GaInAsP-basierende Resonatorstrukturen

Physikalische Grundlagenforschung und anwendungsorientierte physikalische Forschung auf den Gebieten nanoskaliger kristalliner und amorpher fester Körper haben in vielfacher Weise eine große Bedeutung. Neben dem Verständnis für die Struktur der Materie und die Wechselwirkung von Objekten von der Größe einiger Atome ist die Erkenntnis über die physikalischen Eigenschaften nanostrukturierter Systeme von hohem Interesse. Diese Forschung eröffnet die Möglichkeit, die mit der Mikroelektronik begonnene Miniaturisierung fortzusetzen und wird darüber hinaus neue Anwendungsfelder eröffnen. Das Erarbeiten der physikalischen Grundlagen der Methoden zur Herstellung und Strukturierung ist dabei zwingend notwendig, da hier Wirkungsprinzipien dominieren, die erst bei Strukturgrößen im Nanometerbereich auftreten oder hinreichend stark ausgeprägt sind. Insbesondere Halbleitermaterialien sind hier von großem Interesse. Die in dieser Arbeit untersuchten Resonatorstrukturen, die auf dem kristallinen Verbindungshalbleitermaterial GaInAsP/InP basieren, erschließen wichtige Anwendungsfelder im Bereich der optischen Datenübertragung sowie der optischen Sensorik. Hergestellt wird das Halbleitermaterial mit der Metallorganischen Gasphasenepitaxie. Die experimentell besimmten Kenngrößen lassen Rückschlüsse auf die Güte der Materialien, die quantenmechanischen Wirkungsprinzipien und die Bauelementcharakteristik zu und führen zu optimal angepassten Kristallstrukturen. Auf Basis dieser optimierten Materialien wurde ein durchstimmbarer Fabry-Perot-Filter hergestellt, der aus einer Kombination aus InP-Membranen und Luftspalten besteht und elektromechanisch aktuiert werden kann. Das GaInAsP dient hierbei als wenige hundert nm dicke Opferschicht, die ätztechnisch hochselektiv beseitigt wird. Die Qualität der Grenzflächen zum InP ist entscheidend für die Qualität der freigeätzten Kavitäten und damit für die mechanische Gesamtstabilität der Struktur. Der in dieser Arbeit beschriebene Filter hat eine Zentralwellenlänge im Bereich von 1550 nm und weist einen Durchstimmbereich von 221 nm auf. Erzielt wurde dieser Wert durch ein konsistentes Modell der wirkenden Verspannungskomponenten und einer optimierten epitaktischen Kontrolle der Verspannungsparameter. Das realisierte Filterbauelement ist vielversprechend für den Einsatz in der optischen Kommunikation im Bereich von WDM (wavelength division multiplexing) Anwendungen. Als weitere Resonatorstrukur wurde ein Asymmetrisch gekoppelter Quantenfilm als optisch aktives Medium, bestehend aus GaInAsP mit variierender Materialkomposition und Verspannung, untersucht, um sein Potential für eine breitbandige Emission zu untersuchen und mit bekannten Modellen zu vergleichen. Als Bauelementdesign wurde eine kantenemittierende Superlumineszenzleuchtdiode gewählt. Das Ergebnis ist eine Emissionskurve von 100 nm, die eine höhere Unabhängigkeit vom Injektionsstrom aufweist als andere bekannte Konzepte. Die quantenmechanischen Wirkungsprinzipien - im wesentlichen die Kopplung der beiden asymmetrischen Potentialtöpfe und die damit verbundene Kopplung der Wellenfunktionen - werden qualitativ diskutiert. Insgesamt bestätigt sich die Eignung des Materials GaInAsP auch für neuartige, qualitativ höchst anspruchsvolle Resonatorstrukturen und die Bedeutung der vorgestellten und untersuchten Resonatorkonzepte. Die vorgestellten Methoden, Materialien und Bauelemente liefern aufgrund ihrer Konzeption und der eingehenden experimentellen Untersuchungen einen Beitrag sowohl zu den zugrunde liegenden mechanischen, optoelektronischen und quantenmechanischen Wirkungsprinzipien der Strukturen, als auch zur Realisierung neuer optoelektronischer Bauelemente.

Theory of laser-induced ultrafast structural changes in solids

The present thesis is a contribution to the study of laser-solid interaction. Despite the numerous applications resulting from the recent use of laser technology, there is still a lack of satisfactory answers to theoretical questions regarding the mechanism leading to the structural changes induced by femtosecond lasers in materials. We provide here theoretical approaches for the description of the structural response of different solids (cerium, samarium sulfide, bismuth and germanium) to femtosecond laser excitation. Particular interest is given to the description of the effects of the laser pulse on the electronic systems and changes of the potential energy surface for the ions. Although the general approach of laser-excited solids remains the same, the potential energy surface which drives the structural changes is calculated with different theoretical models for each material. This is due to the difference of the electronic properties of the studied systems. We use the Falicov model combined with an hydrodynamic method to study photoinduced phase changes in cerium. The local density approximation (LDA) together with the Hubbard-type Hamiltonian (LDA+U) in the framework of density functional theory (DFT) is used to describe the structural properties of samarium sulfide. We parametrize the time-dependent potential energy surface (calculated using DFT+ LDA) of bismuth on which we perform quantum dynamical simulations to study the experimentally observed amplitude collapse and revival of coherent $A_{1g}$ phonons. On the basis of a time-dependent potential energy surface calculated from a non-orthogonal tight binding Hamiltonian, we perform molecular dynamics simulation to analyze the time evolution (coherent phonons, ultrafast nonthermal melting) of germanium under laser excitation. The thermodynamic equilibrium properties of germanium are also reported. With the obtained results we are able to give many clarifications and interpretations of experimental results and also make predictions.

Optical Antennas for Biosensing Applications

The aim of the thesis is to theoretically investigate optical/plasmonic antennas for biosensing applications. The full 3-D numerical electromagnetic simulations have been performed by using finite integration technique (FIT). The electromagnetic properties of surface plasmon polaritons (SPPs) and the localized surface plasmons (LSPs) based devices are studied for sensing purpose. The surface plasmon resonance (SPR) biosensors offer high refractive index sensitivity at a fixed wavelength but are not enough for the detection of low concentrations of molecules. It has been demonstrated that the sensitivity of SPR sensors can be increased by employing the transverse magneto-optic Kerr effect (TMOKE) in combination with SPPs. The sensor based on the phenomena of TMOKE and SPPs are known as magneto-optic SPR (MOSPR) sensors. The optimized MOSPR sensor is analyzed which provides 8 times higher sensitivity than the SPR sensor, which will be able to detect lower concentration of molecules. But, the range of the refractive index detection is limited, due to the rapid decay of the amplitude of the MOSPR-signal with the increase of the refractive indices. Whereas, LSPs based sensors can detect lower concentrations of molecules, but their sensitivity is small at a fixed wavelength. Therefore, another device configuration known as perfect plasmonic absorber (PPA) is investigated which is based on the phenomena of metal-insulator-metal (MIM) waveguide. The PPA consists of a periodic array of gold nanoparticles and a thick gold film separated by a dielectric spacer. The electromagnetic modes of the PPA system are analyzed for sensing purpose. The second order mode of the PPA at a fixed wavelength has been proposed for the first time for biosensing applications. The PPA based sensor combines the properties of the LSPR sensor and the SPR sensor, for example, it illustrates increment in sensitivity of the LSPR sensor comparable to the SPR and can detect lower concentration of molecules due to the presence of nanoparticles.

Atomistic-continuum modeling of ultrafast laser-induced melting of silicon targets

In this work, we present an atomistic-continuum model for simulations of ultrafast laser-induced melting processes in semiconductors on the example of silicon. The kinetics of transient non-equilibrium phase transition mechanisms is addressed with MD method on the atomic level, whereas the laser light absorption, strong generated electron-phonon nonequilibrium, fast heat conduction, and photo-excited free carrier diffusion are accounted for with a continuum TTM-like model (called nTTM). First, we independently consider the applications of nTTM and MD for the description of silicon, and then construct the combined MD-nTTM model. Its development and thorough testing is followed by a comprehensive computational study of fast nonequilibrium processes induced in silicon by an ultrashort laser irradiation. The new model allowed to investigate the effect of laser-induced pressure and temperature of the lattice on the melting kinetics. Two competing melting mechanisms, heterogeneous and homogeneous, were identified in our big-scale simulations. Apart from the classical heterogeneous melting mechanism, the nucleation of the liquid phase homogeneously inside the material significantly contributes to the melting process. The simulations showed, that due to the open diamond structure of the crystal, the laser-generated internal compressive stresses reduce the crystal stability against the homogeneous melting. Consequently, the latter can take a massive character within several picoseconds upon the laser heating. Due to the large negative volume of melting of silicon, the material contracts upon the phase transition, relaxes the compressive stresses, and the subsequent melting proceeds heterogeneously until the excess of thermal energy is consumed. A series of simulations for a range of absorbed fluences allowed us to find the threshold fluence value at which homogeneous liquid nucleation starts contributing to the classical heterogeneous propagation of the solid-liquid interface. A series of simulations for a range of the material thicknesses showed that the sample width we chosen in our simulations (800 nm) corresponds to a thick sample. Additionally, in order to support the main conclusions, the results were verified for a different interatomic potential. Possible improvements of the model to account for nonthermal effects are discussed and certain restrictions on the suitable interatomic potentials are found. As a first step towards the inclusion of these effects into MD-nTTM, we performed nanometer-scale MD simulations with a new interatomic potential, designed to reproduce ab initio calculations at the laser-induced electronic temperature of 18946 K. The simulations demonstrated that, similarly to thermal melting, nonthermal phase transition occurs through nucleation. A series of simulations showed that higher (lower) initial pressure reinforces (hinders) the creation and the growth of nonthermal liquid nuclei. For the example of Si, the laser melting kinetics of semiconductors was found to be noticeably different from that of metals with a face-centered cubic crystal structure. The results of this study, therefore, have important implications for interpretation of experimental data on the kinetics of melting process of semiconductors.

First-principles electronic theory of non-collinear magnetic order in transition-metal nanowires

The structural, electronic and magnetic properties of one-dimensional 3d transition-metal (TM) monoatomic chains having linear, zigzag and ladder geometries are investigated in the frame-work of first-principles density-functional theory. The stability of long-range magnetic order along the nanowires is determined by computing the corresponding frozen-magnon dispersion relations as a function of the 'spin-wave' vector q. First, we show that the ground-state magnetic orders of V, Mn and Fe linear chains at the equilibrium interatomic distances are non-collinear (NC) spin-density waves (SDWs) with characteristic equilibrium wave vectors q that depend on the composition and interatomic distance. The electronic and magnetic properties of these novel spin-spiral structures are discussed from a local perspective by analyzing the spin-polarized electronic densities of states, the local magnetic moments and the spin-density distributions for representative values q. Second, we investigate the stability of NC spin arrangements in Fe zigzag chains and ladders. We find that the non-collinear SDWs are remarkably stable in the biatomic chains (square ladder), whereas ferromagnetic order (q =0) dominates in zigzag chains (triangular ladders). The different magnetic structures are interpreted in terms of the corresponding effective exchange interactions J(ij) between the local magnetic moments μ(i) and μ(j) at atoms i and j. The effective couplings are derived by fitting a classical Heisenberg model to the ab initio magnon dispersion relations. In addition they are analyzed in the framework of general magnetic phase diagrams having arbitrary first, second, and third nearest-neighbor (NN) interactions J(ij). The effect of external electric fields (EFs) on the stability of NC magnetic order has been quantified for representative monoatomic free-standing and deposited chains. We find that an external EF, which is applied perpendicular to the chains, favors non-collinear order in V chains, whereas it stabilizes the ferromagnetic (FM) order in Fe chains. Moreover, our calculations reveal a change in the magnetic order of V chains deposited on the Cu(110) surface in the presence of external EFs. In this case the NC spiral order, which was unstable in the absence of EF, becomes the most favorable one when perpendicular fields of the order of 0.1 V/Å are applied. As a final application of the theory we study the magnetic interactions within monoatomic TM chains deposited on graphene sheets. One observes that even weak chain substrate hybridizations can modify the magnetic order. Mn and Fe chains show incommensurable NC spin configurations. Remarkably, V chains show a transition from a spiral magnetic order in the freestanding geometry to FM order when they are deposited on a graphene sheet. Some TM-terminated zigzag graphene-nanoribbons, for example V and Fe terminated nanoribbons, also show NC spin configurations. Finally, the magnetic anisotropy energies (MAEs) of TM chains on graphene are investigated. It is shown that Co and Fe chains exhibit significant MAEs and orbital magnetic moments with in-plane easy magnetization axis. The remarkable changes in the magnetic properties of chains on graphene are correlated to charge transfers from the TMs to NN carbon atoms. Goals and limitations of this study and the resulting perspectives of future investigations are discussed.

On the transition from localized to delocalized electronic states in divalent-metal clusters

The transition from van der Waals to covalent bonding, which is expected to occur in divalent-metal clusters with increasing cluster size, is discussed. We propose a model which takes into account, within the same electronic theory, the three main competing contributions, namely the kinetic energy of the electrons, the Coulomb interactions between electrons, and the s \gdw p intraatomic transitions responsible for van der Waals like bonding. The model is solved by taking into account electron correlations using a generalized Gutzwiller approximation (slave boson method). The occurrence of electron localization is studied as a function of the interaction parameters and cluster size.

Theoretical study of magnetism, structure and chemical order in transition-metal alloy clusters

Research on transition-metal nanoalloy clusters composed of a few atoms is fascinating by their unusual properties due to the interplay among the structure, chemical order and magnetism. Such nanoalloy clusters, can be used to construct nanometer devices for technological applications by manipulating their remarkable magnetic, chemical and optical properties. Determining the nanoscopic features exhibited by the magnetic alloy clusters signifies the need for a systematic global and local exploration of their potential-energy surface in order to identify all the relevant energetically low-lying magnetic isomers. In this thesis the sampling of the potential-energy surface has been performed by employing the state-of-the-art spin-polarized density-functional theory in combination with graph theory and the basin-hopping global optimization techniques. This combination is vital for a quantitative analysis of the quantum mechanical energetics. The first approach, i.e., spin-polarized density-functional theory together with the graph theory method, is applied to study the Fe$_m$Rh$_n$ and Co$_m$Pd$_n$ clusters having $N = m+n \leq 8$ atoms. We carried out a thorough and systematic sampling of the potential-energy surface by taking into account all possible initial cluster topologies, all different distributions of the two kinds of atoms within the cluster, the entire concentration range between the pure limits, and different initial magnetic configurations such as ferro- and anti-ferromagnetic coupling. The remarkable magnetic properties shown by FeRh and CoPd nanoclusters are attributed to the extremely reduced coordination number together with the charge transfer from 3$d$ to 4$d$ elements. The second approach, i.e., spin-polarized density-functional theory together with the basin-hopping method is applied to study the small Fe$_6$, Fe$_3$Rh$_3$ and Rh$_6$ and the larger Fe$_{13}$, Fe$_6$Rh$_7$ and Rh$_{13}$ clusters as illustrative benchmark systems. This method is able to identify the true ground-state structures of Fe$_6$ and Fe$_3$Rh$_3$ which were not obtained by using the first approach. However, both approaches predict a similar cluster for the ground-state of Rh$_6$. Moreover, the computational time taken by this approach is found to be significantly lower than the first approach. The ground-state structure of Fe$_{13}$ cluster is found to be an icosahedral structure, whereas Rh$_{13}$ and Fe$_6$Rh$_7$ isomers relax into cage-like and layered-like structures, respectively. All the clusters display a remarkable variety of structural and magnetic behaviors. It is observed that the isomers having similar shape with small distortion with respect to each other can exhibit quite different magnetic moments. This has been interpreted as a probable artifact of spin-rotational symmetry breaking introduced by the spin-polarized GGA. The possibility of combining the spin-polarized density-functional theory with some other global optimization techniques such as minima-hopping method could be the next step in this direction. This combination is expected to be an ideal sampling approach having the advantage of avoiding efficiently the search over irrelevant regions of the potential energy surface.

Magnetic interactions between transition metal impurities and clusters mediated by low-dimensional metallic hosts: A first principles theoretical investigation

The magnetic properties and interactions between transition metal (TM) impurities and clusters in low-dimensional metallic hosts are studied using a first principles theoretical method. In the first part of this work, the effect of magnetic order in 3d-5d systems is addressed from the perspective of its influence on the enhancement of the magnetic anisotropy energy (MAE). In the second part, the possibility of using external electric fields (EFs) to control the magnetic properties and interactions between nanoparticles deposited at noble metal surfaces is investigated. The influence of 3d composition and magnetic order on the spin polarization of the substrate and its consequences on the MAE are analyzed for the case of 3d impurities in one- and two-dimensional polarizable hosts. It is shown that the MAE and easy- axis of monoatomic free standing 3d-Pt wires is mainly determined by the atomic spin-orbit (SO) coupling contributions. The competition between ferromagnetic (FM) and antiferromagnetic (AF) order in FePtn wires is studied in detail for n=1-4 as a function of the relative position between Fe atoms. Our results show an oscillatory behavior of the magnetic polarization of Pt atoms as a function of their distance from the magnetic impurities, which can be correlated to a long-ranged magnetic coupling of the Fe atoms. Exceptionally large variations of the induced spin and orbital moments at the Pt atoms are found as a function of concentration and magnetic order. Along with a violation of the third Hund’s rule at the Fe sites, these variations result in a non trivial behavior of the MAE. In the case of TM impurities and dimers at the Cu(111), the effects of surface charging and applied EFs on the magnetic properties and substrate-mediated magnetic interactions have been investigated. The modifications of the surface electronic structure, impurity local moments and magnetic exchange coupling as a result of the EF-induced metallic screening and charge rearrangements are analysed. In a first study, the properties of surface substitutional Co and Fe impurities are investigated as a function of the external charge per surface atom q. At large inter-impurity distances the effective magnetic exchange coupling ∆E between impurities shows RKKY-like oscillations as a function of the distance which are not significantly affected by the considered values of q. For distances r < 10 Å, important modifications in the magnitude of ∆E, involving changes from FM to AF coupling, are found depending non-monotonously on the value and polarity of q. The interaction energies are analysed from a local perspective. In a second study, the interplay between external EF effects, internal magnetic order and substrate-mediated magnetic coupling has been investigated for Mn dimers on Cu(111). Our calculations show that EF (∼ 1eV/Å) can induce a switching from AF to FM ground-state magnetic order within single Mn dimers. The relative coupling between a pair of dimers also shows RKKY-like oscillations as a function of the inter-dimer distance. Their effective magnetic exchange interaction is found to depend significantly on the magnetic order within the Mn dimers and on their relative orientation on the surface. The dependence of the substrate-mediated interaction on the magnetic state of the dimers is qualitatively explained in terms of the differences in the scattering of surface electrons. At short inter-dimer distances, the ground-state configuration is determined by an interplay between exchange interactions and EF effects. These results demonstrate that external surface charging and applied EFs offer remarkable possibilities of manipulating the sign and strength of the magnetic coupling of surface supported nanoparticles.