PImMS, or Pixel Imaging Mass Spectrometry, is a novel high-speed monolithic CMOS imaging sensor tailored to mass spectrometry requirements, also suitable for other dark-field applications. In its application to time-of-flight mass spectrometry, the sensor permits ion arrival time distributions to be combined with 2D imaging, providing additional information about the initial position or velocity of ions under study. PImMS1, the first generation sensor in this family, comprises an array of 72 by 72 pixels on a 70 µm by 70 µm pitch. Pixels independently record digital timestamps when events occur over an adjustable threshold. Each pixel contains 4 memories to record timestamps at a resolution of 25 ns. The sensor was designed and manufactured in the IN-MAPS 0.18 µm process. This allows the inclusion of significant amounts of circuitry (over 600 transistors) within each pixel while maintaining good detection efficiency. We present an overview of the pixel and sensor architecture, explain its functioning and present test results, ranging from characterisation of the analogue front end of the pixel, to verification of its digital functions, to some first images captured on mass spectrometers. We conclude with an overview of the upcoming second generation of PImMS sensors.

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.

Imaging mass spectrometry is a powerful technique that allows chemical information to be correlated to a spatial coordinate on a sample. By using stigmatic ion microscopy, in conjunction with fast cameras, multiple ion masses can be imaged within a single experimental cycle. This means that fewer laser shots and acquisition cycles are required to obtain a full data set, and samples suffer less degradation as overall collection time is reduced. We present the first spatial imaging mass spectrometry results obtained with a new time-stamping detector, named the pixel imaging mass spectrometry (PImMS) sensor. The sensor is capable of storing multiple time stamps in each pixel for each time-of-flight cycle, which gives it multi-mass imaging capabilities within each pixel. A standard velocity-map ion imaging apparatus was modified to allow for microscope mode spatial imaging of a large sample area (approximately 5 × 5 mm(2)). A variety of samples were imaged using PImMS and a conventional camera to determine the specifications and possible applications of the spectrometer and the PImMS camera.

We present the first multimass velocity-map imaging data acquired using a new ultrafast camera designed for time-resolved particle imaging. The PImMS (Pixel Imaging Mass Spectrometry) sensor allows particle events to be imaged with time resolution as high as 25 ns over data acquisition times of more than 100 μs. In photofragment imaging studies, this allows velocity-map images to be acquired for multiple fragment masses on each time-of-flight cycle. We describe the sensor architecture and present bench-testing data and multimass velocity-map images for photofragments formed in the UV photolysis of two test molecules: Br(2) and N,N-dimethylformamide.

The Pixel Imaging Mass Spectrometry (PImMS) camera is used in proof-of-principle three-dimensional imaging experiments on the photodissociation of carbonyl sulfide and ethyl iodide at wavelengths around 230 nm and 245 nm, respectively. Coupling the PImMS camera with DC-sliced velocity-map imaging allows the complete three-dimensional Newton sphere of photofragment ions to be recorded on each laser pump-probe cycle with a timing precision of 12.5 ns, yielding velocity resolutions along the time-of-flight axis of around 6%-9% in the applications presented.

This work demonstrates the capability of multi-mass, microscope-mode imaging to reduce the acquisition time of spatially distributed analytes such as multi-arrays or biological tissue sections. It also shows that such an instrument can be commissioned by effecting relatively minor modifications to a conventional commercial machine.

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