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The ultimate goal of neuroscience is to correlate the activity of neurons and neuronal networks to higher order behaviors and cognition. This colossal task necessitates a variety of optical tools that can both measure and modulate neuronal activity. This dissertation describes the design, synthesis and characterization of a variety of such tools. In order to interrogate the electrical activity of neuronal circuits directly, we synthesized tetramethylrhodamine-based voltage reporters, or RhoVRs, that possess excitation and emission profiles in the green to orange region of the visible spectrum and use photoinduced electron transfer (PeT) as a trigger for voltage sensing. Two RhoVRs with particularly attractive photophysical properties were developed: RhoVR 1, which possessed the highest voltage sensitivity of any RhoVR (47% ΔF/F per 100 mV), and RhoVR (Me), a less sensitive (13% ΔF/F per 100 mV) but far brighter …