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DOE OSTI2022

Controlling Symmetry Breaking Charge Transfer in BODIPY Pairs

Symmetry breaking charge transfer (SBCT) is a process in which a pair of identical chromophores absorb a photon and use its energy to transfer an electron from one chromophore to the other, breaking the symmetry of the chromophore pair. This excited state phenomenon is observed in photosynthetic organisms where it enables efficient formation of separated charges that ultimately catalyze biosynthesis. SBCT has also been proposed as a means for developing photovoltaics and photocatalytic systems that operate with minimal energy loss. It is known that SBCT in both biological and artificial systems is in part made possible by the local environment in which it occurs, which can move to stabilize the asymmetric SBCT state. However, how environmental degrees of freedom act in concert with steric and structural constraints placed on a chromophore pair to dictate its ability to generate long-lived charge pairs via SBCT remain open topics of investigation. In this work we compare a broad series of dipyrrin dimers that are linked by distinct bridging groups to discern how the spatial separation and mutual orientation of linked chromophores and the structural flexibility of their linker each impact SBCT efficiency. Across this material set, we observe a general trend that SBCT is accelerated as the spatial separation between dimer chromophores decreases, consistent with the expectation that the electronic coupling between these units varies exponentially with their separation. However, one key observation is that the rate of charge recombination following SBCT was found to slow with decreasing interchromophore separation, rather than speed up. This stems from an enhancement of the dimers’ structural rigidity due to increasing steric repulsion as the length of their linker shrinks. This rigidity further inhibits charge recombination in systems where symmetry has already enforced zero HOMO-LUMO overlap. Additionally, for the forward transfer the active torsion is shown to increase LUMO-LUMO coupling, allowing for faster SBCT within bridging groups. Further, by understanding trends for how rates of SBCT and charge recombination depend on a dimer’s internal structure and their environment, we identify design guidelines for creating artificial systems for driving sustained light-induced charge separation. Such systems can find application in solar energy technologies and photocatalytic applications but can serve as a model for light-induced charge separation in biological systems.

14 SOLAR ENERGY↗

NASA NTRS2014

Supernova Bounds on the Dark Photon Using Its Electromagnetic Decay

The hypothetical massive dark photon (gamma′) which has kinetic mixing with the SM photon can decay electromagnetically to e+ e− pairs if its mass m exceeds 2m(sub e), and otherwise into three SM photons. These decays yield cosmological and supernovae associated signatures. We briefly discuss these signatures, particularly in connection with the supernova SN1987A, and delineate the extra constraints that arise on the mass and mixing parameter of the dark photon. In particular, we find that for dark photon mass m(sub gamma') in the 5-20 MeV range arguments based on supernova 1987A observations lead to a bound on epsilon which is about 300 times stronger than the presently existing bounds based on energy loss arguments.

Supernova bounds on the dark photon using its elec↗

DOE OSTI2022

Quantum vacuum processes in the extremely intense light of relativistic plasma mirror sources

Abstract The advent of petawatt-class laser systems allows generating electromagnetic fields of unprecedented strength in a controlled environment, driving increasingly more efforts to probe yet unobserved processes through their interaction with the quantum vacuum. Still, the lowest intensity scale governing these effects lies orders of magnitude beyond foreseen capabilities, so that such endeavor is expected to remain extremely challenging. In recent years, however, plasma mirrors have emerged as a promising bridge across this gap, by enabling the conversion of intense infrared laser pulses into coherently focused Doppler harmonic beams lying in the X-UV range. In this work, we present predictions on the quantum vacuum signatures produced when such beams are focused to intensities between 10 24 and 10 28 W cm −2 , specifically photon–photon scattering and electron–positron pair creation. These signatures are computed via the stimulated vacuum formalism, combined with a model of perfectly focused beam built from PIC-generated harmonics spectra, and implemented on state-of-the-art massively parallel numerical tools. In view of identifying experimentally favorable configurations, we also consider the coupling of the focused harmonic beam with an auxiliary optical beam, and provide comparison with other established schemes. Our results show that a single coherently focused harmonic beam can produce as much scattered photons as two infrared pulses in head-on collision, and confirm that the coupling of the harmonic beam to an auxiliary beam gives rise to significant levels of inelastic scattering, and hence holds the potential to strongly improve the attainable signal to noise ratios in experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1999

Magnetic Photon Splitting: The S-Matrix Formulation in the Landau Representation

Calculations of reaction rates for the third-order QED process of photon splitting gamma yields gamma.gamma in strong magnetic fields traditionally have employed either the effective Lagrangian method or variants of Schwinger's proper-time technique. Recently, Mentzel, Berg and Wunner [1] presented an alternative derivation via an S-matrix formulation in the Landau representation. Advantages of such a formulation include the ability to compute rates near pair resonances above pair threshold. This paper presents new developments of the Landau representation formalism as applied to photon splitting, providing significant, advances beyond the work of [1] by summing over the spin quantum numbers of the electron propagators, and analytically integrating over the component of momentum of the intermediate states that is parallel to field. The ensuing tractable expressions for the scattering amplitudes are satisfyingly compact, and of an appearance familiar to S-matrix theory applications. Such developments can facilitate numerical computations of splitting considerably both below and above pair threshold. Specializations to two regimes of interest are obtained, namely the limit of highly supercritical fields and the domain where photon energies are far inferior to that for the threshold of single-photon pair creation. In particular, for the first time the low-frequency amplitudes are simply expressed in terms of the Gamma function, its integral and its derivatives. In addition, the equivalence of the asymptotic forms in these two domains to extant results from effective Lagrangian/proper- time formulations is demonstrated.

Baring, Matthew G.↗

DOE OSTI2025

Quantum nonlocal modulation cancelation with distributed clocks

We demonstrate nonlocal modulation of entangled photons with truly distributed radio frequency (RF) clocks. Leveraging a custom radio-over-fiber (RFoF) system characterized via classical spectral interference, we validate its effectiveness for quantum networking by multiplexing the RFoF clock with one photon from a frequency-bin-entangled pair and distributing the coexisting quantum-classical signals over fiber. Phase modulation of the two photons reveals nonlocal correlations in excellent agreement with theory: in-phase modulation produces additional sidebands in the joint spectral intensity, while out-of-phase modulation is nonlocally canceled. Our simple, feedback-free design attains subpicosecond synchronization—namely, drift less than ~0.5 ps in a 5.5 km fiber over 30 min (fractionally only ~2×10 -8 of the total fiber delay)—and should facilitate frequency-encoded quantum networking protocols such as high-dimensional quantum key distribution and entanglement swapping, unlocking frequency-bin qubits for practical quantum communications in deployed metropolitan-scale networks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1981

On the theory of Gamma Ray Amplification through Stimulated Annihilation Radiation (GRASAR)

The theory of photon emission, absorption, and scattering in a relativistic plasma of positrons, electrons, and photon was studied. Expressions for the emissivities and absorption coefficients of pair annihilation, pair production, and Compton scattering are given and evaluated numerically. The conditions for negative absorption were investigated. In a system of photons and e(+) - e(-) pairs, an emission line at at approximately 0.43 MeV can be produced by grasar action provided that the pair chemical potential exceeds approximately 1 MeV. At a temperature of approximately 10 to the 9th power. This requires a pair density approximately 10 to the 30th power cm to the (-3) power a value much larger than the thermodynamic equilbrium pair density at this temperature. This emission line could account without a gravitational redshift for the observed lines at this energy from gamma ray bursts.

Ramaty, R.↗

DOE OSTI2022

Measurement of the inclusive and differential $t\overline{t}γ$ cross sections in the dilepton channel and effective field theory interpretation in proton-proton collisions at $\sqrt{s}$ = 13 TeV

The production cross section of a top quark pair in association with a photon is measured in proton-proton collisions in the decay channel with two oppositely charged leptons (e ± μ ∓ , e + e - , or μ + μ - ). The measurement is performed using 138 fb -1 of proton-proton collision data recorded by the CMS experiment at √s = 13 TeV during the 2016–2018 data-taking period of the CERN LHC. A fiducial phase space is defined such that photons radiated by initial-state particles, top quarks, or any of their decay products are included. An inclusive cross section of 175.2 ± 2.5(stat) ± 6.3(syst) fb is measured in a signal region with at least one jet coming from the hadronization of a bottom quark and exactly one photon with transverse momentum above 20 GeV. Differential cross sections are measured as functions of several kinematic observables of the photon, leptons, and jets, and compared to standard model predictions. The measurements are also interpreted in the standard model effective field theory framework, and limits are found on the relevant Wilson coefficients from these results alone and in combination with a previous CMS measurement of the tt¯γ production process using the lepton+jets final state.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Measurement of the inclusive and differential $t\overline{t}γ$ cross sections in the single-lepton channel and EFT interpretation at $\sqrt{s}$ = 13 TeV

The production cross section of a top quark pair in association with a photon is measured in proton-proton collisions at a center-of-mass energy of 13 TeV. The data set, corresponding to an integrated luminosity of 137 fb -1 , was recorded by the CMS experiment during the 2016–2018 data taking of the LHC. The measurements are performed in a fiducial volume defined at the particle level. Events with an isolated, highly energetic lepton, at least three jets from the hadronization of quarks, among which at least one is b tagged, and one isolated photon are selected. The inclusive fiducial $t\overline{t}γ$ cross section, for a photon with transverse momentum greater than 20 GeV and pseudorapidity |η| < 1.4442, is measured to be 798 ± 7(stat) ± 48(syst) fb, in good agreement with the prediction from the standard model at next-to-leading order in quantum chromodynamics. The differential cross sections are also measured as a function of several kinematic observables and interpreted in the framework of the standard model effective field theory (EFT), leading to the most stringent direct limits to date on anomalous electromagnetic dipole moment interactions of the top quark and the photon.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Modulation of Electrostatic Potential in 2D Crystal Engineered by an Array of Alternating Polar Molecules

The moiré potential in rotationally misfit two-dimensional (2D) heterostructures has been used to build artificial exciton and electron lattices, which have become platforms for realizing exotic electronic phases. Here, we demonstrate a different approach to create a superlattice potential in 2D crystals by using the near field of an array of polar molecules. Here, a bilayer of titanyl phthalocyanine (TiOPc), consisting of alternating out-of-plane dipoles, is deposited on monolayer MoS 2 . Time-resolved two-photon photoemission spectroscopy reveals a pair of interlayer exciton states with an energy difference of ~0.1 eV, which is consistent with the electrostatic potential modulation induced by the TiOPc bilayer as determined by density functional theory calculations. Because the symmetry and the period of this potential superlattice can be changed readily by using molecules of different shapes and sizes, molecule/2D heterostructures can be promising platforms for designing artificial exciton and electron lattices.

2D heterostructures↗

DOE OSTI2025

Search for Reactor-Produced Millicharged Particles with Skipper-CCDs at the CONNIE and Atucha-II Experiments

Millicharged particles, proposed by various extensions of the standard model, can be created in pairs by high-energy photons within nuclear reactors and can interact electromagnetically with electrons in matter. Recently, the existence of a plasmon peak in the interaction cross section with silicon in the eV range was highlighted as a promising approach to enhance low-energy sensitivities. The CONNIE and Atucha-II reactor neutrino experiments utilize Skipper-CCD sensors, which enable the detection of interactions in the eV range. We present world-leading limits on the charge of millicharged particles within a mass range spanning 6 orders of magnitude, derived through a comprehensive analysis and the combination of data from both experiments. Published by the American Physical Society 2025

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

New Materials for Photoelectrochemical Energy Conversion

This review concerns light-to-chemical energy conversion, focusing on approaches that could be driven by terrestrial sunlight to produce hydrogen and/or reduce carbon dioxide. Recent advances in photocatalytic (PC) and photoelectrocatalytic (PEC) materials are covered. In both approaches, the electron-hole pairs that are created by photon absorption must travel in specific directions to the sites that mediate multielectron bond making/breaking redox reactions. Thermodynamic requirements for materials stability are described, although some recently discovered materials appear to be exceptions. For PC materials, the importance of rate matching between reduction and oxidation processes and the mass transfer of intermediates and products is emphasized. Surprisingly, metal sulfides appear to be promising for PC carbon dioxide reduction. For PEC materials, recent work elucidating the elementary step mechanism for oxygen evolution on metal oxides and the discovery of chalcogen-based photocathode materials capable of sustained light-driven CO 2 reduction are discussed.

energy conversion↗

NASA NTRS1971

Gamma-ray absorption for a beam model of the Crab nebula pulsar NP0532

A model is discussed for determining gamma ray absorption from NP0532 by estimating the effect of beaming as indicated by the pulsations. The main absorption process is considered to be that of pair production in the intense photon field which occurs during the pulse. The results indicate that for this model, absorption does not occur below 10 GeV.

Stecker, F. W.↗

NASA NTRS1976

Energetics of the midlatitude thermosphere

Thermospheric energetics is examined from the point of view of atomic and molecular processes which convert solar EUV radiative energy into kinetic energy of the ambient electron, ion, and neutral gases. The energy flow from photon to photoelectron-ion pair through energy loss and ion-molecule transfer to eventual electron-ion recombination is traced in detail. Upper and lower bounds are placed on the efficiency of conversion of radiative to thermal energy. Implications for the question of consistency of measured solar EUV fluxes and ionospheric models are discussed.

Stolarski, R. S.↗

NASA NTRS1981

Synchrotron cooling and annihilation of an e/+/-e/-/ plasma - The radiation mechanism for the 5 March, 1979 transient

Positron-electron pair radiation is examined as a mechanism that could be responsible for the impulsive phase emission of the 5 March, 1979 transient. Synchrotron cooling and subsequent annihilation of the pairs can account for the energy spectrum, the very high brightness, and the 0.4 MeV feature observed from this transient, whose source is likely to be a neutron star in the supernova remnant N49 in the Large Magellanic Cloud. In this model, the observed radiation is produced in the skin layer of a hot, radiation-dominated pair atmosphere, probably confined to the vicinity of the neutron star by a strong magnetic field. In this layer, about 10 to the 12th generations of pairs are formed (by photon-photon collisions), cooled and annihilated during the 0.15 s duration of the impulsive phase.

Ramaty, R.↗

NASA NTRS1983

A fireball model for the March 25, 1978 gamma ray burst

It is suggested that the bulk of the gamma-ray emission in the March 25, 1978 burst comes from a fireball of photons and electron-positron pairs expanding from a jet off the polar cap of a neutron star, and that the duration of the burst is defined by the expansion and dissipation times of the fireball. This model makes it possible to determine the total energy, about 10 to the 39th ergs, and the distance, about 1kpc, of the burst and should be applicable to a large class of gamma-ray bursts.

Hueter, G. J.↗

NASA NTRS1983

Positron production by a hot, young pulsar

The paper considers a way of positron production in pulsars: pair production from electron-photon collisions. It is shown that this process must be the dominant one for a young pulsar when its surface temperature is around 10-million K. This model is applied to the observed positron flux coming from the Galactic Center and it is shown that a pulsar with parameters close to those of the Crab at birth can explain, in principle, the flux.

Brecher, K.↗

NASA NTRS1990

Field-Induced-Gap Infrared Detectors

Semimetals become semiconductors under applied magnetic fields. New detectors require less cooling equipment because they operate at temperatures higher than liquid-helium temperatures required by extrinsic-semiconductor detectors. Magnetic fields for detectors provided by electromagnets based on recently-discovered high-transition-temperature superconducting materials. Detector material has to be semiconductor, in which photon absorbed by exciting electron/hole pair across gap Eg of forbidden energies between valence and conduction energy bands. Magnetic- and compositional-tuning effects combined to obtain two-absorber detector having narrow passband. By variation of applied magnetic field, passband swept through spectrum of interest.

Elliott, C. Thomas↗

NASA NTRS1992

Of narrow lines and beaming in the strong-field SSC emission model

The synchrotron self-Compton (SSC) emission model for gamma-ray bursts is capable of producing narrow line features for a variety of modelled field strengths, primary electron injection distributions and burst luminosities. Multiple resonant scattering with synchrotron continuum photons efficiently traps and cools pairs in the ground state to an average energy where the Compton energy loss rate is zero. Annihilation between pairs in these cooled distributions can be very efficient. For isotropic injection of primary electrons, there is an anti-correlation of the intensity of the angular-binned emission between the portions of the continuum spectrum below the cyclotron peak and above the annihilation line feature. Small-angle emission dominates the continuum above the annihilation line feature and is smooth through the line up to the pair production cut-off, which can be above several MeV for small enough angles. The angle-averaged annihilation line is made of components which can have peak emission centered at energies away from 511 keV, due to Doppler shifting. For beamed injection,the annihilation line breaks up into relatively narrow components in the angular emission, which sum into a broad feature in the angle-averaged emission.

Preece, Robert D.↗