With hybrid organic–inorganic perovskites expanding their technological reach, from photovoltaic solar cells that operate at low carrier densities (1011 − 1013 cm−3) to light‐emitting diodes and lasers that operate at higher carrier densities (1013 − 1019 cm−3), it is critical to know how microstructure dictates carrier dynamics at varying injected carrier densities. For fabrication at scale, it is equally critical to know how quickly during the growth process do hybrid perovskites develop their characteristic optoelectronic properties. This work reports on a facile fabrication method that “freezes” different stages of nucleation and growth kinetics of prototypical hybrid perovskite on the same substrate—providing a unique strategy to assess differences in optoelectronic properties and carrier dynamics from nascent nucleating microcrystals to large‐grain thin films. The solution‐processed fabrication technique, optimized to control the nucleation density of an intermediate phase, successfully decouples the nucleation and growth steps that lead to large‐grain thin films. Ultrafast broadband absorption microscopy finds that the nucleating microcrystals already possess the optoelectronic properties of hybrid perovskites and share similar femtosecond‐to‐nanosecond dynamics as large‐grain thin films. When compared to the large‐grain thin films, the confining microcrystals exhibit enhanced carrier interactions, marked by an increase in bimolecular and Auger recombination rates.

Coupling between light and matter strongly depends on the polarization of the electromagnetic field and the nature of the excitations in the material. As hybrid perovskites emerge as a promising...

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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.