Double-slit experiment with a polyatomic molecule: vibrationally resolved C 1s photoelectron spectra of acetylene

作者：Argenti L; Thomas T D; Plesiat E; Liu X J; Miron C; Lischke T; Pruemper G; Sakai K; Ouchi T; Puettner R; Sekushin V; Tanaka T; Hoshino M; Tanaka H; Decleva P; Ueda K^*; Martin F

来源：New Journal of Physics, 2012, 14(3): 033012.

DOI：10.1088/1367-2630/14/3/033012

We report the first evidence for double-slit interferences in a polyatomic molecule, which we have observed in the experimental carbon 1s photoelectron spectra of acetylene (or ethyne). The spectra have been measured over the photon energy range of 310-930 eV and show prominent oscillations in the intensity ratios sigma(g)(upsilon)/sigma(u)(upsilon) for the vibrational quantum numbers upsilon = 0, 1 and for the ratios sigma(s)(upsilon = 1)/sigma(s)(upsilon = 0) for the symmetry s = g, u. The experimental findings are in very good agreement with ab initio density functional theory (DFT) calculations and are compatible with the Cohen-Fano mechanism of coherent emission from two equivalent atomic centers. This interpretation is supported by the qualitative predictions of a simple model in which the effect of nuclear recoil is taken into account to the lowest order. Our results confirm the delocalized character of the core hole created in the primary photoionization event and demonstrate that intramolecular core-hole coherence can survive the decoherent influence associated with the asymmetric nuclear degrees of freedom which are characteristic of polyatomic molecules.

• 出版日期2012-3-12