The double photoionization of a molecule by one photon ejects two electrons and typically creates an unstable dication. Observing the subsequent fragmentation products in coincidence can reveal a surprisingly detailed picture of the dynamics. Determining the time evolution and quantum mechanical states involved leads to deeper understanding of molecular dynamics. Here in a combined experimental and theoretical study, we unambiguously separate the sequential breakup via D + + OD + intermediates, from other processes leading to the same D + + D + + O final products of double ionization of water by a single photon. Moreover, we experimentally identify, separate, and follow step by step, two pathways involving the b 1 Σ + and a 1 Δ electronic states of the intermediate OD + ion. Our classical trajectory calculations on the relevant potential energy surfaces reproduce well the measured data and, combined with the experiment, enable the determination of the internal energy and angular momentum distribution of the OD + intermediate.

Science and Engineering (S&E) fairs are a valuable educational activity and are believed to increase students' engagement and learning in science and engineering. However, due to differences in resources, many schools do not implement fairs to achieve these benefits for their students. This study reports the findings of a program intended to increase the participation of students from low-achieving and under-resourced schools in a regional fair program that feeds into the international fair competition. We found that the number of schools and projects participating in our regional fair increased dramatically since the start of the program. Teachers had mostly positive expectations for the project and expressed buy-in for the effort the project would take. They recruited a diverse pool of students to participate in the school fairs. Quasi-experimental methods allowed us to explore the impact of completing S&E fairs on student gains on science self-efficacy, interest and value perceptions. Controlling for pre-existing differences in these attitudes, we found that students not completing projects showed declines in their science attitudes during the year. Students who completed projects maintained similar attitudes, while those whose projects advanced to the regional fair had substantial gains on all three variables. It is unknown whether this gain can be attributed to the experience of engaging with a quality project, from being the kind of student who completes a quality project, or some other factor. Future research with greater experimental control could address these questions.

We report measurements on the H^{+}+H^{+} fragmentation channel following direct single-photon double ionization of neutral NH_{3} at 61.5 eV, where the two photoelectrons and two protons are measured in coincidence using three-dimensional (3D) momentum imaging. We identify four dication electronic states that contribute to H^{+}+H^{+} dissociation, based on our multireference configuration-interaction calculations of the dication potential energy surfaces. The extracted branching ratios between these four dication electronic states are presented. Of the four dication electronic states, three dissociate in a concerted process, while the fourth undergoes a sequential fragmentation mechanism. We find evidence that the neutral NH fragment or intermediate NH^{+} ion is markedly rovibrationally excited. We also identify differences in the relative emission angle between the two photoelectrons as a function of their energy sharing for the four different dication states, which bare some similarities to previous observations made on atomic targets.

We present state-selective measurements on the NH_2^+ + H^+ and NH^+ + H^+ + H dissociation channels following single-photon double ionization at 61.5 eV of neutral NH_3, where the two photoelectrons and two cations are measured in coincidence using 3-D momentum imaging. Three dication electronic states are identified to contribute to the NH_2^+ + H^+ dissociation channel, where the excitation in one of the three states undergoes intersystem crossing prior to dissociation, producing a cold NH_2^+ fragment. In contrast, the other two states directly dissociate, producing a ro-vibrationally excited NH_2^+ fragment with roughly 1 eV of internal energy. The NH^+ + H^+ + H channel is fed by direct dissociation from three intermediate dication states, one of which is shared with the NH_2^+ + H^+ channel. We find evidence of autoionization contributing to each of the double ionization channels. The distributions of the relative emission angle between the two photoelectrons, as well as the relative angle between the recoil axis of the molecular breakup and the polarization vector of the ionizing field, are also presented to provide insight on both the photoionization and photodissociation mechanisms for the different dication states.

The authors reveal how the emitted photoelectron influences the localization process of the remaining electron in a dissociating diatomic molecular cation upon single photo ionization via retroactive Coulomb interaction. The dependence of the asymmetric photoelectron emission pattern in the molecular frame on the kinetic energy release of the heavy fragments and the electron energy is studied.

We present a combined experimental and theoretical investigation of the electron dynamics and body-frame angular dependence of valence photo-single ionization of CF4 and subsequent dissociation into CF3+ and F. Ionization from a valence t2 orbital shows overlapping shape resonances close to threshold that couple to the same total symmetry, leading to striking changes in the photoelectron angular distributions when viewed in the body-frame.

A dramatic symmetry breaking in K-shell photoionization of the CF4 molecule in which a core-hole vacancy is created in one of four equivalent fluorine atoms is displayed in the molecular frame angular distribution of the photoelectrons. Observing the photoejected electron in coincidence with an F+ atomic ion after Auger decay is shown to select the dissociation path where the core hole was localized almost exclusively on that atom. A combination of measurements and ab initio calculations of the photoelectron angular distribution in the frame of the recoiling CF3+ and F+ atoms elucidates the underlying physics that derives from the Ne-like valence structure of the F(1s(-1)) core-excited atom.