Atomic Layer Engineering of Epsilon‐Near‐Zero Ultrathin Films with Controllable Field Enhancement

Abstract Enhanced and controlled light absorption, as well as field confinement in optically thin materials, are pivotal for energy‐efficient optoelectronics and nonlinear optical devices. Highly doped transparent conducting oxide (TCO) thin films can support the so‐called epsilon near zero (ENZ) modes in a frequency region of near‐zero permittivity, which can lead to the perfect light absorption and ultrastrong electric field intensity enhancement (FIE) within the films. To achieve full control over absorption and FIE, one must be able to tune the ENZ material properties as well as the film thickness. Here, engineered absorption and FIE are experimentally demonstrated in aluminum‐doped zinc oxide (AZO) thin films via control of their ENZ wavelengths, optical losses, and film thicknesses, tuned by adjusting the atomic layer deposition (ALD) parameters such as dopant ratio, deposition temperature, and the number of macrocycles. It is also demonstrated that under ENZ mode excitation, though the absorption and FIE are inherently related, the film thickness required for observing maximum absorption differs significantly from that for maximum FIE. This study on engineering ENZ material properties by optimizing the ALD process will be beneficial for the design and development of next‐generation tailorable photonic devices based on flat, zero‐index optics.