Capturing the Ultrafast Vibrational Decoherence of Hydrogen Bonding in Interfacial Water.
نویسندگان
چکیده
Vibrational sum-frequency generation (vSFG) measurements in the frequency and time domains reveal that the interfacial hydrogen bonded OH stretch at the water/calcium fluoride interface is composed of two populations oriented oppositely. The time-resolved vSFG free-induction decay suggested that, whereas the strongly hydrogen bonded OH vibrational stretches, centered near 3140 ± 11 cm-1, are oriented toward bulk water and lose their collective coherence within ∼70 ± 7 fs, the weakly hydrogen bonded OH species, centered near 3410 ± 12 cm-1, are pointed toward the interface and dephase within ∼50 ± 6 fs.
منابع مشابه
Ultrafast reorientation of dangling OH groups at the air-water interface using femtosecond vibrational spectroscopy.
We report the real-time measurement of the ultrafast reorientational motion of water molecules at the water-air interface, using femtosecond time- and polarization-resolved vibrational sum-frequency spectroscopy. Vibrational excitation of dangling OH bonds along a specific polarization axis induces a transient anisotropy that decays due to the reorientation of vibrationally excited OH groups. T...
متن کاملStrong frequency dependence of vibrational relaxation in bulk and surface water reveals sub-picosecond structural heterogeneity
Because of strong hydrogen bonding in liquid water, intermolecular interactions between water molecules are highly delocalized. Previous two-dimensional infrared spectroscopy experiments have indicated that this delocalization smears out the structural heterogeneity of neat H2O. Here we report on a systematic investigation of the ultrafast vibrational relaxation of bulk and interfacial water us...
متن کاملFemtosecond Hydrogen Bond Dynamics of Bulk‐like and Bound Water at Positively and Negatively Charged Lipid Interfaces Revealed by 2D HD‐VSFG Spectroscopy
Interfacial water in the vicinity of lipids plays an important role in many biological processes, such as drug delivery, ion transportation, and lipid fusion. Hence, molecular-level elucidation of the properties of water at lipid interfaces is of the utmost importance. We report the two-dimensional heterodyne-detected vibrational sum frequency generation (2D HD-VSFG) study of the OH stretch of ...
متن کاملOrdered water structure at hydrophobic graphite interfaces observed by 4D, ultrafast electron crystallography.
Interfacial water has unique properties in various functions. Here, using 4-dimensional (4D), ultrafast electron crystallography with atomic-scale spatial and temporal resolution, we report study of structure and dynamics of interfacial water assembly on a hydrophobic surface. Structurally, vertically stacked bilayers on highly oriented pyrolytic graphite surface were determined to be ordered, ...
متن کاملAn ab initio molecular dynamics study of water–carbon tetrachloride liquid–liquid interface: nature of interfacial structure, hydrogen bonds and dynamics
We present a theoretical study of the structure and dynamics of water–carbon tetrachloride liquid–liquid interface by means of ab initio molecular dynamics simulations. We have studied the density profiles, orientational profiles, hydrogen bond distributions, vibrational power spectra, diffusion, orientational relaxation, hydrogen bond dynamics and vibrational spectral diffusion of bulk and int...
متن کاملذخیره در منابع من
با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید
عنوان ژورنال:
- The journal of physical chemistry letters
دوره 7 24 شماره
صفحات -
تاریخ انتشار 2016