Ultrashort light pulses can selectively excite charges, spins, and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge-density wave (CDW) material 1-TaSe After exciting the material with a femtosecond pulse, fast spatial smearing of the laser-excited electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This finding is in contrast to all previous observations in multiple materials to date, where the electron temperature decreases monotonically via electron-phonon scattering.
View Article and Find Full Text PDFAdsorption energies of chemisorbed molecules on inorganic solids usually scale linearly with molecular size and are well described by additive scaling laws. However, much less is known about scaling laws for physisorbed molecules. Our temperature-programmed desorption experiments demonstrate that the adsorption energy of acenes (benzene to pentacene) on the Au(111) surface in the limit of low coverage is highly nonadditive with respect to the molecular size.
View Article and Find Full Text PDFEnhancing the selectivity of catalytic processes has potential for substantially increasing the sustainability of chemical production. Herein, we establish relationships between reaction selectivity and molecular structure for a homologous series of key intermediates for oxidative coupling of alcohols on gold using a combination of experiment and theory. We establish a scale of binding for molecules with different alkyl structures and chain lengths and thereby demonstrate the critical nature of noncovalent van der Waals interactions in determining the selectivity by modulating the stability of key reaction intermediates bound to the surface.
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