We demonstrate a versatile approach to fine-tuning the ratio of blue to near-infrared emission intensity from ions in nanocrystals by adjusting the pulse widths and excitation wavelengths of red laser beams. The mechanism of color-tunable emission by pulse widths is explored, and a mechanism based on promoting the population of some luminescence levels and cutting off the population of others by suitably adjusting pulse duration is proposed. The underlying reason of excitation wavelength-modulated emission is ascribed to tuning absorption probability ratio of ground state absorption to excited state absorption by tuning the matching degree between the energies of excitation wavelength and ground (excited) state absorption of . The ability of our nanocrystals to emit variable emissions on demand in response to pulse width and excitation wavelength provides keen insights into controlling the population processes of luminescent levels and offers a versatile approach for tuning the spectral output.
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