Energy relaxation dynamics of hydrogen-bonded OH vibration conjugated with free OH bond at an air/water interface

Author(s):  
Tatsuya Ishiyama
2006 ◽  
Vol 110 (29) ◽  
pp. 14292-14299 ◽  
Author(s):  
Stephen M. Martin ◽  
Kristian Kjaer ◽  
Markus J. Weygand ◽  
Isabelle Weissbuch ◽  
Michael D. Ward

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Ken-ichi Inoue ◽  
Mohammed Ahmed ◽  
Satoshi Nihonyanagi ◽  
Tahei Tahara

Abstract The uniqueness of water originates from its three-dimensional hydrogen-bond network, but this hydrogen-bond network is suddenly truncated at the interface and non-hydrogen-bonded OH (free OH) appears. Although this free OH is the most characteristic feature of interfacial water, the molecular-level understanding of its dynamic property is still limited due to the technical difficulty. We study ultrafast vibrational relaxation dynamics of the free OH at the air/water interface using time-resolved heterodyne-detected vibrational sum frequency generation (TR-HD-VSFG) spectroscopy. With the use of singular value decomposition (SVD) analysis, the vibrational relaxation (T1) times of the free OH at the neat H2O and isotopically-diluted water interfaces are determined to be 0.87 ± 0.06 ps (neat H2O), 0.84 ± 0.09 ps (H2O/HOD/D2O = 1/2/1), and 0.88 ± 0.16 ps (H2O/HOD/D2O = 1/8/16). The absence of the isotope effect on the T1 time indicates that the main mechanism of the vibrational relaxation of the free OH is reorientation of the topmost water molecules. The determined sub-picosecond T1 time also suggests that the free OH reorients diffusively without the switching of the hydrogen-bond partner by the topmost water molecule.


1998 ◽  
Vol 276 (11) ◽  
pp. 960-967 ◽  
Author(s):  
F. Monroy ◽  
M. J. Esquinas ◽  
F. Ortega ◽  
R. G. Rubio

2012 ◽  
Vol 116 (31) ◽  
pp. 9467-9481 ◽  
Author(s):  
Ana Vila Verde ◽  
Peter G. Bolhuis ◽  
R. Kramer Campen

2000 ◽  
pp. 769-770 ◽  
Author(s):  
David J. Plaut ◽  
Kristian M. Lund ◽  
Michael D. Ward

Author(s):  
Randall W. Smith ◽  
John Dash

The structure of the air-water interface forms a boundary layer that involves biological ,chemical geological and physical processes in its formation. Freshwater and sea surface microlayers form at the air-water interface and include a diverse assemblage of organic matter, detritus, microorganisms, plankton and heavy metals. The sampling of microlayers and the examination of components is presently a significant area of study because of the input of anthropogenic materials and their accumulation at the air-water interface. The neustonic organisms present in this environment may be sensitive to the toxic components of these inputs. Hardy reports that over 20 different methods have been developed for sampling of microlayers, primarily for bulk chemical analysis. We report here the examination of microlayer films for the documentation of structure and composition.Baier and Gucinski reported the use of Langmuir-Blogett films obtained on germanium prisms for infrared spectroscopic analysis (IR-ATR) of components. The sampling of microlayers has been done by collecting fi1ms on glass plates and teflon drums, We found that microlayers could be collected on 11 mm glass cover slips by pulling a Langmuir-Blogett film from a surface microlayer. Comparative collections were made on methylcel1ulose filter pads. The films could be air-dried or preserved in Lugol's Iodine Several slicks or surface films were sampled in September, 1987 in Chesapeake Bay, Maryland and in August, 1988 in Sequim Bay, Washington, For glass coverslips the films were air-dried, mounted on SEM pegs, ringed with colloidal silver, and sputter coated with Au-Pd, The Langmuir-Blogett film technique maintained the structure of the microlayer intact for examination, SEM observation and EDS analysis were then used to determine organisms and relative concentrations of heavy metals, using a Link AN 10000 EDS system with an ISI SS40 SEM unit. Typical heavy microlayer films are shown in Figure 3.


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