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Register a new userPhoto-excitation Cascade and Multiple Carrier Generation in Graphene
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Added by
Klaas-Jan Tielrooij
Publication date
2012
fields
Physics
and research's language is
English
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The conversion of light into free electron-hole pairs constitutes the key process in the fields of photodetection and photovoltaics. The efficiency of this process depends on the competition of different relaxation pathways and can be greatly enhanced when photoexcited carriers do not lose energy as heat, but instead transfer their excess energy into the production of additional electron-hole pairs via carrier-carrier scattering processes. Here we use Optical pump - Terahertz probe measurements to show that in graphene carrier-carrier scattering is unprecedentedly efficient and dominates the ultrafast energy relaxation of photoexcited carriers, prevailing over optical phonon emission in a wide range of photon wavelengths. Our results indicate that this leads to the production of secondary hot electrons, originating from the conduction band. Since hot electrons in graphene can drive currents, multiple hot carrier generation makes graphene a promising material for highly efficient broadband extraction of light energy into electronic degrees of freedom, enabling high-efficiency optoelectronic applications.
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In conventional light harvesting devices, the absorption of a single photon only excites one electron, which sets the standard limit of power-conversion efficiency, such as the Shockley-Queisser limit. In principle, generating and harnessing multiple carriers per absorbed photon can improve the efficiency and possibly overcome this limit. Here, we report the observation of multiple hot carrier collection in graphene-boron-nitride Moire superlattice structures. A record-high zero-bias photoresponsivity of 0.3 ampere per watt, equivalently, an external quantum efficiency exceeding 50 percent, is achieved utilizing graphene photo-Nernst effect, which demonstrates a collection of at least 5 carriers per absorbed photon. We reveal that this effect arises from the enhanced Nernst coefficient through Lifshtiz transition at low energy Van Hove singularities, which is an emergent phenomenon due to the formation of Moire minibands. Our observation points to a new means for extremely efficient and flexible optoelectronics based on van der Waals heterostructures.
We theoretically examine the effect of carrier-carrier scattering processes (electron-hole and electron-electron) on the intraband radiation absorption and their contribution to the net dynamic conductivity in optically or electrically pumped graphene. We demonstrate that the radiation absorption assisted by the carrier-carrier scattering can be stronger than the Drude absorption due to the carrier scattering on disorder. Since the intraband absorption of radiation effectively competes with its interband amplification, this can substantially affect the conditions of the negative dynamic conductivity in the pumped graphene and, hence, the interband terahertz and infrared lasing. We find the threshold values of the frequency and quasi-Fermi energy of nonequilibrium carriers corresponding to the onset of negative dynamic conductivity. The obtained results show that the effect of carrier-carrier scattering shifts the threshold frequency of the radiation amplification in pumped graphene to higher values. In particular, the negative dynamic conductivity is attainable at the frequencies above 6 THz in graphene on SiO2 substrates at room temperature. The threshold frequency can be decreased to markedly lower values in graphene structures with high-k substrates due to screening of the carrier-carrier scattering, particularly at lower temperatures.
In Dirac materials linear band dispersion blocks momentum-conserving interband transitions, creating a bottleneck for electron-hole pair production and carrier multiplication in the photoexcitation cascade. Here we show that the decays are unblocked and the bottleneck is relieved by subtle many-body effects involving multiple off-shell e-h pairs. The decays result from a collective behavior due to emission of many soft pairs. We discuss characteristic signatures of the off-shell pathways, in particular the sharp angular distribution of secondary carriers, resembling relativistic jets in high-energy physics. The jets can be directly probed using solid-state equivalent of particle detectors. Collinear scattering enhances carrier multiplication, allowing for emission of as many as ${sim}10$ secondary carriers per single absorbed photon.
Graphene is a promising material for ultrafast and broadband photodetection. Earlier studies addressed the general operation of graphene-based photo-thermoelectric devices, and the switching speed, which is limited by the charge carrier cooling time, on the order of picoseconds. However, the generation of the photovoltage could occur at a much faster time scale, as it is associated with the carrier heating time. Here, we measure the photovoltage generation time and find it to be faster than 50 femtoseconds. As a proof-of-principle application of this ultrafast photodetector, we use graphene to directly measure, electrically, the pulse duration of a sub-50 femtosecond laser pulse. The observation that carrier heating is ultrafast suggests that energy from absorbed photons can be efficiently transferred to carrier heat. To study this, we examine the spectral response and find a constant spectral responsivity between 500 and 1500 nm. This is consistent with efficient electron heating. These results are promising for ultrafast femtosecond and broadband photodetector applications.
We investigate electron dynamics at the graphene edge by studying the propagation of collective edge magnetoplasmon (EMP) excitations. By timing the travel of narrow wave-packets on picosecond time scales around exfoliated samples, we find chiral propagation with low attenuation at a velocity which is quantized on Hall plateaus. We extract the carrier drift contribution from the EMP propagation and find it to be slightly less than the Fermi velocity, as expected for an abrupt edge. We also extract the characteristic length for Coulomb interaction at the edge and find it to be smaller than for soft, depletion edge systems.
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