Fourier-Hankel-Abel Nyquist-limited tomography: A spherical harmonic basis function approach to tomographic velocity-map image reconstruction.

A new method for the fully generalized reconstruction of three-dimensional (3D) photoproduct distributions from velocity-map imaging (VMI) projection data is presented. This approach, dubbed Fourier-Hankel-Abel Nyquist-limited TOMography (FHANTOM), builds on recent previous work in tomographic image reconstruction [C. Sparling and D.

The importance of molecular axis alignment and symmetry-breaking in photoelectron elliptical dichroism.

Photoelectron angular distributions (PADs) produced from the photoionization of chiral molecules using elliptically polarized light exhibit a forward/backward asymmetry with respect to the optical propagation direction. By recording these distributions using the velocity-map imaging (VMI) technique, the resulting photoelectron elliptical dichroism (PEELD) has previously been demonstrated as a promising spectroscopic tool for studying chiral molecules in the gas phase. The use of elliptically polarized laser pulses, however, produces PADs (and consequently, PEELD distributions) that do not exhibit cylindrical symmetry about the propagation axis.

Velocity-map imaging of photoelectron circular dichroism in non-volatile molecules using a laser-based desorption source.

We present an initial demonstration of a velocity-map imaging (VMI) experiment using a back-irradiation laser-based desorption source directly integrated into the electrode assembly. This has the potential to greatly expand the utility of the popular VMI approach by permitting its use with high density plumes of non-volatile molecular samples. Photoelectron circular dichroism measurements on the phenylalanine molecule using 400 nm multiphoton ionization are used to illustrate this novel method, revealing forward-backward emission asymmetries on the order of 7%.

Tomographic reconstruction techniques optimized for velocity-map imaging applications.

Examples of extracting meaningful information from image projection data using tomographic reconstruction techniques can be found in many areas of science. Within the photochemical dynamics community, tomography allows for complete three-dimensional (3D) charged particle momentum distributions to be reconstructed following a photodissociation or photoionization event. This permits highly differential velocity- and angle-resolved measurements to be made simultaneously.

Arbitrary image reinflation: A deep learning technique for recovering 3D photoproduct distributions from a single 2D projection.

Many charged particle imaging measurements rely on the inverse Abel transform (or related methods) to reconstruct three-dimensional (3D) photoproduct distributions from a single two-dimensional (2D) projection image. This technique allows for both energy- and angle-resolved information to be recorded in a relatively inexpensive experimental setup, and its use is now widespread within the field of photochemical dynamics. There are restrictions, however, as cylindrical symmetry constraints on the overall form of the distribution mean that it can only be used with a limited range of laser polarization geometries.

Artificial Neural Networks for Noise Removal in Data-Sparse Charged Particle Imaging Experiments.

We present the first demonstration of artificial neural networks (ANNs) for the removal of Poissonian noise in charged particle imaging measurements with very low overall counts. The approach is successfully applied to both simulated and real experimental image data relating to the detection of photoions/photoelectrons in unimolecular photochemical dynamics studies. Specific examples consider the multiphoton ionization of pyrrole and (S)-camphor.