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Register a new userIntense femtosecond photoexcitation of bulk and monolayer MoS2
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Ioannis Paradisanos
Publication date
2015
fields
Physics
and research's language is
English
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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 role of two-photon versus one photon absorption effects is discussed.
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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.
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 resonance of TPA.
Two-dimensional semiconductors such as MoS2 are an emerging material family with wide-ranging potential applications in electronics, optoelectronics and energy harvesting. Large-area growth methods are needed to open the way to the applications. While significant progress to this goal was made, control over lattice orientation during growth still remains a challenge. This is needed in order to minimize or even avoid the formation of grain boundaries which can be detrimental to electrical, optical and mechanical properties of MoS2 and other 2D semiconductors. Here, we report on the uniform growth of high-quality centimeter-scale continuous monolayer MoS2 with control over lattice orientation. Using transmission electron microscopy we show that the monolayer film is composed of coalescing single islands that share a predominant lattice orientation due to an epitaxial growth mechanism. Raman and photoluminescence spectra confirm the high quality of the grown material. Optical absorbance spectra acquired over large areas show new features in the high-energy part of the spectrum, indicating that MoS2 could also be interesting for harvesting this region of the solar spectrum and fabrication of UV-sensitive photodetectors. Even though the interaction between the growth substrate and MoS2 is strong enough to induce lattice alignment, we can easily transfer the grown material and fabricate field-effect transistors on SiO2 substrates showing mobility superior to the exfoliated material.
We demonstrate that the temperature and doping dependencies of the photoluminescence (PL) spectra of a doped MoS2 monolayer have several peculiar characteristics defined by trion radiative decay. While only zero-momentum exciton states are coupled to light, radiative recombination of non-zero momentum trions is also allowed. This leads to an asymmetric broadening of the trion spectral peak and redshift of the emitted light with increasing temperature. The lowest energy trion state is dark, which is manifested by the sharply non-monotonic temperature dependence of the PL intensity. Our calculations combine the Dirac model for the single-particle states, the parameters for which are obtained from the first principle calculations, and the direct solution of the three-particle problem within the Tamm-Dancoff approximation. The numerical results are well captured by a simple model that yields analytical expressions for the temperature dependencies of the PL spectra.
Interactions between two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analogue in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMD MoS2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 meV and 40 meV. In addition, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.
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