We use neutron scattering to study vanadium (hole)-doped LiFe$_{1-x}$V$_x$As. In the undoped state, LiFeAs exhibits superconductivity at $T_c=18$ K and transverse incommensurate spin excitations similar to electron overdoped iron pnictides. Upon vanadium-doping to form LiFe$_{0.955}$V$_{0.045}$, the transverse incommensurate spin excitations in LiFeAs transform into longitudinally elongated in a similar fashion as that of potassium (hole) doped Ba$_{0.7}$K$_{0.3}$Fe$_2$As$_2$, but with dramatically enhanced magnetic scattering and elimination of superconductivity. This is different from the suppression of the overall magnetic excitations in hole doped BaFe$_2$As$_2$ and the enhancement of superconductivity near optimal hole doping. These results are consistent with density function theory plus dynamic mean field theory calculations, suggesting that vanadium-doping in LiFeAs may induce an enlarged effective magnetic moment $S_{eff}$ with a spin crossover ground state arising from the inter-orbital scattering of itinerant electrons.
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