Carrier Relaxation Dynamics in Graphene

Graphene, the two-dimensional lattice of sp-hybridized carbon atoms, has a great potential for future electronics, in particular for opto-electronic devices. The carrier relaxation dynamics, which is of key importance for such applications, is in the main focus of this thesis. Besides a short introduction into the most prominent material properties of graphene and the experimental techniques, this thesis is divided into three main parts. The investigation of the carrier relaxation dynamics in the absence of a magnetic field is presented in Chapter 3. In the first experiment, the anisotropy of the carrier excitation and relaxation in momentum space was investigated by pump-probe measurements in the near-infrared range. While this anisotropy was not considered in all previous experiments, our measurements with a temporal resolution of less than 50 fs revealed the polarization dependence of the carrier excitation and the subsequent relaxation. About 150 fs after the electrons are excited, the carrier distribution in momentum space gets isotropic, caused by electron-phonon scattering. In a second set of two-color pump-probe experiments, the temperature of the hot carrier distribution, which was obtained within the duration of the pump pulse (about 200 fs), could be estimated. Furthermore, a change in sign of the pump-probe signal can be used as an indicator for the Fermi energy of different graphene layers. Pump-probe experiments in the far-infrared range in reflection and transmission geometry were performed at high pump power. A strong saturation of the pump-induced transmission was found in previous experiments, which was attributed to the pump-induced change in absorption. Our investigation shows the strong influence of pump-induced reflection at long wavelengths, as well as a lot smaller influence of the saturation of the pump-induced change in absorption. At a high pump power, the increase of the reflection exceeds the change in absorption strongly, which leads to negative pump-probe signals in transmission geometry. In Chapter 4, investigations of the carrier dynamics of graphene in magnetic fields of up to 7T are presented. Even though the optical properties of Landau-quantized graphene are very interesting, the carrier dynamics were nearly unexplored. A low photon energy of 14meV allows the investigation of the intraband Landau-level (LL) transitions. These experiments revealed two main findings: Firstly, the Landau quantization strongly suppresses the carrier relaxation via optical-phonon scattering, resulting in an increased relaxation time. Secondly, a change in sign of the pumpprobe signal can be observed when the magnetic field is varied. This change in sign indicates a hot carrier distribution shortly after the pump pulse, which means that carrier-carrier scattering remains very strong in magnetic fields. In a second set of pump-probe measurements, carried out at a photon energy of 75meV, the relaxation dynamics of interband LL transitions was investigated. In particular, experiments on the two energetically degenerate LL transitions LL−1 ⇒ LL0 and LL0 ⇒ LL1 showed the influence of extremely strong Auger processes. An ultrafast and extremely broadband terahertz detector, based on a graphene flake, is presented in the last chapter of this thesis. To couple the radiation efficiently to the small flake, the inner part of a logarithmic periodic antenna is connected to it. With a rise time of about 50 ps in a wavelength range of 9μm to 500μm, this detector is very interesting to obtain the temporal overlap in two-color pump-probe experiments with the free-electron laser FELBE. Furthermore, the importance of the substrate material, in particular for the high-speed performance, is discussed.