Electronic access to glass transition in supercooled ionic liquids using ambipolar transistor

Abstract

Relaxation dynamics of supercooled liquids approaching glassy arrest remain a central challenge in integrated electronic architectures, where conventional rheometry becomes incompatible. Here, we demonstrate that an ambipolar PdSe$_2$ field-effect transistor functions as an electrical probe capable of resolving ion-specific relaxation dynamics in fragile ionic glass formers and semiquantitatively inferring rheological parameters within an operating device environment. Temperature evolution of the transfer curve hysteresis and time-resolved current transients under ionic-gate pulse reveal a non-Arrhenius fragile slowdown. We track the continuous reduction of dynamically equilibrated liquid regions approaching the glass transition through an electrically accessible quantity $p_\text{eq}(T)$, quantifying the fraction of the mobile ions able to relax within the experimental timescale. Upon cooling, $p_\text{eq}$ collapses sharply as mobile regions fragment into percolating fractal clusters, consistent with a reduction of configurational entropy predicted for fragile glass formers. This approach enables temperature-dependent scaling of viscosity and extraction of characteristic temperatures marking the ergodic-to-nonergodic crossover, within a solid-state device architecture where conventional rheological characterization is inapplicable. Further, polymer confinement of the ionic liquid shifts these characteristic temperatures upward, demonstrating the sensitivity of this method to structural constraints imposed by the polymer matrix.