It is shown that the ordinary semiclassical theory of the absorption of light by exciton states is not completely satisfactory (in contrast to the case of absorption due to interband transitions). A more complete theory is developed. It is shown that excitons are approximate bosons, and, in interaction with the electromagnetic field, the exciton field plays the role of the classical polarization field. The eigenstates of the system of crystal and radiation field are mixtures of photons and excitons. The ordinary one-quantum optical lifetime of an excitation is infinite. Absorption occurs only when "three-body" processes are introduced. The theory includes "local field" effects, leading to the Lorentz local field correction when it is applicable. A Smakula equation for the oscillator strength in terms of the integrated absorption constant is derived.

a Quantum-Mechanical Theory of the Contribution of Excitons to the Complex Dielectric Constant of Crystals.

Photonics and optoelectronics using nano-structured hybrid perovskite media and their optical cavities

Monolayer MoS2 is a direct-gap two-dimensional semiconductor that exhibits strong electron-hole interactions, leading to the formation of stable excitons and trions. Here we report the existence of efficient exciton-exciton annihilation, a four-body interaction, in this material. Exciton-exciton annihilation was identified experimentally in ultrafast transient absorption measurements through the emergence of a decay channel varying quadratically with exciton density. The rate of exciton-exciton annihilation was determined to be (4.3 ± 1.1) × 10(-2) cm(2)/s at room temperature.

http://absimage.aps.org/image/MAR15/MWS_MAR15-2014-006549.pdf

Observation of Rapid Exciton-Exciton Annihilation in Monolayer Molybdenum Disulfide

Two-dimensional (2D) materials have drawn tremendous attention in recent years. Being atomically thin, stacked with van der Waals force and free of surface chemical dangling bonds, 2D materials exhibit several distinct physical properties. To date, 2D materials include graphene, transition metal dichalcogenides (TMDS), black phosphorus, black P(1-x) Asx , boron nitride (BN) and so forth. Owing to their various bandgaps, 2D materials have been utilized for photonics and optoelectronics. Photodetectors based on 2D materials with different structures and detection mechanisms have been established and present excellent performance. In this Review, localized field enhanced 2D material photodetectors (2DPDs) are introduced with sensitivity over the spectrum from ultraviolet, visible to infrared in the sight of the influence of device structure on photodetector performance instead of directly illustrating the detection mechanisms. Six types of localized fields are summarized. They are: ferroelectric field, photogating electric field, floating gate induced electrostatic field, interlayer built-in field, localized optical field, and photo-induced temperature gradient field, respectively. These localized fields are proved to effectively promote the detection ability of 2DPDs by suppressing background noise, enhancing optical absorption, improving electron-hole separation efficiency, amplifying photoelectric gain and/or extending the detection range.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/smll.201700894

Recent Progress on Localized Field Enhanced Two-dimensional Material Photodetectors from Ultraviolet—Visible to Infrared

Active metamaterials and metadevices: a review

Achieving strong coupling between plasmonic oscillators can significantly modulate their intrinsic optical properties. Here, we report the direct observation of ultrafast plasmonic hot electron transfer from an Au grating array to an MoS2 monolayer in the strong coupling regime between localized surface plasmons (LSPs) and surface plasmon polaritons (SPPs). By means of femtosecond pump-probe spectroscopy, the measured hot electron transfer time is approximately 40 fs with a maximum external quantum yield of 1.65%. Our results suggest that strong coupling between LSPs and SPPs has synergetic effects on the generation of plasmonic hot carriers, where SPPs with a unique nonradiative feature can act as an ‘energy recycle bin’ to reuse the radiative energy of LSPs and contribute to hot carrier generation. Coherent energy exchange between plasmonic modes in the strong coupling regime can further enhance the vertical electric field and promote the transfer of hot electrons between the Au grating and the MoS2 monolayer. Our proposed plasmonic strong coupling configuration overcomes the challenge associated with utilizing hot carriers and is instructive in terms of improving the performance of plasmonic opto-electronic devices. A device that taps into two types of surface plasmon waves offers new opportunities to transform light energy into speedy semiconductor charges. When surface plasmons are confined to nanoscale dimensions, they can rapidly decay and produce “hot” electrons with high kinetic energy. Zheyu Fang from Peking University in Beijing, China, and colleagues have constructed a metal–insulator–metal sandwich structure that improves harvesting of hot electrons for applications including photodetectors. To increase extraction under laser excitation, the team coated the insulator with an electron-attracting molybdenum disulfide monolayer. They also identified surface plasmon polaritons—mobile waves at the metal–insulator interface—in the sandwich structure using a gold grating with variable dimensions as the upper metal layer. Laser conditions that coupled mobile and localized plasmons promoted hot electron production instead of thermal dissipation.

Direct observation of ultrafast plasmonic hot electron transfer in the strong coupling regime.

The manipulation of light in an integrated circuit is crucial for the development of high-speed electro-optic devices. Recently, molybdenum disulfide (MoS2) monolayers generated broad interest for the optoelectronics because of their huge exciton binding energy, tunable optical emission, direct electronic band-gap structure, etc. Miniaturization and multifunctionality of electro-optic devices further require the manipulation of light–matter interaction at the single-nanoparticle level. The strong exciton–plasmon interaction that is generated between the MoS2 monolayers and metallic nanostructures may be a possible solution for compact electro-optic devices at the nanoscale. Here, we demonstrate a nanoplasmonic modulator in the visible spectral region by combining the MoS2 monolayers with a single Au nanodisk. The narrow MoS2 excitons coupled with broad Au plasmons result in a deep Fano resonance, which can be switched on and off by applying different gate voltages on the MoS2 monolayers. A reversible disp...

Single-Nanoparticle Plasmonic Electro-optic Modulator Based on MoS2 Monolayers.

Plasmonic-Functionalized Broadband Perovskite Photodetector

Active Control of Plasmon–Exciton Coupling in MoS2–Ag Hybrid Nanostructures

Optical chirality occurs when materials interact differently with light in a specific circular polarization state. Chiroptical phenomena inspire wide interdisciplinary investigations, which require advanced designs to reach strong chirality for practical applications. The development of artificial intelligence provides a new vision for the manipulation of light-matter interaction beyond the theoretical interpretation. Here, we report a self-consistent framework named the Bayesian optimization and convolutional neural network that combines Bayesian optimization and deep convolutional neural network algorithms to calculate and optimize optical properties of metallic nanostructures. Both electric-field distributions at the near field and reflection spectra at the far field are calculated and self-learned to suggest better structure designs and provide possible explanations for the origin of the optimized properties, which enables wide applications for future nanostructure analysis and design.

Bowen Li

Papers

Direct observation of ultrafast plasmonic hot electron transfer in the strong coupling regime.

Single-Nanoparticle Plasmonic Electro-optic Modulator Based on MoS2 Monolayers.

Plasmonic-Functionalized Broadband Perovskite Photodetector

Active Control of Plasmon–Exciton Coupling in MoS2–Ag Hybrid Nanostructures

Self-Learning Perfect Optical Chirality via a Deep Neural Network.