Photon-counting MCP/Timepix detectors for soft X-ray imaging and spectroscopic applications.

Detectors with microchannel plates (MCPs) provide unique capabilities to detect single photons with high spatial (<10 µm) and timing (<25 ps) resolution. Although this detection technology was originally developed for applications with low event rates, recent progress in readout electronics has enabled their operation at substantially higher rates by simultaneous detection of multiple particles. In this study, the potential use of MCP detectors with Timepix readout for soft X-ray imaging and spectroscopic applications where the position and time of each photon needs to be recorded is investigated. The proof-of-principle experiments conducted at the Advanced Light Source demonstrate the capabilities of MCP/Timepix detectors to operate at relatively high input counting rates, paving the way for the application of these detectors in resonance inelastic X-ray scattering and X-ray photon correlation spectroscopy (XPCS) applications. Local count rate saturation was investigated for the MCP/Timepix detector, which requires optimization of acquisition parameters for a specific scattering pattern. A single photon cluster analysis algorithm was developed to eliminate the charge spreading effects in the detector and increase the spatial resolution to subpixel values. Results of these experiments will guide the ongoing development of future MCP devices optimized for soft X-ray photon-counting applications, which should enable XPCS dynamics measurements down to sub-microsecond timescales.

Development of new photon-counting detectors for single-molecule fluorescence microscopy.

Two optical configurations are commonly used in single-molecule fluorescence microscopy: point-like excitation and detection to study freely diffusing molecules, and wide field illumination and detection to study surface immobilized or slowly diffusing molecules. Both approaches have common features, but also differ in significant aspects. In particular, they use different detectors, which share some requirements but also have major technical differences. Currently, two types of detectors best fulfil the needs of each approach: single-photon-counting avalanche diodes (SPADs) for point-like detection, and electron-multiplying charge-coupled devices (EMCCDs) for wide field detection. However, there is room for improvements in both cases. The first configuration suffers from low throughput owing to the analysis of data from a single location. The second, on the other hand, is limited to relatively low frame rates and loses the benefit of single-photon-counting approaches. During the past few years, new developments in point-like and wide field detectors have started addressing some of these issues. Here, we describe our recent progresses towards increasing the throughput of single-molecule fluorescence spectroscopy in solution using parallel arrays of SPADs. We also discuss our development of large area photon-counting cameras achieving subnanosecond resolution for fluorescence lifetime imaging applications at the single-molecule level.

Phasor imaging with a widefield photon-counting detector.

Fluorescence lifetime can be used as a contrast mechanism to distinguish fluorophores for localization or tracking, for studying molecular interactions, binding, assembly, and aggregation, or for observing conformational changes via Förster resonance energy transfer (FRET) between donor and acceptor molecules. Fluorescence lifetime imaging microscopy (FLIM) is thus a powerful technique but its widespread use has been hampered by demanding hardware and software requirements. FLIM data is often analyzed in terms of multicomponent fluorescence lifetime decays, which requires large signals for a good signal-to-noise ratio. This confines the approach to very low frame rates and limits the number of frames which can be acquired before bleaching the sample. Recently, a computationally efficient and intuitive graphical representation, the phasor approach, has been proposed as an alternative method for FLIM data analysis at the ensemble and single-molecule level. In this article, we illustrate the advantages of combining phasor analysis with a widefield time-resolved single photon-counting detector (the H33D detector) for FLIM applications. In particular we show that phasor analysis allows real-time subsecond identification of species by their lifetimes and rapid representation of their spatial distribution, thanks to the parallel acquisition of FLIM information over a wide field of view by the H33D detector. We also discuss possible improvements of the H33D detector's performance made possible by the simplicity of phasor analysis and its relaxed timing accuracy requirements compared to standard time-correlated single-photon counting (TCSPC) methods.

Microchannel Plate Imaging Photon Counters for Ultraviolet through NIR Detection with High Time Resolution.

Cross strip and cross delay line readout microchannel plate detectors in 18 mm, 25 mm and 40 mm active area formats including open face (UV/particle) and sealed tube (optical) configurations have been constructed. These have been tested with a field programmable gate array based electronics for single event encoding. Using small pore MCPs (6 µm) operated in a pair, we achieve gains of >1 × 106 which is sufficient to provide spatial resolution of ~17 µm FHWM with the 18 mm and 40 mm cross strip readouts. New cross strip electronics can process high output event rates (> 4 MHz) with high spatial resolution, and self triggered event timing accuracy of ~1.5 ns for sealed tube XS optical sensors. A peak quantum efficiency of between 13% and 19% at 500 nm has been achieved with SuperGenII photocathodes with response from 400 nm to 900 nm for both cross strip and cross delay line sealed tubes. Local area counting rates of up to 40 kHz (100µm spot) have been attained with XS sealed tubes, along with image linearity and stability to better than 50 µm. 25mm cross delay line tubes achieve ~50 µm resolution and > 2 MHz output event rates.

New photon-counting detectors for single-molecule fluorescence spectroscopy and imaging.

Solution-based single-molecule fluorescence spectroscopy is a powerful new experimental approach with applications in all fields of natural sciences. Two typical geometries can be used for these experiments: point-like and widefield excitation and detection. In point-like geometries, the basic concept is to excite and collect light from a very small volume (typically femtoliter) and work in a concentration regime resulting in rare burst-like events corresponding to the transit of a single-molecule. Those events are accumulated over time to achieve proper statistical accuracy. Therefore the advantage of extreme sensitivity is somewhat counterbalanced by a very long acquisition time. One way to speed up data acquisition is parallelization. Here we will discuss a general approach to address this issue, using a multispot excitation and detection geometry that can accommodate different types of novel highly-parallel detector arrays. We will illustrate the potential of this approach with fluorescence correlation spectroscopy (FCS) and single-molecule fluorescence measurements. In widefield geometries, the same issues of background reduction and single-molecule concentration apply, but the duration of the experiment is fixed by the time scale of the process studied and the survival time of the fluorescent probe. Temporal resolution on the other hand, is limited by signal-to-noise and/or detector resolution, which calls for new detector concepts. We will briefly present our recent results in this domain.

High Speed Multichannel Charge Sensitive Data Acquisition System with Self-Triggered Event Timing.

A number of modern experiments require simultaneous measurement of charges on multiple channels at > MHz event rates with an accuracy of 100-1000 e(-) rms. One widely used data processing scheme relies on application of specific integrated circuits enabling multichannel analog peak detection asserted by an external trigger followed by a serial/sparsified readout. Although this configuration minimizes the back end electronics, its counting rate capability is limited by the speed of the serial readout. Recent advances in analog to digital converters and FPGA devices enable fully parallel high speed multichannel data processing with digital peak detection enhanced by finite impulse response filtering. Not only can accurate charge values be obtained at high event rates, but the timing of the event on each channel can also be determined with high accuracy.We present the concept and first experimental tests of fully parallel 128-channel charge sensitive data processing electronics capable of measuring charges with accuracy of ~1000 e- rms. Our system does not require an external trigger and, in addition to charge values, it provides the event timing with an accuracy of ~1 ns FWHM. One of the possible applications of this system is high resolution position sensitive event counting detectors with microchannel plates combined with cross strip readout. Implementation of fast data acquisition electronics increases the counting rates of those detectors to multi-MHz level, preserving their unique capability of virtually noiseless detection of both position (with accuracy of ~10 µm FWHM) and timing (~1 ns FWHM) of individual particles, including photons, electrons, ions, neutrals, and neutrons.

Optical properties and quantum efficiency of thin-film alkali halides in the far ultraviolet.

The optical constants of thin films of CsI, KI, and KBr and the quantum efficiency (QE) of planar photocathodes made with these alkali halides in the 53.6-174.4-nm spectral range are presented. The optical constants were obtained from measurements of the reflectance as a function of incidence angle. The effect of film heating and exposure to UV irradiation on the optical properties and on the QE of the three alkali halides was investigated. KBr was found to be the most stable material for both heating and UV irradiation. KI appeared to be close to temperature stable, whereas UV exposure affected its optical constants. CsI optical constants changed after 420 K heating and after UV exposure. The changes in the optical constants were related to the QE changes, and a certain correlation between both variations was determined. However, it was also demonstrated that the QE changes cannot be explained solely by the changes in optical constants.