Strong two-photon absorption (TPA) in monolayer MoS2 is demonstrated in contrast to saturable absorption (SA) in multilayer MoS2 under the excitation of femtosecond laser pulses in the near infrared region. MoS2 in the forms of monolayer single crystal and multilayer triangular islands are grown on either quartz or SiO2/Si by employing the seeding method through chemistry vapor deposition. The nonlinear transmission measurements reveal that monolayer MoS2 possesses a giant nonsaturation TPA coefficient, larger than that of conventional semiconductors. As a result of TPA, two-photon pumped frequency up-converted luminescence is observed directly in the monolayer MoS2. For the multilayer MoS2, the SA response is demonstrated with the ratio of the excited-state absorption cross section to ground-state cross section of 0.18. In addition, the laser damage threshold of the monolayer MoS2 is 97 GW/cm2, larger than that of the multilayer MoS2 of 78 GW/cm2.
By extracting the permittivity of monolayer MoS2 from experiments, the optical absorption of monolayer MoS2 prepared on top of one-dimensional photonic crystal (1DPC) or metal films is investigated theoretically. The 1DPC and metal films act as resonant back reflectors that can enhance absorption of monolayer MoS2 substantially over a broad spectral range due to the Fabry-Perot cavity effect. The absorption of monolayer MoS2 can also be tuned by varying either the distance between the monolayer MoS2 and the back reflector or the thickness of the cover layers.
We report that the refractive index of transition metal dichacolgenide (TMDC) monolayers, such as MoS2, WS2, and WSe2, can be substantially tuned by > 60% in the imaginary part and > 20% in the real part around exciton resonances using CMOS-compatible electrical gating. This giant tunablility is rooted in the dominance of excitonic effects in the refractive index of the monolayers and the strong susceptibility of the excitons to the influence of injected charge carriers. The tunability mainly results from the effects of injected charge carriers to broaden the spectral width of excitonic interb…
The optical nonlinearity of WS2, MoS2 monolayer and few-layer films was investigated using the Z-scan technique with femtosecond pulses from the visible to the near infrared. The dependence of nonlinear absorption of the WS2 and MoS2 films on layer number and excitation wavelength was studied systematically. WS2 with 1~3 layers exhibits a giant two-photon absorption (TPA) coefficient. Saturation of TPA for WS2 with 1~3 layers and MoS2 with 25~27 layers was observed. The giant nonlinearity of WS2 and MoS2 is attributed to two dimensional confinement, a giant exciton effect and the band edge res…
We demonstrate greatly enhanced light absorption by monolayer graphene over a broad spectral range, from visible to near infrared, based on the attenuated total reflection. In the experiment, graphene is sandwiched between two dielectric media referred as superstrate and substrate. Based on numerical calculation and experimental results, the closer the refractive indices of the superstrate and the substrate, the higher the absorption of graphene will be. The light absorption of monolayer graphene up to 42.7% is experimentally achieved.
The light absorption and transmission of monolayer MoS$_{2}$ in a one-dimensional defective photonic crystal (d-1DPC) is theoretically investigated. The study shows that the strong interference effect decreases photon density in particular areas of the microcavity. The d-1DPC can reduce light absorption of monolayer MoS$_{2}$ and enhance light transmission. The impact of monolayer MoS$_{2}$ light absorption on the localization effect of photon is investigated when monolayer MoS$_{2}$ and the organic light-emitting diode are located in the same microcavity. However, monolayer MoS$_{2}$ does not…
A simple perfect absorption structure is proposed to achieve the high efficiency light absorption of monolayer molybdenum disulfide (MoS 2 ) by the critical coupling mechanism of guided resonances. The results of numerical simulation and theoretical analysis show that the light absorption in this atomically thin layer can be as high as 98 . 3% at the visible wavelengths, which is over 12 times more than that of a bare monolayer MoS 2 . In addition, the operating wavelength can be tuned flexibly by adjusting the radius of the air hole and the thickness of the dielectric layers, which is of grea…
Optical extinction and absorption enhancement in the infrared range of a monolayer graphene sheet by patterning split ring resonators (SRRs) is studied. It is found that the electric mode is stronger in enhancing infrared extinction and absorption compared to the magnetic mode and other higher-order modes. We improve the infrared extinction of the SRR graphene sheet by increasing the graphene area ratio in the SRR unit cell design. With the increase of the graphene area ratio, the radiation ability of the electric dipolar mode and dissipation of graphene compete for a maximum infrared absorpti…
We numerically demonstrate a novel monolayer graphene-based perfect absorption multi-layer photonic structure by the mechanism of critical coupling with guided resonance, in which the absorption of graphene can significantly close to 99% at telecommunication wavelengths. The highly efficient absorption and spectral selectivity can be obtained with designing structural parameters in the near infrared ranges. Compared to previous works, we achieve the complete absorption of single-atomic-layer graphene in the perfect absorber for the first time, which not only opens up new methods of enhancing t…
In this study, terahertz (THz) absorption and transmission of monolayer MoS$_{2}$ was calculated under different carrier concentrations. Results showed that the THz absorption of monolayer MoS$_{2}$ is very small even under high carrier concentrations and large incident angle. Equivalent loss of the THz absorption is the total sum of reflection and absorption that is one to three grades lower than that of graphene. The monolayer MoS$_{2}$ transmission is much larger than that of the traditional GaAs and InAs two-dimensional electron gas. The field-effect tubular structure formed by the monolay…
Coherent perfect absorber (CPA) was proposed as the time-reversed counterpart to laser: a resonator containing lossy medium instead of gain medium can absorb the coherent optical fields completely. Here, we exploit a monolayer graphene to realize the CPA in a non-resonant manner. It is found that quasi-CPA point exists in the terahertz regime for suspending monolayer graphene, and the CPA can be implemented with the assistant of proper phase modulation among two incident beams at the quasi-CPA frequencies. The graphene based CPA is found of broadband angular selectivity: CPA point splits into …
We present a monolayer black phosphorus (BP)-based metamaterial structure for tunable anisotropic absorption in the mid-infrared. Based on the critical coupling mechanism of guided resonance, the structure realizes the high absorption efficiency of 99.65$\%$ for TM polarization, while only 2.61$\%$ at the same wavelength for TE polarization due to the intrinsic anisotropy of BP. The absorption characteristics can be flexibly controlled by changing critical coupling conditions, including the electron doping of BP, geometric parameters and incident angles of light. The results show feasibility i…
Vibrational overtone spectroscopy of molecules is a powerful tool for drawing information on molecular structure and dynamics. It relies on absorption of near infrared radiation (NIR) by molecular vibrations. Here we show the experimental evidence of giant enhancement of the absorption of light in solutions of organic molecules due to the switch from ballistic to diffusive propagation of light through a channel silicate glass waveguide. We also experimentally address a dynamics of absorption as a function of time of adsorption of the organic molecules on a waveguide. The observed enhancement i…
The past decades have witnessed marked progresses on the research of interfacial science in complex systems promoted by the advances in novel experimental techniques. Despite its success in many fields, implementation of coherent anti-Stokes Raman spectroscopy (CARS) for tackling the problems at interfaces was hindered by the huge resonant and non-resonant background from the bulk. Here we have developed a novel CARS scheme that is capable of probing a buried interface via suppression of the non-resonant and resonant bulk contribution by at least $10^5$ times. The method utilizes self-destruct…
We investigate the excitonic dynamics in MoSe2 monolayer and bulk samples by femtosecond transient absorption microscopy. Excitons are resonantly injected by a 750-nm and 100-fs laser pulse, and are detected by a probe pulse tuned in the range of 790 - 820 nm. We observe a strong density-dependent initial decay of the exciton population in monolayers, which can be well described by the exciton-exciton annihilation. Such a feature is not observed in the bulk under comparable conditions. We also observe the saturated absorption induced by exciton phase-space filling in both monolayers and the bu…
We investigate 1D aperiodic multilayer microstructures in order to achieve near total absorption in preselected wavelengths in a graphene monolayer. Our structures are designed by a genetic optimization algorithm coupled to a transfer matrix code. Coupled mode theory (CMT) analysis, in accordance with transfer matrix method (TMM) results, indicates the existence of a critical coupling in a graphene monolayer for perfect absorptions. Our findings show that the near-total-absorption peaks are highly tunable and can be controlled simultaneously or independently in wide range of wavelengths in the…
The nonlinear absorption of two-dimensional molybdenum disulfide was analyzed using the Z-scan technique. Sample size corresponding to a number of layer determines the band gap in the materials which play the key role for nonlinearity. Exciton dipole transition from ground state to excited state for monolayer and bilayer/multilayer is determined by the excitation source, ESA and GSA values. If the band gap is wider than the excitation source, two-photon excitation process is dominant which requires the larger ESA than GSA. For narrower bandgap, one-photon excitation is favorable because of the…
We demonstrate that the intrinsic properties of monolayer graphene allow it to act as a more effective saturable absorber for mode-locking fiber lasers compared to multilayer graphene. The absorption of monolayer graphene can be saturated at lower excitation intensity compared to multilayer graphene, graphene with wrinkle-like defects, and functionalized graphene. Monolayer graphene has a remarkable large modulation depth of 95.3%, whereas the modulation depth of multilayer graphene is greatly reduced due to nonsaturable absorption and scattering loss. Picoseconds ultrafast laser pulse (1.23 p…
Enhanced optical absorption of molecules in the vicinity of metallic nanostructures is key to a number of surface-enhanced spectroscopies and of great general interest to the fields of plasmonics and nano-optics. Yet, experimental access to this absorbance has long proven elusive. We here present direct measurements of the intrinsic absorbance of dye-molecules adsorbed onto silver nanospheres, and crucially, at sub-monolayer concentrations where dye--dye interactions become negligible. With a large detuning from the plasmon resonance, distinct shifts and broadening of the molecular resonances …
It is shown that perfect absorption and giant amplification can be realized when a wave impinges on a special metamaterial layer with zero real parts of the permittivity and permeability. The imaginary parts of the permittivity and permeability remain nonzero, corresponding to finite loss or gain. Perfect absorption and giant magnification can still be achieved even if the thickness of the metamaterial layer is arbitrarily thin and the absolute imaginary parts of the permittivity and permeability are very small. The metamaterial layer needs a total-reflection substrate for perfect absorption, …
Strong enhancement of molecular circular dichroism has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost circular dichroism. We use fluorescence-detected circular dichroism spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk array…
Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light-matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultra-low e…
The effect of femtosecond laser irradiation on bulk and single-layer MoS2 on silicon oxide is studied. Optical, Field Emission Scanning Electron Microscopy (FESEM) and Raman microscopies were used to quantify the damage. The intensity of A1g and E2g1 vibrational modes was recorded as a function of the number of irradiation pulses. The observed behavior was attributed to laser-induced bond breaking and subsequent atoms removal due to electronic excitations. The single-pulse optical damage threshold was determined for the monolayer and bulk under 800nm and 1030nm pulsed laser irradiation and the…
Nonlinear optical (NLO) phenomena such as harmonic generation, Kerr, and Pockels effects are of great technological importance for lasers, frequency converters, modulators, switches, etc. Recently, two-dimensional (2D) materials have drawn significant attention due to their strong and unique NLO properties. Here, we describe an efficient first-principles workflow for calculating the quadratic optical response and apply it to 375 non-centrosymmetric semiconductor monolayers from the Computational 2D Materials Database (C2DB). Sorting the non-resonant nonlinearities with respect to bandgap $E_g$…
The light absorption of a monolayer graphene-molybdenum disulfide photovoltaic (GM-PV) cell in a wedge-shaped microcavity with a spectrum-splitting structure is investigated theoretically. The GM-PV cell, which is three times thinner than the traditional photovoltaic cell, exhibits up to 98\% light absorptivity in a wide wavelength range. This rate exceeds the fundamental limit of nanophotonic light trapping in solar cells. The effects of defect layer thickness, GM-PV cell position in the microcavity, incident angle, and lens aberration on the light absorption rate of the GM-PV cell is explore…
The lattice mismatch strain field of core/multishell structures with spherical symmetry is modeled by a linear continuum elasticity approach. The effect of the strain on the energy structure and linear optical absorption in large core/shell/shell spherical semiconductor quantum dots is analyzed. Localization of the photoexcited carriers induced by coating is found to play an important role in explaining the optical stability of large CdSe/CdS/ZnS and ZnTe/ZnSe/ZnS quantum dots.
Resonant modes in metamaterials have been widely utilized to amplify the optical response of 2D materials for practical device applications. However, the high loss at the resonant mode severely hinders metamaterial applications. Here, we introduce a field-enhancement gain (FEG) factor to find the FEG mode for significantly improving light-matter interaction. As a demonstration, we experimentally compared the second harmonic generation enhancement of monolayer MoS2 induced by the optimal FEG and resonant modes in hyperbolic meta-structures. With the optimal FEG mode, we obtained an enhancement …
