Alexander Stöhr

Snapshots of non-equilibrium Dirac carrier distributions in graphene

The optical properties of graphene are made unique by the linear band structure and the vanishing density of states at the Dirac point. It has been proposed that even in the absence of a bandgap, a relaxation bottleneck at the Dirac point may allow for population inversion and lasing at arbitrarily long wavelengths. Furthermore, efficient carrier multiplication by impact ionization has been discussed in the context of light harvesting applications. However, all of these effects are difficult to test quantitatively by measuring the transient optical properties alone, as these only indirectly reflect the energy- and momentum-dependent carrier distributions. Here, we use time- and angle-resolved photoemission spectroscopy with femtosecond extreme-ultraviolet pulses to directly probe the non-equilibrium response of Dirac electrons near the K-point of the Brillouin zone. In lightly hole-doped epitaxial graphene samples, we explore excitation in the mid- and near-infrared, both below and above the minimum photon energy for direct interband transitions. Whereas excitation in the mid-infrared results only in heating of the equilibrium carrier distribution, interband excitations give rise to population inversion, suggesting that terahertz lasing may be possible. However, in neither excitation regime do we find any indication of carrier multiplication, questioning the applicability of graphene for light harvesting.

Evidence for superconductivity in Li-decorated monolayer graphene

Significance Although superconductivity is well-known in intercalated bulk graphite, the ultimate goal of inducing superconductivity in single-layer graphene has not yet been achieved. We have here developed an experiment that combines ultralow-temperature (5 K) and ultrahigh-vacuum (10−11 torr) sample preparation with high-resolution angle-resolved photoemission spectroscopy (ARPES). We show that decorating monolayer graphene with a layer of lithium atoms enhances the electron–phonon coupling to the point where a superconducting state can be stabilized at low temperature. Measurements of the size of the superconducting gap by ARPES suggest a Tc of about 5.9 K. This result constitutes the first observation, to our knowledge, of superconductivity in monolayer graphene. Given the massive scientific and technological interest in graphene, our findings will have significant cross-disciplinary impact. Monolayer graphene exhibits many spectacular electronic properties, with superconductivity being arguably the most notable exception. It was theoretically proposed that superconductivity might be induced by enhancing the electron–phonon coupling through the decoration of graphene with an alkali adatom superlattice [Profeta G, Calandra M, Mauri F (2012) Nat Phys 8(2):131–134]. Although experiments have shown an adatom-induced enhancement of the electron–phonon coupling, superconductivity has never been observed. Using angle-resolved photoemission spectroscopy (ARPES), we show that lithium deposited on graphene at low temperature strongly modifies the phonon density of states, leading to an enhancement of the electron–phonon coupling of up to λ≃0.58. On part of the graphene-derived π∗-band Fermi surface, we then observe the opening of a Δ≃0.9-meV temperature-dependent pairing gap. This result suggests for the first time, to our knowledge, that Li-decorated monolayer graphene is indeed superconducting, with Tc≃5.9 K.

Structural and Electronic Properties of Nitrogen-Doped Graphene

We investigate the structural and electronic properties of nitrogen-doped epitaxial monolayer graphene and quasifreestanding monolayer graphene on 6H-SiC(0001) by the normal incidence x-ray standing wave technique and by angle-resolved photoelectron spectroscopy supported by density functional theory simulations. With the location of various nitrogen species uniquely identified, we observe that for the same doping procedure, the graphene support, consisting of substrate and interface, strongly influences the structural as well as the electronic properties of the resulting doped graphene layer. Compared to epitaxial graphene, quasifreestanding graphene is found to contain fewer nitrogen dopants. However, this lack of dopants is compensated by the proximity of nitrogen atoms at the interface that yield a similar number of charge carriers in graphene.

Population inversion in monolayer and bilayer graphene

The recent demonstration of saturable absorption and negative optical conductivity in the Terahertz range in graphene has opened up new opportunities for optoelectronic applications based on this and other low dimensional materials. Recently, population inversion across the Dirac point has been observed directly by time- and angle-resolved photoemission spectroscopy (tr-ARPES), revealing a relaxation time of only ∼130 femtoseconds. This severely limits the applicability of single layer graphene to, for example, Terahertz light amplification. Here we use tr-ARPES to demonstrate long-lived population inversion in bilayer graphene. The effect is attributed to the small band gap found in this compound. We propose a microscopic model for these observations and speculate that an enhancement of both the pump photon energy and the pump fluence may further increase this lifetime.

Bipolar gating of epitaxial graphene by intercalation of Ge

In this study, the ambivalent behavior of Ge intercalation is studied by means of scanning tunneling microscopy and spectroscopy as well as local 4-point probe transport measurements. In quantitative agreement with angle-resolved photoemission experiments, both p- and n-type doped graphene areas and their doping level were identified by local spectroscopy. The p-doped areas appear higher by 2 A with respect to the n-doped areas suggesting incorporation of thicker Ge-layers accompanied by a modified coupling to the initial SiC-surface. Furthermore, the sheet resistance was measured on each of the patches separately. The intrinsic imbalance between the carrier types in the different areas is well reflected by the transport study. The process of intercalation does not affect the transport properties in comparison to pristine graphene pointing to a sufficient homogeneity of the decoupled graphene layer. Transport measurements across chemically gated pn-junctions reveal increased resistances, possibly due to e...

Ballistic bipolar junctions in chemically gated graphene ribbons.

The realization of ballistic graphene pn-junctions is an essential task in order to study Klein tunneling phenomena. Here we show that intercalation of Ge under the buffer layer of pre-structured SiC-samples succeeds to make truly nano-scaled pn-junctions. By means of local tunneling spectroscopy the junction width is found to be as narrow as 5 nm which is a hundred times smaller compared to electrically gated structures. The ballistic transmission across the junction is directly proven by systematic transport measurements with a 4-tip STM. Various npn- and pnp-junctions are studied with respect to the barrier length. The pn-junctions are shown to act as polarizer and analyzer with the second junction becoming transparent in case of a fully ballistic barrier. This can be attributed to the almost full suppression of electron transmission through the junction away from normal incidence.

Intercalation of graphene on SiC(0001) via ion implantation

Electronic devices based on graphene technology are catching on rapidly and the ability to engineer graphene properties at the nanoscale is becoming, more than ever, indispensable. Here, we present a procedure of graphene functionalization on SiC(0001) that paves the way towards the fabrication of complex graphene electronic chips. The procedure resides on the well-known ion-implantation technique. The efficiency of the working principle is demonstrated by the intercalation of the epitaxial graphene layer on SiC(0001) with Bi atoms, which was not possible following standard procedures. The investigation of the obtained graphene system reveals no clear spin-orbit coupling enhancement expected by theory in addition to the presence of residual structural defects. Our graphene/SiC(0001) intercalation procedure puts forward the ion-beam lithography to nanostructure and functionalize desired graphene chips.