In this letter, we present non-degenerate ultrafast optical pump-probe studies of the carrier recombination dynamics in MoS 2 monolayers. By tuning the probe to wavelengths much longer than the exciton line, we make the probe transmission sensitive to the total population of photoexcited electrons and holes. Our measurement reveals two distinct time scales over which the photoexcited electrons and holes recombine; a fast time scale that lasts ∼2 ps and a slow time scale that lasts longer than ∼100 ps. The temperature and the pump fluence dependence of the observed carrier dynamics are consistent with defect-assisted recombination as being the dominant mechanism for electron-hole recombination in which the electrons and holes are captured by defects via Auger processes. Strong Coulomb interactions in two dimensional atomic materials, together with strong electron and hole correlations in two dimensional metal dichalcogenides, make Auger processes particularly effective for carrier capture by defects. We present a model for carrier recombination dynamics that quantitatively explains all features of our data for different temperatures and pump fluences. The theoretical estimates for the rate constants for Auger carrier capture are in good agreement with the experimentally determined values. Our results underscore the important role played by Auger processes in two dimensional atomic materials. Electron-Hole Recombination Dynamics in Monolayer MoS 2Two-dimensional (2D) transition metal dichalcogenides (TMDs) have emerged as interesting materials both from the perspective of basic science as well as applications [1][2][3][4][5][6][7] . Applications of these materials in electronics and optoelectronics have been extensively explored in recent years 5,6,[8][9][10][11][12][13][14][15][16][17][18] . arXiv:1409.4518v1 [cond-mat.mes-hall] 16 Sep 20142 The bandgaps of most TMDs are in the visible to near-IR wavelength range, making these materials suitable for light emitters, photodetectors, and solar cells 5,10,13,[16][17][18] . In addition, optical control of valley polarization in TMDs has opened opportunities for devices based on the valley degree of freedom 6 . The lifetimes of electrons and holes are critical to all the proposed and demonstrated TMD optoelectronic devices. Despite the recent progress, carrier lifetimes and nonradiative electron-hole recombination mechanisms in TMDs remain poorly understood. Developing a better understanding of the non-radiative electron-hole recombination mechanisms in TMDs is especially important because the reported quantum efficiencies in both TMD light emitters and detectors are extremely poor; in the .0001-.01 range 10,13,[16][17][18] . Similar quantum efficiencies for TMDs have been observed in photoluminescence experiments 2,3 . In contrast, the best reported internal and external quantum efficiencies observed in photoluminescence in III-V semiconductors exceed 0.9 and 0.7, respectively 19 . Therefore, most of the electrons and holes injected either electrically or optically i...
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.
We present results on photoexcited carrier lifetimes in few-layer transition metal dichalcogenide MoS 2 using nondegenerate ultrafast optical pump-probe technique. Our results show a sharp increase of the carrier lifetimes with the number of layers in the sample. Carrier lifetimes increase from few tens of picoseconds in monolayer samples to more than a nanosecond in 10-layer samples. The inverse carrier lifetime was found to scale according to the probability of the carriers being present at the surface layers, as given by the carrier wavefunction in few layer samples, which can be treated as quantum wells. The carrier lifetimes were found to be largely independent of the temperature and the inverse carrier lifetimes scaled linearly with the photoexcited carrier density. These observations are consistent with defect-
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.
Aspergillus fumigatus is able to internalize into lung epithelial cells to escape from immune attack for further dissemination. We previously reported that gliotoxin, a major mycotoxin of A. fumigatus , promotes this internalization; however, the mechanism remained unclear. Here, we report that gliotoxin is able to induce cofilin phosphorylation in A549 type II human pneumocytes. Either too high or too low a level of cofilin phosphorylation blocked the gliotoxin-induced actin cytoskeleton rearrangement and A. fumigatus internalization. LIM domain kinase 1 (LIMK1) and its upstream small GTPases (Cdc42 and RhoA, but not Rac1) predominantly mediated the gliotoxin-induced cofilin phosphorylation and A. fumigatus internalization. Simultaneously, gliotoxin significantly stimulated an increase in cAMP; however, adding an antagonist of PKA did not block gliotoxin-induced A. fumigatus internalization. In vivo , exogenous gliotoxin helped gliotoxin synthesis deficient strain gliPΔ invade into the lung tissue and the lung fungal burden increased markedly in immunosuppressed mice. In conclusion, these data revealed a novel role of gliotoxin in inducing cofilin phosphorylation mostly through the Cdc42/RhoA-LIMK1 signaling pathway to promote actin cytoskeleton rearrangement and internalization of A. fumigatus into type II human pneumocytes.
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