Fig. 2: Experimental evidence of coherent and incoherent phonon dressings of d–d crystal field transitions.
From: Vibrational coherent control of localized d–d electronic excitation
a,c, Pump wavelength dependency of the transmissivity measured for a probe energy EVIS = 1.75 eV (a) and 1.37 eV (c). The long-timescale signals, at λmidIR ≈ 7.7 µm and λmidIR ≈ 11 µm, are associated with a dissipative thermal response12,18 and overlap with the minima of CuGeO3 transmission (right panel of a, data reproduced from ref. 12). b, Time-dependent transmissivity as a function of the probe photon energy for λmidIR = 9 µm pump wavelength. The bottom panel displays time-dependent transmissivity at energies of 1.37 eV, 1.55 eV, 1.70 eV and 1.89 eV (highlighted respectively by the red, orange, green and purple dashed lines in the map). The lowest energy is in the tail of the d–d absorption and the others correspond to the central energies of the d–d bands (right panel, data reproduced from ref. 14). Transparency regions are observed at 1.55 eV in the first 50 fs and below 1.4 eV on longer timescales. d, Fitted map (left) obtained with the transient Gaussian fitting parameters (Δp) of the three d–d absorption peaks (right): amplitude (Ai), central energy (Ei) and bandwidth (σi), and background (BG). The time dependence of the parameters highlights the coherent nature of the fast time evolution of d–d phonon-assisted transitions.
