arXiv subjects

Alfred J. H. Jones

Publications and source records attributed to Alfred J. H. Jones.

23 records · Page 2Linked to original sources

arXiv2020

Observation of Electrically Tunable van Hove Singularities in Twisted Bilayer Graphene from nanoARPES

The possibility of triggering correlated phenomena by placing a singularity of the density of states near the Fermi energy remains an intriguing avenue towards engineering the properties of quantum materials. Twisted bilayer graphene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. While the twist angle-dependence of these properties has been explored, direct demonstration of electrostatic control of the superlattice bands over a wide energy range has, so far, been critically missing. This work examines a functional twisted bilayer graphene device using in-operando angle-resolved photoemission with a nano-focused light spot. A twist angle of 12.2$^{\circ}$ is selected such that the superlattice Brillouin zone is sufficiently large to enable identification of van Hove singularities and flat band segments in momentum space. The doping dependence of these features is extracted over an energy range of 0.4 eV, expanding the combinations of twist angle and doping where they can be placed at the Fermi energy and thereby induce new correlated electronic phases in twisted bilayer graphene.

cond-mat.mtrl-sci↗

arXiv2020

Momentum-resolved view of highly tunable many-body effects in a graphene/hBN field-effect device

Integrating the carrier tunability of a functional two-dimensional material electronic device with a direct probe of energy- and momentum-resolved electronic excitations is essential to gain insights on how many-body interactions are influenced during device operation. Here, we use micro-focused angle-resolved photoemission in order to analyze many-body interactions in back-gated graphene supported on hexagonal boron nitride. By extracting the doping-dependent quasiparticle dispersion and self-energy, we observe how these interactions renormalize the Dirac cone and impact the electron mobility of our device. Our results are not only limited to a finite energy range around the Fermi level, as in electron transport measurements, but describe interactions on a much wider energy scale, extending beyond the regime of hot carrier excitations.

cond-mat.mes-hall↗

arXiv2020

Accessing the spectral function in a current-carrying device

The presence of an electrical transport current in a material is one of the simplest and most important realisations of non-equilibrium physics. The current density breaks the crystalline symmetry and can give rise to dramatic phenomena, such as sliding charge density waves [1], insulator-to-metal transitions [2,3] or gap openings in topologically protected states [4]. Almost nothing is known about how a current influences the electron spectral function, which characterizes most of the solid's electronic, optical and chemical properties. Here we show that angle-resolved photoemission spectroscopy with a nano-scale light spot (nanoARPES) provides not only a wealth of information on local equilibrium properties, but also opens the possibility to access the local non-equilibrium spectral function in the presence of a transport current. Unifying spectroscopic and transport measurements in this way allows non-invasive local measurements of the composition, structure, many-body effects and carrier mobility in the presence of high current densities.

cond-mat.str-el↗

arXiv2019

Transient Hot Electron Dynamics in Single-Layer TaS$_2$

Using time- and angle-resolved photoemission spectroscopy, we study the response of metallic single layer TaS$_2$ in the 1H structural modification to the generation of excited carriers by a femtosecond laser pulse. A complex interplay of band structure modifications and electronic temperature increase is observed and analyzed by direct fits of model spectral functions to the two-dimensional (energy and $k$-dependent) photoemission data. Upon excitation, the partially occupied valence band is found to shift to higher binding energies by up to 150 meV, accompanied by electronic temperatures exceeding 3000~K. These observations are explained by a combination of temperature-induced shifts of the chemical potential, as well as temperature-induced changes in static screening. Both contributions are evaluated in a semi-empirical tight-binding model. The shift resulting from a change in the chemical potential is found to be dominant.

cond-mat.str-el↗

arXiv2018

Mapping the Complete Reaction Path of a Complex Photochemical Reaction

We probe the dynamics of dissociating CS$_2$ molecules across the entire reaction pathway upon excitation. Photoelectron spectroscopy measurements using laboratory-generated femtosecond extreme ultraviolet pulses monitor the competing dissociation, internal conversion, and intersystem crossing dynamics. Dissociation occurs either in the initially excited singlet manifold or, via intersystem crossing, in the triplet manifold. Both product channels are monitored and show that, despite being more rapid, the singlet dissociation is the minor product and that triplet state products dominate the final yield. We explain this by a consideration of accurate potential energy curves for both the singlet and triplet states. We propose that rapid internal conversion stabilizes the singlet population dynamically, allowing for singlet-triplet relaxation via intersystem crossing and the efficient formation of spin-forbidden dissociation products on longer timescales. The study demonstrates the importance of measuring the full reaction pathway for defining accurate reaction mechanisms.

physics.chem-ph↗