We measure the optical absorption spectra and optical conductivities of excitons and trions in monolayers of metal dichalcogenide MoS2 and compare the results with theoretical models. Our results show that the Wannier-Mott model for excitons with modifications to account for small exciton radii and large exciton relative wavefunction spread in momentum space, phase space blocking due to Pauli exclusion in doped materials, and wavevector dependent dielectric constant gives results that agree well with experiments. The measured exciton optical absorption spectra are used to obtain experimental estimates for the exciton radii that fall in the 7 − 10Å range and agree well with theory. The measured trion optical absorption spectra are used to obtain values for the trion radii that also agree well with theory. The measured values of the exciton and trion radii correspond to binding energies that are in good agreement with values obtained from first principles calculations.
We present results on the radiative lifetimes of excitons and trions in a monolayer of metal dichalcogenide MoS2. The small exciton radius and the large exciton optical oscillator strength result in radiative lifetimes in the 0.18-0.30 ps range for excitons that have small in-plane momenta and couple to radiation. Average lifetimes of thermally distributed excitons depend linearly on the exciton temperature and can be in the few picoseconds range at small temperatures and more than a nanosecond near room temperature. Localized excitons exhibit lifetimes in the same range and the lifetime increases as the localization length decreases. The radiative lifetimes of trions are in the hundreds of picosecond range and increase with the increase in the trion momentum. Average lifetimes of thermally distributed trions increase with the trion temperature as the trions acquire thermal energy and larger momenta. We expect our theoretical results to be applicable to most other 2D transition metal dichalcogenides.
The strong light emission and absorption exhibited by single atomic layer transitional metal dichalcogenides in the visible to near-infrared wavelength range make them attractive for optoelectronic applications. In this work, using two-pulse photovoltage correlation technique, we show that monolayer molybdenum disulfide photodetector can have intrinsic response times as short as 3 ps implying photodetection bandwidths as wide as 300 GHz. The fast photodetector response is a result of the short electron–hole and exciton lifetimes in this material. Recombination of photoexcited carriers in most two-dimensional metal dichalcogenides is dominated by nonradiative processes, most notable among which is Auger scattering. The fast response time, and the ease of fabrication of these devices, make them interesting for low-cost ultrafast optical communication links.
The strong Coulomb interactions and the small exciton radii in two-dimensional metal dichalcogenides can result in very fast capture of electrons and holes of excitons by mid-gap defects from Auger processes. In the Auger processes considered here, an exciton is annihilated at a defect site with the capture of the electron (or the hole) by the defect and the hole (or the electron) is scattered to a high energy. In the case of excitons, the probability of finding an electron and a hole near each other is enhanced many folds compared to the case of free uncorrelated electrons and holes. Consequently, the rate of carrier capture by defects from Auger scattering for excitons in metal dichalcogenides can be 100-1000 times larger than for uncorrelated electrons and holes for carrier densities in the 10 11 -10 12 cm −2 range. We calculate the capture times of electrons and holes by defects and show that the capture times can be in the sub-picosecond to a few picoseconds range. The capture rates exhibit linear as well as quadratic dependence on the exciton density. These fast time scales agree well with the recent experimental observations and point to the importance of controlling defects in metal dichalcogenides for optoelectronic applications.
Current methods of chemical vapour deposition (CVD) of graphene on copper are complicated by multiple processing steps and by high temperatures required in both preparing the copper and inducing subsequent film growth. Here we demonstrate a plasma-enhanced CVD chemistry that enables the entire process to take place in a single step, at reduced temperatures (o420°C), and in a matter of minutes. Growth on copper foils is found to nucleate from arrays of well-aligned domains, and the ensuing films possess sub-nanometre smoothness, excellent crystalline quality, low strain, few defects and roomtemperature electrical mobility up to (6.0 ± 1.0) Â 10 4 cm 2 V À 1 s À 1 , better than that of large, single-crystalline graphene derived from thermal CVD growth. These results indicate that elevated temperatures and crystalline substrates are not necessary for synthesizing high-quality graphene.
Graphene, a two-dimensional material with a high mobility and a tunable conductivity, is uniquely suited for plasmonics. The frequency dispersion of plasmons in bulk graphene has been studied both theoretically and experimentally, whereas no theoretical models have been reported and tested against experiments for confined plasmon modes in graphene microstructures. In this paper, we present measurements as well as analytical and computational models for such confined modes. We show that plsmon modes can be described by an eigenvalue equation. We compare the experiments with the theory for plasmon modes in arrays of graphene strips and demonstrate a good agreement. This comparison reveals the important role played by interaction among the plasmon modes of neighboring graphene structures.
A variety of different graphene plasmonic structures and devices have been proposed and demonstrated experimentally. Plasmon modes in graphene microstructures interact strongly via the depolarization fields. An accurate quantitative description of the coupling between plasmon modes is required for designing and understanding complex plasmonic devices. Drawing inspiration from microphotonics, we present a coupled-mode theory for graphene plasmonics in which the plasmon eigenmodes of a coupled system are expressed in terms of the plasmon eigenmodes of its uncoupled sub-systems. The coupled-mode theory enables accurate computation of the coupling between the plasmon modes and of the resulting dynamics. We compare theory with experiments performed on the plasmon modes in coupled arrays of graphene strips. In experiments, we tune the coupling by changing the spacing between the graphene strips in the array. Our results show that the coupling parameters obtained from the coupled-mode theory and the plasmon frequency changes resulting from this coupling agree very well with experiments. The work presented here provides a framework for designing and understanding coupled graphene plasmonic structures.Graphene, a single layer of carbon atoms arranged in honeycomb lattice, has emerged as an important material for plasmonics [1][2][3][4][5][6][7][8]. The high carrier mobility and the widely tunable conductivity in graphene together with the ability to fabricate graphene microstructures of different sizes implies that plasmons in graphene structures can have high quality factors and frequencies tunable from a few THz to more than 100 THz. Graphene plasmonic structures have the potential to form building blocks for novel THz/IR devices such as detectors, emitters, oscillators, switches, filters, and sensors. Several theoretical works have explored techniques to compute the modes in individual as well as in arrays of graphene plasmon resonators [9][10][11][12][13][14]. In order to realize the full potential of graphene plasmonics, and develop the ability to combine several graphene plasmonic resonators and engineer complex device structures, suitable techniques are needed model the interactions between plasmonic resonators in simple, yet effective and accurate, ways. In the field of microphotonics, the equivalent role is played by coupled-mode theories [15,16]. In coupled-mode theories, the field of a coupled system is expanded in terms of the fields of the eigenmodes of its uncoupled subsystems [15,16]. Accurate computation of the coupling parameters and the response of the coupled system without detailed first-principles electromagnetic simulations are few of the main benefits of coupled-mode theories. Coupled-mode theories have proven to be extremely effective tools in designing and understanding complex optical integrated structures [17]. In the field of graphene plasmonics, complex devices incorporating several coupled plasmonic resonators have been proposed and demonstrated for various applications [1,2,[18][19][20][21]...
We present results on the rates of interlayer energy transfer between excitons in two-dimensional transition metal dichalcogenides (TMDs). We consider both radiative (mediated by real photons) and non-radiative (mediated by virtual photons) mechanisms of energy transfer using a unified Green's function approach that takes into account modification of the exciton energy dispersions as a result of interactions. The large optical oscillator strengths associated with excitons in TMDs result in very fast energy transfer rates. The energy transfer times depend on the exciton momentum, exciton linewidth, and the interlayer separation and can range from values less than 100 femtoseconds to more than tens of picoseconds. Whereas inside the light cone the energy transfer rates of longitudinal and transverse excitons are comparable, outside the light cone the energy transfer rates of longitudinal excitons far exceed those of transverse excitons. Average energy transfer times for a thermal ensemble of longitudinal and transverse excitons is temperature dependent and can be smaller than a picosecond at room temperature for interlayer separations smaller than 10 nm. Energy transfer times of localized excitons range from values less than a picosecond to several tens of picoseconds. When the exciton scattering and dephasing rates are small, energy transfer dynamics exhibit coherent oscillations. Our results show that electromagnetic interlayer energy transfer can be an efficient mechanism for energy exchange between TMD monolayers.
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