Electronic and magnetic properties of the charge ordered phase of LuFe 2 O 4 are investigated by means of x-ray spectroscopic and theoretical electronic structure approaches. LuFe 2 O 4 is a compound showing fascinating magnetoelectric coupling via charge ordering. Here, we identify the spin ground state of LuFe 2 O 4 in the charge ordered phase to be a 2:1 ferrimagnetic configuration, ruling out a frustrated magnetic state. An enhanced orbital moment may enhance the magnetoelectric coupling. Furthermore, we determine the densities of states and the corresponding correlation potentials by means of x-ray photoelectron and emission spectroscopies, as well as electronic structure calculations. DOI: 10.1103/PhysRevB.80.220409 PACS number͑s͒: 75.80.ϩq, 71.20.Ϫb, 78.70.Dm, 78.70.En Multiferroic transition metal oxides, i.e., compounds in which more than one ferroic phase coexist, have gained enormous attention during the last few years. 1-4 Besides a number of perovskites and related compounds, 2,5,6 the charge frustrated layered compound LuFe 2 O 4 has attracted intense interest due to its fascinating ferroelectric and magnetoelectric properties. 7,8 LuFe 2 O 4 has a rhombohedral crystal structure ͑space group R3m͒. The underlying layered structure consists of W-like hexagonal Fe 2 O 2.5 and U-like LuO 1.5 layers. 9 The W layers comprise two triangular nets of Fe ions; the resulting electric polarization is induced via a frustrated charge ordering of Fe 2+ and Fe 3+ ions on the resulting honeycomb lattice below 330 K. [10][11][12] Below 240 K a longrange ferrimagnetic order sets in. 7 The fact that the ferroelectricity is caused by correlated electrons from the Fe ions leads to unusual properties and unique capabilities of LuFe 2 O 4 . A large response of the dielectric constant by applying small magnetic fields has been found, opening a possible route for future devices. 8 Phase transitions from the charge ordered ͑CO͒ phase have been very recently associated with a nonlinear current-voltage behavior and an electric-field-induced phase transition, which might be of interest for potential electric-pulse-induced resistive switching applications. 13,14 The large magnetoelectric coupling has been attributed to an intricate interplay between charge and spin degrees of freedom with the crystal lattice and external electrical and magnetic fields to some extent on a short-range order. [15][16][17][18][19] However, there is still some confusion about the nature of spin-charge coupling in LuFe 2 O 4 . In particular a model finding a ͱ 3 ϫ ͱ 3 CO ground state 20,21 is challenged by simulations implying that the electrical polarization in LuFe 2 O 4 is due to spin-charge coupling and a spin frustrated magnetic ground state in a chain CO state. 22,23 On the other hand the first model finds a ferrimagnetic spin ground state where Fe 2+ and 1/3 of Fe 3+ make up the majority spin, and 2/3 of Fe 3+ make up the minority spin.X-ray magnetic circular dichroism ͑XMCD͒ is a very powerful tool to investigate the internal magnetic stru...