This work presents the results of instrumentation developments and scientific studies aimed at better probing the nature of the solar chromosphere. Indeed, the sources of the energy and mass to the chromosphere and corona (and the mechanisms by which the energy is deposited there), remain one of the most mysterious aspects of the structuring of stellar atmospheres. The goal of this thesis is to apply new methods to studies of the solar chromosphere in order to advance our understanding of its structure and dynamics. I perform an analysis of imaging spectroscopy techniques, comparing the spectral fidelity achieved by different classes of instruments and evaluating a metric for the spectral measurement efficiency. I describe an upgrade of the Interferometric Bidimensional Spectrometer (IBIS) to a faster data acquisition system that better allows the application' of image reconstruction techniques and faster sampling of the rapid variations in the solar chromosphere. I use the upgraded system to obtain a unique mosaic providing a comprehensive view of the chromosphere featuring diffraction-limited resolution, full spectral information, and a large field of view. I describe two studies that used this dataset to examine the configuration of the chromospheric magnetic field, revealing that network fields in the upper atmosphere may be largely non-potential. I further examine the chromospheric diagnostics provided by several different lines, exploring the information encoded in chromospheric line widths and combining datasets to reveal different aspects of the chromospheric conditions. I find that the Ha 6563 and Call 8542 A lines, despite differences in appearances, are largely formed in the same plasma volumes.