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Stephen D. Funni

Publications and source records attributed to Stephen D. Funni.

6 recordsLinked to original sources

Controlling Intertwined Electronic Orders in FeSe with Exfoliation

Controlling intertwined electronic orders in two-dimensional superconductors offers an effective route to answering fundamental questions and engineering new quantum devices. However, tuning the balance between competing orders typically requires complex chemistry, strain, or interface engineering. Here, we show that a pristine alternative is the dimensional reduction of the unconventional superconductor FeSe. Exfoliation suppresses the bulk electronic nematic response and switches the superconducting symmetry from bulk s-wave to d-wave-dominant. Transport, electron microscopy, and Raman spectroscopy establish the substantial weakening of nematic order in thin flakes. To probe superconductivity, we perform angle-dependent Andreev reflection spectroscopy on pristine crystal edges. As the junction's orientation is rotated, the spectra evolve from zero-energy bound states to coherence peaks. The injection angle, field, and temperature dependence, along with theoretical modeling, confirm that exfoliation switches the superconducting symmetry. Our results suggest a versatile superconducting platform for engineering quantum orders and provide fresh insights into the underlying pairing mechanisms.

cond-mat.supr-con

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

Scalable and deterministic construction of moir\'e superlattice in 2D materials using stressor films

Moir\'e superlattice in two-dimensional (2D) materials provides a powerful platform to engineer emergent electronic states, yet the construction of moir\'e superlattices remains lab-scale, involving much trial and error and with little control. Here, we demonstrate the construction of a heterostrain-induced moir\'e superlattice in transition metal dichalcogenides using a scalable process that deterministically induces strain to 2D materials. By applying patterned thin-film stressors and probing the resulting structures with scanning transmission electron microscopy, we directly resolve the induced heterostrain, lattice deformations, and stacking variations that produce the moir\'e superlattice. We find that uniaxial and biaxial heterostrain give rise to distinct moir\'e patterns, including stripes and distorted hexagonal patterns. With this approach, we create in-plane polar distortions and thus in-plane polarization at the domain boundaries of the moir\'e superlattice in MoS$_2$. The deterministic and scalable construction of moir\'e patterns using a well-established scalable process opens opportunities to design new moir\'e geometries in 2D materials.

cond-mat.mtrl-sci

Melting point depression of charge density wave in 1T-TiSe$_2$ due to size effects

Classical nucleation theory predicts size-dependent nucleation and melting due to surface and confinement effects at the nanoscale. In correlated electronic states, observation of size-dependent nucleation and melting is rarely reported, likely due to the extremely small length scales necessary to observe such effects for electronic states. Here, using 1T-TiSe$_2$ nanoflakes as a prototypical two-dimensional (2D) charge density wave (CDW) system, we perform in-situ cryogenic electron microscopy with temperature down to 20 K and observe size-dependent nucleation and melting of CDWs. Specifically, we observe a melting point depression of CDW for 1T-TiSe$_2$ flakes with lateral sizes less than 100 nm. By fitting experimental data to a Ginzburg-Landau model, we estimate a zero-temperature correlation length of 10--50 nm, which matches the reported CDW domain size for 1T-TiSe$_2$. As the flake size approaches the correlation length, the divergence of the CDW correlation length near the transition is cut off by the finite flake size, limiting long-range order and thereby lowering the transition temperature. For very small flakes whose size is close to the correlation length, we also observe absence of CDWs, as predicted by the model. We thus show that an electronic phase transition follows classical nucleation theory.

cond-mat.mtrl-sci

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 ($\mu$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

In operando cryo-STEM of pulse-induced charge density wave switching in TaS$_2$

The charge density wave (CDW) material 1T-TaS$_2$ exhibits a pulse-induced insulator-to-metal transition, which shows promise for next-generation electronics such as memristive memory and neuromorphic hardware. However, the rational design of TaS$_2$ devices is hindered by a poor understanding of the switching mechanism, the pulse-induced phase, and the influence of material defects. Here, we operate a 2-terminal TaS$_2$ device within a scanning transmission electron microscope (STEM) at cryogenic temperature, and directly visualize the changing CDW structure with nanoscale spatial resolution and down to 300 μs temporal resolution. We show that the pulse-induced transition is driven by Joule heating, and that the pulse-induced state corresponds to nearly commensurate and incommensurate CDW phases, depending on the applied voltage amplitude. With our in operando cryo-STEM experiments, we directly correlate the CDW structure with the device resistance, and show that dislocations significantly impact device performance. This work resolves fundamental questions of resistive switching in TaS$_2$ devices critical for engineering reliable and scalable TaS$_2$ electronics.

cond-mat.mtrl-sci