Abstract

We have measured the angular distributions of high energy photoelectrons of benzene molecules generated by intense infrared femtosecond laser pulses. These electrons arise from the elastic collisions between the benzene ions with the previously tunnel-ionized electrons that have been driven back by the laser field. Theory shows that laser-free elastic differential cross sections (DCSs) can be extracted from these photoelectrons, and the DCS can be used to retrieve the bond lengths of gas-phase molecules similar to the conventional electron diffraction method. From our experimental results, we have obtained the C-C and C-H bond lengths of benzene with a spatial resolution of about 10 pm. Our results demonstrate that laser induced electron diffraction (LIED) experiments can be carried out with the present-day ultrafast intense lasers already. Looking ahead, with aligned or oriented molecules, more complete spatial information of the molecule can be obtained from LIED, and applying LIED to probe photo-excited molecules, a “molecular movie” of the dynamic system may be created with sub-Ångström spatial and few-ten femtosecond temporal resolutions.

Highlights

  • Imaging the real time evolution of a chemical reaction or a biological function is one of the major frontier research goals in modern science

  • Our results demonstrate that laser induced electron diffraction (LIED) experiments can be carried out with the present-day ultrafast intense lasers already

  • Understanding chemical reactions or biological functions at such a fundamental level would further open up future capabilities for creating conditions to drive the desired chemical processes that lead to favored irreversible chemical products

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Summary

Introduction

Imaging the real time evolution of a chemical reaction or a biological function is one of the major frontier research goals in modern science For such purpose, it requires the development of new tools that are capable of probing molecules with a temporal resolution of a few to tens of femtoseconds and a spatial resolution of a few sub-Angstr€oms.. It requires the development of new tools that are capable of probing molecules with a temporal resolution of a few to tens of femtoseconds and a spatial resolution of a few sub-Angstr€oms.1–3 These tools would enable the observation of changes of molecules near the conical intersection, the presence of transition states, and the ability to follow the dynamics of chemical processes such as proton migration, roaming, and ring opening, to create a “molecular movie” of the motions of atomic constituents.

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