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We use density functional theory calculations to characterize the early stages of fluorination of silver's (100) and (110) surfaces. In the Ag(100) surface, the hollow site is the most favorable for F adatoms. In the Ag(110) surface, three adsorption sites, namely hollow, long bridge, and short bridge, exhibit similar energies. These locations are also more favorable than an F adatom occupying a vacancy site irrespectively of whether the vacancy was present or not in the pristine surface. The computed energy as a function of surface coverage is used to compute the equilibrium thermodynamics phase diagram. We argue that for the typical pressure and temperature of fluorination experiments, the state of the surface is not determined by thermodynamics but by kinetics. Combining these results with scanning tunneling microscopy (STM) topographic simulations, we propose assignments to features observed experimentally. We present a minimal model of the apparent topography of adatoms in different locations in terms of hydrogenic orbitals, explaining the observed trends. The model links the STM apparent topography to structural information and the oxidation states of the Ag atoms near the adatom., Comment: 18 pages, 12 Figures

We use low-temperature scanning tunneling microscopy (LT-STM) to characterize the early stages of silver fluorination. On Ag(100), we observe only one adsorbate species, which shows a bias-dependent STM topography. Notably, at negative bias voltages, $V_{\rm B}<0$, the apparent shape can be described as a round protrusion surrounded by a moat-like depression (sombrero). As the voltage increases, the apparent shape changes, eventually evolving into a round depression. From the STM images, we determine the adsorption site to be the hollow position. On Ag(110) we find adsorbates with three distinct STM topographies. One type exhibits the same shape change with $V_{\rm B}$ as observed on Ag(100), that is, from a sombrero shape to a round depression as the voltage changes from negative to positive values; the other two types are observed as round depressions regardless of $V_{\rm B}$. From the STM images, we find the three adsorbates to be sitting on the short-bridge, hollow and top position on the Ag(110) surface, with a relative abundance of 60\%, 35\% and 5\%., Comment: 13 pages, 7 figures

Graphene quality indicators obtained by Raman spectroscopy have been correlated to the structural changes of the graphene/Germanium interface as a function of in-vacuum thermal annealing. Specifically, it is found that graphene becomes markedly defected at 650 {\deg}C. By combining scanning tunneling microscopy, x-Ray Photoelectron Spectroscopy and Near Edge x-ray Absorption Fine Structure Spectroscopy, we conclude that these defects are due to the release of H_{2} gas trapped at the graphene/Germanium interface. The H_{2} gas was produced following the transition from the as-grown hydrogen-termination of the Ge(110) surface to the emergence of surface reconstructions in the substrate. Interestingly, a complete self-healing process is observed in graphene upon annealing to 800 {\deg}C. The subtle interplay revealed between the microscopic changes occurring at the graphene/Germanium interface and graphene's defect density is valuable for advancing graphene growth, controlled 2D-3D heterogeneous materials interfacing and integrated fabrication technology on semiconductors.

We report a homogeneous quantum cascade laser (QCL) emitting at Terahertz (THz) frequencies, with a total spectral emission of about 0.6 THz centered around 3.3 THz, a current density dynamic range of Jdr=1.53, and a continuous wave output power of 7 mW. The analysis of the intermode beatnote unveils that the devised laser operates as optical frequency comb (FC) synthesizer over the whole laser operational regime, with up to 36 optically active laser modes delivering ~ 200 uW of optical power per comb tooth, a power level unreached so far in any THz QCL FC. A stable and narrow single beatnote, reaching a minimum linewidth of 500 Hz, is observed over a current density range of 240 A/cm2, and even across the negative differential resistance region. We further prove that the QCL frequency comb can be injection locked with moderate RF power at the intermode beatnote frequency, covering a locking range of 1.2 MHz. The demonstration of stable FC operation, in a QCL, over the full current density dynamic range, and without any external dispersion compensation mechanism, makes our proposed homogenous THz QCL an ideal tool for metrological application requiring mode-hop electrical tunability and a tight control of the frequency and phase jitter., Comment: 11 Pages, 5 Figures. This is the authors' version of the submitted article, published in its final form at https://doi.org/10.1515/nanoph-2020-0378

We report electroluminescence originating from L-valley transitions in n-type Ge/Si$_{0.15}$Ge$_{0.85}$ quantum cascade structures centered at 3.4 and 4.9 THz with a line broadening of $\Delta f/f \approx 0.2$. Three strain-compensated heterostructures, grown on a Si substrate by ultrahigh vacuum chemical vapor deposition, have been investigated. The design is based on a single quantum well active region employing a vertical optical transition and the observed spectral features are well described by non-equilibrium Green's function calculations. The presence of two peaks highlights a suboptimal injection in the upper state of the radiative transition. Comparison of the electroluminescence spectra with similar GaAs/AlGaAs structure yields one order of magnitude lower emission efficiency.

We present an electrically switchable graphene terahertz (THz) modulator with a tunable-by-design optical bandwidth and we exploit it to compensate the cavity dispersion of a quantum cascade laser (QCL). Electrostatic gating is achieved by a metal-grating used as a gate electrode, with an HfO2/AlOx gate dielectric on top. This is patterned on a polyimide layer, which acts as a quarter wave resonance cavity, coupled with an Au reflector underneath. We get 90% modulation depth of the intensity, combined with a 20 kHz electrical bandwidth in the 1.9 _ 2.7 THz range. We then integrate our modulator with a multimode THz QCL. By adjusting the modulator operational bandwidth, we demonstrate that the graphene modulator can partially compensates the QCL cavity dispersion, resulting in an integrated laser behaving as a stable frequency comb over 35% of the laser operational range, with 98 equidistant optical modes and with a spectral coverage of ~ 1.2 THz. This has significant potential for frontier applications in the terahertz, as tunable transformation-optics devices, active photonic components, adaptive and quantum optics, and as a metrological tool for spectroscopy at THz frequencies., Comment: 22 pages, 6 figures

Combining scanning tunneling microscopy and angle-resolved photoemission spectroscopy, we demonstrate how to tune the doping of epitaxial graphene from p to n by exploiting the structural changes that occur spontaneously on the Ge surface upon thermal annealing. Furthermore, using first principle calculations we build a model that successfully reproduces the experimental observations. Since the ability to modify graphene electronic properties is of fundamental importance when it comes to applications, our results provide an important contribution towards the integration of graphene with conventional semiconductors.

: n-type Ge/SiGe asymmetric-coupled quantum wells represent the building block of a variety of nanoscale quantum devices, including recently proposed designs for a silicon-based THz quantum cascade laser. In this paper, we combine structural and spectroscopic experiments on 20-module superstructures, each featuring two Ge wells coupled through a Ge-rich tunnel barrier, as a function of the geometry parameters of the design and the P dopant concentration. Through the comparison of THz spectroscopic data with numerical calculations of intersubband optical absorption resonances, we demonstrated that it is possible to tune by design the energy and the spatial overlap of quantum confined subbands in the conduction band of the heterostructures. The high structural/interface quality of the samples and the control achieved on subband hybridization are the promising starting point towards a working electrically pumped light-emitting device.

We develop a generalized theory for the scattering process produced by interface roughness on charge carriers and which is suitable for any semiconductor heterostructure. By exploiting our experimental insights into the three-dimensional atomic landscape obtained on Ge/GeSi heterointerfaces obtained by atom probe tomography, we have been able to define the full set of interface parameters relevant to the scattering potential, including both the in-plane and axial correlation inside real diffuse interfaces. Our experimental findings indicate a partial coherence of the interface roughness along the growth direction within the interfaces. We show that it is necessary to include this feature, previously neglected by theoretical models, when heterointerfaces characterized by finite interface widths are taken into consideration.

Light can be strongly confined in sub-wavelength spatial regions through the interaction with plasmons, the collective electronic modes appearing in metals and semiconductors. This confinement, which is particularly important in the terahertz spectral region, amplifies light-matter interaction and provides a powerful mechanism for efficiently generating non-linear optical phenomena. These effects are particularly relevant in Dirac materials like graphene and Topological Insulators, where massless fermions show a naturally non-linear optical behavior in the terahertz range. The strong interaction scenario has been considered so far from the point of view of light. In this paper, we investigate instead the effect of strong interaction on the plasmon itself. In particular, we will show that Dirac plasmons in Bi$_2$Se$_3$ Topological Insulator are strongly renormalized when excited by high-intensity terahertz radiation by displaying a huge red-shift down to 60% of its characteristic frequency. This opens the road towards tunable terahertz non-linear optical devices based on Topological Insulators.

We systematically investigate the chemical vapor deposition growth of graphene on Ge(110) as a function of the deposition temperature close to the Ge melting point. By merging spectroscopic and morphological information, we find that the quality of graphene films depends critically on the growth temperature improving significantly by increasing this temperature in the 910-930 {\deg}C range. We correlate the abrupt improvement of the graphene quality to the formation of a quasi-liquid Ge surface occurring in the same temperature range, which determines increased atom diffusivity and sublimation rate. Being observed for diverse Ge orientations, this process is of general relevance for graphene synthesis on Ge.

Si/Ge heteroepitaxial dots under tensile strain are grown on nanostructured Ge substrates produced by high-temperature flash heating exploiting the spontaneous faceting of the Ge(001) surface close to the onset of surface melting. A very diverse growth mode is obtained depending on the specific atomic structure and step density of nearby surface domains with different vicinal crystallographic orientations. On highly-miscut areas of the Ge(001) substrate, the critical thickness for islanding is lowered to about 5 ML, in contrast to the 11 ML reported for the flat Ge(001) surface, while on unreconstructed (1x1) domains the growth is Volmer-Weber driven. An explanation is proposed considering the diverse relative contributions of step and surface energies on misoriented substrates. In addition, we show that the bottom-up pattern of the substrate naturally formed by thermal annealing determines a spatial correlation for the dot sites.

By combining scanning probe microscopy with Raman and x-ray photoelectron spectroscopies, we investigate the evolution of CVD-grown graphene/Ge(001) as a function of the deposition temperature in close proximity to the Ge melting point, highlighting an abrupt change of the graphene's quality, morphology, electronic properties and growth mode at 930 degrees. We attribute this discontinuity to the incomplete surface melting of the Ge substrate and show how incomplete melting explains a variety of diverse and long-debated peculiar features of the graphene/Ge(001), including the characteristic nanostructuring of the Ge substrate induced by graphene overgrowth. We find that the quasi-liquid Ge layer formed close to 930 degrees is fundamental to obtain high-quality graphene, while a temperature decrease of 10 degrees already results in a wrinkled and defective graphene film., Comment: in press

n-type Ge/SiGe terahertz quantum cascade laser are investigated using non-equilibrium Green's functions calculations. We compare the temperature dependence of the terahertz gain properties with an equivalent GaAs/AlGaAs QCL design. In the Ge/SiGe case, the gain is found to be much more robust to temperature increase, enabling operation up to room temperature. The better temperature robustness with respect to III-V is attributed to the much weaker interaction with optical phonons. The effect of lower interface quality is investigated and can be partly overcome by engineering smoother quantum confinement via multiple barrier heights., Comment: 5 pages, 5 figures

In this paper we investigate the structural and optical properties of few strain-unbalanced multiple Ge/GeSi quantum wells pseudomorphically grown on GeSi reverse-graded substrates. The obtained high epitaxial quality demonstrates that strain symmetrization is not a mandatory requirement for few quantum-well repetitions. Photoluminescence data, supported by a thorough theoretical modeling, allow us to unambiguously disentangle the spectral features of the quantum wells from those originating in the virtual substrate and to evaluate the impact on the optical properties of key parameters, such as quantum confinement, layer compositions, excess carrier density, and lattice strain. This detailed understanding of the radiative recombination processes is of paramount importance for the development of Ge/GeSi-based optical devices.

An extended formation of faceted pit-like defects on Ge(001) and Ge(111) wafers was obtained by thermal cycles to T> 750 {\deg}C. This temperature range is relevant in many surface-preparation recipes of the Ge surface. The density of the defects depends on the temperature reached, the number of annealing cycles performed and correlates to the surface-energy stability of the specific crystal orientation. We propose that the pits were formed by preferential desorption from the strained regions around dislocation pile-ups. Indeed, the morphology of the pits was the same as that observed for preferential chemical etching of dislocations while the spatial distribution of the pits was clearly non-Poissonian in line with mutual interactions between the core dislocations., Comment: European Union (EU), Horizon 2020, Far-Infrared Lasers Assembled using Silicon Heterostructures,FLASH,Grant number: 766719

In this work we shed light on the early stage of the chemical vapor deposition of graphene on Ge(001) surfaces. By a combined use of microRaman and x-ray photoelectron spectroscopies, and scanning tunneling microscopy and spectroscopy, we were able to individuate a carbon precursor phase to graphene nucleation which coexists with small graphene domains. This precursor phase is made of C aggregates with different size, shape and local ordering which are not fully sp2 hybridized. In some atomic size regions these aggregates show a linear arrangement of atoms as well as the first signature of the hexagonal structure of graphene. The carbon precursor phase evolves in graphene domains through an ordering process, associated to a re-arrangement of the Ge surface morphology. This surface structuring represents the embryo stage of the hills-and-valleys faceting featured by the Ge(001) surface for longer deposition times, when the graphene domains coalesce to form a single layer graphene film.

Germanium is emerging as the substrate of choice for the growth of graphene in CMOS-compatible processes. For future application in next generation devices the accurate control over the properties of high-quality graphene synthesized on Ge surfaces, such as number of layers and domain size, is of paramount importance. Here we investigate the role of the process gas flows on the CVD growth of graphene on Ge(100). The quality and morphology of the deposited material is assessed by using microRaman spectroscopy, x-ray photoemission spectroscopy, scanning electron and atomic force microscopies. We find that by simply varying the carbon precursor flow different growth regimes - yielding to graphene nanoribbons, graphene monolayer and graphene multilayer - are established. We identify the growth conditions yielding to a layer-by-layer growth regime and report on the achievement of homogeneous monolayer graphene with an average intensity ratio of 2D and G bands in the Raman map larger than 3.

The great potential of Dirac electrons for plasmonics and photonics has been readily recognized after their discovery in graphene, followed by applications to smart optical devices. Dirac carriers are also found in topological insulators (TI) --quantum systems having an insulating gap in the bulk and intrinsic Dirac metallic states at the surface--. Here, we investigate the plasmonic response of ring structures patterned in Bi$_2$Se$_3$ TI films, which we investigate through terahertz (THz) spectroscopy. The rings are observed to exhibit a bonding and an antibonding plasmon modes, which we tune in frequency by varying their diameter. We develop an analytical theory based on the THz conductivity of unpatterned films, which accurately describes the strong plasmon-phonon hybridization and Fano interference experimentally observed as the bonding plasmon is swiped across the promineng 2\,THz phonon exhibited by this material. This work opens the road for the investigation of plasmons in topological insulators and for their application in tunable THz devices., Comment: 9 pages, 2 figures. To be published in Advanced Optical Materials

Plasmons are the quantized collective oscillations of electrons in metals and doped semiconductors. The plasmons of ordinary, massive electrons are since a long time basic ingredients of research in plasmonics and in optical metamaterials. Plasmons of massless Dirac electrons were instead recently observed in a purely two-dimensional electron system (2DEG)like graphene, and their properties are promising for new tunable plasmonic metamaterials in the terahertz and the mid-infrared frequency range. Dirac quasi-particles are known to exist also in the two-dimensional electron gas which forms at the surface of topological insulators due to a strong spin-orbit interaction. Therefore,one may look for their collective excitations by using infrared spectroscopy. Here we first report evidence of plasmonic excitations in a topological insulator (Bi2Se3), that was engineered in thin micro-ribbon arrays of different width W and period 2W to select suitable values of the plasmon wavevector k. Their lineshape was found to be extremely robust vs. temperature between 6 and 300 K, as one may expect for the excitations of topological carriers. Moreover, by changing W and measuring in the terahertz range the plasmonic frequency vP vs. k we could show, without using any fitting parameter, that the dispersion curve is in quantitative agreement with that predicted for Dirac plasmons., Comment: 11 pages, 3 figures, published in Nature Nanotechnology (2013)

We report on the fabrication and electronic transport characterisation of Schottky-gated strongly confined Si/SiGe quantum point contacts (QPC). At zero magnetic field and T=450mK the QPC conductance as a function of gate voltage shows a quantization in units of e^2/h, indicative of transport through 1D modes which appear to lack both spin and valley degeneracy., Comment: 2 pages, 2 figure, to be published in Proc. ICPS-28

We fabricated strongly confined Schottky-gated quantum point contacts by etching Si/SiGe heterostructures and observed intriguing conductance quantization in units of approximately 1e2/h. Non-linear conductance measurements were performed depleting the quantum point contacts at fixed mode-energy separation. We report evidences of the formation of a half 1e2/h plateau, supporting the speculation that adiabatic transmission occurs through 1D modes with complete removal of valley and spin degeneracies., Comment: to appear in Physical Review B

Low field magnetotransport revealing signatures of ballistic transport effects in strained Si/SiGe cavities is investigated. We fabricated strained Si/SiGe cavities by confining a high mobility Si/SiGe 2DEG in a bended nanowire geometry defined by electron-beam lithography and reactive ion etching. The main features observed in the low temperature magnetoresistance curves are the presence of a zero-field magnetoresistance peak and of an oscillatory structure at low fields. By adopting a simple geometrical model we explain the oscillatory structure in terms of electron magnetic focusing. A detailed examination of the zero-field peak lineshape clearly shows deviations from the predictions of ballistic weak localization theory., Comment: Submitted to Physical Review B, 25 pages, 7 figures