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Register a new userValley Carrier Dynamics in Monolayer Molybdenum Disulphide from Helicity Resolved Ultrafast Pump-probe Spectroscopy
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We investigate the valley related carrier dynamics in monolayer MoS2 using helicity resolved non-degenerate ultrafast pump-probe spectroscopy at the vicinity of the high-symmetry K point under the temperature down to 78 K. Monolayer MoS2 shows remarkable transient reflection signals, in stark contrast to bilayer and bulk MoS2 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 ps before 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 MoS2 samples. Our experiment and a tight-binding model analysis also show that the perfect valley CD 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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We explore the influence of the nanoporous structure on the thermal relaxation of electrons and holes excited by ultrashort laser pulses ($sim 7$ fs) in thin gold films. Plasmon decay into hot electron-hole pairs results in the generation of a Fermi-Dirac distribution thermalized at a temperature $T_{mathrm{e}}$ higher than the lattice temperature $T_{mathrm{l}}$. The relaxation times of the energy exchange between electrons and lattice, here measured by pump-probe spectroscopy, is slowed down by the nanoporous structure, resulting in much higher peak $T_{mathrm{e}}$ than for bulk gold films. The electron-phonon coupling constant and the Debye temperature are found to scale with the metal filling factor $f$ and a two-temperature model reproduces the data. The results open the way for electron temperature control in metals by engineering of the nanoporous geometry.
Optical pump-probe spectroscopy is a powerful tool for the study of non-equilibrium electronic dynamics and finds wide applications across a range of fields, from physics and chemistry to material science and biology. However, a shortcoming of conventional pump-probe spectroscopy is that photoinduced changes in transmission, reflection and scattering can simultaneously contribute to the measured differential spectra, leading to ambiguities in assigning the origin of spectral signatures and ruling out quantitative interpretation of the spectra. Ideally, these methods would measure the underlying dielectric function (or the complex refractive index) which would then directly provide quantitative information on the transient excited state dynamics free of these ambiguities. Here we present and test a model independent route to transform differential transmission or reflection spectra, measured via conventional optical pump-probe spectroscopy, to changes in the quantitative transient dielectric function. We benchmark this method against changes in the real refractive index measured using time-resolved Frequency Domain Interferometry in prototypical inorganic and organic semiconductor films. Our methodology can be applied to existing and future pump-probe data sets, allowing for an unambiguous and quantitative characterisation of the transient photoexcited spectra of materials. This in turn will accelerate the adoption of pump-probe spectroscopy as a facile and robust materials characterisation and screening tool.
The conducting polymer polyaniline (PANI) has a wide range of optoelectronic applications due to its unique electronic and optical characteristics. Although extensive works have been performed to understand the equilibrium properties, the nature of the charge type that governs its non-equilibrium optical response has been barely understood; a number of studies have debated the nature of photo-generated charge type in PANI, specifically whether it is polaron or exciton based. Here, we report experimental evidence that the charge relaxation dynamics of PANI are dominated by excitons. Utilizing ultrafast spin-resolved pump-probe spectroscopy, we observed that PANI charge dynamics are strongly spin-polarized, exhibiting a spin Pauli-blocking effect. Investigations including both spin-independent and spindependent dynamics reveal that there is no spin-flip process involved in charge relaxation. This provides compelling evidence of an exciton-dominated photo-response in PANI.
Graphene is an ideal material to study fundamental Coulomb- and phonon-induced carrier scattering processes. Its remarkable gapless and linear band structure opens up new carrier relaxation channels. In particular, Auger scattering bridging the valence and the conduction band changes the number of charge carriers and gives rise to a significant carrier multiplication - an ultrafast many-particle phenomenon that is promising for the design of highly efficient photodetectors. Furthermore, the vanishing density of states at the Dirac point combined with ultrafast phonon-induced intraband scattering results in an accumulation of carriers and a population inversion suggesting the design of graphene-based terahertz lasers. Here, we review our work on the ultrafast carrier dynamics in graphene and Landau-quantized graphene is presented providing a microscopic view on the appearance of carrier multiplication and population inversion.
In high-resolution core-valence-valence (CVV) Auger electron spectroscopy from the surface of a solid at thermal equilibrium, the main correlation satellite, visible in the case of strong valence-electron correlations, corresponds to a bound state of the two holes in the final state of the CVV Auger process. We discuss the physical significance of this satellite in nonequilibrium pump-probe Auger spectroscopy by numerical analysis of a single-band Hubbard-type model system including core states and a continuum of high-energy scattering states. It turns out that the spectrum of the photo-doped system, due to the increased double occupancy, shares features with the equilibrium spectrum at higher fillings. The pumping of doublons can be watched when working with overlapping pulses at short $Delta t$. For larger pump-probe delays $Delta t$ and on the typical femtosecond time scale for electronic relaxation processes, spectra are hardly $Delta t$-dependent, reflecting the high stability of bound two-hole states for strong Hubbard-$U$. We argue that taking into account the spatial expansion of single-particle orbitals when these are doubly occupied, as described by the dynamical Hubbard model, produces an oscillation of the barycenter of the satellite as a function of $Delta t$. Pump-probe Auger-electron spectroscopy is thus highly sensitive to dynamical screening of the Coulomb interaction.
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