Photon-matter Interaction Research Articles

Femtosecond Laser‐Induced Regulation of Photo‐ and Persistent Luminescence of Perovskite Crystals

AbstractManipulation of photoluminescence (PL) and persistent luminescence (PersL) provides a powerful tool for anti‐counterfeiting applications. Here, Sb3+‐doped CsCdCl3 perovskite single crystals (SCs) can be selectively irradiated via utilizing ultra‐fast femtosecond (fs) laser, creating tunable PL colors and PersL duration with high precision. The PL color of the synthesized SCs changes from cyan to orange along with the wavelength of the fs laser, for the successful regulation of the optical procedure from a single‐photon to a two‐photon absorption process. Moreover, an orange PersL of CsCdCl3:Sb3+ SC is observed after being charged with a fs laser, and the corresponding duration time can be feasibly controlled with the pump wavelength. In particular, CsCdCl3:Sb3+ is capable of ultrafast carrier capture (1 s) under fs laser compared to ultraviolet lamp pre‐irradiation enabling a high‐resolution micro‐PersL in photon trapping/de‐trapping modes. These findings not only give a new solution for the fabrication high‐resolution micro‐PL and trajectory‐writing micro‐PersL patterns, but also provide a deep insight to understand the photon–matter interactions.

MolDStruct: Modeling the dynamics and structure of matter exposed to ultrafast x-ray lasers with hybrid collisional-radiative/molecular dynamics.

We describe a method to compute photon-matter interaction and atomic dynamics with x-ray lasers using a hybrid code based on classical molecular dynamics and collisional-radiative calculations. The forces between the atoms are dynamically determined based on changes to their electronic occupations and the formation of a free electron cloud created from the irradiation of photons in the x-ray spectrum. The rapid transition from neutral solid matter to dense plasma phase allows the use of screened potentials, reducing the number of non-bonded interactions. In combination with parallelization through domain decomposition, the hybrid code handles large-scale molecular dynamics and ionization. This method is applicable for large enough samples (solids, liquids, proteins, viruses, atomic clusters, and crystals) that, when exposed to an x-ray laser pulse, turn into a plasma in the first few femtoseconds of the interaction. We present four examples demonstrating the applicability of the method. We investigate the non-thermal heating and scattering of bulk water and damage-induced dynamics of a protein crystal using an x-ray pump-probe scheme. In both cases, we compare to the experimental data. For single particle imaging, we simulate the ultrafast dynamics of a methane cluster exposed to a femtosecond x-ray laser. In the context of coherent diffractive imaging, we study the fragmentation as given by an x-ray pump-probe setup to understand the evolution of radiation damage in the time range of hundreds of femtoseconds.

On a Spectral Method for β-particle Bound Excitation Collisions in Kilonovae

The interaction of β-particles with the weakly ionized plasma background is an important mechanism for powering the kilonova (KN) transient signal from neutron star mergers. For this purpose, we present an implementation of the approximate fast-particle collision kernel, described by Inokuti following the seminal formulation of Bethe, in a spectral solver of the Vlasov–Maxwell–Boltzmann equation. In particular, we expand the fast-particle plane-wave atomic excitation kernel into coefficients of the Hermite basis, and derive the relevant discrete spectral system. In this fast-particle limit, the approach permits the direct use of atomic data, including optical oscillator strengths, normally applied to photon–matter interaction. The resulting spectral matrix is implemented in the MASS-APP spectral solver framework, in a way that avoids full matrix storage per spatial zone. We numerically verify aspects of the matrix construction, and present a proof-of-principle 3D simulation of a 2D axisymmetric KN ejecta snapshot. Our preliminary numerical results indicate that a reasonable choice of Hermite basis parameters for β-particles in the KN is a bulk velocity parameter u = 0, a thermal velocity parameter α = 0.5c, and a 9 × 9 × 9 mode velocity basis set (Hermite orders of 0–8 in each dimension). For interior-ejecta sample zones, we estimate that the ratio of thermalization from large-angle (≳2.°5) bound excitation scattering to total thermalization is ∼0.002–0.003.

Exposure Buildup Factors in Concrete, Lead for Point Isotropic and Unidirectional Photon Sources in the Energy Range from 10 to 50 MeV

Abstract The exposure buildup factors in concrete and lead for a point isotropic and flat unidirectional photon source in the energy range from 10 to 50 MeV were determined using Monte Carlo simulation “FLUKA” software. The exposure buildup factors were also obtained for different material thickness up to 40 mpf. The calculations were done in a barrier geometry where the contributions of all photon-matter interactions were taken into account in the performed calculations. Amendments for the barrier-geometry effect for both materials under study were deduced. The results showed that barrier-effect amendments were independent of the material thickness, material type, and energy of the photon source

On the Wave-Particle Duality of the Photons and the Matter-Photon Particle Mixture Model

Relativistic quantum mechanics and many experimental results and observations show that electron-positron annihilation can produce photons; photon-matter and photon-photon interaction can also create electrons and positrons. The photons have no rest mass, e.g. relative to Lab frame, and always travel at the speed of light in the vacuum. In this paper, a rotational moving electric dipole model with negative and positive charges was proposed for photons. In a vacuum, the electric dipoles are moving in a twisted helical motion around their propagation axis (their center of mass). Photon particles are traveling at the speed of light along the propagation axis. This pair of negative and positive charged particles exerts both electrostatic and magnetic force on each other. Both forces are attractive and act as a centripetal force to keep the electric dipole in a continuous helical motion around the axis of rotation. With this model, the wave-particle duality of photons can be described simultaneously. The space is filled by matter (having rest mass relative to Lab frame) and photons (without rest mass); it is a multicomponent mixture fluid. In "vacuum", though there is no rest matter particle, but there are still photon gas particles, the total energy-momentum tensor should include rest matter particles and photon gas particles.

Evaluation of radiation shielding potentials of Ni-based alloys, Inconel-617 and Incoloy-800HT, candidates for high temperature applications especially for nuclear reactors, by EpiXS and Phy-X/PSD codes

In this paper, our purpose is to calculate photon-matter interaction parameters of Ni-based alloys, Inconel-617 and Incoloy-800HT, which are the main candidates for high-temperature applications such as spacecraft, gas turbines, nuclear reactors and rocket motors. The radiation attenuation parameters and buildup factors were obtained in a wide energy range by using Phy-X/PSD and EpiXS softwares to determine the radiation protection capabilities of the alloys. Fast neutron removal cross sections of the alloys were also calculated. It was observed that Inconel-617 has higher shielding ability than Incoloy-800HT. The shielding potentials of the alloys were compared with those of other shielding materials (ordinary concrete, hematite-serpenite, ilmenite-limonite, steel-scrap, basalt-magnetite, steel-magnetite and ilmenite concretes) reported before, and it was concluded that Inconel-617 and Incoloy-800HT have more shielding ability than those.

Effects of Cascading Optical Processes: Part III. Impacts on Spectroscopic Measurements of Fluorescent Samples.

Cascading optical processes involve sequential photon-matter interactions triggered by the same individual excitation photons. Parts I and II of this series explored cascading optical processes in scattering-only solutions (Part I) and solutions with light scatterers and absorbers but no emitters (Part II). The current work (Part III) focuses on the effects of cascading optical processes on spectroscopic measurements of fluorescent samples. Four types of samples were examined: (1) eosin Y (EOY), an absorber and emitter; (2) EOY mixed with plain polystyrene nanoparticles (PSNPs), which are pure scatterers; (3) EOY mixed with dyed PSNPs, which scatter and absorb light but do not emit; and (4) fluorescent PSNPs that are simultaneous light absorbers, scatterers, and emitters. Interference from both forward scattered and emitted photons can cause nonlinearity and spectral distortion in UV-vis extinction measurements. Sample absorption by nonfluorogenic chromophores reduces fluorescence intensity, while the effect of scattering on fluorophore fluorescence is complicated by several competing factors. A revised first-principles model is developed for correlating the experimental fluorescence intensity with the sample absorbance in solutions containing both scatterers and absorbers. The optical properties of fluorescent PSNPs of three different sizes were systematically investigated by using integrating-sphere-assisted resonance synchronous spectroscopy, linearly polarized resonance synchronous spectroscopy, UV-vis, and fluorescence spectroscopy. The insights and methodology provided in this work should help improve the reliability of spectroscopic analyses of fluorescent samples, where the interplay among light absorption, scattering, and emission can be complex.

Radiation and Emission Phenomena in Combination

Radiation and Emission Phenomena in Combination

Topological super-modes engineering with acoustic graphene plasmons.

Acoustic graphene plasmons (AGPs) in a graphene-dielectric-metal structure possess extreme field localization and low loss, which have promising applications in strong photon-matter interaction and integrated photonic devices. Here, we propose two kinds of one-dimensional crystals supporting propagating AGPs with different topological properties, which is confirmed by the Zak phase calculations and the electric field symmetry analysis. Moreover, by combining these two plasmonic crystals to form a superlattice system, the super-modes exist because of the coupling between isolated topological interface states. A flat-like dispersion of super-modes is observed by designing the superlattice. These results should find applications in optical sensing and integrating photonic devices with plasmonic crystals.

On the application of Jacobian-free Riemann solvers for relativistic radiation magnetohydrodynamics under M1 closure

Radiative transfer plays a major role in high-energy astrophysics. In multiple scenarios and in a broad range of energy scales, the coupling between matter and radiation is essential to understand the interplay between theory, observations and numerical simulations. In this paper, we present a novel scheme for solving the equations of radiation relativistic magnetohydrodynamics within the parallel code Lóstrego. These equations, which are formulated taking successive moments of the Boltzmann radiative transfer equation, are solved under the grey-body approximation and the M1 closure using an IMEX time integration scheme. The main novelty of our scheme is that we introduce for the first time in the context of radiation magnetohydrodynamics a family of Jacobian-free Riemann solvers based on internal approximations to the Polynomial Viscosity Matrix, which were demonstrated to be robust and accurate for non-radiative applications. The robustness and the limitations of the new algorithms are tested by solving a collection of one-dimensional and multi-dimensional test problems, both in the free-streaming and in the diffusion radiation transport limits. Due to its stable performance, the applicability of the scheme presented in this paper to real astrophysical scenarios in high-energy astrophysics is promising. In future simulations, we expect to be able to explore the dynamical relevance of photon-matter interactions in the context of relativistic jets and accretion discs, from microquasars and AGN to gamma-ray bursts.

The DREAM Endstation at the Linac Coherent Light Source

Free-electron lasers (FEL), with their ultrashort pulses, ultrahigh intensities, and high repetition rates at short wavelength, have provided new approaches to Atomic and Molecular Optical Science. One such approach is following the birth of a photo electron to observe ion dynamics on an ultrafast timescale. Such an approach presents the opportunity to decipher the photon-initiated structural dynamics of an isolated atomic and molecular species. It is a fundamental step towards understanding single- and non-linear multi-photon processes and coherent electron dynamics in atoms and molecules, ultimately leading to coherent control following FEL research breakthroughs in pulse shaping and polarization control. A key aspect for exploring photoinduced quantum phenomena is visualizing the collective motion of electrons and nuclei in a single reaction process, as dynamics in atoms/ions proceed at femtosecond (10−15 s) timescales while electronic dynamics take place in the attosecond timescale (10−18 s). Here, we report on the design of a Dynamic Reaction Microscope (DREAM) endstation located at the second interaction point of the Time-Resolved Molecular and Optical (TMO) instrument at the Linac Coherent Light Source (LCLS) capable of following the photon–matter interactions by detecting ions and electrons in coincidence. The DREAM endstation takes advantage of the pulse properties and high repetition rate of LCLS-II to perform gas-phase soft X-ray experiments in a wide spectrum of scientific domains. With its design ability to detect multi-ions and electrons in coincidence while operating in step with the high repetition rate of LCLS-II, the DREAM endstation takes advantage of the inherent momentum conservation of reaction product ions with participating electrons to reconstruct the original X-ray photon–matter interactions. In this report, we outline in detail the design of the DREAM endstation and its functionality, with scientific opportunities enabled by this state-of-the-art instrument.

A comprehensive study on structural properties, photon and particle attenuation competence of CoNiFeCr-Ti/Al high entropy alloys (HEAs)

It is well known that high entropy alloys (HEAs) have a wide range of potential applications as radiation shielding due to their superior properties. The CoNiFeCr-Ti/Al compositions were chosen for their low cost as HEA in this study. The HEAs were successfully produced using the mechanical alloying (MA) method with equimolar CoNiFeCr, CoNiFeCrAl, and CoNiFeCrTi compositions. The production and structural properties of the alloys were investigated in detail. Besides, the photon and particle radiation shielding properties of the HEAs were calculated with the help of Phy-X/PSD, SRIM (10 keV-20 MeV), and ESTAR (10 keV-20 MeV) programs. The photon-matter interaction parameters were calculated in both specific photon energies emitted from 241Am, 133Ba, 109Cd, 60Co, 137Cs, 131I, and 22Na nuclides and a continuous energy range of 15 keV-15 MeV. The characterization of the alloys was investigated by using X-ray diffraction (XRD) and scanning electron microscopes (SEM) attached to an energy dispersive spectroscopy (EDX). It was found that the HEAs have a highly amorphous structure due to the selected production method. The crystal size of the alloys was calculated as 70, 35, and 20 nm for CoNiFeCr, CoNiFeCrAl, and CoNiFeCrTi, respectively. In terms of shielding properties, it has been determined that the produced HEAs have better shielding characteristics for photon and particle radiations than standard shielding concretes. In addition, the results demonstrated that CoNiFeCr alloy, which has the best shielding ability among the HEA alloys, can be used as a shielding material application requiring photon, electron, proton, alpha, and neutron radiations.

Relativistic dilation and contraction of the probabilities of quantum states of light at angular incidence

In this work we propose a formulation for the treatment of quantized states of light in photon-matter interaction. It is built in the multidimensional Hilbert space to describe the orbital angular momentum states, in such that probabilities naturally arise in a relativistic setting. Our findings indicate that the classical-relativistic variability of the probabilities can describe the quantized states of light, with the state variable being the variation of the photon angular momentum. It was verified that the probability to find a specific quantized state of light at angular incidence can be treated by relativistic probabilities. Interestingly, our results indicate that, when both states have equal odds, there is a synchronization between source and observer. We found that the relativistic effect in the perspective of the source referential is able to change the odds of an event occurring, dilating and contracting the probabilities of finding a quantized state of light at angular incidence.

Quantitative assessment of a beam hole scatter correction in industrial computed tomography

Abstract In industrial Computed Tomography (CT), scattered radiation causes a loss of quality of the reconstructed 3D volume. Scatter is caused by photon-matter interaction, whereby a photon is deflected from its initial propagation direction. The most prominent contributor to scattered radiation in the scope of photon energies occurring in industrial CT is Compton Scattering. With the used Beam Hole Array (BHA) technology for scatter correction, scatter intensities are determined by subtracting the primary intensities, which are gathered behind small apertures from the total intensities, which are gathered in the absence of the apertures. Intensities measured behind the apertures are assumed to be scatter free, since the transversal components of the radiation are strongly reduced. The scatter correction is performed by subtracting scatter intensities from primary intensities in the projection image. Improvements are evaluated for a newly developed test specimen considering image quality metrics and dimensional accuracy. The contrast could be improved especially for small structures. Cupping artifacts that express as systematic offset of grey values rising with the penetration length were reduced. Measurement deviations towards tactile references were decreased.

Scatter Correction and Contrast Improvement of Concrete Objects Using Monte Carlo Method

Estimating the load-carrying capacity of concrete structures is a major challenge as the infrastructure industry thrives to reduce the consumption of concrete for environmental concerns as well as improving the cost and time efficiency of infrastructural projects. Quantifying such load-carrying capacity needs a detailed study of the micro-structures of the concrete mixture composed of stones, reinforcement, and cement matrix. Computed Tomography (CT) provides a reliable nondestructive technique to analyze and segment the different materials within the concrete structures. However, CT is normally accompanied by different kinds of artifacts that highly degrades the quality of the reconstructed image. Among these artifacts, scatter imposes severe degradation of the quality of the image including reduced contrast between different materials, cupping and streaks artifacts. Several methods were used to remove the scatter effect. The most effective way to correct for the scatter effect is by the use of the Monte Carlo (MC) method due to the accurate modeling of the physics accompanying the photon matter interaction. In this work, a fast MC photon transport model accelerated over the use of the GPU(s) platforms is developed. It is extensively verified against several well-known simulators and experimentally has been used to correct the scatter effect and to improve the contrast between the concrete component.

Imaging of femtosecond bond breaking and charge dynamics in ultracharged peptides.

X-ray free-electrons lasers have revolutionized the method of imaging biological macromolecules such as proteins, viruses and cells by opening the door to structural determination of both single particles and crystals at room temperature. By utilizing high intensity X-ray pulses on femtosecond timescales, the effects of radiation damage can be reduced. Achieving high resolution structures will likely require knowledge of how radiation damage affects the structure on an atomic scale, since the experimentally obtained electron densities will be reconstructed in the presence of radiation damage. Detailed understanding of the expected damage scenarios provides further information, in addition to guiding possible corrections that may need to be made to obtain a damage free reconstruction. In this work, we have quantified the effects of ionizing photon-matter interactions using first principles molecular dynamics. We utilize density functional theory to calculate bond breaking and charge dynamics in three ultracharged molecules and two different structural conformations that are important to the structural integrity of biological macromolecules, comparing to our previous studies on amino acids. The effects of the ultracharged states and subsequent bond breaking in real space are studied in reciprocal space using coherent diffractive imaging of an ensemble of aligned biomolecules in the gas phase.

Intense laser matter interaction in atoms, finite systems and condensed media: recent experiments and theoretical advances

This special issue of the European Journal of Physics: Special Topics entitled “Intense Laser Matter Interaction in Atoms, Finite Systems and Condensed Media” published a set of 21 articles aiming to put in perspective this burgeoning area of science, application and technology. The invention of chirped pulse amplification by Strickland and Mourou, which led to their Nobel prizes in 2018, has ushered in a new era in photon–matter interaction where coherent intense light pulses in the optical and infrared domains play a central role. This development has not only called in creative experimental methods, but has demanded new theoretical approaches working in the non-perturbative and highly nonlinear regimes of light–matter interaction. Both for fundamental physics as well as key applications these have played an essential role. Key pillars of this subject, captured in this collection, are laser-induced nanometer-scale plasmas ignited in unsupported nanoparticles, laser-based particle acceleration taking advantage of unprecedented field gradients, the generation of high-order harmonics opening up attosecond science and ultrafast X-ray spectroscopy, and the generation of terahertz pulses for time-domain spectroscopy of new materials.

Sub pixel resolution using spectral-spatial encoding in x-ray imaging.

Previous efforts at increasing spatial resolution have relied on decreasing focal spot and or detector element size. Many "super resolution" methods require physical movement of a component of the imaging system. This work describes a method for achieving spatial resolution on a scale smaller than the detector pixel without motion of the object or detector. We introduce a weighting of the photon energy spectrum on a length scale smaller than a single pixel using a physical filter that can be placed between the focal spot and the object, between the object and the detector, or integrated into the x-ray source or detector. We refer to the method as sub pixel encoding (SPE). We show that if one acquires multiple measurements (i.e. x-ray projections), information can be synthesized at a spatial scale defined by the spectrum modulation, not the detector element size. Specifically, if one divides a detector pixel into n sub regions, and m photon-matter interactions are present, the number of x-ray measurements needed to solve for the detector response of each sub region is mxn. We discuss realizations of SPE using multiple x-ray spectra with an energy integrating detector, a single spectra with a photon counting detector, and the single photon-matter interaction case. We demonstrate the feasibility of the approach using a simulated energy integrating detector with a detector pitch of 2 mm for 80-140 kV medical and 200-600 kV industrial applications. Phantoms used for both example SPE realization had some features only a 1 mm detector could resolve. We calculate the covariance matrix of SPE output to characterize the and noise propagation and correlation of our test examples. The mathematical foundation of SPE is provided, with details worked out for several detector types and energy ranges. Two numerical simulations were provided to demonstrate feasibility. In both the medical and industrial simulations, some phantom features were only observable with the 1 mm and SPE synthesized 2 mm detector, while the 2 mm detector was not able to visualize them. Covariance matrix analysis demonstrated negative diagonal terms for both example cases. The concept of encoding object information at a length scale smaller than a single pixel element, and then retrieving that information was introduced. SPE simultaneously allows for an increase in spatial resolution and provides "dual energy" like information about the underlying photon-matter interactions.

LaTaON2 Mesoporous Single Crystals for Efficient Photocatalytic Water Oxidation and Z-Scheme Overall Water Splitting.

LaTaON2 porous single crystals (PSCs), integrating structural coherence and porous microstructures, will warrant promising photocatalytic performance. The absence of grain boundaries in PSCs ensures rapid photocarrier transportation from bulk to the surface, thereby mitigating photocarriers' recombination. Porous microstructures not only provide ample reachable surface to host photochemical reactions but also reinforce photon-matter interactions by additional photon reflection/scattering. Here, we have synthesized LaTaON2 PSCs via a topotactic route and show significantly improved photocatalytic performance. Efficient water oxidation into O2 has been realized by LaTaON2 PSCs with an apparent quantum efficiency as high as 5.7% at 420 ± 20 nm. Stable overall water splitting into stoichiometric H2 and O2 has also been achieved in a Z-scheme setup using LaTaON2 PSCs as the O2 evolution photocatalyst. These results not only prove that PSCs facilitate photocarrier migrations, which in turn deliver exceptional photocatalytic performance, but also imply that PSCs are useful to reinvigorate conventional semiconductor photocatalysts toward efficient solar energy conversions.

Trivalent Ions and Their Impacts on Effective Conductivity at 300 K and Radio-Protective Behaviors of Bismo-Borate Glasses: A Comparative Investigation for Al, Y, Nd, Sm, Eu.

We aimed to determine the contribution of various trivalent ions like Al and rare-earths (Y, Nd, Sm, Eu) on resistance behaviors of different types of bismo-borate glasses. Accordingly, eight different bismuth borate glasses from the system: 40Bi2O3–59B2O3–1Tv2O3 (where Tv = Al, Y, Nd, Sm, and Eu) and three glasses of (40Bi2O3–60B2O3; 37.5Bi2O3–62.5B2O3; and 38Bi2O3–60B2O3–2Al2O3) compositions were extensively investigated in terms of their nuclear attenuation shielding properties, along with effective conductivity and buildup factors. The Py-MLBUF online platform was also utilized for determination of some essential parameters. Next, attenuation coefficients, along with half and tenth value layers, have been determined in the 0.015 MeV–15 MeV photon energy range. Moreover, effective atomic numbers and effective atomic weight, along with exposure and energy absorption buildup factors, were determined in the same energy range. The result showed that the type of trivalent ion has a direct effect on behaviors of bismo-borate glasses against ionizing gamma-rays. As incident photon energy increases, the effective thermal conductivity decreases rapidly, especially in the low energy range, where photoelectric effects dominate the photon–matter interaction. Sample 8 had the minimum heat conductivity at low photon energies; our findings showed that Eu-reinforced bismo-borate glass composition, namely 40Bi2O3–59B2O3–1Eu2O3, with a glass density of 6.328 g/cm3 had superior gamma-ray attenuation properties. These outcomes would be useful for the scientific community to observe the most suitable additive rareearth type and related glass composition for providing the aforementioned shielding properties, in terms of needs and utilization requirements.