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Molecules under strong or ultra-strong light–matter coupling present an intriguing route to modify chemical structure, properties, and reactivity. A rigorous theoretical treatment of such systems requires handling matter and photon degrees of freedom on an equal quantum mechanical footing. In the regime of molecular electronic strong or ultra-strong coupling to one or a few molecules, it is desirable to treat the molecular electronic degrees of freedom using the tools of ab initio quantum chemistry, yielding an approach referred to as ab initio cavity quantum electrodynamics (ai-QED), where the photon degrees of freedom are treated at the level of cavity QED. We analyze two complementary approaches to ai-QED: (1) a parameterized ai-QED, a two-step approach where the matter degrees of freedom are computed using existing electronic structure theories, enabling the construction of rigorous ai-QED Hamiltonians in a basis of many-electron eigenstates, and (2) self-consistent ai-QED, a one-step approach where electronic structure methods are generalized to include coupling between electronic and photon degrees of freedom. Although these approaches are equivalent in their exact limits, we identify a disparity between the projection of the two-body dipole self-energy operator that appears in the parameterized approach and its exact counterpart in the self-consistent approach. We provide a theoretical argument that this disparity resolves only under the limit of a complete orbital basis and a complete many-electron basis for the projection. We present numerical results highlighting this disparity and its resolution in a particularly simple molecular system of helium hydride cation, where it is possible to approach these two complete basis limits simultaneously. In this same helium hydride system, we examine and compare the practical issue of the computational cost required to converge each approach toward the complete orbital and many-electron bases limit. Finally, we assess the aspect of photonic convergence for polar and charged species, finding comparable behavior between parameterized and self-consistent approaches. [ABSTRACT FROM AUTHOR]

Collective light–matter interactions have been used to control chemistry and energy transfer, yet accessible approaches that combine ab initio methodology with large many-body quantum optical systems are missing due to the fast increase in computational cost for explicit simulations. We introduce an accessible ab initio quantum embedding concept for many-body quantum optical systems that allows us to treat the collective coupling of molecular many-body systems effectively in the spirit of macroscopic quantum electrodynamics while keeping the rigor of ab initio quantum chemistry for the molecular structure. Our approach fully includes the quantum fluctuations of the polaritonic field and yet remains much simpler and more intuitive than complex embedding approaches such as dynamical mean-field theory. We illustrate the underlying assumptions by comparison to the Tavis–Cummings model. The intuitive application of the quantized embedding approach and its transparent limitations offer a practical framework for the field of ab initio polaritonic chemistry to describe collective effects in realistic molecular ensembles. [ABSTRACT FROM AUTHOR]

In this paper, an exact analytical solution is presented for achieving coherent population transfer and creating arbitrary coherent superposition states in a five-state chainwise system by a train of coincident pulses. We show that the solution of a five-state chainwise system can be reduced to an equivalent three-state Λ-type one with the simplest resonant coupling under the assumption of adiabatic elimination together with a requirement of the relation among the four coincident pulses. In this method, the four coincident pulses at each step all have the same time dependence, but with specific magnitudes. The results show that, by using a train of appropriately coincident pulses, this technique not only enables complete population transfer, but also creates any desired coherent superposition between the initial and final states, while the population in all intermediate states is effectively suppressed. Furthermore, this technique can also exhibit a one-way population transfer behavior. The results are of potential interest in applications where high-fidelity multi-state quantum control is essential, e.g., quantum information, atom optics, formation of ultracold molecules, cavity QED, nuclear coherent population transfer, and light transfer in waveguide arrays. [ABSTRACT FROM AUTHOR]

The results of relativistic calculations of nuclear magnetic resonance shielding tensors (σ) for the thallium monocation (Tl+), thallium hydride (TlH), and thallium halides (TlF, TlCl, TlBr, TlI, and TlAt) are presented as obtained within a four-component polarization propagator formalism and a two-component linear response approach within the zeroth-order regular approximation. In addition to a detailed analysis of relativistic effects performed in this work, some quantum electrodynamical (QED) effects on those nuclear magnetic resonance shieldings and other small contributions are estimated. A strong dependence of σ(Tl) on the bonding partner is found, together with a very weak dependence of QED effects with them. In order to explain the trends observed, the excitation patterns associated with relativistic ee (or paramagnetic-like) and pp (or diamagnetic-like) contributions to σ are analyzed. For this purpose, the electronic spin-free and spin-dependent contributions are separated within the two-component zeroth-order regular approximation, and the influence of spin–orbit coupling on involved molecular orbitals is studied, which allows for a thorough understanding of the underlying mechanisms. [ABSTRACT FROM AUTHOR]

Recent theoretical studies have explored how ultra-strong light–matter coupling can be used as a handle to control chemical transformations. Ab initio cavity quantum electrodynamics calculations demonstrate that large changes to reaction energies or barrier heights can be realized by coupling electronic degrees of freedom to vacuum fluctuations associated with an optical cavity mode, provided that large enough coupling strengths can be achieved. In many cases, the cavity effects display a pronounced orientational dependence. Here, we highlight the critical role that geometry relaxation can play in such studies. As an example, we consider a recent work [Pavošević et al., Nat. Commun. 14, 2766 (2023)] that explored the influence of an optical cavity on Diels–Alder cycloaddition reactions and reported large changes to reaction enthalpies and barrier heights, as well as the observation that changes in orientation can inhibit the reaction or select for one reaction product or another. Those calculations used fixed molecular geometries optimized in the absence of the cavity and fixed relative orientations of the molecules and the cavity mode polarization axis. Here, we show that when given a chance to relax in the presence of the cavity, the molecular species reorient in a way that eliminates the orientational dependence. Moreover, in this case, we find that qualitatively different conclusions regarding the impact of the cavity on the thermodynamics of the reaction can be drawn from calculations that consider relaxed vs unrelaxed molecular structures. [ABSTRACT FROM AUTHOR]

This work is a collection of initial calculations and formal considerations within the Salpeter–Sucher exact equal-time relativistic quantum electrodynamics framework. The calculations are carried out as preparation for the computation of pair, retardation, and radiative corrections to the relativistic energy of correlated two-spin-1/2-fermion systems. In this work, particular attention is paid to the retardation and the "one-loop" self-energy corrections, which are known to be among the largest corrections to the correlated relativistic energy. The theoretical development is supplemented with identifying formal connections to the non-relativistic quantum electrodynamics framework, which is based on a correlated but non-relativistic reference, as well as to the "1/Z approach," which is built on a relativistic but independent-particle zeroth order. The two complementary directions currently provide the theoretical framework for light atomic–molecular precision spectroscopy and heavy-atom phenomena. The present theoretical efforts pave the way for relativistic QED corrections to (explicitly) correlated relativistic computations. [ABSTRACT FROM AUTHOR]

The article discusses various aspects of quantum electrodynamics (QED) Hamiltonians and their formulations. It examines different schemes and equations used in QED calculations, highlighting inconsistencies and incorrect manipulations in some approaches. The text also discusses the nonrelativistic limit of the QED Hamiltonian, the accuracy of different Hamiltonians, and the transformation of equations and variables. It concludes by providing recommendations for the use of certain Hamiltonians and discussing the charge conjugation and time reversal transformations in QED. The work was supported by funding from the National Natural Science Foundation of China and the Mount Tai Scholar Climbing Project of Shandong Province. [Extracted from the article]

This article is a response to a comment made by Professor Liu regarding a previously published paper. The response addresses questions raised by Professor Liu and focuses on three key aspects of the validity of the paper. It explains the use of different contractions in the construction of the QED Hamiltonians and clarifies the commutation relations used in the calculations. The article also highlights that the formulation of the molecular orbital method described in the paper is independent of the ordering of the operators and can derive expressions for various perturbation theories. The response concludes by stating that alternative criteria for the QED Hamiltonians are not ruled out and could be explored in future research. [Extracted from the article]

Born–Huang expansion is the cornerstone for studying potential energy surfaces and non-adiabatic couplings (NACs) in molecular systems. However, the traditional approach is insufficient to describe the molecular system, which strongly interacts with quantum light. Inspired by the work by Schäfer et al., we develop the generalized Born–Huang expansion theory within a macroscopic quantum electrodynamics (QED) framework. The theory we present allows us to describe electromagnetic vacuum fluctuations in dielectric media and incorporate the effects of dressed photons (or polaritons) into NACs. With the help of the generalized Born–Huang expansion, we clearly classify electronic nuclear NACs, polaritonic nuclear NACs, and polaritonic electronic NACs. Furthermore, to demonstrate the advantage of the macroscopic QED framework, we estimate polaritonic electronic NACs without any free parameter, such as the effective mode volume, and demonstrate the distance dependence of the polaritonic electronic NACs in a silver planar system. In addition, we take a hydrogen atom in free space as an example and derive spontaneous emission rates from photonic electronic NACs (polaritonic electronic NACs are reduced to photonic electronic NACs). We believe that this work not only provides an avenue for the theoretical exploration of NACs in a nucleus–electron–polariton coupled system but also offers a more comprehensive understanding for molecules coupled with quantum light. [ABSTRACT FROM AUTHOR]

Polaritonic states, which are formed by resonances between a molecular excitation and the photonic mode of a cavity, have a number of useful properties that offer new routes to control molecular photochemistry using electric fields. To provide a theoretical description of how polaritonic states affect the real-time electron dynamics in molecules, a new method is described where the effects of strong light–molecule coupling are implemented using real-time electronic structure theory. The coupling between the molecular electronic states and the cavity is described by the Pauli–Fierz Hamiltonian, and transitions between polaritonic states are induced via an external time-dependent electric field using time-dependent configuration interaction (TDCI) theory, producing quantum electrodynamics TDCI (QED-TDCI). This method is used to study laser-induced ultrafast charge transfer and dipole-switching dynamics of the LiCN molecule inside a cavity. The increase in cavity coupling strength is found to have a significant impact on the energies and transition dipole moments of the molecule–cavity system. The convergence of the polaritonic state energies as a function of the number of included electronic and photonic basis states is discussed. [ABSTRACT FROM AUTHOR]

Both spontaneous Raman scattering and stimulated Raman scattering (SRS) are cornerstones of modern photonics, spectroscopy, and imaging. However, a unified understanding of the ultimate detectability of Raman scattering is lacking, due to both historical and technical reasons. Starting from quantum electrodynamics, we formulate the fundamental detectability for both spontaneous Raman scattering and SRS. The key concept is recognizing spontaneous Raman scattering as stimulated Raman process driven by vacuum field fluctuation. A simple and unified expression, Eq. (17), is derived, which can be depicted on a two-dimensional phase-diagram-like graph with inherent symmetry. It turns out that the particle nature of light dictates the ultimate detectability of spontaneous Raman scattering, which can be represented by a line on this detectability diagram. Importantly, if provided with a reasonably strong Stokes photon flux, SRS can breach this fundamental limit and open uncharted territory of drastically accelerated measurement speed and much lower detection concentration relevant to biological imaging. Such new territory in the detectability diagram is otherwise forbidden by the spontaneous counterpart. Diagrammatical analysis explains the empirical observations, provides quantitative insights, and makes new predictions. Notably, recent experimental applications of SRS microscopy can almost entirely be captured by this diagram, further supporting the explanatory power of the theory. Thus, this unified diagrammatic approach outlines a framework to understand all Raman-based measurement and provides a theoretical explanation for the remarkable utility of the emerging SRS microscopy. [ABSTRACT FROM AUTHOR]

Two-level quantum systems are fundamental physical models that continue to attract growing interest due to their crucial role as a building block of quantum technologies. The exact analytical solution of the dynamics of these systems is central to control theory and its applications, such as that to quantum computing. In this study, we reconsider the two-state charge transfer problem by extending and using a methodology developed to study (pseudo)spin systems in quantum electrodynamics contexts. This approach allows us to build a time evolution operator for the charge transfer system and to show new opportunities for the coherent control of the system dynamics, with a particular emphasis on the critical dynamic region around the transition state coordinate, where the avoided crossing of the energy levels occurs. We identify and propose possible experimental implementations of a class of rotations of the charge donor (or acceptor) that endow the electronic coupling matrix element with a time-dependent phase that can be employed to realize controllable coherent dynamics of the system across the avoided level crossing. The analogy of these rotations to reference frame rotations in generalized semiclassical Rabi models is discussed. We also show that the physical rotations in the charge-transfer systems can be performed so as to implement quantum gates relevant to quantum computing. From an exquisitely physical–mathematical viewpoint, our approach brings to light situations in which the time-dependent state of the system can be obtained without resorting to the special functions appearing in the Landau–Zener approach. [ABSTRACT FROM AUTHOR]

Since it was first predicted 100 years ago, Raman scattering has been a cornerstone of molecular spectroscopy with a widespread impact on science and technology. Nearly all theoretical frameworks have employed Raman cross sections (σRaman) to characterize and quantify molecular Raman response. The recently introduced absolute stimulated Raman scattering cross section (σSRS), on the other hand, provides an alternative way of interpreting molecular responses under two coherent laser sources. However, the theoretical connection between σRaman and σSRS remains unclear. Herein, we are inspired by Einstein's A and B coefficients for spontaneous and stimulated emissions and derived an analogous equation [Eq. (16)] for Raman scattering from an approach along quantum electrodynamics. Equation (16) decomposes Raman cross sections into a contribution from the vacuum electromagnetic field and an underlying molecular response captured by stimulated Raman cross sections (in the unit of Göppert–Mayer). This theoretical relation is supported by recent experimental measurements on methanol as a model compound. Foremost, it provides a connection between experimentally defined σRaman and σSRS under certain approximations. In addition, it quantitatively shows that it is the weak vacuum field of the Stokes channel that makes Raman cross sections appear so small, corroborating the conventional Raman theory. Moreover, it suggests stimulated Raman cross sections to be a vacuum-decoupled intrinsic quantity for characterizing molecular response during Raman scattering. Remarkably, stimulated Raman cross sections turn out to be not weak when compared to two-photon absorption, narrowing the conventional gap of cross sections between spontaneous Raman and UV–vis absorption by more than 1010 folds. [ABSTRACT FROM AUTHOR]

Exciton transport in extended molecular systems and how to manipulate such transport in a complex environment are essential to many energy and optical-related applications. We investigate the mechanism of plasmon-coupled exciton transport by using the Pauli master equation approach, combined with kinetic rates derived from macroscopic quantum electrodynamics. Through our theoretical framework, we demonstrate that the presence of a silver nanorod induces significant frequency dependence in the ability of transporting exciton through a molecule chain, indicated by the exciton diffusion coefficient, due to the dispersive nature of the silver dielectric response. Compared with the same system in vacuum, great enhancement (up to a factor of 103) in the diffusion coefficient can be achieved by coupling the resonance energy transfer process to localized surface plasmon polariton modes of the nanorod. Furthermore, our analysis reveals that the diffusion coefficients with the nearest-neighbor coupling approximation are ∼10 times smaller than the results obtained beyond this approximation, emphasizing the significance of long-range coupling in exciton transport influenced by plasmonic nanostructures. This study not only paves the way for exploring practical approaches to study plasmon-coupled exciton transport but also provides crucial insights for the design of innovative plasmon-assisted photovoltaic applications. [ABSTRACT FROM AUTHOR]

In this work, expressions for the third-harmonic scattering optical activity (THS-OA) spectroscopic responses are derived by combining molecular quantum electrodynamics (QED) and response theory, allowing their computational implementation. The QED theory of THS-OA presented here is meant to be an extension of a previous study by Andrews [Symmetry 12, 1466 (2020)]. In particular, the THS-OA phenomena are described within the Power–Zienau–Woolley multipolar Hamiltonian by including the electric-dipole, magnetic-dipole, and electric-quadrupole interactions for the absorption as well as the emission processes between the dynamic electromagnetic field (the photons) and matter. Moreover, we derive the expressions for the differential scattering ratios as a function of the scattering angle defined by the wavevectors of the incident and scattered photons. We show how the pure and mixed second hyperpolarizabilities can be obtained in the framework of response theory as specific cases of a generic cubic response function, thus enabling the computational implementation of THS-OA spectroscopy. We prove the origin-independence of the theory for exact wavefunctions. Preliminary computations on a prototype chiral molecule (methyloxirane) are considered together with an analysis of the basis set convergence and of the origin-dependence. [ABSTRACT FROM AUTHOR]

In the presence of spacetime torsion, the momentum components do not commute; therefore, in quantum field theory, summation over the momentum eigenvalues will replace integration over the momentum. In the Einstein–Cartan theory of gravity, in which torsion is coupled to spin, the separation between the eigenvalues increases with the magnitude of the momentum. Consequently, this replacement regularizes divergent integrals in Feynman diagrams with loops by turning them into convergent sums. In this article, we apply torsional regularization to the self-energy of a charged lepton in quantum electrodynamics. We show that torsion eliminates the ultraviolet divergence of the standard self-energy. We also show that the infrared divergence is absent. In the end, we calculate the finite bare masses of the electron, muon, and tau lepton: 0.4329 MeV , 90.95 MeV , and 1543 MeV , respectively. These values constitute about 85% of the observed, re-normalized masses. [ABSTRACT FROM AUTHOR]

Accelerating a free electron to high‐energy forms the basis for studying particle and nuclear physics. Here it is shown that the wave function of such an energetic electron can be further manipulated with the femtosecond intense lasers. During the scattering between a high‐energy electron and a circularly polarized laser pulse, a regime is found where the enormous spin angular momenta of laser photons can be efficiently transferred to the electron orbital angular momentum (OAM). The wave function of the scattered electron is twisted from its initial plane‐wave state to the quantum vortex state. Nonlinear quantum electrodynamics (QED) theory suggests that the GeV‐level electrons acquire average intrinsic OAM beyond ⟨l⟩∼100ℏ$\langle l \rangle \sim 100\hbar $ at laser intensities of 1020 W cm−2 with linear scaling. These electrons emit γ‐photons with two‐peak spectrum, which sets them apart from the ordinary electrons. The findings demonstrate a proficient method for generating relativistic leptons with the vortex wave functions based on existing laser technology, thereby fostering a novel source for particle and nuclear physics. [ABSTRACT FROM AUTHOR]

It is known that the electromagnetic vacuum is responsible for the Lamb shift, which is a crucial phenomenon in quantum electrodynamics (QED). In circuit QED, the readout or bus resonators that are dispersively coupled can result in a significant Lamb shift of the qubit. However, previous approaches or proposals for controlling the Lamb shift in circuit QED demand overheads in circuit designs or non-perturbative renormalization of the system's eigenbases, which can impose formidable limitations. In this work, we propose and demonstrate an all-microwave method for controlling the Lamb shift of fixed-frequency transmons. We employ the drive-induced longitudinal coupling between the transmon and resonator. By simply using an off-resonant monochromatic drive near the resonator frequency, we can control the net Lamb shift up to ±30 MHz and engineer it to zero with the drive-induced longitudinal coupling without facing the aforementioned challenges. Our work establishes an efficient way of engineering the fundamental effects of the electromagnetic vacuum and provides greater flexibility in non-parametric frequency controls of multilevel systems. Engineering the Lamb shifts of superconducting qubits opens new opportunities in resonant frequency tunings and other applications. Here, the authors devise and demonstrate an all-microwave approach that can be utilized with fixed-frequency superconducting qubits. [ABSTRACT FROM AUTHOR]

This Technical Design Report presents a detailed description of all aspects of the LUXE (Laser Und XFEL Experiment), an experiment that will combine the high-quality and high-energy electron beam of the European XFEL with a high-intensity laser, to explore the uncharted terrain of strong-field quantum electrodynamics characterised by both high energy and high intensity, reaching the Schwinger field and beyond. The further implications for the search of physics beyond the Standard Model are also discussed. [ABSTRACT FROM AUTHOR]

The photochemical acid generation is refined from the first principles of quantum electrodynamics. First, we briefly review the formulation of the quantum theory of light based on the quantum electrodynamics framework to establish the probability of acid generation at a given spacetime point. The quantum mechanical acid generation is then combined with the deprotection mechanism to obtain a probabilistic description of the deprotection density directly related to feature formation in a photoresist. A statistical analysis of the random deprotection density is presented to reveal the leading characteristics of stochastic feature formation. [ABSTRACT FROM AUTHOR]

In this study, we report highly precise and accurate measurements of the P(5), P(6), and O(3) transitions of the 2-0 band of HD occurring at approximately 1.5 µm. HD spectra were acquired in the pressure range of 100-900 Torr using a cavity ring-down spectrometer linked to an optical frequency comb. The line-shape analysis was performed using the Hartmann-Tran profile in the so-called β-corrected version. For the P(5) transition, we improved the accuracy of previous line center frequency determinations by more than two orders of magnitude. Moreover, for the P(5) and P(6) line centers, the total standard uncertainty is below 3 MHz, similar to those provided by quantum electrodynamics predictions, making them useful for direct comparisons that might foster future improvements of the theoretical model. [ABSTRACT FROM AUTHOR]

A relativistic version of the correspondence principle, a limit in which classical electrodynamics may be derived from quantum electrodynamics (QED), has never been clear, especially when including gravitational mass. Here we introduce a novel classical field theory formulation of electromagnetism, and then show that it approximates QED in the limit of a quantum state which corresponds to a classical charged continua. Our formulation of electromagnetism features a Lagrangian which is gauge invariant, includes a classical complex field from which a divergenceless four-current may be derived, and reproduces all aspects of the classical theory of charged massive continua without any quantum effects. Taking a geometric approach, we identify the four-current as being in the direction of extremal phase velocity of the classical field; the field equations of motion determine this phase velocity as being equal to the mass, which makes the rest density proportional to the squared modulus of the field. [ABSTRACT FROM AUTHOR]

Phenomena of free-electron X-ray radiation are treated almost exclusively with classical electrodynamics, despite the intrinsic interaction being that of quantum electrodynamics. The lack of quantumness arises from the vast disparity between the electron energy and the much smaller photon energy, resulting in a small cross-section that makes quantum effects negligible. Here we identify a fundamentally distinct phenomenon of electron radiation that bypasses this energy disparity, and thus displays extremely strong quantum features. This phenomenon arises when free-electron transverse scattering occurs during the radiation process, creating entanglement between each transversely recoiled electron and the photons it emitted. This phenomenon profoundly modifies the characteristics of free-electron radiation mediated by crystals, compared to conventional classical analysis and even previous quantum analysis. We also analyze conditions to detect this phenomenon using low-emittance electron beams and high-resolution X-ray spectrometers. These quantum radiation features could guide the development of compact coherent X-ray sources facilitated by nanophotonics and quantum optics. Free-electron X-ray radiation is typically treated classically. Here, the authors identify unprecedented quantum features of X-ray emission from crystals, due to transversely recoiled electron-photon entanglement, enabling precisely tuned emission via quantum control of free electrons. [ABSTRACT FROM AUTHOR]

Multiquanta correlation between n$n$ quanta of a completely different nature is an important resource for hybrid quantum information processing since it allows quantum states of matters to be manipulated by other degrees of freedom. Here, a method is proposed to realize the hybrid bundle emission of strongly correlated single photons and magnons. The optically driven multiquanta resonance leads to the super‐Rabi oscillation between the vacuum state and photon‐magnon state, which, combined with system dissipations, generates photon‐magnon bundle emission. Interestingly, accompanied by this bundle emission, the photon‐magnon entanglement and fully inseparable photon‐magnon‐qubit tripartite entanglement are achieved. This allows the proposed hybrid system to serve as a quantum emitter of entangled photon‐magnon bundle, which is useful for building hybrid quantum network and the engineering of new types of quantum devices. [ABSTRACT FROM AUTHOR]

Spontaneous light emission is central to a vast range of physical systems and is a founding pillar for the theory of light–matter interactions. In the presence of complex photonic media, the description of spontaneous light emission usually requires advanced theoretical quantum optics tools such as macroscopic quantum electrodynamics, involving quantized electromagnetic fields. Although rigorous and comprehensive, the complexity of such models can obscure the intuitive understanding of many quantum-optical phenomena. Here, we review a method for calculating spontaneous emission and other quantum-optical processes without making explicit use of quantized electromagnetic fields. Instead, we introduce the concept of transition currents, comprising charges in matter that undergo transitions between initial and final quantum states. We show how predictions that usually demand advanced methods in quantum electrodynamics or quantum optics can be reproduced by feeding these transition currents as sources to the classical Maxwell equations. One then obtains the relevant quantum observables from the resulting classical field amplitudes, without washing out quantum optical effects. We show that this procedure allows for a straightforward description of quantum phenomena, even when going beyond the dipole approximation and single emitters. As illustrative examples, we calculate emission patterns and Purcell-enhanced emission rates in both bound-electron and free-electron systems. For the latter, we derive cathodoluminescence emission and energy-loss probabilities of free electrons interacting with nanostructured samples. In addition, we calculate quantum-beat phenomena in bound-electron systems and wave function-dependent optical coherence in free-electron systems. Remarkably, the transition-current formalism captures more complex phenomena, such as many-body interference effects and super-radiance of both bound- and free-electron systems, second-order processes such as two-photon emission, and quantum recoil corrections to free-electron radiation. We review a variety of light–matter interactions in fields ranging from electron microscopy to nanophotonics and quantum optics, for which the transition-current theoretical formalism facilitates practical simulations and a deeper understanding of novel applications. [ABSTRACT FROM AUTHOR]

We extend the Sim (2) invariant infrared regularization of Very Special Relativity models, that we have proposed recently, to include γ 5 Dirac matrix. Then, we solve the Very Special Relativity Schwinger model, find the chiral anomaly, and clarify its meaning in the new context. In addition, we show that the triangle anomaly in four space-time dimensions agrees with the same object in standard quantum electrodynamics. Finally, we apply the infrared regularization to compute the large N limit of the Very Special Relativity Gross–Neveu model. [ABSTRACT FROM AUTHOR]

Gauge theory underpins the quantum field theories of the standard model, and in a previous paper was shown via a geometric approach to describe classical electromagnetism in a form which approximates quantum electrodynamics. Here we formalize and generalize the notion of a geometric gauge theory, then apply this framework to classical physical models, including an improved Lagrangian for matter field electromagnetism. We find a remarkably consistent series of actions, with straightforward limits under which each previous one may be obtained. Ancillary benefits include a gauge-independent Galilean Lagrangian, a geometric interpretation for the unusual metric dependence of four-momentum, a modern treatment of the effects of worldline variation on the four-current, a gauge theory of gravity which includes a matter field, and consistent units for matter field electromagnetism. [ABSTRACT FROM AUTHOR]

Quantum Hall insulators in artificial systems have become a rapidly developing research field in recent years, and have made significant breakthroughs in observing many novel topological phenomena. However, there are few reports about quantum magnon‐photon Hall insulators. Here, a scheme is proposed for implementing a 1D cavity magnonics lattice that exhibits quantum magnon‐photon Hall insulator behaviors, where each unit cell comprises cavity photons and magnons. By adjusting the system parameters, it is found that not only different energy spectrum structures can be triggered, but also the distribution of the edge states can show the flipping process, which allows the achievement of the multi‐channel topological quantum state transmission. In addition, considering the presence of defects, dissipation, and disorder, it is found that appropriate defects can trigger new topological phases, while dissipation only causes shifts in energy levels without changing the position and period of edge states, and disorder leads to shifts in band structures and edge states, thus demonstrating the robustness of edge states. This work offers an effective way to study topological magnon‐photon Hall insulators, which will have promising applications in magnon‐based quantum information processing. [ABSTRACT FROM AUTHOR]

Abstract In this paper, we propose employing electron scattering to realize unitary quantum gates that are controlled by three qubits. Using Feynman’s rules, we find an expression for the transition amplitude for scattering from an external electromagnetic source. In this context, the scattering amplitude is modeled as a unitary gate whose state can be regulated. The optimal value of the vector potential needed to implement the gate is obtained by minimizing the difference between the designed gate and the target gate, with the total energy consumed as a constraint. The design algorithm is obtained by discretizing the resulting integral equations into vector equations. This design algorithm can be applied in various fields such as quantum computing, communication, and sensing. It offers a promising approach for developing efficient and accurate gates for quantum information processing. Furthermore, this approach can also be extended to design gates for multi-qubit systems, which are essential for large-scale quantum computing. The use of this algorithm can significantly contribute to the development of practical quantum technologies.

The photochemical acid generation is refined from the first principles of quan-tum electrodynamics. First, we briefly review the formulation of the quantum theory of light based on the quantum electrodynamics framework to establish the probability of acid generation at a given spacetime point. The quantum mechanical acid generation is then combined with the deprotection mecha-nism to obtain a probabilistic description of the deprotection density directly related to feature formation in a photoresist. A statistical analysis of the ran-dom deprotection density is presented to reveal the leading characteristics of stochastic feature formation.

Theoretical discussions are given on issues in relativistic molecular orbital theory to which the quantum electrodynamics (QED) Hamiltonian is applied. First, several QED Hamiltonians previously proposed are sifted by the orbital rotation invariance, the charge conjugation and time reversal invariance, and the nonrelativistic limit. The discussion on orbital rotation invariance shows that orbitals giving a stationary point of total energy should be adopted for QED Hamiltonians that are not orbital rotation invariant. A new total energy expression is then proposed, in which a counter term corresponding to the energy of the polarized vacuum is subtracted from the total energy. This expression prevents the possibility of total energy divergence due to electron correlations, stemming from the fact that the QED Hamiltonian does not conserve the number of particles. Finally, based on the Hamiltonian and energy expression, the Dirac–Hartree–Fock (DHF) and electron correlation methods are reintroduced. The QED-based DHF equation is shown to give information on positrons from negative-energy orbitals while having the same form as the conventional DHF equation. Three electron correlation methods are derived: the QED-based configuration interactions and single- and multireference perturbation methods. Numerical calculations show that the total energy of the QED Hamiltonian indeed diverged and that the counter term is effective in avoiding the divergence. The relativistic molecular orbital theory presented in this article also provides a methodology for dealing with systems containing positrons based on the QED Hamiltonian. [ABSTRACT FROM AUTHOR]

We consider a one-dimensional effective quantum electrodynamics (QED) model of the relativistic hydrogen-like atom using delta-potential interactions. We discuss the general exact theory and the Hartree–Fock approximation. The present one-dimensional effective QED model shares the essential physical feature of the three-dimensional theory: the nuclear charge polarizes the vacuum state (creation of electron–positron pairs), which results in a QED Lamb-type shift of the bound-state energy. Yet, this 1D effective QED model eliminates some of the most serious technical difficulties of the three-dimensional theory coming from renormalization. We show how to calculate the vacuum-polarization density at zeroth order in the two-particle interaction and the QED Lamb-type shift of the bound-state energy at first order in the two-particle interaction. The present work may be considered a step toward the development of a quantum-chemistry effective QED theory of atoms and molecules. [ABSTRACT FROM AUTHOR]

Resonance energy transfer (RET) is an important and ubiquitous process whereby energy is transferred from a donor chromophore to an acceptor chromophore without contact via Coulombic coupling. There have been a number of recent advances exploiting the quantum electrodynamics (QED) framework for RET. Here, we extend the QED RET theory to investigate whether real photon exchange can allow for excitation transfer over very long distances if the exchanged photon is waveguided. To study this problem, we consider RET in two spatial dimensions. We derive the RET matrix element using QED in two dimensions, consider an even greater confinement by deriving the RET matrix element for a two-dimensional waveguide using ray theory, and compare the resulting RET elements in 3D and 2D and for the 2D waveguide. We see greatly enhanced RET rates over long distances for both the 2D and 2D waveguide systems and see a great preference for transverse photon mediated transfer in the 2D waveguide system. [ABSTRACT FROM AUTHOR]

This work reports on the first computational quantum-chemistry implementation of the hyper-Rayleigh scattering optical activity (HRS-OA), a nonlinear chiroptical phenomenon. First, from the basics of the theory, which is based on quantum electrodynamics, and focusing on the electric dipole, magnetic-dipole, and electric-quadrupole interactions, the equations for the simulation of the differential scattering ratios of HRS-OA are re-derived. Then, for the first time, computations of HRS-OA quantities are presented and analyzed. They have been enacted on a prototypical chiral organic molecule (methyloxirane) at the time-dependent density functional theory level using a broad range of atomic orbital basis sets. In particular, (i) we analyze the basis set convergence, demonstrating that converged results require basis sets with both diffuse and polarization functions, (ii) we discuss the relative amplitudes of the five contributions to the differential scattering ratios, and (iii) we study the effects of origin-dependence and derived the expression of the tensor shifts and we prove the origin-independence of the theory for exact wavefunctions. Our computations show the ability of HRS-OA as a nonlinear chiroptical method, able to distinguish between the enantiomers of the same chiral molecule. [ABSTRACT FROM AUTHOR]

Bound states in the continuum (BICs), manifesting themselves as the collapse of Fano resonance, are observed in many photonic and plasmonic systems. The BICs have been studied systematically through various methods such as the topological photonics analysis, temporal coupled mode theory, multipole decomposition method, and the cavity quantum electrodynamics (CQED) method. Since CQED can give a macroscopic and intrinsic description of light–matter interaction, it is expected to study BIC that participates in strong coupling. What is more, the relation between coupling strength, the Fano parameter, and the asymmetry property of BICs needs to be clarified. In this paper, we investigated the strong coupling between the cavity mode and Bloch-surface plasmon polariton (Bloch-SPP) mode induced by BICs within the plasmonic lattices of the metal-dielectric-metal (MDM) layer. The properties of strong coupling and BIC were revealed theoretically by the quantum model based on the CQED. The increase in the Fano parameters of BICs was proved to facilitate the coupling strength, which was indicated by the monotonically increasing relation between the Fano parameter and the coupling strength. This work may pave the way for flexible modulation and application of BIC in the fields of high-quality plasmonic nanocavity, low-threshold nano-lasers, and quantum information. [ABSTRACT FROM AUTHOR]

Real time modeling of fluorescence with vibronic resolution entails the representation of the light–matter interaction coupled to a quantum-mechanical description of the phonons and is therefore a challenging problem. In this work, taking advantage of the difference in timescales characterizing internal conversion and radiative relaxation—which allows us to decouple these two phenomena by sequentially modeling one after the other—we simulate the electron dynamics of fluorescence through a master equation derived from the Redfield formalism. Moreover, we explore the use of a recent semiclassical dissipative equation of motion [C. M. Bustamante et al., Phys. Rev. Lett. 126, 087401 (2021)], termed coherent electron electric-field dynamics (CEED), to describe the radiative stage. By comparing the results with those from the full quantum-electrodynamics treatment, we find that the semiclassical model does not reproduce the right amplitudes in the emission spectra when the radiative process involves the de-excitation to a manifold of closely lying states. We argue that this flaw is inherent to any mean-field approach and is the case with CEED. This effect is critical for the study of light–matter interaction, and this work is, to our knowledge, the first one to report this problem. We note that CEED reproduces the correct frequencies in agreement with quantum electrodynamics. This is a major asset of the semiclassical model, since the emission peak positions will be predicted correctly without any prior assumption about the nature of the molecular Hamiltonian. This is not so for the quantum electrodynamics approach, where access to the spectral information relies on knowledge of the Hamiltonian eigenvalues. [ABSTRACT FROM AUTHOR]

By consistently applying the formalism of quantum electrodynamics, we developed a comprehensive theoretical framework describing the interaction of single microwave photons with an array of superconducting transmon qubits in a waveguide cavity resonator. In particular, we analyze the effects of microwave photons on the array's response to a weak probe signal exciting the resonator. The study reveals that high quality factor cavities provide a better spectral resolution of the response, while cavities with moderate quality factors allow better sensitivity for a single-photon detection. Remarkably, our analysis showed that a single-photon signal can be detected by even a sole qubit in a cavity under the realistic range of system parameters. We also discuss how the quantum properties of the microwave radiation and electrodynamical properties of resonators affect the response of qubits' array. Our results provide an efficient theoretical background for informing the development and design of quantum devices consisting of arrays of qubits, especially for those using a cavity where an explicit expression for the transmission or reflection is required. [ABSTRACT FROM AUTHOR]

Carbon nanotubes are a telecom band emitter compatible with silicon photonics, and when coupled to microcavities, they present opportunities for exploiting quantum electrodynamical effects. Microdisk resonators demonstrate the feasibility of integration into the silicon platform. Efficient coupling is achieved using photonic crystal air-mode nanobeam cavities. The molecular screening effect on nanotube emission allows for spectral tuning of the coupling. The Purcell effect of the coupled cavity-exciton system reveals near-unity radiative quantum efficiencies of the excitons in carbon nanotubes.

High-dimensional quantum information processing has emerged as a promising avenue to transcend hardware limitations and advance the frontiers of quantum technologies. Harnessing the untapped potential of the so-called qudits necessitates the development of quantum protocols beyond the established qubit methodologies. Here, we present a robust, hardware-efficient, and scalable approach for operating multidimensional solid-state systems using Raman-assisted two-photon interactions. We then utilize them to construct extensible multi-qubit operations, realize highly entangled multidimensional states including atomic squeezed states and Schrödinger cat states, and implement programmable entanglement distribution along a qudit array. Our work illuminates the quantum electrodynamics of strongly driven multi-qudit systems and provides the experimental foundation for the future development of high-dimensional quantum applications such as quantum sensing and fault-tolerant quantum computing. The full-fledged development of qudits in superconducting circuits is hindered by limited interaction toolkit and stringent requirements on frequencies and anharmonicities. Here, the authors propose and demonstrate an alternative scheme to perform multi-qudit gates in transmon-based devices, which is based on Raman-assisted two-photon interactions. [ABSTRACT FROM AUTHOR]

Quantum fluctuations can inhibit long-range ordering in frustrated magnets and potentially lead to quantum spin liquid (QSL) phases. A prime example are gapless QSLs with emergent U(1) gauge fields, which have been understood to be described in terms of quantum electrodynamics in 2+1 dimension (QED3). Despite several promising candidate materials, however, a complicating factor for their realisation is the presence of other degrees of freedom. In particular lattice distortions can act to relieve magnetic frustration, precipitating conventionally ordered states. In this work, we use field-theoretic arguments as well as extensive numerical simulations to show that the U(1) Dirac QSL on the triangular and kagome lattices exhibits a weak-coupling instability due to the coupling of monopoles of the emergent gauge field to lattice distortions, leading to valence-bond solid ordering. This generalises the spin-Peierls instability of one-dimensional quantum critical spin chains to two-dimensional algebraic QSLs. We study static distortions as well as quantum-mechanical phonons. Even in regimes where the QSL is stable, the singular spin-lattice coupling leads to marked temperature-dependent corrections to the phonon spectrum, which provide salient experimental signatures of spin fractionalisation. We discuss the coupling of QSLs to the lattice as a general tool for their discovery and characterisation. Quantum spin liquids can emerge in frustrated magnets where quantum fluctuations prevent long-range order. Seifert et al. show that spin-lattice couplings can relieve magnetic frustration and destabilise 2D gapless quantum spin liquid states with fractionalised excitations, analogous to the 1D spin-Peierls instability. [ABSTRACT FROM AUTHOR]

The interaction of light and matter at the single-photon level is of central importance in various fields of physics, including, e.g., condensed matter physics, astronomy, quantum optics, and quantum information. Amplification of such quantum light–matter interaction can be highly beneficial to, e.g., improve device performance, explore novel phenomena, and understand fundamental physics, and has therefore been a long-standing goal. Furthermore, simulation of light–matter interaction in the regime of ultrastrong coupling, where the interaction strength is comparable to the bare frequencies of the uncoupled systems, has also become a hot research topic, and considerable progress has been made both theoretically and experimentally in the past decade. In this review, we provide a detailed introduction of recent advances in amplification of quantum light–matter interaction and simulation of ultrastrong light–matter interaction, particularly in cavity and circuit quantum electrodynamics and in cavity optomechanics. [ABSTRACT FROM AUTHOR]