Room‐Temperature Organic Spintronic Devices with Wide Range Magnetocurrent Tuning and Multifunctionality via Electro‐Optical Compensation Strategy

In spintronics, devices exhibiting large, widely tunable magnetocurrent (MC) values at room temperature are particularly appealing due to their potential in advanced sensing, data storage, and multifunctional technologies. Organic semiconductors (OSCs), with their rich and unique spin-dependent and (opto-)electronic properties, hold significant promise for realizing such devices. However, current organic devices are constrained by limited design strategies, yielding MC values typically confined to tens of percent, thereby restricting their potential for multifunctional applications. Here, this study introduces an electro-optical compensation strategy to modulate MC values, which synergistically integrates and manages the interplays among carrier transport, spin-dependent reactions, and photogenerated carrier dynamics in OSCs-based devices. This approach achieves ultrahigh room-temperature MC values of +13 200% and -10 600% in the designed devices, with continuous and precise tunability over this range-marking a breakthrough in organic spintronic devices. Building on this achievement, by integrating multiple controllable parameters-light, bias, magnetic field, and mechanical flexibility-into a single device, a flexible, room-temperature, multifunctional device is activated, functioning as the high-sensitivity magnetic field sensor, composite field sensor, magnetic current inverter, and magnetically-controlled artificial synaptic, etc. These findings open an avenue for designing high-performance, multifunctional devices with broad implications for future spintronic-related technologies.