Quantum Electrodynamic Effects Research Articles

Move Aside Pentacene: Diazapentacene-Doped para-Terphenyl, a Zero-Field Room-Temperature Maser with Strong Coupling for Cavity Quantum Electrodynamics.

Masers can deliver ultralow-noise amplification of microwave signals in medical imaging and deep-space communication, with recent research being rekindled through the discovery of gain media operating at room-temperature, eschewing bulky cryogenics that hindered their use. This work shows the discovery of 6,13-diazapentacene doped in para-terphenyl (DAP:PTP) as a maser gain medium that can operate at room-temperature, without an external magnetic field. With a maser output power of -10 dBm, it is on par with pentacene-doped para-terphenyl in masing power, while possessing compelling advantages such as faster amplification startup times, being pumped by longer wavelength light at 620 nm and greater chemical stability from nitrogen groups. Furthermore, the maser bursts from DAP:PTP allow one to reach the strong coupling regime for cavity quantum electrodynamics, with a highcooperativity of 182. The optical and microwave spin dynamics of DAP:PTP are studied in order to evaluate its capabilities as a maser gain medium, where it features fast intersystem crossing and an advantageously higher triplet quantum yield. The results pave the way for the future discovery of similar maser materials and help designate them as promising candidates for quantum sensors, optoelectronic devices and the study of cavity quantum electrodynamic effects atroom-temperature.

Efficient generation of collimated multi-GeV gamma-rays along solid surfaces

Bright γ -ray sources are of great significance for fundamental research, medicine, and industry. However, γ -ray production by bremsstrahlung, Compton scattering, and synchrotron radiation is often subjected to large divergence, wide size, and/or low efficiency, making it difficult to achieve high-brightness γ -ray sources. Here, we have found an efficient mechanism to generate γ -rays with, to our knowledge, unprecedented brilliance by use of an ultrarelativistic electron beam with nC charge incident onto a solid surface at grazing incidence. With this interaction configuration, extreme high quasistatic magnetic fields up to the gigagauss level or effective electric fields up to 10 14 V / m are induced by the background electron backflows at the target surface. Subsequently, the electron beam is strongly focused by such fields by over an order of magnitude to submicrometer diameter, and its density is increased beyond the solid density; the induced effective fields are high enough to trigger quantum electrodynamics (QED) effects. These result in the production of extremely brilliant dense γ -ray beams with photon energy reaching multi-GeV, where the electron-to-photon energy conversion efficiency can exceed 60%. This offers a promising route to push the beam–target interaction to the QED regime, leading to ultrabright γ -ray sources for various applications.

LIBGRPP: A Library for the Evaluation of Molecular Integrals of the Generalized Relativistic Pseudopotential Operator over Gaussian Functions

Generalized relativistic pseudopotentials (GRPP) of atomic cores implying the use of different potentials for atomic electronic shells with different principal quantum numbers give rise to accurate and reliable relativistic electronic structure models of atoms, molecules, clusters, and solids. These models readily incorporate the effects of Breit electron–electron interactions and one-loop quantum electrodynamics effects. Here, we report the computational procedure for evaluating one-electron integrals of GRPP over contracted Gaussian functions. This procedure was implemented in a library of routines named LIBGRPP, which can be integrated into existing quantum chemistry software, thus enabling the application of various methods to solve the many-electron problem with GRPPs. Pilot applications to electronic transitions in the ThO and UO2 molecules using the new library and intermediate-Hamiltonian Fock space relativistic coupled cluster method are presented. Deviations of excitation energies obtained within the GRPP approach from their all-electron Dirac–Coulomb–Gaunt counterparts do not exceed 50 cm−1 for the 31 lowest-energy states of ThO and 110 cm−1 for the 79 states of UO2. The results clearly demonstrate that rather economical tiny-core GRPP models can exceed in accuracy relativistic all-electron models defined by Dirac–Coulomb and Dirac–Coulomb–Gaunt Hamiltonians.

The van der Waals interactions in systems involving superheavy elements: the case of oganesson (Z = 118).

This work presents a study involving dimers composed of He, Ne, Ar, Kr, Xe, Rn, and Og noble gases with oganesson, a super-heavy closed-shell element (Z = 118). He-Og, Ne-Og, Ar-Og, Kr-Og, Xe-Og, Rn-Og, and Og-Og ground state electronic potential energy curves were calculated based on the 4-component (4c) Dirac-Coulomb Hamiltonian and were counterpoise corrected. For the 4c calculations, the electron correlation was taken into account using the same methodology (MP2-srLDA) and basis set quality (Dyall's acv3z and Dunning's aug-cc-PVTZ). All calculations included quantum electrodynamics effects at the Gaunt interaction level. For all the aforementioned dimers the vibration energies, spectroscopic constants (ωe, ωexe, ωeye, αe, and γe), and lifetime as a function of the temperature (which ranged from 200 to 500 K) were also calculated. The obtained results suggest that the inclusion of quantum electrodynamics effects reduces the value of the dissociation energy of all hetero-nuclear molecules with a percentage contribution ranging from 0.48% (for the He-Og dimer) to 9.63% (for the Rn-Og dimer). The lifetime calculations indicate that the Og-He dimer is close to the edge of instability and that Ng-Og dimers are relatively less stable when the Gaunt correction is considered. Exploiting scaling laws that adopt the polarizability of involved partners as scaling factors, it has also been demonstrated that in such systems the interaction is of van der Waals nature (size repulsion plus dispersion attraction) and this permitted an estimation of dissociation energy and equilibrium distance in the Og-Og dimer. This further information has been exploited to evaluate the rovibrational levels in this symmetric dimer and to cast light on the macroscopic properties of condensed phases concerning the complete noble gas family, emphasizing some anomalies of Og.

Generalized relativistic small‐core pseudopotentials accounting for quantum electrodynamic effects: Construction and pilot applications

AbstractA simple procedure to incorporate one‐loop quantum electrodynamic (QED) corrections into the generalized (Gatchina) nonlocal shape‐consistent relativistic pseudopotential model is described. The pseudopotentials for Lu, Tl, and Ra replacing only inner core shells (with principal quantum numbersn ≤ 3 for the two former elements andn ≤ 4 for the latter one) are derived from the solutions of reference atomic SCF problems with the Dirac–Coulomb–Breit Hamiltonian to which the model Lamb shift operator added. QED contributions to atomic valence excitation energies evaluated at the SCF level are demonstrated to exceed the errors introduced by the pseudopotential approximation itself by an order of magnitude. Pilot applications of the new model to calculations of excitation energies of two‐valence‐electron atomic systems using the intermediate‐Hamiltonian relativistic Fock space coupled cluster method reformulated here for incomplete main model spaces are reported. Implications for high‐accuracy molecular excited state calculations are discussed.

Perspective: Simultaneous treatment of relativity, correlation, and QED

AbstractElectronic structure calculations of many‐electron systems should in principle treat relativistic, correlation, and quantum electrodynamics (QED) effects simultaneously to a high precision, so as to match experimental measurements as close as possible. While both relativistic and QED effects can readily be built into the many‐electron Hamiltonian, electron correlation is more difficult to describe due to the exponential growth of the number of parameters in the wave function. Compared with the spin‐free case, spin–orbit interaction results in the loss of spin symmetry and concomitant complex algebra, thereby rendering the treatment of electron correlation even more difficult. Possible solutions to these issues are highlighted here.This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods

Achieving relativistically intense X-rays from structured plasma lens

Focusing of high-power X-rays is still a great challenge and the intensity of X-ray attained in existing focusing schemes is still far below the relativistic threshold. Here, we propose that solid density plasma lens can potentially focus X-ray lasers at very high power levels. The interaction of high-power X-ray laser with solid-density plasmas is systematically studied. It is theoretically shown that there exists a certain range of wavelengths for X-ray lasers that can be focused in solid-density plasmas when the input power and plasma density are determined. To avoid the essential laser-plasma instabilities and obtain high-gain intensity amplification for X-ray, we design concave structured plasma lens. Particle-in-cell simulation results show that such regime can effectively avoid the instabilities and focus X-ray of micrometer-sized spot and multi-TW power, and thus lead to the generation of relativistic intensity X-ray. The parameters of the concave structures and the effects of quantum electrodynamics are also discussed and it indicates that our scheme is quite robust. We further demonstrate that the relativistic X-ray laser interacting with thin-foil leads to high-quality attosecond electron bunches.

Quantum Electrodynamic Behavior of Chlorophyll in a Plasmonic Nanocavity.

Plasmonic nanocavities have been used as a novel platform for studying strong light-matter coupling, opening access to quantum chemistry, material science, and enhanced sensing. However, the biomolecular study of cavity quantum electrodynamics (QED) is lacking. Here, we report the quantum electrodynamic behavior of chlorophyll-a in a plasmonic nanocavity. We construct an extreme plasmonic nanocavity using Au nanocages with various linker molecules and Au mirrors to obtain a strong coupling regime. Plasmon resonance energy transfer (PRET)-based hyperspectral imaging is applied to study the electrodynamic behaviors of chlorophyll-a in the nanocavity. Furthermore, we observe the energy level splitting of chlorophyll-a, similar to the cavity QED effects due to the light-matter interactions in the cavity. Our study will provide insight for further studies in quantum biological electron or energy transfer, electrodynamics, the electron transport chain of mitochondria, and energy harvesting, sensing, and conversion in both biological and biophysical systems.

Excitation energies, lifetimes, and transition data for Zr XXIX

The energies and lifetimes of the lowest 303 fine-structure levels belonging to the 3s2, 3s3p, 3s3d, 3p3d, 3d2, 3snl (n = 4 − 6; l = 0 − 5), 3pnl (n = 4 − 5; l = 0 − 4), 3p6s, and 3dnl (n = 4 − 5; l = 0 − 4) configurations of Mg-like zirconium, Zr XXIX, are calculated using the relativistic multiconfiguration Dirac-Hartree-Fack (MCDHF) method employed in the GRASP2018 atomic structure computer package. The MCDHF wavelengths, transition probabilities, weighted oscillator strengths, and line strengths for the electric dipole (E1), electric quadrupole (E2), magnetic dipole (M1), and magnetic quadrupole (M2) transitions between the levels considered are presented. The Breit-interaciton (BI) and quantum electrodynamics (QED) effects are considered in the computations. Comparisons with available experimental and other theoretical data are carried out to evaluate the accuracy of the present results.

Extended Calculations of Atomic Structure Parameters for Na-like Ar, Kr and Xe Ions Using Relativistic MCDHF and MBPT Methods

In this study, comprehensive calculations of energies, hyperfine structure constants, Landé gJ factors and isotope shifts have been performed for the lowest 71 states of Na-like Ar7+, Kr25+ and Xe43+ ions. Radiative parameters viz., wavelengths, transition rates, oscillator strengths and lifetimes are estimated for the electric dipole E1 transitions among these levels. The states under consideration include 1s22s22p6nl for n = 3–9, l = 0–6, and the fully relativistic multiconfiguration Dirac–Hartree–Fock (MCDHF) method integrated in the latest version of the general-purpose relativistic atomic structure package (GRASP2018) is used for the calculations. The additional corrections, such as the Breit interaction and quantum electrodynamics effects are included in the relativistic configuration interaction calculations, and their effects on energies and other parameters are analysed. We examined the impact of including the core–core and core–valence correlations on level energies. Furthermore, to inspect the reliability of our MCDHF results, we performed another set of calculations using the many-body perturbation theory built into the Flexible Atomic Code (FAC). Moreover, we estimated the uncertainties in the computed lifetimes and transition parameters and assigned their accuracy class. A thorough comparison between the two obtained calculations and with the previous theoretical and experimental results, wherever available, is carried out and a good agreement is observed.

Implications of gauge freedom for nonrelativistic quantum electrodynamics

Gauge freedom in quantum electrodynamics (QED) outside of textbook regimes is reviewed. It is emphasized that QED subsystems are defined relative to a choice of gauge. Each definition uses different gauge-invariant observables. This relativity is eliminated only if a sufficient number of Markovian and weak-coupling approximations are employed. All physical predictions are gauge invariant, including subsystem properties such as photon number and entanglement. However, subsystem properties naturally differ for different physical subsystems. Gauge ambiguities arise not because it is unclear how to obtain gauge-invariant predictions, but because it is not always clear which physical observables are the most operationally relevant. The gauge invariance of a prediction is necessary but not sufficient to ensure its operational relevance. It is shown that, in controlling which gauge invariant observables are used to define a material system, the choice of gauge affects the balance between the material system's localization and its electromagnetic dressing. Various implications of subsystem gauge relativity for deriving effective models, for describing time-dependent interactions, for photodetection theory, and for describing matter within a cavity are reviewed.

Microwave mode cooling and cavity quantum electrodynamics effects at room temperature with optically cooled nitrogen-vacancy center spins

Recent experimental and theoretical studies demonstrated microwave mode cooling and cavity quantum electrodynamics (C-QED) effects at room temperature by using optically cooled nitrogen-vacancy (NV) spins. In this article, we consider improvements of these effects by exploring parameters in recent diamond maser experiments with a high frequency microwave resonator. By accounting for the rich electronic and spin levels, we provide a more complete treatment of optical pumping and dissipation in NV centers, and study the dependence of system performance on laser power. We predict the reduction of microwave photon number down to 261 (equivalent to a temperature of 116 K), about five times lower than the values reported recently. We also predict the laser-power controlled C-QED effects across weak-to-strong coupling regimes, and observe saturation of these effects under strong laser pumping. Our model can be modified straightforwardly to investigate similar effects with other solid-state spins and possible C-QED effects in maser operation.

4-component relativistic Hamiltonian with effective QED potentials for molecular calculations.

We report the implementation of effective quantum electrodynamics (QED) potentials for all-electron four-component relativistic molecular calculations using the DIRAC code. The potentials are also available for two-component calculations, being properly picture-change transformed. The latter point is important; we demonstrate through atomic calculations that picture-change errors are sizable. Specifically, we have implemented the Uehling potential [E. A. Uehling, Phys. Rev. 48, 55 (1935)] for vacuum polarization and two effective potentials [P. Pyykkö and L.-B. Zhao, J. Phys. B: At., Mol. Opt. Phys. 36, 1469 (2003) and V. V. Flambaum and J. S. M. Ginges, Phys. Rev. A 72, 052115 (2005)] for electron self-energy. We provide extensive theoretical background for these potentials, hopefully reaching an audience beyond QED specialists. We report the following sample applications: (i) We first confirm the conjecture of P. Pyykkö that QED effects are observable for the AuCN molecule by directly calculating ground-state rotational constants B0 of the three isotopomers studied by microwave spectroscopy; QED brings the corresponding substitution Au-C bond length rs from 0.23 to 0.04pm agreement with experiment. (ii) In regard to spectroscopic constants of van der Waals dimers M2 (M = Hg, Rn, Cn, Og), QED induces bond length expansions on the order of 0.15(0.30) pm for row 6(7) dimers. (iii) We confirm that there is a significant change of valence s population of Pb in the reaction PbH4 → PbH2 + H2, which is thereby a good candidate for observing QED effects in chemical reactions, as proposed in [K. G. Dyall et al., Chem. Phys. Lett. 348, 497 (2001)]. We also find that whereas in PbH4 the valence 6s1/2 population resides in bonding orbitals, it is mainly found in nonbonding orbitals in PbH2. QED contributes 0.32 kcal/mol to the reaction energy, thereby reducing its magnitude by -1.27%. For corresponding hydrides of superheavy flerovium, the electronic structures are quite similar. Interestingly, the QED contribution to the reaction energy is of quite similar magnitude (0.35 kcal/mol), whereas the relative change is significantly smaller (-0.50%). This curious observation can be explained by the faster increase in negative vacuum polarization over positive electron self-energy contributions as a function of nuclear charge.

Transition energies and transition probabilities for the core-excited state [formula omitted] of Li-like ions with [formula omitted] 6–92

The transition energies and radiative transition probabilities for the transition from the (1s2s2p)3/2 group to the ground state 1s22s involving the electric dipole (E1) and magnetic quadrupole (M2) transitions have been systematically calculated for ions along the Li isoelectronic sequence from Z=6 to Z=92. The calculations are performed by using the full relativistic multi-configuration Dirac–Fock (MCDF) method, in which the leading quantum electrodynamics (QED) shifts and the frequency dependence of the Breit interaction are also considered. The present calculation results are in good agreement with available previous results. It is found that the transition probabilities generally increase along with nuclear number Z; however, the abnormal behavior with the minima transition probabilities at Z=28 and Z=25 emerges in the [(1s2s)02p3/2]3/2→1s22s via E1 transition and the [(1s2s)12p3/2]3/2→1s22s via M2 transition, respectively; the M2 transition probabilities become comparable with that of E1 in mid-Z ions, and particularly for the q line of Z=28 ion, the M2 and E1 transition probabilities would be of the same order of magnitude. In addition, the present results show that the electron correlations impact on the energy levels and transition probabilities mainly work on the low-Z ions, while, the QED and Breit effects mainly work on the high-Z ions. This work should be of particular interest to the analysis of the spectrum and the effects of multipole mixing on the X-ray properties.

Ditauonium spectroscopy

We examine the properties of ditauonium, an exotic atom consisting of a pair of opposite-sign tau leptons bound together by the quantum electrodynamics (QED) interaction in a hydrogen-like state. The energy levels, decay modes and associated partial widths, as well as total widths and lifetimes of the ortho- and para-ditauonium states are calculated. Higher-order QED effects – including Lamb shifts, hyperfine splitting structure, and partial decay widths corrections – are incorporated up to approximately next-to-next-to-leading-order (NNLO) accuracy. Beyond the dominant diphoton and difermion decays, the rates of rare decay channels – including Dalitz, radiative, triple-photon, double-Dalitz, four-fermion, and neutrinos final states – are determined.

Cavity-Free Quantum-Electrodynamic Electron Transfer Reactions.

Richard Feynman stated that "The theory behind chemistry is quantum electrodynamics". However, harnessing quantum-electrodynamic (QED) effects to modify chemical reactions is a grand challenge and currently has only been reported in experiments using cavities due to the limitation of strong light-matter coupling. In this article, we demonstrate that QED effects can significantly enhance the rate of electron transfer (ET) by several orders of magnitude in the absence of cavities, which is implicitly supported by experimental reports. To understand how cavity-free QED effects are involved in ET reactions, we incorporate the effect of infinite one-photon states into Marcus theory, derive an explicit expression for the rate of radiative ET, and develop the concept of "electron transfer overlap". Moreover, QED effects may lead to a barrier-free ET reaction whose rate is dependent on the energy-gap power law. This study thus provides new insights into fundamental chemical principles, with promising prospects for QED-based chemical reactions.

Quantum electrodynamics of two-body systems with arbitrary masses up to α6 order

We perform a calculation of quantum electrodynamics effects in excited states with $l>1$ of arbitrary two-body systems up to $\alpha^6\,\mu$ order. The obtained results are valid for hadronic atoms, as long as the strong interaction effects are negligible. We demonstrate that for circular states with $l\sim n$, the effective expansion parameter is $Z\,\alpha/n$, which extends the applicability of the derived formulas to heavy ions. Moreover, inclusion of higher-order terms is feasible, which indicates that accurate measurements of excited states of, for example, muonic or antiprotonic hydrogenic ions can be used to determine the fundamental constants and to search for the existence of yet unknown long-range interactions.

Charged particle motion and radiation in strong electromagnetic fields

The dynamics of charged particles in electromagnetic fields is an essential component of understanding the most extreme environments in our Universe. In electromagnetic fields of sufficient magnitude, radiation emission dominates the particle motion and effects of nonlinear quantum electrodynamics (QED) are crucial, which triggers electron-positron pair cascades and counterintuitive particle-trapping phenomena. As a result of recent progress in laser technology, high-power lasers provide a platform to create and probe such fields in the laboratory. With new large-scale laser facilities on the horizon and the prospect of investigating these hitherto unexplored regimes, we review the basic physical processes of radiation reaction and QED in strong fields, how they are treated theoretically and in simulation, the new collective dynamics they unlock, recent experimental progress and plans, as well as possible applications for high-flux particle and radiation sources.

GRASP: The Future?

The theoretical foundations of relativistic electronic structure theory within quantum electrodynamics (QED) and the computational basis of the atomic structure code GRASP are briefly surveyed. A class of four-component basis set is introduced, which we denote the CKG-spinor set, that enforces the charge-conjugation symmetry of the Dirac equation. This formalism has been implemented using the Gaussian function technology that is routinely used in computational quantum chemistry, including in our relativistic molecular structure code, BERTHA. We demonstrate that, unlike the kinetically matched two-component basis sets that are widely employed in relativistic quantum chemistry, the CKG-spinor basis is able to reproduce the well-known eigenvalue spectrum of point-nuclear hydrogenic systems to high accuracy for all atomic symmetry types. Calculations are reported of third- and higher-order vacuum polarization effects in hydrogenic systems using the CKG-spinor set. These results reveal that Gaussian basis set expansions are able to calculate accurately these QED effects without recourse to the apparatus of regularization and in agreement with existing methods. An approach to the evaluation of the electron self-energy is outlined that extends our earlier work using partial-wave expansions in QED. Combined with the treatment of vacuum polarization effects described in this article, these basis set methods suggest the development of a comprehensive ab initio approach to the calculation of radiative and QED effects in future versions of the GRASP code.

QED effects at grazing incidence on solid-state targets

New laser facilities will reach intensities of 10^{23} text {W cm}^{-2}. This advance enables novel experimental setups in the study of laser–plasma interaction. In these setups with extreme fields, quantum electrodynamic (QED) effects such as photon emission via nonlinear Compton scattering and Breit–Wheeler pair production become important. We study high-intensity lasers grazing the surface of a solid-state target by two-dimensional particle-in-cell simulations with QED effects included. The two laser beams collide at the target surface at a grazing angle. Due to the fields near the target surface, electrons are extracted and accelerated. Finally, the extracted electrons collide with the counter-propagating laser, which triggers many QED effects and leads to a QED cascade under a sufficient laser intensity. Here, the processes are studied for various laser intensities and angle of incidence and finally compared with a seeded vacuum cascade. Our results show that the proposed target can yield many orders of magnitude more secondary particles and develop a QED cascade at lower laser intensities than the seeded vacuum alone.