Reprogrammable and Reconfigurable Photonic Molecular Logic Gates Based on Ln3+ Ions

The miniaturization of the silicon chips is reaching its physical limits, and the transistors are so small that current leakage will become an insurmountable problem. Additionally, the actual chip shortage makes clear the excessive world dependence on silicon, stressing the need for silicon‐free computing strategies. Quantum computing process information by manipulating photons, and computation performed by individual molecules are being proposed as alternatives, with potential benefits in terms of miniaturization, performance enhancement, and energy efficiency. Molecular logics can play a decisive role in the future of the computer industry, and the unique photonic characteristics of trivalent lanthanide ions make them suitable candidates to integrate future molecular logic applications. In this work, a Eu3+/Tb3+ co‐doped organic–inorganic hybrid is presented as an illustrative all‐photonic logic platform constructed through the decay dynamics of both lanthanide and hybrid host emissions. Besides combinatory AND, NAND, and INH logic gates, this system presents on‐choice Eu3+, Tb3+, or host emission enabling the development of reprogrammable and reconfigurable photonic molecular logic gates. All‐photonic temperature‐reprogrammable changes from AND to INH logic gates and a reconfiguration among INH and AND1 or AND2 gates, based on the excitation wavelength are demonstrated, showing a clear step forward toward mirroring electronic logic counterparts. Organic–inorganic hybrid materials based on di‐ureasils doped with Ln3+ can perform molecular logic operations based on physical inputs. Under UV radiation, the reconfiguration of the system through simple logic operations is achieved. Exploiting the distinctive emission features of the Ln3+ and the organic–inorganic hybrid host, novel reprogrammable and reconfigurable photonic molecular logic gates are developed.