TY - JOUR
T1 - Chemisorbed-molecule potential energy surfaces and DIET processes
AU - Jennison, D. R.
AU - Stechel, E. B.
AU - Burns, A. R.
AU - Li, Y. S.
N1 - Funding Information:
In Section 2, we present the results of studies of chemisorbed NO and ammonia on Pd( 1 1 1). The DMol computer code [6] was used with clusters of 9-19 Pd atoms, simulating the Pd( 1 1 1) surface. We compare our calculations with the latest data concerning site preferences, binding energy, and vibrational frequencies. We * Corresponding author. E-mail drjenni@sandia.gov. ’ Work supported by the US Department of Energy under Contract DE-AC04-94AL85000.
PY - 1995/6/3
Y1 - 1995/6/3
N2 - We report the use of the local-density approximation, with and without gradient corrections, for the calculation of ground-state potential energy surfaces (PESs) for chemisorbed molecules. We focus on chemisorbed NO and ammonia on Pd(1 1 1) and compare our results with the latest experimental information. We then turn to two aspects of excited-state PESs. First, we compare first-principles calculations of the forces on an ammonia ion as a function of distance from the surface. We find that the image-charge model fails significantly at distances which are the most relevant for dynamics, closer than ∼3 Å, and discuss reasons for the failure. We then summarize a purely electronic adiabatic model of the moleuule-surface bond and use empirical parameters to estimate hot carrier-produced excited states of chemisorbed NO. We find multiple PESs and a novel interpretation of the π* resonance, seen in inverse photoemission.
AB - We report the use of the local-density approximation, with and without gradient corrections, for the calculation of ground-state potential energy surfaces (PESs) for chemisorbed molecules. We focus on chemisorbed NO and ammonia on Pd(1 1 1) and compare our results with the latest experimental information. We then turn to two aspects of excited-state PESs. First, we compare first-principles calculations of the forces on an ammonia ion as a function of distance from the surface. We find that the image-charge model fails significantly at distances which are the most relevant for dynamics, closer than ∼3 Å, and discuss reasons for the failure. We then summarize a purely electronic adiabatic model of the moleuule-surface bond and use empirical parameters to estimate hot carrier-produced excited states of chemisorbed NO. We find multiple PESs and a novel interpretation of the π* resonance, seen in inverse photoemission.
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U2 - 10.1016/0168-583X(95)00292-8
DO - 10.1016/0168-583X(95)00292-8
M3 - Article
AN - SCOPUS:0002368695
VL - 101
SP - 22
EP - 30
JO - Nuclear Instruments and Methods in Physics Research, Section B: Beam Interactions with Materials and Atoms
JF - Nuclear Instruments and Methods in Physics Research, Section B: Beam Interactions with Materials and Atoms
SN - 0168-583X
IS - 1-2
ER -