期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 111, 期 52, 页码 18442-18447出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1422194112
关键词
2D IR spectroscopy; metal-organic framework; UiO-66 MOF; ultrafast structural fluctuations; solvent confinement effect
资金
- Stanford Graduate Fellowships
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy (DOE) [DE-FG03-84ER13251]
- Air Force Office of Scientific Research (AFOSR) [FA9550-12-1-0050]
- AFOSR
- DOE
- National Science Foundation, Division of Materials Research [DMR-1262226]
- Swedish Research Council
- Swedish Energy Agency
- Knut and Alice Wallenberg Foundation
The structural elasticity of metal-organic frameworks (MOFs) is a key property for their functionality. Here, we show that 2D IR spectroscopy with pulse-shaping techniques can probe the ultrafast structural fluctuations of MOFs. 2D IR data, obtained from a vibrational probe attached to the linkers of UiO-66 MOF in low concentration, revealed that the structural fluctuations have time constants of 7 and 670 ps with no solvent. Filling the MOF pores with dimethylformamide (DMF) slows the structural fluctuations by reducing the ability of the MOF to undergo deformations, and the dynamics of the DMF molecules are also greatly restricted. Methodology advances were required to remove the severe light scattering caused by the macroscopic-sizedMOF particles, eliminate interfering oscillatory components from the 2D IR data, and address Forster vibrational excitation transfer.
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