Jason Horng, Eric W. Martin, Yu-Hsun Chou, Emmanuel Courtade, Tsu-chi Chang, Chu-Yuan Hsu, Michael-Henr Wentzel, Hanna G. Ruth, Tien-chang Lu, Steven T. Cundiff… 展开作者
Jason Horng, Eric W. Martin, Yu-Hsun Chou, Emmanuel Courtade, Tsu-chi Chang, Chu-Yuan Hsu, Michael-Henr Wentzel, Hanna G. Ruth, Tien-chang Lu, Steven T. Cundiff, Feng Wang, Hui Deng
Optical absorption is one of fundamental light-matter interactions. In most materials, optical absorption is a weak perturbation to the light. In this regime, absorption and emission are irreversible, incoherent processes due to strong damping. Excitons in monolayer transition metal dichalcogenides, however, interact strongly with light, leading to optical absorption in the non-perturbative regime where coherent re-emission of the light has to be considered. Between the incoherent and coherent limits, we show that a robust critical coupling condition exists, leading to perfect optical absorption. Up to 99.6% absorption is measured in a sub-nanometer thick MoSe2 monolayer placed in front of a mirror. The perfect absorption is controlled by tuning the exciton-phonon, exciton-exciton, and exciton-photon interactions by temperature, pulsed laser excitation, and a movable mirror, respectively. Our work suggests unprecedented opportunities for engineering exciton-light interactions using two-dimensional atomically thin crystals, enabling novel photonic applications including ultrafast light modulators and sensitive optical sensing.
The atomic structure of graphene edges is critical in determining the electrical, magnetic, and chemical properties of truncated graphene structures, notably nanoribbons. Unfortunately, graphene edges are typically far from ideal and suffer from atomic-scale defects, structural distortion, and unintended chemical functionalization, leading to unpredictable properties. Here we report that graphene edges fabricated by electron-beam-initiated mechanical rupture or tearing in high vacuum are clean and largely atomically perfect, oriented in either the armchair or zigzag direction. Via aberration-c…
A simple tight-binding theoretical model is proposed for spin dependent, current-in-plane transport in highly coherent spin valve structures under specularity conditions. Using quantum-mechanically coherent and spatially quantized Fermi states in the considered multilayered system, a system of partial Boltzmann kinetic equations is built for relevant subbands to yield the expressions for conductance in parallel or antiparallel spin valve states and thus for the magneto-conductance. It is shown that specularity favors the magnetoresistance to reach its theoretical maximum for this structure clo…
We perform absorption and photoluminescence spectroscopy of trions in hBN-encapsulated WSe$_2$, WS$_2$, MoSe$_2$, and MoS$_2$ monolayers, depending on temperature. The different trends for W- and Mo-based materials are excellently reproduced considering a Fermi-Dirac distribution of bright and dark trions. We find a dark trion, $\rm{X_D^-}$ 19 meV $\textit{below}$ the lowest bright trion, $\rm{X}_1^-$ in WSe$_2$ and WS$_2$. In MoSe$_2$, $\rm{X_D^-}$ lies 6 meV $\textit{above}$ $\rm{X}_1^-$, while $\rm{X_D^-}$ and $\rm{X}_1^-$ almost coincide in MoS$_2$. Our results agree with GW-BSE $\textit{a…
The ability to modulate light at high speeds is of paramount importance for telecommunications, information processing, and medical imaging technologies. This has stimulated intense efforts to master optoelectronic switching at visible and near-infrared frequencies, although coping with current computer speeds in integrated architectures still remains a major challenge. As a partial success, midinfrared light modulation has been recently achieved through gating patterned graphene. Here we show that atomically thin noble metal nanoislands can extend optical modulation to the visible and near-in…
Magnetism in semiconductor two-dimensional (2D) materials is gaining popularity due to its potential application in memory devices, sensors, spintronic and biomedical applications. Here, 2D Cobalt Telluride (CoTe) has been synthesized from its bulk crystals using a simple and scalable liquid-phase exfoliation method. The atomically thin CoTe shows over four hundred times enhancement in its magnetic saturation values compared to the bulk form. The UV-Vis absorption spectra reveal superior absorption in the high energy region, suggesting a semiconducting nature. Furthermore, we explain bandgap a…
Above-light-line surface plasmon polaritons can arise at the interface between a metal and epsilon-near-zero metamaterial. This unique feature induces unusual fast-wave non-radiative modes in a epsilon-near-zero material/metal bilayer. Excitation of this peculiar mode leads to wide-angle perfect absorption in low-loss ultrathin metamaterials. The ratio of the perfect absorption wavelength to the thickness of the epsilon-near-zero metamaterial can be as high as 10^4; the electromagnetic energy can be confined in a layer as thin as λ/10000. Unlike conventional fast-wave leaky modes, these fast-w…
Van der Waals junctions of two-dimensional materials with an atomically sharp interface open up unprecedented opportunities to design and study functional heterostructures. Semiconducting transition metal dichalcogenides have shown tremendous potential for future applications due to their unique electronic properties and strong light-matter interaction. However, many important optoelectronic applications, such as broadband photodetection, are severely hindered by their limited spectral range and reduced light absorption. Here, we present a p-g-n heterostructure formed by sandwiching graphene w…
We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photo…
Atomically-thin molybdenum disulfide is emerging as a new nanomaterial with potential applications in the fields of electronic and photonics. Charge carrier dynamics plays an essential role in determining its electronic and optical properties. We report spatially and temporally resolved pump-probe studies of charge carriers in atomically-thin molybdenum disulfide samples fabricated by mechanical exfoliation. Carriers are injected by interband absorption of a 390-nm pump pulse and detected by measuring differential reflection of a time-delayed and spatially-scanned probe pulse that is tuned to …
Relating the electromagnetic scattering and absorption properties of an individual particle to the reflection and transmission coefficients of a two-dimensional material composed of these particles is a crucial concept that has driven both fundamental and applied physics. It is at the heart of both the characterization of material properties as well as the phase and amplitude engineering of a wave. Here we propose a multipolar description of the reflection and transmission coefficients across a monolayer of particles using a vector spherical harmonic decomposition. This enables us to provide a…
Magnetic and spintronic media have offered fundamental scientific subjects and technological applications. Magneto-optic Kerr effect (MOKE) microscopy provides the most accessible platform to study the dynamics of spins, magnetic quasi-particles, and domain walls. However, in the research of nanoscale spin textures and state-of-the-art spintronic devices, optical techniques are generally restricted by the extremely weak magneto-optical activity and diffraction limit. Highly sophisticated, expensive electron microscopy and scanning probe methods thus have come to the forefront. Here, we show th…
We present an electrostatic theory of band gap renormalization in atomically-thin semiconductors that captures the strong sensitivity to the surrounding dielectric environment. In particular, our theory aims to correct known band gaps, such as that of the three-dimensional bulk crystal. Combining our quasiparticle band gaps with an effective mass theory of excitons yields environmentally-sensitive optical gaps as would be observed in absorption or photoluminescence. For an isolated monolayer of MoS$_2$, the presented theory is in good agreement with ab initio results based on the GW approximat…
This work reports the incompatibility of the Stokes relation for time reversibility of wave's propagation and the usage of complex atomic form-factor in diffraction theories. The implications behind a diffraction theory that obeys the Stokes relation is discussed.
We exploited graphene nanoribbons based meta-surface to realize coherent perfect absorption (CPA) in the mid-infrared regime. It was shown that quasi-CPA frequencies, at which CPA can be demonstrated with proper phase modulations, exist for the graphene meta-surface with strong resonant behaviors. The CPA can be tuned substantially by merging the geometric design of the meta-surface and the electrical tunability of graphene. Furthermore, we found that the graphene nanoribbon meta-surface based CPA is realizable with experimental graphene data. The findings of CPA with graphene meta-surface can…
The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N = 1, 2, ... 6 S-Mo-S monolayers have been investigated by optical spectroscopy. Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the material's electronic structure. With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 0.6 eV. This leads to a crossover to a direct-gap material in the limit of the single monolayer. Unlike the bulk…
Silicon (Si) is one of the most extensively studied materials owing to its significance to semiconductor science and technology. While efforts to find a new three-dimensional (3D) Si crystal with unusual properties have made some progress, its two-dimensional (2D) phases have not yet been explored as much. Here, based on a newly developed systematic $ab$ $initio$ materials searching strategy, we report a series of novel 2D Si crystals with unprecedented structural and electronic properties. The new structures exhibit perfectly planar outermost surface layers of a distorted hexagonal network wi…
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 …
Metallic layers are known to be used for the suppression of wave transmission when their thickness is sufficiently higher than the skin depth of metal. If in addition to blocking the transmission, metallic layers have the feature of blocking the reflection, too, they would make perfect absorbers. In this work, we propose an experimental approach of using a single thin layer of Manganese (Mn) as both the transmission suppresser and the reflection suppresser. This approach leads to obtaining lithography-free ultra-broadband perfect absorption in an ultra-wide spectrum ranging from Ultraviolet (U…
We report successful deposition of high quantum efficiency (QE) bialkali antimonide K2CsSb photocathodes on graphene films. The results pave a pathway towards an ultimate goal of encapsulating technologically-relevant photocathodes for accelerator technology with an atomically-thin protecting layer to enhance lifetime while minimizing QE losses. A QE of 17 % at ~3.1 eV (405 nm) is the highest value reported so far on graphene substrates and is comparable to that obtained on stainless steel and nickel reference substrates. The spectral responses of the photocathodes on graphene exhibit signatur…
Near-perfect absorbers (NPAs) efficiently absorb visible light with a layered nanostructure that is thinner than the diffusion lengths of photogenerated charge carriers. We overcame existing limitations in fabricating their nanoparticulate surface by depositing \textit{plasmene}, a tightly-packed two-dimensional lattice of metal nanoparticles formed through self-assembly. The plasmene NPAs absorb up to 98\% of incident visible light, with modelling showing the improvement on existing NPAs arises from the structural ordering of the plasmene. We also demonstrate control of NPAs' absorption profi…
We report experimental observation of electrically-tunable coherent perfect absorption (CPA) of terahertz (THz) radiation in graphene. We develop a reflection-type tunable THz cavity formed by a large-area graphene layer, a metallic reflective electrode and an electrolytic medium in between. Ionic gating in the THz cavity allows us to tune the Fermi energy of graphene up to 1eV and to achieve critical coupling condition at 2.8 THz with absorption of 99%. With the enhanced THz absorption, we were able to measure the Fermi energy dependence of the transport scattering time of highly doped graphe…
Using the density functional theory of electronic structure, we compute the anisotropic dielectric response of bulk black phosphorus subject to strain. Employing the obtained permittivity tensor, we solve Maxwell's equations and study the electromagnetic response of a layered structure comprising a film of black phosphorus stacked on a metallic substrate. Our results reveal that a small compressive or tensile strain, $\sim 4\%$, exerted either perpendicular or in the plane to the black phosphorus growth direction, efficiently controls the epsilon-near-zero response, and allows a perfect absorp…
Geometrical confinement effect in exfoliated sheets of layered materials leads to significant evolution of energy dispersion with decreasing layer thickness. Molybdenum disulphide (MoS2) was recently found to exhibit indirect to direct gap transition when the thickness is reduced to a single monolayer. This leads to remarkable enhancement in the photoluminescence efficiency, which opens up new opportunities for the optoelectronic applications of the material. Here we report differential reflectance and photoluminescence (PL) spectra of mono- to few-layer WS2 and WSe2 that indicate that the ban…
Optoelectronic devices based on graphene and other two-dimensional (2D) materials, such as transition metal dichalcogenides (TMDs) are the focus of wide research interest. The characterization these emerging atomically thin materials and devices strongly relies on a set of measurements involving both optical and electronic instrumentation ranging from scanning photocurrent mapping to Raman and photoluminescence (PL) spectroscopy. Furthermore, proof-of-concept devices are usually fabricated from micro-meter size flakes, requiring microscopy techniques to characterize them. Current state-of-the-…
The realization of mixtures of excitons and charge carriers in van-der-Waals materials presents a new frontier for the study of the many-body physics of strongly interacting Bose-Fermi mixtures. In order to derive an effective low-energy model for such systems, we develop an exact diagonalization approach based on a discrete variable representation that predicts the scattering and bound state properties of three charges in two-dimensional transition metal dichalcogenides. From the solution of the quantum mechanical three-body problem we thus obtain the bound state energies of excitons and trio…
We demonstrate, for the first time, a spatially dependent metamaterial perfect absorber operating in the infrared regime. We achieve an experimental absorption of 97% at a wavelength of 6.0 microns, and our results agree well with numerical full-wave simulations. By using two different metamaterial sublattices we experimentally demonstrate a spatial and frequency varying absorption which may have many relevant applications including hyperspectral sub-sampling imaging
