A pulse train comprising chirped pulses can be used to excite a sample, such as for spectroscopic analysis. The respective chirped pulses can include a frequency sweep to establish a first frequency-domain comb. A width of frequency-domain comb peaks can be established at least in part by a total duration of the pulse train, and a bandwidth of the first frequency-domain comb can be determined at least in part by a bandwidth of the frequency sweep of the respective chirped pulses. A free-space or enclosed sample interaction region can be used.