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- Bavarian Center for Applied Energy Research (ZAE Bayern), 97074 Würzburg, Germany (1)
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- Genelux Corporation, San Diego Science Center, 3030 Bunker Hill Street, Suite 310, San Diego, California 92109, USA (1)
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- D-1250-2010 (1)
The production of W bosons in association with two jets in proton–proton collisions at a centre-of-mass energy of \(\sqrt{s}=7\),TeV has been analysed for the presence of double-parton interactions using data corresponding to an integrated luminosity of \(36 pb^{−1}\), collected with the ATLAS detector at the Large Hadron Collider. The fraction of events arising from double-parton interactions, \(f^D_{DP}\), has been measured through the pT balance between the two jets and amounts to \(f^D_{DP}\) = 0.08 ± 0.01 (stat.) ± 0.02 (sys.) for jets with transverse momentum \(p_T\) > 20 GeV and rapidity |y| < 2.8. This corresponds to a measurement of the effective area parameter for hard double-parton interactions of \(\sigma_{eff} = 15 ± 3 (stat.)^{+5}_{−3} (sys.)\) mb.
Organic semiconductors are attractive for optical sensing applications due to the effortless processing on large active area of several \(cm^2\), which is difficult to achieve with solid-state devices. However, compared to silicon photodiodes, sensitivity and dynamic behavior remain a major challenge with organic sensors. Here, we show that charge trapping phenomena deteriorate the bandwidth of organic photodiodes (OPDs) to a few Hz at low-light levels. We demonstrate that, despite the large OPD capacitances of similar to 10 nF \(cm^{-2}\), a frequency response in the kHz regime can be achieved at light levels as low as 20 nW \(cm^{-2}\) by appropriate interface engineering, which corresponds to a 1000-fold increase compared to state-of-the-art OPDs. Such device characteristics indicate that large active area OPDs are suitable for industrial sensing and even match medical requirements for single X-ray pulse detection in the millisecond range.
Background: Cystic fibrosis (CF) patients would benefit from a safe and effective tool to detect early-stage, regional lung disease to allow for early intervention. Magnetic Resonance Imaging (MRI) is a safe, non-invasive procedure capable of providing quantitative assessments of disease without ionizing radiation. We developed a rapid normalized T1 MRI technique to detect regional lung disease in early-stage CF patients.
Materials and Methods: Conventional multislice, pulmonary T1 relaxation time maps were obtained for 10 adult CF patients with normal spirometry and 5 healthy non-CF control subjects using a rapid Look-Locker MRI acquisition (5 seconds/imaging slice). Each lung absolute T1 map was separated into six regions of interest (ROI) by manually selecting upper, central, and lower lung regions in the left and right lungs. In order to reduce the effects of subject-to-subject variation, normalized T1 maps were calculated by dividing each pixel in the absolute T1 maps by the mean T1 time in the central lung region. The primary outcome was the differences in mean normalized T1 values in the upper lung regions between CF patients with normal spirometry and healthy volunteers.
Results: Normalized T1 (nT1) maps showed visibly reduced subject-to-subject variation in comparison to conventional absolute T1 maps for healthy volunteers. An ROI analysis showed that the variation in the nT1 values in all regions was <= 2% of the mean. The primary outcome, the mean (SD) of the normalized T1 values in the upper right lung regions, was significantly lower in the CF subjects [.914 (.037)] compared to the upper right lung regions of the healthy subjects [.983 (.003)] [difference of .069 (95% confidence interval .032-.105); p=.001). Similar results were seen in the upper left lung region.
Conclusion: Rapid normalized T1 MRI relaxometry obtained in 5 seconds/imaging slice may be used to detect regional early-stage lung disease in CF patients.
The discovery of the quantum spin Hall (QSH) state, and topological insulators in general, has sparked strong experimental efforts. Transport studies of the quantum spin Hall state have confirmed the presence of edge states, showed ballistic edge transport in micron-sized samples, and demonstrated the spin polarization of the helical edge states. While these experiments have confirmed the broad theoretical model, the properties of the QSH edge states have not yet been investigated on a local scale. Using scanning gate microscopy to perturb the QSH edge states on a submicron scale, we identify well-localized scattering sites which likely limit the expected nondissipative transport in the helical edge channels. In the micron-sized regions between the scattering sites, the edge states appear to propagate unperturbed, as expected for an ideal QSH system, and are found to be robust against weak induced potential fluctuations.
We report on electrically pumped quantum dot-microlasers in the presence of polarized self-feedback. The high-\(\beta\) microlasers show two orthogonal, linearly polarized emission modes which are coupled via the common gain medium. This coupling is explained in terms of gain competition between the two lasing modes and leads to distinct differences in their input-output characteristics. By applying polarized self-feedback via an external mirror, we are able to control the laser characteristics of the emission modes in terms of the output power, the coherence time and the photon statistics. We find that linearly polarized self-feedback stabilizes the lasing of a given mode, while cross-polarized feedback between the two modes reduces strongly the intensity of the other emission mode showing particular high-intensity fluctuations and even super-thermal values of the photon autocorrelation function \(g^{(2)} (\tau)\) at zero delay. Measurements of \(g^{(2)} (\tau)\) under external feedback also allow us to detect revival peaks associated with the round trip time of the external cavity. Analyzing the damping and shape of the \(g^{(2)} (\tau)\) revival peaks by a phenomenological model provides us insight into the underlying physics such as the effective exciton lifetime and gain characteristics of the quantum dots in the active region of these microlasers.
Dirac particles, massless relativistic entities, obey linear energy dispersions and hold important implications in particle physics. The recent discovery of Dirac fermions in condensed matter systems including graphene and topological insulators has generated a great deal of interest in exploring the relativistic properties associated with Dirac physics in solid-state materials. In addition, there are stimulating research activities to engineer Dirac particles, elucidating their exotic physical properties in a controllable setting. One of the successful platforms is the ultracold atom-optical lattice system, whose dynamics can be manipulated and probed in a clean environment. A microcavity exciton-polariton-lattice system offers the advantage of forming high-orbital condensation in non-equilibrium conditions, which enables one to explore novel quantum orbital order in two dimensions. In this paper, we experimentally construct the band structures near Dirac points, the vertices of the first hexagonal Brillouin zone with exciton-polariton condensates trapped in a triangular lattice. Due to the finite spectral linewidth, the direct map of band structures at Dirac points is elusive; however, we identify the linear part above Dirac points and its associated velocity value is similar to ~0.9-2 x \(10^8 cm s^{-1}\), consistent with the theoretical estimate \(1 x 10^8 cm s^{-1}\) with a \(2 \mu m\) lattice constant. We envision that the exciton-polariton condensates in lattices would be a promising solid-state platform, where the system order parameter can be accessed in both real and momentum spaces.
Interaction between light and matter generates optical nonlinearities, which are particularly pronounced in the quantum strong coupling regime. When a single bosonic mode couples to a single fermionic mode, a Jaynes-Cummings (JC) ladder is formed, which we realize here using cavity photons and quantum dot excitons. We measure and model the coherent anharmonic response of this strongly coupled exciton-cavity system at resonance. Injecting two photons into the cavity, we demonstrate a \(\sqrt 2\) larger polariton splitting with respect to the vacuum Rabi splitting. This is achieved using coherent nonlinear spectroscopy, specifically four-wave mixing, where the coherence between the ground state and the first (second) rung of the JC ladder can be interrogated for positive (negative) delays. With increasing excitation intensity and thus rising average number of injected photons, we observe spectral signatures of the quantum-to-classical crossover of the strong coupling regime.
We report a detailed experimental and theoretical study of the electronic structure of \(Mo_{1-x}Re_x\) random alloys. We have measured electronic band dispersions for clean and hydrogen-covered \(Mo_{1-x}Re_x\) ( 110) with x = 0-0.25 using angle-resolved photoemission spectroscopy. Our results suggest that the bulk and most surface electronic bands shift relative to the Fermi level systematically and approximately rigidly with Re concentration. We distinguish and quantify two contributions to these shifts: a raise of the Fermi energy and an increase of the overall bandwidth. Alloy bands calculated using the first-principles Korringa-Kohn-Rostoker coherent-potential-approximation method accurately predict both of these effects. As derived from the rigid band model, the Fermi energy shift is inversely related to the bulk density of states in this energy region. Using our results, we also characterize an electronic topological transition of the bulk Fermi surface and relate this to bulk transport properties. Finally, we distinguish effects beyond the rigid band approximation: a highly surface-localized state and a composition-dependent impact of the spin-orbit interaction.
Carbonaceous aerosols are responsible for large uncertainties in climate models, degraded visibility, and adverse health effects. The Carbonaceous Aerosols and Radiative Effects Study (CARES) was designed to study carbonaceous aerosols in the natural environment of the Central Valley, California, and learn more about their atmospheric formation and aging. This paper presents results from spectro-microscopic measurements of carbonaceous particles collected during CARES at the time of a pollution accumulation event (27-29 June 2010), when in situ measurements indicated an increase in the organic carbon content of aerosols as the Sacramento urban plume aged. Computer-controlled scanning electron microscopy coupled with an energy dispersive X-ray detector (CCSEM/EDX) and scanning transmission X-ray microscopy coupled with near-edge X-ray absorption spectroscopy (STXM/NEXAFS) were used to probe the chemical composition and morphology of individual particles. It was found that the mass of organic carbon on individual particles increased through condensation of secondary organic aerosol. STXM/NEXAFS indicated that the number fraction of homogenous organic particles lacking inorganic inclusions (greater than similar to 50 nm equivalent circular diameter) increased with plume age, as did the organic mass per particle. Comparison of the CARES spectro-microscopic dataset with a similar dataset obtained in Mexico City during the MILAGRO campaign showed that fresh particles in Mexico City contained three times as much carbon as those sampled during CARES. The number fraction of soot particles at the Mexico City urban site (ranging from 16.6 to 47.3 %) was larger than at the CARES urban site (13.4-15.7%), and the most aged samples from CARES contained fewer carbon-carbon double bonds. Differences between carbonaceous particles in Mexico City and California result from different sources, photochemical conditions, gas phase reactants, and secondary organic aerosol precursors. The detailed results provided by these spectro-microscopic measurements will allow for a comprehensive evaluation of aerosol process models used in climate research.
For determination of structures and structural dynamics of proteins organic fluorophores are a standard instrument. Intra- and intermolecular contact of biomolecular structures are determined in time-resolved and stationary fluorescence microscopy experiments by quenching of organic fluorophores due to Photoinduced Electron Transfer (PET) and dimerization interactions. Using PET we show in this work that end-to-end contact dynamics of serine-glycine peptides are slowed down by glycosylation. This slow down is due to a change in reaction enthalpy for end-to-end contact and is partly compensated by entropic effects. In a second step we test how dimerization of MR121 fluorophore pairs reports on end-to-end contact dynamics. We show that in aqueous solutions containing strong denaturants MR121 dimerization reports advantageously on contact dynamics for glycine-serine oligopeptides compared to the previously used MR121/tryptophane PET reporters. Then we analyze dimer interactions and quenching properties of different commercially available fluorophores being standards in Förster Resonance Energy Transfer (FRET) measurements. Distances in biomolecules are determinable using FRET, but for very flexible biomolecules the analysis of masurement data can be distorted if contact of the two FRET fluorophores is likely. We quantify how strong the quenching of fluorophore pairs with two different or two identical fluorophores is. Dimer spectra and association constants are quantified to estimate if fluophores are applicable in various applications, e.g. in FRET measurements with unstructured peptides and proteins.
Atherosclerosis is an active and progressive condition where the vascular cell adhesion molecules as VCAM-1 play a vital role controlling the recruitment of immune cells within the early and advanced plaques. Therefore targeting of VCAM-1 molecules with specific contrast agent bears the possibility to monitor the VCAM-1 expression, visualize the plaque progression starting at the early alterations, and help to establish early prevention of atherosclerosis before the origin of the thrombus formation, of which late recognition leads to myocardial infarction. Furthermore noninvasive magnetic resonance imaging (MRI) offers the benefit of combining the molecular and anatomic data and would thus enable specific detection of VCAM-1 targeted iron oxide contrast agent within inflammatory process of atherosclerosis. This thesis exactly presents the VCAM-1 concept as a suitable molecular approach and the potential of specific ultrasmall superparamagnetic iron oxide (USPIO) conjugated to the VCAM-1 binding peptide over unspecific non-targeted USPIO particles for evaluation of atherosclerosis. This work firstly demonstrated that selection of VCAM-1 molecules offers a good and potential strategy for imaging of atherosclerosis, as these vascular cell adhesion molecules are highly expressed in the early phase of inflammation and also continuously up-regulated within the advanced plaques. Secondly, this thesis showed the proof of principle and capability of the newly designed USPIO contrast agent conjugated to the specific cyclic peptide for VCAM-1 recognition. The experimental studies including ultra-high field MRI enabled further ex vivo and in vivo detection of applied USPIO-VCAM-1 particles within the aortic root region of early and advanced atherosclerotic plaques of 12 and 30 week old apolipoprotein E deficient (ApoE-/-) mice. Using a combination of histology and electron microscopy, this study for the first time pointed to distribution of targeted USPIO-VCAM-1 particles within plaque cells expressing VCAM-1 not only in luminal regions but also in deeper medial smooth muscle cell areas. Hence functionalized USPIO particles targeting VCAM-1 molecules allow specific and sensitive detection of early and advanced plaques at the molecular level, giving the new possibilities for early recognition of atherosclerotic plaques before the appearance of advanced and prone to rupture lesions. In contrast to the functionalized USPIO-VCAM-1, utilized non-targeted USPIO particles did not succeed in early plaque 6 identification limiting visualization of atherosclerosis to advanced forms in atherosclerotic ApoE-/- mice.
Background
The aortic pulse-wave velocity (PWV) is an important indicator of cardiovascular risk. In recent studies MRI methods have been developed to measure this parameter noninvasively in mice. Present techniques require additional hardware for cardiac and respiratory gating. In this work a robust self-gated measurement of the local PWV in mice without the need of triggering probes is proposed.
Methods
The local PWV of 6-months-old wild-type C57BL/6J mice (n=6) was measured in the abdominal aorta with a retrospectively triggered radial Phase Contrast (PC) MR sequence using the flow-area (QA) method. A navigator signal was extracted from the CMR data of highly asymmetric radial projections with short repetition time (TR=3 ms) and post-processed with high-pass and low-pass filters for retrospective cardiac and respiratory gating. The self-gating signal was used for a reconstruction of high-resolution Cine frames of the aortic motion. To assess the local PWV the volume flow Q and the cross-sectional area A of the aorta were determined. The results were compared with the values measured with a triggered Cartesian and an undersampled triggered radial PC-Cine sequence.
Results
In all examined animals a self-gating signal could be extracted and used for retrospective breath-gating and PC-Cine reconstruction. With the non-triggered measurement PWV values of 2.3±0.2 m/s were determined. These values are in agreement with those measured with the triggered Cartesian (2.4±0.2 m/s) and the triggered radial (2.3±0.2 m/s) measurement. Due to the strong robustness of the radial trajectory against undersampling an acceleration of more than two relative to the prospectively triggered Cartesian sampling could be achieved with the retrospective method.
Conclusion
With the radial flow-encoding sequence the extraction of a self-gating signal is feasible. The retrospective method enables a robust and fast measurement of the local PWV without the need of additional trigger hardware.
Silicon carbide light-emitting diode as a prospective room temperature source for single photons
(2013)
Generation of single photons has been demonstrated in several systems. However, none of them satisfies all the conditions, e.g. room temperature functionality, telecom wavelength operation, high efficiency, as required for practical applications. Here, we report the fabrication of light-emitting diodes (LEDs) based on intrinsic defects in silicon carbide (SiC). To fabricate our devices we used a standard semiconductor manufacturing technology in combination with high-energy electron irradiation. The room temperature electroluminescence (EL) of our LEDs reveals two strong emission bands in the visible and near infrared (NIR) spectral ranges, associated with two different intrinsic defects. As these defects can potentially be generated at a low or even single defect level, our approach can be used to realize electrically driven single photon source for quantum telecommunication and information processing.
Background
Malignant pleural effusion (MPE) is associated with advanced stages of lung cancer and is mainly dependent on invasion of the pleura and expression of vascular endothelial growth factor (VEGF) by cancer cells. As MPE indicates an incurable disease with limited palliative treatment options and poor outcome, there is an urgent need for new and efficient treatment options.
Methods
In this study, we used subcutaneously generated PC14PE6 lung adenocarcinoma xenografts in athymic mice that developed subcutaneous malignant effusions (ME) which mimic pleural effusions of the orthotopic model. Using this approach monitoring of therapeutic intervention was facilitated by direct observation of subcutaneous ME formation without the need of sacrificing mice or special imaging equipment as in case of MPE. Further, we tested oncolytic virotherapy using Vaccinia virus as a novel treatment modality against ME in this subcutaneous PC14PE6 xenograft model of advanced lung adenocarcinoma.
Results
We demonstrated significant therapeutic efficacy of Vaccinia virus treatment of both advanced lung adenocarcinoma and tumor-associated ME. We attribute the efficacy to the virus-mediated reduction of tumor cell-derived VEGF levels in tumors, decreased invasion of tumor cells into the peritumoral tissue, and to viral infection of the blood vessel-invading tumor cells. Moreover, we showed that the use of oncolytic Vaccinia virus encoding for a single-chain antibody (scAb) against VEGF (GLAF-1) significantly enhanced mono-therapy of oncolytic treatment.
Conclusions
Here, we demonstrate for the first time that oncolytic virotherapy using tumor-specific Vaccinia virus represents a novel and promising treatment modality for therapy of ME associated with advanced lung cancer.
Nuclear spins in motion is an intrinsic component of any dynamic process when studied using magnetic resonance imaging (MRI). Moving spins define many functional characteristics of the human body such as diffusion, perfusion and blood flow. Quantitative MRI of moving spins
can provide valuable information about the human physiology or of a technical system. In particular, phase-contrast MRI, which is based on two images with and without a flow-encoding gradient, has emerged as an important diagnostic tool in medicine to quantify human blood flow. Unfortunately, however, its clinical usage is hampered by long acquisition times which only provide mean data averaged across multiple cardiac cycles and therefore preclude Monitoring the immediate physiological responses to stress or exercise. These limitations are expected to be overcome by real-time imaging which constitutes a primary aim of this thesis.
Short image acquisition times, as the core for real-time phase-contrast MRI, can be mainly realized through undersampling of the acquired data. Therefore the development focused on related technical aspects such as pulse sequence design, k-space encoding schemes and image
reconstruction. A radial encoding scheme was experimentally found to be robust to motion and
less sensitive to undersampling than Cartesian encoding. Radial encoding was combined with a FLASH acquisition technique for building an efficient real-time phase-contrast MRI sequence.
The sequence was further optimized through overlapping of gradients to achieve the shortest possible echo time. Regularized nonlinear inverse reconstruction (NLINV), a technique which jointly estimates the image content and its corresponding coil sensitivities, was used for image
reconstruction. NLINV was adapted specifically for phase-contrast MRI to produce both Magnitude images and phase-contrast maps. Real-time phase-contrast MRI therefore combined two highly undersampled (up to a factor of 30) radial gradient-echo acquisitions with and without a
flow-encoding gradient with modified NLINV reconstructions. The developed method achieved
real-time phase-contrast MRI at both high spatial (1.3 mm) and temporal resolution (40 ms).
Applications to healthy human subjects as well as preliminary studies of patients demonstrated
real-time phase-contrast MRI to offer improved patient compliance (e.g., free breathing) and immediate access to physiological variations of flow parameters (e.g., response to enhanced intrathoracic pressure). In most cases, quantitative blood flow was measured in the ascending aorta as an important blood vessel of the cardiovascular circulation system commonly studied
in the clinic. The performance of real-time phase-contrast MRI was validated in comparison to standard Cine phase-contrast MRI using studies of flow phantoms as well as under in vivo conditions. The evaluations confirmed good agreement for comparable results.
As a further extension to real-time phase-contrast MRI, this thesis implemented and explored a dual-echo phase-contrast MRI method which employs two sequential gradient echoes with and without flow encoding. The introduction of a flow-encoding gradient in between the two echoes
aids in the further reduction of acquisition time. Although this technique was efficient under in vitro conditions, in vivo studies showed the influence of additional motion-induced Phase contributions. Due to these additional temporal phase information, the approach showed Little promise for quantitative flow MRI.
As a further method three-dimensional real-time phase-contrast MRI was developed in this thesis to visualize and quantify multi-directional flow at about twice the measuring time of the standard real-time MRI method, i.e. at about 100 ms temporal resolution. This was achieved
through velocity mapping along all three physical gradient directions. Although the method is still too slow to adequately cover cardiovascular blood flow, the preliminary results were found to be promising for future applications in tissues and organ systems outside the heart. Finally, future developments are expected to benefit from the adaptation of model-based reconstruction
techniques to real-time phase-contrast MRI.
In the field of organic photovoltaics, one of the most intensely researched topics to date is the charge carrier photogeneration in organic bulk heterojunction solar cells whose thorough understanding is crucial for achieving higher power conversion efficiencies. In particular, the mechanism of singlet exciton dissociation at the polymer–fullerene interface is still controversially debated.
This work addresses the dissociation pathway via relaxed charge transfer states (CTS) by investigating its field dependence for reference material systems consisting of MDMO-PPV and one of the fullerene derivatives PC61BM, bisPCBM and PC71BM. Field dependent photoluminescence (PL(F)) and transient absorption (TA(F)) measurements give insight into the recombination of charge transfer excitons (CTE) and the generation of polarons, respectively. Optically detected magnetic resonance and atomic force microscopy are used to characterize the morphology of the samples.
The comparison of the experimental field dependent exciton recombination recorded by PL(F) and the theoretical exciton dissociation probability given by the Onsager–Braun model yields the exciton binding energy as one of the key parameters determining the dissociation efficiency. The binding energies of both the singlet exciton in neat MDMO-PPV and the CTE in MDMO-PPV:PC61BM 1:1 are extracted, the latter turning out to be significantly reduced with respect to the one of the singlet exciton.
Based on these results, the field dependence of CTE dissociation is evaluated for MDMO-PPV:PC61BM blends with varying fullerene loads by PL(F) and TA(F). For higher PC61BM contents, the CTE binding energies decrease notably. This behavior is ascribed to a larger effective dielectric constant for well-intermixed blends and to an interplay between dielectric constant and CTE delocalization length for phase separated morphologies, emphasizing the importance of high dielectric constants for the charge carrier photogeneration process.
Finally, the CTE binding energies are determined for MDMO-PPV blends with different fullerene derivatives, focusing on the influence of the acceptor LUMO energy. Here, the experimental results suggest the latter having no or at least no significant impact on the binding energy of the CTE. Variations of this binding energy are rather related to different trap levels in the acceptors which seem to be involved in CTS formation.
In this work, we take a look at the connection of gamma-ray bursts (GRBs) and ultra-high-energy cosmic rays (UHECR) as well as the possibilities how to verify this connection. The currently most promising approach is based on the detection of high-energy neutrinos, which are associated with the acceleration of cosmic rays. We detail how the prompt gamma-ray emission is connected to the prediction of a neutrino signal. We focus on the interactions of photons and protons in this regard. At the example of the current ANTARES GRB neutrino analysis, we show the differences between numerical predictions and older analytical methods. Moreover, we discuss the possibilities how cosmic ray particles can escape from GRBs, assuming that UHECR are entirely made up of protons. For this, we compare the commonly assumed neutron escape model with a new component of direct proton escape. Additionally, we will show that the different components, which contribute to the cosmic ray flux, strongly depend on the burst parameters, and test the applicability on some chosen GRBs. In a further step, we continue with the considerations regarding the connection of GRBs and UHECR by connecting the GRB source model with the cosmic
ray observations using a simple cosmic ray propagation code. We test if it is possible to achieve the observed cosmic ray energy densities with our simple model and what the consequences are regarding the prompt GRB neutrino flux predictions as well as the cosmogenic neutrinos. Furthermore, we consider the question of neutrino lifetime and how it affects the prompt GRB neutrino flux predictions. In a final chapter, we show that it is possible to apply the basic source model with photohadronic interactions to other types of sources, using the example of the microquasar Cygnus X-3.
The study of magnetic phases in spintronic materials is crucial to both our fundamental understanding of magnetic interactions and for finding new effects for future applications.
In this thesis, we study the basic electrical and magnetic transport properties of both epitaxially-grown MnSi thin films, a helimagnetic metal only starting to be developed within our group, and parabolic-doped ultra-thin (Ga,Mn)As layers for future studies and applications.
The focus of this work is studying recombination mechanisms occurring in organic solar cells, as well as their impact on one of their most important parameters — the open circuit voltage Voc.
Firstly, the relationship between Voc and the respective charge carrier density n in the active layer under open circuit conditions is analyzed. Therefor, a model after Shockley for the open circuit voltage is used, whose validity is proven with the aid of fits to the measured data. Thereby, it is emphasized that the equation is only valid under special conditions. In the used reference system P3HT:PC61BM the fits are in agreement with the measurement data only in the range of high temperatures (150 - 300 K), where Voc increases linearly with decreasing temperature. At lower temperatures (50 – 150 K), the experiment shows a saturation of Voc. This saturation cannot be explained with the model by the measured falling charge carrier density with decreasing temperatures. In this temperature range Voc is not directly related to the intrinsic properties of the active layer. Voc saturation is due to injection energy barriers at the contacts, which is ascertained by macroscopic simulations. Furthermore, it is observed that Voc in the case of saturation is equivalent to the so-called built-in potential. The difference between the built-in potential and the energy gap corresponds thereby to the sum of the energy barriers at both contacts.
With the knowledge of the Voc(n) dependency for not contact limited solar cells, it is possible to investigate the recombination mechanisms of charge carriers in the active layer. For Langevin recombination the recombination rate is Rn2 (recombination order RO = 2), for Shockley-Read-Hall (SRH) Rn1 (RO=1); in various publications RO higher than two is reported with two main explanations.
1: Trap states for charge carriers exist in the respective separated phases, i.e. electrons in the acceptor phase and holes in the donor phase, which leads to a delayed recombination of the charge carriers at the interface of both phases and finally to an apparent recombination order higher than 2.
2: The enhanced R(n) dependency is attributed to the so called recombination prefactor, which again is dependent from n dependent mobility µ.
It is shown that for the system P3HT:PC61BM at room temperature the µ(n) dependency does nearly completely explain the higher RO but not at lower temperatures which in this case supports the first explanation. In the material system PTB7:PC71BM the increased RO cannot be explained by the µ(n) dependency even at room temperature.
To support the importance of trap states in combination with a phase separation for the explanation of the enhanced RO, additional trap states were incorporated in the solar cells to investigate their influence on the recombination mechanisms. To achieve this, P3HT:PC61BM solar cells were exposed to synthetic air (in the dark and under illumination) or TCNQ was added in small concentrations to the active layer which act as electron traps. For the oxygen degraded solar cell the recombination order is determined by a combination of open Voc-transients and Voc(n) measurements. Thereby, a continuous increase of the recombination order from 2.4 to more than 5 is observed with higher degradation times. By the evaluation of the ideality factor it can be shown that the impact of SRH recombination is increasing with higher trap concentration in relation to Langevin recombination. A similar picture is revealed for solar cells with TCNQ as extrinsic trap states.
Finally, a phenomenon called s-shaped IV-curves is investigated, which can sometimes occur for solar cells under illumination. As course of this a reduced surface recombination velocity can be found. Experimentally, the solar cells were fabricated using a special plasma treatment of the ITO contact. The measured IV-curves of such solar cells are reproduced by macroscopic simulations, where the surface recombination velocity is reduced. Hereby, it has to be distinguished between the surface recombination of majority and minority charge carriers at the respective contacts. The theory can be experimentally confirmed by illumination level dependent IV-curves as well as short circuit current density and open circuit voltage transients.
Continuously increasing energy prices have considerably influenced the cost of living over the last decades. At the same time increasingly extreme weather conditions, drought-filled summers as well as autumns and winters with heavier rainfall and worsening storms have been reported. These are possibly the harbingers of the expected approaching global climate change. Considering the depletability of fossil energy sources and a rising distrust in nuclear power, investigations into new and innovative renewable energy sources are necessary to prepare for the coming future.
In addition to wind, hydro and biomass technologies, electricity generated by the direct conversion of incident sunlight is one of the most promising approaches. Since the syntheses and detailed studies of organic semiconducting polymers and fullerenes were intensified, a new kind of solar cell fabrication became conceivable. In addition to classical vacuum deposition techniques, organic cells were now also able to be processed from a solution, even on flexible substrates like plastic, fabric or paper.
An organic solar cell represents a complex electrical device influenced for instance by light interference for charge carrier generation. Also charge carrier recombination and transport mechanisms are important to its performance. In accordance to Coulomb interaction, this results in a specific distribution of the charge carriers and the electric field, which finally yield the measured current-voltage characteristics. Changes of certain parameters result in a complex response in the investigated device due to interactions between the physical processes. Consequently, it is necessary to find a way to generally predict the response of such a device to temperature changes for example.
In this work, a numerical, one-dimensional simulation has been developed based on the drift-diffusion equations for electrons, holes and excitons. The generation and recombination rates of the single species are defined according to a detailed balance approach. The Coulomb interaction between the single charge carriers is considered through the Poisson equation. An analytically non-solvable differential equation system is consequently set-up. With numerical approaches, valid solutions describing the macroscopic processes in organic solar cells can be found. An additional optical simulation is used to determine the spatially resolved charge carrier generation rates due to interference.
Concepts regarding organic semiconductors and solar cells are introduced in the first part of this work. All chapters are based on previous ones and logically outline the basic physics, device architectures, models of charge carrier generation and recombination as well as the mathematic and numerical approaches to obtain valid simulation results.
In the second part, the simulation is used to elaborate issues of current interest in organic solar cell research. This includes a basic understanding of how the open circuit voltage is generated and which processes limit its value. S-shaped current-voltage characteristics are explained assigning finite surface recombination velocities at metal electrodes piling-up local space charges. The power conversion efficiency is identified as a trade-off between charge carrier accumulation and charge extraction. This leads to an optimum of the power conversion efficiency at moderate to high charge carrier mobilities. Differences between recombination rates determined by different interpretations of identical experimental results are assigned to a spatially inhomogeneous recombination, relevant for almost all low mobility semiconductor devices.
In the context of this thesis, the novel method soft X-ray energy-dispersive NEXAFS spectroscopy was explored and utilized to investigate intermolecular coupling and post-growth processes with a temporal resolution of seconds. 1,4,5,8- naphthalene tetracarboxylic acid dianhydride (NTCDA)multilayer films were the chosen model system for these investigations. The core hole-electron correlation in coherently coupled molecules was studied by means of energy-dispersive near-edge X-ray absorption fine-structure spectroscopy. A transient phase was found which exists during the transition between a disordered condensed phase and the bulk structure. This phase is characterized by distinct changes in the spectral line shape and energetic position of the X-ray absorption signal at the C K-edge. The findings were explained with the help of theoretical models based on the coupling of transition dipole moments, which are well established for optically excited systems. In consequence, the experimental results provides evidence for a core hole-electron pair delocalized over several molecules. Furthermore, the structure formation of NTCDA multilayer films on Ag(111) surfaces was investigated. With time-resolved and energy-dispersive NEXAFS experiments the intensity evolution in s- and p-polarization showed a very characteristic behavior. By combining these findings with the results of time-dependent photoemission measurements, several sub-processes were identified in the post- growth behavior. Upon annealing, the amorphous but preferentially flat-lying molecules flip into an upright orientation. After that follows a phase characterized by strong intermolecular coupling. Finally, three-dimensional islands are established. Employing the Kolmogorov-Johnson-Mehl-Avrami model, the activation energies of the sub-processes were determined.
Besides established, conventional inorganic photovoltaics—mainly based on silicon—organic photovoltaics (OPV) are well on the way to represent a lowcost, environment friendly, complementary technology in near future. Production costs, solar cell lifetime and performance are the relevant factors which need to be optimized to enable a market launch of OPV. In this work, the efficiency of organic solar cells and their limitation due to charge carrier recombination are investigated. To analyze solar cells under operating conditions, time-resolved techniques such as transient photovoltage (TPV), transient photocurrent (TPC) and charge extraction (CE) are applied in combination with time delayed collection field (TDCF) measurements. Solution processed and evaporated samples of different material composition and varying device architectures are studied. The standard OPV reference system, P3HT:PC61BM, is analyzed for various temperatures in terms of charge carrier lifetime and charge carrier density for a range of illumination intensities. The applicability of the Shockley Equation for organic solar cells is validated in case of field-independent charge photogeneration. In addition, a consistent model is presented, directly relating the ideality factor to the recombination of free with trapped charge carriers in an exponential density of states. An approach known as j=V reconstruction enables to identify the performance limiting loss mechanism of as-prepared and thermally treated P3HT:PC61BM solar cells. This procedure, involving TPV, CE and TDCF measurements, is extended to samples based on the rather new, low-band gap polymer PTB7 in combination with PC71BM. While in the devices processed from pure chlorobenzene solution considerable geminate and nongeminate losses are observed, the use of a solvent additive facilitates efficient polaron pair dissociation minimizing geminate recombination. Finally, in collaboration with the IMEC institute in Leuven, the two main organic solar cell device architectures, planar and bulk heterojunction—both based on CuPc and C60—are directly compared in terms of nongeminate recombination and charge carrier distribution. Two experimental techniques, TPV and CE, as well as a macroscopic device simulation are applied to reveal the origin of different Voc vs. light intensity dependence.
The present thesis studies the (Ga,Mn)As material in terms of optimization of very thin (4 nm) (Ga,Mn)As layers, epitaxially fabricated by the molecular beam epitaxy (MBE) technology. First of all, the ferromagnetic semiconductor (Ga,Mn)As with its structural, magnetic and electrical properties is introduced. The influences of point defects, interface and surface effects on bulk and thin (Ga,Mn)As layers are discussed by simplified self-consistent band alignment calculations. The experimental part is divided in three blocks: The first part studies the influence of epitaxial growth parameter conditions on electrical and magnetic properties of bulk (70 nm) (Ga,Mn)As layers. The second part introduces an alternative, parabolical Mn doping-profile instead of a 4 nm layer with a homogeneous Mn doping-profile. Improved properties of the parabolic layer have been observed as well as comparable magnetic and electrical properties to bulk (Ga,Mn)As layers, both with a Mn content of 4%. MBE growth parameters for the (Ga,Mn)As layers with a parabolically graded Mn profile and lowered nominal Mn content of 2.5% have been investigated. A narrow growth window has been found in which low-temperature (LT) layer properties are improved. The last part of this thesis presents an application of magnetic anisotropy control of a bulk (Ga,Mn)As layer.
The present thesis deals with the fabrication, optimization of growth process and characterization of silicon based materials with molecular beam epitaxy. Two material systems are investigated in the course of this work: silicon/silicon suboxide multilayer structures and mono manganese silicide thin films. Mono manganese silicide (MnSi) is grown on Si(111) substrates with an hydrogen passivated surface, that is prepared by wet chemical processes. The growth start is performed by deposition of an amorphous Mn wetting layer that is subsequently annealed to form a MnSi seed layer on which the MnSi molecular beam epitaxy (MBE) is achieved. An amorphous or a crystalline Si cap layer is deposited onto the MnSi film to finalize the growth process and protect the sample from oxidation. With Raman spectroscopy it is shown that the crystalline cap layer is in fact single crystalline silicon. Results of x-ray diffraction and Raman spectroscopy confirm the growth of mono manganese silicide in contrast to other existing manganese silicide phases. In addition, in-plane and out-of-plane residual strain, and twinning of the MnSi thin film is detected with x-ray diffraction of symmetric and asymmetric reflections. Orientation between the Si substrate and the MnSi film is determined with the parallel lattice planes MnSi(210) and Si(511). Transport measurements show a T^2 dependence of the resistivity below 30K and metallic behavior above, a magneto resistance of 0.9% and an unusual memory like effect of the resistance for an in-plane magnetic field sweep measurement. Silicon/Silicon suboxide (SiOx) multilayer structures are grown on Si(100) by interrupting the Si growth and oxidizing the surface with molecular oxygen. During oxidation the RHEED pattern changes from the Si(2x1) reconstruction to an amorphous pattern. When silicon growth is resumed a spotty RHEED pattern emerges, indicating a rough, three dimensional surface. The rough surface can be smoothed out with Si growth at substrate temperatures between 600°C and 700°C. Measurements with transmission electron microscopy show that a silicon suboxide layer of about 1nm embedded in single crystalline silicon is formed with the procedure. Multilayer structures are achieved by repeating the oxidation procedure when the Si spacer layer has a smooth and flat surface. The oxygen content of the suboxide layers can be varied between 7.6% and 26.8%, as determined with secondary ion mass spectrometry and custom-built simulations models for the x-ray diffraction. Structural stability of the multilayer structures is investigated by x-ray diffraction before and after rapid thermal annealing. For temperatures up to 1000°C the multilayer structures show no modification of the SiOx layer in x-ray diffraction.
The present thesis is concerned with the impact of alkali metal-doping on the electronic structure of semiconducting organic thin films. The organic molecular systems which have been studied are the polycyclic aromatic hydrocarbons picene, pentacene, and coronene. Motivated by reports about exceptional behavior like superconductivity and electronic correlations of their alkali metal-doped compounds, high quality films fabricated from the above named molecules have been studied. The electronic structure of the pristine materials and their doped compounds has been investigated using photoelectron spectroscopy. Core level and valence band studies of undoped films yield excellent photoemission spectra agreeing with or even outperforming previously reported data from the literature. Alkali metal-doping manifests itself in a uniform manner in the electronic structure for all probed samples: Opposed to reports from the literature about metallicity and even superconductivity in alkali metal-doped picene, pentacene, and coronene, all films exhibit insulating nature with an energy gap of the order of one electron-volt. Remarkably, this is independent of the doping concentration and the type of dopant, i.e., potassium, cesium, or sodium. Based on the interplay between narrow bandwidths in organic semiconductors and sufficiently high on-molecule Coulomb repulsion, the non-metallicity is attributed to the strong influence of electronic correlations leading to the formation of a Mott insulator. In the case of picene, this is consolidated by calculations using a combination of density functional theory and dynamical mean-field theory. Beyond the extensive considerations regarding electronic correlations, further intriguing aspects have been observed. The deposition of thin picene films leads to the formation of a non-equilibrium situation between substrate and film surface. Here, the establishment of a homogeneous chemical potential is hampered due to the only weak van der Waals-interactions between the molecular layers in the films. Consequently, spectral weight is measurable above the reference chemical potential in photoemission. Furthermore, it has been found that the acceptance of additional electrons in pentacene is limited. While picene and coronene are able to host up to three extra electrons, in pentacene the limit is already reached for one electron. Finally, further extrinsic effects, coming along with alkali metal-doping, have been scrutinized. The oxidation of potassium atoms induced by the reaction with molecular oxygen in the residual gas of the ultra-high vacuum system turned out to significantly influence the electronic structure of alkali metal-doped picene and coronene. Moreover, also the applied X-ray and UV irradiation caused a certain impact on the photoemission spectra. Surprisingly, both effects did not play a role in the studies of potassium-doped pentacene.
In the presented thesis, the various excited states encountered in conjugated organic semiconductors are investigated with respect to their utilization in organic thin-film solar cells. Most of these states are spin-baring and can therefore be addressed by means of magnetic resonance spectroscopy. The primary singlet excitation (spin 0), as well as positive and negative polaronic charge carriers (spin 1/2) are discussed. Additionally, triplet excitons (spin 1) and charge transfer complexes are examined, focussing on their differing spin-spin interaction strength. For the investigation of these spin-baring states especially methods of electron paramagnetic resonance (EPR) are best suited. Therefore according experimental methods were implemented in the course of this work to study conjugated polymers, fullerenes and their blends with continuous wave as well as time-resolved EPR and optically detected magnetic resonance.
Atomare Ketten, sogenannte Nano-Drähte, entstehen durch Selbstorganisation adsorbierter Metallatome auf einer Halbleiteroberfläche. Aufgrund der starken räumlichen Einschränkung der Ladungsträger innerhalb dieser Ketten entsteht dabei oftmals eine metallische Bandstruktur mit starker Anisotropie. Im Falle phononischer Ankopplung an das Substrat kann so ein eindimensionales (1D) Metall instabil gegen eine periodische Gitterverzerrung werden, bei der es zu einer Ausbildung einer Energielücke kommt. Dieser Metall-Isolator-Übergang wird dabei als Peierls Übergang bezeichnet. Für verschwindend geringe Kopplung der Ketten untereinander bzw. an das Substrat, d.h. im strikt eindimensionalen Fall, bricht das Fermi Flüssigkeitsmodell für dreidimensionale (3D) Metalle zusammen. Dessen Quasiteilchen werden durch kollektive Anregungen von Spin und Ladung ersetzt. Diesen Zustand bezeichnet man als Tomonaga-Luttinger Flüssigkeit. Beide Phänomene, Peierlsübergang und Tomonaga-Luttinger Flüssigkeit lassen sich anhand der elektronischen Bandstruktur experimentell nachweisen. Bei dem hier untersuchten Probensystem handelt es sich um Gold-induzierte Nandrähte auf der Germanium (001)-Oberfläche, kurz Au/Ge(001). Deren Wachstum erfolgt epitaktisch entlang der durch das Substrat vorgegebenen Dimer-Reihen, welche die freie Germaniumoberfläche in Form einer (2×1)-Symmetrie einnimmt. Die abwechselnde Stapelfolge ABAB des Substrates führt dabei zu zwei unterschiedlichen Drahtrichtungen, die jeweils um 90° zueinander gedreht sind, wenn man eine Einfachstufe von 1.4 A von einer A-Terrasse auf eine B-Terrasse oder umgekehrt geht. Die vorherrschende Kinetik während der Gold-Deposition bzw. das Benetzungsverhalten ermöglicht dabei eine vollständige Bedeckung der vormals freien Oberfläche mit Nanodrähten, deren Abmessungen einzig und allein durch Defekte bzw. die Größe der darunterliegenden Ge-Terrasse begrenzt sind. Um die Längenskala der Subtrat-Terrassen zu optimieren, wurde eine Reinigungsprozedur für Ge (001) entwickelt, bei der nass-chemisches Ätzen mit anschliessender Trocken-Oxidation zum Einsatz kommt. Die darauf aufbauenden Nanodrähte wurden im Anschluss mittels winkelaufgelöster Photoelektronenspektroskopie auf ihre elektronische Bandstruktur untersucht. Dabei wurden zwei neuartige Zustände beobachtet: ein metallischer, zweidimensionaler Loch-Zustand, der seinen Ursprung höchstwahrscheinlich in tieferen Schichten des Germaniums hat; und ein eindimensionaler Oberflächenzustand mit elektronenartiger Dispersion, dessen bandintegrierte Spektralfunktion von der einer Fermiflüssigkeit abweicht. Stattdessen wird ein exponentieller Abfall des spektralen Gewichtes als Funktion der Energie zum Ferminiveau hin beobachtet. Dieses Verhalten kann über einen weiten Temperaturbereich beobachtet werden und lässt sich mit der Tomonaga-Luttinger Flüssigkeit für strikt eindimensionale Systeme erklären. Zum weiteren theoretischen Verständnis dieses Phänomes, beispielsweise durch Bandstrukuturrechnungen mittels Dichte-Funktional-Theorie, bedarf es der genauen Kenntnis der atomaren Struktur dieser Ketten. Selbige wurde mittels Oberflächenröntgenbeugung (engl. surface x-ray diffraction, SXRD) untersucht. Auf Basis der gewonnenen Patterson-Karte lassen sich Rückschlüsse auf die interatomaren Abstände der Goldatome untereinander in der Einheitszelle ziehen. Dies stellt einen ersten wichtigen Schritt auf dem Weg zu einem vollständigen Strukturmodell dar. Darüber hinaus wurden erste vielversprechende Schritte unternommen, das Nanodrahtsystem kontrolliert zu manipulieren. Durch geringfügige, zusätzliche Deposition von Kalium konnte dabei eine schrittweise Erhöhung der Bandfüllung erzielt werden. Für weitergehende Kaliumanlagerungen im (Sub-)Monolagenbereich konnte sogar eine neue Rekonstruktion erzielt werden.