Scanning Probe Microscopy

Strongly correlated two-dimensional systems provide compelling platforms for investigating exotic quantum phenomena. Niobium chloride (Nb$_3$Cl$_8$), a single-band Mott insulator, exhibits a remarkable out-of-plane polarization in its topmost layer that oscillates with layer parity, manifesting as an odd-even effect. Using atomic force microscopy (AFM) and Kelvin probe force microscopy (KPFM), this layer-parity-dependent polarization can be effectively characterized through surface morphology and potential mapping, enabling the unambiguous identification of different surface phases. We then fabricated dual-gate Hall devices by coupling different surface phases of Nb$_3$Cl$_8$ with monolayer graphene to investigate how the topmost-layer out-of-plane polarization influences interfacial coupling and the resulting transport behavior. Our results reveal significant phase-dependent variations in charge transfer, carrier densities, and hybridization gaps (25.2 meV for Phase 1 and 30.0 meV for Phase 2). Density functional theory calculations corroborate these experimental findings, showing that distinct out-of-plane polarizations in the topmost layer lead to different orbital overlaps and interfacial coupling strengths. These findings highlight the critical importance of surface polarization and orbital orientation in engineering the properties of strongly correlated van der Waals heterostructures.

Tip-induced switching in ferroelectrics is commonly framed as a field-driven process controlled by domain-wall kinetics. Here we argue for a more universal viewpoint: under a scanning probe, polarization reversal is fundamentally constrained by how fast screening charge can be supplied and redistributed. By combining local switching experiments with finite-element simulations, we identify a screening-current-limited mechanism in which charge injection and its space-charge-limited relaxation set the pace of switching and the scaling of domain growth. This framework naturally explains regime changes and the apparent breakdown of intrinsic domain-wall laws often inferred in the nanoscale piezoelectric hysteresis measurements. Beyond a reinterpretation of tip switching, the results position screening currents as a hidden control parameter of ferroelectric reversal across materials, turning current regulation into a practical handle for deterministic nanoscale domain engineering.

We present a compact millikelvin scanning tunneling microscope (STM) operating at 270mK with topographic navigation to micron-scale targets. Two piezoelectric low-temperature nanopositioners extend the accessible sample area, while a multi-stage copper powder and capillary filter scheme preserves millikelvin energy resolution, verified by BCS spectroscopy on aluminium thin films. A lithographically fabricated binary-encoded gold pattern encodes unique 16-bit coordinates in 4x4 pixels of 200nm$\times$200nm each. We demonstrate absolute positioning across a 350$\times$350$\mathrm{\mu}$m$^2$ area from a single STM scan. Requiring only a single lithography step and no hardware modifications to existing STM setups, the navigation system provides a versatile platform for scanning tunneling spectroscopy of nanoflakes and nanoscale devices.

Atomic-resolution imaging on molten metal/solid interfaces at temperatures above 200 {\deg}C was achieved using a high-temperature, high-speed atomic force microscope (AFM) equipped with a qPlus sensor. A tip-scanning high-speed Quadpod scanner for a large mass load of qPlus sensor (2.3 g) was developed to enhance thermal drift tolerance by high-speed scanning and thermal insulation from the heated specimen. This scanner has dominant resonant frequencies of 7.05 kHz (lateral) / 29.7 kHz (vertical) without a load. In addition, the Hybrid-loop frequency demodulation technique for low-resonant-frequency ($f_0$) sensors with a wider bandwidth than conventional phase-locked loop was also established, providing a demodulation bandwidth of $B_{\Delta f_\mathrm{inst}}\sim 0.26 f_0$ without exceeding the theoretical noise of the input deflection signal. Combining these techniques enabled atomic-resolution imaging on the molten $\mathrm{Ga/PtGa_x}$ interface at $\sim$210 {\deg}C. The topographic images obtained at $\sim$210 {\deg}C showed a relatively low-symmetry surface with an oblique lattice with a superstructure, which differed from the primitive rectangular lattice observed in the non-heated sample left at room temperature for 96 h. This demonstrates that the developed high-temperature, high-speed AFM techniques for qPlus sensors enable visualization of non-aqueous liquid/solid interfaces above 200 {\deg}C at atomic resolution, which has various potential applications, such as injection modeling, soldering, and the fabrication of liquid-metal-based catalysts.

Hybrid systems composed of graphene (Gr) and carbon nanotubes (CNTs), such as films and aerogels, have attracted broad attention for applications in electronics, mechanics, energy, and environmental science. Since the microstructures of Gr-CNT hybrids strongly affect their properties, it is essential to establish mechanical principles that govern these structures. In this study, we investigated the structural stability and mechanical behavior of Gr-CNT hybrid systems by combining molecular dynamics (MD) simulations and nanoindentation experiments. MD simulations of stacked Gr-CNT structures, in which two Gr layers confine CNTs between them, identified the energetically stable configurations and their governing parameters, i.e., intertube spacing, CNT diameter, and wall number. Specifically, under certain conditions, the structures exhibit mechanical bistability with two stable configurations: adhesion and separation of the Gr layers, arising from the competition between interlayer van der Waals attraction and elastic deformation of Gr and CNTs. Simulated loading--unloading curves display hysteresis and energy dissipation related to the stable configurations. In addition, reduced graphene oxide (rGO)-CNT hybrid films were experimentally fabricated as macroscopic assemblies of the unit structures modeled in the simulations. Atomic force microscopy-based nanoindentation measurements on the rGO-CNT films exhibit clear hysteresis and higher dissipation energy compared with pure rGO, in good agreement with the simulation results. These results provide valuable insights into Gr-CNT hybrid systems and offer guidance for designing microstructures with enhanced properties for advanced applications.

Strongly correlated quantum states, such as charge density waves (CDWs), are exquisitely sensitive to Fermi surface topology and lattice symmetry, and are typically quenched by heavy carrier doping. In two-dimensional (2D) systems, however, macroscopic geometric curvature emerges as a novel structural degree of freedom to modulate microscopic quantum coherence. This raises a compelling physical question: can non-Euclidean geometric deformations compete with extreme electronic perturbations to reshape, or even revive, a quenched macroscopic quantum order? Here, by constructing monolayer TiSe$_2$-NbSe$_2$ heterostructure on a BLG/SiC substrate for the first time, we report the curvature-driven revival of a frustrated charge order in a non-Euclidean space. Low-temperature angle-resolved photoemission spectroscopy (ARPES) reveals a massive interfacial charge transfer, which destroys the global Fermi surface nesting and completely suppresses the long-range CDW order in Euclidean flat regions. Strikingly, high-resolution scanning tunneling microscopy (STM) reveals that a novel, non-linear CDW state miraculously survives, remaining strictly localized within morphologically distorted, non-Euclidean nanoscale curved regions. Atomistic simulations unravel the structural origin of this phenomenon, demonstrating that interfacial twist and lattice mismatch spontaneously generate a corrugated superlattice.

In conventional superconductors, Cooper pairs form in an even-parity spin-singlet state. Noncentrosymmetric superconductors, which lack inversion symmetry, exhibit antisymmetric spin-orbit coupling (ASOC) that can combine even-parity spin-singlet and odd-parity spin-triplet pairs into a mixed-parity order parameter. Spin-triplet components are highly beneficial for superspintronic devices. Whether ASOC alone $-$ without strong electronic correlations $-$ is sufficient to generate a measurable triplet component remains a central open question. Here, we resolve this question in Nb$_{18}$Re$_{82}$ (Nb-Re), a weakly-correlated noncentrosymmetric metal whose superconducting pairing symmetry has been actively debated. Using low-temperature scanning tunneling spectroscopy on single crystals with four distinct crystallographic orientations, find a pronounced orientation-dependent anisotropy in the local density of states. Supported by a symmetry-constrained model, we show that the complete set of tunneling spectra requires a mixed-parity order parameter with the triplet amplitude reaching up to half of the singlet component. These results reconcile the conflicting reports in the literature on Nb-Re and demonstrate that ASOC is sufficient to foster a sizable spin-triplet component even without strong electronic correlations, suggesting that mixed-parity superconducting states may be more widespread than previously assumed. Since Nb-Re can be readily fabricated in thin-film form, these findings position it as an accessible platform for superspintronic devices and establish orientation-resolved tunneling spectroscopy as a general protocol for the detection of mixed-parity order parameters.

The realization of the axion insulator phase in magnetic topological insulators is often hindered by crystalline symmetries that protect gapless surface states, even when time-reversal symmetry is broken. Here, we use variable-temperature scanning tunneling microscopy (STM) and spectroscopy (STS), complemented with density functional theory (DFT), to investigate the local electronic structure of the antiferromagnetic (AFM) topological insulator EuSn$_2$As$_2$ across its N\'eel transition at $T_N = 24$ K. On the (001) surface, we observe a substantial density of intrinsic Sn vacancies that introduce nanoscale electronic inhomogeneity and p-type doping. Upon cooling below $T_N$, we resolve the emergence of two distinct magnetically driven gaps: a $\sim$100 meV gap near the Fermi level and a $\sim$50 meV gap at the ARPES-resolved Dirac point. We attribute the former gap to AFM Brillouin-zone folding and hybridization. The characteristics of the 50 meV gap point toward the lifting of mirror-symmetry protection by Sn vacancies and the consequent mass gapping of the Dirac point, although contributions from AFM-induced folding hybridization cannot be entirely ruled out. Our findings provide real-space evidence for strong coupling between localized moments and itinerant topological states, highlighting exfoliable EuSn$_2$As$_2$ as a potential candidate for realizing axion-insulator-based devices.

We investigate electronic instabilities in 2H-TaS\textsubscript{2} and a self-intercalated variant, 2H$^\dagger$-Ta\textsubscript{1+$\delta$}S\textsubscript{2}. In conventional samples, which we determine to be slightly hole-doped, spectral gaps and backfolded features are found as fingerprints of the $3\times3$ charge density wave (CDW). Notably, the backfolded features emerge only at a temperatures below $T\approx$~65~K, substantially lower than the established CDW temperature of 78~K, suggesting an incommensurate-commensurate lock-in transition analogous to the phenomenology of the 2H-TaSe\textsubscript{2}. In contrast, the self-intercalated 2H$^\dagger$ sample exhibits substantial electron doping and signatures of a novel \tworootthree CDW. Using \textit{ab initio} calculations of the phonon spectrum, we demonstrate that the \threebythree instability ($\mathbf{q}=\sfrac{2}{3}\mathbf{\Gamma M}$) is highly sensitive to band filling. Furthermore, with increased interlayer spacing, a competing soft phonon mode emerges near $\mathbf{q}=\sfrac{1}{2}\mathbf{\Gamma K}$, corresponding to the superstructure observed in the 2H$^\dagger$ phase, although in our calculations this instability arises under hole doping rather than the electron doping inferred experimentally. These results establish band filling and interlayer spacing as key control parameters for CDW ordering vectors in 2H-TaS\textsubscript{2}, and highlight a route to engineering electronic instabilities in a prototypical layered material.

Piezoresponse force microscopy (PFM) has established itself as a very successful and reliable imaging and spectroscopic tool for measuring a wide variety of nanoscale electromechanical functionalities. Quantitative imaging of nanoscale electromechanical phenomena requires high sensitivity while avoiding artifacts induced by large drive biases. Conventional PFM often relies on high voltages to overcome optical detection noise, leading to various non-ideal effects including electrostatic crosstalk, Joule heating, and tip-induced switching. To mitigate this situation, we introduce interferometrically detected, resonance-enhanced dual AC resonance tracking (iDART), which combines femtometer-scale displacement sensitivity of quadrature phase differential interferometry with contact resonance amplification. Through this combination, iDART achieves 10x or greater signal-to-noise improvement over current state of the art PFM approaches including both single frequency interferometric PFM or conventional, resonance enhanced PFM using optical beam detection. In this work, we demonstrate a >10x improvement of imaging sensitivity on PZT and Y-HfO. Switching spectroscopy shows similar improvements, where further demonstrates reliable hysteresis loops at small biases, mitigating nonlinearities and device failures that can occur at higher excitation amplitudes. These results position iDART as a powerful approach for probing conventional ferroelectrics with extremely high signal to noise down to weak piezoelectric systems, extending functional imaging capabilities to thin films, 2D ferroelectrics, beyond-CMOS technologies and bio-materials.

The engineering of superlattices in two-dimensional van der Waals materials has enabled the realization of rich phase diagrams hosting topological and strongly correlated phases. While incommensurability is widespread in three-dimensional systems, the role of moir\'e potentials in bulk materials remains largely unexplored. Here, using scanning tunneling microscopy, we demonstrate that a bulk transition-metal dichalcogenide polytype, 4Hb-TaS$_2$, hosts an emergent incommensurate potential between its alternating 1T and 1H layers. Interplay with a concomitant incommensurate charge-density wave suppresses the long-range order of this potential, leading to intricate coupling with electronic correlations in the doped 1T surface layer. Combining density functional theory with dynamical mean-field theory, we show that the lattice mismatch locally modulates the interlayer distance, thereby tuning both hybridization and charge transfer between the correlated 1T and metallic 1H layers. This redistribution of charge drives the system towards a doped Mott regime, in which the remaining local moments become self-screened, giving rise to a zero-bias resonance. We further find that bulk superconductivity competes with both the underlying landscape and the associated charge transfer. Our results establish incommensurate potentials as a previously overlooked ingredient in hybrid transition-metal dichalcogenides, highlighting their central role in the interplay between electronic correlations, charge-density-wave order, and unconventional superconductivity.

FeCl2 is a promising single-layer material with sizeable magnetic susceptibility and insulating character that can be easily grown by molecular beam epitaxy on various surfaces. In order to include it into the select palette of van der Waals materials used to engineer functional heterostructures, it is necessary to confirm its magnetic and electronic ground states, and understand the influence of the supporting substrate. In this work, we unambiguously demonstrate ferromagnetic ordering in a single-layer FeCl2 on Au(111) by means of spin-polarized scanning tunnelling microscopy. The material features a relatively wide insulating gap of 3.3 eV and a strongly spin-polarized conduction band that emerges at 1.5 eV above the Fermi level. Atomic scale defects with triangular shape play a primary role in the electronic gap and spin density distribution. Specifically, in a region of 1.6 nm around each defect, the conduction band is locally suppressed and the tunnelling magneto-conductance is reduced a factor of four. By tracking the spin-dependent tunnelling conductance as a function of the applied magnetic field, we record atomically resolved hysteresis loops, revealing a soft ferromagnetic ground state with pronounced out-of-plane anisotropy and coercive fields in the range of 15-50 mT.