  In a recent letter (PRL,121,246101,2018), Sun et al. reported that combined
MD simulation and sum frequency generation vibrational spectroscopy (SFG-VS)
measurements led to conclusions of a broad and exponentially decaying
orientational distribution, and the presence of the free O-H group pointing
down to the bulk at the air/water interface. In this comment, we show that
their main conclusions are based on questionable interpretation of the SFG-VS
data presented in the letter [1], and are also contrary to the established data
analysis and interpretations in the literature [2-5].
