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Mengkun Liu

Publications and source records attributed to Mengkun Liu.

At least 37 records · Page 2Linked to original sources

Machine Learning for Optical Scanning Probe Nanoscopy

The ability to perform nanometer-scale optical imaging and spectroscopy is key to deciphering the low-energy effects in quantum materials, as well as vibrational fingerprints in planetary and extraterrestrial particles, catalytic substances, and aqueous biological samples. The scattering-type scanning near-field optical microscopy (s-SNOM) technique has recently spread to many research fields and enabled notable discoveries. In this brief perspective, we show that the s-SNOM, together with scanning probe research in general, can benefit in many ways from artificial intelligence (AI) and machine learning (ML) algorithms. We show that, with the help of AI- and ML-enhanced data acquisition and analysis, scanning probe optical nanoscopy is poised to become more efficient, accurate, and intelligent.

physics.optics↗

Deep-Learning-Aided Extraction of Optical Constants in Scanning Near-Field Optical Microscopy

Scanning near-field optical microscopy is one of the most effective techniques for spectroscopy of nanoscale systems. However, inferring optical constants from the measured near-field signal can be challenging because of a complicated and highly nonlinear interaction between the scanned probe and the sample. Conventional fitting methods applied to this problem often suffer from the lack of convergence or require human intervention. Here we develop an alternative approach where the optical parameter extraction is automated by a deep learning network. Compared to its traditional counterparts, our method demonstrates superior accuracy, stability against noise, and computational speed when applied to simulated near-field spectra.

physics.optics↗

Doping-driven topological polaritons in graphene/α-MoO3 heterostructures

Controlling the charge carrier density provides an efficient way to trigger phase transitions and modulate the optoelectronic properties in natural materials. This approach could be used to induce topological transitions in the optical response of photonic systems. Here, we predict a topological transition in the isofrequency dispersion contours of hybrid polaritons supported by a two-dimensional heterostructure consisting of graphene and $α$-phase molybdenum trioxide ($α$-MoO3). By chemically changing the doping level of graphene, we experimentally demonstrate that the contour topology of polariton isofrequency surfaces transforms from open to closed shapes as a result of doping-dependent polariton hybridization. Moreover, by changing the substrate medium for the heterostructure, the dispersion contour can be further engineered into a rather flattened shape at the topological transition, thus supporting tunable polariton canalization and providing the means to locally control the topology. We demonstrate this idea to achieve extremely subwavelength focusing by using a 1.2-$μ$m-wide silica substrate as a negative refraction lens. Our findings open a disruptive approach toward promising on-chip applications in nanoimaging, optical sensing, and manipulation of nanoscale energy transfer.

physics.optics↗

Robust and tunable Weyl phases by coherent infrared phonons in ZrTe$_5$

Ultrafast optical control of the structural and electronic properties of various quantum materials has recently sparked great interest. In particular, photoinduced quantum phase transition between distinct topological phases has been considered as a promising route to realize ultrafast topological quantum computers. Here we use first-principles and effective Hamiltonian methods to show that in ZrTe$_5$, a layered topological material, lattice distortions corresponding to all three types of zone-center infrared optical phonon modes can drive the system from the strong or weak topological insulating phase to a Weyl semimetal by breaking the global inversion symmetry. Thus achieved Weyl phases are robust, highly tunable and one of the cleanest ones due to the proximity of the Weyl points to the Fermi level and a lack of other carriers. We further show that the amount of infrared-mode pumping necessary to induce such Weyl phases can be reduced if used in conjunction with an A$_g$ Raman-mode pumping that first drives the system to the Dirac semimetal state. We also find that Berry curvature dipole moment (BCDM), induced by the dynamical inversion symmetry breaking, gives rise to various nonlinear effects that oscillate with the amplitude of the phonon modes. These nonlinear effects present a novel switch for controlling the Weyltronics enabled quantum system.

cond-mat.mtrl-sci↗

Simulation of Scanning Near-Field Optical Microscopy Spectra of 1D Plasmonic Graphene Junctions

We present numerical simulations of scattering-type Scanning Near-Field Optical Microscopy (s-SNOM) of 1D plasmonic graphene junctions. A comprehensive analysis of simulated s-SNOM spectra is performed for three types of junctions. We find conditions when the conventional interpretation of the plasmon reflection coefficients from s-SNOM measurements does not apply. Our results are applicable to other conducting 2D materials and provide a comprehensive understanding of the s-SNOM techniques for probing local transport properties of 2D materials.

cond-mat.mtrl-sci↗

Hybrid Machine Learning for Scanning Near-field Optical Spectroscopy

The underlying physics behind an experimental observation often lacks a simple analytical description. This is especially the case for scanning probe microscopy techniques, where the interaction between the probe and the sample is nontrivial. Realistic modeling to include the details of the probe is always exponentially more difficult than its "spherical cow" counterparts. On the other hand, a well-trained artificial neural network based on real data can grasp the hidden correlation between the signal and sample properties. In this work, we show that, via a combination of model calculation and experimental data acquisition, a physics-infused hybrid neural network can predict the tip-sample interaction in the widely used scattering-type scanning near-field optical microscope. This hybrid network provides a long-sought solution for accurate extraction of material properties from tip-specific raw data. The methodology can be extended to other scanning probe microscopy techniques as well as other data-oriented physical problems in general.

physics.optics↗

THz Near-Field Imaging of Extreme Subwavelength Metal Structures

Modern scattering-type scanning near-field optical microscopy (s-SNOM) has become an indispensable tool in material research. However, as the s-SNOM technique marches into the far-infrared (IR) and terahertz (THz) regimes, emerging experiments sometimes produce puzzling results. For example, anomalies in the near-field optical contrast have been widely reported. In this Letter, we systematically investigate a series of extreme subwavelength metallic nanostructures via s-SNOM near-field imaging in the GHz to THz frequency range. We find that the near-field material contrast is greatly impacted by the lateral size of the nanostructure, while the spatial resolution is practically independent of it. The contrast is also strongly affected by the connectivity of the metallic structures to a larger metallic ground plane. The observed effect can be largely explained by a quasi-electrostatic analysis. We also compare the THz s-SNOM results to those of the mid-IR regime, where the size-dependence becomes significant only for smaller structures. Our results reveal that the quantitative analysis of the near-field optical material contrasts in the long-wavelength regime requires a careful assessment of the size and configuration of metallic (optically conductive) structures.

physics.optics↗

Strain control of the metal-insulator transition in epitaxial SrCrO$_{3}$ thin films

In the perovskite oxide SrCrO$_{3}$ the interplay between crystal structure, strain and orbital ordering enables a transition from a metallic to an insulating electronic structure under certain conditions. We identified a narrow window of oxygen partial pressure in which highly strained SrCrO$_{3}$ thin films can be grown using radio-frequency (RF) off-axis magnetron sputtering on three different substrates, (LaAlO$_{3}$)$_{0.3}$-(Sr$_{2}$TaAlO$_{6}$)$_{0.7}$ (LSAT), SrTiO$_{3}$ (STO) and DyScO$_{3}$ (DSO). X-ray diffraction and atomic force microscopy confirmed the quality of the films and a metal-insulator transition driven by the substrate induced strain was demonstrated.

cond-mat.mtrl-sci↗

Moiré Engineering of Electronic Phenomena in Correlated Oxides

Moiré engineering has recently emerged as a capable approach to control quantum phenomena in condensed matter systems. In van der Waals heterostructures, moiré patterns can be formed by lattice misorientation between adjacent atomic layers, creating long range electronic order. To date, moiré engineering has been executed solely in stacked van der Waals multilayers. Herein, we describe our discovery of electronic moiré patterns in films of a prototypical magnetoresistive oxide La0.67Sr0.33MnO3 (LSMO) epitaxially grown on LaAlO3 (LAO) substrates. Using scanning probe nano-imaging, we observe microscopic moiré profiles attributed to the coexistence and interaction of two distinct incommensurate patterns of strain modulation within these films. The net effect is that both electronic conductivity and ferromagnetism of LSMO are modulated by periodic moiré textures extending over mesoscopic scales. Our work provides an entirely new route with potential to achieve spatially patterned electronic textures on demand in strained epitaxial materials.

cond-mat.mes-hall↗

Scattering of electromagnetic waves from a cone with conformal mapping: application to scanning near-field optical microscope

We study the response of a conical metallic surface to an external electromagnetic (EM) field by representing the fields in basis functions containing integrable singularities at the tip of the cone. A fast analytical solution is obtained by the conformal mapping between the cone and a round disk. We apply our calculation to the scattering- based scanning near-field optical microscope (s-SNOM) and successfully quantify the elastic light scattering from a vibrating metallic tip over a uniform sample. We find that the field-induced charge distribution consists of localized terms at the tip and the base and an extended bulk term along the body of the cone far away from the tip. In recent s-SNOM experiments at the visible-IR range (600nm - 1$μm$) the fundamental is found to be much larger than the higher harmonics whereas at THz range ($100 μm-3mm$) the fundamental becomes comparable to the higher harmonics. We find that the localized tip charge dominates the contribution to the higher harmonics and becomes bigger for the THz experiments, thus providing an intuitive understanding of the origin of the near-field signals. We demonstrate the application of our method by extracting a two-dimensional effective dielectric constant map from the s-SNOM image of a finite metallic disk, where the variation comes from the charge density induced by the EM field.

cond-mat.mes-hall↗

Artifact Free Transient Near-Field Nanoscopy

We report on the first implementation of ultrafast near field nanoscopy carried out with the transient pseudoheterodyne detection method (Tr-pHD). This method is well suited for efficient and artifact free pump-probe scattering-type near-field optical microscopy with nanometer scale resolution. The Tr-pHD technique is critically compared to other data acquisition methods and found to offer significant advantages. Experimental evidence for the advantages of Tr-pHD is provided in the Near-IR frequency range. Crucial factors involved in achieving proper performance of the Tr-pHD method with pulsed laser sources are analyzed and detailed in this work. We applied this novel method to time-resolved and spatially resolved studies of the photo-induced effects in the insulator-to-metal transition system vanadium dioxide with nanometer scale resolution.

cond-mat.mes-hall↗

Relative efficiency of polariton emission in two-dimensional materials

We investigated emission and propagation of polaritons in a two dimensional van der Waals material hexagonal boron nitride (hBN). Our specific emphasis in this work is on hyperbolic phonon polariton emission that we investigated by means of scattering-type scanning near-field optical microscopy. Real-space nano-images detail how the polaritons are launched in several common arrangements including: light scattering by the edges of the crystal, metallic nanostructures deposited on the surface of hBN crystals, as well as random defects and impurities. Notably, the scanned tip of the near-field microscope is itself an efficient polariton launcher. Our analysis reveals that the scanning tips are superior to other types of emitters we have investigated. Furthermore, the study of polariton emission and emission efficiency may provide insights for development of polaritonic devices and for fundamental studies of collective modes in other van der Waals materials.

cond-mat.mes-hall↗

Ultrafast Electron-Lattice Coupling Dynamics in VO2 and V2O3 Thin Films

Ultrafast optical pump - optical probe and optical pump - terahertz probe spectroscopy were performed on vanadium dioxide (VO2) and vanadium sesquioxide (V2O3) thin films over a wide temperature range. A comparison of the experimental data from these two different techniques and two different vanadium oxides, in particular a comparison of the electronic oscillations generated by the photoinduced longitudinal acoustic modulation, reveals the strong electron-phonon coupling that exists in the metallic state of both materials. The low energy Drude response of V2O3 appears more susceptible than VO2 to ultrafast strain control. Additionally, our results provide a measurement of the temperature dependence of the sound velocity in both systems, revealing a four- to fivefold increase in VO2 and a three- to fivefold increase in V2O3 across the phase transition. Our data also confirm observations of strong damping and phonon anharmonicity in the metallic phase of VO2, and suggest that a similar phenomenon might be at play in the metallic phase of V2O3. More generally, our simple table-top approach provides relevant and detailed information about dynamical lattice properties of vanadium oxides, opening the way to similar studies in other complex materials.

cond-mat.str-el↗

Cooperative photoinduced metastable phase control in strained manganite films

A major challenge in condensed matter physics is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic-lattice coupling that, in turn, stabilize the metallic phase. These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.

cond-mat.str-el↗

Phase transition in bulk single crystals and thin films of VO2 by nano-infrared spectroscopy and imaging

We have systematically studied a variety of vanadium dioxide (VO2) crystalline forms, including bulk single crystals and oriented thin films, using infrared (IR) near-field spectroscopic imaging techniques. By measuring the IR spectroscopic responses of electrons and phonons in VO2 with sub-grain-size spatial resolution (~20 nm), we show that epitaxial strain in VO2 thin films not only triggers spontaneous local phase separations but also leads to intermediate electronic and lattice states that are intrinsically different from those found in bulk. Generalized rules of strain and symmetry dependent mesoscopic phase inhomogeneity are also discussed. These results set the stage for a comprehensive understanding of complex energy landscapes that may not be readily determined by macroscopic approaches.

cond-mat.str-el↗

Dynamic conductivity scaling in photoexcited V2O3 thin films

Optical-pump terahertz-probe spectroscopy is used to investigate ultrafast far-infrared conductivity dynamics during the insulator-to-metal transition (IMT) in vanadium sesquioxide (V2O3). The resultant conductivity increase occurs on a tens of ps timescale, exhibiting a strong dependence on the initial temperature and fluence. We have identified a scaling of the conductivity dynamics upon renormalizing the time axis with a simple power law (alpha = 1/2) that depends solely on the initial, final, and conductivity onset temperatures. Qualitative and quantitative considerations indicate that the dynamics arise from nucleation and growth of the metallic phase which can be described by the Avrami model. We show that the temporal scaling arises from spatial scaling of the growth of the metallic volume fraction, highlighting the self-similar nature of the dynamics. Our results illustrate the important role played by mesoscopic effects in phase transition dynamics.

cond-mat.mtrl-sci↗

Ultrafast and Nanoscale Plasmonic Phenomena in Exfoliated Graphene Revealed by Infrared Pump-Probe Nanoscopy

Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ~20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate exfoliated graphene single-layers on SiO2 at technologically significant mid-infrared (MIR) frequencies where the local optical conductivity becomes experimentally accessible through the excitation of surface plasmons via the s-SNOM tip. Optical pumping at near-infrared (NIR) frequencies prompts distinct changes in the plasmonic behavior on 200 femtosecond (fs) time scales. The origin of the pump-induced, enhanced plasmonic response is identified as an increase in the effective electron temperature up to several thousand Kelvin, as deduced directly from the Drude weight associated with the plasmonic resonances.

cond-mat.mes-hall↗

Nonlinear terahertz metamaterials via field-enhanced carrier dynamics in GaAs

We demonstrate nonlinear metamaterial split ring resonators (SRRs) on GaAs at terahertz frequencies. For SRRs on doped GaAs films, incident terahertz radiation with peak fields of ~20 - 160 kV/cm drives intervalley scattering. This reduces the carrier mobility and enhances the SRR LC response due to a conductivity decrease in the doped thin film. Above ~160 kV/cm, electric field enhancement within the SRR gaps leads to efficient impact ionization, increasing the carrier density and the conductivity which, in turn, suppresses the SRR resonance. We demonstrate an increase of up to 10 orders of magnitude in the carrier density in the SRR gaps on semi-insulating GaAs substrate. Furthermore, we show that the effective permittivity can be swept from negative to positive values with increasing terahertz field strength in the impact ionization regime, enabling new possibilities for nonlinear metamaterials.

physics.optics↗