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Irena Feldman

Publications and source records attributed to Irena Feldman.

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Ultrasound Evidence for a Low-Temperature Anomaly Inside the Superconducting State of 4Hb-TaS$_2$

We report low-temperature ultrasound measurements on single crystals of the layered van der Waals superconductor 4Hb-TaS$_2$. Specific heat and ac magnetic susceptibility show a sharp bulk superconducting transition at $T_{\rm c}\approx 2.9$~K. Ultrasound measurements reveal an additional anomaly deep inside the superconducting state near $T^{*}\approx 1$~K. The most direct signature is observed in the relative ultrasonic attenuation change $\Delta\alpha$: instead of being rapidly suppressed at $T_{\rm c}$, $\Delta\alpha$ remains large throughout the intermediate superconducting regime and drops strongly only near $T^{*}$. This loss of acoustic dissipation is accompanied by a pronounced anomaly in the relative sound velocity change $\Delta v/v$, indicating strong coupling to the lattice. The low-temperature anomaly is rapidly suppressed by magnetic field and by Se substitution, suggesting a possible superconducting origin of the anomaly. We speculate that this feature may be related to induced superconductivity in the 1T layers.

cond-mat.supr-con

Light-induced trion-exciton competition revealed by ultrafast photoemission

Strong Coulomb interactions in low-dimensional quantum materials give rise to emergent bound states such as excitons and trions. Trions are conventionally secondary excitations, requiring both optical excitation and charge doping. In quasi-one-dimensional Ta$_2$NiS$_5$, however, an exceptionally large binding energy exceeding the single-particle band gap stabilizes an equilibrium trion gas under surface doping alone. Here, using time- and angle-resolved photoemission spectroscopy, we show that trions can also be generated purely optically, without external charge. Following photoexcitation of pristine Ta$_2$NiS$_5$ we observe a bright, momentum-localized, in-gap feature with a slow, fluence-dependent relaxation. Rate-equation modeling identifies it as a mixed population of trions and excitons, with the trions formed via an unconventional single-particle pathway that requires no photoexcited hole. The trion-exciton composition is controlled by pump fluence, with trions dominating the late-time relaxation. In surface doped samples, the same model with unchanged rates reproduces the full dynamics, linking the light-induced trions to their equilibrium counterparts through pump-induced dissociation and recapture. These results establish trARPES as a direct probe of charged quasiparticles far from equilibrium and open routes to optical control of neutral and charged excitations in correlated materials.

cond-mat.str-el

Microscopic evidence of dominant excitonic instability in Ta2NiSe5

An excitonic insulator (EI) is a charge-neutral bosonic condensate of spontaneously formed electron-hole pairs. Exotic quantum phenomena such as dissipationless charge neutral transport and huge potential for optoelectronic applications have led to an extensive search for intrinsic bulk materials that are EIs at ambient pressure without sophisticated device fabrication. The narrow gap semimetal Ta2NiSe5 has been proposed as a rare example of an intrinsic EI, but its ground state has remained controversial since the EI phase transition is accompanied by a structural distortion. Here, we use scanning tunneling microscopy and spectroscopy to present microscopic evidence that supports an excitonic origin of the insulating phase in Ta2NiSe5. First, we find that the insulating gap persists at structural domain boundaries where the bulk structural distortion is absent suggesting that the structural distortion is not the primary origin of insulating ground state. Second, the insulating gap is suppressed at localized charge puddles which indicates that charge correlations are important in producing the insulating gap. Finally, the decay length of the in-gap states at the puddles shows similar value to the estimated size of the exciton wavefunction from previous photoemission studies. Taken together, these findings suggest that Ta2NiSe5 is an EI and may be a versatile platform to study the physics of bosonic condensates in solid-state system at ambient conditions.

cond-mat.str-el

Trion gas on the surface of a failed excitonic insulator

Trions, three-body bound states composed of an exciton and an additional charge, are typically fragile and require external excitation to form. Here, we report the spontaneous emergence of a stable trion gas at the surface of the layered semiconductor Ta2NiS5, revealed through angle-resolved photoemission spectroscopy. We observe a sharp, highly localized in-gap feature that cannot be explained by conventional band-theory. Instead, we argue that it arises from the formation of negative trions, stabilized by surface-induced band bending and the material's quasi-one-dimensional geometry. Unlike excitons, these trions form without optical pumping and persist at equilibrium, marking a rare example of an interaction-driven surface state in a nominally conventional semiconductor. Our findings establish Ta2NiS5 as a unique platform for exploring many-body physics at surfaces and open new avenues for studying and controlling collective excitations in low-dimensional systems.

cond-mat.str-el

Chiral charge density wave in 4Hb- and 1T-TaS$_2$: The Role of interlayer coupling

We use micro-angle-resolved photoemission spectroscopy (micro-ARPES) to investigate chiral charge density waves (CDWs) in 4Hb-TaS$_2$ with micron-scale spatial resolution. In the 1T layers of 4Hb-TaS$_2$, we uncover coexisting left- and right-handed CDW domains and resolve four distinct spectral patterns arising from the interplay of chirality and rotational stacking. In contrast, bulk 1T-TaS$_2$ exhibits a uniform chirality. In addition, 4Hb-TaS$_2$ shows negligible out-of-plane dispersion of the 1T-derived bands, in contrast to the pronounced interlayer coupling observed in bulk 1T-TaS$_2$. Density functional theory (DFT) calculations corroborate this picture, revealing that the interlayer interaction of the chiral order in 4Hb-TaS$_2$ is nearly two orders of magnitude weaker than in the 1T polytype. Our findings establish 4Hb-TaS$_2$ as a quasi-two-dimensional platform for exploring tunable chiral CDW phenomena.

cond-mat.str-el

Emergence of a Fermi-surface in the current-driven Hidden state of 1T-TaS$_2$

The origin of the insulating state in 1T-TaS$_2$ has long been a subject of debate. A short current pulse transforms this insulating state into a metastable metallic phase. Using micro-ARPES, we investigate the electronic structure of this phase and uncover spatially dependent modifications caused by the current pulse. In some regions of the sample, a Fermi surface emerges, while others remain gapped. Detailed band structure analysis reveals that the metallic regions exhibit an electronic structure similar to that observed in the high-temperature phase of 1T-TaS$_2$, characterized by suppressed energy gaps and bands crossing the Fermi level. Furthermore, the metallic and insulating regions display distinct dispersions along the out-of-plane direction. These observations suggest a scenario in which the current pulse breaks the star-of-David dimers characteristic of the insulating phase, implicating these dimers as the likely origin of the insulating behavior in 1T-TaS$_2$.

cond-mat.str-el

Ramp reversal memory in bulk crystals of 1T-TaS2

The ramp reversal memory (RRM) is a non-volatile memory effect previously observed in correlated oxides exhibiting temperature-driven metal-insulator transitions (MITs). In essence, when a system displaying RRM is heated to a specific temperature within the MIT regime - where metallic and insulating domains coexist - and then cooled by reversing the temperature ramp, the resistance increases in the subsequent heating cycle. Crucially, this increase occurs only in the vicinity of the reversal temperature, indicating that the system 'remembers' this temperature. However, this memory is erased in the next heating loop. While such an effect could potentially manifest in various systems, to date, it has only been reported in thin films of correlated transition metal oxides, including VO2, V2O3, and NdNiO3. In this work, we report the observation of RRM in macroscopic crystals of the layered material 1T-TaS2, which undergoes an MIT near 190 K along charge-density wave transitions. Our findings provide compelling evidence that RRM is a general phenomenon, extending beyond the previously studied oxides. Interestingly, the RRM in TaS2 displays significantly different characteristics: it is observed when reversing from cooling to heating (as opposed to heating to cooling), and its magnitude - representing the 'strength' of the memory - is nearly an order of magnitude larger than in correlated oxides. While we discuss potential mechanisms for the RRM in TaS2, a comprehensive first-principles model is still lacking. We hope that this study will prompt further investigation into the underlying mechanisms of ramp reversal memory, enhancing our understanding of this intriguing phenomenon.

cond-mat.str-el

Charge transfer and Spin-Valley locking in 4Hb-TaS$_{2}$

4Hb-TaS$_2$ is a superconductor that exhibits unique characteristics such as time-reversal symmetry breaking, hidden magnetic memory, and topological edge modes. It is a naturally occurring heterostructure comprising of alternating layers of 1H-TaS$_2$ and 1T-TaS$_2$. The former is a well-known superconductor, while the latter is a correlated insulator with a possible non-trivial magnetic ground state. In this study, we use angle resolved photoemission spectroscopy to investigate the normal state electronic structure of this unconventional superconductor. Our findings reveal that the band structure of 4H-TaS$_2$ fundamentally differs from that of its constituent materials. Specifically, we observe a significant charge transfer from the 1T layers to the 1H layers that drives the 1T layers away from half-filling. In addition, we find a substantial reduction in inter-layer coupling in 4Hb-TaS$_2$ compared to the coupling in 2H-TaS$_2$ that results in a pronounced spin-valley locking within 4Hb-TaS$_2$

cond-mat.supr-con

First Order Quantum Phase Transition in the Hybrid Metal-Mott Insulator Transition Metal Dichalcogenide 4Hb-TaS2

Coupling together distinct correlated and topologically non-trivial electronic phases of matter can potentially induce novel electronic orders and phase transitions among them. Transition metal dichalcogenide compounds serve as a bedrock for exploration of such hybrid systems. They host a variety of exotic electronic phases and their Van der Waals nature enables to admix them, either by exfoliation and stacking or by stoichiometric growth, and thereby induce novel correlated complexes. Here we investigate the compound 4Hb-TaS$_2$ that interleaves the Mott-insulating state of 1T-TaS$_2$ and the putative spin liquid it hosts together with the metallic state of 2H-TaS$_2$ and the low temperature superconducting phase it harbors. We reveal a thermodynamic phase diagram that hosts a first order quantum phase transition between a correlated Kondo cluster state and a flat band state in which the Kondo cluster becomes depleted. We demonstrate that this intrinsic transition can be induced by an electric field and temperature as well as by manipulation of the interlayer coupling with the probe tip, hence allowing to reversibly toggle between the Kondo cluster and the flat band states. The phase transition is manifested by a discontinuous change of the complete electronic spectrum accompanied by hysteresis and low frequency noise. We find that the shape of the transition line in the phase diagram is determined by the local compressibility and the entropy of the two electronic states. Our findings set such heterogeneous structures as an exciting platform for systematic investigation and manipulation of Mott-metal transitions and strongly correlated phases and quantum phase transitions therein.

cond-mat.str-el

Evidence of a two-component order parameter in 4Hb-TaS2 in the Little-Parks effect

Finding unambiguous evidence of non-trivial pairing states is one of the greatest experimental challenges in the field of unconventional superconductivity. Such evidence requires phase-sensitive probes susceptible to the internal structure of the order parameter. We measure the Little-Parks effect to provide clear evidence of an unconventional superconducting order parameter in 4Hb-TaS$_2$. Namely, we find a $π$-shift in the transition-temperature oscillations of rings made of a single crystal. We argue that such an effect can only occur if the underlying order parameter belongs to a two-dimensional representation, in other words there are two degenerate order parameters right at the transition. Additionally, we show that $T_c$ is enhanced as a function of the out-of-plane field when a constant in-plane field is applied. Such an increase is consistent with a chiral state, which again, in general only emerges from a two-component order parameter. In combination with previous experiments, our results strongly indicate that 4Hb-TaS$_2$ indeed realizes a chiral superconductor.

cond-mat.supr-con

Magnetic memory and spontaneous vortices in a van der Waals superconductor

Doped Mott insulators exhibit some of the most intriguing quantum phases of matter, including quantum spin-liquids, unconventional superconductors, and non-Fermi liquid metals. Such phases often arise when itinerant electrons are close to a Mott insulating state, and thus experience strong spatial correlations. Proximity between different layers of van der Waals heterostructures naturally realizes a platform for experimentally studying the relationship between localized, correlated electrons and itinerant electrons. Here, we explore this relationship by studying the magnetic landscape of 4Hb-TaS2, which realizes an alternate stack of a candidate spin liquid and a superconductor. We report on a spontaneous vortex phase whose vortex density can be trained in the normal state. We show that time reversal symmetry is broken above Tc, indicating the presence of a magnetic phase independent of the superconductor. Strikingly, this phase does not generate detectable magnetic signals. We use scanning superconducting quantum interference device (SQUID) microscopy to show that it is incompatible with ferromagnetic ordering. The discovery of this new form of hidden magnetism illustrates how combining superconductivity with a strongly correlated system can lead to new, unexpected physics.

cond-mat.supr-con

Failed excitonic quantum phase transition in Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$

We study the electronic phase diagram of the excitonic insulator candidates Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$ [x=0, ... ,1] using Raman spectroscopy. Critical excitonic fluctuations are observed, that diminish with $x$ and ultimately shift to high energies, characteristic of a quantum phase transition. Nonetheless, a symmetry-breaking transition at finite temperatures is detected for all $x$, exposing a cooperating lattice instability that takes over for large $x$. Our study reveals a failed excitonic quantum phase transition, masked by a preemptive structural order.

cond-mat.str-el

Visualization of Topological Boundary Modes Manifesting Topological Nodal-Point Superconductivity

The extension of the topological classification of band insulators to topological semimetals gave way to the topology classes of Dirac, Weyl, and nodal line semimetals with their unique Fermi arc and drum head boundary modes. Similarly, there are several suggestions to employ the classification of topological superconductors for topological nodal superconductors with Majorana boundary modes. Here, we show that the surface 1H termination of the transition metal dichalcogenide compound 4Hb-TaS$_2$, in which 1T-TaS$_2$ and 1H-TaS$_2$ layers are interleaved, has the phenomenology of a topological nodal point superconductor. We find in scanning tunneling spectroscopy a residual density of states within the superconducting gap. An exponentially decaying bound mode is imaged within the superconducting gap along the boundaries of the exposed 1H layer characteristic of a gapless Majorana edge mode. The anisotropic nature of the localization length of the edge mode aims towards topological nodal superconductivity. A zero-bias conductance peak is further imaged within fairly isotropic vortex cores. All our observations are accommodated by a theoretical model of a two-dimensional nodal Weyl-like superconducting state, which ensues from inter-orbital Cooper pairing. The observation of an intrinsic topological nodal superconductivity in a layered material will pave the way for further studies of Majorana edge modes and its applications in quantum information processing.

cond-mat.supr-con

Lattice dynamics of the excitonic insulator Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$

Recently, we employed electronic polarization-resolved Raman spectroscopy to reveal the strongly correlated excitonic insulator (EI) nature of Ta2NiSe5, Volkov et al. [arXiv:2007.07344], and also showed that for Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$ alloys the critical excitonic fluctuations diminish with sulfur concentration x exposing a cooperating lattice instability that takes over for large x, Volkov et al. [arXiv:2104.07032]. Here we focus on the lattice dynamics of this EI family. We identify all Raman-active optical phonons of fully symmetric and ac-quadrupole-like symmetries and study their evolution with temperature and sulfur concentration. We demonstrate the change of selection rules at temperatures below the orthorhombic-to-monoclinic transition at Tc(x) that is related to the EI phase. We find that Tc(x) decrease monotonically from 328 K for Ta2NiSe5 to 120 K for Ta2NiS5 and that the magnitude of lattice distortion also decreases with the sulfur concentration x. For x < 0.7, the two lowest-frequency B2g phonon modes show strongly asymmetric lineshapes at high temperatures due to Fano interference with the broad excitonic continuum present in a semimetallic state. Within the framework of extended Fano model, we develop a quantitative description of the interacting exciton-phonon excitation lineshape, enabling us to derive the intrinsic phonon parameters and determine the exciton-phonon interaction strength, that affects the transition temperature Tc(x). We also observe signatures of the acoustic mode scattered assisted by the structural domain walls formed below Tc. Based on our results, we additionally present a consistent interpretation of the origin of oscillations observed in time-resolved pump-probe experiments.

cond-mat.str-el

Critical charge fluctuations and emergent coherence in a strongly correlated excitonic insulator

Excitonic insulator is a coherent electronic phase that results from the formation of a macroscopic population of bound particle-hole pairs - excitons. With only a few candidate materials known, the collective excitonic behavior is challenging to observe, being obscured by crystalline lattice effects. Here we use polarization-resolved Raman spectroscopy to reveal the quadrupolar excitonic mode in the candidate zero-gap semiconductor Ta$_2$NiSe$_5$ disentangling it from the lattice phonons. The excitonic mode pronouncedly softens close to the phase transition, showing its electronic character, while its coupling to non-critical lattice modes is shown to enhance the transition temperature. On cooling, we observe the gradual emergence of coherent superpositions of band states at the correlated insulator gap edge, with strong departures from mean-field theory predictions. Our results demonstrate the realization of a strongly correlated excitonic state in an equilibrium bulk material.

cond-mat.str-el