Using ab initio calculations based on the correlated band theory, we have investigated the quasi-one-dimensional chain system $\beta$-V$_2$O(PO$_4$), showing both charge and spin orderings. Even in the uncorrelated region, the pure transition from the tetragonal to the monoclinic structure leads to a sizable charge difference between the two types of V ions, regardless of magnetic orders. In the ferrimagnetic phase, inclusion of the on-site Coulomb repulsion $U$ leads to a full orbital-polarization of V1 ($t_{ 2g}^{ 3\uparrow}$, $S=\frac{ 3}{ 2}$) and V2 ($a_{ 1g}^{ 1\downarrow}e_g^{ \prime{ 1\downarrow}}$, $S=1$) above $U^c_{ eff}\approx3.5$ eV, leading to local spin moments of 2.30 and --1.54 $\mu_B$, respectively, with small orbital moments of several hundredth $\mu_B$. So, the net moment is nearly 1 $\mu_B$ per formula unit, which is about 2--3 times larger than the experimental value. Our results show significant variations, strongly depending on the strength of $U_{ eff}$, in energy differences between various magnetic states as well as a small magnetic anisotropy. These results suggest that the substantial difference between the calculated and experimental moments is attributed to quantum fluctuation of the pyrochlore-like weakly linked V$_4$ tetrahedral structure. Our findings are expected to provide a good platform to investigate the interplay among the charge-, spin-, and lattice-degrees of freedom, and geometrical frustration.
Categories: cond-mat.str-el cond-mat.mtrl-sci