Abstract
Electron momentum spectroscopy is a unique tool for imaging orbital-specific electron density of molecule in momentum space. However, the molecular geometry information is usually veiled due to the single-centered character of momentum space wavefunction of molecular orbital (MO). Here we demonstrate the retrieval of interatomic distances from the multicenter interference effect revealed in the ratios of electron momentum profiles between two MOs with symmetric and anti-symmetric characters. A very sensitive dependence of the oscillation period on interatomic distance is observed, which is used to determine F-F distance in CF4 and O-O distance in CO2 with sub-Ångström precision. Thus, using one spectrometer, and in one measurement, the electron density distributions of MOs and the molecular geometry information can be obtained simultaneously. Our approach provides a new robust tool for imaging molecules with high precision and has potential to apply to ultrafast imaging of molecular dynamics if combined with ultrashort electron pulses in the future.
Highlights
IntroductionA very sensitive dependence of the oscillation interference pattern on the interatomic F-F distance is expected, as shown in Fig. 1c by the clear shift in fringe maximum by about 0.15 a.u. for small changes of 0.1 Å in RFF
We demonstrate a robust method for the retrieval of the interatomic distances from the multicenter interference effect of molecules with EMS
A sensitive dependence of the oscillation period on the interatomic distance is observed in the ratios of electron momentum profiles between two MOs with oscillations in antiphase
Summary
A very sensitive dependence of the oscillation interference pattern on the interatomic F-F distance is expected, as shown in Fig. 1c by the clear shift in fringe maximum by about 0.15 a.u. for small changes of 0.1 Å in RFF This dependence may provide a means of accurate determination of molecular geometries with sub-Ångström precision. The present observation of interference effect totally depends on the experimental measurements and does not rely on the comparison with the one-center atomic cross section These features make our approach a robust tool for imaging molecules with high precision and has the potential to apply to ultrafast imaging of molecular dynamics if combined with the ultrashort electron pulses[43] in the future
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