Time-correlated Single Photon Counting System Research Articles

Enhancing the spatial resolution of time-of-flight based non-line-of-sight imaging via instrument response function deconvolution.

Non-line-of-sight (NLOS) imaging retrieves the hidden scenes by utilizing the signals indirectly reflected by the relay wall. Benefiting from the picosecond-level timing accuracy, time-correlated single photon counting (TCSPC) based NLOS imaging can achieve theoretical spatial resolutions up to millimeter level. However, in practical applications, the total temporal resolution (also known as total time jitter, TTJ) of most current TCSPC systems exceeds hundreds of picoseconds due to the combined effects of multiple electronic devices, which restricts the underlying spatial resolution of NLOS imaging. In this paper, an instrument response function deconvolution (IRF-DC) method is proposed to overcome the constraints of a TCSPC system's TTJ on the spatial resolution of NLOS imaging. Specifically, we model the transient measurements as Poisson convolution process with the normalized IRF as convolution kernel, and solve the inverse problem with iterative deconvolution algorithm, which significantly improves the spatial resolution of NLOS imaging after reconstruction. Numerical simulations show that the IRF-DC facilitates light-cone transform and frequency-wavenumber migration solver to achieve successful reconstruction even when the system's TTJ reaches 1200 ps, which is equivalent to what was previously possible when TTJ was about 200ps. In addition, the IRF-DC produces satisfactory reconstruction outcomes when the signal-to-noise ratio (SNR) is low. Furthermore, the effectiveness of the proposed method has also been experimentally verified. The proposed IRF-DC method is highly applicable and efficient, which may promote the development of high-resolution NLOS imaging.

64 picosecond time resolved time-correlated single photon counting imaging.

High-speed imaging of dynamic scenes is a challenging and important task in many applications. However, conventional imaging methods based on charge coupled devices or complementary metal oxide semiconductors have limitations in temporal resolution and photon sensitivity. To address this problem, we propose a novel high-speed imaging scheme that combines single-pixel imaging with single photon detection and time-correlated single photon counting. Our scheme can achieve high-speed imaging with 64ps resolution by repeating the motion scenes and using binary outputs from single photon detectors. We demonstrate our scheme by reconstructing the switching process of a digital micro-mirror device and a liquid crystal spatial light modulator. Our scheme can be further improved to 1ps resolution by using a more accurate time-correlated single photon counting system. Moreover, our scheme can adapt to different speed scenes by adjusting the temporal resolution and reducing the sampling time. Our high temporal resolution imaging scheme further expands the application areas of single-pixel imaging and provides solutions for scenes requiring single photon detection and higher temporal resolution, such as reproducible chemical reaction processes imaging, cellular or sub-cellular bio imaging, single-molecule imaging of rotary motors, high-speed equipment inspection, and other periodic high-speed scenes imaging.

High-Flux Fast Photon-Counting 3D Imaging Based on Empirical Depth Error Correction

The time-correlated single-photon-counting (TCSPC) three-dimensional (3D) imaging lidar system has broad application prospects in the field of low-light 3D imaging because of its single-photon detection sensitivity and picoseconds temporal resolution. However, conventional TCSPC systems always limit the echo photon flux to an ultra-low level to obtain high-accuracy depth images, thus needing to spend amounts of acquisition time to accumulate sufficient photon detection events to form a reliable histogram. When the echo photon flux is increased to medium or even high, the data acquisition time can be shortened, but the photon pile-up effect can seriously distort the photon histogram and cause depth errors. To realize high accuracy TCSPC depth imaging with a shorter acquisition time, we propose a high-flux fast photon-counting 3D imaging method based on empirical depth error correction. First, we derive the photon flux estimation formula and calculate the depth error of our photon-counting lidar under different photon fluxes with experimental data. Then, a function correction model between the depth errors and the number of echo photons is established by numerical fitting. Finally, the function correction model is used to correct depth images at high photon flux with different acquisition times. Experimental results show that the empirical error correction method can shorten the image acquisition time by about one order of magnitude while ensuring a moderate accuracy of the depth image.

Integration of Decay Time Analysis and Radiation Measurement for Quantum-Dot-Based Scintillator’s Characterization

In this study, we demonstrated the process of an integrated apparatus for decay time analysis and gamma radiation measurement with a liquid-scintillator-based cadmium-doped zinc oxide (CZO) nanomaterial. Generally, time-resolved photon counting is an essential analysis method in the field of precision measurement in the quantum domain. Such photon counting equipment requires a pulse laser that can be repeated quickly while having a sharp pulse width of picoseconds or femtoseconds as a light source. Time-correlated single photon counting (TCSPC) equipment, which is currently a commercial product, is inconvenient for recent development research because the scintillator size and shape are limited. Here, neodymium-doped yttrium aluminum garnet (Nd/YAG) laser TCSPC equipment was constructed to analyze the fluorescence characteristics of scintillators having various sizes and shapes. Then, a liquid scintillator added with CZO nanomaterial was prepared and the Nd/YAG laser TCSPC equipment test was performed. As a result of measuring the scintillator using the manufactured Nd/YAG laser TCSPC equipment, the non-CZO liquid scintillator was analyzed at 2.30 ns and the liquid scintillator equipped with CZO-loaded nanomaterial was analyzed at 11.95 ns. It showed an error within 5% when compared with the result of commercial TCSPC equipment. In addition, it was verified that the Nd/YAG laser TCSPC system can sufficiently measure the decay time in nanoseconds (ns). Moreover, it was presented that the Compton edge energy of Cs−137 is 477.3 keV, which hardly generates a photoelectric effect, and Compton scattering mainly occurs.

Above pile-up fluorescence microscopy with a 32 Mc/s single-channel time-resolved SPAD system.

One of the major drawbacks of time-correlated single-photon counting (TCSPC) is generally represented by pile-up distortion, which strongly bounds the maximum acquisition speed to a few percent of the laser excitation rate. Based on a previous theoretical analysis, recently we presented the first, to the best of our knowledge, low-distortion and high-speed TCSPC system capable of overcoming the pile-up limitation by perfectly matching the single-photon avalanche diode (SPAD) dead time to the laser period. In this work, we validate the proposed system in a standard fluorescence measurement by comparing experimental data with the reference theoretical framework. As a result, a count rate of 32 Mc/s was achieved with a single-channel system still observing a negligible lifetime distortion.

Absolute spectral backscatter measurements of large-core multimode PMMA polymer optical fibers.

To our knowledge, we are the first to measure the absolute value of the backscattering coefficient of a standard 1 mm core-diameter, multimode (MM) step-index (SI) polymethylmethacrylate (PMMA) polymer optical fiber (POF) for the spectral range of 450 nm to 700 nm. Our optical time domain reflectometer (OTDR) setup consists of a femtosecond supercontinuum laser with an acousto-optical filter as a tunable light source with short pulses and a time-correlated single-photon counting system as a receiver with a high dynamic range. The backscattering coefficient is calculated from the ratio between the energy within the fiber end reflex and the distributed backscattering level. We also measured the spectral attenuation with our OTDR setup and compared it with a standardized measurement method. At the attenuation minima within the measured spectral range the backscattering level of a 1 ns pulse is about -46dB at 520 nm, -48dB at 570 nm, and -51 dB at 650 nm. We were also able to show by the observed wavelength dependence that Rayleigh scattering causes a majority of the scattering.

Excimer Formation of Perylene Bisimide Dyes within Stacking-Restrained Folda-Dimers: Insight into Anomalous Temperature Responsive Dual Fluorescence

Excimer Formation of Perylene Bisimide Dyes within Stacking-Restrained Folda-Dimers: Insight into Anomalous Temperature Responsive Dual Fluorescence

Toward ultra-fast time-correlated single-photon counting: A compact module to surpass the pile-up limit.

Time-Correlated Single-Photon Counting (TCSPC) is an excellent technique used in a great variety of scientific experiments to acquire exceptionally fast and faint light signals. Above all, in Fluorescence Lifetime Imaging (FLIM), it is widely recognized as the gold standard to record sub-nanosecond transient phenomena with picosecond precision. Unfortunately, TCSPC has an intrinsic limitation: to avoid the so-called pile-up distortion, the experiments have been historically carried out, limiting the acquisition rate below 5% of the excitation frequency. In 2017, we demonstrated that such a limitation can be overcome if the detector dead time is exactly matched with the excitation period, thus paving the way to unprecedented speedup of FLIM measurements. In this paper, we present the first single-channel system that implements the novel proposed methodology to be used in modern TCSPC experimental setups. To achieve this goal, we designed a compact detection head, including a custom single-photon avalanche diode externally driven by a fully integrated Active Quenching Circuit (AQC), featuring a finely tunable dead time and a short reset time. The output timing signal is extracted by using a picosecond precision Pick-Up Circuit (PUC) and fed to a newly developed timing module consisting of a mixed-architecture Fast Time to Amplitude Converter (F-TAC) followed by high-performance Analog-to-Digital Converters (ADCs). Data are transmitted in real-time to a Personal Computer (PC) at USB 3.0 rate for specific and custom elaboration. Preliminary experimental results show that the new TCSPC system is suitable for implementing the proposed technique, achieving, indeed, high timing precision along with a count rate as high as 40 Mcps.

Label-free multimodal nonlinear optical microscopy for biomedical applications

This paper addresses the application of multimodal nonlinear optical (MNLO) microscopy to clinical research within the context of label-free non-invasive molecular imaging. Here, a compact MNLO microscope based on a laser scanning microscope, a femtosecond laser, a time-correlated single-photon counting system, and a photonic crystal fiber are introduced for biomedical applications. By integrating two-photon fluorescence, two-photon fluorescence lifetime imaging, second-harmonic generation, and coherent anti-Stokes Raman scattering microscopy, the proposed scheme provides profound insights into the physicochemical properties related to 3D molecular orientation distribution, inter- and intra-molecular interactions, and disease progression in biological systems and organs. The high peak power and the low average intensity of near-infrared laser pulses allow for deep-penetration imaging without compromising sample vitality. Linking nonlinear optical phenomena with time/spectral/polarization-resolved imaging also makes it possible to obtain multidimensional information to address complex biomedical questions.

Lead-halide Cs4PbBr6 single crystals for high-sensitivity radiation detection

Low-dimensional perovskite materials and their derivatives with excellent optical performance are promising candidates for light-emission applications. Herein, centimeter lead-halide Cs4PbBr6 single crystals (SCs), which have been used for radiation detection with the indirect conversion method, were synthesized by a facile solution process. The Cs4PbBr6 scintillator exhibits bright green emission peaking at 525 nm and a high photoluminescence quantum yield (up to 86.7%) under 375 nm laser excitation. The Cs4PbBr6 SCs exhibit high sensitivity to 40 keV X-rays, with a favorable linearity with the X-ray exposure dose rate, and the detection limit is as low as 64.4 nGyair/s. The scintillation time-response performance of the Cs4PbBr6 SCs was acquired by a time-correlated single-photon counting system under alpha-particle excitation. The Cs4PbBr6 SCs exhibit a very fast time response (τav = 1.46 ns) to alpha particles from a 241Am radiation source. This value is comparable to that of the commercial plastic scintillator EJ-228 (τav = 1.31 ns) and much faster than that of the LYSO(Ce) scintillator (τav = 36.17 ns). Conceptual X-ray imaging and alpha-particle pulse height spectroscopy experiments were also performed. These results demonstrated the potential of Cs4PbBr6 SCs for radiation detection applications, including X-ray imaging and charged particle detection with fast scintillation decay time and high sensitivity.

Achieving a high photon count rate in digital time-correlated single photon counting using a hybrid photodetector.

We report an enhanced photon count rate in a digitally implemented time-correlated single-photon counting (TCSPC) system by utilizing a hybrid photodetector (HPD). In our digital TCSPC scheme, the photoelectronic responses from a single photon-sensitive photodetector are digitally analyzed through a high-speed analog-to-digital convertor (ADC). By virtue of the HPD which provides nearly a constant signal gain, the single-photon pulses can be effectively distinguished from pulses of simultaneously detected multiple photons by the pulse heights. Consequently, our digital TCSPC system can selectively collect single-photon signals even in the presence of intense multi-photon detections with its temporal accuracy not to be compromised. In our experiment of fluorescence lifetime measurement, the maximum count rate of single photons nearly reached the theoretical limit given by the Poisson statistics. This demonstrated that the digital TCSPC combined with the HPD provides an ultimate solution for the TCSPC implementation for high photon count rates.

FLIM data analysis based on Laguerre polynomial decomposition and machine-learning.

Significance: The potential of fluorescence lifetime imaging microscopy (FLIM) is recently being recognized, especially in biological studies. However, FLIM does not directly measure the lifetimes, rather it records the fluorescence decay traces. The lifetimes and/or abundances have to be estimated from these traces during the phase of data processing. To precisely estimate these parameters is challenging and requires a well-designed computer program. Conventionally employed methods, which are based on curve fitting, are computationally expensive and limited in performance especially for highly noisy FLIM data. The graphical analysis, while free of fit, requires calibration samples for a quantitative analysis.Aim: We propose to extract the lifetimes and abundances directly from the decay traces through machine learning (ML).Approach: The ML-based approach was verified with simulated testing data in which the lifetimes and abundances were known exactly. Thereafter, we compared its performance with the commercial software SPCImage based on datasets measured from biological samples on a time-correlated single photon counting system. We reconstructed the decay traces using the lifetime and abundance values estimated by ML and SPCImage methods and utilized the root-mean-squared-error (RMSE) as marker.Results: The RMSE, which represents the difference between the reconstructed and measured decay traces, was observed to be lower for ML than for SPCImage. In addition, we could demonstrate with a three-component analysis the high potential and flexibility of the ML method to deal with more than two lifetime components.Conclusions: The ML-based approach shows great performance in FLIM data analysis.

Structural, Optical and Decay Properties of Zinc(II) 8-Hydroxyquinoline and Its Thin Film

Zinc(II) 8-hydroxyquinoline (Znq2) green luminescent material and its blended thin film in a poly(methyl methacrylate) (PMMA) matrix have been prepared. XRD analysis confirms the formation of the compound and its presence in the PMMA blended thin film. The orbital molecular geometry, quantum chemical calculations and band gap energy of Znq2 phosphor have been confirmed from the DFT study. The morphology of the phosphor was shown by the SEM images. UV–Vis absorption, photoluminescence and decay analysis of zinc(II) 8-hydroxyquinoline phosphor confirms its suitability as a green emitter for organic light-emitting diodes. Uniform distribution of Znq2 powder in the PMMA matrix and its roughness was estimated by AFM analysis. Luminescence decay study was utilized to demonstrate its lifetime analysis by the time-correlated single-photon counting (TCSPC) system.

Photon arrival time tagging with many channels, sub-nanosecond deadtime, very high throughput, and fiber optic remote synchronization.

Time-Correlated Single Photon Counting (TCSPC) and time tagging of individual photon detections are powerful tools in many quantum optical experiments and other areas of applied physics. Using TCSPC, e.g., for the purpose of fluorescence lifetime measurements, is often limited in speed due to dead-time losses and pileup. We show that this limitation can be lifted by reducing the dead-time of the timing electronics to the absolute minimum imposed by the speed of the detector signals while maintaining high temporal resolution. A complementing approach to speedy data acquisition is parallelization by means of simultaneous readout of many detector channels. This puts high demands on the data throughput of the TCSPC system, especially in time tagging of individual photon arrivals. Here, we present a new design approach, supporting up to 16 input channels, an extremely short dead-time of 650 ps, very high time tagging throughput, and a timing resolution of 80 ps. In order to facilitate remote synchronization of multiple such instruments with highest precision, the new TCSPC electronics provide an interface for White Rabbit fiber optic networks. Beside fundamental research in the field of astronomy, such remote synchronization tasks arise routinely in quantum communication networks with node to node distances on the order of tens of kilometers. In addition to showing design features and benchmark results of new TCSPC electronics, we present application results from spectrally resolved and high-speed fluorescence lifetime imaging in medical research. We furthermore show how pulse-pileup occurring in the detector signals at high photon flux can be corrected for and how this data acquisition scheme performs in terms of accuracy and efficiency.

Resolution and contrast enhancement of laser-scanning multiphoton microscopy using thulium-doped upconversion nanoparticles

High-contrast optical imaging is achievable using phosphorescent labels to suppress the short-lived background due to the optical backscatter and autofluorescence. However, the long-lived phosphorescence is generally incompatible with high-speed laser-scanning imaging modalities. Here, we show that upconversion nanoparticles of structure NaYF4:Yb co-doped with 8% Tm (8T-UCNP) in combination with a commercial laser-scanning multiphoton microscopy are uniquely suited for labeling biological systems to acquire high-resolution images with the enhanced contrast. In comparison with many phosphorescent labels, the 8T-UCNP emission lifetime of ∼ 15 µs affords rapid image acquisition. The high-order optical nonlinearity of the 8T-UCNP (n ≈ 4, as confirmed experimentally and theoretically) afforded pushing the resolution limit attainable with UCNPs to the diffraction-limit. The contrast enhancement was achieved by suppressing the background using (i) bandpass spectral filtering of the narrow emission peak of 8T-UCNP at 455-nm, and (ii) time-gating implemented with a time-correlated single-photon counting system that demonstrated the contrast enhancement of > 2.5-fold of polyethyleneimine-coated 8T-UCNPs taken up by human breast adenocarcinoma cells SK-BR-3. As a result, discrete 8T-UCNP nanoparticles became clearly observable in the freshly excised spleen tissue of laboratory mice 15-min post intravenous injection of an 8T-UCNP solution. The demonstrated approach paves the way for high-contrast, high-resolution, and high-speed multiphoton microscopy in challenging environments of intense autofluorescence, exogenous staining, and turbidity, as typically occur in intravital imaging.

A Low-Cost Time-Correlated Single Photon Counting Portable DNA Analyzer.

Photon-counting analysis of nucleic acids plays a key role in many diagnostics applications for its accurate and non-invasive nature. However, conventional photon-counting instrumentations are bulky and expensive due to the use of conventional optics and a lack of optimization of electronics. In this paper, we present a portable, low-cost time-correlated single photon-counting (TCSPC) analysis system for DNA detection. Both optical and electronic subsystems are carefully designed to provide effective emission filtering and size reduction, delivering good DNA detection and fluorescence lifetime extraction performance. DNA detection has been verified by fluorescence lifetime measurements of a V-carbazole conjugated fluorophore lifetime bioassay. The time-to-digital module of the proposed TCSPC system achieves a full width at half maximum (FWHM) timing resolution from 121 to 145 ps and a differential non-linearity (DNL) between −8.5% and +9.7% of the least significant bit (LSB) within the 500 ns full-scale range (FSR). With a detection limit of 6.25 nM and a dynamic range of 6.8 ns, the proposed TCSPC system demonstrates the enabling technology for rapid, point-of-care DNA diagnostics.

In situ measurement of temperature dependent picosecond resolved carrier dynamics in near infrared (NIR) sensitive device on action.

The carrier dynamics study of emerging near infrared (NIR) absorbing materials is an essential need to develop device technology toward enhanced NIR light harvesting. In this study, we have documented the design of an indigenously developed time correlated single photoncounting (TCSPC) system working in the NIR (900 nm-1700 nm) spectral region. The system is compatible to study transient photoluminescence of device samples under tunable bias voltages. The liquid nitrogen cooling and electrical heating of the sample chamber provides additional flexibility of temperature dependent study starting from -196 °C to 400 °C. As a model system to study, we have chosen a multilayer InAs/InGaAs/GaAs/AlGaAs dot in the dual well device sample as the thin film quantum dot heterostructures are of huge relevance in various NIR harvesting devices. We have investigated the detail carrier dynamics of the device sample using the transient photoluminescence upon varying temperature (80 K-300 K), varying emission energy and different bias voltages (0 V-15 V). The critical temperature (160 K) and critical bias (12 V) of achieving longest excited state lifetime has been mechanistically explained using various competing photophysical phenomena such as hole diffusion, energy relaxation, etc. The emission wavelength dependent study at below and above critical temperature further provides an insight into the dominance of carrier capture and thermal escape at the two different temperature zones. Along with the detail understanding of the carrier dynamics, the results can be helpful to get an idea of the electrical stability of the device and the operability temperature as well. The reasonable good resolution of the NIR TCSPC system and considerable good results ensure the future application of the same for other devices also.

Influence of thermal treatment on the structural and optical properties of methoxy-substituted 2, 4-diphenyl quinoline

Herein, we report blue-emitting methoxy-substituted 2, 4-diphenyl quinoline phosphor prepared using acid-catalyzed Friedlander reaction along with the enhancement in the phase purity due to employed thermal treatment in Ar atmosphere. Improvement in the phase purity of the phosphor leading to a change in their optical properties is reported. XRD and FTIR analyses confirm the formation and improvement in the phase purity of the phosphor. TG/DTA analysis endorses the change in their behavior and thermal stability. The modification in optical band gap of the phosphors due to thermal treatment has been confirmed from the UV–vis spectroscopy. Enhancement in the fluorescence intensity of blue-emitting phosphor due to thermal treatment has been described through photoluminescence analysis. Luminescence decay profile has also been recorded using time-correlated single-photon counting (TCSPC) system for the lifetime analysis of the phosphors which supports the obtained PL analysis. The overall study indicates that methoxy-substituted 2, 4-diphenyl quinoline phosphor which was annealed at 90 °C in Ar atmosphere serves better fluorescence intensity, thermal stability and lifetime profile, and may be utilized for the organic display applications.

Low Detection Limit Time-Correlated Single Photon Counting Lifetime Analytical System for Point-of-Care Applications

Photon-counting analysis plays a key role in many areas, such as biology, chemistry, and medicine. In this paper, we present an integrated time-correlated single photon counting (TCSPC) lifetime analytical system with a complete signal path—from fluorophore excitation, emission detection, to lifetime extraction. The time-to-digital module of the proposed TCSPC system achieves a root-mean-square differential non-linearity of 4% of the least significant bit and a full width at half maximum temporal resolution from 121 to 145 ps within the 500-ns full-scale range. To evaluate the lifetime extraction and detection limit of the proposed TCSPC system, a wide variety of samples, such as fluorescein in water, coumarin 6 in dimethyl sulfoxide, and rhodamine 6G in water, each prepared in 14 concentrations from 0.5 nM (nanomolar, $10^{-9}$ mol/L) to $25~\mu \text{M}$ (micromolar, $10^{-6}$ mol/L), are tested. With the optimized hardware and firmware design, the proposed TCSPC system can accurately extract the fluorescence lifetime of fluorescein, coumarin 6, and rhodamine 6G down to the concentration of 1, 1, and 2.5 nM, respectively, significantly outperforming similar fluorescence lifetime analysis systems.

Experimental research on noninvasive reconstruction of optical parameter fields based on transient radiative transfer equation for diagnosis applications

The noninvasive reconstruction of optical parameter fields in participating phantom is investigated experimentally based on the measured time-resolved radiative signals, which are detected by the time-correlated single-photon counting system. The discrete ordinate method is employed to solve the forward transient radiative transfer equation to simulate the time-resolved radiative transfer in the physical phantom exposed to ultra-short pulse laser irradiation. On top of that, the sequential quadratic programming algorithm based on the generalized Gaussian Markov random field is applied to solve the inverse problem. To improve the computational efficiency, an adjoint equation technique is adopted to determine the gradient of objective function. Good agreement was obtained between the predicted optical parameter fields and realistic ones. All the reconstruction results demonstrate that the proposed reconstruction methods are proved to be accurate and efficient experimentally.