Part of the relaxed structure of the fcc Ne matrix with NO impurity in the ground state. The NO is in cyan, the first shell (closest face centers) is in red, the second one (closest vertices) is in violet, the third one (next closest face centers) is in green, and the fourth one (next closest vertices across a face diagonal) is in blue. The distances are in atomic units. Note that the simulations are performed using one NO and a total of 4212 Ne atoms.
Expectation values of the shell displacements (with respect to the pure crystal) imposed by the presence of the NO impurity in a substitutional site in the matrix. Squares and triangles correspond to the impurity ground state, and circles and diamonds to its first Rydberg state. Orange and red curves: MCTDH radial model,49 black and blue curves: G-TDH model (this work).
Time evolution of the radial densities of shells 1 (top) and 4 (bottom), as defined by Eq. (19) on the left panel and Eq. (25) on the right panel.
Time-dependent radial displacement values of the shell atoms, after impulsive excitation of the central NO impurity. Black lines: values obtained by the G-TDH method, red lines: values obtained by the MCTDH radial model. Left panel: shells forming the principal axes, showing a large, successive dynamical displacement (“bubble formation”). Right panel: other close-by shells, showing a less pronounced dynamics.
Total energy of all atoms lying on the principal axes (Eq. (26)). The decrease reflects the transfer of energy to the remaining atoms.
Pump-probe spectra, as a function of delay time T and probe wavelength λ, simulated using the G-TDH method (upper panel) and the MCTDH radial shell model (lower panel).
Lennard-Jones V LJ = 4ε((σ/r)12 − (σ/r)6)51,52 and exponential V exp = A exp( − β(r − r 0)) parameters used in this work, as obtained by adjustment to experimental absorption spectra (in atomic units, Ref. 53).
Shell structure and main properties of the NO–Ne model, as obtained by the relaxation method for both approaches. First column: shell number. Second column: number of atoms n s . Columns 3 and 4: radius of shells, assuming a pure matrix, ⟨R s ⟩ p obtained by the shell model, obtained by the full-dimensional G-TDH model. Columns 5–8: expectation values of the shell radii for the relaxed matrix, with NO(X), (columns 5 and 6) and NO(A) (columns 7 and 8) using the above mentioned methods, notation as above. All distances are expressed in atomic units.
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