements enabling theoretical models to understand the emergence of superconductivity.

cond-mat.str-el↗

arXiv2025

Tracing the horizon of tetragonal-to-monoclinic distortion in pressurized trilayer nickelate La4Ni3O10

The crux of understanding the superconducting mechanism in pressurized Ruddlesden-Popper nickelates hinges on elucidating their structural phases. Under ambient conditions, the trilayer nickelate La4Ni3O10 stabilizes in a twinned monoclinic structure with space group P21/c. Upon heating, it undergoes a structural transition to the tetragonal I4/mmm phase at Ts ~ 1030 K, while a second transition associated with the onset of density-weave (DW) ordering emerges upon cooling below TDW ~ 135 K. Here from pressure-temperature x-ray diffraction on high quality flux-grown single crystals we demonstrate a direct tetragonal-to-monoclinic transition without an intermediate orthorhombic Bmab phase. Ab initio density-functional theory calculations as a function of pressure corroborate the experimental observations. The tetragonal-to-monoclinic transition unfolds as the formation of a two-fold superstructure, as evidenced by the emergence of commensurate superlattice reflections and can be progressively suppressed from 1030 K down to 20 K under 14 GPa. Notably, from XRD we establish the observation of weak incommensurate satellite reflections associated with the DW ordering in flux-grown samples, as previous findings were confined only to crystals grown by the floating-zone technique. This is further reinforced by Raman spectroscopy that reveal the emergence of additional phonon modes below 130 K, concomitant with the onset of the incommensurate DW state.

cond-mat.str-el↗

arXiv2025

Evidence of electronic instability driven structural distortion in the nodal line semimetal CoSn$_2$

Understanding the mechanisms that drive spontaneous rotational symmetry breaking in correlated electron systems is a central challenge in condensed matter physics. Although such symmetry breaking phases have been studied in low-dimensional and strongly correlated materials, its emergence in structurally simpler compounds remains less explored. Here, we investigate non-magnetic CoSn$_2$ that is a centrosymmetric intermetallic compound crystallizing in a tetragonal structure at ambient conditions, and discover an electronically driven symmetry breaking instability. Electrical resistivity reveals a distinct change in the slope below 25 K, deviating from the expected Bloch-Gr\"uneisen behavior. This anomaly is attributed towards a structural change as at 22 K single crystal X-ray diffraction using synchrotron radiation uncovers weak superlattice reflections that leads to a doubling of $\textbf{a}$ and $\textbf{c}$, resulting in a 4-fold superstructure. The symmetry of the lattice reduces from tetragonal to acentric monoclinic but without any discernible monoclinic distortion down to 10 K. This structural transition is accompanied by a twofold symmetry in angular magnetoresistance, contrasting the fourfold symmetry observed at higher temperatures. First-principles calculations show no phonon softening but reveal enhanced electronic susceptibility, suggesting an electronic instability. Polarization-dependent ARPES measurements further identify a strong orbital anisotropy dominated by the in-plane Co-$d_{xy}$ states. Collectively, our results point to an electronic instability driven structural distortion in CoSn$_2$, offering a rare platform to study symmetry breaking in a non-magnetic metallic system.

cond-mat.mtrl-sci↗

arXiv2025

An underdog story: Re-emergence of a polar instability at high pressure in KNbO3

Ferroelectricity in perovskites is known to be suppressed by a moderate hydrostatic pressure. The notion that a polar instability should reappear in a higher pressure regime is well accepted theoretically but experiments have failed so far to provide a conclusive evidence for it. Here, we investigate a classical but comparatively underlooked ferroelectric perovskite KNbO3. We use single crystal X-ray diffraction, infrared and Raman spectroscopy and second-harmonic generation to explore the phase transition sequence at high pressures up to 63 GPa. We show that the ferroelectric instability manifests itself in the emergence of an incommensurate modulation of the perovskite structure that combines cation displacements and tilts of the oxygen octahedra. Soft modes associated to the tilts and the modulation are clearly observed along with persistent order-disorder signatures. This demonstrates the presence of the high-pressure polar instability in a lead-free perovskite in spite of the centrosymmetric character of all observed high-pressure phases.

cond-mat.mtrl-sci↗

arXiv2025

Broken inversion symmetry in the charge density wave phase in EuAl$_4$

EuAl$_4$ exhibits a complex phase diagram, including the development of a charge density wave (CDW) below $T_{CDW} = 145$ K. Below $T_{N}=15.4$ K, a series of antiferromagnetically (AFM) ordered phases appear, while non-trivial topological phases, like skyrmion lattices, are stabilized under an applied magnetic field. The symmetries of the variously ordered phases are a major issue concerning the understanding of the stabilization of the ordered phases as well as concerning the interplay between the various types of order. EuAl$_4$ at room temperature has tetragonal symmetry with space group $I4/mmm$. The CDW phase has an incommensurately modulated crystal structure described by the modulation wave vector $\mathbf{q} \approx 0.17\mathbf{c}^{*}$. On the basis of various experiments, including elastic and inelastic x-ray scattering, and second-harmonic generation, it has been proposed that the symmetry of the CDW phase of EuAl$_4$ could be centrosymmetric orthorhombic, non-centrosymmetric orthorhombic or non-centrosymmetric tetragonal. Here, we report temperature-dependent, single-crystal x-ray diffraction experiments that show that the CDW is a transverse CDW with phason disorder, and with non-centrosymmetric symmetry according to the orthorhombic superspace group $F222(0\,0\,\sigma)00s$.Essential for this finding is the availability of a sufficient number of second-order ($2\mathbf{q}$) satellite reflections in the x-ray diffraction data set. The broken inversion symmetry implies that skyrmions might form due to Dzyaloshinskii-Moriya (DM) interactions, instead of a more exotic mechanism as it is required for centrosymmetric structures.

cond-mat.str-el↗

arXiv2025

Multilayer Crystal Field states from locally broken centrosymmetry

Local charge, spin, or orbital degrees of freedom with intersite interactions are oftentimes sufficient to construct most quantum orders. This is conventionally true for f-electron systems, where the extent of the f-electrons and their associated crystal-electric-field (CEF) states are strongly localized. Here, polarized Raman spectroscopy measurements of a locally non-centrosymmetric compound, CeCoSi, unveil more CEF excitations than expected in the local model. We interpret this as experimental evidence for the entanglement of CEF states between cerium layers. This composite sublattice, spin, and orbital degree of freedom provides an unconsidered means to form novel orders, not only in this system, but in any system exhibiting globally preserved yet locally broken centrosymmetry.

cond-mat.str-el↗

arXiv2025

Unveiling the interplay of magnetic order and electronic band structure on the evolution of anomalous Hall effect in MnPtGa single crystal

The recent studies on the anomalous Hall effect (AHE) have revealed an intrinsic relationship between the topological band structure and the experimentally observed transverse conductivity. Consequently, this has led to a heightened focus on examining the topological aspects of AHE. Here we have studied sign reversal of anomalous Hall conductivity with temperature in the single crystalline MnPtGa (space group: $P6_3/mmc$). From the interdependence of the linear resistance, we claim that the origin of such behavior is intrinsic. By systematically studying the electronic band structure and Berry curvature of MnPtGa using first principle calculations supported by magnetic susceptibility and isothermal magnetization measurements we demonstrate that the temperature dependent complex magnetic structure plays a significant role and leads to the sign reversal of anomalous Hall conductivity. We proposed a continuous evolution of the magnetic structure, supported by the ab initio calculations, which is consistent with the experimental data. Our studies have established that the critical temperature ($\approx$110 K), where the sign reversal appears is associated with the magnetic structure and the magnitude of Mn moments.

cond-mat.mtrl-sci↗

arXiv2024

Structural Evolution from Hyper-Honeycomb to Honeycomb Networks and Superconductivity in LaPt$_x$Si$_{2-x}$

We report the crystal structures and superconductivity (SC) of LaPt$_{x}$Si$_{2-x}$ ($0.5 \leq x \leq 1.0$) that are solid solutions of LaSi$_{2}$ and LaPtSi with centrosymmetric tetragonal ($I4_{1}/amd$, $D_{4h}^{19}$, \#141) and non-centrosymmetric tetragonal ($I4_{1}md$, $C_{4v}^{11}$, \#109) structures, respectively. It was found that at $0.86 \leq x \leq 1.00$, the non-centrosymmetric tetragonal symmetry is preserved, while partial disorder appears in alternating Pt and Si of the hyper-honeycomb network. The superconducting transition temperature $T_{\rm c}$ was drastically reduced from 3.9 K to 1.5 K as $x$ varies from 1.0 to 0.86. Additionally, a hexagonal phase with an AlB$_{2}$-type structure ($P6/mmm$, $D_{6h}^{1}$, \#191) has been discovered at $0.50 \leq x \leq 0.71$ with a honeycomb network of statistically distributed Pt and Si atoms. The hexagonal phase exhibited SC at $T_{\rm c} = 0.38$ K. This system provides an opportunity to investigate the relationship between topological electronic states, SC, and disorders

cond-mat.supr-con↗

arXiv2024

I-centered vs F-centered orthorhombic symmetry and negative thermal expansion of the charge density wave of EuAl2Ga2

Together with EuGa4 and EuAl4, EuAl2Ga2 belongs to the BaAl4 structure type with space group symmetry I4/mmm. EuAl2Ga2 develops an incommensurate charge density wave (CDW) at temperatures below TCDW = 51 K. On the basis of temperature dependent single-crystal X-ray diffraction (SXRD) data, the incommensurately modulated CDW crystal structure of EuAl2Ga2 is determined to possess orthorhombic superspace symmetry Immm(00g)s00. This symmetry is different from the orthorhombic Fmmm based symmetry of the CDW state of EuAl4. Nevertheless, both symmetries Immm(00g)s00 and Fmmm(00g)s00 lead to the same conclusion, that the CDW is supported by the layers of Al1 type atoms, while the Eu and Al2 or Ga atoms are not directly involved in CDW formation. The different symmetries of the CDW states of EuAl4 and EuAl2Ga2, as well as the observation of negative thermal expansion in the CDW state of EuAl2Ga2 might be explained by the effects of Ga substitution in the latter compound.

cond-mat.str-el↗

arXiv2024

Atypical antiferromagnetic ordering in single crystalline quasi-2D honeycomb magnet YbI$_3$

Here, we study YbI$_3$, a quasi-2D layered material with Yb atoms arranged on an ideal honeycomb network of edge-sharing YbI$_6$ octahedra, analogous to the low-temperature phase of $α-$RuCl$_3$. High quality single crystals of YbI$_3$ are grown from Yb and I as starting precursors, using the vapor transport technique. The grown crystals are characterized by single crystal x-ray diffraction, Raman spectroscopy, magnetization, and heat capacity probes. The crystal-field split ground state of Yb$^{3+}$ in \Yb~ is a well-isolated Kramers doublet with an effective moment $\rm J_{eff} = 1/2$. Upon cooling, the low-temperature heat capacity of \Yb~ reveals a broad peak at $\rm T_1 = 0.95$~K due to short-range ordering of the Yb moments, followed by a sharp peak at $\rm T_2 = T_N = 0.6$~K due to long-range ordering. The magnetic behavior is found to be weakly anisotropic with $χ^\parallel > χ^\perp$, where $χ^\parallel$ and $χ^\perp$ refers to the in-plane ($H \parallel ab$) and out-of-plane ($H \perp ab$) susceptibilities. The 2~K isothermal magnetization saturates at $\rm \approx~1.5~μ_B/Yb^{3+}$ (in-plane) and $\rm \approx~1~μ_B/Yb^{3+}$ (out-of-plane), suggesting the anisotropy to be easy-plane type. Low-temperature heat capacity, well below T$_N$, is found to vary as T$^α$ with $α~\approx~2.5$, indicating a possible unconventional magnetic ground state for YbI$_3$.

cond-mat.str-el↗

arXiv2024

Room temperature charge density wave in a tetragonal polymorph of Gd2Os3Si5 and study of its origin in the RE2T3X5 (RE = Rare earth, T = transition metal, X = Si, Ge) series

Charge density wave (CDW) systems are proposed to exhibit application potential for electronic and optoelectronic devices. Therefore, identifying new materials that exhibit a CDW state at room temperature is crucial for the development of CDW-based devices. Here, we present a non-layered tetragonal polymorph of Gd2Os3Si5, which exhibits a CDW state at room temperature. Gd2Os3Si5 crystallizes in the U2Mn3Si5-type tetragonal crystal structure with the space group P4/mnc. Single-crystal x-ray diffraction (SXRD) analysis shows that Gd2Os3Si5 possesses an incommensurately modulated structure with modulation wave vector q = (0.53, 0, 0), while the modulation reduces the symmetry to orthorhombic Cccm(σ00)0s0. This differs in contrast to isostructural Sm2Ru3Ge5, where the modulated phase has been reported to possess the superspace symmetry Pm(α 0 γ)0. However, reinvestigation of Sm2Ru3Ge5 suggests that its modulated crystal structure can alternatively be described by Cccm(σ00)0s0, with modulations similar to Gd2Os3Si5. The magnetic susceptibility, \c{hi}(T), exhibits a maximum at low temperatures that indicates an antiferromagnetic transition at TN = 5.5 K. The \c{hi}(T) furthermore shows an anomaly at around 345 K, suggesting a CDW transition at TCDW = 345 K, that corroborates the result from high-temperature SXRD measurements. Interestingly, R2T3X5 compounds are known to crystallize either in the tetragonal Sc2Fe3Si5 type structure or in the orthorhombic U2Co3Si5 structure type. Not all of the compounds in the R2T3X5 series undergo CDW phase transitions. We find that R2T3X5 compounds will exhibit a CDW transition, if the condition : 0.526 < c/sqrt(ab) < 0.543 is satisfied. We suggest the wave vector-dependent electron-phonon coupling to be the dominant mechanism of CDW formation in the tetragonal polymorph of Gd2Os3Si5.

cond-mat.str-el↗

arXiv2024

Charge density wave with suppressed long-range structural modulation in canted antiferromagnetic kagome FeGe

Kagome lattice can host abundant exotic quantum states such as superconductivity and charge density wave (CDW). Recently, successive orders of A-type antiferromagnetism (AFM), CDW and canted AFM have been manifested upon cooling in kagome FeGe. However, the mechanism of CDW and interaction with magnetism remains unclear. Here we investigate the evolution of CDW with temperature across the canted AFM by single-crystal x-ray diffraction, scanning tunneling microscope (STM) and resonant elastic x-ray scattering (REXS). Interestingly, CDW-induced superlattice reflections become weak after the canted AFM, although long-range CDW order is still detectable by STM and REXS. We uncover a novel long-range CDW order with suppressed structural modulation, likely due to the competition for the underlying crystal structure between CDW and canted AFM. Additionally, occupational modulations of Ge1 in the kagome plane and displacive modulations of all atoms were extracted. The results confirm Ge dimerization along the c axis and suggest a dynamic transformation between different CDW domains.

cond-mat.str-el↗

arXiv2024

Non-centrosymmetric, transverse structural modulation in SrAl4, and elucidation of its origin in the BaAl4 family of compounds

At ambient conditions SrAl4 adopts the BaAl4 structure type with space group I4/mmm. It undergoes a charge-density-wave (CDW) transition at TCDW = 243 K, followed by a structural transition at TS = 87 K. Temperature-dependent single-crystal X-ray diffraction (SXRD) leads to the observation of incommensurate superlattice reflections at q = σc* with σ= 0.1116 at 200 K. The CDW has orthorhombic symmetry with the acentric superspace group F222(00sigma)00s, where F222 is a subgroup of Fmmm as well as of I4/mmm. Atomic displacements mainly represent a transverse wave, with displacements that are 90 deg out of phase between the two diagonal directions of the I-centered unit cell, resulting in a helical wave. Small longitudinal displacements are provided by the second harmonic modulation. The orthorhombic phase realized in SrAl4 is similar to that found in EuAl4. Electronic structure calculations and phonon calculations by density functional theory (DFT) have failed to reveal the mechanism of CDW formation. However, DFT reveals that Al atoms dominate the density of states near the Fermi level, thus, corroborating the SXRD measurements. SrAl4 remains incommensurately modulated at the structural transition, where the symmetry lowers from orthorhombic to b-unique monoclinic. We have identified a simple criterion, that correlates the presence of a phase transition with the interatomic distances. Only those compounds XAl4-xGax(X = Ba, Eu, Sr, Ca; 0 < x <4) undergo phase transitions, for which the ratio c/a falls within the narrow range 2.51 < c/a < 2.54.

cond-mat.str-el↗

arXiv2023

Annealing-induced long-range charge density wave order in magnetic kagome FeGe: fluctuations and disordered structure

Charge density wave (CDW) in kagome materials with the geometric frustration is able to carry unconventional characteristics. Recently, a CDW has been observed below the antiferromagnetic order in kagome FeGe, in which magnetism and CDW are intertwined to form an emergent quantum ground state. However, the CDW is only short-ranged and the structural modulation originating from it has yet to be determined experimentally. Here we realize a long-range CDW order by post-annealing process, and resolve the structure model through single crystal x-ray diffraction. Occupational disorder of Ge resulting from short-range CDW correlations above $T_\mathrm{CDW}$ is identified from structure refinements. The partial dimerization of Ge along the $c$ axis is unveiled to be the dominant distortion for the CDW. Occupational disorder of Ge is also proved to exist in the CDW phase due to the random selection of partially dimerized Ge sites. Our work provides useful insights for understanding the unconventional nature of the CDW in FeGe.

cond-mat.str-el↗

arXiv2023

Enhancement of density of states and suppression of superconductivity in site-disordered topological metal LaPtSi

Single crystals of non-centrosymmetric $s$-wave superconductor LaPt$_{0.88}$Si$_{1.12}$ have been grown by the Czochralski (Cz) technique, whose crystal structure is described by the space group $I4{_1}md$ at ambient conditions. The inter-site mixing between platinum and silicon is confirmed by both single-crystal x-ray diffraction (SXRD) and electron probe micro-analyzer (EPMA). The disordered material exhibits a lower superconducting (SC) transition temperature $T_c$ at 2.02 K as opposed to the highest value of 3.9 K reported in polycrystalline LaPtSi without inter-site mixing. From specific heat, the Sommerfeld coefficient ($γ$) is estimated to be 7.85 mJ/mol K$^2$, which is much larger than the values reported for the samples exhibiting higher $T_c$. This is unprecedented as $T_c$ seems to decrease with increase in the electron density of states (DOS) at the Fermi energy and thus $γ$. The present work reports on the anomalous behaviour of SC and normal state properties of LaPt$_{x}$Si$_{2-x}$, presumably caused due to the existence of non-trivial topological bands.

cond-mat.supr-con↗

arXiv2023

Realization of Z$_2$ Topological Metal in Single-Crystalline Nickel Deficient NiV$_2$Se$_4$

Temperature-dependent electronic and magnetic properties are reported for a Z2 topological metal single-crystalline nickel-deficient NiV$_2$Se$_4$. It is found to crystallize in the monoclinic Cr3S4 structure type with space group I2=m. From single-crystal x-ray diffraction, we find that there are vacancies on the Ni site, resulting in the composition Ni0:85V2Se4 in agreement with our electron-probe microanalysis. The electrical resistivity shows metallic behavior with a broad anomaly around 150{200 K that is also observed in the heat capacity data. This anomaly indicates a change of state of the material below 150 K. We believe that this anomaly could be due to spin fluctuations or charge-density-wave (CDW) fluctuations, where the lack of long-range order is caused by vacancies at the Ni site of Ni0:85V2Se4. Although we fail to observe any structural distortion in this crystal down to 1.5 K, its electronic and thermal properties are anomalous. The observation of non-linear temperature dependence of resistivity as well as an enhanced value of the Sommerfeld coefficient = 104.0(1) mJ/molK2 suggests strong electron-electron correlations in this material. The first-principles calculations performed for NiV$_2$Se$_4$, which are also applicable to Ni0:85V2Se4, classify this material as a topological metal with Z2 = (1; 110) and coexisting electron and hole pockets at the Fermi level. The phonon spectrum lacks any soft phonon mode, consistent with the absence of periodic lattice distortion in the present experiments.

cond-mat.str-el↗

arXiv2022

Fragile electronic superconductivity in Bi Single crystal

It was presumed that semimetal Bismuth (Bi) would not show superconductivity (SC) even at ultra-low temperatures ($<$10 mK) due to its very low carrier density ($\approx 3\times10^{17}$cm$^{-3}$). Recently, we have established bulk superconductivity in ultra-pure (99.9999\%) Bi single crystal at $\mathrm{T_C = 0.53}$ mK with an extrapolated upper critical field $\mathrm{H_C(0) = 5.2μ}$T measured along the [$0001$] (trigonal) -crystallographic direction. At very low concentrations of the charge carriers, we are dealing with fragile Cooper pairs with an estimated large coherence length $\mathrm{ξ_{GL}(0)\approx 96 μ}$m. We also stated that one needs to go beyond the conventional electron-phonon coupling (BCS-like) mechanism to understand the SC state in Bi. Bi is a compensated semi-metal with electrons and holes as charge carriers. In order to find the charge carriers responsible for the SC, we report the temperature dependence of the anisotropic critical field along the [$01\bar 10$] (bisectrix)-crystallographic direction and compared it with the earlier data from measurements along the trigonal. Our theoretical analysis of the anisotropy of critical fields suggests that the light electrons in the three pockets of Bi bands are responsible for the SC and indicates that Bi is an extremely weak type-II (close to type-I) superconductor. Finally, we review the current theories proposed to explain the SC in Bi.

cond-mat.supr-con↗

arXiv2022

Coupling between colossal charge density wave ordering and magnetism in Ho2Ir3Si5

Ho2Ir3Si5 belongs to the family of three-dimensional (3D) R2Ir3Si5 (R = Lu, Er and Ho) compounds that exhibit a colossal first-order charge density wave (CDW) transition where there is a strong orthorhombic-to-triclinic distortion of the lattice accompanied by superlattice reflections. The analysis by single-crystal X-ray diffraction (SXRD) has revealed that the Ir-Ir zigzag chains along c are responsible for the CDW in all three compounds. The replacement of the rare earth element from non-magnetic Lu to magnetic Er or Ho lowers TCDW, where TCDWLu = 200 K, TCDWEr = 150 K and TCDWHo = 90 K. Out of the three compounds, Ho2Ir3Si5 is the only system where second-order superlattice reflections could be observed, indicative of an anharmonic shape of the modulation wave. The CDW transition is observed as anomalies in the temperature dependencies of the specific heat, electrical conductivity and magnetic susceptibility, which includes a large hysteresis of 90 to 130 K for all measured properties, thus corroborating the SXRD measurements. Similar to previously reported Er2Ir3Si5, there appears to be a coupling between CDW and magnetism such that the Ho3+ magnetic moments are influenced by the CDW transition, even in the paramagnetic state. Moreover, earlier investigations on polycrystalline material revealed antiferromagnetic (AFM) ordering at TN = 5.1 K, whereas AFM order is suppressed and only the CDW is present in our highly ordered single-crystal. First-principles calculations predict Ho2Ir3Si5 to be a metal with coexisting electron and hole pockets at the Fermi level. The Ho and Ir atoms have spherically symmetric metallic-type charge density distributions that are prone to CDW distortion. Phonon calculations affirm that the Ir atoms are primarily responsible for the CDW distortion, which is in agreement with the experiment.

cond-mat.str-el↗