Optical probing of spin fluctuations of a single paramagnetic Mn atom in a semiconductor quantum dot

We analyzed the photoluminescence intermittency generated by a single paramagnetic spin localized in an individual semiconductor quantum dot. The statistics of the photons emitted by the quantum dot reflect the quantum fluctuations of the localized spin interacting with the injected carriers. Photon correlation measurements, which are reported here, reveal unique signatures of these fluctuations. A phenomenological model is proposed to quantitatively describe these observations, allowing a measurement of the spin dynamics of an individual magnetic atom at zero magnetic field. These results demonstrate the existence of an efficient spin-relaxation channel arising from a spin exchange with individual carriers surrounding the quantum dot. A theoretical description of a spin-flip mechanism involving spin exchange with surrounding carriers gives relaxation times in good agreement with the measured dynamics.

Electrical control of a single Mn atom in a quantum dot

We report on the reversible electrical control of the magnetic properties of a single Mn atom in an individual quantum dot. Our device permits us to prepare the dot in states with three different electric charges, 0, +1e, and -1e which result in dramatically different spin properties, as revealed by photoluminescence. Whereas in the neutral configuration the quantum dot is paramagnetic, the electron-doped dot spin states are spin rotationally invariant and the hole-doped dot spins states are quantized along the growth direction.

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.

Pencil it in: pencil drawn electrochemical sensing platforms

Inspired by recent reports concerning the utilisation of hand drawn pencil macroelectrodes (PDEs), we report the fabrication, characterisation (physicochemical and electrochemical) and implementation (electrochemical sensing) of various PDEs drawn upon a flexible polyester substrate. Electrochemical characterisation reveals that there are no quantifiable electrochemical responses upon utilising these PDEs with an electroactive analyte that requires an electrochemical oxidation step first, therefore the PDEs have been examined towards the electroactive redox probes hexaammineruthenium(III) chloride, potassium ferricyanide and ammonium iron(II) sulfate. For the first time, characterisation of the number of drawn pencil layers and the grade of pencil are examined; these parameters are commonly overlooked when utilising PDEs. It is demonstrated that a PDE drawn ten times with a 6B pencil presented the most advantageous electrochemical platform, in terms of electrochemical reversibility and peak height/analytical signal. In consideration of the aforementioned limitation, analytes requiring an electrochemical reduction as the first process were solely analysed. We demonstrate the beneficial electroanalytical capabilities of these PDEs towards p-benzoquinone and the simultaneous detection of heavy metals, namely lead(II) and cadmium(II), all of which are explored for the first time utilising PDEs. Initially, the detection limits of this system were higher than desired for electroanalytical platforms, however upon implementation of the PDEs in a back-to-back configuration (in which two PDEs are placed back-to-back sharing a single connection to the potentiostat), the detection limits for lead(II) and cadmium(II) correspond to 10 μg L−1 and 98 μg L−1 respectively within model aqueous (0.1 M HCl) solutions.