Far-from-Equilibrium Electron-Phonon Interactions in Optically Excited Graphene.

Comprehending far-from-equilibrium many-body interactions is one of the major goals of current ultrafast condensed matter physics research. Here, a particularly interesting but barely understood situation occurs during a strong optical excitation, where the electron and phonon systems can be significantly perturbed and the quasiparticle distributions cannot be described with equilibrium functions. In this work, we use time- and angle-resolved photoelectron spectroscopy to study such far-from-equilibrium many-body interactions for the prototypical material graphene. In accordance with theoretical simulations, we find remarkable transient renormalizations of the quasiparticle self-energy caused by the photoinduced nonequilibrium conditions. These observations can be understood by ultrafast scatterings between nonequilibrium electrons and strongly coupled optical phonons, which signify the crucial role of ultrafast nonequilibrium dynamics on many-body interactions. Our results advance the understanding of many-body physics in extreme conditions, which is important for any endeavor to optically manipulate or create non-equilibrium states of matter.

Graphene Quantum Hall Effect Devices for AC and DC Electrical Metrology.

A new type of graphene-based quantum Hall standards is tested for electrical quantum metrology applications at alternating current (ac) and direct current (dc). The devices are functionalized with Cr(CO)3 to control the charge carrier density and have branched Hall contacts based on NbTiN superconducting material. The work is an in-depth study about the characteristic capacitances and related losses in the ac regime of the devices and about their performance during precision resistance measurements at dc and ac.

Trapping and Counting Ballistic Nonequilibrium Electrons.

We demonstrate the trapping of electrons propagating ballistically at far-above-equilibrium energies in GaAs/AlGaAs heterostructures in high magnetic field. We find low-loss transport along a gate-modified mesa edge in contrast to an effective decay of excess energy for the loop around a neighboring, mesa-confined node, enabling high-fidelity trapping. Measuring the full counting statistics via single-charge detection yields the trapping (and escape) probabilities of electrons scattered (and excited) within the node. Energetic and arrival-time distributions of captured electron wave packets are characterized by modulating tunnel barrier transmission.

Compressed sensing FTIR nano-spectroscopy and nano-imaging.

Infrared scattering scanning near-field optical microscopy (IR s-SNOM) provides for spectroscopic imaging with nanometer spatial resolution, yet full spatio-spectral imaging is constrained by long measurement times. Here, we demonstrate the application of compressed sensing algorithms to achieve hyperspectral FTIR-based nano-imaging at an order of magnitude faster imaging speed to achieve the same spectral content compared to conventional approaches. At the example of the spectroscopy of a single vibrational resonance, we discuss the relationship of prior knowledge of sparseness of the employed Fourier base functions and sub-sampling. Compressed sensing nano-FTIR spectroscopy promises both rapid and sensitive chemical nano-imaging which is highly relevant in academic and industrial settings for fundamental and applied nano- and bio-materials research.

Detection of the Anomalous Velocity with Subpicosecond Time Resolution in Semiconductor Nanostructures.

We report on the time-resolved detection of the anomalous velocity, constituting charge carriers moving perpendicular to an electric driving field, in undoped GaAs quantum wells. For this we optically excite the quantum wells with circularly polarized femtosecond laser pulses, thereby creating a state which breaks time-inversion symmetry. We then employ a quasi-single-cycle terahertz pulse as an electric driving field to induce the anomalous velocity. The electromagnetic radiation emitted from the anomalous velocity is studied with a subpicosecond time resolution and reveals intriguing results. We are able to distinguish between intrinsic (linked to the Berry curvature) and extrinsic (linked to scattering) contributions to the anomalous velocity both originating from the valence band and observe local energy space dependence of the anomalous velocity. Our results thus constitute a significant step towards noninvasive probing of the anomalous velocity locally in the full energy-momentum space and enable the investigation of many popular physical effects such as the anomalous Hall effect and spin Hall effect on ultrafast time scales.

Optical spin noise of a single hole spin localized in an (InGa)As quantum dot.

We advance spin noise spectroscopy to the ultimate limit of single spin detection. This technique enables the measurement of the spin dynamic of a single heavy hole localized in a flat (InGa)As quantum dot. Magnetic field and light intensity dependent studies reveal even at low magnetic fields a strong magnetic field dependence of the longitudinal heavy hole spin relaxation time with an extremely long T1 of ≥180 µs at 31 mT and 5 K. The wavelength dependence of the spin noise power discloses for finite light intensities an inhomogeneous single quantum dot spin noise spectrum which is explained by charge fluctuations in the direct neighborhood of the quantum dot. The charge fluctuations are corroborated by the distinct intensity dependence of the effective spin relaxation rate.

Self-referenced single-electron quantized current source.

The future redefinition of the international system of units in terms of natural constants requires a robust, high-precision quantum standard for the electrical base unit ampere. However, the reliability of any single-electron current source generating a nominally quantized output current I=ef by delivering single electrons with charge e at a frequency f is eventually limited by the stochastic nature of the underlying quantum mechanical tunneling process. We experimentally explore a path to overcome this fundamental limitation by serially connecting clocked single-electron emitters with multiple in situ single-electron detectors. Correlation analysis of the detector signatures during current generation reveals erroneous pumping events and enables us to determine the deviation of the output current from the nominal quantized value ef. This demonstrates the concept of a self-referenced single-electron source for electrical quantum metrology.

Harmonic oscillator wave functions of a self-assembled InAs quantum dot measured by scanning tunneling microscopy.

InAs quantum dots embedded in an AlAs matrix inside a double barrier resonant tunneling diode are investigated by cross-sectional scanning tunneling spectroscopy. The wave functions of the bound quantum dot states are spatially and energetically resolved. These bound states are known to be responsible for resonant tunneling phenomena in such quantum dot diodes. The wave functions reveal a textbook-like one-dimensional harmonic oscillator behavior showing up to five equidistant energy levels of 80 meV spacing. The derived effective oscillator mass of m* = 0.24m0 is 1 order of magnitude higher than the effective electron mass of bulk InAs that we attribute to the influence of the surrounding AlAs matrix. This underlines the importance of the matrix material for tailored QD devices with well-defined properties.

Counting statistics for electron capture in a dynamic quantum dot.

We report noninvasive single-charge detection of the full probability distribution P(n) of the initialization of a quantum dot with n electrons for rapid decoupling from an electron reservoir. We analyze the data in the context of a model for sequential tunneling pinch-off, which has generic solutions corresponding to two opposing mechanisms. One limit considers sequential "freeze-out" of an adiabatically evolving grand canonical distribution, the other one is an athermal limit equivalent to the solution of a generalized decay cascade model. We identify the athermal capturing mechanism in our sample, testifying to the high precision of our combined theoretical and experimental methods. The distinction between the capturing mechanisms allows us to derive efficient experimental strategies for improving the initialization.

Two electrons interacting at a mesoscopic beam splitter.

The nonlinear response of a beam splitter to the coincident arrival of interacting particles enables numerous applications in quantum engineering and metrology. Yet, it poses considerable challenges to control interactions on the individual particle level. Here, we probe the coincidence correlations at a mesoscopic constriction between individual ballistic electrons in a system with unscreened Coulomb interactions and introduce concepts to quantify the associated parametric nonlinearity. The full counting statistics of joint detection allows us to explore the interaction-mediated energy exchange. We observe an increase from 50% up to 70% in coincidence counts between statistically indistinguishable on-demand sources and a correlation signature consistent with the independent tomography of the electron emission. Analytical modelling and numerical simulations underpin the consistency of the experimental results with Coulomb interactions between two electrons counterpropagating in a quadratic saddle potential. Coulomb repulsion energy and beam splitter dispersion define a figure of merit, which in this experiment is demonstrated to be sufficiently large to enable future applications, such as single-shot in-flight detection and quantum logic gates.

All-optically induced ultrafast photocurrents: beyond the instantaneous coherent response.

It is demonstrated that the noninstantaneous response of the optically induced coherent polarization tremendously influences the real-space shift of electronic charges in semiconductors. The possibility of coherently controlling this real-space shift with temporally nonoverlapping excitation pulses allows for the observation of a new type of shift current, which only exists for certain polarization-shaped excitation pulses and vanishes in the continuous-wave limit. In contrast to previously studied shift currents, the new current requires a phase mismatch between two orthogonal transition dipole moments and leads, within a nonlinear second-order description, to a tensor which is antisymmetric with respect to the order of the two exciting electric field amplitudes. These observations, which can even be made at room temperature and are expected to occur in a variety of semiconductor crystal classes, contribute to a better understanding of light-matter interaction involving degenerate bands. Thus, they are expected to prove important for future studies of coherent and nonlinear optical effects in semiconductors.

Impact of Polymer-Assisted Epitaxial Graphene Growth on Various Types of SiC Substrates.

The growth parameters for epitaxial growth of graphene on silicon carbide (SiC) have been the focus of research over the past few years. However, besides the standard growth parameters, the influence of the substrate pretreatment and properties of the underlying SiC wafer are critical parameters for optimizing the quality of monolayer graphene on SiC. In this systematic study, we show how the surface properties and the pretreatment determine the quality of monolayer graphene using polymer-assisted sublimation growth (PASG) on SiC. Using the spin-on deposition technique of PASG, several polymer concentrations have been investigated to understand the influence of the polymer content on the final monolayer coverage using wafers of different miscut angles and different polytypes. Confocal laser scanning microscopy (CLSM), atomic force microscopy (AFM), Raman spectroscopy, and scanning electron microscopy (SEM) were used to characterize these films. The results show that, even for SiC substrates with high miscut angles, high-quality graphene is obtained when an appropriate polymer concentration is applied. This is in excellent agreement with the model understanding that an insufficient carbon supply from SiC step edge decomposition can be compensated by additionally providing carbon from a polymer source. The described methods make the PASG spin-on deposition technique more convenient for commercial use.

Substrate induced nanoscale resistance variation in epitaxial graphene.

Graphene, the first true two-dimensional material, still reveals the most remarkable transport properties among the growing class of two-dimensional materials. Although many studies have investigated fundamental scattering processes, the surprisingly large variation in the experimentally determined resistances is still an open issue. Here, we quantitatively investigate local transport properties of graphene prepared by polymer assisted sublimation growth using scanning tunneling potentiometry. These samples exhibit a spatially homogeneous current density, which allows to analyze variations in the local electrochemical potential with high precision. We utilize this possibility by examining the local sheet resistance finding a significant variation of up to 270% at low temperatures. We identify a correlation of the sheet resistance with the stacking sequence of the 6H silicon carbide substrate and with the distance between the graphene and the substrate. Our results experimentally quantify the impact of the graphene-substrate interaction on the local transport properties of graphene.

Correction to Infrared Nanospectroscopy of Phospholipid and Surfactin Monolayer Domains.

[This corrects the article DOI: 10.1021/acsomega.7b01931.].

Infrared Nanospectroscopy of Phospholipid and Surfactin Monolayer Domains.

A main challenge in understanding the structure of a cell membrane and its interactions with drugs is the ability to chemically study the different molecular species on the nanoscale. We have achieved this for a model system consisting of mixed monolayers (MLs) of the biologically relevant phospholipid 1,2-distearoyl-sn-glycero-phosphatidylcholine and the antibiotic surfactin. By employing nano-infrared (IR) microscopy and spectroscopy in combination with atomic force microscopy imaging, it was possible to identify and chemically detect domain formation of the two constituents as well as to obtain IR spectra of these species with a spatial resolution on the nanoscale. A novel method to enhance the near-field imaging contrast of organic MLs by plasmon interferometry is proposed and demonstrated. In this technique, the organic layer is deposited on gold and ML graphene substrates, the latter of which supports propagating surface plasmons. Plasmon reflections arising from changes in the dielectric environment provided by the organic layer lead to an additional contrast mechanism. Using this approach, the interfacial region between surfactin and the phospholipid has been mapped and a transition region is identified.

Partitioning of on-demand electron pairs.

The on-demand generation and separation of entangled photon pairs are key components of quantum information processing in quantum optics. In an electronic analogue, the decomposition of electron pairs represents an essential building block for using the quantum state of ballistic electrons in electron quantum optics. The scattering of electrons has been used to probe the particle statistics of stochastic sources in Hanbury Brown and Twiss experiments and the recent advent of on-demand sources further offers the possibility to achieve indistinguishability between multiple sources in Hong-Ou-Mandel experiments. Cooper pairs impinging stochastically at a mesoscopic beamsplitter have been successfully partitioned, as verified by measuring the coincidence of arrival. Here, we demonstrate the splitting of electron pairs generated on demand. Coincidence correlation measurements allow the reconstruction of the full counting statistics, revealing regimes of statistically independent, distinguishable or correlated partitioning, and have been envisioned as a source of information on the quantum state of the electron pair. The high pair-splitting fidelity opens a path to future on-demand generation of spin-entangled electron pairs from a suitably prepared two-electron quantum-dot ground state.

Epitaxial graphene on SiC: modification of structural and electron transport properties by substrate pretreatment.

The electrical transport properties of epitaxial graphene layers are correlated with the SiC surface morphology. In this study we show by atomic force microscopy and Raman measurements that the surface morphology and the structure of the epitaxial graphene layers change significantly when different pretreatment procedures are applied to nearly on-axis 6H-SiC(0 0 0 1) substrates. It turns out that the often used hydrogen etching of the substrate is responsible for undesirable high macro-steps evolving during graphene growth. A more advantageous type of sub-nanometer stepped graphene layers is obtained with a new method: a high-temperature conditioning of the SiC surface in argon atmosphere. The results can be explained by the observed graphene buffer layer domains after the conditioning process which suppress giant step bunching and graphene step flow growth. The superior electronic quality is demonstrated by a less extrinsic resistance anisotropy obtained in nano-probe transport experiments and by the excellent quantization of the Hall resistance in low-temperature magneto-transport measurements. The quantum Hall resistance agrees with the nominal value (half of the von Klitzing constant) within a standard deviation of 4.5 × 10(-9) which qualifies this method for the fabrication of electrical quantum standards.