Single-exciton spectroscopy of single Mn doped InAs quantum dots

The optical spectroscopy of a single InAs quantum dot doped with a single Mn atom is studied using a model Hamiltonian that includes the exchange interactions between the spins of the quantum dot electron-hole pair, the Mn atom, and the acceptor hole. Our model permits linking the photoluminescence spectra to the Mn spin states after photon emission. We focus on the relation between the charge state of the Mn, A0 or A−, and the different spectra which result through either band-to-band or band-to-acceptor transitions. We consider both neutral and negatively charged dots. Our model is able to account for recent experimental results on single Mn doped InAs photoluminescence spectra and can be used to account for future experiments in GaAs quantum dots. Similarities and differences with the case of single Mn doped CdTe quantum dots are discussed.

Optical control of the spin state of two Mn atoms in a quantum dot

We report on the optical spectroscopy of the spin of two magnetic atoms (Mn) embedded in an individual quantum dot interacting with a single electron, a single exciton, or a single trion. As a result of their interaction to a common entity, the Mn spins become correlated. The dynamics of this process is probed by time-resolved spectroscopy, which permits us to determine an optical orientation time in the range of a few tens of nanoseconds. In addition, we show that the energy of the collective spin states of the two Mn atoms can be tuned through the optical Stark effect induced by a resonant laser field.

Single-electron transport in electrically tunable nanomagnets

We study a single-electron transistor (SET) based upon a II–VI semiconductor quantum dot doped with a single-Mn ion. We present evidence that this system behaves like a quantum nanomagnet whose total spin and magnetic anisotropy depend dramatically both on the number of carriers and their orbital nature. Thereby, the magnetic properties of the nanomagnet can be controlled electrically. Conversely, the electrical properties of this SET depend on the quantum state of the Mn spin, giving rise to spin-dependent charging energies and hysteresis in the Coulomb blockade oscillations of the linear conductance.

Graphene single-electron transistor as a spin sensor for magnetic adsorbates

We study single-electron transport through a graphene quantum dot with magnetic adsorbates. We focus on the relation between the spin order of the adsorbates and the linear conductance of the device. The electronic structure of the graphene dot with magnetic adsorbates is modeled through numerical diagonalization of a tight-binding model with an exchange potential. We consider several mechanisms by which the adsorbate magnetic state can influence transport in a single-electron transistor: tuning the addition energy, changing the tunneling rate, and in the case of spin-polarized electrodes, through magnetoresistive effects. Whereas the first mechanism is always present, the others require that the electrode has to have either an energy- or spin-dependent density of states. We find that graphene dots are optimal systems to detect the spin state of a few magnetic centers.

Single-walled carbon nanotube buckypapers as electrocatalyst supports for methanol oxidation

This work studies the use of various single-walled carbon nanotube (SWCNT) buckypapers as catalyst supports for methanol electro-oxidation in acid media. Buckypapers were obtained by vacuum filtration from pristine and oxidized SWCNT suspensions in different liquid media. Pt–Ru catalysts supported on the buckypapers were prepared by multiple potentiostatic pulses using a diluted solution of Pt and Ru salts (2 mM H2PtCl6 + 2 mM RuCl3) in acid media. The resulting materials were characterized via SEM, TEM, EDX and ICP-OES analysis. Well dispersed rounded nanoparticles between 2 and 15 nm were successfully electrodeposited on the SWCNT buckypapers. The ruthenium content in the bimetallic deposits was between 32 and 48 at. %, while the specific surface areas of the catalysts were in the range of 72–113 m2 g−1. It was found that the solvent used to prepare the SWCNT buckypaper films has a strong influence on the catalyst dispersion, particle size and metal loading. Cyclic voltammetry and chronoamperometry experiments point out that the most active electrodes for methanol electro-oxidation were prepared with the buckypaper supports that were obtained from SWCNT dispersions in N-methyl-pyrrolidone.

Electrocatalytic reduction of CO2 to formate using particulate Sn electrodes: Effect of metal loading and particle size

The development of electrochemical processes for the conversion of CO2 into value-added products allows innovative carbon capture & utilization (CCU) instead of carbon capture & storage (CCS). In addition, coupling this conversion with renewable energy sources would make it possible to chemically store electricity from these intermittent renewable sources. The electroreduction of CO2 to formate in aqueous solution has been performed using Sn particles deposited over a carbon support. The effect of the particle size and Sn metal loading has been evaluated using cyclic voltammetry and chronoamperometry. The selected electrode has been tested on an experimental filter-press type cell system for continuous and single pass CO2 electroreduction to obtain formate as main product at ambient pressure and temperature. Experimental results show that using electrodes with 0.75 mg Sn cm−2, 150 nm Sn particles, and working at a current density of 90 mA cm−2, it is possible to achieve rates of formate production over 3.2 mmol m−2 s−1 and faradaic efficiencies around 70% for 90 min of continuous operation. These experimental conditions allow formate concentrations of about 1.5 g L−1 to be obtained on a continuous mode and with a single pass of catholyte through the cell.

Controlled Complete Suppression of Single-Atom Inelastic Spin and Orbital Cotunneling

The inelastic portion of the tunnel current through an individual magnetic atom grants unique access to read out and change the atom’s spin state, but it also provides a path for spontaneous relaxation and decoherence. Controlled closure of the inelastic channel would allow for the latter to be switched off at will, paving the way to coherent spin manipulation in single atoms. Here, we demonstrate complete closure of the inelastic channels for both spin and orbital transitions due to a controlled geometric modification of the atom’s environment, using scanning tunneling microscopy (STM). The observed suppression of the excitation signal, which occurs for Co atoms assembled into chains on a Cu2N substrate, indicates a structural transition affecting the dz2 orbital, effectively cutting off the STM tip from the spin-flip cotunneling path.