We have used a relatively long, contiguous VHF observation of a bright cosmic radio source (Cygnus A) with the Very Large Array (VLA) to demonstrate the capability of this instrument to study the ionosphere. This interferometer, and others like it, can observe ionospheric total electron content (TEC) fluctuations on a much wider range of scales than is possible with many other instruments. We have shown that with a bright source, the VLA can measure differential TEC values between pairs of antennas (delta-TEC) with an precision of 0.0003 TECU. Here, we detail the data reduction and processing techniques used to achieve this level of precision. In addition, we demonstrate techniques for exploiting these high-precision delta-TEC measurements to compute the TEC gradient observed by the array as well as small-scale fluctuations within the TEC gradient surface. A companion paper details specialized spectral analysis techniques used to characterize the properties of wave-like fluctuations within this data.