Tracking Ultrafast Bond Dissociation Dynamics at 0.1 Å Resolution by Femtosecond Extreme Ultraviolet Absorption Spectroscopy

The Journal of Physical Chemistry Letters
Zhengrong WeiZhi-Heng Loh

Abstract

Visualizing the real-time dissociation of chemical bonds represents a challenge in the study of ultrafast molecular dynamics due to the simultaneous need for sub-angstrom spatial and femtosecond temporal resolution. Here, we follow the C-I dissociation dynamics of strong-field-ionized 2-iodopropane (2-C3H7I) with femtosecond extreme ultraviolet (XUV) absorption spectroscopy. By probing the iodine 4 d core-level absorption, we resolve a continuous XUV spectral shift on the sub-100 fs time scale that accompanies the dissociation of the 2-C3H7I+ spin-orbit-excited 2 E1/2 state to yield atomic I in the 2 P3/2 state. In combination with ab initio calculations of the C-I distance-dependent XUV transition energy, we reconstruct the temporal evolution of the C-I distance from the Franck-Condon region to the asymptotic region with 10 fs and 0.1 Å resolution. The C-I bond elongation appears to couple to coherent vibrational motion along the HC(CH3)2 umbrella mode of the 2-C3H7+ fragment, whose effect on the I 4 d XUV transition even at C-I distances of 3.5 Å points to the long-range nature of XUV absorption probing. Our results suggest that femtosecond XUV absorption spectroscopy, in combination with ab initio simulations of XUV transiti...Continue Reading

References

Jun 30, 2007·The Journal of Chemical Physics·Aleksey B AlekseyevSergei N Yurchenko
Dec 7, 2007·The Journal of Chemical Physics·Dominik GeisslerThomas Weinacht
Jan 15, 2014·Physical Chemistry Chemical Physics : PCCP·María E CorralesAhmed H Zewail
Jan 17, 2013·The Journal of Physical Chemistry Letters·Zhi-Heng Loh, Stephen R Leone
May 18, 2016·Physical Chemistry Chemical Physics : PCCP·Adam S ChatterleyOliver Gessner
Apr 8, 2017·Science·Andrew R AttarStephen R Leone
Jul 26, 2017·The Journal of Physical Chemistry Letters·Yao ZhangPeter M Weber
Oct 31, 2017·Journal of the American Chemical Society·Aditi BhattacherjeeStephen R Leone

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Citations

Nov 30, 2019·The Journal of Chemical Physics·Yuki KobayashiStephen R Leone

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