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We present an approach that combines photon spectrum correlation analysis with the reconstruction of three-dimensional momentum distribution from velocity map images in an efficient, single-step procedure. We demonstrate its efficacy with the results from the photoionization of the 2  p -shell of argon using the Free-electron LASer in Hamburg free-electron laser (FEL). Distinct spectral features due to the spin-orbit splitting of Ar + ( 2 p − 1 ) are resolved, despite the large average bandwidth of the ionizing pulses from the FEL. This demonstrates a clear advantage over the conventional analysis method, and it will be broadly beneficial for velocity map imaging experiments with FEL sources. The retrieved linewidth of the binding energy spectrum approaches the resolution limitation prescribed by the spectrometers used to collect the data. Our approach presents a path to extend spectral-domain ghost imaging to the case where the photoproduct observable is high-dimensional.

Pixellated scintillation detectors have the potential to overcome several limitations of conventional microchannel-plate-based detectors employed in time-of-flight mass spectrometry (ToF-MS), such as extending detector lifetime, reducing vacuum requirements, or increasing the ion throughput. We have developed a prototype comprising a fast organic scintillator (Exalite 404) coupled to an array of 16 silicon photomultipliers (SiPMs), with read-out electronics based on the FastIC application-specific integrated circuit (ASIC). Each SiPM signal processed by FastIC is fed into its own time-to-digital converter (TDC). The dead time of a single channel can be as short as ∼20 ns. As a result, our system have the potential to process ion rates above 109 cm−2 s−1. We have evaluated the performance of our prototype using a velocity-map imaging ToF-MS instrument, recording the time-of-flight mass spectra of C3H6 and CF3I samples. We achieved time resolutions of (3.3±0.1) and (2.5±0.2) ns FWHM for ions of mass-to-charge ratio (m/z) values of 196 and 18, respectively. This corresponds to a mass resolution of ∼1000 for m/z<200, which we found to be dominated by the spread in ion arrival times.

Polycyclic aromatic hydrocarbons, in various charge and protonation states, are key compounds relevant to combustion chemistry and astrochemistry. Here, we probe the vibrational and electronic spectroscopy of gas-phase 9-, 1-, and 2-anthracenyl radicals (C14H₉) by photodetachment of the corresponding cryogenically cooled anions via slow photoelectron velocity-map imaging (cryo-SEVI). The use of a newly designed velocity-map imaging lens in combination with ion cooling yields photoelectron spectra with <2 cm−1 resolution. Isomer selection of the anions is achieved using gas-phase synthesis techniques, resulting in observation and interpretation of detailed vibronic structure of the ground and lowest excited states for the three anthracenyl radical isomers. The ground-state bands yield electron affinities and vibrational frequencies for several Franck–Condon active modes of the 9-, 1-, and 2-anthracenyl radicals; term energies of the first excited states of these species are also measured. Spectra are interpreted through comparison with ab initio quantum chemistry calculations, Franck–Condon simulations, and calculations of threshold photodetachment cross sections and anisotropies. Experimental measures of the subtle differences in energetics and relative stabilities of these radical isomers are of interest from the perspective of fundamental physical organic chemistry and aid in understanding their behavior and reactivity in interstellar and combustion environments. Additionally, spectroscopic characterization of these species in the laboratory is essential for their potential identification in astrochemical data.

Internal structure imaging of the Earth, along with determining basin structure, can aid in evaluating potential seismic hazards. However, the high operating cost limits the current geophysical exploration methods; moreover, it is difficult to apply these techniques over a large area, which limits our understanding of the Quaternary structure and the development of earthquake prevention science. A combination of dense array observation technology and ambient noise surface wave tomography is being rapidly developed as a high-resolution urban detection method. Here, we report the ambient noise imaging results of a high-density array experiment. In the ambient noise surface wave tomography method (e.g., surface wave tomography; Eikonal tomography), the signal is assumed to be a single mode. However, several multimode signals were detected in this dataset. With the use of traditional methods to measure the dispersion, mode confusion occurs and the extracted dispersion curve jumps. To solve this problem, by combining the advantages of phase-matched filtering and dispersion compensation, we realized the automatic pickup of fundamental group velocity using reference phase velocity. From this, a Rayleigh wave group velocity map was obtained. The regional average phase velocity information was included in the inversion steps to reduce the uncertainty in the inversion of shear wave velocity. Finally, an S-wave velocity structure model was obtained within a depth of 500 m. The velocity structure was roughly layered and grew with depth. In the depth range of 240–320 m, obvious decreases in the S-wave velocity were observed. Compared with geothermal drilling data, this was speculated to be the reflection of a water-rich (confined water) sand layer. This study provides a technical approach for and a processing example of a high-density array, and its velocity model can be used as a reference for urban subsurface structure, underground space utilization, and earthquake disaster prevention and control.

Computational fluid dynamics (CFD) modelers require high-quality experimental data sets for validation of their numerical tools. Preferred features for numerical simulations of a sooting, turbulent test case flame are simplicity (no pilot flame), well-defined boundary conditions, and sufficient soot production. This paper proposes a non-premixed C2H 4/air turbulent jet flame to fill this role and presents an extensive database for soot model validation. The sooting turbulent jet flame has a total visible flame length of approximately 400 mm and a fuel-jet Reynolds number of 10,000. The flame has a measured lift-off height of 26 mm which acts as a sensitive marker for CFD model validation, while this novel compiled experimental database of soot properties, temperature and velocity maps are useful for the validation of kinetic soot models and numerical flame simulations. Due to the relatively simple burner design which produces a flame with sufficient soot concentration while meeting modelers' needs with respect to boundary conditions and flame specifications as well as the present lack of a sooting \"standard flame\", this flame is suggested as a new reference turbulent sooting flame. The flame characterization presented here involved a variety of optical diagnostics including quantitative 2D laser-induced incandescence (2D-LII), shifted-vibrational coherent anti-Stokes Raman spectroscopy (SV-CARS), and particle image velocimetry (PIV). Producing an accurate and comprehensive characterization of a transient sooting flame was challenging and required optimization of these diagnostics. In this respect, we present the first simultaneous, instantaneous PIV, and LII measurements in a heavily sooting flame environment. Simultaneous soot and flow field measurements can provide new insights into the interaction between a turbulent vortex and flame chemistry, especially since soot structures in turbulent flames are known to be small and often treated in a statistical manner. © 2011 Springer-Verlag.

The velocity map imaging of the methyl radical formed by 266 nm photolysis of methyl iodide using the 213 nm non-resonant multi-photon ionization (NRMPI) method is presented. Comparison of the NRMPI method with the well-known 2+1 resonance enhanced multi-photon ionization (REMPI) method at 333.45 nm, which selectively probes the Q-branch of band-origin transition of the methyl radical, indicates that the NRMPI method yields a significantly higher I/I* branching, even though the velocity map images of both the methods are qualitatively similar. The higher I/I* branching ratio obtained in the NRMPI method is attributed to the non-resonant ionization of higher quanta states of the umbrella bending mode along with higher rotational states of the methyl fragment in the CH 3 +I dissociation channel. Further, photodissociation of the organic molecules yielding photofragments such as NO, CF 3 , CO, and several others could be detected and imaged using a 213 nm probe laser. Thus, results obtained in the present work signify that a 213 nm light source, which is easily available as the fifth harmonic of Nd:YAG laser, can be used as an alternative and efficient probe to investigate photodissociation dynamics of polyatomic molecules. Graphical abstract The utility of 213 nm (fifth harmonic of the Nd:YAG laser) as a universal ionization source in the imaging of several photodissociation products such as NO, CH 3 , CF 3 , CO, and other molecular fragments either via REMPI or NRMPI ionization methods is explored.

Ancient mining and quarrying activities left anthropogenic geomorphologies that have shaped the natural landscape and affected environmental equilibria. The artificial structures and their related effects on the surrounding environment are analyzed here to characterize the quarrying landscape in the southeast area of Rome in terms of its dimensions, typology, state of preservation and interface with the urban environment. The increased occurrence of sinkhole events in urban areas has already been scientifically correlated to ancient cavities under increasing urban pressure. In this scenario, additional interacting anthropogenic factors, such as the aerial bombardments perpetrated during the Second World War, are considered here. These three factors have been investigated by employing a combined geomatic methodology. Information on air raids has been organized in vector archives. A dataset of historical aerial photographs has been processed into Digital Surface Models and orthomosaics to reconstruct the quarry landscape and its evolution, identify typologies of exploitation and forms of collapse and corroborate the discussion concerning the induced historical and recent subsidence phenomena, comparing these outputs with photogrammetric products obtained from recent satellite data. Geological and urbanistic characterization of the study area allowed a better connection between these historical and environmental factors. In light of the information gathered so far, SAR interferometric products allowed a preliminary interpretation of ground instabilities surrounding historical quarries, air raids and recent subsidence events. Various sub-areas of the AOI where the presence of the considered factors also corresponds to areas in slight subsidence in the SAR velocity maps have been highlighted. Bivariate hotspot analysis allowed substantiating the hypothesis of a spatial correlation between these multiple aspects.

In pump-probe experiments employing a free-electron laser (FEL) in combination with a synchronized optical femtosecond laser, the arrival-time jitter between the FEL pulse and the optical laser pulse often severely limits the temporal resolution that can be achieved. Here, we present a pump-probe experiment on the UV-induced dissociation of 2,6-difluoroiodobenzene (C6H3F2I) molecules performed at the FLASH FEL that takes advantage of recent upgrades of the FLASH timing and synchronization system to obtain high-quality data that are not limited by the FEL arrival-time jitter. We discuss in detail the necessary data analysis steps and describe the origin of the time-dependent effects in the yields and kinetic energies of the fragment ions that we observe in the experiment.

A velocity map imaging (VMI) spectrometer to investigate photodissociation dynamics was designed and fabricated. This spectrometer combines a skimmed molecular beam with a multi-stage time-of-flight mass spectrometer equipped with position-sensitive detection. Investigations on the 266 nm photodissociation of o-xylene leading to sp2C–Csp3 bond cleavage resulting in CH3 and C6H4CH3 fragments reveal that the kinetic energy partitioning in the centre-of-mass frame is almost identical in both the fragments indicating a single dissociation mechanism with CH3 radical produced almost exclusively in the ν = 0 level of the ground electronic state. The weakening of the sp2C–Csp3 bond by about 17 kcal mol−1 in the cationic ground state relative to the neutral ground state of o-xylene facilitates the dissociation, propelled by the three-photon absorption process.Graphic abstractA velocity map imaging (VMI) spectrometer to investigate photodissociation dynamics was designed and fabricated. This spectrometer combines a skimmed molecular beam with a multi-stage time-of-flight mass spectrometer equipped with position-sensitive detection.

Chemical reaction dynamics and, particularly, photodissociation in the gas phase are generally studied using pump-probe schemes where a first laser pulse induces the process under study and a second one detects the produced fragments. Providing an efficient detection of ro-vibrationally state-selected photofragments, the resonance enhanced multiphoton ionization (REMPI) technique is, without question, the most popular approach used for the probe step, while non-resonant multiphoton ionization (NRMPI) detection of the products is scarce. The main goal of this work is to test the sensitivity of the NRMPI technique to fragment vibrational distributions arising from molecular photodissociation processes. We revisit the well-known process of methyl iodide photodissociation in the A-band at around 280 nm, using the velocity-map imaging technique in conjunction with NRMPI of the methyl fragment. The detection wavelength, carefully selected to avoid any REMPI transition, was scanned between 325 and 335 nm seeking correlations between the different observables—the product vibrational, translational and angular distributions—and the excitation wavelength of the probe laser pulse. The experimental results have been discussed on the base of quantum dynamics calculations of photofragment vibrational populations carried out on available ab initio potential-energy surfaces using a four-dimensional model. This article is part of the themed issue 'Theoretical and computational studies of nonequilibrium and non-statistical dynamics in the gas phase, in the condensed phase and at interfaces'.