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A highly sensitive CMOS-based sensing system is proposed for permittivity detection and mixture characterization of organic chemicals at microwave frequencies. The system determines permittivity by measuring the frequency difference between two voltage-controlled oscillators (VCOs); a sensor oscillator with an operating frequency that shifts with the change in tank capacitance due to exposure to the material under test (MUT) and a reference oscillator insensitive to the MUT. This relative measurement approach improves sensor accuracy by tracking frequency drifts due to environmental variations. Embedding the sensor and reference VCOs in a fractional-N phase-locked loop (PLL) frequency synthesizer enables material characterization at a precise frequency and provides an efficient material-induced frequency shift read-out mechanism with a low-complexity bang–bang control loop that adjusts a fractional frequency divider. The majority of the PLL-based sensor system, except for an external fractional frequency divider, is implemented with a 90-nm CMOS prototype that consumes 22 mW when characterizing material near 10 GHz. Material-induced frequency shifts are detected at an accuracy level of 15 \ppmrms and binary mixture characterization of organic chemicals yield maximum errors in permittivity of <1.5%. [ABSTRACT FROM PUBLISHER]