Slicing Newton spheres with a two-camera 3D imaging system

Ranathunga, Yasashri; Olowolafe, Temitayo; Orunesajo, Emmanuel; Musah, Hackim; Lee, Suk Kyoung; Li, Wen

doi:10.1063/5.0151048

The Journal of Chemical Physics

2023

DOI: 10.1063/5.0151048

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Slicing Newton spheres with a two-camera 3D imaging system

Yasashri Ranathunga,

Temitayo Olowolafe,

Emmanuel Orunesajo

et al.

Abstract: We demonstrate a simple approach to achieve three-dimensional ion momentum imaging. The method employs two complementary metal–oxide–semiconductor cameras in addition to a standard microchannel plates/phosphor screen imaging detector. The two cameras are timed to measure the decay of luminescence excited by ion hits to extract the time of flight. The achieved time resolution is better than 10 ns, which is mainly limited by camera jitters. A better than 5 ns resolution can be achieved when the jitter is suppres… Show more

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Cited by 3 publications

References 38 publications

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

Sparling,

Ruget,

Ireland

et al. 2023

The Journal of Chemical Physics

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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. This leads to significant limitations and challenges when employing conventional VMI acquisition and data processing strategies. Using novel photoelectron image analysis methods based around Hankel transform reconstruction tomography and machine learning, however, we have quantified—for the first time—significant symmetry-breaking contributions to PEELD signals that are of a comparable magnitude to the symmetric terms in the multiphoton ionization of (1R,4R)-(+)- and (1S,4S)-(−)-camphor. This contradicts any assumptions that symmetry-breaking can be ignored when reconstructing VMI data. Furthermore, these same symmetry-breaking terms are expected to appear in any experiment where circular and linear laser fields are used together. This ionization scheme is particularly relevant for investigating dynamics in chiral molecules, but it is not limited to them. Developing a full understanding of these terms and the role they play in the photoionization of chiral molecules is of clear importance if the potential of PEELD and related effects for future practical applications is to be fully realized.

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

Sparling,

Ruget,

Ireland

et al. 2023

The Journal of Chemical Physics

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

Sparling,

Rajak,

Blanchet

et al. 2024

Review of Scientific Instruments

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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. Townsend, J. Chem. Phys. 157, 114201 (2022)] and takes advantage of the fact that the distributions produced in typical VMI experiments can be simply described as a sum over a small number of spherical harmonic functions. Knowing the solution is constrained in this way dramatically simplifies the reconstruction process and leads to a considerable reduction in the number of projections required for robust tomographic analysis. Our new method significantly extends basis set expansion approaches previously developed for the reconstruction of photoproduct distributions possessing an axis of cylindrical symmetry. FHANTOM, however, can be applied generally to any distribution—cylindrically symmetric or otherwise—that can be suitably described by an expansion in spherical harmonics. Using both simulated and real experimental data, this new approach is tested and benchmarked against other tomographic reconstruction strategies. In particular, the reconstruction of photoelectron angular distributions recorded in a strong-field ionization regime—marked by their extensive expansion in terms of spherical harmonics—serves as a key test of the FHANTOM methodology. With the increasing use of exotic optical polarization geometries in photoionization experiments, it is anticipated that FHANTOM and related reconstruction techniques will provide an easily accessible and relatively low-cost alternative to more advanced 3D-VMI spectrometers.

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A multi-mass and multi-hit two-camera 3D ion momentum imaging system

Orunesajo,

Abubakar,

Oguh

et al. 2024

Review of Scientific Instruments

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We demonstrate an improved two-camera system for multi-mass and multi-hit three-dimensional (3D) momentum imaging of ions. The imaging system employs two conventional complementary metal–oxide–semiconductor cameras. We have shown previously that the system can time slice ion Newton spheres with a time resolution of 8.8 ns, limited by camera timing jitter [J. Chem. Phys., 158, 191104 (2023)]. In this work, a jitter correction method was developed to suppress the camera jitter and improve the time resolution to better than 2 ns. With this resolution, full 3D momentum distributions of ions can be obtained. We further show that this method can detect two ions with different masses when utilizing both the rising and falling edges of the cameras.

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Slicing Newton spheres with a two-camera 3D imaging system

Cited by 3 publications

References 38 publications

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

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

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

A multi-mass and multi-hit two-camera 3D ion momentum imaging system

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