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Ping-Heng Tan

Publications and source records attributed to Ping-Heng Tan.

At least 19 recordsLinked to original sources

TACoS: Weakly Supervised Learning of Two-Dimensional Materials from Scribble Annotations to Precise Segmentation

The precise pixel-level localization of 2D material flakes is crucial for high-throughput screening. However, traditional fully supervised methods rely on dense annotations, which are costly and time-consuming, severely limiting the practical deployment of segmentation models. This paper proposes TACoS, a specialized scribble segmentation framework tailored for 2D materials. First, we design a unified framework that integrates semi-supervised consistency learning with structured tree energy constraints. This framework comprises two core components: an unlabeled weak-strong distribution alignment module and a tree energy regularization module. The former employs cosine consistency constraints to enhance prediction alignment across views. Meanwhile, the latter utilizes minimum spanning trees to establish pixel affinity relationships and generate structure-aware soft pseudo labels for online semantic guidance. Next, we introduce asymmetric regional contrast learning. This approach fuses high-confidence predictions from the weak augmentation branch with scribbles to form augmented labels, and construct category prototypes in the representation space. Simultaneously, we prioritize contrastive constraints on challenging pixels in boundary-unlabeled regions. This strategy enhances intra-class cohesion and inter-class separation at the representation level, effectively reducing category confusion in low-contrast edges and complex backgrounds. Experiments conducted on the constructed graphene and MoS2 datasets demonstrate that our method TACoS achieves over 96% of fully supervised performance using less than 0.6% annotated data. Furthermore, it exhibits superior structural coherence and boundary stability in scenarios with weakly contrasting edges and complex backgrounds, providing an efficient and scalable solution for automated high-throughput screening of 2D material flakes.

cs.CV

Identification and Structural Characterization of Twisted Atomically Thin Bilayer Materials by Deep Learning

Two-dimensional materials are expected to play an important role in next-generation electronics and optoelectronic devices. Recently, twisted bilayer graphene and transition metal dichalcogenides have attracted significant attention due to their unique physical properties and potential applications. In this study we describe the use of optical microscopy to collect the color space of chemical vapor deposition (CVD) molybdenum disulfide ($\mbox{MoS}_2$), and the application of a semantic segmentation convolutional neural network (CNN) to accurately and rapidly identify thicknesses of $\mbox{MoS}_2$ flakes. A second CNN model is trained to provide precise predictions on the twist angle of CVD-grown bilayer flakes. This model harnessed a dataset comprising over 10,000 synthetic images, encompassing geometries spanning from hexagonal to triangular shapes. Subsequent validation of the deep learning predictions on twist angles was executed through the second harmonic generation and Raman spectroscopy. Our results introduce a scalable methodology for automated inspection of twisted atomically thin CVD-grown bilayer.

cond-mat.mtrl-sci

Birefringence-Driven Anisotropic $\alpha$-MoO3 Optical Cavities

Many anisotropic layered materials, despite their strong in-plane birefringence, exhibit substantial visible absorption, which severely restricts cavity lengths and hinders the observation of purely birefringence-governed optical phenomena. Here, we realize a birefringence-driven anisotropic optical cavity using $\alpha$-MoO3 flakes, capitalizing on their ultralow optical loss and pronounced in-plane birefringence. Using angle-resolved polarized Raman (ARPR) spectroscopy, we observe a mode-sensitive enhancement of anisotropy, dependent on both flake thickness and Raman shift. A unified model that incorporates the intrinsic Raman tensor, birefringence, and chromatic dispersion accurately reproduces the experimental data, elucidating how cavity resonances at both excitation and scattered wavelengths interact. Within this framework, the intrinsic phonon anisotropy is quantified, providing invaluable insights for accurately predicting ARPR responses and identifying crystallographic orientation. This work provides fundamental insights into birefringence-governed cavities and opens avenues for high-performance birefringent optics and cavity-enhanced anisotropic phenomena.

physics.optics

Raman Forbidden Layer-Breathing Modes in Layered Semiconductor Materials Activated by Phonon and Optical Cavity Effects

We report Raman forbidden layer-breathing modes (LBMs) in layered semiconductor materials (LSMs). The intensity distribution of all observed LBMs depends on layer number, incident light wavelength and refractive index mismatch between LSM and underlying substrate. These results are understood by a Raman scattering theory via the proposed spatial interference model, where the naturally occurring optical and phonon cavities in LSMs enable spatially coherent photon-phonon coupling mediated by the corresponding one-dimensional periodic electronic states. Our work reveals the spatial coherence of photon and phonon fields on the phonon excitation via photon/phonon cavity engineering.

cond-mat.mtrl-sci

Intrinsic exciton transport and recombination in single-crystal lead bromide perovskite

Photogenerated carrier transport and recombination in metal halide perovskites are critical to device performance. Despite considerable efforts, sample quality issues and measurement techniques have limited the access to their intrinsic physics. Here, by utilizing high-purity CsPbBr3 single crystals and contact-free transient grating spectroscopy, we directly monitor exciton diffusive transport from 26 to 300 K. As the temperature (T) increases, the carrier mobility ({\mu}) decreases rapidly below 100 K wtih a {\mu}~T^{-3.0} scaling, and then follows a more gradual {\mu}~T^{-1.7} trend at higher temperatures. First-principles calculations perfectly reproduce this experimental trend and reveal that optical phonon scattering governs carrier mobility shifts over the entire temperature range, with a single longitudinal optical mode dominating room-temperature transport. Time-resolved photoluminescence further identifies a substantial increase in exciton radiative lifetime with temperature, attributed to increased exciton population in momentum-dark states caused by phonon scattering. Our findings unambiguously resolve previous theory-experiment discrepancies, providing benchmarks for future optoelectronic design.

cond-mat.mtrl-sci

Exciton Enhanced Giant Correlated Stoke AntiStokes Scattering of Multiorder Phonons in Semiconductor

The correlated Stoke antiStokes (SaS) scattering plays a crucial role in quantum information processing, such as heralded light sources, Fock state dynamics, and write read protocol for quantum memory. However, several reported materials exhibit low degree of SaS correlation and require high-power pulse laser excitation, limiting further applications. Herein, we explore the giant correlated multiorder SaS scattering under low power continuous laser excitation through red-sideband resonance of exciton in semiconductor ZnTe nanobelts. At low temperatures, we observe an unexpectedly strong anti-Stokes signal for multiorder longitudinal optical phonons, with SaS correlations two or four orders of magnitude larger than reported results. Furthermore, we observed the mitigation of laser heating effect for longitudinal optical phonon in SaS scattering. This finding paves a new pathway to study multiorder quantum correlated photon pairs produced through exciton-resonant Raman scattering.

cond-mat.mes-hall

Cavity-enhanced circular dichroism in a van der Waals antiferromagnet

Broken symmetry plays a pivotal role in determining the macroscopic electrical, optical, magnetic, and topological properties of materials. Circular dichroism (CD) has been widely employed to probe broken symmetry in various systems, from small molecules to bulk crystals, but designing CD responses on demand remains a challenge, especially for antiferromagnetic materials. Here, we develop a cavity-enhanced CD technique to sensitively probe the magnetic order and broken symmetry in the van der Waals antiferromagnet FePS3. By introducing interfacial inversion asymmetry in cavity-coupled FePS3 crystals, we demonstrate that the induced CD is strongly coupled with the zig-zag antiferromagnetic order of FePS3 and can be tuned both spectrally and in magnitude by varying the cavity length and FePS3 thickness. Our findings open new avenues for using cavity-modulated CD as a sensitive diagnostic probe to detect weak broken symmetries, particularly at hidden interfaces, and in systems exhibiting hidden spin polarization or strong correlations.

cond-mat.mes-hall

Interplay of phonon directionality and emission polarization in two-dimensional layered metal halide perovskites

With polarized and angle-resolved Raman spectroscopy studies on single two-dimensional layered perovskites (2DLP) flakes with different ammonium molecules as organic cations, in 2020 we revealed the very rich phonon spectra in the low-frequency regime. Although the phonon bands at low frequency can generally be attributed to the vibrations of the inorganic lattice, we found very different phonon spectra for the same lead-bromide octahedra composition by only changing the type of the organic cations. In addition, the intensity of the different phonon modes depended strongly on the angle of the linearly polarized excitation beam with respect to the in-plane axes of the octahedra lattice. In 2022, we mapped this angular dependence of the phonon modes, which enabled to identify the directionality of the different lattice vibrations. By correlating the phonon spectra with the temperature-dependent emission for a set of 2DLPs that featured very different STE emission, we demonstrated that the exciton relaxation cannot be related to coupling with a single (longitudinal optical) phonon band, and that several phonon bands should be involved in the emission process. We performed angle-resolved polarized emission and Raman spectroscopy on the same two-dimensional lead iodide perovskite microcrystals, which revealed the impact of the organic cations on the linear polarization of the emission, and corroborated our interpretation that multiple phonon bands should be involved in the radiative recombination process. Our studies revealed a wealth of highly directional low-frequency phonons in 2DLPs from which several bands are involved in the emission process, which leads to diverse optical and vibrational properties depending on the type of organic cation in the material.

cond-mat.mtrl-sci

Anomalous Gate-tunable Capacitance in Van der Waals Heterostructures

The ferroelectricity emerging in non-polar graphene/hexagonal boron nitride (hBN) heterostructures has drawn considerable attention because of its fascinating properties and promising high-frequency electrical polarization switching. Yet, the underlying mechanism is still under debate. Here in twisted double bilayer graphene (TDBLG) aligned with its neighboring hBN, we observed two types of hysteresis - delayed hysteresis in top gate induced by the anomalous screening, and advanced hysteresis in back gate caused by the anomalous gate-tunable capacitance. To investigate the role played by moir\'e potential in the anomalous hysteresis, we studied a moir\'eless graphene heterostructure as control experiment. Unexpectedly, we observed exactly the same phenomena in this control device. Our findings suggest that the anomalous ferroelectricity in graphene/hBN heterostructures may originate from the dielectric material hBN, calling for further structural investigations on hBN. The observation of gate-tunable capacitance provides more insights in the mysterious ferroelectricity in graphene/hBN heterostructures, and should enable new design of memory devices such as memcapacitor based on tunable capacitance.

cond-mat.mes-hall

Phonon Directionality Impacts Electron-Phonon Coupling and Polarization of the Band-Edge Emission in Two-Dimensional Metal Halide Perovskites

Two-dimensional metal-halide perovskites are highly versatile for light-driven applications due to their exceptional variety in material composition, which can be exploited for tunability of mechanical and optoelectronic properties. The band edge emission is defined by structure and composition of both organic and inorganic layers, and electron-phonon coupling plays a crucial role in the recombination dynamics. However, the nature of the electron-phonon coupling and which kind of phonons are involved is still under debate. Here we investigate the emission, reflectance and phonon response from single two-dimensional lead-iodide microcrystals with angle-resolved polarized spectroscopy. We find an intricate dependence of the emission polarization with the vibrational directionality in the materials, which reveals that several bands of the low-frequency phonons with non-orthogonal directionality contribute to the band edge emission. Such complex electron-phonon coupling requires adequate models to predict the thermal broadening of the emission and provides opportunities to design its polarization properties.

cond-mat.mtrl-sci

Quantitatively predicting angle-resolved polarized Raman intensity of anisotropic layered materials

Angle-resolved polarized Raman (ARPR) spectroscopy provides insights into optical anisotropy and symmetry-related electron-photon/electron-phonon couplings of anisotropic layered materials (ALMs). However, since their discovery over ten years ago, ARPR responses in ALM flakes has exhibited a puzzling dependence on flake thickness, excitation wavelength, and dielectric environment, complicating their understanding and prediction. By taking black phosphorus (BP) (large than 20 nm) flakes and four-layer Td-WTe2 as examples, this study introduces intrinsic Raman tensors (Rint) and proposes strategies to predict the ARPR intensity profiles of thick and atomically-thin ALM flakes by considering birefringence, linear dichroism and multilayer interference inside multilayered structures with experimentally determined complex refractive indexes along in-plane axes and complex tensor elements of Rint for the corresponding phonon modes. The tensor elements of effective Raman tensors (Reff), which are directly linked to the polarization vectors of incident and scattered light outside the ALM surface, were derived to quantitatively predict ARPR intensity for these ALM flakes, showing intricate dependence on ALM thickness, dielectric substrates, and excitation wavelengths. This framework can be extended to other ALM flakes from atomically-thin layers to bulk limit, facilitating comprehensive prediction of their ARPR intensity regardless of layer-dependent electronic properties.

cond-mat.mes-hall

Control of Raman scattering quantum interference pathways in graphene

Graphene is an ideal platform to study the coherence of quantum interference pathways by tuning doping or laser excitation energy. The latter produces a Raman excitation profile that provides direct insight into the lifetimes of intermediate electronic excitations and, therefore, on quantum interference, which has so far remained elusive. Here, we control the Raman scattering pathways by tuning the laser excitation energy in graphene doped up to 1.05eV, above what achievable with electrostatic doping. The Raman excitation profile of the G mode indicates its position and full width at half maximum are linearly dependent on doping. Doping-enhanced electron-electron interactions dominate the lifetime of Raman scattering pathways, and reduce Raman interference. This paves the way for engineering quantum pathways in doped graphene, nanotubes and topological insulators.

cond-mat.mes-hall

Ultrafast coherent interlayer phonon dynamics in atomically thin layers of MnBi2Te4

The atomically thin MnBi2Te4 crystal is a novel magnetic topological insulator, exhibiting exotic quantum physics. Here we report a systematic investigation of ultrafast carrier dynamics and coherent interlayer phonons in few-layer MnBi2Te4 as a function of layer number using time-resolved pump-probe reflectivity spectroscopy. Pronounced coherent phonon oscillations from the interlayer breathing mode are directly observed in the time domain. We find that the coherent oscillation frequency, the photocarrier and coherent phonon decay rates all depend sensitively on the sample thickness. The time-resolved measurements are complemented by ultralow-frequency Raman spectroscopy measurements, which both confirm the interlayer breathing mode and additionally enable observation of the interlayer shear mode. The layer dependence of these modes allows us to extract both the out-of-plane and in-plane interlayer force constants. Our studies not only reveal the interlayer van der Waals coupling strengths, but also shed light on the ultrafast optical properties of this novel two-dimensional material.

cond-mat.mes-hall

Phonon-assisted electronic states modulation of few-layer PdSe2 at terahertz frequencies

Information technology demands high-speed optoelectronic devices, but going beyond the one terahertz (THz) barrier is challenging due to the difficulties associated with generating, detecting, and processing high-frequency signals. Here, we show that femtosecond-laser-driven phonons can be utilized to coherently manipulate the excitonic properties of semiconductors at THz frequencies. The precise control of the pump and subsequent time-delayed broadband probe pulses enables the simultaneous generation and detection processes of both periodic lattice vibrations and their couplings with electronic states. Combining ultralow frequency Raman spectroscopy with first-principles calculations, we identify the unique phonon mode-selective and probe-energy dependent features of electron-phonon interactions in layered PdSe2. Two distinctive types of coherent phonon excitations could couple preferentially to different types of electronic excitations: the intralayer (4.3 THz) mode to carriers and the interlayer (0.35 THz) mode to excitons. This work provides new insights to understand the excited-state phonon interactions of 2D materials, and to achieve future applications of optoelectronic devices operating at THz frequencies.

cond-mat.mes-hall

Robust Ultraviolet to Near-infrared Quantum Emitters in Hexagonal Boron Nitride up to 1100 K

A stable single-photon source working at high temperatures with high brightness and covering full band emission from one host material is critically important for quantum technologies. Here, we find that the certain hBN single-photon emissions (SPEs) can be significantly enhanced by lasers with special wavelengths, which largely broaden the wavelength range of the hBN emitters, down to ultraviolet (357 nm) and up to near-infrared (912 nm). Importantly, these hBN SPEs are still stable even at the temperature up to 1100 Kelvin. The decoupling between single-photon and acoustic phonon is observed at high temperatures. Our work suggests that hBN can be a good host material for generating single-photon sources with ultrabroad wavelength range.

physics.app-ph

Superconductivity in Layered van der Waals Hydrogenated Germanene at High Pressure

Structural and superconducting transitions of layered van der Waals (vdW) hydrogenated germanene (GeH) were observed under high-pressure compression and decompression processes. GeH possesses a superconducting transition at critical temperature (Tc) of 5.41 K at 8.39 GPa. A crystalline to amorphous transition occurs at 16.80 GPa while superconductivity remains. An abnormally increased Tc up to 6.1 K has been observed in the decompression process while the GeH remained amorphous. Thorough in-situ high-pressure synchrotron X-ray diffraction and in-situ high-pressure Raman spectroscopy with the density functional theory simulations suggest that the superconductivity of GeH should be attributed to the increased density of states at the Fermi level as well as the enhanced electron-phonon coupling effect under high pressure. The decompression-driven superconductivity enhancement arises from pressure-induced phonon softening related to an in-plane Ge-Ge phonon mode. As an amorphous metal hydride superconductor, GeH provides a platform to study amorphous hydride superconductivity in layered vdW materials.

cond-mat.supr-con

s-d coupling enhanced phonon anharmonicity in copper-based compounds

Materials with ultralow thermal conductivity are of great interest for efficient energy conversion and thermal barrier coating. Copper-based semiconductors such as copper chalcogenides and copper halides are known to possess extreme low thermal conductivity, whereas the fundamental origin of the low thermal conductivity observed in the copper-based materials remains elusive. Here, we reveal that s-d coupling induced giant phonon anharmonicity is the fundamental mechanism responsible for the ultralow thermal conductivity of copper compounds. The symmetry controlled strong coupling of high-lying occupied copper 3d orbital with the unoccupied 4s state under thermal vibration remarkably lowers the lattice potential barrier, which enhances anharmonic scattering between phonons. This understanding is confirmed by temperature-dependent Raman spectra measurements. Our study offers an insight at atomic level connecting electronic structures with phonon vibration modes, and thus sheds light on materials properties that rely on electron-phonon coupling, such as thermoelectricity and superconductivity.

cond-mat.mtrl-sci

Measuring bulk and surface acoustic modes in diamond by angle-resolved Brillouin spectroscopy

The acoustic modes of diamond not only are of profound significance for studying its thermal conductivity, mechanical properties and optical properties, but also play a determined role in the performance of high-frequency and high-power acoustic wave devices. Here we report the bulk acoustic waves (BAWs) and surface acoustic waves (SAWs) of single crystal diamond by using the angle-resolved Brillouin light scattering (BLS) spectroscopy. We identify two high-velocity surface skimming bulk waves, with sound velocities of 1.277x10^6 and 1.727x10^6 cm/s, respectively. Furthermore, we conduct the relationship among the refractive index, incident angle and the velocities of BAWs propagating along an arbitrary direction. Our results may provide a valuable reference for fundamental researches and devices engineering in the community of diamond-based acoustic study.

cond-mat.mtrl-sci