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Structural Dynamics of a Catalytic Monolayer Probed by Ultrafast 2D IR Vibrational Echoes.

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Title: Structural Dynamics of a Catalytic Monolayer Probed by Ultrafast 2D IR Vibrational Echoes.
Authors: Rosenfeld, Daniel E., Gengeliczki, Zsolt, Smith, Brian J., Stack, T. D. P., Fayer, M. D.
Source: Science (pre-March 2025). 11/4/2011, Vol. 334 Issue 6056, p634-639. 6p.
Subjects: Structural dynamics, Infrared spectroscopy, Carbonyl compounds, Vibrational spectra, Ultrashort laser pulses, Monomolecular films
Abstract: Ultrafast two-dimensional infrared (2D IR) vibrational echo spectroscopy has proven broadly useful for studying molecular dynamics in solutions. Here, we extend the technique to probing the interfacial dynamics and structure of a silica surface-tethered transition metal carbonyl complex-tricarbonyl (1,10-phenanthroline)rhenium chloride-of interest as a photoreduction catalyst. We interpret the data using a theoretical framework devised to separate the roles of structural evolution and excitation transfer in inducing spectral diffusion. The structural dynamics, as reported on by a carbonyl stretch vibration of the surface-bound complex, have a characteristic time of -150 picoseconds in the absence of solvent, decrease in duration by a factor of three upon addition of chloroform, and decrease another order of magnitude for the bulk solution. Conversely, solvent-complex interactions increase the lifetime of the probed vibration by 160% when solvent is applied to the monolayer. [ABSTRACT FROM AUTHOR]
Copyright of Science (pre-March 2025) is the property of American Association for the Advancement of Science and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
Database: Psychology and Behavioral Sciences Collection
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  Data: Structural Dynamics of a Catalytic Monolayer Probed by Ultrafast 2D IR Vibrational Echoes.
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  Data: <searchLink fieldCode="JN" term="%22Science+%28pre-March+2025%29%22">Science (pre-March 2025)</searchLink>. 11/4/2011, Vol. 334 Issue 6056, p634-639. 6p.
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  Data: <searchLink fieldCode="DE" term="%22Structural+dynamics%22">Structural dynamics</searchLink><br /><searchLink fieldCode="DE" term="%22Infrared+spectroscopy%22">Infrared spectroscopy</searchLink><br /><searchLink fieldCode="DE" term="%22Carbonyl+compounds%22">Carbonyl compounds</searchLink><br /><searchLink fieldCode="DE" term="%22Vibrational+spectra%22">Vibrational spectra</searchLink><br /><searchLink fieldCode="DE" term="%22Ultrashort+laser+pulses%22">Ultrashort laser pulses</searchLink><br /><searchLink fieldCode="DE" term="%22Monomolecular+films%22">Monomolecular films</searchLink>
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  Data: Ultrafast two-dimensional infrared (2D IR) vibrational echo spectroscopy has proven broadly useful for studying molecular dynamics in solutions. Here, we extend the technique to probing the interfacial dynamics and structure of a silica surface-tethered transition metal carbonyl complex-tricarbonyl (1,10-phenanthroline)rhenium chloride-of interest as a photoreduction catalyst. We interpret the data using a theoretical framework devised to separate the roles of structural evolution and excitation transfer in inducing spectral diffusion. The structural dynamics, as reported on by a carbonyl stretch vibration of the surface-bound complex, have a characteristic time of -150 picoseconds in the absence of solvent, decrease in duration by a factor of three upon addition of chloroform, and decrease another order of magnitude for the bulk solution. Conversely, solvent-complex interactions increase the lifetime of the probed vibration by 160% when solvent is applied to the monolayer. [ABSTRACT FROM AUTHOR]
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  Data: <i>Copyright of Science (pre-March 2025) is the property of American Association for the Advancement of Science and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1126/science.1211350
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        Text: English
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      – SubjectFull: Infrared spectroscopy
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      – SubjectFull: Carbonyl compounds
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      – SubjectFull: Vibrational spectra
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      – SubjectFull: Ultrashort laser pulses
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              Text: 11/4/2011
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