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Inspired by graphene, I investigate the properties of several different real and artificial Dirac materials. Firstly, I consider a two-dimensional honeycomb lattice of metallic nanoparticles, each supporting localised surface plasmons, and study the quantum properties of the collective plasmons resulting from the near field dipolar interaction between the nanoparticles. I analytically investigate the dispersion, the effective Hamiltonian and the eigenstates of the collective plasmons for an arbitrary orientation of the individual dipole moments. When the polarisation points close to normal to the plane the spectrum presents Dirac cones, similar to those present in the electronic band structure of graphene. I derive the effective Dirac Hamiltonian for the collective plasmons and show that the corresponding spinor eigenstates represent chiral Dirac-like massless bosonic excitations that present similar effects to those of electrons in graphene, such as a non-trivial Berry phase and the absence of backscattering from smooth inhomogeneities. I further discuss how one can manipulate the Dirac points in the Brillouin zone and open a gap in the collective plasmon dispersion by modifying the polarisation of the localized surface plasmons, paving the way for a fully tunable plasmonic analogue of graphene. I present a phase diagram of gapless and gapped phases in the collective plasmon dispersion depending on the dipole orientation. When the inversion symmetry of the honeycomb structure is broken, the collective plasmons become gapped chiral Dirac modes with an energy-dependent Berry phase. I show that this concept can be generalised to describe many real and artificial graphene-like systems, labeling them Dirac materials with a linear gapped spectrum. I also show that biased bilayer graphene is another Dirac material with an energy dependent Berry phase, but with a parabolic gapped spectrum. I analyse the relativistic phenomenon of Klein Tunneling in both types of system. The Klein paradox is one of the most counter-intuitive results from quantum electrodynamics but it has been seen experimentally to occur in both monolayer and bilayer graphene, due to the chiral nature of the Dirac quasiparticles in these materials. The non-trivial Berry phase of pi in monolayer graphene leads to remarkable effects in transmission through potential barriers, whereas there is always zero transmission at normal incidence in unbiased bilayer graphene in the npn regime. These, and many other 2D materials have attracted attention due to their possible usefulness for the next generation of nano-electronic devices, but some of their Klein tunneling results may be a hindrance to this application. I will highlight how breaking the inversion symmetry of the system allows for results that are not possible in these system's inversion symmetrical counterparts.

In this work, we explored one material from the broad family of 2D semiconductors, namely WSe2 to serve as an enabler for advanced, low-power, high-performance nanoelectronics and optoelectronic devices. A 2D WSe2 based field-effect-transistor (FET) was designed and fabricated using electron-beam lithography, that revealed an ultra-high mobility of ~ 625 cm2/V-s, with tunable charge transport behavior in the WSe2 channel, making it a promising candidate for high speed Si-based complimentary-metal-oxide-semiconductor (CMOS) technology. Furthermore, optoelectronic properties in 2D WSe2 based photodetectors and 2D WSe2/2D MoS2 based p-n junction diodes were also analyzed, where the photoresponsivity R and external quantum efficiency were exceptional. The monolayer WSe2 based photodetector, fabricated with Al metal contacts, showed a high R ~502 AW-1 under white light illumination. The EQE was also found to vary from 2.74×101 % - 4.02×103 % within the 400 nm -1100 nm spectral range of the tunable laser source. The interfacial metal-2D WSe2 junction characteristics, which promotes the use of such devices for end-use optoelectronics and quantum scale systems, were also studied and the interfacial stated density Dit in Al/2D WSe2 junction was computed to be the lowest reported to date ~ 3.45×1012 cm-2 eV-1. We also examined the large exciton binding energy present in WSe2 through temperature-dependent Raman and photoluminescence spectroscopy, where localized exciton states perpetuated at 78 K that are gaining increasing attention for single photon emitters for quantum information processing. The exciton and phonon dynamics in 2D WSe2 were further analyzed to unveil other multi-body states besides localized excitons, such as trions whose population densities also evolved with temperature. The phonon lifetime, which is another interesting aspect of phonon dynamics, is calculated in 2D layered WSe2 using Raman spectroscopy for the first time and the influence of external stimuli such as temperature and laser power on the phonon behavior was also studied. Furthermore, we investigated the thermal properties in 2D WSe2 in a suspended architecture platform, and the thermal conductivity in suspended WSe2 was found to be ~ 1940 W/mK which was enhanced by ~ 4X when compared with substrate supported regions. We also studied the use of halide-assisted low-pressure chemical vapor deposition (CVD) with NaCl to help to reduce the growth temperature to ∼750 °C, which is lower than the typical temperatures needed with conventional CVD for realizing 1L WSe2. The synthesis of monolayer WSe2 with high crystalline and optical quality using a halide assisted CVD method was successfully demonstrated where the role of substrate was deemed to play an important role to control the optical quality of the as-grown 2D WSe2. For example, the crystalline, optical and optoelectronics quality in CVD-grown monolayer WSe2 found to improve when sapphire was used as the substrate. Our work provides fundamental insights into the electronic, optoelectronic and quantum properties of WSe2 to pave the way for high-performance electronic, optoelectronic, and quantum-optoelectronic devices using scalable synthesis routes.

Die untersuchten Ferekristalle sind neuartige Verwachsungs-Schichtverbindungen aus m Monolagen von Niobdiselenid (NbSe2), die wiederholt mit n atomaren Bilagen von Bleiselenid (PbSe) oder Zinnselenid (SnSe) geschichtet sind. Niobdiselenid als Volumenmaterial besitzt eine Schichtstruktur und ist ein Supraleiter. Aufgrund ihrer gezielt einstellbaren atomar geschichteten Struktur können Ferekristalle als Modellsysteme für geschichtete Supraleiter dienen. In dieser Arbeit werden ihre strukturellen und elektrischen Eigenschaften untersucht. Mittels Transmissionselektronenmikroskopie wird ihre turbostratisch ungeordnete, nanokristalline Struktur nachgewiesen. Die atomare Struktur innerhalb der einzelnen Schichten ist ähnlich wie in den Volumenmaterialien NbSe2, PbSe und SnSe, wobei die kristallographischen c-Achsen parallel zur Stapelrichtung der Ferekristalle zeigen. Eine quantitative Analyse unter Verwendung eines Zwei-Schicht-Modells für den spezifischen Widerstand, Hall-Koeffizienten und Magnetwiderstand liefert ähnliche Ladungsträgersorten, -dichten und –beweglichkeiten in den NbSe2-Schichten, wie sie für isolierte Einzellagen von NbSe2 berichtet wurden. Diese unterscheiden sich von denen des Volumenmaterials NbSe2. Erstmals wurde ein Übergang der Ferekristalle in den supraleitenden Zustand nachgewiesen. Die Sprungtemperaturen sind dabei in etwa auf die Hälfte der Sprungtemperaturen der jeweiligen nicht turbostratisch ungeordneten Misfit-Schichtverbindungen reduziert. Diese Reduzierung kann der turbostratischen Unordnung der Ferekristalle zugeordnet werden. Das Verhältnis zwischen der schichtsenkrechten Ginzburg-Landau-Kohärenzlänge und dem Abstand zwischen den supraleitenden Schichten ist bei den Ferekristallen kleiner als bei den nicht ungeordneten Misfit-Schichtverbindungen, was Ferekristalle zu vielversprechenden Kandidaten für (quasi-)zweidimensionale Supraleiter macht. / The investigated ferecrystals are novel layered intergrowth compounds consisting of m monolayers of niobium diselenide (NbSe2) stacked repeatedly with n atomic bilayers of lead selenide (PbSe) or tin selenide (SnSe). Bulk NbSe2 is a layered compound showing superconductivity. Due to their artificially atomic-scale layered structure, which is tunable on the atomic scale, ferecrystals can serve as model systems for layered superconductors. In this study, their structural and electrical properties are investigated. Using transmission electron microscopy their turbostratically disordered, nanocrystalline structure is revealed. The atomic structure within the individual layers is similar as for bulk NbSe2, PbSe and SnSe, with the crystallographic c-axes parallel to the stacking direction in the ferecrystals. A quantitative analysis using a two-layer model fit for the electrical resistivity, Hall coefficient and magnetoresistance yields a similar carrier type, density and mobility in the NbSe2 layers as reported for isolated NbSe2 monolayers. These values differ from those of bulk NbSe2. For the first time, a normal-to-superconducting transition has been detected in ferecrystals. The transition temperatures of the ferecrystals are reduced to about a half of those of analogous non-disordered misfit layer compounds. This reduction in transition temperature can be correlated to the turbostratic disorder in ferecrystals. The ratio between the cross-plane Ginzburg-Landau coherence length and the cross-plane distance between the NbSe2 layers for the ferecrystals is lower than for non-disordered misfit layer compounds, making ferecrystals promising candidates for (quasi-)two-dimensional superconductors.

Discovery of grapheme has paved way for experimental realization of many physical phenomena such as massless Dirac fermions, quantum hall effect and zero-field conductivity. Search for other two dimensional (2D) materials led to the discovery of boron nitride, transition metal dichalcogenides(TMDs),transition metal oxides(MO2)and silicene. All of these materials exhibit different electronic and transport properties and are very promising for nanodevices such as nano-electromechanical-systems(NEMS), field effect transistors(FETs),sensors, hydrogen storage, nano photonics and many more. For practical utility of these materials in electronic and photonic applications, varying the band gap is very essential. Tuning of band gap has been achieved by doping, functionalization, lateral confinement, formation of hybrid structures and application of electric field. However, most of these techniques have limitations in practical applications. While, there is a lack of effective method of doping or functionalization in a controlled fashion, growth of specific sized nanostructures (e.g., nanoribbons and quantum dots),freestanding or embedded is yet to be achieved experimentally. The requirement of high electric field as well as the need for an extra electrode is another disadvantage in electric field induced tuning of band gap in low dimensional materials. Development of simpler yet effective methods is thus necessary to achieve this goal experimentally for potential application of these materials in various nano-devices. In this thesis, novel methods for tuning band gap of few 2D materials, based on strain and stacking, have been proposed theoretically using first principles based density functional theory(DFT) calculations. Electronic properties of few layered nanomaterials are studied subjected to mechanical and chemical strain of various kinds along with the effect of stacking pattern. These methods offer promising ways for controlled tuning of band gap in low dimensional materials. Detailed methodology of these proposed methods and their effect on electronic, structural or vibrational properties have also been studied. The thesis has been organized as follows: Chapter1 provides a general introduction to the low dimensional materials: their importance and potential application. An overview of the systems studied here is also given along with the traditional methods followed in the literature to tune their electronic properties. The motivation of the current research work has also been highlighted in this chapter. Chapter 2 describes the theoretical methodology adopted in this work. It gives brief understanding of first principles based Density Functional Theory(DFT) and various exchange and correlation energy functionals used here to obtain electronic, structural, vibrational and magnetic properties of the concerned materials. Chapter 3 deals with finding the origin of a novel experimental phenomenon, where electromechanical oscillations were observed on an array of buckled multiwalled carbon nanotubes (MWCNTs)subjected to axial compression. The effect of structural changes in CNTs in terms of buckling on electronic properties was studied. Contribution from intra-as well as inter-wall interactions was investigated separately by using single-and double-walled CNTs. Chapter 4 presents a method to manipulate electronic and transport properties of graphene bilayer by sliding one of the layers. Sliding caused breaking of symmetry in the graphene bilayer, which resulted in change in dispersion in the low energy bands. A transition from linear dispersion in AA stacking to parabolic dispersion in AB stacking is discussed in details. This shows a possibility to use these slid bilayers to tailor graphene based devices. Chapter 5 develops a method to tune band gap of bilayers of semiconducting transition metal dichalcogenides(TMDs) by the application of normal compressive strain. A reversible semiconductor to metal(S-M) transition was reported in this chapter for bilayers of TMDs. Chapter 6 shows the evolution of S-M transition from few layers to the bulk MoS2 under various in-plane and out of plane strains. S-M transition as a function of layer number has been studied for different strain types. A comparison between the in-plan and normal strain on modifying electronic properties is also presented. Chapter 7 discusses the electronic phase transition of bulk MoS2 under hydrostatic pressure. A hydrostatic pressure includes a combined effect of both in-plane and normal strain on the structure. The origin of metallic transition under pressure has been studied here in terms of electronic structure, density of states and charge analysis. Chapter 8 studies the chemical strain present in boron nitride nanoribbons and its effect on structural, electronic and magnetic properties of these ribbons. Properties of two achiral (armchair and zig-zag) edges have been analyzed in terms of edge energy and edge stress to predict stability of the edges. Chapter9 summarizes and concludes the work presented in this thesis.

This work is focused on the study of luminescence of atomic thin layers of transition metal chalkogenides (eg. MoS2). In the experimental part, the work deals with the preparation of atomic thin layers of semiconducting chalcogenides and the subsequent manufacturing of plasmonic interference structures around these layers. The illumination of the interference structure will create a standing plasmonic wave that will excite the photoluminescence of the semiconductor. Photoluminescence was studied both by far-field spectroscopy and near-field optical microscopy.

<div> <div> <div> <p> </p><div> <div> <div> <div> <div> <div> <p> </p><div> <div> <div> <p>Two-dimensional (2D) transition-metal dichalcogenides (TMDCs) and transition metal carbides/nitrides (MXenes), have been recently receiving attention for gas sensing applications due to their high specific area and rich surface functionalities. However, using pristine 2D materials for gas-sensing applications presents some drawbacks, including high operation temperatures, low gas response, and poor selectivity, limiting their practical sensing applications. Moreover, one of the long-standing challenges of MXenes is their poor stability against hydration and oxidation in a humid environment, which negatively influences their long- term storage and applications. Many studies have reported that the sensitivity and selectivity of 2D materials can be improved by surface functionalization and hybridization with other materials.</p><p>In this work, the effects of surface functionalization and/or hybridization of these two materials classes (TMDCs and MXenes) on their gas sensing performance have been investigated. In one of the lines of research, 2D MoS2 nanoflakes were functionalized with Au nanoparticles as a sensing material, providing a performance enhancement towards sensing of volatile organic compounds (VOCs) at room temperature. Next, a nanocomposite film composed of exfoliated MoS2, single-walled carbon nanotubes, and Cu(I)−tris(mercaptoimidazolyl)borate complexes was the sensing material used for the design of a chemiresistive sensor for the selective detection of ethylene (C2H4). Moreover, the hybridization of MXene (Ti3C2Tx) and TMDC (WSe2) as gas-sensing materials was also proposed. The Ti3C2Tx/WSe2 hybrid sensor reveals high sensitivity, good selectivity, low noise level, and ultrafast response/recovery times for the detection of various VOCs. Lastly, we demonstrated a surface functionalization strategy for Ti3C2Tx with fluoroalkylsilane (FOTS) molecules, providing a superhydrophobic surface, mechanical/environmental stability, and excellent sensing performance. The strategies presented here can be an effective solution for not only improving materials' stability, but also enhancing sensor performance, shedding light on the development of next-generation field-deployable sensors.</p> </div> </div> </div><div><div><div><div><div><div> </div> </div> </div> </div> </div> </div></div></div></div> </div> </div> </div></div></div></div><div><div><div> </div> </div> </div>

The thesis deals with study of thin layers of transition metal dichalcogenides, especially of molybdenum disulfide. Nanostructures were fabricated on two-dimensional crystals of MoS2 and WSe2. Within followed analysis attention was paid to the photoluminescence properties. In the thesis transition metal dichalcogenides are reviewed and description of the modified process of preparation by micromechanical exfoliation is given.

This work is divided in two thematic parts. The first part shows a refurbishment of a Omicron low temperature STM set-up and its utilization for preparation of superconducting-magnetic interfaces. First, a cleaning procedure of suitable metallic substrates, specifically W(110) and Ir(111), is shown. It is followed by results of iron monolayer deposition on Ir(111) (Fe-Ir(111) interface). The last section deals with study of vanadium growth on pure Ir(111) substrate as well as on mentioned Fe-Ir(111) interface. The second thematic part deals with magnetism of cobalt atoms on a monolayer metal dichalcogenide WS2. It focuses primarily on studying their magnetic moment and magnetic anisotropy using X-ray magnetic circular dichroism (XMCD).

The interplay between different self-organized electronically ordered states and their relation to unconventional electronic properties like superconductivity constitutes one of the most exciting challenges of modern condensed matter physics. In the present thesis this issue is thoroughly investigated for the prototypical layered material 1T-TaS2 both experimentally and theoretically. At first the static charge density wave order in 1T-TaS2 is investigated as a function of pressure and temperature by means of X-ray diffraction. These data indeed reveal that the superconductivity in this material coexists with an inhomogeneous charge density wave on a macroscopic scale in real space. This result is fundamentally different from a previously proposed separation of superconducting and insulating regions in real space. Furthermore, the X-ray diffraction data uncover the important role of interlayer correlations in 1T-TaS2. Based on the detailed insights into the charge density wave structure obtained by the X-ray diffraction experiments, density functional theory models are deduced in order to describe the electronic structure of 1T-TaS2 in the second part of this thesis. As opposed to most previous studies, these calculations take the three-dimensional character of the charge density wave into account. Indeed the electronic structure calculations uncover complex orbital textures, which are interwoven with the charge density wave order and cause dramatic differences in the electronic structure depending on the alignment of the orbitals between neighboring layers. Furthermore, it is demonstrated that these orbital-mediated effects provide a route to drive semiconductor-to-metal transitions with technologically pertinent gaps and on ultrafast timescales. These results are particularly relevant for the ongoing development of novel, miniaturized and ultrafast devices based on layered transition metal dichalcogenides. The discovery of orbital textures also helps to explain a number of long-standing puzzles concerning the electronic self-organization in 1T-TaS2 : the ultrafast response to optical excitations, the high sensitivity to pressure as well as a mysterious commensurate phase that is commonly thought to be a special phase a so-called “Mott phase” and that is not found in any other isostructural modification.