LAUSR

Neuromorphic electronics, being inspired by how the brain works, hold great promise to the successful implementation of smart artificial systems. Among several neuromorphic hardware issues, a robust device functionality under extreme temperature is of particular importance for practical applications. Given that the organic memristors for artificial synapse applications are demonstrated under room temperature, achieving a robust device performance at extremely low or high temperature is still utterly challenging. In this work, the temperature issue is addressed by tuning the functionality of the solution‐based organic polymeric memristor. The optimized memristor demonstrates a reliable performance under both the cryogenic and high‐temperature environments. The unencapsulated organic polymeric memristor shows a robust memristive response under test temperature ranging from 77 to 573 K. Utilizing X‐ray photoelectron spectroscopy (XPS) and time‐of‐flight secondary‐ion mass spectrometry (ToF‐SIMS) depth profiling, the device working mechanism is unveiled by comparing the compositional profiles of the fresh and written organic polymeric memristors. A reversible ion migration induced by an applied voltage contributes to the characteristic switching behavior of the memristor. Herein, both the robust memristive response achieved at extreme temperatures and the verified device working mechanism will remarkably accelerate the development of memristors in neuromorphic systems.