Abstract Graphene has led the exploration of nonlinear optical responses in two-dimensional materials with exceptionally strong third-order nonlinearity and its electrical controllability. Nonlinear wave mixing with difference-frequency is particularly interesting in graphene because of the divergent nature of third-order susceptibility as the frequency difference approaches zero, but the study on nearly degenerated four-wave mixing (NDFWM) process in graphene is largely unexplored. In this work, we report the giant third-order susceptibility of monolayer graphene, reaching the order of 10–13 m2 V−2 at the optical telecom C-band via the NDFWM process, and its electrical tunability with a high on–off contrast of 23 dB. Moreover, we observed that the NDFWM response under electrical doping exhibits a resonance feature at low pump intensity in ambient conditions, which is substantially altered by varying the pump power. Through non-perturbative quantum master equation calculations, we revealed that our observation is closely related to the dephasing nature of the Dirac fermion of graphene. The decoherence time of photoexcited carriers is estimated up to 70 fs at low pump intensity, which regime is not accessible by other nonlinear means such as high harmonic generation requiring high intensity light. Our findings not only pave an unprecedented route for probing nonlinear dynamics of photoexcited carriers across a wide range but also have a significant impact on ultrafast nonlinear information processing in graphene.

This article is dedicated to the cherished memory of Prof. Dai-Sik Kim, a visionary leader and an inspiring mentor who profoundly shaped international as well as domestic landscape of optical science, and addresses topics that were central to his scientific passion in nanophotonics. Prof. Kim's research spanned surface plasmonics, near-field optics, and terahertz plasmonics and spectroscopy, each reflecting his enduring commitment to exploring the interaction between light and matter beyond conventional limits.

Terahertz (THz) waves occupy the electromagnetic spectrum between microwave and infrared radiation, with frequencies typically ranging from 0.1 to 10 THz. Compared with other optic and electronic tools, this frequency range allows for unique sensing applications such as nondestructive, label‐free, and fast detection. Despite the promising features of THz sensing applications, the dimensional mismatch between THz wavelength and nanoscale agents hinders practical applications, especially in biosensing and chemical sensing. Several recent studies propose that engineered THz resonators, such as split ring resonators, linear dipole and slot antennas, and nanogap loop antennas, enhance the sensitivity for detecting trace amounts of target molecules, such as viruses and explosives. When combined with near‐field imaging techniques in the THz range, these THz nanosensors may revolutionize our understanding of complex nanoscale systems, including 2D materials, as researchers can observe quantum dynamics directly in molecules, mobile carriers in semiconductors, THz quantum nonlocal effects, and dynamics of excitons and polaritons at THz frequencies. Additionally, THz biomolecular sensors are also discussed, where the sensor platforms will lead to a great impact in the advancement of ultrasmall‐quantity characterization of proteins, label‐free diagnosis of Alzheimer's disease, and conformational dynamics of biomolecules in their aqueous environment.

We demonstrated an ultra-sensitive terahertz virus detection method combined with virus-sized gold nanogaps filled with Al2O3. Large-area high-density 20 nm-gap rectangular loop structures, containing a resonant frequency in the terahertz range, were fabricated on a 4-inch wafer using atomic layer lithography. When target viruses with a 60 nm diameter were located on the nanogaps, we observed a significant redshift of the resonant peak already with an average number of about 100 viruses per unit loop due to the strong field confinement and enhancement near the gap. Furthermore, when the virus was tightly attached to an etched gap like a bridge connecting metals, its sensitivity is doubled compared to the unetched gap, which resulted in 400% more resonance frequency shift per single virus particle than our previous work. Full-wave simulations and theoretical calculations based on modal expansions were in good agreement with the experiments, revealing that the resonant transmission spectrum was mostly determined by the change in refractive index in a two-dimensional-like optical hotspot near the nanogap. A further step could be taken to increase sensitivity by tuning nanogap-loops to the absorption frequencies associated with the intermolecular vibrational modes of the viruses and fingerprinting them as well.

Graphene has arisen as an efficient photothermal (PT) nanomaterial owing to the strong light-matter interaction, ultrafast and nonradiative annihilation of the photoexcited carriers, and high thermal conductivity. Combined with the unique optical properties such as universal absorption coefficient at broadband wavelengths, the PT effect in graphene can be synergistically utilized for all-optical control of light. Here, we report an efficient transmission control of propagating light in graphene-covered side-polished fiber through the PT effect of graphene. When the local heat was generated via PT effect in graphene, a significant change in optical transmission was observed through two different mechanisms. The first one was implemented by the absorption change at the graphene layer via the asymmetrical reshaping of the mode-field distribution, resulting in the optical transmission change of up to 25 dB. The other mechanism was realized by the guiding property switching from the radiation mode to the guided mode of the light, resulting in the all-optical transmission control of over 56 dB at 1550 nm. The proposed method proves that the PT effect assists the broadband and efficient all-optical control with great versatility in graphene-integrated all-fiber devices.

With the rapid advancement of 5G/6G communications using millimeter wavelengths, the concomitant usage of these long wavelength radiation for remote sensing and monitoring of biological and chemical agents is anticipated. However, the ability to detect and identify these agents with sizes ranging from nanometers to microns is hampered by its millimeter wavelength, which drastically reduces the interaction cross‐section. Herein, it is reported that single gold nanoparticles (NPs) drop‐casted on the nanoresonator can be observed by monitoring the far‐field transmitting spectra of individual terahertz (THz) nanoresonators, which enhance the electric field hundreds of times on the nanoscale. Despite the enormous mismatch in length scales, full‐wave 3D numerical modeling of the single THz nanoresonator is also performed to interpret the experimental results, indicating the possibility to turn off the resonance using only one NP embedded in the hotspot of the nanoresonator. Such NP detection becomes the most sensitive when the particle, whose size is comparable to the gap width, is tightly fitted into the nanoresonator. This work unveils the potential associated with refractive index sensing and hyperspectral absorption spectroscopy for detecting and fingerprinting ultra‐low density of bio/chemical molecules such as viruses, lipid vesicles, and explosives.

Twisted bilayer graphene (tBLG) has received substantial attention in various research fields due to its unconventional physical properties originating from Moiré superlattices. The electronic band structure in tBLG modified by interlayer interactions enables the emergence of low-energy van Hove singularities in the density of states, allowing the observation of intriguing features such as increased optical conductivity and photocurrent at visible or near-infrared wavelengths. Here, we show that the third-order optical nonlinearity can be considerably modified depending on the stacking angle in tBLG. The third-harmonic generation (THG) efficiency is found to significantly increase when the energy gap at the van Hove singularity matches the three-photon resonance of incident light. Further study on electrically tuneable optical nonlinearity reveals that the gate-controlled THG enhancement varies with the twist angle in tBLG, resulting in a THG enhanced up to 60 times compared to neutral monolayer graphene. Our results prove that the twist angle opens up a new way to control and increase the optical nonlinearity of tBLG, suggesting rotation-induced tuneable nonlinear optics in stacked two-dimensional material systems.

Electrons in indirect semiconductors can optically transit between the valance and conduction band edges only when the momentum conservation is satisfied with help of a third quasi-particle, such as a phonon. In this report, we theoretically demonstrate that indirect interband transition of graphene electrons can be optically enabled only by light with highly enhanced transversal modes, which can be generated by scattering of point dipole radiation with periodic metal slits fabricated in a natural hyperbolic material. The light-matter interaction for graphene electrons is reformulated by using indirect transition matrix elements, and interband polarizations of graphene are obtained by solving quantum kinetic equations of motion in the semi-classical regime. The interband optical current density of graphene as a function of the polarization angle of the incident field shows clear hexagonal response to the high transversal modes of light, which results from the low dependence on dephasing rate and dominance of the indirect polarizations over the direct interband contributions.

Plasmonic coupling of metallic nanostructures with two-dimensional molybdenum disulfide (MoS2) atomic layers is an important topic because it provides a pathway to manipulate the optoelectronic properties and to overcome the limited optical cross-section of the materials. Plasmonic enhanced light-matter interaction of a MoS2 layer is known to be mainly governed by optical field enhancement and the Purcell effect, while the discrimination of the contribution from each mechanism to the plasmonic enhancement is challenging. Here, we investigate photoluminescence (PL) enhancement from few-layer MoS2 transferred on Au nanostructure arrays with controlled localized surface plasmon resonance (LSPR) spectral positions that were detuned from the excitation wavelengths. Two distinctive regimes in LSPR mode-dependent PL enhancement were revealed showing a maximum enhancement (∼40-fold) with zero detuning and a modest enhancement (∼10-fold) with the red-shift detuned LSPR from the excitation wavelength, which were attributed to LSPR-induced optical field enhancement and the Purcell effect, respectively. By applying the experimental parameters into the Purcell effect formalism, an effective mode volume of ∼0.016λ03 was estimated. Our work provides an insight into how to utilize few-layer MoS2 as a base material for optoelectronics by harnessing Purcell-enhanced optical responsivity.

The resonance frequency shift and the radiative decay rate of single quantum dot excitions in close proximity to a dielectric-hyperbolic material interface are theoretically investigated. The previous nonlocal susceptibility model for a quantum-confined exciton in inhomogeneous surroundings has been substantially upgraded in a way to incorporate exciton’s envelope functions with a non-zero orbital angular momentum and a dyadic Green function tensor for uniaxially anisotropic multilayer structures. Different eigenstates of spatially localized excitons are considered with a distance to the interface of half-infinite Tetradymites(Bi2Se3), a natural hyperbolic material in a visible-to-near infrared wavelength range. From numerically obtained self-energy corrections (SEC) of the exciton as a function of its spatial confinement, eigenfunction, and distance, where the real and imaginary parts correspond to the resonance frequency shift and the radiative decay rate of the exciton, respectively, both optical properties show a significant dependence on the spatial confinement of the exciton than expected. The SEC of very weakly confined (quasi free) two-dimensional excitons is almost immune to specific choice of the eigenfunction and to anisotropic properties of the hyperbolic material even at a close distance, while such conditions are decisive for the SEC of strongly confined excitons.

Organic–inorganic halide perovskite nanocrystals or quantum dots (PQDs) are excellent candidates for optoelectronic applications, such as lasers, solar cells, light emitting diodes, and single photon sources. However, the potential applications of PQDs can expand once the photoluminescence, and in particular, the blinking behaviors of single PQDs are understood. Although the blinking of PQDs has been studied extensively recently, the underlying mechanism of the blinking behaviors is still under debate. In this study, we confirmed that type-A and type-B-HC (hot carrier) blinking, contributed to PQD blinking using their fluorescence lifetime intensity distribution (FLID). Type-B-HC blinking was experimentally confirmed for the first time for formamidinium based PQDs, and the simultaneous contributions of type-A and type-B blinking were clearly specified. Further, we related different FLID data to the ON/OFF time distribution as distinct features of different blinking types. We also emphasized that detection capability was crucial for correctly elucidating the blinking mechanism.

Lead halide perovskite has emerged as a potential material for a wide range of applications, including solar cells, light-emitting diode displays, lasing, and single photon emitters. To optimize their utilization in optoelectronic devices, the fundamental photophysical properties, especially their charge carrier transition and blinking behaviors, must be elucidated. In this study, we investigate the blinking behaviors of single formamidinium bromide perovskite quantum dots (FAPbBr3 PQDs) on the n-type TiO2 substrate. It is suggested that the electrons from TiO2 fill the trap states of FAPbBr3 PQD during Fermi-level equilibrium, which can reduce the possibility of capturing the hot electrons from PQD into the trap states. In addition, charge separation and charge recombination processes between PQD and TiO2 are expected to shorten the duration of the OFF state, thus stabilizing the fluorescence of PQDs.

Terahertz radiation and its nonlinear optical manipulation may possess potential for a variety of applications in next-generation electronics and optics. Pioneering studies have shown that the nonlinearity of carrier drift in semiconductors and graphene can be utilized for nonlinear optical processes at terahertz frequencies. However, because of the symmetric response of carriers to the terahertz field direction, most experiments have confirmed only the presence of odd-order nonlinear processes. In this study, electric-field-induced terahertz second-harmonic generation (SHG) in photoexcited gallium arsenide is demonstrated, where an applied bias field breaks the directional symmetry of the drift transport of electrons. The amplitudes of odd- and even-harmonic waves are found to be highly controllable using the bias field. The measured conversion efficiency of SHG reaches beyond 10(-5), substantially higher than the value previously reported. This terahertz harmonic generation platform with electrical controllability may be useful for future nonlinear applications at terahertz frequencies.

We theoretically investigate temporal dynamics of the second order cross correlation function at zero delay time ( G 12 ( 2 ) ( t ) ) and spectral entanglement of two photons emitted from an atomic three-level cascade. In Heisenberg’s picture, a closed set of quantum kinetic equations of motion for G 12 ( 2 ) ( t ) is derived within density matrix formalism with cluster expansion rule. G 12 ( 2 ) ( t ) shows qualitatively distinctive features depending on the spectral entanglement of two photons. Although incoherent photon pairs generated from spontaneous radiation of the excited electron are not entangled, their correlation and anti-correlation properties can be found in G 12 ( 2 ) ( t ) depending on the radiative decay rates. In the coherent excitation regime where the light emitter is located in a high Q-cavity, and its atomic polarizations are predominantly initialized, spectral entanglement between two coherent photons is established. We show that G 12 ( 2 ) ( t ) is well fitted by the entanglement criterion by Duan-Giedke-Cirac-Zoller and explain the close relationship between them by means of the optically forbidden transition in the three-level cascade.

We investigate the impact of optically induced Forster coupling in van der Waals heterostructures consisting of graphene and a monolayer transition-metal dichalcogenide (TMD). In particular, we predict the corresponding dephasing rates and a fast energy transfer between the TMD layer and graphene being in the picosecond range. Exemplary we find a transition rate of thermalized excitons of about 4 ps-1 in a MoSe2-graphene stack at room temperature. This time scale is in good agreement with the recently measured exciton lifetime in this heterostructure.

Photon pairs generated from electronic transitions in atomic three-level systems are now considered as a highly promising quantum state for constructing qubit, because of easy on-demand generation and low photon-photon interaction [1]. While polarization-entangled biphotonic states have been successfully demonstrated by using diamond-shaped four level systems with degenerated intermediates states in atoms and quantum dots and verified through the violation of Bell inequality [2,3], quantifying spectrally entangled photon pairs in experiments is still hardly available even with state-of-art techniques. In this theoretical study, we investigated the possibility of the cross correlation function of two photons as an observable for verifying the entanglement. To calculate the cross photon density-density correlation function and the degree of entanglement, Heisenberg's quantum kinetic equations of motion for single electron interacting with photons and two coherent pump fields are derived within the framework of density matrix formalism. In figure 1 (a), the energy configuration of a three-level light emitter is depicted with specially focused observables such as photon number densities (C <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">k</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">†</sup> C <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">k</sub> ) and (C <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">q</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">†</sup> C <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">q</sub> ) and their normalized cross correlation function g <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">12</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">(2)</sup> (t) = (c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">k</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">†</sup> c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">q</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">†</sup> c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">q</sub> c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">k</sub> )/(c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">k</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">†</sup> c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">k</sub> )(c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">q</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">†</sup> c <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">q</sub> ). We compared (2) the temporal behavior of g <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">(2)</sup> 12(t) and the entanglement criterion D(t) introduced by Duan et al. [4] and find peculiar similarities between them for coherently generated photon pairs, as presented in figure (b).

High-power the vortex beam was generated based on optical rectification in nonlinear optical crystal and mode conversion by employing a polymeric spiral phase plate. Subsequent application of the vortex beam for nonlinear spectroscopy in graphene shows interesting enhanced nonlinear characteristics.

In the past decade, lead halide perovskite nano-crystals or quantum dots (QDs) have attracted keen interest due to their potential applications in many optoelectronic systems. In addition, all-inorganic (CsPbX3) perovskite QDs are suggested to be efficient single photon emitting centers. Herein, we study the photon emission properties of recently synthesized organic-inorganic FAPbBr(3) QDs. Our results show that individual FAPbBr3 QDs can act as good single-photon sources with very low multiphoton emission probability achieved by extremely fast nonradiative Auger recombination. However, they exhibit photodegradation and fluorescence intensity intermittency, called blinking. By analyzing the ON(OFF) duration time distribution, particularly the OFF duration times, we suggest that two types of blinking (type-A and type-B) simultaneously contribute to the blinking behavior of FAPbBr(3) QDs. In type-A and type-B blinking, the ON/OFF periods are attributed to charged/discharged states and to activation/deactivation of fast nonradiative recombination centers, respectively. By analyzing the ON/OFF duration cutoff time as a function of the excitation intensity, we verify that type-A blinking is caused mainly by diffusion-controlled electron transfer, partially accompanied by Auger ionization processes.

We investigate the competing terahertz (THz) nonlinear harmonic generations in photo-doped GaAs with variation of bias voltages. Due to the intrinsic third-order nonlinearity, THz third harmonic generation (THG) is observed in the photo-doped GaAs without bias voltages. While such THG decreases as the bias increases, the second harmonic generation (SHG) is observed by the induced second-order nonlinear polarization, and unlike THG, the efficiency of SHG increases as the bias increases. This electrical switching behavior between THG and SHG could be understood from the surface current saturation in GaAs.

We theoretically studied coherent excitation energy transfer between self-growth semiconductor quantum dots (QDs) by solving Heisenberg’s equations of motion for density matrix elements in second quantization regime. In a local excitation condition where only one QD electron is optically excited by the pump laser field, coherent excitation energy transfer to the other QD electron can be achieved through Coulomb (Förster) and electron-photon (radiation field) interactions. We calculated three diagonal and one off-diagonal Coulomb coupling constants, which are responsible for the biexcitonic frequency renormalization and the coherent energy transfer between QDs, respectively, and radiation field coupling coefficients by using electron and hole wave functions derived from eight-band kp-theorem, whose validity has already been tested by comparison with experiment. In linear optical regime where the occupation densities of electrons at higher energy level are negligibly small, we could successfully derive fully analytical behaviors of temporal dynamics of the interband polarizations and level occupation densities of both QDs by using Hartree-Fock approximation (HFA), in eventual, the stationary photoluminescence of the coupled QDs in an analytical form. Additionally, the validity of the HFA was examined by comparing the numerical results with those obtained from the exact correlation expansion model for different values of the pump field intensity.