No description available.

Graphene, the two-dimensional lattice of sp2-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 pump-probe 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)->LL(0) and LL(0)->LL(1) 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 9 μm to 500 μm, 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.

No description available.

With increasing global energy demand and diminishing fossil fuel supplies, the development of clean and affordable renewable energy technology is more important than ever. Photovoltaic devices harvest the sun’s energy to produce electricity and produce very little pollution compared to nonrenewable sources. In order to make these devices affordable, however, technological advances are required. In this dissertation a novel photovoltaic device architecture that is designed to enhance sunlight-to-electricity conversion efficiency of photovoltaics is proposed and demonstrated. The increase in efficiency arises due to enhancement of the internal quantum efficiency of photoexcitation in the semiconductor absorber. In other words, the probability that the absorption of a single photon will produce two or more electron-hole pairs, instead of just one, is increased. This occurs through the process of impact ionization, by which a highly excited charge carrier (via absorption of a high energy photon) relaxes by excitation of a second electron-hole pair. The result is an increased photocurrent, and efficiency, of the photovoltaic device. Using thin films of ZnS on Si substrates, we demonstrate that the probability of impact ionization is enhanced at the (unbiased) heterojunction between these layers. The magnitude of enhancement depends on material properties, including crystallinity of the ZnS film as well as concentration of oxygen (impurity) at the interface. Thin films of ZnSe on Si substrates do not exhibit heterojunction-assisted impact ionization, but they do display promising characteristics that make them an intriguing system for future work. The same is true for ZnS/Si materials fabricated by O2-free chemical bath deposition. For the analysis of plain Si as well as ZnS/Si and ZnSe/Si heterostructures, we employ a novel pump-probe transient transmission and reflection spectroscopy technique. A method is demonstrated for using this technique to quantify internal quantum efficiency as well as interface recombination velocity in each of these materials. In bulk silicon, a free carrier absorption cross section that depends on free carrier concentration (above 1018 cm-3) is observed and the relationship is quantified. This dissertation includes unpublished and previously published co-authored material.

Ultrafast carrier dynamics studies have been carried out on samples with single layers of self-assembled In0.4Ga0.6As/GaAs quantum dots (QDs). Measurements were made using femtosecond degenerate pump-probe differential reflectivity with an 800-nm, 28-fs Ti-sapphire oscillator as the source. The QDs were grown via modified Stranski-Krastanov growth. This modified growth process consists of two steps: low-temperature growth and high-temperature annealing. Specifically, the InGaAs QD structures are fabricated on n-type GaAs(001) using molecular beam epitaxy. The InGaAs layer is deposited at 350-3700C followed by QD self assembly at 420-4900C. Finally, these QDs are capped with 10 nm or 100 nm of GaAs. The measured width and height of these QDs are typically 25 nm and 8 nm, respectively. Dots annealed at higher temperature have larger base area (width and length) and reduced height, as compared to those annealed at lower temperature. We have used a model consisting of a linear combination of an exponential decaying function to describe the carrier dynamics and fit the reflectivity data, revealing trends in the carrier capture and relaxation times associated with the InGaAs layer versus laser excitation level and QD morphology. Capture times are ~ 1 ps for the 100-nm capped samples, but slightly shorter for the 10-nm capped thin samples, indicating carrier transport plays a role in dynamics. The carrier dynamics in 10-nm capped samples are correlated with sample annealing temperature, indicating QD morphology affects carrier capture. Versus laser intensity, and thus carrier excitation level, the dynamics generally become slower, suggesting state filling is important in both the capture and relaxation of excited carriers in these samples.

Carrier dynamics in GaAs-based photoconductive terahertz (THz) sources is investigated using Monte Carlo techniques to optimize the emitted THz transients. A self-consistent Monte Carlo-Poisson solver is developed for the spatio-temporal carrier transport properties. The screening contributions to the THz radiation associated with the Coulomb and radiation fields are obtained self-consistently by incorporating the three-dimensional Maxwell equations into the solver. In addition, the enhancement of THz emission by a large trap-enhance field (TEF) near the anode in semi-insulating (SI) photoconductors is investigated. The transport properties of the photoexcited carriers in photoconductive THz sources depend markedly on the initial spatial distribution of those carriers. Thus, considerable control of the emitted THz spectrum can be attained by judiciously choosing the optical excitation spot shape on the photoconductor, since the carrier dynamics that provide the source of the THz radiation are strongly affected by the ensuing screenings. The screening contributions due to the Coulomb and radiation parts of the electromagnetic field acting back on the carrier dynamics are distinguished. The dominant component of the screening field crosses over at an excitation aperture size with full width at half maximum (FWHM) of ~100 um for a range of reasonable excitation levels. In addition, the key mechanisms responsible for the TEF near the anode of SI photoconductors are elucidated in detail. For a given optical excitation power, an enhancement of THz radiation power can be obtained using a maximally broadened excitation aperture in the TEF area elongated along the anode due to the reduction in the Coulomb and radiation screening of the TEF.

Electromagnetic radiation in the frequency range between about 100 GHz and 5 THz can be used for spectroscopy and microscopy, but it is also promising for security screening and even wireless communication. In the present thesis a planar photoconducting large-area THz radiation source is presented. The device exhibits outstanding properties, in particular high THz field strength and generation efficiency and large spectral bandwidth with short THz pulse length. The THz emission is based on acceleration and deceleration of photoexcited carriers in semiconductor substrates. A metallic interdigitated structure at the surface of semi-insulating GaAs provides the electrodes of an Auston switch. In a biased structure photoexcited charge carriers are accelerated. Hence electromagnetic waves are emitted. An appropriately structured second metallization, electrically isolated from the electrodes, prevents destructive interference of the emitted waves. The structure investigated here combines several advantages of different conventional photoconducting THz sources. First, it provides high electric acceleration fields at moderate voltages owing to the small electrode separation. Second, the large active area in the mm2 range allows excitation by large optical powers of some mW. Optical excitation with near-infrared femtosecond lasers is possible with repetition rates in the GHz range. The presented results point out the excellent characteristics regarding the emitted THz field strength, average power, spectral properties, and easy handling of the interdigitated structure in comparison to various conventional emitter structures. Various modifications of the semiconductor substrate and the optimum excitation conditions were investigated. In the second part of this thesis the dynamic conductivity of GaAs/AlxGa1-xAs superlattices in an applied static electric field was investigated with time-resolved THz spectroscopy. The original goal was to explore whether the predicted effect of gain of electromagnetic radiation at THz frequencies is present in such structures. Superlattice samples were grown according to the experimental requirements, which include high specific resistance and sufficient THz transparency. The characterization of the superlattices by Fourier transform infrared spectroscopy and photoluminescence spectroscopy confirms the pronounced miniband properties of the bandstructure. Furthermore indications of Bloch oscillations were found by transport measurements. However, we could not measure a change of the dynamic conductivity when the electric field was toggled. Specific reasons for this and related experiments of other groups are discussed. / Elektromagnetische Strahlung im Frequenzbereich zwischen etwa 100 GHz und 5 THz wird für verschiedene Anwendungen wie Spektroskopie und Mikroskopie genutzt, kann aber auch für Sicherheitstechnik oder sogar Datenübertragung interessant sein. In der hier vorgestellten Forschungsarbeit wird eine großflächige fotoleitende THz-Strahlungsquelle beschrieben, die sich durch eine große THz-Feldstärke und große spektrale Bandbreite auszeichnet. Die THz-Emission basiert auf der Beschleunigung und Verzögerung fotogenerierter Ladungen in Halbleitersubstraten. Eine metallische Interdigitalstruktur auf der Oberfläche von semi-isolierendem GaAs bildet die Elektroden eines Fotoschalters. Ist an diese Struktur eine Spannung angeschlossen, werden optisch generierte Ladungsträger beschleunigt und strahlen elektromagnetische Wellen ab. Eine geeignet strukturierte und isolierte zweite Metallisierung verhindert destruktive Interferenzen der abgestrahlten Wellen. Die vorgeschlagene Struktur vereinigt dabei die Vorteile verschiedener herkömmlicher fotoleitender THz-Quellen. Einerseits ermöglicht der kleine Elektrodenabstand große elektrische Felder zur Beschleunigung fotogenerierter Ladungen schon bei moderaten Spannungen. Andererseits kann die große aktive Fläche von einigen mm2 mit großen optischen Leistungen im Bereich einiger mW angeregt werden. Die optische Anregung mit Nahinfrarot-Femtosekunden- Lasern kann mit Wiederholraten bis in den GHz-Bereich geschehen. Bedingt durch die Eigenschaften der Anregungspulse entstehen kurze spektral breite THz-Pulse. Die vorliegenden Ergebnisse verdeutlichen die hervorragenden Eigenschaften der Interdigitalstruktur im Vergleich zu verschiedenen herkömmlichen Geometrien bezüglich der Feldstärke der abgestrahlten Wellen, der mittleren Leistung und der spektralen Eigenschaften. Dabei ist die Struktur sehr einfach zu handhaben. Es wurden verschiedene Modifikationen des Substrates und die optimalen Bedingungen der optischen Anregung untersucht. Der zweite Teil dieser Arbeit behandelt die Erforschung der dynamische Leitfähigkeit von GaAs/AlxGa1-xAs-Übergittern in Abhängigkeit von einem elektrischen Feld mit Hilfe der zeitaufgelösten THz-Spektroskopie. Es sollte geklärt werden, ob der vorhergesagte Effekt der Verstärkung elektro-magnetischer Strahlung in solchen Strukturen möglich ist. Dazu wurden Übergitterproben gemäß den experimentellen Anforderungen hergestellt. Zu den Vorgaben gehört ein hoher spezifischer Widerstand und ausreichende Transparenz im THz-Bereich. Die Charakterisierung der Übergitter mit Fotolumineszenz- und Fourier-Transformations-IR-Spektroskopie bestätigte die ausgeprägten Minibandeigenschaften der Bandstruktur. Hinweise auf Bloch-Oszillationen wurden durch Ladungstransportmessungen gefunden. Dennoch war eine Änderung der dynamischen Leitfähigkeit beim Schalten des elektrischen Feldes nicht messbar. Gründe dafür und ähnliche Experimente anderer Gruppen werden diskutiert.

Graphene, the two-dimensional lattice of sp2-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 pump-probe 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)->LL(0) and LL(0)->LL(1) 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 9 μm to 500 μm, 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.

Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第19007号 / 工博第4049号 / 新制||工||1623 / 31958 / 京都大学大学院工学研究科高分子化学専攻 / (主査)教授 伊藤 紳三郎, 教授 赤木 和夫, 教授 辻井 敬亘 / 学位規則第4条第1項該当

This thesis reports results from the investigation of optically-induced carrier dynamics in graphite and graphitic carbon nanostructures. In this first set of experiments, the dynamics of photo-excited carriers in exfoliated graphene and thin graphitic films are studied by optical pump-probe spectroscopy. Samples ranging in thickness from 1 to 260 carbon layers are deposited onto an oxidized silicon substrate. Time-resolved reflectivity and transmissivity are measured at 1300 nm, following excitation by 150 fs, 800 nm pump pulses at room temperature. Two time scales are identified over which the extracted transient dielectric function returns to its quiescent value. A fast decay time of ~200 fs in graphene is associated with hot phonon emission and increases to ~300 fs for thicknesses greater than only a few carbon layers. The slow decay time, associated with hot phonon interaction and/or carrier recombination, increases more gradually, from ~2.5 to 5 ps over ~30 layers. A simple model suggests the thickness dependence of the slow decay time is likely a result of thermal diffusion into the substrate. In the second set of experiments, coherently-controlled two-colour injection photocurrents are generated via quantum interference of single- and two-photon absorption in bulk graphite and a variety of single-walled carbon nanotube samples, such as a CVD-grown aligned forest of nanotubes (tube diameter dt = 2.5 ± 1.5 nm), and both arc discharge (dt = 1.44 ± 0.15 nm) and HiPco (dt = 0.96 ± 0.14 nm) nanotube films separated by electronic type (metallic vs. semiconducting). At pump wavelengths of 1500 and 750 nm, the emitted terahertz radiation is used to estimate a peak current density of ~12 kA/cm² in graphite and a peak current of ~8 nA per nanotube. From the dependence of the injected current on pump polarization, the relative values of the current injection tensor elements are measured, and information is gained on the alignment and birefringence of the nanotube samples. The dependence of the injected current on pump wavelength implies that the currents are likely based on band-band electronic transitions and not on excitonic effects, which govern most linear optical processes.