Schematic representation of the FCC shell structure of the solid, with NO being on a substitution site (d is the nearest neighbor distance). Note that the indicated atoms are not in a plane in the real three-dimensional FCC structure.
Expectation values of the shell displacements R s (with respect to the pure crystal) imposed by the presence of the NO impurity in a substitutional site in the matrix. Squares correspond to the impurity ground state and circles to its first Rydberg state.
Simulated absorption and emission spectra of the doped solid. Upper panel (a) shows the transitions between the ground electronic state and the first Rydberg state of the impurity molecule. Panel (b) depicts the absorption bands from the ground to the excited C and D electronic states of the nitric oxide. Solid lines represent the computed lineshapes, while the empty circles represent experimental data points (Ref. 27).
Wave packet densities for the first few shells, obtained for a pulse excitation of 280 fs (left panel) and 30 fs (right). Especially, is strongly affected by pulse shape effects. The vertical line indicates the departing time of the outward motion of the fourth shell.
Time evolution mean position (left panel) and kinetic energy (right panel) of different shells during the first 2 ps. For comparison, “silent” shells s = 2 and s = 9a are included as dashed curves in the first and third panels, respectively. Vertical dotted lines in each diagram indicate the time at which the following shell along the main axis is set in motion.
Potential differences for , α = C, D, which allow to determine the transient F.C. points for different probe pulses central frequencies.
Pump-probe signals as a function of pump laser wavelength. Left and right panels correspond to excitation pulse widths of 280 fs and 30 fs simulated for excitation to the C and D states, respectively.
Transient absorption P(T) as a function of pump-probe delay T (full lines) and its contributions P C (T) (dashed lines) and P D (T) (doted lines). Circles with error bars indicate the experimental values (from Ref. 27).
Lennard-Jones (Refs. 54 and 55) and exponential parameters used in this work, as obtained by adjustment to experimental absorption spectra (in atomic units, see text).
Shell structure and main properties of the radial model. First column: shell number. Second column: number of atoms n s . Third column: radius of shells, assuming a pure matrix. Fourth column: radial expectation values of relaxed matrix, with NO(X), Fifth column: radial expectation values of relaxed matrix, with NO(A). All distances are expressed in atomic units.
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