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Sudipta Chatterjee

Publications and source records attributed to Sudipta Chatterjee.

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New Superconductors in the PtPb$_3$Bi Structure Type

The quest for new superconductors is of both fundamental and technological importance. Recently, an artificial intelligence method correctly predicted PtPb$_3$Bi to be a superconductor. In this work, we find superconductivity in the newly synthesized $M$Pb$_{4-x}$Bi$_x$ ($M$ = Au, Pd, and Rh), of which PtPb$_3$Bi is a member. When $M$ = Ni, whose radius is considerably smaller, the structure instead collapses into the different, Pb-substituted NiBi$_3$ type. Interestingly, the stoichiometric parameter $x$ shifts across the three compounds to keep the total valence electron count close to 20 per formula unit. The superconducting transitions occur at 4.9, 4.2, and 3.4 K, for $M$ = Au, Pd, and Rh, respectively. Using electrical resistivity, magnetization, and specific heat measurements, we establish the bulk nature of the superconducting state and determine the critical fields, characteristic length scales, and anisotropy ratios. All three compounds are moderately anisotropic type-II superconductors, with modest upper critical field anisotropies of $H_{c2}^{\parallel c}/H_{c2}^{\perp c} \approx 1.2$ to $1.5$. These results establish $M$Pb$_{4-x}$Bi$_x$ as a family of anisotropic superconductors and a platform for studying how site disorder and Pb-Bi mixing govern superconductivity in heavy-element intermetallics.

cond-mat.supr-con

Tunable magnetotransport through kinetically hindered first-order phase transitions in an antiferromagnetic metal

Controllable multilevel resistance states are of interest for memory technologies like neuromorphic computing, but robust materials platforms toward such behavior remain limited. Here, we show that the non-centrosymmetric antiferromagnetic metal CeCoGe$_3$ suggests one such route through a kinetically hindered first-order magnetic transition. Cooling through the kinetically hindered first-order transition in an applied magnetic field produces a magnetic glass state in which high- and low-temperature magnetic phases coexist. The relative fraction of these phases can be controlled by the applied field in which the sample is cooled, and the electrical resistance is directly sensitive to that fraction. As a result, it is demonstrated that CeCoGe$_3$ supports stable multilevel resistive states. These results identify kinetically hindered first-order phase transitions as a promising route towards controllable multilevel magnetoresistive states.

cond-mat.str-el

Stripping Symmetry: Electrochemical Oxidation to a Superconducting Polar Metal in Au2Pb0.914P2

Polar metals and noncentrosymmetric superconductors are exceptionally rare, yet their broken inversion symmetry can give rise to emergent electronic phenomena including mixed singlet-triplet superconducting pairing. As only a few such materials have been found among known compounds, accessing new examples requires synthetic strategies that go beyond conventional crystal growth. Here, we use electrochemical topotactic deintercalation to remove Pb from the centrosymmetric parent compound Au$_2$PbP$_2$, producing the polar metal Au$_2$Pb$_{0.914}$P$_2$. Unlike conventional chemical doping, this transformation actively drives structural symmetry-breaking: the partial removal of Pb triggers a cooperative electronic and geometric rearrangement, mediated by a second-order Jahn-Teller effect and stereochemically active lone pairs, that locks the product into a polar, noncentrosymmetric superspace group Ama2(01g)ss0. We solve the complete (3+1)D modulated structure by synchrotron single-crystal X-ray diffraction and confirm the polar assignment through nonlinear electronic transport. Below T$_c$ = 1.52 K, Au$_2$Pb$_{0.914}$P$_2$ becomes a type-II superconductor whose heat capacity and AC susceptibility both exhibit power-law behavior, suggestive of a gap structure governed by the broken inversion symmetry of the host lattice. This work establishes electrochemical oxidation as a rational route to metastable noncentrosymmetric superconductors through chemically directed symmetry-breaking.

cond-mat.supr-con

Spin-reorientation as a switch for electronic topology in van der Waals ferromagnets

The interplay between spin reorientation and topological electronic structure in two-dimensional (2D) van der Waals (vdW) ferromagnets is central to understanding how magnetic anisotropy shapes charge transport. Although spin-reorientation transitions (SRTs) are common in 2D metallic ferromagnets, their impact on electronic-topology-driven thermodynamic and transport properties remains largely unexplored. Here we investigate this issue in Fe$_4$GeTe$_2$ (F4GT), a room-temperature quasi-2D vdW ferromagnet, using temperature-dependent magnetization, specific heat, magnetotransport, and thermoelectric measurements. Magnetization and specific heat establish a reorientation of the magnetic easy axis near $T_{\mathrm{SRT}} \sim 100$~K, in addition to ferromagnetic ordering at $T_C \sim 270$~K. Across the SRT, the Seebeck coefficient and anisotropic magnetoresistance show clear anomalies, indicating Fermi-surface reconstruction. The magnetoresistance exhibits a two-step field dependence: a low-field enhancement near the SRT associated with scattering from canted spins and evolving domains, followed by a higher-field negative response as spin fluctuations are suppressed. The simultaneous sign change of the ordinary Hall coefficient $R_0$ and the sharp anomaly in the anomalous Hall resistivity $\rho^{A}_{yx}$ further point to a temperature-driven modification of the underlying band topology. Analysis of the anomalous Hall conductivity $\sigma^{A}_{xy}$ and the scaling of $\rho^{A}_{yx}$ shows that the Berry-curvature-driven anomalous Hall response below $T_{\mathrm{SRT}}$ is strongly modified above the transition. Our results identify spin reorientation as an internal control parameter for switching between distinct topological transport regimes in a 2D vdW ferromagnet, providing a symmetry-controlled route to engineer spin-polarized electronic states and domain-texture-driven functionalities.

cond-mat.str-el

Collinear spin density wave state in distorted square-lattice GdNiSn$_4$

We characterize the magnetic ground state of the newly synthesized lanthanide intermetallic GdNiSn$_4$ via resonant elastic x-ray scattering measurements. This compound forms distorted square nets of Gd that initially order magnetically below 23 K followed by a lower temperature transition at 16 K. Our scattering data identify the ground state order as a single-$q$ incommensurate, collinear order that slides towards a commensurate wave vector above the 16 K transition. Magnetic symmetry analysis combined with azimuthal dependence resolves the ground state magnetic structure as a moment-modulated spin density wave state with Gd moments oriented parallel to the in-plane a-axis. We discuss connections between the observed magnetic order and electronic properties in this square-net compound.

cond-mat.str-el

New Crystal Structures Hide in Plain Sight: A Stress Test for AI-Guided Materials Discovery

New types of crystal structures are discovered only rarely, and the artificial intelligence (AI) models now reshaping materials discovery have so far produced new chemical compositions within known structural families rather than genuinely new structures. We report GdNiSn4 and LuNiSn4, intermetallics that adopt a previously unreported structure type, found not by computation but by exploratory synthesis. Single-crystal diffraction shows that the structure is an intergrowth of two known structural units. We then use this system as a benchmark for two leading generative models, MatterGen and DiffCSP++. For DiffCSP++, the benchmark is performed in its crystallographically constrained setting, using the required space-group and Wyckoff-position inputs. Under our sampling budget, neither model recovers the experimentally reported monoclinic structure within the structural-matching tolerance. The generated structures are evaluated without further structural relaxation using the nonmagnetic analog LuNiSn4, where we rule out 4f magnetism as the cause. Because the new structure is built from familiar building blocks, it should be derivable. We argue that encoding chemical reasoning, such as the stacking of known motifs, is a concrete path toward AI that can discover structurally novel materials.

cond-mat.mtrl-sci

Measuring the Hall effect in hysteretic materials

Measurement of the Hall effect is a ubiquitous probe for materials discovery, characterization, and metrology. Inherent to the Hall measurement geometry, the measured signal is often contaminated by unwanted contributions, so the data must be processed to isolate the Hall response. The standard approach invokes Onsager-Casimir reciprocity and antisymmetrizes the raw signal about zero applied magnetic field. In hysteretic materials this becomes nontrivial, since Onsager-Casimir relations apply only to microscopically reversible states. Incorrect antisymmetrization can lead to artifacts that mimic anomalous or topological Hall signatures. The situation is especially subtle when hysteresis loops are not centered at zero applied field, as in exchange-biased systems. A practical reference for generically extracting the Hall response in hysteretic materials is lacking. Here, using Co$_3$Sn$_2$S$_2$ as a bulk single-crystal model that can be prepared with or without exchange-biased hysteresis, we demonstrate two procedures that can be used to extract the Hall effect: (1) reverse-magnetic-field reciprocity and (2) antisymmetrization with respect to applied field. We then measure the Hall effect on CeCoGe$_3$, a noncentrosymmetric antiferromagnet which can be prepared to have asymmetric magnetization and magnetoresistance, and demonstrate how improper processing can generate artificial anomalous Hall signals. These methods are generic and can be applied to any conductor.

cond-mat.str-el

Emergence of a hidden-order phase well below the charge density wave transition in a topological Weyl semimetal (TaSe$_4$)$_2$I

The emergence of a charge density wave (CDW) in a Weyl semimetal -- a correlated topological phase, is exceptionally rare in condensed matter systems. In this context, the quasi-one-dimensional type-III Weyl semimetal (TaSe$_4$)$_2$I undergoes a CDW transition at $T_{\mathrm{CDW}} \approx 263$~K, providing an exceptional platform to investigate correlated topological CDW states. Here, we uncover an additional hidden-order phase transition at $T^* \sim 100$ K, well below the CDW onset, using low-frequency resistance noise spectroscopy, electrical transport, and thermoelectric measurements. This transition is characterized by a sharp enhancement in the noise exponent ($\alpha$) and variance of resistance fluctuations. Analysis of higher-order statistics of resistance fluctuations reveals the correlated dynamics underlying the transition. A pronounced anomaly in the Seebeck coefficient near $T^*$ further suggests a Fermi surface reconstruction. First-principles calculations reveal a structural distortion from the high-symmetry $I422$ phase to a low-symmetry $C2$ phase, via an intermediate $I4$ symmetry. This leads to renormalization of the electronic structure near the Fermi level and opening of a bandgap in the hidden-order phase. These findings demonstrate a previously unidentified correlated phase transition in the topological CDW-Weyl semimetal (TaSe$_4$)$_2$I, enriching the phase diagram of this material and establishing it as an ideal platform for studying intertwined electronic and structural orders.

cond-mat.str-el

Electron-affinity difference distributions as an organizing principle for superconductivity, enabling the discovery of PtPb$_3$Bi

Predicting the superconducting transition temperature ($T_c$) from crystal structure and composition remains a central challenge in condensed-matter physics, reflecting the absence of a broadly predictive framework connecting microscopic bonding to macroscopic quantum behavior. Here, we introduce $\mathcal{GP}$-$T_c$, an interpretable, structure- and chemistry-aware Gaussian process model that enables uncertainty-quantified $T_c$ prediction from experimentally accessible inputs. By encoding local bonding environments as graphlet histograms, we find that the predictive space collapses to a compact set of descriptors: the distribution of electron-affinity (EA) differences between neighboring atoms, together with interatomic distances and simple elemental features, suffices to predict $T_c$ across disparate superconducting families---identifying an overlooked chemical control parameter that underscores the essential role of local structure beyond composition-only approaches. Our results demonstrate that the EA differences serves as an accessible window into electronic structure providing a mechanism-agnostic physical basis that captures $T_c$ across conventional and unconventional families, including doped charge transfer insulators. $\mathcal{GP}$-$T_c$ reproduces the experimentally reported $T_c$ range of the infinite-layer nickelate Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, and we predict and experimentally confirm superconductivity in stoichiometric PtPb$_3$Bi ($T_c \approx 3$~K). To facilitate broad community use, $\mathcal{GP}$-$T_c$ is made available through a web interface for crystal-structure-based prediction, and the same framework identifies additional high-priority superconducting candidates---including SrNiO$_2$ and K(PRh)$_2$---that provide concrete targets for ongoing and future experimental exploration.

cond-mat.supr-con

Signatures of emergent surface states across a displacive topological phase transition in Bi$_4$I$_4$

Topological phase transitions involving crystalline symmetry breaking provide a fertile ground to explore the interplay between symmetry, topology, and emergent quantum phenomena. Recently discovered quasi-one-dimensional topological material, Bi$_4$I$_4$, has been predicted to host topologically non-trivial gapless surfaces at high temperature, which undergo a finite temperature phase transition to a low temperature gapped phase. Here we present experimental signatures of this room temperature phase transition from a high-temperature $\beta$-phase with a surface state to a gapped $\alpha$-phase hosting hinge states. Using real-space current mapping and resistance fluctuation spectroscopy, we identify signatures of a displacive topological phase transition mediated by a first-order thermodynamic structural change. Near the emergence of $\beta$-phase, we observe pronounced telegraphic noise, indicating fluctuating phase domains with topological surface states. The spatially resolved current map reveals electron transport via the gapless surface states in the $\beta$-phase, which vanishes upon transitioning to the $\alpha$-phase with localized conduction channels (or hinge modes). Our experimental results, supported by first principles estimates and effective theory of a topological displacive phase transition, establish Bi$_4$I$_4$ as a candidate material showing intricate interplay of classical thermodynamic phase transitions with topological quantum phenomena.

cond-mat.str-el

Accessing quasi-flat $\textit{f}$-bands to harvest large Berry curvature in NdGaSi

In typical rare-earth lanthanide compounds, the localized 4\textit{f}-electrons have a weak effect on the electrical conduction, limiting their influence on the Berry curvature and, hence, the intrinsic anomalous Hall effect. A comprehensive study of the magnetic, thermodynamic, and transport properties of single-crystalline NdGaSi, guided by first-principles calculations, reveals a ferromagnetic ground state that induces a splitting of quasi-flat 4\textit{f} electronic bands and positions them near the Fermi energy. The observation of an extraordinarily large intrinsic anomalous Hall conductivity of 1165 $\Omega^{-1}$ cm$^{-1}$ implies the direct involvement of localized states in the generation of non-trivial band crossings around the Fermi energy. The angle-resolved photoemission spectroscopy measurements provide direct evidence of non-trivial crossing of the 4\textit{f}-bands with dispersive bands. These results are remarkable when compared to ferrimagnetic NdAlSi, which differs only in a non-magnetic atom (a change in the principal quantum number \textit{n} of the outer \textit{p }orbital) with the same number of valence electrons and does not exhibit any measurable anomalous Hall conductivity.

cond-mat.mtrl-sci

Directionally Locked Heteroepitaxy with a Structurally Modulated van der Waals Material

Precise orientation of symmetry-mismatched epilayers on van der Waals (vdW) substrates via heteroepitaxy has commonly been achieved through surface treatment processes to accommodate weak interlayer registry and bonding strength, thereby limiting the range of material combinations for heterostructure design. In this study, we investigate the influence of lattice instabilities in a structurally modulated vdW TaCo2Te2 substrate on the growth and alignment of a symmetry-mismatched bulk CoxTey epilayer using in situ heating in a transmission electron microscope (TEM). We show that a Peierls-like lattice instability occurs in TaCo2Te2 at a transition temperature of ~523 K, which was corroborated by phonon calculations. Post-heat-treated samples reveal a thermally induced surface diffusion process and the dominant lateral growth of the CoxTey epilayer on the TaCo2Te2 vdW layers, as observed in cross-sectional TEM images. Temperature-dependent selected area electron diffraction (SAED) patterns reveal that the quasi-vdW CoxTey/TaCo2Te2 heterointerface acquires directional locking by aligning larger interlayer lattice mismatch along the lattice instability axis of TaCo2Te2, while preserving a strong lattice matching along the orthogonal direction. This heterostructure exhibits precise interlayer registry with one-dimensional lattice incommensuration along the lattice instability axis, resulting from structural distortion to accommodate lattice-mismatch strain. Moreover, the interfacial reconstruction of TaCo2Te2 back to the distorted phase stabilizes the lattice-locking of the quasi-vdW heterointerface at elevated temperatures. These findings encourage the expansion of material diversity for designing and predicting novel multi-dimensional heterostructures by leveraging lattice instabilities to guide epitaxy.

cond-mat.mtrl-sci

Giant anisotropic anomalous Hall effect in antiferromagnetic topological metal NdGaSi

The interplay between magnetism and strong electron correlation in magnetic materials discerns a variety of intriguing topological features. Here, we report a systematic investigation of the magnetic, thermodynamic, and electrical transport properties in NdGaSi single crystals. The magnetic measurements reveal a magnetic ordering below T_N (11 K), with spins aligning antiferromagnetically in-plane, and it orders ferromagnetically (FM) out-of-plane. The longitudinal resistivity data and heat capacity exhibit a significant anomaly as a consequence of the magnetic ordering at TN. The magnetoresistance study shows significantly different behavior when measured along either direction, resulting from the complex nature of the magnetic structure, stemming from complete saturation of moments in one direction and subsequent spin flop transitions in the other. Remarkably, we have also noticed an unusual anisotropic anomalous Hall response. We have observed a giant anomalous Hall conductivity (AHC) of 1730 ohm-1 cm-1 and 490 ohm-1 cm-1 at 2 K, with B // [001] and B // [100], respectively. Our scaling analysis of AHC reveals that the anomalous Hall effect in the studied compound is dominated by the Berry phase-driven intrinsic mechanism. These astonishing findings in NdGaSi open up new possibilities for antiferromagnetic spintronics in rare-earth-based intermetallic compounds.

cond-mat.mes-hall

Barrier height inhomogeneity and origin of 1/f-noise in topological insulator-based photo-detector

Topological insulators (TIs) with symmetry-protected surface states, offer exciting opportunities for next-generation photonic and optoelectronic device applications. The heterojunctions of TIs and semiconductors (e.g. Si, Ge) have been observed to excellent photo-responsive characteristics. However, the realization of high-frequency operations in these heterojunctions can be hindered by unwanted 1/f (or Flicker) noise and phase noise. Therefore, an in-depth understanding of 1/f noise figures becomes paramount for the effective utilization of such materials.Here we report optoelectronic response and 1/f noise characteristics of a p-n diode fabricated using topological insulator, Bi2Se3 and silicon for potential photo-detector. Through meticulous temperature-dependent current-voltage (I-V) and capacitance-voltage (C-V) measurements, we ascertain crucial parameters like barrier height, ideality factor, and reverse saturation current of the photodetector. The low-frequency 1/f conductance noise spectra suggest a significant presence of trap states influencing the optoelectronic transport properties. The forward noise characteristics exhibit typical 1/f features, having a uni-slope across four decades of frequency, suggesting a homogeneous distribution of barrier height. The spectral and photocurrent-dependent responses show the power law behavior of noise level on photon flux. The hybrid heterojunction demonstrates excellent photo-response and reasonably low noise level, promising signatures for the room-temperature visible photodetector applications.

cond-mat.str-el

Anomalous Hall effect induced by Berry curvature in topological nodal-line van der Waals ferromagnet Fe$_4$GeTe$_2$

The exploration of nontrivial transport phenomena associated with the interplay between magnetic order and spin-orbit coupling (SOC), particularly in van der Waals (vdW) systems has gained a resurgence of interest due to their easy exfoliation, ideal for two-dimensional (2D) spintronics. We report the near room temperature quasi-2D ferromagnet, Fe$_4$GeTe$_2$ from the iron-based vdW family (Fe$_n$GeTe$_2$, $n$=3,4,5), exhibiting a large anomalous Hall conductivity (AHC), $\sigma^A_{xy}$ $\sim$ 490 $\Omega^{-1}\textrm{cm}^{-1}$ at 2 K. The near quadratic behavior of anomalous Hall resistivity ($\rho^{A}_{xy}$) with the longitudinal resistivity ($\rho_{xx}$) suggests that a dominant AHC contribution is coming from an intrinsic Berry curvature (BC) mechanism. Concomitantly, the electronic structure calculations reveal a large BC arising from SOC induced gaped nodal lines around the Fermi level, governing such large AHC property. Moreover, we also report an exceptionally large anomalous Hall angle ($\simeq$ 10.6\%) and Hall factor ($\simeq$ 0.22 V$^{-1}$) values which so far, are the largest in compared to those for other members in this vdW family.

cond-mat.str-el

Exceptionally Slow, Long Range, and Non-Gaussian Critical Fluctuations Dominate the Charge Density Wave Transition

$(TaSe_4)_2I$ is a well-studied quasi-one-dimensional compound long-known to have a charge-density wave (CDW) transition around 263 K. We argue that the critical fluctuations of the pinned CDW order parameter near the transition can be inferred from the resistance noise on account of their coupling to the dissipative normal carriers. Remarkably, the critical fluctuations of the CDW order parameter are slow enough to survive the thermodynamic limit and dominate the low-frequency resistance noise. The noise variance and relaxation time show rapid growth (critical opalescence and critical slowing down) within a temperature window of $ \varepsilon \approx \pm 0.1$, where $\varepsilon$ is the reduced temperature. This is very wide but consistent with the Ginzburg criterion. We further show that this resistance noise can be quantitatively used to extract the associated critical exponents. Below $|\varepsilon | \lesssim 0.02$, we observe a crossover from mean-field to a fluctuation-dominated regime with the critical exponents taking anomalously low values. The distribution of fluctuations in the critical transition region is skewed and strongly non-Gaussian. This non-Gaussianity is interpreted as the breakdown of the validity of the central limit theorem as the diverging coherence volume becomes comparable to the macroscopic sample size. The large magnitude critical fluctuations observed over an extended temperature range, as well as the crossover from the mean-field to the fluctuation-dominated regime highlight the role of the quasi-one dimensional character in controlling the phase transition.

cond-mat.str-el

Observation of decoupling of electrons from phonon bath close to a correlation driven metal-insulator transition

We observed that close to a Mott transition, over a small temperature range, the predominance of slow relaxations leads to decoupling of electrons from the thermal bath. This has been established by observation of large deviation of the thermal noise in the films of Mott system $NdNiO_{3}$ from the canonical Johnson-Nyquist value of $4k_{B}TR$ close to the transition. It is suggested that such a large noise arise from small isolated pockets of nanometric metallic phases (estimated size $\sim$ 15-20 nm) within the insulating phase with the charging energy as the control parameter.

cond-mat.str-el

Tetrathiomolybdate Modified Au Electrodes: Convenient Tuning of the kinetics of Electron Transfer and its application in Electrocatalysis

Ammonium tetrathiomolybdate (ATM) spontaneously self assembles on Au electrodes forming a hydrophilic, air stable, pH (3-11) tolerant multilayer that is stable over a reasonably large potential window. The ATM functionalized Au electrodes can adsorb iron porphyrin catalysts and act as O2 reducing electrodes. These electrodes are stable enough to perform rotating disk electrochemistry (RDE) as well as rotating ring disk electrochemistry (RRDE) experiments. The X-ray photoelectron spectroscopy (XPS) data indicate that the sulphide atoms of ATM anchors a single ATM layer on to Au and the subsequent layers grow vertically due to the presence of hydrogen bonding NH4+ counter-ions. The formation and growth of these ATM adlayers is investigated using atomic force microscopy (AFM), scanning electron microscopy (SEM) and a series of electrochemical data. The ATM functionalized Au electrodes have double layer capacitance comparable to those reported for Au electrode bearing short chain alkyl thiol self assembled monolayer (SAM). Importantly, the rate of interfacial charge transfer (CT) can be tuned by controlling the thickness of the adlayers by simply adjusting the deposition time. Importantly the kinetics of a catalyst adsorbed on this ATM adlayer can be switched from mass transfer limited to CT limited regime by adjusting the deposition time.

cond-mat.mtrl-sci