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Ratnadwip Singha

Publications and source records attributed to Ratnadwip Singha.

At least 19 recordsLinked to original sources
arXiv2026

Large Thermopower with Sign-Alternating Quantum Oscillations in Insulating Monolayer WTe2

The detection of Landau-level-like energy structures near the chemical potential of an insulator is essential to the search for a class of correlated electronic matter hosting charge-neutral fermions and Fermi surfaces, a long-proposed concept that remains elusive experimentally. Here we introduce and demonstrate that the magneto-thermoelectric response of a quantum insulator can reveal critical information not available via other approaches. We report the observation of large thermopower together with quantum oscillations (QOs) in the hole-doped insulating state of monolayer tungsten ditelluride (WTe2) in magnetic fields. The measured low temperature magneto-thermopower exceeds k_B/e by more than an order of magnitude, where k_B is the Boltzmann constant and e the elementary charge. This large thermopower is a characteristic of an insulating state, consistent with high resistivity. However, as the magnetic field is swept, QOs develop in the thermopower, which remarkably undergoes sign-changes that mimic the quantum characteristic of metals due to Landau quantization. The resistivity of the sample is orders of magnitude larger than the value expected from the QOs. The sign-change in the thermoelectric response directly implies the presence of a field-induced Landau-level-like structure at the chemical potential of the insulator. Neither the large thermopower nor the sign-changes can be induced by the metallic gate nearby. Our results demonstrate a new dilemma for investigating low energy excitations in correlated materials featuring mixed quantum characteristics of metals and insulators.

cond-mat.str-el↗
arXiv2026

Reversible Superdense Ordering of Tetragonal Lithium in a Layered Material

Understanding lithium (Li) ordering and dynamics is foundational in energy storage. X-ray based experimental methods do not simultaneously provide atomic structure information together with chemical composition and local bonding information for lithium in solids. Here we employ scanning transmission electron microscopy (STEM) and combine imaging, spectroscopy, and diffraction within a single experiment, to observe, in situ, an all-solid-state electrochemical cell. By integrating multimodal STEM with other complementary techniques, we report a complete mapping of lithium intercalation in a layered system, LaTe3. We identify three ordered phases of LixLaTe3 with x ranging from 1/3 to 3 with in-plane strain of up to 5%. At a very high lithium concentration of Li3LaTe3, we discover an unexpected three-layer, superdense lithium phase with tetragonal symmetry occupying the van der Waals gap. This represents a new Li phase that is reversible. Our multimodal approach thus enables complete tracking of lithium ordering and dynamics, important for next-generation energy storage applications.

cond-mat.mtrl-sci↗
arXiv2026

Probing the topological protection of edge states in multilayer tungsten ditelluride with the superconducting proximity effect

The topology of WTe2, a transition metal dichalcogenide with large spin-orbit interactions, is thought to combine type II Weyl semimetal and second-order topological insulator (SOTI) character. The SOTI character should endow WTe2 multilayer crystals with topologically protected helical states at its hinges, and, indeed, 1D states have been detected thanks to Josephson interferometry. However, the immunity to backscattering conferred to those states by their helical nature has so far not been tested. To probe the topological protection of WTe2 edge states, we have fabricated Superconducting Quantum Interference Devices (SQUIDs) in which the supercurrent through a junction on the crystal edge interferes with the supercurrent through a junction in the bulk of the crystal. We find behaviors ranging from a Symmetric SQUID pattern to asymmetric SQUID patterns, including one in which the modulation by magnetic field reveals a sawtooth-like supercurrent versus phase relation for the edge junction, demonstrating that the supercurrent at the edge is carried by ballistic channels over 600 nm, a tell-tale sign of the SOTI character of WTe2.

cond-mat.mes-hall↗
arXiv2026

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↗
arXiv2025

Clustering-Enhanced Time- and Angle-Resolved Photoemission Study of LaTe$_3$: Absence of a Photoinduced Secondary CDW in the Electronic Structure

Optical control offers a compelling route for tailoring material properties on an ultrafast time scale. Ordered states such as charge density waves (CDWs) can be transiently melted by an ultrafast light excitation. This is also the case for the rare-earth tritelluride LaTe$_3$, a prototypical CDW compound. For this material it has recently been reported that the suppression of the primary CDW allows the transient formation of a second CDW, whose wave vector is orthogonal to the primary one. This creates the intriguing scenario where light enables switching between two distinct ordered phases of the material. While the second CDW has so far been observed by structural techniques, it remains an open question how the interplay of the two CDW phases is reflected in the material's electronic structure. We investigate this via time- and angle-resolved photoemission measurements of LaTe$_3$. The complex Fermi contour is probed using a FeSuMa analyzer, which records the photoemission intensity of the entire Fermi contour at once. The dynamics revealed by the FeSuMa analyzer are complemented by measurements using a conventional hemispherical electron analyzer. We combine conventional data analysis with $k$-means clustering, an unsupervised machine learning technique, demonstrating its strong potential for disentangling large datasets. While we do not find any features that cannot be explained by the melting and re-establishment of the primary CDW, distinct dynamics and coherent oscillations are observed in the different branches of the Fermi contour.

cond-mat.str-el↗
arXiv2025

Unconventional Superconducting Phase Diagram of Monolayer WTe2

The existence of a quantum critical point (QCP) and fluctuations around it are believed to be important for understanding the phase diagram in unconventional superconductors such as cuprates, iron pnictides, and heavy fermion superconductors. However, the QCP is usually buried deep within the superconducting dome and is difficult to investigate. The connection between quantum critical fluctuations and superconductivity remains an outstanding problem in condensed matter. Here combining both electrical transport and Nernst experiments, we explicitly demonstrate the onset of superconductivity at an unconventional QCP in gate-tuned monolayer tungsten ditelluride (WTe2), with features incompatible with the conventional Bardeen-Cooper-Schrieffer (BCS) scenario. The results lead to a novel superconducting phase diagram that is distinguished from other known superconductors. Two distinct gate-tuned quantum phase transitions are observed at the ends of the superconducting dome. We find that quantum fluctuations around the QCP of the underdoped regime are essential for understanding how the monolayer superconductivity is established. The unconventional phase diagram we report here illustrates a previously unknown relation between superconductivity and QCP.

cond-mat.mes-hall↗
arXiv2024

Uncovering the Hidden Ferroaxial Density Wave as the Origin of the Axial Higgs Mode in RTe$_3$

The recent discovery of an axial amplitude (Higgs) mode in the long-studied charge density wave (CDW) systems GdTe$_3$ and LaTe$_3$ suggests a heretofore unidentified hidden order. A theoretical study proposed that the axial Higgs results from a hidden ferroaxial component of the CDW, which could arise from non-trivial orbital texture. Here, we report extensive experimental studies on ErTe$_3$ and HoTe$_3$ that possess a high-temperature CDW similar to other RTe$_3$ (R = rare earth), along with an additional low-temperature CDW with an orthogonal ordering vector. Combining Raman spectroscopy with large-angle convergent beam electron diffraction (LACBED), rotational anisotropy second-harmonic generation (RA-SHG), and muon-spin relaxation ($μ$SR), we provide unambiguous evidence that the high-temperature CDW breaks translation, rotation, and all vertical and diagonal mirror symmetries, but not time-reversal or inversion. In contrast, the low-temperature CDW only additionally breaks translation symmetry. Simultaneously, Raman scattering shows the high-temperature CDW produces an axial Higgs mode while the low-temperature mode is scalar. The weak monoclinic structural distortion and clear axial response in Raman and SHG are consistent with a ferroaxial phase in RTe$_3$ driven by coupled orbital and charge orders. Thus, our study provides a new standard for uncovering unconventional orders and confirms the power of Higgs modes to reveal them.

cond-mat.str-el↗
arXiv2024

Superconductivity from On-Chip Metallization on 2D Topological Chalcogenides

Two-dimensional (2D) transition metal dichalcogenides (TMDs) is a versatile class of quantum materials of interest to various fields including, e.g., nanoelectronics, optical devices, and topological and correlated quantum matter. Tailoring the electronic properties of TMDs is essential to their applications in many directions. Here, we report that a highly controllable and uniform on-chip 2D metallization process converts a class of atomically thin TMDs into robust superconductors, a property belonging to none of the starting materials. As examples, we demonstrate the introduction of superconductivity into a class of 2D air-sensitive topological TMDs, including monolayers of Td-WTe2, 1T'-MoTe2 and 2H-MoTe2, as well as their natural and twisted bilayers, metalized with an ultrathin layer of Palladium. This class of TMDs are known to exhibit intriguing topological phases ranging from topological insulator, Weyl semimetal to fractional Chern insulator. The unique, high-quality two-dimensional metallization process is based on our recent findings of the long-distance, non-Fickian in-plane mass transport and chemistry in 2D that occur at relatively low temperatures and in devices fully encapsulated with inert insulating layers. Highly compatible with existing nanofabrication techniques for van der Waals (vdW) stacks, our results offer a route to designing and engineering superconductivity and topological phases in a class of correlated 2D materials.

cond-mat.mes-hall↗
arXiv2023

A Platform for Far-Infrared Spectroscopy of Quantum Materials at Millikelvin Temperatures

Optical spectroscopy of quantum materials at ultralow temperatures is rarely explored, yet it may provide critical characterizations of quantum phases not possible using other approaches. We describe the development of a novel experimental platform that enables optical spectroscopic studies, together with standard electronic transport, of materials at millikelvin temperatures inside a dilution refrigerator. The instrument is capable of measuring both bulk crystals and micron-sized two-dimensional van der Waals materials and devices. We demonstrate the performance by implementing photocurrent-based Fourier transform infrared spectroscopy on a monolayer WTe$_2$ device and a multilayer 1T-TaS$_2$ crystal, with a spectral range available from the near-infrared to the terahertz regime and in magnetic fields up to 5 T. In the far-infrared regime, we achieve spectroscopic measurements at a base temperature as low as ~ 43 mK and a sample electron temperature of ~ 450 mK. Possible experiments and potential future upgrades of this versatile instrumental platform are envisioned.

cond-mat.mes-hall↗
arXiv2023

Detection of nontrivial topology driven by charge density wave in a semi-Dirac metal

The presence of electron correlations in a system with topological order can lead to exotic ground states. Considering single crystals of LaAgSb2 which has a square net crystal structure, one finds multiple charge density wave transitions (CDW) as the temperature is lowered. We find large planar Hall (PHE) signals in the CDW phase, which are still finite in the high temperature phase though they change sign. Optimising the structure within first-principles calculations, one finds an unusual chiral metallic phase. This is because as the temperature is lowered, the electrons on the Ag atoms get more localized, leading to stronger repulsions between electrons associated with atoms on different layers. This leads to successive layers sliding with respect to each other, thereby stabilising a chiral structure in which inversion symmetry is also broken. The large Berry curvature associated with the low temperature structure explains the low temperature PHE. At high temperature the PHE arises from the changes induced in the tilted Dirac cone in a magnetic field. Our work represents a route towards detecting and understanding the mechanism in a correlation driven topological transition through electron transport measurements, complemented by ab-initio electronic structure calculations.

cond-mat.mtrl-sci↗
arXiv2023

Evidence for Two Dimensional Anisotropic Luttinger Liquids at Millikelvin Temperatures

While Landau's Fermi liquid theory provides the standard description for two- and three-dimensional (2D/3D) conductors, the physics of interacting one-dimensional (1D) conductors is governed by the distinct Luttinger liquid (LL) theory. Can a LL-like state, in which electronic excitations are fractionalized modes, emerge in a 2D system as a stable zero-temperature phase? This long-standing question, first brought up by Anderson decades ago, is crucial in the study of non-Fermi liquids but remains unsettled. A recent experiment identified a moiré superlattice of twisted bilayer tungsten ditelluride (tWTe_2) with a small interlayer twist angle as a 2D host of the LL physics at temperatures of a few kelvins. Here we report experimental evidence for a 2D anisotropic LL state in a substantially reduced temperature regime, down to at least 50 mK, spontaneously formed in a tWTe_2 system with a twist angle of ~ 3 degree. While the system is metallic-like and nearly isotropic above 2 K, a dramatically enhanced electronic anisotropy develops in the millikelvin regime, featuring distinct transport behaviors along two orthogonal in-plane directions. In the strongly anisotropic phase, we observe transport characteristics of a 2D LL phase, i.e., the universal power law scaling behaviors in across-wire conductance and a zero-bias dip in the differential resistance along the wire direction. Our results represent a step forward in the search for stable LL physics beyond 1D and related unconventional quantum matter.

cond-mat.mes-hall↗
arXiv2023

Surface-Confined Two-Dimensional Crystal Growth on a Monolayer

Conventional vapor deposition or epitaxial growth of two-dimensional (2D) materials and heterostructures is conducted in a large chamber in which masses transport from the source to the substrate. Here we report a chamber-free, on-chip approach for growing a 2D crystalline structures directly in a nanoscale surface-confined 2D space. The method is based on a surprising discovery of a rapid, long-distance, non-Fickian transport of a uniform layer of atomically thin palladium (Pd) on a monolayer crystal of tungsten ditelluride (WTe2), at temperatures well below the known melting points of all materials involved. The resulting nanoconfined growth realizes a controlled formation of a stable new 2D crystalline material, Pd7WTe2 , when the monolayer seed is either free-standing or fully encapsulated in a van der Waals stack. The approach is generalizable and highly compatible with nanodevice fabrication, promising to expand the library of 2D materials and their functionalities.

cond-mat.mes-hall↗
arXiv2023

Unconventional Superconducting Quantum Criticality in Monolayer WTe2

The superconductor to insulator or metal transition in two dimensions (2D) provides a valuable platform for studying continuous quantum phase transitions (QPTs) and critical phenomena. Distinct theoretical models, including both fermionic and bosonic localization scenarios, have been developed, but many questions remain unsettled despite decades of research. Extending Nernst experiments down to millikelvin temperatures, we uncover anomalous quantum fluctuations and identify an unconventional superconducting quantum critical point (QCP) in a gate-tuned excitonic quantum spin Hall insulator (QSHI), the monolayer tungsten ditelluride (WTe2). The observed vortex Nernst effect reveals singular superconducting fluctuations in the resistive normal state induced by magnetic fields or temperature, even well above the transition. Near the doping-induced QCP, the Nernst signal driven by quantum fluctuations is exceptionally large in the millikelvin regime, with a coefficient of ~ 4,100 uV/KT at zero magnetic field, an indication of the proliferation of vortices. Surprisingly, the Nernst signal abruptly disappears when the doping falls below the critical value, in striking conflict with conventional expectations. This series of phenomena, which have no prior analogue, call for careful examinations of the mechanism of the QCP, including the possibility of a continuous QPT between two distinct ordered phases in the monolayer. Our experiments open a new avenue for studying unconventional QPTs and quantum critical matter.

cond-mat.mes-hall↗
arXiv2022

Charge density wave-generated Fermi surfaces in NdTe$_3$

The electronic structure of NdTe$_3$ in the charge density wave phase (CDW) is investigated by angle-resolved photoemission spectroscopy. The combination of high-quality crystals and careful surface preparation reveals subtle and previously unobserved details in the Fermi surface topology, allowing an interpretation of the rich and unexplained quantum oscillations in the rare earth tritellurides RTe$_3$. In particular, several closed Fermi surface elements can be observed that are related to CDW-induced replicas of the original bands, leading to the curious situation in which a CDW does not only remove Fermi surface elements but creates new ones that are observable in transport experiments. Moreover, a large residual Fermi surface is found in the CDW gap, very close to the position of the gapped normal-state Fermi surface. Its area agrees very well with high-frequency quantum oscillations in NdTe$_3$ and its presence is explained by strong electron-phonon coupling combined with the quasi one-dimensional character of the CDW. Finally, we identify the origin of the low-frequency $α$ quantum oscillations ubiquitous for the lighter R elements in the RTe$_3$ family and responsible for the high mobility in these compounds.

cond-mat.str-el↗
arXiv2022

Colossal negative magnetoresistance in the complex charge density wave regime of an antiferromagnetic Dirac semimetal

Colossal magnetoresistance (MR) is a well-known phenomenon, notably observed in hole-doped ferromagnetic manganites. It remains a major research topic due to its potential in technological applications. Though topological semimetals also show large MR, its origin and nature are completely different. Here, we show that in the highly electron doped region, the Dirac semimetal CeSbTe demonstrates similar properties as the manganites. CeSb$_{0.11}$Te$_{1.90}$ hosts multiple charge density wave (CDW) modulation-vectors and has a complex magnetic phase diagram. We confirm that this compound is an antiferromagnetic Dirac semimetal. Despite having a metallic Fermi surface, the electronic transport properties are semiconductor-like and deviate from known theoretical models. An external magnetic field induces a semiconductor-metal-like transition, which results in a colossal negative MR. Moreover, signatures of the coupling between the CDW and a spin modulation are observed in resistivity. This spin modulation also produces a giant anomalous Hall response.

cond-mat.mtrl-sci↗
arXiv2022

Synthesis of an aqueous, air-stable, superconducting 1T'-WS$_2$ monolayer-ink

Liquid-phase chemical exfoliation is ideal to achieve industry scale production of two-dimensional (2D) materials for a wide range of application such as printable electronics, catalysis and energy storage. However, many impactful 2D materials with potentials in quantum technologies can only be studied in lab settings due to their air-sensitivity, and loss of physical performance after chemical processing. Here, we report a simple chemical exfoliation method to create a stable, aqueous, surfactant-free, superconducting ink containing phase-pure 1T'-WS$_2$ monolayers that are isotructural to the air-sensitive topological insulator 1T'-WTe$_2$. We demonstrate that thin films can be cast on both hard and flexible substrates. The printed film is metallic at room temperature and superconducting below 7.3 K, shows strong anisotropic unconventional superconducting behavior with an in-plane and out-of-plane upper critical magnetic field of 30.1 T and 5.3 T, has a critical current of 44 mA, and is stable at ambient conditions for at least 30 days. Our results show that chemical processing can provide an engineering solution, which makes non-trivial 2D materials that used to be only studied in laboratories commercially accessible.

cond-mat.mtrl-sci↗
arXiv2022

A Class of Magnetic Topological Material Candidates with Hypervalent Bi Chains

The link between crystal and electronic structure is crucial for understanding structure-property relations in solid-state chemistry. In particular, it has been instrumental in understanding topological materials, where electrons behave differently than they would in conventional solids. Herein, we identify 1D Bi chains as a structural motif of interest for topological materials. We focus on Sm$_3$ZrBi$_5$, a new quasi-one-dimensional (1D) compound in the Ln$_3$MPn$_5$ (Ln = lanthanide; M = metal; Pn = pnictide) family that crystallizes in the P$6_{3}$/mcm space group. Density functional theory calculations indicate a complex, topologically non-trivial electronic structure that changes significantly in the presence of spin-orbit coupling. Magnetic measurements show a quasi-1D antiferromagnetic structure with two magnetic transitions at 11.7 and 10.7 K that are invariant to applied field up to 9 T, indicating magnetically frustrated spins. Heat capacity, electrical, and thermal transport measurements support this claim and suggest complex scattering behavior in Sm$_3$ZrBi$_5$. This work highlights 1D chains as an unexplored structural motif for identifying topological materials, as well as the potential for rich physical phenomena in the Ln$_3$MPn$_5$ family.

cond-mat.mtrl-sci↗
arXiv2021

One-Dimensional Luttinger Liquids in a Two-Dimensional Moiré Lattice

The Luttinger liquid (LL) model of one-dimensional (1D) electronic systems provides a powerful tool for understanding strongly correlated physics including phenomena such as spin-charge separation. Substantial theoretical efforts have attempted to extend the LL phenomenology to two dimensions (2D), especially in models of closely packed arrays of 1D quantum wires, each being described as a LL. Such coupled-wire models have been successfully used to construct 2D anisotropic non-Fermi liquids, quantum Hall states, topological phases, and quantum spin liquids. However, an experimental demonstration of high-quality arrays of 1D LLs suitable for realizing these models remains absent. Here we report the experimental realization of 2D arrays of 1D LLs with crystalline quality in a moiré superlattice made of twisted bilayer tungsten ditelluride (tWTe$_{2}$). Originating from the anisotropic lattice of the monolayer, the moiré pattern of tWTe$_{2}$ hosts identical, parallel 1D electronic channels, separated by a fixed nanoscale distance, which is tunable by the interlayer twist angle. At a twist angle of ~ 5 degrees, we find that hole-doped tWTe$_{2}$ exhibits exceptionally large transport anisotropy with a resistance ratio of ~ 1000 between two orthogonal in-plane directions. The across-wire conductance exhibits power-law scaling behaviors, consistent with the formation of a 2D anisotropic phase that resembles an array of LLs. Our results open the door for realizing a variety of correlated and topological quantum phases based on coupled-wire models and LL physics.

cond-mat.mes-hall↗