arXiv subjects

Chih-Wei Luo

Publications and source records attributed to Chih-Wei Luo.

10 recordsLinked to original sources

arXiv2026

Phonon-driven Floquet engineering for electronic states

Controlling material excitations offers access to novel fundamental and technological properties. The paradigm of Floquet engineering, the manipulation of the electronic structure using a coherent and time-periodic driving source, has attracted significant attention. While most realizations rely on strong optical fields, coherent phonons provide an alternative route to realizing Floquet-Bloch states and are expected to enable substantially longer-lived Floquet-Bloch states. We show that laser-excited coherent phonons drive Floquet-Bloch states. Using time-resolved multiphoton photoemission combined with quantum beat spectroscopy on graphene-covered Ir(111), we track the coherent electronic dynamics of the image-potential states dressed by coherent phonons. The beat signal indicates the presence of sideband structure with the coherent-phonon frequency as its fundamental period, consistent with Floquet theory. Furthermore, an independent oscillation in intensity at the same frequency was observed, confirming excitation of the coherent phonon mode. Compared with conventional light-driven Floquet-Bloch states, the observed phonon-driven Floquet-Bloch states persist for one to two orders of magnitude longer. These results establish coherent phonons as a material-driven route to Floquet engineering and demonstrate the long-lived dressing of electronic states beyond the optical excitation window.

cond-mat.mtrl-sci↗

arXiv2026

Nitrogen doping induced metal-insulator transition with iso-symmetric character in rutile VO2

Metal-insulator transitions (MITs) in correlated oxides offer immense potential for next-generation Mottronic devices. However, their integration into practical applications is often hindered by the coupling of MITs with symmetry-lowering structural phase transitions, which limits switching speed and endurance. In this study, we engineered an iso-symmetric MIT on average in epitaxial rutile VO2 thin films via an in-situ nitrogen doping strategy. Nitrogen incorporation effectively suppresses V-V dimerization, enabling an iso-symmetric MIT, while preserving the original crystal symmetry. Furthermore, in-operando time-resolved optical reflectivity measurements revealed a shortened switching time in nitrogen-doped films, highlighting their enhanced performance. Our findings provide critical insights into the underlying mechanisms of MITs and introduce anion doping as a powerful tool for tailoring phase transitions in strongly correlated electron systems. This approach opens new avenues for the development of high-performance electronic and photonic devices.

cond-mat.mtrl-sci↗

arXiv2024

Two-fluid model analysis of the terahertz conductivity of YBaCuO samples: optimally doped, underdoped and overdoped cases

The complex conductivity of underdoped and optimally doped YBa$_2$Cu$_3$O$_{7-δ}$ samples and overdoped similar compound Y$_{0.7}$Ca$_{0.3}$Ba$_2$Cu$_3$O$_{7-δ}$ was measured using time-domain terahertz spectroscopy. In the normal state, the frequency dependence is described by the Drude model. Below the critical temperature $T_\mathrm{c}$, the two-fluid model was successfully employed to fit all the spectra, from 5 K up to $T_\mathrm{c}$. The temperature behaviour of fundamental parameters such as the scattering rate $1/τ$, the superfluid (normal) fraction $f_\mathrm{s}$ ($f_\mathrm{n}$) and the conductivity $σ$ was investigated at given frequencies. For the optimally doped and the overdoped samples, even at 5 K, a fifth of the electrons do not condense to the superfluid fraction. We observed that a substantial fraction of electrons do not condense to the superfluid fraction even at 5 K for optimally doped and overdoped samples. The real part of the conductivity $σ_1(T)$ exhibits a peak at low frequencies. It can be observed for all three stoichiometries and its exact shape depends on the quality of the sample. A further analysis shows that this peak is a consequence of the competition between the scattering time $τ(T)$ and the superfluid fraction $f_\mathrm{s}(T)$.

cond-mat.supr-con↗

arXiv2024

Ultrafast spintronics with geometric effects in non-adiabatic wave-packet dynamics

Motivated by the intriguing possibilities of steering ultrafast non-adiabatic processes through the geometric properties of bands in quantum materials by laser pulses, we extend a wave-packet transport theory, previously well-established in the adiabatic regime that intuitively captured geometric properties of bands, to the transient and non-adiabatic regime. This extension facilitates us to investigate macroscopic ways of manifesting microscopic band-geometric effects that highlight the special capability of non-adiabatic drivings not available to adiabatic drivings. These include imprinting band-geometric properties to the current rate after switching off the laser pulses and the induction of intrinsic macroscopic spin polarisation with an orientation not accessible by adiabatic processes. In particular, the microscopic geometrically-rooted intrinsic spin coherence is shown to underlie the spin-mediated parts of the macroscopic photocurrents. Through explicit calculations of an example with Rashba spin-orbit coupling, the spin-mediated part is shown to be discernible from the non-spin-mediated part in terms of the anisotropy of the photocurrents. Working principles behind the above theoretical results allegedly applicable beyond the Rashba example are distilled to inspect experimental data collected for SnSe, exhibiting considerable anisotropic effects. Consistency between theory and experiment is observed, paving the way of further exploration into the above intended direction.

cond-mat.mes-hall↗

arXiv2023

High-speed scanless entire bandwidth mid-infrared chemical imaging

Mid-infrared spectroscopy probes molecular vibrations to identify chemical species and functional groups. Therefore, mid-infrared hyperspectral imaging is one of the most powerful and promising candidates for chemical imaging using optical methods. Yet high-speed and entire bandwidth mid-infrared hyperspectral imaging has not been realized. Here we report a mid-infrared hyperspectral chemical imaging technique that uses chirped pulse upconversion of sub-cycle pulses at the image plane. This technique offers a lateral resolution of 15 $μ$m, and the field of view is adjustable between 800 $μ$m $\times$ 600 $μ$m to 12 mm $\times$ 9 mm. The hyperspectral imaging produces a 640 $\times$ 480 pixel image in 8 s, which covers a spectral range of 640-3015 cm$^{-1}$, comprising 1069 wavelength points and offering a wavenumber resolution of 2.6-3.7 cm$^{-1}$. For discrete frequency mid-infrared imaging, the measurement speed reaches a frame rate of 5 kHz, the repetition rate of the laser. As a demonstration, we effectively identified and mapped different components in a microfluidic device, plant cell, and mouse embryo section. The great capacity and latent force of this technique in chemical imaging promise to be applied to many fields such as chemical analysis, biology, and medicine.

physics.optics↗

arXiv2023

Dielectric breakdown and sub-wavelength patterning of monolayer hexagonal boron nitride using femtosecond pulses

Hexagonal boron nitride (hBN) has emerged as a promising two-dimensional (2D) material for many applications in photonics. Although its linear and nonlinear optical properties have been extensively studied, its interaction with high-intensity laser pulses, which is important for high-harmonic generation, fabricating quantum emitters, and maskless patterning of hBN, has not been investigated. Here we report the first study of dielectric breakdown in hBN monolayers induced by single femtosecond laser pulses. We show that hBN has the highest breakdown threshold among all existing 2D materials. This enables us to observe clearly for the first time a linear dependence of breakdown threshold on the bandgap energy for 2D materials, demonstrating such a linear dependency is a universal scaling law independent of the dimensionality. We also observe counter-intuitively that hBN, which has a larger bandgap and mechanical strength than quartz, has a lower breakdown threshold. This implies carrier generation in hBN is much more efficient. Furthermore, we demonstrate the clean removal of hBN without damage to the surrounding hBN film or the substrate, indicating that hBN is optically very robust. The ablated features are shown to possess very small edge roughness, which is attributed to its ultrahigh fracture toughness. Finally, we demonstrate femtosecond laser patterning of hBN with sub-wavelength resolution, including an isolated stripe width of 200 nm. Our work advances the knowledge of light-hBN interaction in the strong field regime and firmly establishes femtosecond lasers as novel and promising tools for one-step deterministic patterning of hBN monolayers.

physics.optics↗

arXiv2021

Ultrafast Multi-Shot Ablation and Defect Generation in Monolayer Transition Metal Dichalcogenides

Transition metal dichalcogenides are known to possess large optical nonlinearities and driving these materials at high intensities is desirable for many applications. Understanding their optical responses under repetitive intense excitation is essential to improve the performance limit of these strong-field devices and to achieve efficient laser patterning. Here, we report the incubation study of monolayer MoS${}_{2}$ and WS${}_{2}$ induced by 160 fs, 800 nm pulses in air to examine how their ablation threshold scales with the number of admitted laser pulses. Both materials were shown to outperform graphene and most bulk materials; specifically, MoS${}_{2}$ is as resistant to radiation degradation as the best of the bulk thin films with a record fast saturation. Our modeling provides convincing evidence that the small reduction in threshold and fast saturation of MoS${}_{2}$ originates in its excellent bonding integrity against radiation-induced softening. Sub-ablation damages, in the forms of vacancies, lattice disorder, and nano-voids, were revealed by transmission electron microscopy, photoluminescence, Raman, and second harmonic generation studies, which were attributed to the observed incubation. For the first time, a sub-ablation damage threshold is identified for monolayer MoS${}_{2}$ to be 78% of single-shot ablation threshold, below which MoS${}_{2}$ remains intact for many laser pulses. Our results firmly establish MoS${}_{2}$ as a robust material for strong-field devices and for high-throughput laser patterning.

physics.optics↗

arXiv2021

Ultrafast Laser Ablation, Intrinsic Threshold, and Nanopatterning of Monolayer Molybdenum Disulfide

Laser direct writing is an attractive method for patterning 2D materials without contamination. Literature shows that the femtosecond ablation threshold of graphene across substrates varies by an order of magnitude. Some attribute it to the thermal coupling to the substrates, but it remains by and large an open question. For the first time the effect of substrates on femtosecond ablation of 2D materials is studied using MoS$_{2}$ as an example. We show unambiguously that femtosecond ablation of MoS$_{2}$ is an adiabatic process with negligible heat transfer to the substrates. The observed threshold variation is due to the etalon effect which was not identified before for the laser ablation of 2D materials. Subsequently, an intrinsic ablation threshold is proposed as a true threshold parameter for 2D materials. Additionally, we demonstrate for the first time femtosecond laser patterning of monolayer MoS$_{2}$ with sub-micron resolution and mm/s speed. Moreover, engineered substrates are shown to enhance the ablation efficiency, enabling patterning with low-power femtosecond oscillators. Finally, a zero-thickness approximation is introduced to predict the field enhancement with simple analytical expressions. Our work clarifies the role of substrates on ablation and firmly establishes femtosecond laser ablation as a viable route to pattern 2D materials.

physics.optics↗

arXiv2016

Experimental violation of Bell inequalities for multi-dimensional systems

Quantum correlations between spatially separated parts of a $d$-dimensional bipartite system ($d\geq 2$) have no classical analog. Such correlations, also called entanglements, are not only conceptually important, but also have a profound impact on information science. In theory the violation of Bell inequalities based on local realistic theories for $d$-dimensional systems provides evidence of quantum nonlocality. Experimental verification is required to confirm whether a quantum system of extremely large dimension can possess this feature, however it has never been performed for large dimension (e.g., $d\geq 1000$). Here, we report that Bell inequalities are experimentally violated for bipartite quantum systems of extremely high dimensionality with the usual ensembles of polarization-entangled photon pairs. Our entanglement source violates Bell inequalities for extremely high dimensionality of $d>4000$. The designed scenario offers a possible new method to investigate the entanglement of multipartite systems of large dimensionality and their application in quantum information processing.

quant-ph↗

arXiv2012

Pulsed THz radiation due to phonon-polariton effect in [110] ZnTe crystal

Pulsed terahertz (THz) radiation, generated through optical rectification (OR) by exciting [110] ZnTe crystal with ultrafast optical pulses, typically consists of only a few cycles of electromagnetic field oscillations with a duration about a couple of picoseconds. However, it is possible, under appropriate conditions, to generate a long damped oscillation tail (LDOT) following the main cycles. The LDOT can last tens of picoseconds and its Fourier transform shows a higher and narrower frequency peak than that of the main pulse. We have demonstrated that the generation of the LDOT depends on both the duration of the optical pulse and its central wavelength. Furthermore, we have also performed theoretical calculations based upon the OR effect coupled with the phonon-polariton mode of ZnTe and obtained theoretical THz waveforms in good agreement with our experimental observation.

physics.optics↗