Thomas J. Preston, Michael A. Shaloski, and F. Fleming Crim Infrared Transient Absorption Spectroscopy of Bromoform Isomerization.

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Presentation transcript:

Thomas J. Preston, Michael A. Shaloski, and F. Fleming Crim Infrared Transient Absorption Spectroscopy of Bromoform Isomerization

Isomerization of Halomethanes Preston et al. J. Chem. Phys. 2011, 135,

Potential Energy Surface for Isomerization Preston et al. J. Chem. Phys. 2011, 135,

Bromoform Isomerization Carrier et al. J. Phys. Chem. A. 2010, 114, 1548

Infrared Probing (Matrix Studies) George et al. J. Chem. Phys. 2011, 135, Mode Description Transition Frequency in cm -1 CHBr 3 C-H Stretch3051 iso-CHBr 2 -BrC-H Stretch3076

Infrared Probing (Time-Resolved) Transition Frequency in cm -1 IR Bleach3027 IR Absorbance3052

Infrared Probing (Time-Resolved) Feature τ 1 τ 2 IR Bleach5.3±2.622±7 IR Absorbance9.0±0.698± nm Absorbance19±1.0124±44

Assignments George et al. J. Chem. Phys. 2011, 135,

Early Feature Assignment Time-Dependent DFT -M06-2x functional -Sadlej-pVTZ basis set Species / nm  / M -1 cm -1 Br--CHBr Br--CHBr CHBr 3 --Br--CHBr CHBr 3 --Br--CHBr Chromophore should be dependent on bromoform concentration

Dilution Study Repeated 267 pump, 350 – 700 nm probe -Varied concentration from 100% – 2% bromoform -Normalized 1 ns signals -Scaled 2 ps signal by same factor

Summary IR Results Photolysis leads to prompt bleach in C-H region of bromoform Absorption feature of iso-bromoform appears with a characteristic time of 9.0 ps Lasts > 1 ns UV/Visible Results 490 feature assigned to isomer 390 feature assigned to Br – CHBr 3 contact pair Electronic structure calc. Dilution experiment

Acknowledgements NSF Funding Crim Group Fleming Crim Thomas J. Preston Collaborators Bob McMahon Scott Reid Ned Sibert