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| 概要 |
We explore laboratory-frame photoelectron angular distributions (LF-PADs) originating from the outermost two orbitals, σ_u [the highest occupied molecular orbital (HOMO)] and σ_g (HOMO−1), of the silv...er trimer anion (Ag_3^−) in the S_0(^1Σ_g^+) state. The experiment was performed by our novel photoelectron imaging technique using a high-repetition-rate tunable laser [T. Horio et al., J. Chem. Phys. 162, 026101 (2025)]. The LF-PAD for σ_u is found to be highly energy-dependent in a photoelectron kinetic energy (PKE) range from 0 to 1.57 eV; an isotropic LF-PAD with an anisotropy parameter β ∼ 0 is observed at the detachment threshold, exemplifying the Wigner threshold law, whereas the β value decreases down to β = −0.4 at 0.46 eV, followed by an increase up to β = 0.6 at 1.57 eV, as PKE increases. A small dip discernible in the PKE range of 1.2–1.3 eV suggests an influence of the autodetachment process on the β value, which is via bound electronic state(s) embedded in the D_0(^2Σ_u^+) + e^− continuum. On the other hand, the LF-PAD for σ_g exhibits a strong anisotropy parallel to the laser polarization with β of ∼1 in 0–0.39 eV. These contrasted trends are qualitatively reproduced by theoretical modeling of LF-PAD that accounts for photoelectron partial waves allowed for each photodetachment process. Furthermore, two-photon detachment spectra via the excited S_1(^1Σ_u^+) state are presented, where the relative band intensities for the two detachment channels, D_0(^2Σ_u^+) + e^− ← S_1(^1Σ_u^+) and D_1(^2Σ_g^+) + e^− ← S_1(^1Σ_u^+), are discussed in terms of their leading electronic configurations.続きを見る
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Mendeley出力
7420557_AM