Increasingly stringent emissions regulations will require the development of advanced gas sensors for a variety of applications. For example, compact, inexpensive sensors are needed for detection of regulated pollutants, including hydrocarbons (HCs), CO, and NO(sub x), in automotive exhaust. Of particular importance will be a sensor for NO(sub x) to ensure the proper operation of the catalyst system in the next generation of diesel (CIDI) automobiles. Because many emerging applications, particularly monitoring of automotive exhaust, involve operation in harsh, high-temperature environments, robust ceramic-oxide-based electrochemical sensors are a promising technology. Sensors using yttria-stabilized zirconia (YSZ) as an oxygen-ion-conducting electrolyte have been widely reported for both amperometric and potentiometric modes of operation. These include the well-known exhaust gas oxygen (EGO) sensor. More recently, ac impedance-based (i.e., impedance-metric) sensing techniques using YSZ have been reported for sensing water vapor, hydrocarbons, CO, and NO(sub x). Typically small-amplitude alternating signal is applied, and the sensor response is measured at a specified frequency. Most impedance-metric techniques have used the modulus (or magnitude) at low frequencies (< 1 Hz) as the sensing signal and attribute the measured response to interfacial phenomena.