Timing measurements with silicon single photon avalanche diodes: principles and perspectives [Invited].

Picosecond timing of single photons has laid the foundation of a great variety of applications, from life sciences to quantum communication, thanks to the combination of ultimate sensitivity with a bandwidth that cannot be reached by analog recording techniques. Nowadays, more and more applications could still be enabled or advanced by progress in the available instrumentation, resulting in a steadily increasing research interest in this field. In this scenario, single-photon avalanche diodes (SPADs) have gained a key position, thanks to the remarkable precision they are able to provide, along with other key advantages like ruggedness, compactness, large signal amplitude, and room temperature operation, which neatly distinguish them from other solutions like superconducting nanowire single-photon detectors and silicon photomultipliers. With this work, we aim at filling a gap in the literature by providing a thorough discussion of the main design rules and tradeoffs for silicon SPADs and the electronics employed along them to achieve high timing precision. In the end, we conclude with our outlook on the future by summarizing new routes that could benefit from present and prospective timing features of silicon SPADs.

Custom silicon technology for SPAD-arrays with red-enhanced sensitivity and low timing jitter.

Single-photon detection is an invaluable tool for many applications ranging from basic research to consumer electronics. In this respect, the Single Photon Avalanche Diode (SPAD) plays a key role in enabling a broad diffusion of these techniques thanks to its remarkable performance, room-temperature operation, and scalability. In this paper we present a silicon technology that allows the fabrication of SPAD-arrays with an unprecedented combination of low timing jitter (95 ps FWHM) and high detection efficiency at red and near infrared wavelengths (peak of 70% at 650 nm, 45% at 800 nm). We discuss the device structure, the fabrication process, and we present a thorough experimental characterization of the fabricated detectors. We think that these results can pave the way to new exciting developments in many fields, ranging from quantum optics to single molecule spectroscopy.

48-spot single-molecule FRET setup with periodic acceptor excitation.

Single-molecule Förster resonance energy transfer (smFRET) allows measuring distances between donor and acceptor fluorophores on the 3-10 nm range. Solution-based smFRET allows measurement of binding-unbinding events or conformational changes of dye-labeled biomolecules without ensemble averaging and free from surface perturbations. When employing dual (or multi) laser excitation, smFRET allows resolving the number of fluorescent labels on each molecule, greatly enhancing the ability to study heterogeneous samples. A major drawback to solution-based smFRET is the low throughput, which renders repetitive measurements expensive and hinders the ability to study kinetic phenomena in real-time. Here we demonstrate a high-throughput smFRET system that multiplexes acquisition by using 48 excitation spots and two 48-pixel single-photon avalanche diode array detectors. The system employs two excitation lasers allowing separation of species with one or two active fluorophores. The performance of the system is demonstrated on a set of doubly labeled double-stranded DNA oligonucleotides with different distances between donor and acceptor dyes along the DNA duplex. We show that the acquisition time for accurate subpopulation identification is reduced from several minutes to seconds, opening the way to high-throughput screening applications and real-time kinetics studies of enzymatic reactions such as DNA transcription by bacterial RNA polymerase.

Red-Enhanced Photon Detection Module Featuring a 32 × 1 Single-Photon Avalanche Diode Array.

In this letter, the development and the experimental characterization of a new photon detection module, based on a 32×1 red-enhanced single-photon avalanche diode (RE-SPAD) array, are presented. A custom-developed technology has been exploited to design a detector having large-area pixels (50-µm diameter) with optimized performance. With an excess bias voltage Voυ = 15 V, a photon detection efficiency as high as 57% at 600 nm (33% at 800 nm) is achieved, along with dark count rate in the kHz range and optical crosstalk probability as low as 0.29%. The remarkable detection efficiency of the RE-SPAD array makes the module particularly suitable for all applications where high detection efficiency in the red/near-infrared range is mandatory. As an example, the performance of the array module is demonstrated to match the demanding requirements of multispot single-molecule fluorescence spectroscopy.

Optical crosstalk in SPAD arrays for high-throughput single-molecule fluorescence spectroscopy.

Single-molecule fluorescence spectroscopy (SMFS), based on the detection of individual molecules freely diffusing through the excitation spot of a confocal microscope, has allowed unprecedented insights into biological processes at the molecular level, but suffers from limited throughput. We have recently introduced a multispot version of SMFS, which allows achieving high-throughput SMFS by virtue of parallelization, and relies on custom silicon single-photon avalanche diode (SPAD) detector arrays. Here, we examine the premise of this parallelization approach, which is that data acquired from different spots is uncorrelated. In particular, we measure the optical crosstalk characteristics of the two 48-pixel SPAD arrays used in our recent SMFS studies, and demonstrate that it is negligible (crosstalk probability ≤ 1.1 10-3) and undetectable in cross-correlation analysis of actual single-molecule fluorescence data.

Development and characterization of an 8×8 SPAD-array module for gigacount per second applications.

In recent years the development of Single-Photon Avalanche Diodes (SPADs) had a big impact on single-photon counting applications requiring high-performance detectors in terms of Dark Count Rate (DCR), Photon Detection Efficiency (PDE), afterpulsing probability, etc. Among these, it is possible to find applications in single-molecule fluorescence spectroscopy that suffer from long-time measurements. In these cases SPAD arrays can be a solution in order to shorten the measurement time, thanks to the high grade of parallelism they can provide. Moreover, applications in other fields (e.g. astronomy) demand for large-area single-photon detectors, able also to handle very high count rates. For these reasons we developed a new single-photon detection module, featuring an 8 × 8 SPAD array. Thanks to a dedicated silicon technology, the performance of the detector have been finely optimized, reaching a 49% detection efficiency at 550 nm, as well as low dark counts (2 kcount/s maximum all over the array). This module can be used in two different modes: the first is a multi-spot configuration, allowing the acquisition of 64 optical signals at the same time and considerably reducing the time needed for a measurement. The second operation mode instead exploits all the pixels in a combined mode, allowing the detection of a 64-times higher maximum photon rate (up to 2 Gcount/s). In addition, this configuration provides also an extended dynamic range and allows to attain photon number resolving capabilities. Dark counts, detection efficiency, linearity, afterpulsing and crosstalk probability have been characterized at different operating conditions.

Erratum: Bright nanoscale source of deterministic entangled photon pairs violating Bell's inequality.

A correction to this article has been published and is linked from the HTML version of this paper. The error has been fixed in the paper.

16-Ch Time-resolved Single-Molecule Spectroscopy Using Line Excitation.

Single-molecule spectroscopy on freely-diffusing molecules allows detecting conformational changes of biomolecules without perturbation from surface immobilization. Resolving fluorescence lifetimes increases the sensitivity in detecting conformational changes and overcomes artifacts common in intensity-based measurements. Common to all freely-diffusing techniques, however, are the long acquisition times. We report a time-resolved multispot system employing a 16-channel SPAD array and TCSPC electronics, which overcomes the throughput issue. Excitation is obtained by shaping a 532 nm pulsed laser into a line, matching the linear SPAD array geometry. We show that the line-excitation is a robust and cost-effective approach to implement multispot systems based on linear detector arrays.

Bright nanoscale source of deterministic entangled photon pairs violating Bell's inequality.

Global, secure quantum channels will require efficient distribution of entangled photons. Long distance, low-loss interconnects can only be realized using photons as quantum information carriers. However, a quantum light source combining both high qubit fidelity and on-demand bright emission has proven elusive. Here, we show a bright photonic nanostructure generating polarization-entangled photon pairs that strongly violates Bell's inequality. A highly symmetric InAsP quantum dot generating entangled photons is encapsulated in a tapered nanowire waveguide to ensure directional emission and efficient light extraction. We collect ~200 kHz entangled photon pairs at the first lens under 80 MHz pulsed excitation, which is a 20 times enhancement as compared to a bare quantum dot without a photonic nanostructure. The performed Bell test using the Clauser-Horne-Shimony-Holt inequality reveals a clear violation (S CHSH > 2) by up to 9.3 standard deviations. By using a novel quasi-resonant excitation scheme at the wurtzite InP nanowire resonance to reduce multi-photon emission, the entanglement fidelity (F = 0.817 ± 0.002) is further enhanced without temporal post-selection, allowing for the violation of Bell's inequality in the rectilinear-circular basis by 25 standard deviations. Our results on nanowire-based quantum light sources highlight their potential application in secure data communication utilizing measurement-device-independent quantum key distribution and quantum repeater protocols.

Multispot single-molecule FRET: High-throughput analysis of freely diffusing molecules.

We describe an 8-spot confocal setup for high-throughput smFRET assays and illustrate its performance with two characteristic experiments. First, measurements on a series of freely diffusing doubly-labeled dsDNA samples allow us to demonstrate that data acquired in multiple spots in parallel can be properly corrected and result in measured sample characteristics consistent with those obtained with a standard single-spot setup. We then take advantage of the higher throughput provided by parallel acquisition to address an outstanding question about the kinetics of the initial steps of bacterial RNA transcription. Our real-time kinetic analysis of promoter escape by bacterial RNA polymerase confirms results obtained by a more indirect route, shedding additional light on the initial steps of transcription. Finally, we discuss the advantages of our multispot setup, while pointing potential limitations of the current single laser excitation design, as well as analysis challenges and their solutions.

Time-domain diffuse correlation spectroscopy.

Physiological monitoring of oxygen delivery to the brain has great significance for improving the management of patients at risk for brain injury. Diffuse correlation spectroscopy (DCS) is a rapidly growing optical technology able to non-invasively assess the blood flow index (BFi) at the bedside. The current limitations of DCS are the contamination introduced by extracerebral tissue and the need to know the tissue's optical properties to correctly quantify the BFi. To overcome these limitations, we have developed a new technology for time-resolved diffuse correlation spectroscopy. By operating DCS in the time domain (TD-DCS), we are able to simultaneously acquire the temporal point-spread function to quantify tissue optical properties and the autocorrelation function to quantify the BFi. More importantly, by applying time-gated strategies to the DCS autocorrelation functions, we are able to differentiate between short and long photon paths through the tissue and determine the BFi for different depths. Here, we present the novel device and we report the first experiments in tissue-like phantoms and in rodents. The TD-DCS method opens many possibilities for improved non-invasive monitoring of oxygen delivery in humans.

Silicon technologies for arrays of Single Photon Avalanche Diodes.

In order to fulfill the requirements of many applications, we recently developed a new technology aimed at combining the advantages of traditional thin and thick silicon Single Photon Avalanche Diodes (SPAD). In particular we demonstrated single-pixel detectors with a remarkable improvement in the Photon Detection Efficiency in the red/near-infrared spectrum (e.g. 40% at 800nm) while maintaining a timing jitter better than 100ps. In this paper we discuss the limitations of such Red-Enhanced (RE) technology from the point of view of the fabrication of small arrays of SPAD and we propose modifications to the structure aimed at overcoming these issues. We also report the first preliminary experimental results attained on devices fabricated adopting the improved structure.

High-voltage integrated active quenching circuit for single photon count rate up to 80 Mcounts/s.

Single photon avalanche diodes (SPADs) have been subject to a fast improvement in recent years. In particular, custom technologies specifically developed to fabricate SPAD devices give the designer the freedom to pursue the best detector performance required by applications. A significant breakthrough in this field is represented by the recent introduction of a red enhanced SPAD (RE-SPAD) technology, capable of attaining a good photon detection efficiency in the near infrared range (e.g. 40% at a wavelength of 800 nm) while maintaining a remarkable timing resolution of about 100ps full width at half maximum. Being planar, the RE-SPAD custom technology opened the way to the development of SPAD arrays particularly suited for demanding applications in the field of life sciences. However, to achieve such excellent performance custom SPAD detectors must be operated with an external active quenching circuit (AQC) designed on purpose. Next steps toward the development of compact and practical multichannel systems will require a new generation of monolithically integrated AQC arrays. In this paper we present a new, fully integrated AQC fabricated in a high-voltage 0.18 µm CMOS technology able to provide quenching pulses up to 50 Volts with fast leading and trailing edges. Although specifically designed for optimal operation of RE-SPAD devices, the new AQC is quite versatile: it can be used with any SPAD detector, regardless its fabrication technology, reaching remarkable count rates up to 80 Mcounts/s and generating a photon detection pulse with a timing jitter as low as 119 ps full width at half maximum. The compact design of our circuit has been specifically laid out to make this IC a suitable building block for monolithically integrated AQC arrays.

Gigacount/second Photon Detection Module Based on an 8 × 8 Single-Photon Avalanche Diode Array.

In this letter we present a compact photon detection module, based on an 8×8 array of single-photon avalanche diodes (SPADs). The use of a dedicated silicon technology for the fabrication of the sensors allows us to combine large active areas (50-µm diameter), high photon detection efficiency (49% at 550-nm wavelength) and low dark count rate. Thanks to a fully parallel architecture, the module provides voltage pulses synchronous to each photon detection for a maximum global count rate exceeding 1 Gcps. These properties makes the system suitable for operation in two different free-running modes. The first, suitable to acquire faint signals, allows multi-spot acquisitions and can be used to considerably reduce the measurement time in applications like single-molecule analysis. With the second it is possible to use all the pixels in a combined mode, to extend and move the dynamic range of the module to very high count rates and to attain number resolving capabilities.

Observation of strongly entangled photon pairs from a nanowire quantum dot.

A bright photon source that combines high-fidelity entanglement, on-demand generation, high extraction efficiency, directional and coherent emission, as well as position control at the nanoscale is required for implementing ambitious schemes in quantum information processing, such as that of a quantum repeater. Still, all of these properties have not yet been achieved in a single device. Semiconductor quantum dots embedded in nanowire waveguides potentially satisfy all of these requirements; however, although theoretically predicted, entanglement has not yet been demonstrated for a nanowire quantum dot. Here, we demonstrate a bright and coherent source of strongly entangled photon pairs from a position-controlled nanowire quantum dot with a fidelity as high as 0.859±0.006 and concurrence of 0.80±0.02. The two-photon quantum state is modified via the nanowire shape. Our new nanoscale entangled photon source can be integrated at desired positions in a quantum photonic circuit, single-electron devices and light-emitting diodes.

Silicon photon-counting avalanche diodes for single-molecule fluorescence spectroscopy.

Solution-based single-molecule fluorescence spectroscopy is a powerful experimental tool with applications in cell biology, biochemistry and biophysics. The basic feature of this technique is to excite and collect light from a very small volume and work in a low concentration regime resulting in rare burst-like events corresponding to the transit of a single molecule. Detecting photon bursts is a challenging task: the small number of emitted photons in each burst calls for high detector sensitivity. Bursts are very brief, requiring detectors with fast response time and capable of sustaining high count rates. Finally, many bursts need to be accumulated to achieve proper statistical accuracy, resulting in long measurement time unless parallelization strategies are implemented to speed up data acquisition. In this paper we will show that silicon single-photon avalanche diodes (SPADs) best meet the needs of single-molecule detection. We will review the key SPAD parameters and highlight the issues to be addressed in their design, fabrication and operation. After surveying the state-of-the-art SPAD technologies, we will describe our recent progress towards increasing the throughput of single-molecule fluorescence spectroscopy in solution using parallel arrays of SPADs. The potential of this approach is illustrated with single-molecule Förster resonance energy transfer measurements.

Single-molecule FRET experiments with a red-enhanced custom technology SPAD.

Single-molecule fluorescence spectroscopy of freely diffusing molecules in solution is a powerful tool used to investigate the properties of individual molecules. Single-Photon Avalanche Diodes (SPADs) are the detectors of choice for these applications. Recently a new type of SPAD detector was introduced, dubbed red-enhanced SPAD (RE-SPAD), with good sensitivity throughout the visible spectrum and with excellent timing performance. We report a characterization of this new detector for single-molecule fluorescence resonant energy transfer (smFRET) studies on freely diffusing molecules in a confocal geometry and alternating laser excitation (ALEX) scheme. We use a series of doubly-labeled DNA molecules with donor-to-acceptor distances covering the whole range of useful FRET values. Both intensity-based (µs-ALEX) and lifetime-based (ns-ALEX) measurements are presented and compared to identical measurements performed with standard thick SPADs. Our results demonstrate the great potential of this new detector for smFRET measurements and beyond.

New silicon technologies enable high-performance arrays of Single Photon Avalanche Diodes.

In order to fulfill the requirements of many applications, we recently developed a new technology aimed at combining the advantages of traditional thin and thick silicon Single Photon Avalanche Diodes (SPAD). In particular we demonstrated single-pixel detectors with a remarkable improvement in the Photon Detection Efficiency at the longer wavelengths (e.g. 40% at 800nm) while maintaining a timing jitter better than 100ps. In this paper we will analyze the factors the currently prevent the fabrication of arrays of SPADs by adopting such a Red-Enhanced (RE) technology and we will propose further modifications to the device structure that will enable the fabrication of high performance RE-SPAD arrays for photon timing applications.

A 48-pixel array of Single Photon Avalanche Diodes for multispot Single Molecule analysis.

In this paper we present an array of 48 Single Photon Avalanche Diodes (SPADs) specifically designed for multispot Single Molecule Analysis. The detectors have been arranged in a 12×4 square geometry with a pitch-to-diameter ratio of ten in order to minimize the collection of the light from non-conjugated excitation spots. In order to explore the trade-offs between the detectors' performance and the optical coupling with the experimental setup, SPADs with an active diameter of 25 and of 50µm have been manufactured. The use of a custom technology, specifically designed for the fabrication of the detectors, allowed us to combine a high photon detection efficiency (peak close to 50% at a wavelength of 550nm) with a low dark count rate compatible with true single molecule detection. In order to allow easy integration into the optical setup for parallel single-molecule analysis, the SPAD array has been incorporated in a compact module containing all the electronics needed for a proper operation of the detectors.

Improving the performance of bright quantum dot single photon sources using temporal filtering via amplitude modulation.

Single epitaxially-grown semiconductor quantum dots have great potential as single photon sources for photonic quantum technologies, though in practice devices often exhibit nonideal behavior. Here, we demonstrate that amplitude modulation can improve the performance of quantum-dot-based sources. Starting with a bright source consisting of a single quantum dot in a fiber-coupled microdisk cavity, we use synchronized amplitude modulation to temporally filter the emitted light. We observe that the single photon purity, temporal overlap between successive emission events, and indistinguishability can be greatly improved with this technique. As this method can be applied to any triggered single photon source, independent of geometry and after device fabrication, it is a flexible approach to improve the performance of systems based on single solid-state quantum emitters, which often suffer from excess dephasing and multi-photon background emission.