Coincidence Experiments Research Articles

Setup for multicoincidence experiments of photons in the extreme ultraviolet to visible spectral range and charged particles-The solid angle maximization approach.

The coincident detection of particles is a powerful method in experimental physics, enabling the investigation of a variety of projectile-target interactions. The vast majority of coincidence experiments is performed with charged particles, as they can be guided by electric or magnetic fields to yield large detection probabilities. When a neutral species or a photon is one of the particles recorded in coincidence, its detection probability typically suffers from small solid angles. Here, we present two optical assemblies considerably enhancing the solid angle for photon detection in the extreme ultraviolet to visible spectral range. The efficiency and versatility of these assemblies are demonstrated for electron-photon coincidence detection, where electrons and photons emerge from fundamental processes after photoexcitation of gaseous samples by synchrotron radiation.

Fine structure of the pygmy quadrupole resonance in 112,114Sn

The electric quadrupole response in 112,114Sn isotopes is investigated by energy-density functional (EDF) and three-phonon quasiparticle-phonon model (QPM) theory with special emphasis on electric quadrupole excitations located above the first collective 2+ state and below 5 MeV. Additional quadrupole strength clustering as a sequence of states similar to the recently observed pygmy quadrupole resonance in 124Sn is found. The spectral distributions and transition densities of these 2+ states show special features being compatible with oscillations of a neutron skin against the isospin-symmetric nuclear core. Furthermore, two (p, p′γ) Doppler-shift attenuation (DSA) coincidence experiments were performed at the SONIC@HORUS setup. 2+ states with excitation energies up to 4.2 MeV were populated in 112,114Sn. Lifetimes and branching ratios were measured allowing for the determination of E2 transition strengths to the ground state. A stringent comparison of the new data to EDF+QPM theory in 112Sn and 114Sn isotopes hints at the occurrence of a low-energy quadrupole mode of unique character which could be interpreted as pygmy quadrupole resonance.

Nuclear level densities and γ -ray strength functions of Ta180,181,182

Particle-$\gamma$ coincidence experiments were performed at the Oslo Cyclotron Laboratory with the $^{181}$Ta(d,X) and $^{181}$Ta($^{3}$He,X) reactions, to measure the nuclear level densities (NLDs) and $\gamma$-ray strength functions ($\gamma$SFs) of $^{180, 181, 182}$Ta using the Oslo method. The Back-shifted Fermi-Gas, Constant Temperature plus Fermi Gas, and Hartree-Fock-Bogoliubov plus Combinatorial models where used for the absolute normalisations of the experimental NLDs at the neutron separation energies. The NLDs and $\gamma$SFs are used to calculate the corresponding $^{181}$Ta(n,$\gamma$) cross sections and these are compared to results from other techniques. The energy region of the scissors resonance strength is investigated and from the data and comparison to prior work it is concluded that the scissors strength splits into two distinct parts. This splitting may allow for the determination of triaxiality and a $\gamma$ deformation of $14.9^{\circ} \pm 1.8^{\circ}$ was determined for $^{181}$Ta.

A coincidence velocity map imaging spectrometer for ions and high-energy electrons to study inner-shell photoionization of gas-phase molecules.

We report on the design and performance of a double-sided coincidence velocity map imaging spectrometer optimized for electron-ion and ion-ion coincidence experiments studying inner-shell photoionization of gas-phase molecules with soft X-ray synchrotron radiation. The apparatus employs two microchannel plate detectors equipped with delay-line anodes for coincident, time- and position-resolved detection of photoelectrons and Auger electrons with kinetic energies up to 300 eV on one side of the spectrometer and photoions up to 25 eV per unit charge on the opposite side. We demonstrate its capabilities by measuring valence photoelectrons and ion spectra of neon and nitrogen and by studying channel-resolved photoelectron and Auger spectra along with fragment-ion momentum correlations for chlorine 2p inner-shell ionization of cis- and trans-1,2-dichloroethene.

Spectroscopic coincidence experiments in transmission electron microscopy

We demonstrate the feasibility of coincidence measurements on a conventional transmission electron microscope, revealing the temporal correlation between electron energy loss spectroscopy (EELS) and energy dispersive X-ray (EDX) spectroscopy events. We make use of a delay line detector with ps-range time resolution attached to a modified EELS spectrometer. We demonstrate that coincidence between both events, related to the excitation and deexcitation of atoms in a crystal, provides added information not present in the individual EELS or EDX spectra. In particular, the method provides EELS with a significantly suppressed or even removed background, overcoming the many difficulties with conventional parametric background fitting as it uses no assumptions on the shape of the background, requires no user input and does not suffer from counting noise originating from the background signal. This is highly attractive, especially when low concentrations of elements need to be detected in a matrix of other elements.

Photodouble ionization of water studied by photoelectron–photoelectron coincidence experiments

The photodouble ionization of the water molecule has been studied at about 20 eV excess energy by detecting in coincidence two photoelectrons of equal energy. Two types of measurements have been performed. In the first one the photon energy has been scanned in order to reconstruct the spectrum of the H2O2+ states; in the second, the photon energy has been fixed, the direction of one photoelectron has been chosen along the direction of the polarization axis of the incident radiation and the coincidence angular distribution of the two photoelectrons has been measured. The angular distributions show that, at variance with previous measurements in diatomic molecules, the emission of the two electrons along the antiparallel direction is highly favored.

Pentadiynylidene and Its Methyl-Substituted Derivates: Threshold Photoelectron Spectroscopy of R1-C5-R2 Triplet Carbon Chains.

Mass-selective threshold photoelectron spectroscopy in the gas phase was employed to characterize the dialkynyl triplet carbenes pentadiynylidene (HC5H), methylpentadiynylidene (MeC5H), and dimethylpentadiynylidene (MeC5Me). Diazo compounds were employed as precursors to generate the carbenes by flash pyrolysis. The R1-C5-R2 carbon chains were photoionized by vacuum ultraviolet (VUV) synchrotron radiation in photoelectron photoion coincidence (PEPICO) experiments. High-level ab initio computations were carried out to support the interpretation of the experiments. For the unsubstituted pentadiynylidene (R1 = R2 = H) the recorded spectrum yields an adiabatic ionization energy (IEad) of 8.36 ± 0.03 eV. In addition, a second carbene isomer, 3-(didehydrovinylidene)cyclopropene, with a singlet electronic ground state, was identified in the spectrum based on the IEad of 8.60 ± 0.03 eV and Franck-Condon simulations. We found that multireference computations are required to reliably calculate the IEad for this molecule. CASPT2 computations predicted an IEad = 8.55 eV, while coupled-cluster computations significantly overestimate the IE. The cyclic isomer is most likely formed from another isomer of the precursor present in the sample. Stepwise methyl-substitution of the carbene leads to a reduction of the IE to 7.77 ± 0.04 eV for methylpentadiynylidene and 7.27 ± 0.06 eV for dimethylpentadiynylidene. The photoionization and dissociative photoionization of the precursors is investigated as well.

Bayesian Analysis of Femtosecond Pump-Probe Photoelectron-Photoion Coincidence Spectra with Fluctuating Laser Intensities.

This paper employs Bayesian probability theory for analyzing data generated in femtosecond pump-probe photoelectron-photoion coincidence (PEPICO) experiments. These experiments allow investigating ultrafast dynamical processes in photoexcited molecules. Bayesian probability theory is consistently applied to data analysis problems occurring in these types of experiments such as background subtraction and false coincidences. We previously demonstrated that the Bayesian formalism has many advantages, amongst which are compensation of false coincidences, no overestimation of pump-only contributions, significantly increased signal-to-noise ratio, and applicability to any experimental situation and noise statistics. Most importantly, by accounting for false coincidences, our approach allows running experiments at higher ionization rates, resulting in an appreciable reduction of data acquisition times. In addition to our previous paper, we include fluctuating laser intensities, of which the straightforward implementation highlights yet another advantage of the Bayesian formalism. Our method is thoroughly scrutinized by challenging mock data, where we find a minor impact of laser fluctuations on false coincidences, yet a noteworthy influence on background subtraction. We apply our algorithm to data obtained in experiments and discuss the impact of laser fluctuations on the data analysis.

Bayesian probability theory to identify false coincidences in coincidence experiments

We describe a Bayesian formalism to analyse femtosecond pump-probe photoionization experiments with photoelectron-photoion coincidence (PEPICO) detection. This approach overcomes the drawback of extraordinary long data acquisition times of PEPICO detection. In extension to simply excluding false coincidences as previously [1], we here present an investigation of their influence on the underlying spectrum. The software is provided at https://github.com/fslab-tugraz/PEPICOBayes/.

Disentanglement of a Singlet Spin State in a Coincidence Stern-Gerlach Device

We analyze the spin coincidence experiment considered by Bell in the derivation of Bells theorem. We solve the equation of motion for the spin system with a spin Hamiltonian, Hz, where the magnetic field is only in the z-direction. For the specific case of the coincidence experiment where the two magnets have the same orientation the Hamiltonian Hz commutes with the total spin Iz, which thus emerges as a constant of the motion. Bells argument is then that an observation of spin up at one magnet A necessarily implies spin down at the other B. For an isolated spin system A-B with classical translational degrees of freedom and an initial spin singlet state there is no force on the spin particles A and B. The spins are fully entangled but none of the spin particles A or B are deflected by the Stern-Gerlach magnets. This result is not compatible with Bells assumption that spin 1/2 particles are deected in a Stern-Gerlach device. Assuming a more realistic Hamiltonian Hz + Hx including a gradient in x direction the total Iz is not conserved and fully entanglement is not expected in this case. The conclusion is that Bells theorem is not applicable to spin coincidence measurement originally discussed by Bell.

Time-resolved imaging of bound and dissociating nuclear wave packets in strong-field ionized iodomethane.

We report the results of a time-resolved coincident ion momentum imaging experiment probing nuclear wave packet dynamics in the strong-field ionization and dissociation of iodomethane (CH3I), a prototypical polyatomic system for photochemistry and ultrafast laser science. By measuring yields, kinetic energies, and angular distributions of CH3+ + I+ and CH3+ + I++ ion pairs as a function of the delay between two 25 fs, 790 nm pump and probe pulses, we map both, bound and dissociating nuclear wave packets in intermediate cationic states, thereby tracking different ionization and dissociation pathways. In both channels, we find oscillatory features with a 130 fs periodicity resulting from vibrational motion (C-I symmetric stretch mode) in the first electronically excited state of CH3I+. This vibrational wave packet dephases within 1 ps, in good agreement with a simple wave packet propagation model. Our results indicate that the first excited cationic state plays a key role in the dissociative ionization of CH3I and that it represents an important intermediate in the sequential double and multiple ionization at moderate intensities.

Recent studies of heavy ion transfer reactions using large solid angle spectrometers

We present selected results recently obtained in the study of heavy ion transfer reactions at energies close to the Coulomb barrier by employing the large solid angle magnetic spectrometer PRISMA. We discuss the production of neutron-rich heavy nuclei via multinucleon transfer processes and the related effects of secondary processes, in particular nucleon evaporation, studied in a high resolution kinematic coincidence experiment. We also present the recent results in the studies of neutron-neutron correlations for closed shell and superfluid systems.

Breakdown of the Spectator Concept in Low-Electron-Energy Resonant Decay Processes.

We suggest that low-energy electrons, released by resonant decay processes, experience substantial scattering on the electron density of excited electrons, which remain a spectator during the decay. As a result, the angular emission distribution is altered significantly. This effect is expected to be a common feature of low-energy secondary electron emission. In this Letter, we exemplify our idea by examining the spectator resonant interatomic Coulombic decay of Ne dimers. Our theoretical predictions are confirmed by a corresponding coincidence experiment.

Quantum Entanglement in Corpuses of Documents

We show that data collected from corpuses of documents violate the Clauser-Horne-Shimony-Holt version of Bell’s inequality (CHSH inequality) and therefore indicate the presence of quantum entanglement in their structure. We obtain this result by considering two concepts and their combination and coincidence operations consisting of searches of co-occurrences of exemplars of these concepts in specific corpuses of documents. Measuring the frequencies of these co-occurrences and calculating the relative frequencies as approximate probabilities entering in the CHSH inequality, we obtain manifest violations of the latter for all considered corpuses of documents. In comparing these violations with those analogously obtained in an earlier work for the same combined concepts in psychological coincidence experiments with human participants, also violating the CHSH inequality, we identify the entanglement as being carried by the meaning connection between the two considered concepts within the combination they form. We explain the stronger violation for the corpuses of documents, as compared to the violation in the psychology experiments, as being due to the superior meaning domain of the human mind and, on the other side, to the latter reaching a broader domain of meaning and being possibly also actively influenced during the experimentation. We mention some of the issues to be analyzed in future work such as the violations of the CHSH inequality being larger than the ‘Cirel’son bound’ for all of the considered corpuses of documents.

Time and position sensitive photon detector for coincidence measurements in the keV energy range.

The detection efficiency η of any particle detector is important, concerning acquisition time, but becomes even more critical when two particles are detected in coincidence, with a total efficiency η1η2, in order to allow a deeper understanding of complex processes induced by light or particle interaction with matter. Efficiency and resolution of a time and position sensitive x-ray detector are reported here. This system consists of a multilayer transmission photocathode and two micro-channel plates (MCPs) equipped with a delay line anode (DLA). The efficiency is found to be about 20% for Al Kα photons, while the spatial resolution is comparable to that of a standard DLA detector (about 100 μm). The fast response time of the detector combined with its efficiency should allow coincidence experiments between x-ray photons and other particles (electron, ions, etc.).

Selectivity of the Br 3d−1 Auger decays in HBr

The Auger decay of the spin-orbit and molecular-field split Br $3{d}^{\ensuremath{-}1}$ core holes in HBr is investigated, both by a photoelectron--Auger-electron coincidence experiment and by ab initio calculations based on the one-center approximation. The branching ratios for the Auger decay of the five different core-hole states to the $4p{(\ensuremath{\sigma},\ensuremath{\pi})}^{\ensuremath{-}2}$ dicationic final states are determined. Experimental and theoretical data are in good agreement and conform to results for the $4p{\ensuremath{\pi}}^{\ensuremath{-}2}$ final states from a previous analysis of the high-resolution conventional Auger-electron spectrum. The branching ratios for the Br $3{d}^{\ensuremath{-}1}$ Auger decay to the $4p{(\ensuremath{\sigma},\ensuremath{\pi})}^{\ensuremath{-}2}$ with \ensuremath{\Sigma} symmetry follow the propensity rule of ${L}_{2,3}VV$ Auger decay [S. Svensson, A. Ausmees, S. J. Osborne, G. Bray, F. Gel'mukhanov, H. \AA{}gren, A. Naves de Brito, O.-P. Sairanen, A. Kivim\aki, E. N\~ommiste, H. Aksela, and S. Aksela, Phys. Rev. Lett. 72, 3021 (1994)] stating that the oriented core holes decay preferentially by involving a valence electron from an orbital with the same spatial orientation. For the ${M}_{4,5}VV$ decay in HBr this propensity rule has to be supplemented by the requirement that the Auger-electron channel and the other valence orbital have the same preferential orientation. We also probe the influence of the Auger kinetic energy on the distortion of the photoline caused by the postcollision interaction effect. For small kinetic energies, differences between experimental results and theoretical predictions are identified.

All-optical atom trap as a target for MOTRIMS-like collision experiments

Momentum-resolved scattering experiments with laser-cooled atomic targets have been performed since almost two decades with MOTRIMS (Magneto-Optical Trap Recoil Ion Momentum Spectroscopy) setups. Compared to experiments with gas-jet targets, MOTRIMS features significantly lower target temperatures allowing for an excellent recoil ion momentum resolution. However, the coincident and momentum-resolved detection of electrons was long rendered impossible due to incompatible magnetic field requirements. Here we report on a novel experimental approach which is based on an all-optical $^6$Li atom trap that -- in contrast to magneto-optical traps -- does not require magnetic field gradients in the trapping region. Atom temperatures of about 2 mK and number densities up to 10$^9$ cm$^{-3}$ make this trap ideally suited for momentum-resolved electron-ion coincidence experiments. The overall configuration of the new trap is very similar to conventional magneto-optical traps. It mainly requires small modifications of laser beam geometries and polarization which makes it easily implementable in other existing MOTRIMS experiments.

Insights into 2- and 4(5)-Nitroimidazole Decomposition into Relevant Ions and Molecules Induced by VUV Ionization.

Nitromidazoles are relevant compounds of multidisciplinary interest, and knowledge of their physical-chemical parameters as well as their decomposition under photon irradiation is needed. Here we report an experimental and theoretical study of the mechanisms of VUV photofragmentation of 2- and 4(5)-nitromidazoles, compounds used as radiosensitizers in conjunction with radiotherapy as well as high-energy density materials. Photoelectron-photoion coincidence experiments, measurements of the appearance energies of the most important ionic fragments, density functional theory, and single-point coupled cluster calculations have been used to provide an overall insight into the energetics and structure of the different ionic/neutral products of the fragmentation processes. The results show that these compounds can be an efficient source of relevant CO, HCN, NO, and NO2 molecules and produce ions of particular astrophysical interest, like the isomers of azirinyl cation ( m/ z 40), predicted to exist in the interstellar medium, and protonated hydrogen cyanide ( m/ z 28).

Two-center interference in electron-impact ionization of molecular hydrogen

Fast (${E}_{0}=520\phantom{\rule{0.16em}{0ex}}\mathrm{eV}$) electron-impact ionization of molecular hydrogen (${\mathrm{H}}_{2}$) is studied experimentally and theoretically for a resolved molecular axis angle and 10 eV ejected electron energy. Fully differential cross sections were measured using an electron-electron-ion triple coincidence experiment in which the molecular axis direction is obtained for ionic ground-state dissociation. While predictions from the standard two-wave interference model are in strong disagreement with experiment a multicenter distorted-wave method obtains much better results. This demonstrates the importance of the multicenter ionic potential for the electron emission pattern at low energy and the failure of hitherto widely used simple models which treat molecular ionization as the coherent sum of atomic ionization amplitudes.

Unveiling a Selective Mechanism for the Inhibition of α-Synuclein Aggregation by β-Synuclein.

α-Synuclein (αS) is an intrinsically disordered protein that is associated with Parkinson’s disease (PD) through its ability to self-assemble into oligomers and fibrils. Inhibition of this oligomerization cascade is an interesting approach to developing therapeutical strategies and β-synuclein (βS) has been described as a natural negative regulator of this process. However, the biological background and molecular mechanisms by which this inhibition occurs is unclear. Herein, we focused on assessing the effect of βS on the aggregation of five αS pathological mutants linked to early-onset PD (A30P, E46K, H50Q, G51D and A53T). By coupling single molecule fluorescence spectroscopy to a cell-free protein expression system, we validated the ability of βS to act as a chaperone of αS, effectively inhibiting its aggregation. Interestingly, we found that βS does so in a selective manner, i.e., is a more effective inhibitor for certain αS pathological mutants—A30P and G51D—as compared to E46K, H50Q and A53T. Moreover, two-color coincidence experiments proved that this discrepancy is due to a preferential incorporation of βS into smaller oligomers of αS. This was validated by showing that the chaperoning effect was lost when proteins were mixed after being expressed individually. This study highlights the potential of fluorescence spectroscopy to deconstruct αS aggregation cascade and its interplay with βS.