The data sets stored here accompany the related research article, showing details of spectroscopic investigations. The opj. file contains spectroscopic data for four figures in manuscript. The file can be opened by Origin. Figure 1 contains upconversion emission spectra of NaYF4@NaYbF4:Tm@NaYF4:X(X=Tb3+ or Eu3+) in presence and absence of surface molecules. Figure 2a and 2b are plotted by Tb emission intensity as a function of ligand content and Tb content, respectively. Figure 2c is upconversion emission spectral of CPPOA-coated nanoparticles under different excitation power. Figure 2f is comparative upconversion emission spectra of CPPOA-modified NaYF4@NaYbF4:Tm (1 mol%)@NaYF4:Tb (red) and NaYbF4:Tm (1 mol%)@NaYF4:Tb (black) nanocrystals. Figure 3 contains transient absorption spectra and kinetics analysis of samples. Figure 4 contains upconversion spectra of CPPOA-coated microparticles. The txt file contains the code for Monte Carlo simulation