Computational screening study towards redox-active metal-organic frameworks

The metal-organic framework (MOF) MFU-4l containing Co(II) centers and Cl- ligands has recently shown promising redox activity. Aiming for further improved MOF catalysts for oxidation processes employing molecular oxygen we present a density-functional theory (DFT) based computational screening approach to identify promising metal center and ligand combinations within the MFU-4l structural family. Using the O2 binding energy as a descriptor for the redox property, we show that relative energetic trends in this descriptor can reliably be obtained at the hybrid functional DFT level and using small cluster (scorpionate-type complex) models. Within this efficient computational protocol we screen a range of metal center / ligand combinations and identify several candidate systems that offer more exothermic O2 binding than the original Co/Cl-based MFU-4l framework.Comment: 9 pages, 4 figure

Magneto-optical probing of weak disorder in a two-dimensional hole gas

In two-beam magneto-photoluminescence spectra of a two-dimensional valence hole gas we identify the three-level energy spectrum of a free positive trion with a field-induced singlet-triplet transition. The recombination spectrum of acceptor-bound trions is also detected, including a cyclotron replica corresponding to the hole shake-up process. The emergence of a shake-up peak at low temperature is shown to be a sensitive probe of the presence of a small number of impurities inside the high-mobility quantum well, and its relative position is directly related to the hole cyclotron mass.Comment: 4 pages, 5 figure

Magneto-capacitance probing of the many-particle states in InAs dots

We use frequency-dependent capacitance-voltage spectroscopy to measure the tunneling probability into self-assembled InAs quantum dots. Using an in-plane magnetic field of variable strength and orientation, we are able to obtain information on the quasi-particle wave functions in momentum space for 1 to 6 electrons per dot. For the lowest two energy states, we find a good agreement with Gaussian functions for a harmonic potential. The high energy orbitals exhibit signatures of anisotropic confinement and correlation effects.Comment: 3 pages, 3 figure

Noise thermometry in narrow 2D electron gas heat baths connected to a quasi-1D interferometer

Thermal voltage noise measurements are performed in order to determine the electron temperature in nanopatterned channels of a GaAs/AlGaAs heterostructure at bath temperatures of 4.2 and 1.4 K. Two narrow two-dimensional (2D) heating channels, close to the transition to the one-dimensional (1D) regime, are connected by a quasi-1D quantum interferometer. Under dc current heating of the electrons in one heating channel, we perform cross-correlated noise measurements locally in the directly heated channel and nonlocally in the other channel, which is indirectly heated by hot electron diffusion across the quasi-1D connection. We observe the same functional dependence of the thermal noise on the heating current. The temperature dependence of the electron energy-loss rate is reduced compared to wider 2D systems. In the quantum interferometer, we show the decoherence due to the diffusion of hot electrons from the heating channel into the quasi-1D system, which causes a thermal gradient.Comment: 6 pages, 5 figure

Single-hole transistor in p-type GaAs/AlGaAs heterostructures

A single-hole transistor is patterned in a p-type, C-doped GaAs/AlGaAs heterostructure by AFM oxidation lithography. Clear Coulomb blockade resonances have been observed at T=300 mK. A charging energy of ~ 1.5 meV is extracted from Coulomb diamond measurements, in agreement with the lithographic dimensions of the dot. The absence of excited states in Coulomb diamond measurements, as well as the temperature dependence of Coulomb peak heights indicate that the dot is in the multi-level transport regime. Fluctuations in peak spacings larger than the estimated mean single-particle level spacing are observed.Comment: 4 pages, 5 figure