We investigate the ultrafast relaxation dynamics of hot Dirac fermionic quasiparticles in multilayer epitaxial graphene using ultrafast optical differential transmission spectroscopy. We observe differential transmission spectra which are well described by interband transitions with no electron-hole interaction. Following the initial thermalization and emission of high-energy phonons, the electron cooling is determined by electron-acoustic phonon scattering, found to occur on the time scale of 1 ps for highly doped layers, and 4-11 ps in undoped layers. The spectra also provide strong evidence for the multilayer structure and doping profile of thermally grown epitaxial graphene on SiC.
The combination of its high electron mobility, broadband absorption and ultrafast luminescence make graphene attractive for optoelectronic and photonic applications, including transparent electrodes, mode-locked lasers and high-speed optical modulators. Photo-excited carriers that have not cooled to the temperature of the graphene lattice are known as hot carriers, and may limit device speed and energy efficiency. However, their roles in charge and energy transport are not fully understood. Here, we use time-resolved scanning photocurrent microscopy to demonstrate that hot carriers, rather than phonons, dominate energy transport across a tunable graphene p-n junction excited by ultrafast laser pulses. The photocurrent response time varies from 1.5 ps at room temperature to 4 ps at 20 K, implying a fundamental bandwidth of ∼500 GHz (refs 12, 13, 21). Gate-dependent pump-probe measurements demonstrate that both thermoelectric and built-in electric field effects contribute to the photocurrent, with the contribution from each depending on the junction configuration. The photocurrent produced by a single pulsed laser also displays multiple polarity reversals as a function of carrier density, which is a possible signature of impact ionization.
We investigate the valley-related carrier dynamics in monolayer molybdenum disulfide using helicity-resolved nondegenerate ultrafast pump-probe spectroscopy at the vicinity of the high-symmetry K point under the temperature down to 78 K. Monolayer molybdenum disulfide shows remarkable transient reflection signals, in stark contrast to bilayer and bulk molybdenum disulfide due to the enhancement of many-body effect at reduced dimensionality. The helicity-resolved ultrafast time-resolved result shows that the valley polarization is preserved for only several picoseconds before the scattering process makes it undistinguishable. We suggest that the dynamical degradation of valley polarization is attributable primarily to the exciton trapping by defect states in the exfoliated molybdenum disulfide samples. Our experiment and a tight-binding model analysis also show that the perfect valley circular dichroism selectivity is fairly robust against disorder at the K point but quickly decays from the high-symmetry point in the momentum space in the presence of disorder.
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