Coherent Hemodynamics Spectroscopy (CHS) is a technique based on inducing cerebral hemodynamic oscillations at multiple frequencies, measuring them with near-infrared spectroscopy (NIRS), and analyzing them with a hemodynamic model to obtain physiological information such as blood transit times in the microvasculature and the autoregulation cutoff frequency. We have previously demonstrated that such oscillations can be induced one frequency at a time. Here we demonstrate that CHS can be performed by a single inflation of two pneumatic thigh cuffs (duration: 2 min; pressure: 200 mmHg), whose sudden release produces a step response in systemic arterial blood pressure that lasts for ~20 s and induces cerebral hemodynamics that contain all the frequency information necessary for CHS. Following a validation study on simulated data, we performed measurements on human subjects with this new method based on a single occlusion/release of the thigh cuffs and with the previous method based on sequential sets of cyclic inflation/deflation one frequency at a time, and demonstrated that the two methods yield the same CHS spectra and the same physiological parameters (within measurement errors). The advantages of the new method presented here are that CHS spectra cover the entire bandwidth of the induced hemodynamic response, they are measured over ~20 s thus better satisfying the requirement of time invariance of physiological conditions, and they can be measured every ~2.5 min thus achieving finer temporal sampling in monitoring applications.