We present a joint experimental and theoretical study of spin coherence properties of 39 K, 85 Rb, 87 Rb, and 133 Cs atoms trapped in a solid parahydrogen matrix. We use optical pumping to prepare the spin states of the implanted atoms and circular dichroism to measure their spin states. Optical pumping signals show order-of-magnitude differences depending on both matrix growth conditions and atomic species. We measure the ensemble transverse relaxation times (T * 2 ) of the spin states of the alkali-metal atoms. Different alkali species exhibit dramatically different T * 2 times, ranging from sub-microsecond coherence times for high mF states of 87 Rb, to ∼ 10 2 microseconds for 39 K. These are the longest ensemble T * 2 times reported for an electron spin system at high densities (n 10 16 cm −3 ). To interpret these observations, we develop a theory of inhomogenous broadening of hyperfine transitions of 2 S atoms in weakly-interacting solid matrices. Our calculated ensemble transverse relaxation times agree well with experiment, and suggest ways to longer coherence times in future work. arXiv:1910.05430v1 [physics.atom-ph]