arXiv subjects

Kainan Chang

Publications and source records attributed to Kainan Chang.

9 recordsLinked to original sources

arXiv2026

Strain-Induced Tuning of Third-Harmonic Generation in Monolayer Black Phosphorene

Based on the tight-binding model and the semiconductor Bloch equations, this work systematically reveals the microscopic mechanism of strain engineering in turning of third-harmonic generation (THG) in monolayer black phosphorene (BP). % The results show that under strain-free conditions, monolayer BP exhibits significant in-plane anisotropy, and its dominant susceptibility component reaches a maximum of $\chi^{(3);xxxx} = 1.8 \times 10^{-17} \, \text{m}^2/\text{V}^2$, agreeing well with the experimental results. % By applying uniaxial and biaxial strains along the armchair ($x$), zigzag ($y$), and out-of-plane ($z$) directions, we find that the THG response presents strong direction dependence and unique spectral shifting behaviors: in-plane compressive strain and out-of-plane tensile strain both significantly enhance the THG conductivity and induce a redshift, whereas in-plane tensile strain and out-of-plane compression lead to suppression and a blueshift, with the tuning efficiency following the order of $z > y > x$. The microscopic origin of these phenomena is identified as the synergistic modulation of the bandgap and Berry connection by strain. % Furthermore, the synergistic or competitive effects of biaxial strain further enrich the manipulation of THG signals. % Strain engineering can serve as an effective strategy for dynamically controlling nonlinear optical processes in two-dimensional materials, and it also lays a theoretical foundation for the development of high-performance reconfigurable infrared photonic devices.

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arXiv2026

Photogalvanic effect in few layer graphene

We systematically investigate the nonlinear photogalvanic effect in few-layer graphene with various stacking orders, including AA- and AB-stacked bilayers, and AAA-, ABA-, and ABC-stacked trilayers. Using a tight-binding model to describe the electronic states, the shift current conductivity and jerk current conductivity are calculated over a broad spectral range from terahertz to visible frequencies. Our symmetry analysis reveals that a nonvanishing shift current emerges only in ABA-stacked trilayer graphene due to its broken inversion symmetry, with a peak conductivity reaching approximately $1.21 \times 10^{-13}$ A$\cdot$m/V$^2$ at optimal doping. In contrast, the jerk current, permitted in all structures, requires an in-plane static electric field and exhibits pronounced spectral tunability with chemical potential. These findings establish a comprehensive symmetry-band-field coupling paradigm for nonlinear photocurrents in layered graphene and provide design principles for tunable, polarization-sensitive photodetection and energy-harvesting devices based on van der Waals heterostructures.

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arXiv2026

Photogalvanic Effects in Surface States of Topological Insulators under Perpendicular Magnetic Fields

We present a theoretical study of the nonlinear magneto-optical shift conductivity in the surface states of the prototypical topological insulator Bi$_2$Se$_3$ under a perpendicular quantizing magnetic field. By describing the electronic states as Landau levels and using a perturbative approach, we derive the microscopic expression for the shift conductivity $\sigma^{(2);\alpha\beta\gamma}(-\omega,\omega)$, where $\alpha,\beta,\gamma=\pm$ stand for the circular polarization of light and $\omega$ is the light frequency; the spectra are further decomposed into contributions from the interband and intraband optical transitions, for which the selection rules are identified. Considering that the system possesses $C_3$ point group of symmetry, the nonzero components of the conductivity tensor are $\sigma^{(2);-++}=[\sigma^{(2);+--}]^\ast$. Therefore, a pure circularly polarized light generates zero shift current. In the clean limit, the conductivities are nonzero only for discrete photon energies because of the discrete Landau levels and energy conservation, and they become Lorentzian lineshapes with the inclusion of damping, which relaxes the condition of energy conservation. The dependence of the spectra on the damping parameters, the magnetic fields, and the chemical potentials is investigated in detail. Our results reveal that the shift current is highly tunable by the chemical potential and the magnetic field. These results underscore the potential of topological insulators for tunable, strong nonlinear magneto-optical applications.

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arXiv2026

Excitation Energy Transfer in Nanohybrid System of Organic Molecule and Inorganic Transition Metal Dichalcogenides Nanoflake

Excitation energy transfer (EET) in an organic/inorganic nanohybrid system, composed of a single \textit{para}-sexiphenyl (6P) molecule physisorbed on a finite-sized MoS$_2$ nanoflake, is investigated theoretically. % The electronic structure of the MoS$_2$ nanoflake is described by using an 11-band tight-binding model, in which edge states are passivated with H atoms to restore a well-defined bandgap. % Within a configuration-interaction scheme, excitonic states are constructed and, for computational efficiency, approximated by uncorrelated electron-hole pairs in the relevant high-energy window. % The EET rates are evaluated via Fermi's golden rule, incorporating Coulomb coupling, thermal broadening, and spectral overlap between the molecular excitation and the MoS$_2$ nanoflake's electron-hole pairs. % Our results reveal that energy transfer from the molecule to the nanoflake is the dominant process, and its efficiency depends strongly on the size of the MoS$_2$ nanoflake, as well as the molecule's vertical distance and lateral position relative to the nanoflake.

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arXiv2025

Gate Voltage Tunable Second Harmonic Generation in Mono- and Bi-layer Black Phosphene

Black phosphorene (BP) has emerged as a promising platform for tunable nonlinear photonics due to its layer-dependent bandgap, high carrier mobility, and remarkable in-plane anisotropy. This study investigates the second-harmonic generation (SHG) of monolayer and bilayer BP under an external static electric field, with describing the electronic states by a tight-binding model and the dynamics by semiconductor Bloch equations. Our results reveal that BP exhibits large second-order nonlinear optical response along the armchair direction, with significant resonant enhancement when the incident photon energy approaches half of its bandgap. Under an applied electric field of $10^7$ V/m, the effective second-order nonlinear susceptibility of BP can be as large as $10^3$ pm/V, surpassing that of the conventional nonlinear crystal AgGaSe$_2$ by more than an order of magnitude. With respect to the static electric field induced by gate voltage, we discuss the relation between the electric-field-induced second harmonic (EFISH) generation and conventional SHG -- under lower gate voltage, the EFISH approach agrees well with the SHG solutions, whereas the former is no longer applicable under higher gate voltage. Specifically, as the increasing gate voltage, monolayer BP exhibits the bandgap expansion and the corresponding blue-shift in the SHG resonant peak. In contrast, bilayer BP undergoes a semiconductor-to-semimetal transition, forming Dirac cone and generating divergent SHG spectra as photon energy goes to zero. Additionally, the chemical potential allows for precise control over interband and intraband nonlinear responses. This work provides important theoretical foundations for the development of BP-based tunable nonlinear photonic devices and expands the application potential of anisotropic two-dimensional materials in nonlinear optics.

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arXiv2025

Harmonic generation of graphene quantum dots in Hartree-Fock approximation

We theoretically investigate harmonic generation in graphene quantum dots under linearly polarized optical pulses, focusing on excitonic effects. Combining the tight-binding model and the single-particle density matrix approach, we derive a semiconductor Bloch equation under a static-screened Hartree-Fock approximation. This framework characterizes the electron-electron interaction through local Hartree potentials for direct Coulomb interaction and nonlocal Fock potentials for exchange interaction. Distinct confgurations of Hartree and Fock terms yield various approximation methods, including independent-particle approximation, mean-feld approximation, random phase approximation, and excitonic effects. We thoroughly analyze how these approximation methods affect the electronic energy levels, linear optical absorption, and nonlinear harmonic generation. Within excitonic effects, we present the dependence of harmonic generation on the geometric variations of graphene quantum dots (sizes, triangular/hexagonal shapes, and armchair/zigzag edges) and the amplitude and polarization of electric fields. Our findings show that excitonic effects significantly enhance optical responses of graphene nanostructures. For a dot ensemble formed by randomly oriented graphene quantum dots, only odd-order harmonics exist along the polarization direction of the incident light. Crucially, harmonic generation in graphene quantum dots exhibits high tunability via geometric configuration, making them promising candidates for nonlinear optical nanodevices.

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arXiv2024

Second Harmonic Generation in Topological Insulators under Quantizing Magnetic Fields

We theoretically investigate the second harmonic generation (SHG) of topological insulator surface states in a perpendicular magnetic field. Our theory is based on the microscopic expression of the second-order magneto-optical conductivity developed from the density matrix formalism, taking into account hexagonal warping effects on the surface states' band structure. Using numerically exact Landau level energies and wavefunctions including hexagonal warping, we calculate the spectrum of SHG conductivities under normal incidence for different values of magnetic field and chemical potential. The imaginary parts of the SHG conductivities show prominent resonant peaks corresponding to one-photon and two-photon inter-Landau level transitions. Treating the hexagonal warping term perturbatively, these transitions are clarified analytically within a perturbation theory from which approximate selection rules for the allowable optical transitions for SHG are determined. Our results show extremely high SHG susceptibility that is easily tunable by magnetic field and doping level for topological surface states in the far-infrared regime, exceeding that of many conventional nonlinear materials. This work highlights the key role of hexagonal warping effects in generating second-order optical responses and provides new insights on the nonlinear magneto-optical properties of the topological insulators.

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arXiv2023

Gate voltage induced injection and shift currents in AA- and AB-stacked bilayer graphene

Generating photogalvanic effects in centrosymmetric materials can provide new opportunities for developing passive photodetectors and energy harvesting devices. In this work, we investigate the photogalvanic effects in centrosymmetric two-dimensional materials, AA- and AB-stacked bilayer graphene, by applying an external gate voltage to break the symmetry. Using a tight-binding model to describe the electronic states, the injection coefficients for circular photogalvanic effects and shift conductivities for linear photogalvanic effects are calculated for both materials with light wavelengths ranging from THz to visible. We find that gate voltage induced photogalvanic effects can be very significant for AB-stacked bilayer graphene, with generating a maximal dc current in the order of mA for a 1 $μ$m wide sample illuminated by a light intensity of 0.1 GW/cm$^2$, which is determined by the optical transition around the band gap and van Hove singularity points. Although such effects in AA-stacked bilayer graphene are about two orders of magnitude smaller than those in AB-stacked bilayer graphene, the spectrum is interestingly limited in a very narrow photon energy window, which is associated with the interlayer coupling strength. A detailed analysis of the light polarization dependence is also performed. The gate voltage and chemical potential can be used to effectively control the photogalvanic effects.

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arXiv2021

Picocavity-controlled Sub-nanometer Resolved Single Molecule Non-linear Fluorescence

In this article, we address fluorescence of single molecule inside a plasmonic picocavity by proposing a semi-classical theory via combining the macroscopic quantum electrodynamics theory and the open quantum system theory. To gain insights into the experimental results [Nat. Photonics, 14, 693 (2020)], we have further equipped this theory with the classical electromagnetic simulation of the pico-cavity, formed by single atom decorated silver STM tip and a silver substrate, and the time-dependent density functional theory calculation of zinc phthalocyanine molecule. Our simulations not only reproduce the fluorescence spectrum as measured in the experiment, confirming the influence of extreme field confinement afforded by the picocavity, but also reveal Rabi oscillation dynamics and Mollow triplets spectrum for moderate laser excitation. Thus, our study highlights the possibility of coherently manipulating the molecular state and exploring non-linear optical phenomena with the plasmonic picocavity.

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