Designing electronic magnetoelectric matter with organic quantum spin trimers

Magnetoelectric (ME) phenomena are commonly driven by spin-lattice coupling. Here we demonstrate a different route based on frustrated quantum spin trimers that intrinsically intertwine magnetic moments and electric dipoles. Using molecular design principles, we realize a weakly coupled lattice of equilateral $S=1/2$ spin trimers in the organic radical crystal TNN$\cdot$CH$_3$CN. In this material, correlated electronic fluctuations within each trimer generate electric dipoles, while geometrically frustrated intertrimer interactions organize them into collective ME states. Magnetization, thermodynamic, and dielectric measurements reveal multiple magnetic-field-induced phases, including the $1/3$-magnetization plateau marked by pronounced dielectric anomalies. Effective low-energy theories and numerical simulations show that these phenomena are driven by electronically generated trimer dipoles whose collective order is stabilized by frustration relief of the intertrimer interactions, establishing a direct connection between geometric frustration and emergent magnetoelectricity. Our results identify quantum spin trimers as multifunctional building blocks, providing a bottom-up route for designing correlated ME materials from electronically active quantum spin clusters.