Large‐Area Lasing in Nanoscale Complex Media: The Critical Role of Local Dielectric Environment

Abstract Controlling how electromagnetic waves interact with complex media is critical for applications in imaging and focusing. Such lightwave interactions with complex media can lead to dramatic optical effects like lasing. While much work in random lasing focus on understanding how gain and scattering co‐operatively generate lasing, little work has focused on how to manipulate the lasing threshold without modifying the structural disorder. Here, a simple, mostly unexplored, strategy is demonstrated that employs atomic layer deposition (ALD) to tune the local near‐field environment while preserving the underpinning disorder—controlling lasing in a nanoscale complex medium on a large scale (>cm²). The nanoscale complex medium is a quasi‐2D system of coupled zinc oxide nanospheres with overall thickness deep in the sub‐wavelength regime (≈λ/4). Near‐ultraviolet femtosecond spectroscopy probes the broadband response of the gain nanomaterial, details how ALD process fundamentally modifies the fast‐picosecond and slow‐nanosecond carrier dynamics, and informs on the relevant timescales critical for lasing. Full‐field electromagnetic simulations provide critical insights about how near‐field dielectric environment modifies the nanostructure's scattering cross‐section, which ultimately results in enhanced lasing. These results highlight a simple path to control how electromagnetic waves interact in a complex medium, a key step toward large‐scale implementation of complex lasers.