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Dynamics of Carriers and Photoinjected Currents in Carbon Nanotubes and GrapheneNewson, Ryan William 23 February 2011 (has links)
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.
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Krūvininkų rekombinacija plačiatarpiuose nitridiniuose puslaidininkiuose / Carrier recombination in wide-band-gap nitride semiconductorsMickevičius, Jūras 21 November 2009 (has links)
Disertacija skirta krūvininkų rekombinacijos tyrimams plačiatarpiuose nitridiniuose puslaidininkiuose bei jų dariniuose. Kompleksiniai eksperimentiniai tyrimai buvo atlikti naudojant kelias skirtingas metodikas. Atlikti krūvininkų dinamikos GaN sluoksniuose tyrimai labai žemų ir aukštų sužadinimų sąlygomis. Pasiūlytas naujas liuminescencijos gesimo kinetikų interpretavimo metodas, siejant liuminescencijos ir šviesa indukuotų dinaminių gardelių kinetikas. Naujas požiūris į geltonosios liuminescencijos juostą GaN sluoksniuose leido susieti geltonosios liuminescencijos intensyvumą su krūvininkų gyvavimo trukme. Skirtingomis technologijomis augintų AlGaN sluoksnių palyginimas suteikė informacijos apie juostos potencialo fliuktuacijas bei krūvininkų gyvavimo trukmę ribojančius veiksnius AlGaN medžiagose. Atskleista naujų krūvininkų dinamikos daugialakštėse AlGaN/AlGaN kvantinėse duobėse ypatumų – vidinio elektrinio lauko bei kvantinės duobės pločio fliuktuacijų sąlygotos lokalizacijos įtaka krūvininkų dinamikai. Dauguma tirtų bandinių buvo auginti naudojant MEMOCVDTM technologiją ir tyrimai patvirtino šios technologijos potencialą siekiant pagerinti medžiagų kokybę. / The thesis is dedicated to carrier recombination investigations in wide-band-gap semiconductors and their structures. The complex experimental studies were performed by combining several different techniques. Carrier dynamics in GaN epilayers were investigated under extremely low and high excitation conditions. A new method for interpreting photoluminescence decay kinetics was suggested by interrelating luminescence and light-induced grating decay transients. The new approach for studies of yellow band in GaN was shown by linking the carrier lifetime with yellow band intensity. Two AlGaN epilayers grown by different novel growth techniques were compared and the factors limiting carrier lifetime were identified. Moreover, more evidence on alloy mixing and band potential fluctuations in AlGaN was provided by our study. Essential knowledge was attained about carrier dynamics in high-Al-content AlGaN/AlGaN multiple quantum well structures: the influence of built-in electric field and carrier localization on carrier dynamics. Most of the samples under study were grown by MEMOCVDTM growth technique, and our study confirmed the high potential of this innovative growth technique for improving material quality.
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Carrier recombination in wide-band-gap nitride semiconductors / Krūvininkų rekombinacija plačiatarpiuose nitridiniuose puslaidininkiuoseMickevičius, Jūras 21 November 2009 (has links)
The thesis is dedicated to carrier recombination investigations in wide-band-gap semiconductors and their structures. The complex experimental studies were performed by combining several different techniques. Carrier dynamics in GaN epilayers were investigated under extremely low and high excitation conditions. A new method for interpreting photoluminescence decay kinetics was suggested by interrelating luminescence and light-induced grating decay transients. The new approach for studies of yellow band in GaN was shown by linking the carrier lifetime with yellow band intensity. Two AlGaN epilayers grown by different novel growth techniques were compared and the factors limiting carrier lifetime were identified. Moreover, more evidence on alloy mixing and band potential fluctuations in AlGaN was provided by our study. Essential knowledge was attained about carrier dynamics in high-Al-content AlGaN/AlGaN multiple quantum well structures: the influence of built-in electric field and carrier localization on carrier dynamics. Most of the samples under study were grown by MEMOCVDTM growth technique, and our study confirmed the high potential of this innovative growth technique for improving material quality. / Disertacija skirta krūvininkų rekombinacijos tyrimams plačiatarpiuose nitridiniuose puslaidininkiuose bei jų dariniuose. Kompleksiniai eksperimentiniai tyrimai buvo atlikti naudojant kelias skirtingas metodikas. Atlikti krūvininkų dinamikos GaN sluoksniuose tyrimai labai žemų ir aukštų sužadinimų sąlygomis. Pasiūlytas naujas liuminescencijos gesimo kinetikų interpretavimo metodas, siejant liuminescencijos ir šviesa indukuotų dinaminių gardelių kinetikas. Naujas požiūris į geltonosios liuminescencijos juostą GaN sluoksniuose leido susieti geltonosios liuminescencijos intensyvumą su krūvininkų gyvavimo trukme. Skirtingomis technologijomis augintų AlGaN sluoksnių palyginimas suteikė informacijos apie juostos potencialo fliuktuacijas bei krūvininkų gyvavimo trukmę ribojančius veiksnius AlGaN medžiagose. Atskleista naujų krūvininkų dinamikos daugialakštėse AlGaN/AlGaN kvantinėse duobėse ypatumų – vidinio elektrinio lauko bei kvantinės duobės pločio fliuktuacijų sąlygotos lokalizacijos įtaka krūvininkų dinamikai. Dauguma tirtų bandinių buvo auginti naudojant MEMOCVDTM technologiją ir tyrimai patvirtino šios technologijos potencialą siekiant pagerinti medžiagų kokybę.
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Ultrafast exciton and charge carrier dynamics in nanostructured molecular layers / Ultrasparti eksitonų ir krūvininkų dinamika nanostruktūrizuotuose molekulių sluoksniuosePeckus, Domantas 20 December 2013 (has links)
Due to their unique properties organic semiconductors may be used for various applications in organic optoelectronic devices: light emitting devices, lasers, field-effect transistors, photovoltaic cells and etc. Despite high perspectives of organic semiconductors they are still upstaged by their inorganic counterparts. Development of organic electronics requires better understanding of electrooptical properties of organic semiconductors and relationships between their structure and functions.
The main goal of this thesis is a detailed investigation of ultrafast exciton and charge carrier processes in pure organic semiconductors and their blends with fullerene derivatives. Investigated organic or silicon organic semiconductors were poly-di-n-hexylsilane (PDHS), polyfluorenes F8BT and PSF-BT, merocyanine MD376. C60 fullerene and its derivative PCBM were used in blends. Ultrafast transient absorption, fluorescence, and integral mode photocurrent measurements were used for investigations.
The investigation of PDHS nanocomposites revealed that PDHS incorporation into nanopores can be used for improvement of fluorescence properties.
Formation of intramolecular charge transfer state was proposed for PSF-BT neat films. Charge transfer scheme of the formation of long-lived charge pair state in PSF-BT/PCBM blend was presented.
The charge pair and free charge carrier generation scheme in merocyanine blends with fullerene derivatives were discussed in detail.
Analysis of measurement... [to full text] / Dėl savo unikalių savybių organiniai puslaidininkiai gali būti plačiai pritaikyti įvairiuose optoelektroniniuose prietaisuose: organiniuose šviestukuose, organiniuose lazeriuose, organiniuose tranzistoriuose ir organiniuose šviesos elementuose. Visi šie pritaikymai yra galimi dėl organinių molekulių laidumo. Nepaisant didelių organinių puslaidininkių perspektyvų, jie vis dar yra nukonkuruojami neorganinių puslaidininkių.
Pagrindinis šių tezių tikslas yra detaliai ištirti eksitonų ir krūvininkų dinamikos procesus grynuose organiniuose puslaidininkiuose ir jų mišiniuose su fulereno dariniais. Buvo matuoti organiniai ir silicio organiniai puslaidininkiai: poli-di-n-heksilsilanas (PDHS), polifluoreno dariniai F8BT ir PSF-BT, merocianinas MD376. Mišiniuose naudoti fulerenai buvo C60 ir jo darinys PCBM. Tyrimams buvo naudoti ultraspartūs skirtuminės sugerties, fluorescencijos ir integralinės fotosrovės matavimai.
PDHS tyrimai atskleidė, kad neorganinės matricos sumažina nespindulinį relaksacijos kanalą. PDHS nanokompozitai gali būti naudojami polimero fluorescencijos savybių: stabilumo, kvantinio našumo pagerinimui.
Polifluorenų F8BT ir PSF-BT grynų plėvelių tyrimų metu nustatyti eksitonų-eksitonų anihiliacijos ir eksitonų migracijos skirtumai. Vidumolekulinės krūvio pernašos būsenos formavimasis buvo pasiūlytas PSF-BT grynoms plėvelėms. Pristatyta ilgi gyvuojančių krūvininkų porų formavimosi schema PSF-BT/PCBM mišiniuose.
Krūvio pernašos būsenų formavimasis buvo ištirtas... [toliau žr. visą tekstą]
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Ultrasparti eksitonų ir krūvininkų dinamika nanostruktūrizuotuose molekulių sluoksniuose / Ultrafast exciton and charge carrier dynamics in nanostructured molecular layersPeckus, Domantas 20 December 2013 (has links)
Dėl savo unikalių savybių organiniai puslaidininkiai gali būti plačiai pritaikyti įvairiuose optoelektroniniuose prietaisuose: organiniuose šviestukuose, organiniuose lazeriuose, organiniuose tranzistoriuose ir organiniuose šviesos elementuose. Visi šie pritaikymai yra galimi dėl organinių molekulių laidumo. Nepaisant didelių organinių puslaidininkių perspektyvų, jie vis dar yra nukonkuruojami neorganinių puslaidininkių.
Pagrindinis šių tezių tikslas yra detaliai ištirti eksitonų ir krūvininkų dinamikos procesus grynuose organiniuose puslaidininkiuose ir jų mišiniuose su fulereno dariniais. Buvo matuoti organiniai ir silicio organiniai puslaidininkiai: poli-di-n-heksilsilanas (PDHS), polifluoreno dariniai F8BT ir PSF-BT, merocianinas MD376. Mišiniuose naudoti fulerenai buvo C60 ir jo darinys PCBM. Tyrimams buvo naudoti ultraspartūs skirtuminės sugerties, fluorescencijos ir integralinės fotosrovės matavimai.
PDHS tyrimai atskleidė, kad neorganinės matricos sumažina nespindulinį relaksacijos kanalą. PDHS nanokompozitai gali būti naudojami polimero fluorescencijos savybių: stabilumo, kvantinio našumo pagerinimui.
Polifluorenų F8BT ir PSF-BT grynų plėvelių tyrimų metu nustatyti eksitonų-eksitonų anihiliacijos ir eksitonų migracijos skirtumai. Vidumolekulinės krūvio pernašos būsenos formavimasis buvo pasiūlytas PSF-BT grynoms plėvelėms. Pristatyta ilgi gyvuojančių krūvininkų porų formavimosi schema PSF-BT/PCBM mišiniuose.
Krūvio pernašos būsenų formavimasis buvo ištirtas... [toliau žr. visą tekstą] / Due to their unique properties organic semiconductors may be used for various applications in organic optoelectronic devices: light emitting devices, lasers, field-effect transistors and photovoltaic cells and etc. Despite high perspectives of organic semiconductors they are still upstaged by their inorganic counterpart. The efficiency of electrooptical properties of organic semiconductors is tried to increase.
The main goal of this thesis is a detailed investigation of ultrafast exciton and charge carrier processes in pure organic semiconductors and their blends with fullerene derivatives. Measured organic or silicon organic semiconductors were poly-di-n-hexylsilane (PDHS), polyfluorenes F8BT and PSF-BT, merocyanine MD376. Fullerenes used in blends were C60 and its derivative PCBM. Ultrafast transient absorption, fluorescence, and integral mode photocurrent measurements were used for investigations.
The investigation of PDHS revealed that PDHS nanocomposites can be used for improvement of neat PDHS films fluorescence properties.
The formation of intramolecular charge transfer state was proposed for PSF-BT neat films. Charge transfer scheme of the formation of long-lived charge pair state in PSF-BT/PCBM blend was presented.
The formation of charge transfer states was explored in neat merocyanine films and blends with fullerene derivatives. The scheme of generation of charge pairs and free charge carriers in merocyanine blends with fullerene derivatives was discussed in... [to full text]
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Study of the photoelectrochemical properties of nanostructured titanium oxide electrodes sensitized with quantum dots: application to hybrid solar cellsGuijarro, Nestor 14 May 2013 (has links)
No description available.
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Étude par Time Resolved Microwave Conductivity de photocatalyseurs pour la dépollution de l’eau / Study by Time Resolved Microwave Conductivity of photocatalysts for wastewater treatment.Hérissan, Alexandre 16 November 2015 (has links)
La photocatalyse se base sur l’excitation d’un semi-conducteur par des photons d’énergie supérieure ou égale à son gap, générant des paires électron-trous. Celles-ci sont très réactives et susceptibles de réagir à l’interface pour réaliser par exemple l’oxydation totale d’un composé organique. Cette méthode peut être appliquée sur des eaux usées pour éliminer totalement les polluants organiques qui y sont présents. Dans la perspective d’une utilisation du soleil comme source de lumière, cette méthode peut s’avérer très économique et écologique pour le traitement de l’eau.L’interaction lumière-semi-conducteur et la dynamique des porteurs de charge sont des processus physico-chimiques primordiaux pour la photocatalyse, et il est nécessaire de bien les comprendre pour maîtriser le procédé et développer des matériaux plus efficaces. La Time Resolved Microwave Conductivity (TRMC) est une technique qui se base sur la réflexion des micro-ondes sur un semi-conducteur excité qui est directement reliée avec le nombre de porteurs de charge photo-générés. Il s’agit d’un moyen de sonder en temps réel la dynamique des porteurs de charge dans les semi-conducteurs.Ce travail s’inscrit dans le cadre du projet ANR PhotoNorm. Il consiste en une étude par TRMC de dioxyde de titane TiO2 utilisé pour la dépollution de l’eau par photocatalyse. Une partie de cette étude concerne la caractérisation des propriétés opto-électroniques des matériaux, pour lesquels la dynamique des porteurs de charge sera comparée à l’activité photocatalytique. L’effet bénéfique en photocatalyse de la déposition de nanoparticules d'or, d'argent ou bimetallique or-cuivre sur des TiO2 commerciaux sera relié à une capture d’électrons libres observée en TRMC. L’effet bénéfique sur la photocatalyse en lumière visible a été relié à une injection d’électrons dans le TiO2 par des nanoparticules de bismuth. L’autre partie de ce travail consiste en une étude plus fondamentale de la dynamique des porteurs de charge dans des TiO2 commerciaux ou synthétisés dans le cadre du projet PhotoNorm. Il y sera montré l’importance de la longueur d’onde et de l’intensité d’excitation du matériau sur le rendement de génération de porteurs de charge. L’importance des effets de surface et de l’environnement seront aussi mis en évidence de plusieurs façons. La première consiste simplement en un traitement chimique de la surface (lavage), qui peut avoir une grande influence à la fois sur la dynamique des porteurs de charge et sur la photocatalyse, sûrement en lien avec la présence d’impuretés de surface. La seconde consiste à imprégner le TiO2 par des colorants organiques présentant une forte absorption en lumière visible. Les mesures de TRMC sur ces systèmes permettent de mettre en évidence l’interaction entre le semi-conducteur et les molécules extérieures adsorbées à sa surface, notamment l’injection d’électrons du colorant excité vers le semi-conducteur, mais aussi des effets de recombinaison accrus. La troisième méthode consiste à modifier l’atmosphère de travail en TRMC. Il y est observé notamment l’importance de l’oxygène sur la dynamique des porteurs de charge, et notamment les effets de captures d’électrons, phénomènes qui entrent en jeu dans le processus de photocatalyse.Au final, la TRMC s’avère être un bon moyen d’étude de la durée de vie des porteurs de charge dans les semi-conducteurs, qui peut permettre de mieux comprendre les processus fondamentaux associés à la photocatalyse. / The photocatalysis is based on the excitation of semiconductor by photons with an energy superior or equal to the gap, generating electron-hole pairs. These are very reactive and able to react at the interface, involving for exemple the total oxidation of an organic compound. This method can be used on wastewater to eliminate the organic pollutants. With a view to use the sun as a light source this method may become an economical and ecological way for the water treatment. Light interaction between light and semiconductor and the charge-carrier dynamics are fundamental processes for photocatalysis and it is necessary to understand them in order to manage with this process and develop more efficient materials. The Time Resolved Microwave Conductivity (TRMC) is a method based on the reflexion of microwaves on an excited semiconductor which is linked to the number of photo-generated charge-carriers. This method allows us to probe in real time the charge-carrier dynamics in semiconductor. This work is included in the ANR Photonorm project. It consists in a TRMC study on titanium dioxyde TiO2 used for water depollution by photocatalysis. One part of this study consists in the characterization of the opto-electronic properties of materials for which the charge-carrier dynamics will be compared with the photocatalytic activity. The beneficial effect of nanoparticles deposition of gold, silver or gold-copper bimetallics on commercial TiO2 will be linked to the observation of free electrons observed by TRMC . The beneficial effect on photocatalysis in visible light was linked to an electron injection in TiO2 by bismuth nanoparticles. The second part of this work consists in a more fundamental study of charge-carrier dynamics on commercial or synthetized for the Photonorm project. I will be shown the importance of excitation wavelength and intensities on charge carrier generation. The importance of surface effect and environment will be emphasized by several ways. The first one just consist in surface treatment which can have a major importance on charge-carrier dynamics and photocatalysis, probably in connection with the presence or not of impurities on the surface. The second way consists in impregnating TiO2 by organic dyes which show a strong visible light absorption. The TRMC measurements highlight the interaction between the adsorbed molecules and the semiconducteur, including the electron injection from the excited dye to the TiO2 but also an increased recombination effect. The third method consist in modified the working atmosphere in TRMC. The major role of oxygen is so observed on charge-carrier dynamics, with an effect of electron capture, involving in photocatalytic mechanism.Finally TRMC proves to be a convenient method for studying charge-carrier dynamics in semiconductors, which allow a better understanding of fundamental processes bound to photocatalysis.
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Development of a femtosecond time-resolved spectroscopic ellipsometry setupHerrfurth, Oliver 26 July 2019 (has links)
The developement of a femtosecond-time-resolved spectroscopic ellipsometry setup based on a pump-probe technique is described. The characterization of the setup is presented as well as first results of experiments on a c-plane oriented ZnO thin film are shown. Indications for the study of fast charge-carrier dynamics are given.:Introduction 1
1 Theoretical framework 3
1.1 Zinc oxide . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
1.1.1 Crystal and band structure . . . . . . . . . . . . . . . . . . . . . 3
1.1.2 Excitons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
1.2 Dielectric function and electronic transitions . . . . . . . . . . . . . . . . 5
1.2.1 Electronic transitions . . . . . . . . . . . . . . . . . . . . . . . . . 5
1.2.2 Dielectric function . . . . . . . . . . . . . . . . . . . . . . . . . . 5
1.3 Charge carrier dynamics . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
1.3.1 High excitation effects . . . . . . . . . . . . . . . . . . . . . . . . 8
1.3.2 Charge carrier density-dependent dielectric function model . . . . 9
1.4 Light polarization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
2 Preliminary experiments 14
2.1 Methods and instrumentation . . . . . . . . . . . . . . . . . . . . . . . . 14
2.2 Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
2.3 Experimental challenges . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
2.4 Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
2.4.1 Time-integrated micro-ellipsometry . . . . . . . . . . . . . . . . . 28
2.4.2 Time-resolved ellipsometry . . . . . . . . . . . . . . . . . . . . . . 31
2.4.3 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33
3 Conclusive experiments at ELI Beamlines 35
3.1 Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36
3.2 Samples . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 48
3.3 Demonstration of functionality . . . . . . . . . . . . . . . . . . . . . . . . 49
3.3.1 Time-resolved reflectometry . . . . . . . . . . . . . . . . . . . . . 49
3.3.2 Time-resolved ellipsometry . . . . . . . . . . . . . . . . . . . . . . 51
4 Results and discussion 55
4.1 Time-resolved reflectometry . . . . . . . . . . . . . . . . . . . . . . . . . 55
4.2 Time-resolved ellipsometry . . . . . . . . . . . . . . . . . . . . . . . . . . 60
5 Summary and outlook 63
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Carrier Relaxation Dynamics in GrapheneMittendorff, Martin 03 November 2014 (has links)
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.
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Carrier Relaxation Dynamics in GrapheneMittendorff, Martin January 2015 (has links)
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.
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