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Precision laser spectroscopy of the 229-thorium nuclear isomer transition in a solid-state environment would represent a significant milestone in the field of metrology, opening the door to the realization of a nuclear clock. Working toward this goal, experimental methods require knowledge of various properties of a large band-gap material, such as calcium fluoride doped with specific isotopes of the heavy elements thorium, actinium, cerium, neptunium, and uranium. By accurately determining the atomic structure of potential charge compensation schemes by using a generalized gradient approximation within the ab-initio framework of density functional theory, calculations of electric field gradients on the dopants become accessible, which cause a quadrupole splitting of the nuclear-level structure that can be probed experimentally. Band gaps and absorption coefficients in the range of the 229-thorium nuclear transition are estimated by using the G0W0 method and by solving the Bethe–Salpeter equation.

Single quantum dots and other materials exhibit irregular switching between on and off states; these on-off states follow power-law statistics giving rise to 1/f noise. We transfer this phenomenon (also referred to as on-off intermittency) to the generation and recombination (g-r) process in semiconductor materials. In addition to g-r noise we obtain 1/f noise that can be provided in the form of the Hooge relation. The predicted Hooge coefficient depends on the parameters of the g-r noise and on the parameters of the intermittency. Due to the power-law distribution of the on-times, the coefficient for intermittency shows a smooth dependence on time t. We also suggest an alternative form of the 1/f noise formula by Hooge relating the 1/f noise to the number of centers (such as donor or trap atoms) rather than to the number of charge carriers as defined by Hooge., Comment: 17 pages, 9 figures

We present laser-induced photothermal synthesis of atomically precise graphene nanoribbons (GNRs). The kinetics of photothermal bottom-up GNR growth are unravelled by in situ Raman spectroscopy carried out in ultrahigh vacuum. We photothermally drive the reaction steps by short periods of laser irradiation and subsequently analyze the Raman spectra of the reactants in the irradiated area. Growth kinetics of chevron GNRs (CGNRs) and seven atoms wide armchair GNRs (7-AGNRs) is investigated. The reaction rate constants for polymerization, cyclodehydrogenation, and interribbon fusion are experimentally determined. We find that the limiting rate constants for CGNR growth are several hundred times smaller than for 7-AGNR growth and that interribbon fusion is an important elementary reaction occurring during 7-AGNR growth. Our work highlights that photothermal synthesis and in situ Raman spectroscopy are a powerful tandem for the investigation of on-surface reactions.

openaire: EC/H2020/648589/EU//SUPER-2D By combining scanning tunneling microscopy, low-energy electron diffraction, photoluminescence and Raman spectroscopy experiments with molecular dynamics simulations, a comprehensive picture of the structural and electronic response of a monolayer of MoS 2 to 500 eV Xe + irradiation is obtained. The MoS 2 layer is epitaxially grown on graphene/Ir(1 1 1) and analyzed before and after irradiation in situ under ultra-high vacuum conditions. Through optimized irradiation conditions using low-energy ions with grazing trajectories, amorphization of the monolayer is induced already at low ion fluences of 1.5 × 10 14 ions cm -2 and without inducing damage underneath the MoS 2 layer. The crystalline-to-amorphous transformation is accompanied by changes in the electronic properties from semiconductor-to-metal and an extinction of photoluminescence. Upon thermal annealing, the re-crystallization occurs with restoration of the semiconducting properties, but residual defects prevent the recovery of photoluminescence.

We show that Cs intercalated bilayer graphene acts as a substrate for the growth of a strained Cs film hosting quantum well states with high electronic quality. The Cs film grows in an fcc phase with a substantially reduced lattice constant of 4.9 Å corresponding to a compressive strain of 11% compared to bulk Cs. We investigate its electronic structure using angle-resolved photoemission spectroscopy and show the coexistence of massless Dirac and massive Schrödinger charge carriers in two dimensions. Analysis of the electronic self-energy of the massive charge carriers reveals the crystallographic direction in which a two-dimensional Fermi gas is realized. Our work introduces the growth of strained metal quantum wells on intercalated Dirac matter., Cesium atoms that are grown on intercalated bilayer graphene can create an ordered epitaxial film. Here, the authors report that such a strained film can host quantum well states with high electronic quality as characterized through angle-resolved photoemission spectroscopy.

A flat energy dispersion of electrons at the Fermi level of a material leads to instabilities in the electronic system and can drive phase transitions. Here we introduce a method to induce a flat band in two-dimensional (2D) materials. We show that the flat band can be achieved by sandwiching the 2D material by two cesium (Cs) layers. We apply this method to monolayer graphene and investigate the flat band by a combination of angle-resolved photoemission spectroscopy experiment and the calculation. Our work highlights that charge transfer, zone folding of graphene bands and the covalent bonding between C and Cs atoms are at the origin of the flat energy band formation. The presented approach is an alternative route for obtaining flat band materials to twisting bilayer graphene which yields thermodynamically stable flat band materials in large areas., 22 pages, 4 Figures

The photoluminescence from aligned 7-atom wide armchair-edge graphene nanoribbons coupled to plasmonic nanoantennas was recently observed to display blinking. Photoluminescence blinking is a hallmark of emission from single quantum emitters. Here we explore the origin of the blinking. We study the influence of the local field enhancement in the vicinity of nanoantennas on the photoluminescence blinking. We observe a clear correlation between the blinking amplitudes and the plasmonic enhancement. For non-resonant metal nanostructures the blinking vanishes almost completely. Our results allow us to conclude that the blinking is an intrinsic feature of the emission from the graphene nanoribbons. This is in contrast to the case of single-molecule surface-enhanced Raman scattering, where it is known that ballistic charge transfer between plasmonic nanoparticles and the molecule under study critically contributes to the blinking.

We measure the absolute absorbance of a single layer of seven atom wide armchair graphene nanoribbons and study the influence of laser-induced defects on the absorption spectrum of the ribbons. We find that the absorption spectrum shows a broad peak at approximately 2.4 eV that is attributed to excitonic transitions and a smaller peak at 1.77 eV. The low-energy peak is diminished when we induce defects in the material. Simultaneously the photoluminescence is significantly enhanced. We thus attribute the 1.77 eV spectral feature in the absorption spectrum to a quenching state, which energetically coincides with the emission. Our results clearly demonstrate the significance of this state in photoluminescence processes in the ribbons. We additionally measure the dependence of the generation of defects on the energy of the incident photons and the photoluminescence excitation spectrum. The photoluminescence excitation efficiency peaks at a higher photon energy than the maximum absorption, hinting at an efficient decay from higher energetic states to the emissive state.

Scanning tunneling microscopy and spectroscopy are used to image the charge density wave at the surface of cleaved ${\mathrm{VSe}}_{2}$ and to probe its local density of states at 5 K. The main features in the spectrum are linked to the contributions of the $p$-like and $d$-like bands of ${\mathrm{VSe}}_{2}$ found in angle-resolved photoemission spectroscopy and tight-binding calculations. Different from previous tunneling spectroscopy work, we find a narrow partial gap at the Fermi level that we associate with the charge density wave phase. The energy scale of the gap found in the experiment is in good agreement with the charge density wave transition temperature of ${\mathrm{VSe}}_{2}$, under the assumption of weak electron-phonon coupling, consistent with the Peierls model of Fermi surface nesting. The role of defects is investigated, which reveals that the partial gap in the density of states and hence the charge density wave itself is extremely stable, though the order, phase, and amplitude of the charge density waves on the surface are strongly perturbed by defects.

The master-equation approach provides generation-recombination (g-r) noise in bulk semiconductors in terms of parameters of conduction electrons. It is shown that the g-r bulk noise can also be described by the random succession of elementary g-r pulses. This enables g-r bulk noise to be interpreted in terms of the numbers of traps. The transition from g-r bulk noise to discrete switching in small-area semiconductors is found by reducing the number of traps to just one single active trap. The resulting g-r noise spectrum is shown to be equivalent to Machlups noise spectrum. The probability of an overlap of succeeding g-r pulses is calculated. Such an overlap is attributed to the occupation of an empty single trap by an electron transferred from a neighboring trap. Simulating a g-r pulse train we find a large variety of patterns similar to those observed in MOSFETs. Excluding overlapping g-r pulses, the up and down distribution of succeeding g-r pulses is estimated., 13 pages, 9 figures and addendum

A setup for the preparation of oriented Au(111)/mica thin films of ∼100 nm thickness as an active substrate for graphene nanoribbon growth is shown. Low-energy electron diffraction shows that the Au(111) thin films have a single crystallographic orientation over the whole surface area. Graphene nanoribbons are synthesized by the bottom-up approach via surface polymerization of precursor molecules that are evaporated onto the catalytically active Au(111)/mica substrate. The graphene nanoribbons are investigated by a combination of resonance Raman, X-ray photoemission spectroscopy, and near-edge X-ray absorption fine structure spectroscopy confirming a nanoribbon quality equal to nanoribbons grown on commercially available single-crystal Au(111) substrates. The present work, therefore, establishes the insitu preparation of Au(111)/mica as an inexpensive and simple method to prepare substrates of desired shape and thickness for surface polymerization reactions which are of interest to a growing community of researchers working on graphene nanoribbons.

A lowest limit of 1/f noise in semiconductor materials has not yet been reported; we do not even know if such a lowest limit exists. 1/f noise in semiconductors has recently been brought into relation with 1/f noise in quantum dots and other materials. These materials exhibit on-off states which are power-law distributed over a wide range of timescales. We transfer such findings to semiconductors, assuming that the g-r process is also controlled by such on-off states. As a result, we obtain 1/f noise which can be expressed in the form of the Hooge relation. Based on the intermittent g-r process, we estimate the lowest limit of 1/f noise in semiconductor materials. We show that this limit is inversely proportional to the dopant concentration; to detect the lowest limit of 1/f noise, the number of centers should be as small as possible. We also find a smooth dependence of 1/f noise and g-r noise on time., 10 pages, 9 figures. arXiv admin note: substantial text overlap with arXiv:2108.07155

We employ ultra-high vacuum (UHV) Raman spectroscopy in tandem with angle-resolved photoemission (ARPES) to investigate the doping-dependent Raman spectrum of epitaxial graphene on Ir(111). The evolution of Raman spectra from pristine to heavily Cs doped graphene up to a carrier concentration of 4.4*10^14cm^-2 is investigated. At this doping graphene is at the onset of the Lifshitz transition and renormalization effects reduce the electronic bandwidth. The optical transition at the saddle point in the Brillouin zone then becomes experimentally accessible by ultraviolet (UV) light excitation which achieves resonance Raman conditions in close vicinity to the van Hove singularity in the joint density of states. The position of the Raman G band of fully doped graphene/Ir(111) shifts down by ~60cm^-1. The G band asymmetry of Cs doped epitaxial graphene assumes an unusual strong Fano asymmetry opposite to that of the G band of doped graphene on insulators. Our calculations can fully explain these observations by substrate dependent quantum interference effects in the scattering pathways for vibrational and electronic Raman scattering.

Stannous selenide is a layered semiconductor that is a polar analogue of black phosphorus, and of great interest as a thermoelectric material. Unusually, hole doped SnSe supports a large Seebeck coefficient at high conductivity, which has not been explained to date. Angle resolved photo-emission spectroscopy, optical reflection spectroscopy and magnetotransport measurements reveal a multiple-valley valence band structure and a quasi two-dimensional dispersion, realizing a Hicks-Dresselhaus thermoelectric contributing to the high Seebeck coefficient at high carrier density. We further demonstrate that the hole accumulation layer in exfoliated SnSe transistors exhibits a field effect mobility of up to $250~\mathrm{cm^2/Vs}$ at $T=1.3~\mathrm{K}$. SnSe is thus found to be a high quality, quasi two-dimensional semiconductor ideal for thermoelectric applications., 10 pages, 5 figures, plus supporting information

The phase diagrams of correlated systems like cuprates or pnictides high-temperature superconductors are characterized by a topological change of the Fermi surface under continuous variation of an external parameter, the so-called Lifshitz transition. However, the large number of low-temperature instabilities and the interplay of multiple energy scales complicate the study of this phenomenon. Here we first identify the optical signatures of a pressure-induced Lifshitz transition in a clean elemental system, black phosphorus. By applying external pressures above 1.5 GPa, we observe a change in the pressure dependence of the Drude plasma frequency due to the appearance of massless Dirac fermions. At higher pressures, optical signatures of two structural phase transitions are also identified. Our findings suggest that a key fingerprint of the Lifshitz transition in solid state systems, and in absence of structural phase transitions, is a discontinuity of the Drude plasma frequency due to the change of Fermi surface topology.

We couple photoluminescent semiconducting 7-atom wide armchair edge graphene nanoribbons to plasmonic nanoantenna arrays and demonstrate an enhancement of the photoluminescence and Raman scattering intensity of the nanoribbons by more than an order of magnitude averaged over large areas, and by three orders of magnitude in the hot spots of plasmonic antennas. The increase in signal allows us to study Raman spectra with high signal-to-noise ratio. Using plasmonic enhancement we are able to detect the off-resonant Raman scattering from the modified radial breathing-like mode (RBLM) due to physisorbed molecules, the 3rd order RBLM, and C-H vibrations. We find excellent agreement between experimental data and simulations describing the spectral dependence of the enhancement and modifications of the polarization anisotropy. The strong field gradients in the optical near-field further allow us to probe the subwavelength coherence properties of the phonon modes in the nanoribbons. We theoretically model this considering a finite phonon correlation length along the GNR direction. Our results allow estimating the correlation length in graphene nanoribbons.

Using angle-resolved photoemission spectroscopy (ARPES), we study the electronic structure and electron-phonon coupling in a Li-doped graphene monolayer decoupled from the Co(0001) substrate by intercalation of silicon. Based on the photoelectron diffraction measurements, we disclose the structural properties of the Si/Co interface. Our density functional theory calculations demonstrate that in the studied Li/graphene/Si/Co system the magnetism of Co substrate induces notable magnetic moments on Li and Si atoms. At the same time graphene remains almost nonmagnetic and clamped between two magnetically active atomic layers with antiparallel magnetizations. ARPES maps of the graphene Fermi surface reveal strong electron doping, which may lead to superconductivity mediated by electron-phonon coupling (EPC). Analysis of the spectral function of photoelectrons reveals apparent anisotropy of EPC in the k space. These properties make the studied system tempting for studying the relation between superconductivity and magnetism in two-dimensional materials., D.Yu.U., D.V.V., and A.V.F. acknowledge SPbU for research Grant No. 11.65.42.2017 and RFBR (Grant No. 17-02-00427). D.Yu.U., I.I.O., and M.V.K. acknowledge RFBR (Grant No. 16-29-06410). C.L. acknowledges DFG (Grant No. LA655-17/1). A.G. and A.V.F. acknowledge ERC Grant No. 648589 “SUPER-2D” and funding from DFG project CRC 1238 (project A1) and DFG project GR 3708/2-1. We acknowledge Helmholtz-Zentrum Berlin für Materialien und Energie for support within the bilateral Russian-German Laboratory program.

International audience; We present a first-principles density functional theory study on the structural, electronic and dynamical properties of a novel barium doped graphene phase. Low energy electron diffraction of barium doped graphene presents clear evidence of (2 × 2) spots induced by barium adatoms with BaC8 stoichiometry. First principles calculations reveals that the phase is thermodynamically stable but unstable to segregation towards the competitive BaC6 monolayer phase. The calculation of phonon spectrum confirms the dynamical stability of the BaC8 phase indicating its metastability, probably stabilized by doping and strain conditions due to the substrate. Barium induces a relevant doping of the graphene π states and new barium-derived hole Fermi surface at the M-point of the (2 × 2) Brillouin zone. In view of possible superconducting phase induced by foreign dopants in graphene, we studied the electron–phonon coupling of this novel (2 × 2) obtaining λ = 0.26, which excludes the stabilization of a superconducting phase.

We report a Cs-doping-induced band inversion and the direct observation of a surface resonance state with an elliptical Fermi surface in black phosphorus (BP) using angle-resolved photoemission spectroscopy. By selectively inducing a higher electron concentration (1.7×1014cm-2) in the topmost layer, the changes in the Coulomb potential are sufficiently large to cause surface band inversion between the parabolic valence band of BP and a parabolic surface state around the Γ point of the BP Brillouin zone. Tight-binding calculations reveal that band gap openings at the crossing points in the two high-symmetry directions of the Brillouin zone require out-of-plane hopping and breaking of the glide mirror symmetry. Ab initio calculations are in very good agreement with the experiment if a stacking fault on the BP surface is taken into account. The demonstrated level of control over the band structure suggests the potential application of few-layer phosphorene in topological field-effect transistors.

© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim A semiconductor-to-metal transition in N = 7 armchair graphene nanoribbons causes drastic changes in its electron and phonon system. By using angle-resolved photoemission spectroscopy of lithium-doped graphene nanoribbons, a quasiparticle band gap renormalization from 2.4 to 2.1 eV is observed. Reaching high doping levels (0.05 electrons per atom), it is found that the effective mass of the conduction band carriers increases to a value equal to the free electron mass. This giant increase in the effective mass by doping is a means to enhance the density of states at the Fermi level which can have palpable impact on the transport and optical properties. Electron doping also reduces the Raman intensity by one order of magnitude, and results in relatively small (4 cm−1) hardening of the G phonon and softening of the D phonon. This suggests the importance of both lattice expansion and dynamic effects. The present work highlights that doping of a semiconducting 1D system is strikingly different from its 2D or 3D counterparts and introduces doped graphene nanoribbons as a new tunable quantum material with high potential for basic research and applications.

© 2017 American Chemical Society. We demonstrate the alignment-preserving transfer of parallel graphene nanoribbons (GNRs) onto insulating substrates. The photophysics of such samples is characterized by polarized Raman and photoluminescence (PL) spectroscopies. The Raman scattered light and the PL are polarized along the GNR axis. The Raman cross section as a function of excitation energy has distinct excitonic peaks associated with transitions between the one-dimensional parabolic subbands. We find that the PL of GNRs is intrinsically low but can be strongly enhanced by blue laser irradiation in ambient conditions or hydrogenation in ultrahigh vacuum. These functionalization routes cause the formation of sp3 defects in GNRs. We demonstrate the laser writing of luminescent patterns in GNR films for maskless lithography by the controlled generation of defects. Our findings set the stage for further exploration of the optical properties of GNRs on insulating substrates and in device geometries.

In recent years, solid-state spin systems have emerged as promising candidates for quantum information processing (QIP). Prominent examples are the Nitrogen-Vacancy (NV) center in diamond, phosphorous dopants in silicon (Si:P), rare-earth ions in solids and V$_{\text{Si}}$-centers in Silicon-carbide (SiC). The Si:P system has demonstrated, that by eliminating the electron spin of the dopant, its nuclear spins can yield exceedingly long spin coherence times. For NV centers, however, a proper charge state for storage of nuclear spin qubit coherence has not been identified yet. Here, we identify and characterize the positively charged NV center as an electron-spin-less and optically inactive state by utilizing the nuclear spin qubit as a probe. We control the electronic charge and spin utilizing nanometer scale gate electrodes. We achieve a lengthening of the nuclear spin coherence times by a factor of 20. Surprisingly, the new charge state allows switching the optical response of single nodes facilitating full individual addressability., 8 pages, 4 figures, 1 table

We report a systematic ab-initio density functional theory investigation of Ni(111) surface alloyed with elements of group IV (Si, Ge and Sn), demonstrating the possibility to use it to grow high quality graphene. Ni(111) surface represents an ideal substrate for graphene, due to its catalytic properties and perfect matching with the graphene lattice constant. However, Dirac bands of graphene growth on Ni(111) are completely destroyed due to the strong hybridization between carbon pz and Ni d orbitals. Group IV atoms, namely Si, Ge and Sn, once deposited on Ni(111) surface, form an ordered alloyed surface with √ 3 × √ 3-R30◦ reconstruction. We demonstrate that, at variance with the pure Ni(111) surface, alloyed surfaces effectively decouple graphene from the substrate, resulting unstrained due to the nearly perfect lattice matching and preserves linear Dirac bands without the strong hybridization with Ni d states. The proposed surfaces can be prepared before graphene growth without resorting on post-growth processes which necessarily alter the electronic and structural properties of graphene.

Many propositions have been already put forth for the practical use of N-graphene in various devices, such as batteries, sensors, ultracapacitors, and next generation electronics. However, the chemistry of nitrogen imperfections in this material still remains an enigma. Here we demonstrate a method to handle N-impurities in graphene, which allows efficient conversion of pyridinic N to graphitic N and therefore precise tuning of the charge carrier concentration. By applying photoemission spectroscopy and density functional calculations, we show that the electron doping effect of graphitic N is strongly suppressed by pyridinic N. As the latter is converted into the graphitic configuration, the efficiency of doping rises up to half of electron charge per N atom.

The electronic properties and surface structures of K-doped graphene supported on Ir(111) are characterized as a function of temperature and coverage by combining low-energy electron diffraction, angle-resolved photoemission spectroscopy, and density functional theory (DFT) calculations. Deposition of K on graphene at room temperature (RT) yields a stable $(\ensuremath{\surd}3\ifmmode\times\else\texttimes\fi{}\ensuremath{\surd}3)$ R30\ifmmode^\circ\else\textdegree\fi{} surface structure having an intrinsic electron doping that shifts the graphene Dirac point by ${E}_{D}=1.30\phantom{\rule{0.16em}{0ex}}\mathrm{eV}$ below the Fermi level. Keeping the graphene substrate at 80 K during deposition generates instead a $(2\ifmmode\times\else\texttimes\fi{}2)$ phase, which is stable until full monolayer coverage. Further deposition of K followed by RT annealing develops a double-layer K-doped graphene that effectively doubles the K coverage and the related charge transfer, as well as maximizing the doping level $({E}_{D}=1.61\phantom{\rule{0.16em}{0ex}}\mathrm{eV})$. The measured electron doping and the surface reconstructions are rationalized by DFT calculations. These indicate a large thermodynamic driving force for K intercalation below the graphene layer. The electron doping and Dirac point shifts calculated for the different structures are in agreement with the experimental measurements. In particular, the ${\mathrm{K}}_{4s}$ bands are shown to be sensitive to both the K intercalation and periodicity and are therefore suggested as a fingerprint for the location and ordering of the K dopants.

A novel strategy for efficient growth of nitrogen-doped graphene (N-graphene) on a large scale from s-triazine molecules is presented. The growth process has been unveiled in situ using time-dependent photoemission. It has been established that a postannealing of N-graphene after gold intercalation causes a conversion of the N environment from pyridinic to graphitic, allowing to obtain more than 80% of all embedded nitrogen in graphitic form, which is essential for the electron doping in graphene. A band gap, a doping level of 300 meV, and a charge-carrier concentration of ∼8×10(12) electrons per cm2, induced by 0.4 atom % of graphitic nitrogen, have been detected by angle-resolved photoemission spectroscopy, which offers great promise for implementation of this system in next generation electronic devices.

D. Haberer*,1, L. Petaccia2, Y. Wang3, H. Quian3, M. Farjam4, S. A. Jafari4,5, H. Sachdev6,7, A. V. Federov8, D. Usachov8, D. V. Vyalikh8,9, X. Liu10, O. Vilkov8,9, V. K. Adamchuk8, S. Irle3, M. Knupfer1, B. Buchner1, and A. Gruneis1,10 1 IFW Dresden, P.O. Box 270116, 01171 Dresden, Germany 2 Elettra Synchrotron Light Laboratory, Sincrotrone Trieste SCpA, S.S. 14 Km 163.5, 34149 Trieste, Italy 3 Department of Chemistry, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8602, Japan 4 Institute for Research in Fundamental Sciences (IPM), P.O. Box 19395-5531, Tehran, Iran 5 Department of Physics, Sharif University of Technology, Tehran 11155-9161, Iran 6 Anorganische Chemie 8.11, Universitat des Saarlandes, 66041 Saarbrucken, Germany 7 Max-Planck-Institut fur Polymerforschung, Ackermannweg 10, 55128 Mainz, Germany 8 St. Petersburg State University, St. Petersburg 198504, Russia 9 Institut fur Festkorperphysik, TU Dresden, Mommsenstrasse 13, 01069 Dresden, Germany 10 Faculty of Physics, University of Vienna, Strudlhofgasse 4, 1090 Wien, Austria

We demonstrate the growth of high quality graphene layers by chemical vapor deposition (CVD) on insulating and conductive SiC substrates. This method provides key advantages over the well-developed epitaxial graphene growth by Si sublimation that has been known for decades. (1) CVD growth is much less sensitive to SiC surface defects resulting in high electron mobilities of ∼1800 cm(2)/(V s) and enables the controlled synthesis of a determined number of graphene layers with a defined doping level. The high quality of graphene is evidenced by a unique combination of angle-resolved photoemission spectroscopy, Raman spectroscopy, transport measurements, scanning tunneling microscopy and ellipsometry. Our measurements indicate that CVD grown graphene is under less compressive strain than its epitaxial counterpart and confirms the existence of an electronic energy band gap. These features are essential for future applications of graphene electronics based on wafer scale graphene growth.

We investigate fixed dopants in the presence of mobile point defects. A defect entering the first Bohr radius RB of a dopant will modulate the generation-recombination (g-r) process. The times a defect walks inside and outside of RB are found to be power-law distributed; correspondingly, the modulated g-r process exhibits 1/fb noise. The predicted Hooge coefficient depends on RB, on the normalized fluctuations of charge carriers, the number of lattice sites and on the modulation depth of the g-r process.

Carbon nanotubes are archetypical one dimensional systems, with peculiar anisotropic electronic properties. Only recently μm thick films of vertically aligned SWNT became available. The vertical alignment of the nanotube mats allows the realization of scattering geometries promoting specific dipole transitions parallel and normal to the axis of the SWNT. We find well expressed mosaic spreads for the π* and σ* resonances. Full three dimensional modelling of the dipole transitions as well as of the alignment demonstrate polarization dependent X-ray absorption to be an accurate, versatile non destructive and reliable tool to quantify the alignment of SWNT on a bulk scale.

The growth process of inner-shell tubes from C 60 peapods and ferrocene (FeCp 2 ) filled single-wall carbon nanotubes was studied with Raman spectroscopy and X-ray diffraction (XRD). In the peapod case, it is shown that the Raman signal of the fullerenes decays about a factor five faster than the XRD peak of the 1D fullerene chain. The growth of the inner-shell tubes coincides well with the 1D chain decay. In the FeCp 2 case, the inner tubes grow already at 600 °C in about one hour. Additionally, even for the same starting material, the inner-outer tube pair distribution is different than for C 60 based inner tubes.

Defined n-doping of carbon nanotubes can find potential application in nanoelectronics and sensors. An efficient doping can be achieved by substituting Carbon by heteroatoms such as Nitrogen. We explored the formation process of N doped single-walled nanotubes within hot wall chemical vapor deposition employing different (C/N) feedstocks and catalysts. The process was optimized regarding the formation of substitutionally doped SWCNT and double wall CNTs. Analysis of N content and bonding environment is presented.

We investigate fixed dopants in the presence of mobile point defects like foreign atoms or vacancies. A mobile defect entering the first Bohr radius RB of a dopant will modulate the generation-recombination process. The times a defect walks inside or outside RB are shown to be power-law distributed giving rise to 1 / fb noise. The predicted Hooge coefficient αdef depends on RB, on the normalized fluctuations of charge carriers and on the number of charge carriers compared to lattice sites; our model suggests that the magnitude of 1/ f noise can be decreased at will by increasing the ionization of dopants.

We employ Hartree–Fock, second-order Moller-Plesset perturbation, coupled cluster singles and doubles (CCSD) as well as CCSD plus perturbative triples (CCSD(T)) theory to study the pressure induced transition from the rocksalt to the cesium chloride crystal structure in LiH. We show that the calculated transition pressure converges rapidly in this series of increasingly accurate many-electron wave function based theories. Using CCSD(T) theory, we predict a transition pressure for the structural phase transition in the LiH crystal of 340 GPa. Furthermore, we investigate the potential energy surface for this transition in the parameter space of the Buerger path.

The synthesis of high quality isotope engineered SWCNT by means of laser ablation and the use of Pt-Rh-Re catalyst mixtures has been established. Optical absorption and Raman spectroscopy as well as transmission electron microscopy are utilized to characterize the obtained SWCNTs with regard to purity and yield. The absence of any ferromagnetic materials, as well as the remarkably low abundance of amorphous carbon renders this material ideal for magnetic studies. The controlled augmentation of 13 C is conveniently confirmed by phonon softening and broadening observed in Raman spectroscopy. Isotope labelling at constant sample quality was achieved in the whole range from 1% 13 C up to 98% 13 C.

Nanotube growth by chemical vapour deposition carbon is carried out for two different catalyst preparation methods: a wet chemistry catalyst is compared to a thin metal film multilayer catalyst. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) micrographs are recorded to investigate the nanotube alignment and the number of walls. Resonance Raman spectroscopy is used for analysis of diameters and the defect concentration.

We discuss here how the trigonal warping effect of the electronic structure is relevant to optical processes in graphite and carbon nanotubes. The electron-photon, electron-phonon, and elastic scattering matrix elements have a common factor of the coefficients of Bloch wave funtions of the A and B atoms in the graphite unit cell. Because of the three fold symmetry around the Fermi energy point (the K or K′ point), the matrix elements show a trigonal anisotropy which can be observed in both resonance Raman and photoluminescence spectroscopy. This anisotropy is essential for understanding the chirality dependence of the Raman intensity and the optical response of single wall carbon nanotubes.

The electron–phonon (e–ph) interaction and the relaxation time of photo-excited electrons are calculated in graphite within the tight-binding scheme. The e–ph matrix element thus obtained, shows anisotropy in k-space. The calculated relaxation time is of the same order of magnitude as the experimental one. Moreover, below an energy close to the Fermi energy, the absorption rate exceeds the emission rate, which indicates that graphite can emit far infra-red electro-magnetic waves by absorbing heat. We also compare this result with Planck's formula for black-body radiation.