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An experimental continuous-wave (cw) pump–probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. In particular, 6Li atoms are initially prepared in optically pumped 22S1/2 and 22P3/2 states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods, such as standard cold-target recoil ion momentum spectroscopy or velocity map imaging, cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron–recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation. 

Abstract On 2022 February 15–16, multiple spacecraft measured one of the most intense solar energetic particle (SEP) events observed so far in Solar Cycle 25. This study provides an overview of interesting observations made by multiple spacecraft during this event. Parker Solar Probe (PSP) and BepiColombo were close to each other at 0.34–0.37 au (a radial separation of ∼0.03 au) as they were impacted by the flank of the associated coronal mass ejection (CME). At about 100° in the retrograde direction and 1.5 au away from the Sun, the radiation detector on board the Curiosity surface rover observed the largest ground-level enhancement on Mars since surface measurements began. At intermediate distances (0.7–1.0 au), the presence of stream interaction regions (SIRs) during the SEP arrival time provides additional complexities regarding the analysis of the distinct contributions of CME-driven versus SIR-driven events in observations by spacecraft such as Solar Orbiter and STEREO-A, and by near-Earth spacecraft like ACE, SOHO, and WIND. The proximity of PSP and BepiColombo also enables us to directly compare their measurements and perform cross-calibration for the energetic particle instruments on board the two spacecraft. Our analysis indicates that energetic proton measurements from BepiColombo and PSP are in reasonable agreement with each other to within a factor of ∼1.35. Finally, this study introduces the various ongoing efforts that will collectively improve our understanding of this impactful, widespread SEP event. 

Abstract. Photoacoustic spectroscopy (PAS) has become a popular technique for measuringabsorption of light by atmospheric aerosols in both the laboratory andfield campaigns. It has low detection limits, measures suspended aerosols,and is insensitive to scattering. But PAS requires rigorous calibration to beapplied quantitatively. Often, a PAS instrument is either filled with a gasof known concentration and absorption cross section, such that the absorptionin the cell can be calculated from the product of the two, or the absorptionis measured independently with a technique such as cavity ring-downspectroscopy. Then, the PAS signal can be regressed upon the known absorptionto determine a calibration slope that reflects the sensitivity constant ofthe cell and microphone. Ozone has been used for calibrating PAS instrumentsdue to its well-known UV–visible absorption spectrum and the ease with whichit can be generated. However, it is known to photodissociate up toapproximately 1120nm via the O₃ + $h\mathit{\nu }(\>1.1\mathrm{eV})\to {\mathrm{O}}_2{(}^3{\mathrm{\Sigma }}_g^{-})$ + O(³P) pathway, which is likely tolead to inaccuracies in aerosol measurements. Two recent studies haveinvestigated the use of O₃ for PAS calibration but have reachedseemingly contradictory conclusions with one finding that it results in asensitivity that is a factor of 2 low and the other concluding that it isaccurate. The present work is meant to add to this discussion by exploringthe extent to which O₃ photodissociates in the PAS cell and the rolethat the identity of the bath gas plays in determining the PAS sensitivity.We find a 5% loss in PAS signal attributable to photodissociation at 532nmin N₂ but no loss in a 5% mixture of O₂ in N₂.Furthermore, we discovered a dramatic increase of more than a factor of 2in the PAS sensitivity as we increased the O₂ fraction in the bathgas, which reached an asymptote near 100% O₂ that nearly matched thesensitivity measured with both NO₂ and nigrosin particles. Weinterpret this dependence with a kinetic model that suggests the reason forthe observed results is a more efficient transfer of energy from excitedO₃ to O₂ than to N₂ by a factor of 22–55 depending onexcitation wavelength. Notably, the two prior studies on this topic useddifferent bath gas compositions, and although the results presented here donot fully resolve the differences in their results, they may at leastpartially explain them.