Figure shows the simulated 19 F- 7 Li polarization transfer curves comparing the OPTIANS and the CP. All the simulations were performed on a four spins system (three 19 F and one 7 Li) with both 19 F-19 F and 19 F- 7 Li dipolar couplings present (details are given in the methods section). The OPTIANS shapes, i.e., the optimized amplitude and phase profiles for the 19 F and 7 Li channels are shown in Figure , SI and their Fourier Transforms are in Figure , SI. The pulse shapes do not show any obvious pattern yet the results in Figure indicate systematic polarization transfer curves under different anisotropic interaction strengths. Though the optimization simulations used the conditions 400 MHz proton Larmor and 42 kHz MAS frequency, the resulting pulse sequence is effective in a broad range of experimental conditions. The simulations in Figure show performance of CP and OPTIANS at two different conditions: 400 MHz spectrometer, 42 kHz MAS and 600 MHz spectrometer, 30 kHz MAS. Note that the experiments, shown later, were performed at 600 MHz spectrometer with MAS 30 kHz. The large 19 F CSA (𝜈 !"# $ = 210 ppm) and 7 Li QC ,𝜈 % &' = 250 kHz1 deteriorate CP performance resulting into near zero polarization transfer, as shown in blue curves in Figure . On the other hand, the OPTIANS polarization transfer curve (red lines in Figure ) shows higher efficiency and transient oscillations. The maximum polarization transfer occurs at the contact time (t ()*+,(+ ) of 1200 𝜇s (36 rotor periods) in the case of 600 MHz spectrometer and 30 kHz MAS conditions and at 880 𝜇s (37 rotor periods) in the case of 400 MHz and 42 kHz spinning. To understand the effect of the two anisotropic interactions, CSA, and QC, on the polarization transfer curves, simulations performed with one of the interactions zero are shown in Figure and Figure . Figure presents the case where both the 7 Li quadrupolar and 19 F CSA interactions are zero. Upon removal of the 7 Li quadrupolar interaction the CP efficiency gets better (Figure ) but remains significantly lower than the OPTIANS. However, a decrement in the peak transfer efficiency from ~0.18 to ~0.11 was observed for the case of OPTIANS. The counter-intuitive trend of decreased efficiency in the absence of quadrupolar interaction suggests that the OPTIANS polarization transfer mechanism exploits the anisotropic interactions to enhance the efficiency. Furthermore, the faster oscillations that were present in Figure case, became significantly more pronounced in Figure indicating that the CSA has a central role in their origin. Figure shows that while the peak transfer goes up ~0.13 for the OPTIANS in the absence of CSA, the fast oscillations were observed to be less pronounced compared to Figure , fostering the hypothesis that the fast oscillations originate from the CSA while the peak efficiency goes up by the quadrupolar interaction. In the absence of both the anisotropic interactions (Figure ), CP performance is significantly better as expected, while the OPTIANS efficiency deteriorates due to the lack of supporting CSA and quadrupolar interaction. Apart from the large 19 F CSA and 7 Li quadrupolar interaction the strong 19 F- 19 F homonuclear coupling and the strength of 19 F- 7 Li dipolar interaction also influence polarization transfer efficiency in CP and the present method. As shown in Figure in SI, the 19 F-19 F homonuclear dipolar interaction strengths do not affect the maximum polarization transfer and the fast oscillation in a significant manner. The 19 F- 7 Li couplings on the other hand have a clear impact on the transfer efficiency, as expected. values for both the CPMAS and OPTIANS. The intensities in all the plots are normalized with respect to the maximum intensity obtained in that dataset. Figure shows a drastic loss in the CP efficiency with increasing the strengths of the anisotropic interactions, 𝜈 % &' and 𝜈 !"# $ . The same trend is observed at 400 MHz, 42 kHz experimental conditions as well (Figure ). The poor efficiency of the CP under large CSAs hinders its applications at higher magnetic fields due to the larger CSA values, also as shown in the plot of efficiency versus external field strength in Figure in SI. On the other hand, the OPTIANS works the best in the ranges 30 ppm < 𝜈 !"# $ < 175 ppm and 100 kHz < 𝜈 % &' < 350 kHz, at 14.1 T spectrometer. The same analysis at 9.4 T is shown in Figure , where OPTIANS works the best in the ranges 80 ppm < 𝜈 !"# $ < 280 ppm and 150 kHz < 𝜈 % &' < 350 kHz, which are near the target values of 210 ppm and 250 kHz, respectively. Note that the optimal region for the OPTIANS shifts with the magnetic field strength due to its impact on the CSA and the higher order cross-terms. The OPTIANS efficiency doesn't show a monotonic increment with the strength of the anisotropic interactions indicating a complex dependence on CSA and quadrupolar such that there is a sweet spot in the target range. This could be due to recoupling of multiple higher order terms in the Hamiltonian with different regime of their dominance as discussed later.