Intermolecular NO-matrix potential curves for the ground and the lowest three Rydberg states in a configurational coordinate model as derived from Ref. 19. In the experiment, the pump pulse excites the state of NO by two-photon absorption. The subsequent evolution on the excited state surface is probed by inducing transitions from the to the and states and monitoring, as a function of the pump-probe time delay, the depletion of the fluorescence. Note that different probe wavelengths open different observation windows, and that more than one configuration can be associated with the same probe energy (e.g., ). A schematic representation of the impurity (full black circle) and the matrix species (open circles) at different stages is also shown.
Fluorescence depletion trace measured with vertical pump, probe, and detection (empty circles), same signal measured with horizontal pump (filled circles), and difference of the two traces (filled squares).
Left panels: Subpicosecond depletion scans measured at different probe wavelengths. The values shown on the left indicate the rise time of the signals (from Gaussian fits). In the transient corresponding to , the pump-probe cross-correlation signal (fitted by a Gaussian of FWHM) is superimposed to the fluorescence depletion signal. The vertical lines indicate the ends of the two different regimes observed in the dynamics. Right panels: Windows opened by the probes to the (dotted trace) and (dashed trace) states.
Left panel: Time dependence of the cage radius increment retrieved from the correspondence between the configurations probed (Fig. 3, left panels) and the associated transients (Fig. 3 right panels). The vertical error bars correspond to the width of the probe windows (Ref. 23). The horizontal error bars account for the width of the structures in the experimental depletion traces. Right panel: Excess energy above the minimum of the state at different time delays, corresponding to the radial increments shown in the left panel. The uncertainties on energy are determined considering the potential energy range spanned by each probe window (Ref. 23). The uncertainties on time correspond to those in the left plot.
Pump-probe fluorescence depletion scans over long times. The intensity of the probe beams indicated in parentheses is relative to the intensity at , . Lower panel inset: Depletion signal at obtained at higher probe intensity. The arrow indicates the position of the recurrence.
Pump (left panels) and probe (right panels) power dependences at fixed probe wavelength . The good overlap of the traces normalized to the level of their offset at long delays, presented in the lower panels, indicates that the picosecond rise is independent from the beam intensities.
NO fluorescence depletion scans measured in (empty circles) and (filled circles).
Radial distribution functions of solid hydrogen from path integral monte carlo (PIMC) simulations (Ref. 9, squares), MD simulations at (this work, dashed trace), and MD simulations at (this work, full trace). Inset: Silvera-Goldman pair potential, and temperature of the classical MD simulations at (dashed horizontal line) and at (full horizontal line).
Calculated radial distribution function of neat (dashed trace) and around the impurity in NO doped (full trace).
Experimental (circles) and simulated (full trace) absorption and emission line shapes.
Time dependent at the excitation (full trace) and at delays of (dashed trace), (empty circles), (black dots), and (triangles). Inset: Comparison of the at (triangles) and at (full trace).
Radius increment of the lattice shells around the impurity: first shell (full trace), second shell (dashed trace), and third shell (dotted trace). The empty circles correspond to the cage radius increment from Fig. 4 scaled to match the maximum of the simulated radius of the first shell. Vertical lines: breaks in medium response extracted from the experimental measurements.
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