Most photon-counting detectors (PCDs) being developed use cadmium telluride (CdTe), which has nonoptimal characteristic x-ray emission with energies in the range used for breast imaging. New PCD using a gallium arsenide (GaAs) has been developed. Since GaAs has characteristic x-rays lower in energy than those of CdTe, it is hypothesized that this new PCD might be beneficial for spectral x-ray breast imaging. We performed simulations using realistic mammography x-ray spectra with both CdTe and GaAs PCDs. Five different experiments were conducted, each comparing the performance of CdTe and GaAs: (1) sensitivity of iodine quantification to charge cloud size and electronic noise, (2) effect of photon spectrum on iodine quantification, (3) effect of varying the number of energy bins, (4) a dose analysis to assess any possible dose reduction from using either detector, and (5) spectral performance of ideal CdTe and GaAs PCDs. For each study, 3 sets of 5000 noise realizations were used to calculate the Cramer-Rao lower bound (CRLB) of iodine quantification. For all spectra studied, GaAs gave a lower CRLB for iodine quantification, with 10 of the 12 spectra showing a statistically significant difference ( ). The photon energy spectrum that optimized iodine detection for both detector materials was the 40 kVp beam with 2-mm Al filtration, which produced CRLBs of and for CdTe and GaAs, respectively, when using five energy bins. GaAs is a promising detector material for contrast-enhanced spectral mammography that offers better spectral performance than CdTe.