The "pixel imaging mass spectrometry" camera is used to perform femtosecond laser-induced Coulomb explosion imaging of 3,5-dibromo-3 ,5-difluoro-4-cyanobiphenyl molecules prealigned in space. The experiment allows the concurrent detection of the correlated two-dimensional momentum images of all the ionic fragments resulting from fragmentation of multiple molecules in each acquisition cycle. The Coulomb explosion studies provide rich information about the parent molecular structure and fragmentation dynamics, and open new opportunities for real-time imaging of intramolecular processes.

The torsional motion of a molecule composed of two substituted benzene rings, linked by a single bond, is coherently controlled by a pair of strong (3×10^{13}  W cm^{-2}), nonresonant (800 nm) 200-fs-long laser pulses-both linearly polarized perpendicular to the single-bond axis. If the second pulse is sent at the time when the two benzene rings rotate toward (away from) each other the amplitude of the torsion is strongly enhanced (reduced). The torsional motion persists for more than 150 ps corresponding to approximately 120 torsional oscillations. Our calculations show that the key to control is the strong transient modification of the natural torsional potential by the laser-induced dynamic Stark effect.

Femtosecond laser-induced Coulomb-explosion imaging of 3,5-dibromo-3 ,5-difluoro-4-cyanobiphenyl molecules prealigned in space is explored using a pixel-imaging mass-spectrometry (PImMS) camera. The fast-event-triggered camera allows the concurrent detection of the correlated two-dimensional momentum images, or covariance maps, of all the ionic fragments resulting from fragmentation of multiple molecules in each acquisition cycle. Detailed simulation of the covariance maps reveals that they provide rich information about the parent molecular structure and fragmentation dynamics. Future opportunities for imaging the real-time dynamics of intramolecular processes are considered.

The development of sensors capable of detecting particles and radiation with both high time and high positional resolution is key to improving our understanding in many areas of science. Example applications of such sensors range from fundamental scattering studies of chemical reaction mechanisms through to imaging mass spectrometry of surfaces, neutron scattering studies aimed at probing the structure of materials, and time-resolved fluorescence measurements to elucidate the structure and function of biomolecules. In addition to improved throughput resulting from parallelisation of data collection - imaging of multiple different fragments in velocity-map imaging studies, for example - fast image sensors also offer a number of fundamentally new capabilities in areas such as coincidence detection. In this Perspective, we review recent developments in fast image sensor technology, provide examples of their implementation in a range of different experimental contexts, and discuss potential future developments and applications.

We report on 'proof of concept' experiments in Pixel Imaging Mass Spectrometry (PImMS) using an ultra-fast frame-transfer CCD camera and also describe an intelligent CMOS sensor which is being developed for this application by the PImMS collaboration in the UK. PImMS is a combination of traditional TOF mass spectrometry and ion imaging. Information provided by the ion imaging gives access to valuable structural information of the molecule under investigation, in addition to the normal mass spectrum. Recording of the 2D spatial information of the arriving ions allows to reconstruct the ion velocity distributions for separate ion masses and to correlate them to each other. The new PImMS sensor will be capable of time stamping up to four arriving ions per pixel during the 200 µsec acquisition cycle with 100 nsec resolution which should meet the demanding requirements of complete recording of mass spectra of complex organic molecules.