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We present an ab-initio study of photocarrier dynamics in graphene due to electron-phonon (EP) interactions. Using the Boltzmann relaxation-time approximation with parameters determined from density functional theory (DFT) and a complementary, explicitly solvable model we show that the photocarrier thermalization time changes by orders of magnitude, when the excitation energy is reduced from 1 eV to the 100 meV range. In detail, the ultrafast thermalization at low temperatures takes place on a femtosecond timescale via optical phonon emission, but slows down to picoseconds once excitation energies become comparable with these optical phonon energy quanta. In the latter regime, thermalization times exhibit a pronounced dependence on temperature. Our DFT model includes all the inter- and intraband transitions due to EP scattering. Thanks to the high melting point of graphene we extend our studies up to 2000~K and show that such high temperatures reduce the photocarrier thermalization time through phonon absorption.
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Direct and inverse Auger scattering are amongst the primary processes that mediate the thermalization of hot carriers in semiconductors. These two processes involve the annihilation or generation of an electron-hole pair by exchanging energy with a third carrier, which is either accelerated or decelerated. Inverse Auger scattering is generally suppressed, as the decelerated carriers must have excess energies higher than the band gap itself. In graphene, which is gapless, inverse Auger scattering is instead predicted to be dominant at the earliest time delays. Here, $<8$ femtosecond extreme-ultraviolet pulses are used to detect this imbalance, tracking both the number of excited electrons and their kinetic energy with time- and angle-resolved photoemission spectroscopy. Over a time window of approximately 25 fs after absorption of the pump pulse, we observe an increase in conduction band carrier density and a simultaneous decrease of the average carrier kinetic energy, revealing that relaxation is in fact dominated by inverse Auger scattering. Measurements of carrier scattering at extreme timescales by photoemission will serve as a guide to ultrafast control of electronic properties in solids for PetaHertz electronics.
We determine the information scrambling rate $lambda_{L}$ due to electron-electron Coulomb interaction in graphene. $lambda_{L}$ characterizes the growth of chaos and has been argued to give information about the thermalization and hydrodynamic transport coefficients of a many-body system. We demonstrate that $lambda_{L}$ behaves for strong coupling similar to transport and energy relaxation rates. A weak coupling analysis, however, reveals that scrambling is related to dephasing or single particle relaxation. Furthermore, $lambda_{L}$ is found to be parametrically larger than the collision rate relevant for hydrodynamic processes, such as electrical conduction or viscous flow, and the rate of energy relaxation, relevant for thermalization. Thus, while scrambling is obviously necessary for thermalization and quantum transport, it does generically not set the time scale for these processes. In addition we derive a quantum kinetic theory for information scrambling that resembles the celebrated Boltzmann equation and offers a physically transparent insight into quantum chaos in many-body systems.
The stability of two-dimensional (2D) layers and membranes is subject of a long standing theoretical debate. According to the so called Mermin-Wagner theorem, long wavelength fluctuations destroy the long-range order for 2D crystals. Similarly, 2D membranes embedded in a 3D space have a tendency to be crumpled. These dangerous fluctuations can, however, be suppressed by anharmonic coupling between bending and stretching modes making that a two-dimensional membrane can exist but should present strong height fluctuations. The discovery of graphene, the first truly 2D crystal and the recent experimental observation of ripples in freely hanging graphene makes these issues especially important. Beside the academic interest, understanding the mechanisms of stability of graphene is crucial for understanding electronic transport in this material that is attracting so much interest for its unusual Dirac spectrum and electronic properties. Here we address the nature of these height fluctuations by means of straightforward atomistic Monte Carlo simulations based on a very accurate many-body interatomic potential for carbon. We find that ripples spontaneously appear due to thermal fluctuations with a size distribution peaked around 70 AA which is compatible with experimental findings (50-100 AA) but not with the current understanding of stability of flexible membranes. This unexpected result seems to be due to the multiplicity of chemical bonding in carbon.
The band structure of MoS$_2$ strongly depends on the number of layers, and a transition from indirect to direct-gap semiconductor has been observed recently for a single layer of MoS$_2$. Single-layer MoS$_2$ therefore becomes an efficient emitter of photoluminescence even at room temperature. Here, we report on scanning Raman and on temperature-dependent, as well as time-resolved photoluminescence measurements on single-layer MoS$_2$ flakes prepared by exfoliation. We observe the emergence of two distinct photoluminescence peaks at low temperatures. The photocarrier recombination at low temperatures occurs on the few-picosecond timescale, but with increasing temperatures, a biexponential photoluminescence decay with a longer-lived component is observed.
In this work, high field carrier transport in two dimensional (2D) graphene is investigated. Analytical models are applied to estimate the saturation currents in graphene, based on the high scattering rate of optical phonon emission. Non-equilibrium (hot) phonon effect was studied by Monte Carlo (MC) simulations. MC simulation confirms that hot phonon effects play a dominant role in current saturation in graphene. Current degradation due to elastic scattering events is much smaller compared to the hot phonon effect. Transient phenomenon as such as velocity overshoot was also studied using MC simulation. The simulation results shows promising potential for graphene to be used in high speed electronic devices by shrinking the channel length below 100nm if electrostatic control can be exercised in the absence of a band gap.
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