Jared H. Strait

Ultrafast Optical-Pump Terahertz-Probe Spectroscopy of the Carrier Relaxation and Recombination Dynamics in Epitaxial Graphene

The ultrafast relaxation and recombination dynamics of photogenerated electrons and holes in epitaxial graphene are studied using optical-pump terahertz-probe spectroscopy. The conductivity in graphene at terahertz frequencies depends on the carrier concentration as well as the carrier distribution in energy. Time-resolved studies of the conductivity can therefore be used to probe the dynamics associated with carrier intraband relaxation and interband recombination. We report the electron-hole recombination times in epitaxial graphene for the first time. Our results show that carrier cooling occurs on subpicosecond time scales and that interband recombination times are carrier density dependent.

Measurement of the optical absorption spectra of epitaxial graphene from terahertz to visible

We present experimental results on the optical absorption spectra of epitaxial graphene from the visible to the terahertz frequency range. In the terahertz range, the absorption is dominated by intraband processes with a frequency dependence similar to the Drude model. In the near-IR range, the absorption is due to interband processes and the measured optical conductivity is close to the theoretical value of e2/4ℏ. We extract values for the carrier densities, the number of carbon atom layers, and the intraband scattering times from the measurements.

Ultrafast relaxation dynamics of hot optical phonons in graphene

Using ultrafast optical pump-probe spectroscopy, we study the relaxation dynamics of hot optical phonons in few-layer and multilayer graphene films grown by epitaxy on silicon carbide substrates and by chemical vapor deposition on nickel substrates. In the first few hundred femtoseconds after photoexcitation, the hot carriers lose most of their energy to the generation of hot optical phonons which then present the main bottleneck to subsequent cooling. Optical phonon cooling on short time scales is found to be independent of the graphene growth technique, the number of layers, and the type of the substrate. We find average phonon lifetimes in the 2.5–2.55 ps range. We model the relaxation dynamics of the coupled carrier-phonon system with rate equations and find a good agreement between the experimental data and the theory. The extracted optical phonon lifetimes agree very well with the theory based on anharmonic phonon interactions.

Carrier recombination and generation rates for intravalley and intervalley phonon scattering in graphene

Electron-hole generation and recombination rates for intravalley and intervalley phonon scattering in graphene are presented. The transverse and the longitudinal optical phonon modes E2g modes near the zone center point contribute to intravalley interband carrier scattering. At the zone edge KK point, only the transverse optical phonon mode A 1 mode contributes significantly to intervalley interband scattering with recombination rates faster than those due to zone-center phonons. The calculated recombination times range from less than a picosecond to more than hundreds of picoseconds and are strong functions of temperature and electron and hole densities. The theoretical calculations agree well with experimental measurements of the recombination rates of photoexcited carriers in graphene.

Very Slow Cooling Dynamics of Photoexcited Carriers in Graphene Observed by Optical-Pump Terahertz-Probe Spectroscopy

Using optical-pump terahertz-probe spectroscopy, we study the relaxation dynamics of photoexcited carriers in graphene at different substrate temperatures. We find that at lower temperatures the tail of the relaxation transients measured by the differential probe transmission become slower, extending beyond several hundred picoseconds below 50 K. We interpret the observed relaxation transients as resulting from the cooling of the photoexcited carriers via phonon emission. The slow cooling of the photoexcited carriers at low temperatures is attributed to the bulk of the electron and hole energy distributions moving close enough to the Dirac point that both intraband and interband scattering of carriers via optical phonon emission become inefficient for removing heat from the carriers. Our model, which includes intraband carrier scattering and interband carrier recombination and generation, agrees very well with the experimental observations.

High intrinsic mobility and ultrafast carrier dynamics in multilayer metal-dichalcogenide MoS2

The ultimate limitations on carrier mobilities in metal dichalcogenides, and the dynamics associated with carrier relaxation, are unclear. We present measurements of the frequency-dependent conductivity of multilayer dichalcogenide MoS2 by optical-pump terahertz-probe spectroscopy. We find mobilities in this material approaching 4200 cm2/Vs at low temperatures. The temperature dependence of scattering indicates that the mobility, an order of magnitude larger than previously reported for MoS2, is intrinsically limited by acoustic phonon scattering at THz frequencies. Our measurements of carrier relaxation reveal picosecond cooling times followed by recombination lasting tens of nanoseconds and dominated by Auger scattering into defects. Our results provide a useful context in which to understand and evaluate the performance of MoS2-based electronic and optoelectronic devices.

Measurements of the Carrier Dynamics and Terahertz Response of Oriented Germanium Nanowires using Optical-Pump Terahertz-Probe Spectroscopy

We have measured the terahertz response of oriented Germanium nanowires using ultrafast optical-pump terahertz-probe spectroscopy. We present results on the time, frequency, and polarization dependence of the terahertz response. Our results indicate intraband energy relaxation times of photoexcited carriers in the 1.5-2.0 ps range, carrier density dependent interband electron-hole recombination times in the 75-125 ps range, and carrier momentum scattering rates in the 60-90 fs range. Additionally, the terahertz response of the nanowires is strongly polarization dependent despite the subwavelength dimensions of the nanowires. The differential terahertz transmission is found to be large when the field is polarized parallel to the nanowires and very small when the field is polarized perpendicular to the nanowires. This polarization dependence of the terahertz response can be explained in terms of the induced depolarization fields and the resulting magnitudes of the surface plasmon frequencies.

Ultrafast carrier recombination and generation rates for plasmon emission and absorption in graphene

Electron-hole generation and recombination rates for plasmon emission and absorption in Graphene are presented. The recombination times of carriers due to plasmon emission have been found to be in the tens of femtoseconds to hundreds of picoseconds range. The recombination times depend sensitively on the carrier energy, carrier density, temperature, and the plasmon dispersion. Carriers near the Dirac point are found to have much longer lifetimes compared to carriers at higher energies. Plasmons in a Graphene layer on a polar substrate hybridize with the surface optical phonons and this hybridization modifies the plasmon dispersion. We also present generation and recombination rates of carriers due to plasmon emission and absorption in Graphene layers on polar substrates.

Fast exciton annihilation by capture of electrons or holes by defects via Auger scattering in monolayer metal dichalcogenides

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

Emission of terahertz radiation from SiC

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