Torben Winzer

Carrier Multiplication in Graphene

Graphene as a zero-bandgap semiconductor is an ideal model structure to study the carrier relaxation channels, which are inefficient in conventional semiconductors. In particular, it is of fundamental interest to address the question whether Auger-type processes significantly influence the carrier dynamics in graphene. These scattering channels bridge the valence and conduction band allowing carrier multiplication, a process that generates multiple charge carriers from the absorption of a single photon. This has been suggested in literature for improving the efficiency of solar cells. Here we show, based on microscopic calculations within the density matrix formalism, that Auger processes do play an unusually strong role for the relaxation dynamics of photoexcited charge carriers in graphene. We predict that a considerable carrier multiplication takes place, confirming the potential of graphene as a new material for high-efficiency photodevices.

Carrier relaxation in epitaxial graphene photoexcited near the Dirac point.

We study the carrier dynamics in epitaxially grown graphene in the range of photon energies from 10 to 250 meV. The experiments complemented by microscopic modeling reveal that the carrier relaxation is significantly slowed down as the photon energy is tuned to values below the optical-phonon frequency; however, owing to the presence of hot carriers, optical-phonon emission is still the predominant relaxation process. For photon energies about twice the value of the Fermi energy, a transition from pump-induced transmission to pump-induced absorption occurs due to the interplay of interband and intraband processes.

Impact of Auger processes on carrier dynamics in graphene

Auger processes are of great importance for both fundamental research and technological applications, since they change the number of charge carriers in a system. Here, we present a microscopic study on the influence of Auger relaxation channels on the carrier dynamics in graphene. The presented time-, momentum-, and angle-resolved calculations reveal the importance of the impact excitation giving rise to a significant multiplication of optically excited carriers and a remarkable Coulomb-induced carrier cooling effect. We propose low pump fluence, high excitation energy, and low ambient temperature as optimal conditions for an efficient carrier multiplication reaching values of up to

Experimental verification of carrier multiplication in graphene.

2.5

Absorption saturation in optically excited graphene

even in the presence of phonons. The optimal regime is confirmed by an analytic expression for the carrier multiplication, which gives further insights into the role of Auger processes for a Dirac-like carrier system. Our results can help to guide future experiments to demonstrate the carrier multiplication in graphene and related structures.

Anisotropy of excitation and relaxation of photogenerated charge carriers in graphene.

We report on the first direct experimental observation of carrier multiplication in graphene reaching a multiplication factor of up to 2 and persisting on a picoseconds time scale. Exploiting multicolor pump-probe measurement techniques, the excited nonequilibrium carrier distribution is retrieved on an ultrafast time scale. This provides access to the temporal evolution of the optically excited carrier density and thus allows quantitative conclusions on possible carrier multiplication. Microscopic time- and momentum-resolved calculations on the ultrafast relaxation dynamics of optically excited carriers confirm the observation of carrier multiplication under corresponding experimental conditions, suggesting graphene as a promising material for novel high-efficiency photodetection devices.

Time-resolved spectroscopy on epitaxial graphene in the infrared spectral range: relaxation dynamics and saturation behavior

We investigate the saturation of the optical absorption in graphene induced by ultrafast optical pulses. Within a microscopic theory, we study the momentum-, angle-, and time-resolved interplay of anisotropic excitation, carrier-carrier, and carrier-phonon scattering, and its influence on the saturation of absorption and transmission. In agreement with performed experiments, we observe a linear regime for the intensity-dependence of the transmission at low pump fluences and a nonlinear saturation in the high excitation regime. Applying 10 fs-pulses, we obtain a saturation fluence of approximately 0.65 mJ/cm2. We demonstrate how the interplay of Pauli-blocking and intensity-dependent relaxation determines the saturation behavior.

Microscopic mechanism for transient population inversion and optical gain in graphene

We present a pump-probe experiment on graphene, which reveals a pronounced dependence of the pump-induced transmission on the angle between pump and probe polarization. It reflects a strong anisotropy of the pump-induced occupation of photogenerated carriers in momentum space. Within 150 fs after excitation, an isotropic carrier distribution is established. The experiments are well described by microscopic modeling, which identifies carrier-phonon scattering to be the main relaxation mechanism giving rise to an isotropic carrier distribution.

Current relaxation due to hot carrier scattering in graphene

We present the results of pump–probe experiments on multilayer graphene samples performed in a wide spectral range, namely from the near infrared (photon energy 1.5 eV) to the terahertz (photon energy 8 meV) spectral range. In the near infrared, exciting carriers and probing at higher photon energies provides direct evidence for a hot carrier distribution. Furthermore, spectroscopic signatures of the highly doped graphene layers at the interface to SiC are observed in the near-infrared range. In the mid-infrared range, the various relaxation mechanisms, in particular scattering via optical phonons and Auger-type processes, are identified by comparing the experimental results to microscopic modeling. Changes from induced transmission to induced absorption are attributed to probing above or below the Fermi edge of the graphene layers. This effect occurs for certain photon energies in the near-infrared range, where it is related to highly doped graphene layers at the interface to SiC, and in the far-infrared range for the quasi-intrinsic graphene layers. In addition to the relaxation dynamics, the saturation of pump-induced bleaching of graphene is studied. Here a quadratic dependence of the saturation fluence on the pump photon energy in the infrared spectral range is revealed.

Efficient orientational carrier relaxation in optically excited graphene

A transient femtosecond population inversion in graphene was recently reported by Li et al., Phys. Rev. Lett. 108, 167401 (2012). Based on a microscopic theory we clarify the underlying microscopic mechanism: Transient gain and population inversion in graphene occurs due to a complex interplay of strong optical pumping and carrier cooling that fills states close to the Dirac point giving rise to a relaxation bottleneck. The subsequent femtosecond decay of the optical gain is mainly driven by Coulomb-induced Auger recombination.