Photon Burst Research Articles

Dicke Superradiance in Ordered Arrays of Multilevel Atoms

In inverted atomic ensembles, photon-mediated interactions give rise to Dicke superradiance, a form of many-body decay that results in a rapid release of energy as a photon burst. While originally studied in pointlike ensembles, this phenomenon persists in extended ordered systems if the interparticle distance is below a certain bound. Here, we investigate Dicke superradiance in a realistic experimental setting using ordered arrays of alkaline-earth(-like) atoms, such as strontium and ytterbium. Such atoms offer exciting new opportunities for light-matter interactions, as their internal structure allows for trapping at short interatomic distances compared to their long-wavelength transitions, providing the potential for collectively enhanced dissipative interactions. Despite their intricate electronic structure, we show that two-dimensional arrays of these atomic species should exhibit many-body superradiance for achievable lattice constants. Moreover, superradiance effectively “closes” transitions, such that multilevel atoms become more two-level like. This occurs because the avalanchelike decay funnels the emission of most photons into the dominant transition, overcoming the single-atom decay ratios dictated by their fine structure and Zeeman branching. Our work represents an important step in harnessing alkaline-earth atoms as quantum optical sources and as platforms to explore many-body dissipative dynamics. Published by the American Physical Society 2024

A photon burst clears the earliest dusty galaxies: modelling dust in high-redshift galaxies from ALMA to JWST

ABSTRACT The generation and evolution of dust in galaxies are important tracers for star formation, and can characterize the rest-frame ultraviolet to infrared emission from the galaxies. In particular understanding dust in high-redshift galaxies are important for observational cosmology, as they would be necessary to extract information on star formation in the early Universe. We update the public semi-analytical model Ancient Stars and Local Observables by Tracing Halos (a-sloth) to model the evolution of dust, focusing on high-redshift star-forming galaxies with stellar masses of ∼108–1010 M⊙ observed by ALMA (z ≈ 7) and JWST (z ≈ 11). We find that these galaxies should qualitatively differ in their star formation properties; while the samples in ALMA are explained by dust growth in normal star-forming galaxies, the lack of dust in the samples by JWST requires dust ejection by radiation pressure due to recent highly efficient star formation within a few 10 Myr, with order 100 times higher efficiency than normal galaxies calibrated by a-sloth. Depending on where the JWST galaxies locate on the luminosity function, their bursty star formation histories inferred from our model can have impacts for rates of star formation, supernova explosion, stellar feedback, and detectability of dusty, mature galaxies in the very early Universe.

Many-Body Superradiance and Dynamical Mirror Symmetry Breaking in Waveguide QED.

The many-body decay of extended collections of two-level systems remains an open problem. Here, we investigate whether an array of emitters coupled to a one-dimensional bath undergoes Dicke superradiance. This is a process whereby a completely inverted system becomes correlated via dissipation, leading to the release of all the energy in the form of a rapid photon burst. We derive the minimal conditions for the burst to happen as a function of the number of emitters, the chirality of the waveguide, and the single-emitter optical depth, both for ordered and disordered ensembles. Many-body superradiance occurs because the initial fluctuation that triggers the emission is amplified throughout the decay process. In one-dimensional baths, this avalanchelike behavior leads to a spontaneous mirror symmetry breaking, with large shot-to-shot fluctuations in the number of photons emitted to the left and right. Superradiant bursts may thus be a smoking gun for the generation of correlated photon states of exotic quantum statistics.

Deterministic measurement of a Rydberg superatom qubit via cavity-enhanced single-photon emission

With Rydberg dipole interactions, a mesoscopic atomic ensemble becomes a superatom that behaves like a single atom but couples collectively with photons. It is potentially a strong candidate as a qubit in quantum information science, especially for quantum networks. In this paper, we report a cavity-enhanced single-photon interface for a Rydberg superatom and demonstrate deterministic qubit readout via a photon burst. We make use of a low-finesse ring cavity to enhance the atom–photon interaction and obtain in-fiber single-photon generation efficiency of 44%. Harnessing the dipole interaction between two Rydberg levels, we may create either a sequence of multiple single photons or nothing, conditioned on an initial qubit state. We achieve a measurement fidelity of 93.0% in 4.8 µs. Our work complements the experimental toolbox of harnessing Rydberg superatoms for quantum information applications.

The Theoretical Model, Method, and Applications of Scattering Photon Burst Counting Based on an Objective Scanning Technique.

Scattering photon burst counting (SPBC) is a single-particle detection method, which is based on measuring scattering photon bursting of single nanoparticles through a detection volume of <1 fL. Although SPBC has been used for bioassays and analysis of nanoparticles, it is necessary to establish its theoretical model and develop a new detection mode in order to further enhance its sensitivity and enlarge its application fields. In this paper, we proposed a theoretical model for the confocal SPBC method and developed a novel SPBC detection mode using the fast objective scanning technique. The computer simulations and experiments documented that this model well describes the relation between photon counts and experimental parameters (such as nanoparticle concentration and diameter, temperature, and viscosity). Based on this model, we developed a novel SPBC detection mode by using the fast objective scanning technique. Compared to the current confocal SPBC method, the sensitivity of this new method was significantly increased due to the significantly increased photon counts per sampling time, the linear detection range is from 0.9 to 90 pM, and the limit of detection is reduced to 40 fM for 30 nm gold nanoparticles. Furthermore, this new method was successfully applied to determine the enzyme activity of caspase-3 and evaluate the inhibition effectiveness of some inhibitors.

Single-Particle Catalytic Analysis by a Photon Burst Counting Technique Combined with a Microfluidic Chip.

Single-particle catalytic analysis plays an important role to understand the catalytic mechanism of nanocatalysts. Currently, some methods are used to study the relationship between single-particle catalytic activity and morphology. However, there is still lack of a simple and rapid analysis method for evaluating the catalytic activity of an individual nanocatalyst that freely moves in solution. Here, we proposed a novel single-particle catalytic analysis method for investigating the catalytic activity of a free nanocatalyst. Its working principle is based on the photon burst counting analysis on fluorescent catalytic products of an individual nanocatalyst combined with a microfluidic chip. In this study, we used the reduction reaction of resazurin (RZ) to resorufin (RF) catalyzed by gold nanoparticles (GNPs) as a model. When nonfluorescent RZ molecules in one microchannel of the microfluidic chip mixed with the GNPs flowing in another channel under the control of flow rates, each individual photon burst from the catalytic product RF by GNPs was measured in real time with a constructed flow single-particle catalytic analysis (SPCA) system. With the method, the obtained intensity of each photon burst reflects the capacity of a particle to catalyze RZ molecules into RF(s). The number of photon burst within sampling time reflects the particle number of GNPs with catalytic activity. The experimental conditions including the mixing mode of the nanocatalyst and the substrate, the flow rate, RZ concentration, and detection time were optimized. Finally, the method was successfully used to study the catalytic activity of GNPs with different sizes and morphologies.

Laboratory Measurements of X‐Ray Emissions From Centimeter‐Long Streamer Corona Discharges

AbstractWe provide extensive evidence that runaway electron acceleration and subsequent bremsstrahlung X‐ray emission are a common feature in negative electrical discharges with voltages as low as 100 kV, indicating that all negative lightning could potentially produce runaway electrons. Centimeter long streamer corona discharges produce bursts of X‐ray radiation, emitted by a source highly compact in space and time, leading to photon pileup. Median photon burst energies vary between 33 and 96 keV in 100 kV discharges. Statistical analysis of 5,000+ discharges shows that X‐rays are observed in as many as 60% of the triggers, depending on the configuration. X‐ray detection is more frequent when streamers are not followed by a spark, the detector is oriented perpendicular to the gap, and a thicker anode is used. In an 8‐cm‐long gap, X‐rays are produced when runaway electrons hit the anode, and the electron acceleration is not necessarily correlated with streamer collisions.

Detection of rotavirus in clinical specimens using an immunosensor prototype based on the photon burst counting technique.

In this study, a sensitive fluorescence sensor was developed for the detection of small, fluorescence-labeled particles dispersed in a solution. The prototype system comprises of a laser confocal optical system and a mechanical sample stage to detect photon bursting of fluorescence-labeled small particles in sample volumes less than 5 μL within 3 minutes. To examine the feasibility of the prototype system as a diagnostic tool, assemblages of rotavirus and fluorescence-labeled antibody were analyzed. The detection sensitivity for rotavirus was 1 × 104 pfu/mL. Rotavirus in stool samples from patients with acute gastroenteritis was also detected. The advantages and disadvantages of this immunosensor with respect to ELISA and RT-PCR, the current gold standards for virus detection, are discussed.

Acceleration of Radiative Decay of Photon Counts With Increasing Numbers of Measurement Units: A Potential Large Scale Negative Zeno Effect That Matches With Lorentz Contraction and Photon Acceleration Durations

         The reverse Zeno effect whereby an unstable quantum state associated with radiative decay is accelerated by frequent measurements was demonstrated experimentally for numbers of “spontaneous” photons in a 3 m3 hyperdark chamber during the 60 s following a burst of applied photons. Numbers of photon counts were measured from one digital photomultiplier unit when either 1 (the reference) or 2, 3, or 4 units were measuring simultaneously. There was a median decrease of 50 photons per s with the addition of each additional simultaneous measurement by another unit. The energy was ~ 10-17 J per s and is equivalent to a wavelength of 10 nm. This quantity is equivalent to the energy of one neuron in the human brain displaying its upper limit (~1 kHz). The results suggest that this increment of energy may be a standard quantity that reflects the numbers of measurements by similar photoelectric currents to the decay of a single photon burst. The approximately 30 to 40 s required for the decay of photons per unit to inflect towards asymptote is consistent with the solution for the Lorentz contraction for the shift in electron mass-energy (10-17 J) with a wavelength of ~10 nm. The 30 to 40 s value is a solution for several applications to novel calculations involving fundamental parameters within the structure of space-time.

Homogeneous immunoassays by using photon burst counting technique of single gold nanoparticles

In this paper, we reported a sensitive single particle method by combining the photon burst counting technique with gold nanoparticles (GNPs) as labeling probes. The photon bursting of single GNPs will be generated in a highly focused laser beam (less than 1fL) due to the plasmon resonance scattering and Brownian motion of GNPs. We observed an excellent linear relationship between the photon burst counts and the number of particles in GNPs solution. We investigated the statistical behaviors of background noise and photon burst signal of GNPs, and proposed the data processing method based on Gaussian distribution of the background noise. A new homogeneous sandwich immunoassay was developed by using this single particle method. We evaluated the performance of this method by using prostate-specific antigen (PSA) as a model. The linear range of PSA was 1–1000pmol/L and the detection limit was 0.8pmol/L. This novel method was successfully used for the direct detection of cancer biomarker PSA in human serum samples. Our results were in good agreement with conventional ELISA assays.

Approach for LIDAR signals with multiple returns.

Time-correlated single photon counting (TCSPC) and burst illumination laser (BIL) data can be used for depth reconstruction of a target surface; the problem is how to analyze the response for the reconstruction. We propose a fast-approach STMCMC (Simulated Tempering Markov Chain Monte Carlo) for LIDAR signals with multiple return, in order to obtain a complete characterization of a 3D surface by the laser range system. STMCMC is used to explore the spaces by the preset distributions instead of the prior distributions. Added active intervention tempering makes the Markov chain mix better through the temporary expansion of the solutions. The added step keeps the operation under control and yet retains the Markov characteristic of the operation. The theoretical analysis and the demonstrations on the practical data show flexible operation, and the parameters can be estimated to a high degree of accuracy.

Novel 1:1 labeling and purification process for C-terminal thioester and single cysteine recombinant proteins using generic peptidic toolbox reagents.

We developed a versatile set of chemical labeling reagents which allow dye ligation to the C-terminus of a protein or a single internal cysteine and target purification in a simple two-step process. This simple process results in a fully 1:1 labeled conjugate suitable for all quantitative fluorescence spectroscopy and imaging experiments. We refer to a "generic labeling toolbox" because of the flexibility to choose one of many available dyes, spacers of different lengths and compositions which increase the target solubility, a variety of affinity purification tags, and different cleavage chemistries to release the 1:1 labeled proteins. Studying protein function in vitro or in the context of live cells and organisms is of vital importance in biological research. Although label free detection technologies gain increasing interest in molecular recognition science, fluorescence spectroscopy is still the most often used detection technique for assays and screens both in academic as well as in industrial groups. For generations, fluorescence spectroscopists have labeled their proteins of interest with small fluorescent dyes by random chemical linking on the proteins' exposed lysines and cysteines. Chemical reactions with a certain excess of activated esters or maleimides of longer wavelength dyes hardly ever result in quantitative labeling of the target protein. Most of the time, more than one exposed amino acid side chain reacts. This results in a mixture of dye-protein complexes of different labeling stoichiometries and labeling sites. Only mass spectrometry allows resolving the precise chemical composition of the conjugates. In "classical" ensemble averaging fluorescent experiments, these labeled proteins are still useful, and quantification of, e.g., ligand binding experiments, is achieved via knowledge of the overall protein concentration and a fluorescent signal change which is proportional to the amount of complex formed. With the development of fluorescence fluctuation analysis techniques working at single molecule resolution, like fluorescence correlation spectroscopy (FCS), fluorescence cross correlation spectroscopy (FCCS), fluorescence intensity diffusion analysis (FIDA), etc., it became important to work with homogeneously labeled target proteins. Each molecule participating in a binding equilibrium should be detectable when it freely fluctuates through the confocal focus of a microscope. The measured photon burst for each transition contains information about the size and the stoichiometry of a protein complex. Therefore, it is important to work with reagents that contain an exact number of tracers per protein at identical positions. The ideal fluorescent tracer-protein complex stoichiometry is 1:1. While genetic tags such as fluorescent proteins (FPs) are widely used to detect proteins, FPs have several limitations compared to chemical tags. For example, FPs cannot easily compete with organic dyes in the flexibility of modification and spectral range; moreover, FPs have disadvantages in brightness and photostability and are therefore not ideal for most biochemical single molecule studies. We present the synthesis of a series of exemplaric toolbox reagents and labeling results on three target proteins which were needed for high throughput screening experiments using fluorescence fluctuation analysis at single molecule resolution. On one target, Hu-antigen R (HuR), we demonstrated the activity of the 1:1 labeled protein in ribonucleic acid (RNA) binding, and the ease of resolving the stoichiometry of an RNA-HuR complex using the same dye on protein and RNA by Fluorescence Intensity Multiple Distribution Analysis (FIMDA) detection.

Microfluidic three-dimensional hydrodynamic flow focusing for the rapid protein concentration analysis

A simple microfluidic 3D hydrodynamic flow focusing device has been developed and demonstrated quantitative determinations of quantum dot 525 with antibody (QD525-antibody) and hemagglutinin epitope tagged MAX (HA-MAX) protein concentrations. This device had a step depth cross junction structure at a hydrodynamic flow focusing point at which the analyte stream was flowed into a main detection channel and pinched not only horizontally but also vertically by two sheath streams. As a result, a triangular cross-sectional flow profile of the analyte stream was formed and the laser was focused on the top of the triangular shaped analyte stream. Since the detection volume was smaller than the radius of laser spot, a photon burst histogram showed Gaussian distribution, which was necessary for the quantitative analysis of protein concentration. By using this approach, a linear concentration curve of QD525-antibody down to 10 pM was demonstrated. In addition, the concentration of HA-MAX protein in HEK293 cell lysate was determined as 0.283 ± 0.015 nM. This approach requires for only 1 min determining protein concentration. As the best of our knowledge, this is the first time to determinate protein concentration by using single molecule detection techniques.

Log-normal distribution of single molecule fluorescence bursts in micro/nano-fluidic channels

The width and shape of photon burst histograms pose significant limitations to the identification of single molecules in micro/nano-fluidic channels, and the nature of these histograms is not fully understood. To reach a deeper understanding, we performed computer simulations based on a Gaussian beam intensity profile with various fluidic channel diameters and assuming (1) a deterministic (noise-free) case, (2) photon emission/absorption noise, and (3) photon noise with diffusion. Photon noise in narrow channels yields a Gaussian burst distribution while additional strong diffusion produces skewed histograms. We use the fluctuating residence time picture [J. Söderlund et al., Phys. Rev. Lett. 80, 2386 (1998)] and conclude that the skewness of the photon number distribution is caused by the longitudinal diffusive component of the motion of the molecules as they traverse the laser beam. In the case of strong diffusion in narrow channels, this effect leads to a log-normal distribution. We show that the same effect can transform the separate peaks of the photon burst histograms of multiple molecule mixtures into a single log-normal shape.

Rapid detection of two-protein interaction with a single fluorophore by using a microfluidic device

We have developed a microfluidics based platform and methodology named MAPS (microfluidic system for analyzing proteins in single complex) for detecting two protein interactions rapidly using a single fluorophore. Target proteins were labelled with Quantum dot 525 (QD525) via specific polyclonal antibodies, and were transported through the microfluidic channel subsequently, where the 375 nm excitation laser light was focused to form a detection volume. Photon bursts from target proteins passing through the detection volume were recorded and their photon burst histograms were plotted which demonstrated roughly the specific protein interaction ratio based on their population and statistical behavior. As a proof of concept, Src/STAT3 protein complex interaction ratios with and without EGF stimulation were obtained by MAPS within 1 h and the results were well matched with the one obtained by the conventional immunoprecipitation/Western blot (IP/WB).

Subunit Movements in Single Membrane-bound H+-ATP Synthases from Chloroplasts during ATP Synthesis

Subunit movements within the H(+)-ATP synthase from chloroplasts (CF(0)F(1)) are investigated during ATP synthesis. The gamma-subunit (gammaCys-322) is covalently labeled with a fluorescence donor (ATTO532). A fluorescence acceptor (adenosine 5'-(beta,gamma-imino)triphosphate (AMPPNP)-ATTO665) is noncovalently bound to a noncatalytic site at one alpha-subunit. The labeled CF(0)F(1) is integrated into liposomes, and a transmembrane pH difference is generated by an acid base transition. Single-pair fluorescence resonance energy transfer is measured in freely diffusing proteoliposomes with a confocal two-channel microscope. The fluorescence time traces reveal a repetitive three-step rotation of the gamma-subunit relative to the alpha-subunit during ATP synthesis. Some traces show splitting into sublevels with fluctuations between the sublevels. During catalysis the central stalk interacts, with equal probability, with each alphabeta-pair. Without catalysis the central stalk interacts with only one specific alphabeta-pair, and no stepping between FRET levels is observed. Two inactive states of the enzyme are identified: one in the presence of AMPPNP and one in the presence of ADP.

Single-pair fluorescence resonance energy transfer (spFRET) for the high sensitivity analysis of low-abundance proteins using aptamers as molecular recognition elements.

We have developed a strategy for the detection of single protein molecules, which uses single-pair fluorescence resonance energy transfer (spFRET) as the readout modality and provides exquisite analytical sensitivity and reduced assay turn-around-time by eliminating various sample pre-processing steps. The single-protein detection assay uses two independent aptamer recognition events to form an assembly conducive to intramolecular hybridization of oligonucleotide complements that are tethered to the aptamers. This hybridization brings a donor-acceptor pair within the Förster distance to create a fluorescence signature indicative of the presence of the protein-aptamer(s) association complex. As an example of spFRET, we demonstrate the technique for the analysis of serum thrombin. The assay requires co-association of two distinct epitope-binding aptamers, each of which is labeled with a donor or acceptor fluorescent dye (Cy3 or Cy5, respectively) to produce a FRET response. The FRET response between Cy3 and Cy5 was monitored by single-molecule photon-burst detection, which provides high analytical sensitivity when the number of single-molecule events is plotted versus the target concentration. We are able to identify thrombin with high efficiency based on photon burst events transduced in the Cy5 detection channel. We also demonstrate that the technique can discriminate thrombin molecules from its analogue prothrombin. The analytical sensitivity was >200-fold better than an ensemble measurement.

Single Gold Nanoparticles Counter: An Ultrasensitive Detection Platform for One-Step Homogeneous Immunoassays and DNA Hybridization Assays

In this paper, we present for the first time a single gold nanoparticle counter (SGNPC) in solution based on the photon bursting in a highly focused laser beam (less than 1 fL) due to the plasmon resonance scattering and Brownian motion of gold nanoparticles (GNPs). The photon burst intensity of single 36 nm GNPs is several tens to hundreds times stronger than that of quantum dots (QDs) and organic dyes. The relationship between the photon burst counts and GNPs concentration shows an excellent linearity. The linear range is over 4 orders of magnitude, and the detection limit of GNPs (36 nm) is 17 fM. On the basis of this single nanoparticle technique, we developed an ultrasensitive and highly selective detection platform for homogeneous immunoassay and DNA hybridization assays using GNPs as probes, which were 2-5 orders of magnitude more sensitive than current homogeneous methods. We used this technology to construct homogeneous sandwich immunoassays for cancer biomarkers, such as carcinoembryonic antigen (CEA) and alpha fetal protein (AFP), and aptamer recognition for thrombin. The detection limits are 130 fM for CEA, 714 fM for AFP and 2.72 pM for thrombin. Our method was successfully applied for direct determination of CEA, AFP and thrombin levels in sera from healthy subjects and cancer patients. In homogeneous DNA hybridization detection, we chose methylenetetrahydrofolate reductase (MTHFR) gene as a target. This assay successfully distinguished DNA sequences with single base mismatches, and the detection limits for the target were at 1 fM level.

Photon burst detection of single atoms in an optical cavity

An approach that combines fluorescence and cavity-QED methods enables the fast and reliable detection of single atoms, and should be useful for a series of atomic-physics and quantum-information protocols. Many protocols in atomic physics and quantum information hinge on the ability to detect the presence of neutral atoms1,2,3,4. Up to now, two avenues have been favoured: the direct detection of spontaneously emitted photons using high-quality optics5,6,7, or the observation of changes in light transmission through cavity mirrors due to strong atom–photon coupling8,9,10,11. Here, we present an approach that combines these two methods by detecting an atom in a driven cavity mode through the collection of spontaneous emission and forward scattering into an undriven, orthogonally polarized cavity mode. Moderate atom–cavity coupling enhances the signal, enabling the detection of multiple photons from the same atom. This real-time measurement can establish the presence of a single freely moving atom in less than 1 μs with more than 99.7% confidence, using coincidence measurements to decrease the rate of false detections.

Nanofluidic Devices for Single Molecule Identification

In this letter, detection of target protein molecules has been demonstrated by a two-dimensional (2D) photon burst analysis technique and microfluidic channel device. Individual molecule events are scatter plotted in terms of their photon counts and burst width in 2D photon burst analysis. Detection of target protein is verified by a higher counts-per-bin for rabbit anti-HA polyclonal antibody sample than that of the control sample from the 2D photon burst analysis. Since this is microfluidic single molecule detection scheme, it has the advantages of high sensitivity, small sample consumption and reduced processing time, comparing to the conventional immunological ensemble measurements, such as western blot, immuno-precipitation, etc.