The ability to make electrical contact to single molecules creates opportunities to examine fundamental processes governing electron flow on the smallest possible length scales. We report experiments in which we controllably stretched individual cobalt complexes having spin S = 1, while simultaneously measuring current flow through the molecule. The molecule's spin states and magnetic anisotropy were manipulated in the absence of a magnetic field by modification of the molecular symmetry. This control enabled quantitative studies of the underscreened Kondo effect, in which conduction electrons only partially compensate the molecular spin. Our findings demonstrate a mechanism of spin control in single-molecule devices and establish that they can serve as model systems for making precision tests of correlated-electron theories.

Femtosecond time-resolved photoemission is used to investigate the time evolution of electronic structure in the Mott insulator 1T-TaS2. A collapse of the electronic gap is observed within 100 femtoseconds after optical excitation. The photoemission spectra and the spectral function calculated by dynamical mean field theory show that this insulator-metal transition is driven solely by hot electrons. A coherently excited lattice displacement results in a periodic shift of the spectra lasting for 20 ps without perturbing the insulating phase. This capability to disentangle electronic and phononic excitations opens new directions to study electron correlation in solids.