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The occurrence of antiferromagnetism (AFM) in  κ ‐(ET) 2 X can be understood within an effective 1/2‐filled band with dimers of ET molecules containing one hole each. We argue that while this effective model can describe the presence of AFM, a complete description for these materials requires the correct carrier density of one‐half per molecule. For dimerized and strongly frustrated 1/4‐filled lattices we show that a singlet‐paired statecoexisting with charge ordering occurs that we have termed the paired electron crystal (PEC). Here we investigate the 1/4‐filled model on a dimerized lattice, showing regions where AFM, PEC, and the Wigner‐crystal occur. We point out the need to go beyond quantum spin liquid concepts for highly frustrated materials such as  κ ‐(ET) 2 Cu 2 (CN) 3  and  β ′‐EtMe 3 Sb[Pd(dmit) 2 ] 2  which we believe are PECs at low temperatures.

Beyond the quantum spin liquid concept in frustrated two dimensional organic superconductors