We present an experimental and theoretical study of photoexcitation and decay mechanisms of doubly excited resonances in neon. New spin-orbit induced effects are identified in the angleresolved and photoelectron-resolved differential cross sections for a parity-unfavored transition. These observations are facilitated using a two-dimensional imaging technique, and highlight the importance of considering spin-orbit induced effects when studying detailed spectra in atomic systems as light as neon.[S0031-9007(98)06291-7] PACS numbers: 32.80.Fb, 31.50. + w, 32.80.Dz The simultaneous excitation of two atomic electrons by a single photon has been the subject of numerous experimental and theoretical investigations. These intermediate resonance states reveal higher-order, interelectron correlation effects, and provide a more stringent testing ground for the accuracy of existing theoretical and computational methods. Helium, due to its relative simplicity, has been studied extensively [1]. The case of neon, however, is more complicated than helium due to the occupied 2p subshell, which leads to a dense grouping of the Ne 1 2p 4 nl states and hence more complex resonances. Nevertheless, many studies have been performed on this system as well, and some have observed spin-orbit effects. Early photoabsorption results demonstrated departure from LScoupling predictions (i.e., the neglect of spin-orbit effects), by observing the fine-structure splittings of the 2p 4 ͑ 3 P͒3s͑ 2 P 1͞2,3͞2 ͒nl resonances [2]. Later measurements [3][4][5] were able to observe additional spin-orbit effects by detecting resonance contributions in the photoionization excitation to quartet ionic states, which is a forbidden process in LS coupling. More recently, the fine-structure splitting of resonance series was observed in greater detail [6] than was possible in the earlier studies [2]. These results established the existence of certain spin-orbit effects in the photoionization of neon, but they lacked additional information provided by highly differential measurements. Furthermore, in the earlier cases, only small spin-orbit corrections were observed.The purpose of the present Letter is to demonstrate that for certain neon resonances, the angular distribution of photoelectrons and the ratio of partial cross sections to individual fine-structure levels both exhibit behavior that deviates markedly from LS-coupling predictions. Such observations provide further quantitative determination of the breakdown of LS coupling. Particular attention will be given to the 2p 4 3pns, nd doubly excited resonances in photoionization excitation to the Ne 1 2p 4 ͑ 3 P͒3s͑ 2 P͒ state. These findings were achieved using high-resolution measurements of photoionization cross sections that are differential in photon energy, photoelectron energy, and photoelectron angle.The 2p 4 3pns, nd resonances are particularly strong because the ϳ10% mixing of the 2p 5 3p configuration in the 2p 6 ground state leads to the one-electron photoexcitation 2p 5 3p ! 2p 4 3pns, nd [6]. Br...