Title: Adsorption and desorption of hydrogen at nonpolar GaN(1-100) surfaces: Kinetics and impact on surface vibrational and electronic properties,
Abstract: The adsorption of hydrogen at nonpolar GaN(1-100) surfaces and its impact on
the electronic and vibrational properties is investigated using surface
electron spectroscopy in combination with density functional theory (DFT)
calculations. For the surface mediated dissociation of H2 and the subsequent
adsorption of H, an energy barrier of 0.55 eV has to be overcome. The
calculated kinetic surface phase diagram indicates that the reaction is
kinetically hindered at low pressures and low temperatures. At higher
temperatures ab-initio thermodynamics show, that the H-free surface is
energetically favored. To validate these theoretical predictions experiments at
room temperature and under ultrahigh vacuum conditions were performed. They
reveal that molecular hydrogen does not dissociatively adsorb at the GaN(1-100)
surface. Only activated atomic hydrogen atoms attach to the surface. At
temperatures above 820 K, the attached hydrogen gets desorbed. The adsorbed
hydrogen atoms saturate the dangling bonds of the gallium and nitrogen surface
atoms and result in an inversion of the Ga-N surface dimer buckling. The
signatures of the Ga-H and N-H vibrational modes on the H-covered surface have
experimentally been identified and are in good agreement with the DFT
calculations of the surface phonon modes. Both theory and experiment show that
H adsorption results in a removal of occupied and unoccupied intragap electron
states of the clean GaN(1-100) surface and a reduction of the surface upward
band bending by 0.4 eV. The latter mechanism largely reduces surface electron
depletion.