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Corrected calculation for the non-local solution to the g − 2 anomaly and novel results in non-local QED
We provide the corrected calculation of the (g − 2) μ in non-local QED previously done in the literature. In specific, we show the proper technique for calculating loops in non-local QED and use it to find the form factors F 1 (q 2 ) and F 2 (q 2 ) in non-local QED. We also utilize this technique to calculate some novel results in non-local QED, including calculating the correction to the photon self-energy, the modification to the classical Coulomb potential, the modification to the energy levels of the hydrogen atom, and the contribution to the Lamb shift. We also discuss charge dequantization through non-locality, and show that the experimental bounds on the electric charge on Dirac neutrinos, translate into strong flavor-dependent bounds on the scale on non-locality that range between 10 5 −10 10 TeV. We also discuss the inconsistencies of unrenormalized non-local Quantum Field Theories (QFTs) and the need for renormalizing them, even when they are free from UV divergences.
Cavity Controlled Upconversion in CdSe Nanoplatelet Polaritons
Exciton-polaritons provide a versatile platform for investigating quantum electrodynamics effects in chemical systems, such as polariton-altered chemical reactivity. However, using polaritons in chemical contexts will require a better understanding of their photophysical properties under ambient conditions, where chemistry is typically performed. Here, we used cavity quality factor to control strong light–matter interactions and in particular the excited state dynamics of colloidal CdSe nanoplatelets (NPLs) coupled to a Fabry– Pérot optical cavity. With increasing cavity quality factor, we observe significant population of the upper polariton (UP) state, exemplified by the rare observation of substantial UP photoluminescence (PL). Excitation of the lower polariton (LP) states results in upconverted PL emission from the UP branch due to efficient exchange of population between the LP, UP and the reservoir of dark states present in collectively coupled polaritonic systems. In addition, we measure time scales for polariton dynamics ~100 ps, implying great potential for NPL based polariton systems to affect photochemical reaction rates. State-of-the-art quantum dynamical simulations show outstanding quantitative agreement with experiments, and thus provide important insight into polariton photophysical dynamics of collectively coupled nanocrystal-based systems. These findings represent a significant step toward the development of practical polariton photochemistry platforms.
Mirror Birefringence in a Fabry-Perot Cavity and the Detection of Vacuum Birefringence in a Magnetic Field
We discuss the effect of mirror birefringence in two optical schemes designed to detect the quantum-electrodynamics (QED) predictions of vacuum birefringence under the influence of a strong magnetic field, B. Both schemes make use of a high finesse Fabry-Perot cavity (F-P) to increase the average path length of the light in the magnetic field. The first scheme, which we called the frequency scheme, is based on measurement of the beat frequency of two orthogonal polarized laser beams in the cavity. We show that mirror birefringence contributes to the detection uncertainties in first order, resulting in a high susceptibility to small thermal disturbances. We estimate that an unreasonably high thermal stability of ~10-9 K is required to resolve the effect to 0.1%. In the second scheme, which we called the polarization rotation scheme, laser polarized at 45 relative to the B field is injected into the cavity.
Dual-rail encoding with superconducting cavities
The design of quantum hardware that reduces and mitigates errors is essential for practical quantum error correction (QEC) and useful quantum computation. To this end, we introduce the circuit-Quantum Electrodynamics (QED) dual-rail qubit in which our physical qubit is encoded in the single-photon subspace, { | 01 〉 , | 10 〉 } , of two superconducting microwave cavities. The dominant photon loss errors can be detected and converted into erasure errors, which are in general much easier to correct. In contrast to linear optics, a circuit-QED implementation of the dual-rail code offers unique capabilities. Using just one additional transmon ancilla per dual-rail qubit, we describe how to perform a gate-based set of universal operations that includes state preparation, logical readout, and parametrizable single and two-qubit gates. Moreover, first-order hardware errors in the cavities and the transmon can be detected and converted to erasure errors in all operations, leaving background Pauli errors that are orders of magnitude smaller. Hence, the dual-rail cavity qubit exhibits a favorable hierarchy of error rates and is expected to perform well below the relevant QEC thresholds with today’s coherence times.
Floquet-engineered fast SNAP gates in weakly coupled circuit-QED systems
Superconducting cavities with high quality factors, coupled to a fixed-frequency transmon, provide a state-of-the-art platform for quantum information storage and manipulation. The commonly used selective number-dependent arbitrary phase ( SNAP ) gate faces significant challenges in ultrahigh-coherence cavities, where the weak dispersive shifts necessary for preserving high coherence typically result in prolonged gate times. Here, in this work, we propose a protocol to achieve high-fidelity SNAP gates that are orders of magnitude faster than the standard implementation, surpassing the speed limit set by the bare dispersive shift. We achieve this enhancement by dynamically amplifying the dispersive coupling via sideband interactions, followed by quantum optimal control on the Floquet-engineered system. We also present a unified perturbation theory that explains both the gate acceleration and the associated benign drive-induced decoherence, corroborated by Floquet-Markov simulations. These results pave the way for the experimental realization of high-fidelity, selective control of weakly coupled, high-coherence cavities, and expanding the scope of optimal control techniques to a broader class of Floquet quantum systems.
Shining light on the microscopic resonant mechanism responsible for cavity-mediated chemical reactivity
Strong light–matter interaction in cavity environments is emerging as a promising approach to control chemical reactions in a non-intrusive and efficient manner. The underlying mechanism that distinguishes between steering, accelerating, or decelerating a chemical reaction has, however, remained unclear, hampering progress in this frontier area of research. We leverage quantum-electrodynamical density-functional theory to unveil the microscopic mechanism behind the experimentally observed reduced reaction rate under cavity induced resonant vibrational strong light-matter coupling. We observe multiple resonances and obtain the thus far theoretically elusive but experimentally critical resonant feature for a single strongly coupled molecule undergoing the reaction. While we describe only a single mode and do not explicitly account for collective coupling or intermolecular interactions, the qualitative agreement with experimental measurements suggests that our conclusions can be largely abstracted towards the experimental realization. Specifically, we find that the cavity mode acts as mediator between different vibrational modes. In effect, vibrational energy localized in single bonds that are critical for the reaction is redistributed differently which ultimately inhibits the reaction.
A Meta-Generalized Gradient Approximation for the Cavity-Dependent Exchange-Correlation Interaction in Strongly Coupled Light–Matter Systems
Strong light–matter coupling in optical cavities enables the manipulation of chemical and physical properties without altering molecular composition. Theoretical modeling of such phenomena requires exchange-correlation (XC) functionals that account for both electron–electron and electron–photon (ep) interactions within quantum electrodynamical density functional theory (QEDFT). In this work, we develop a meta-generalized gradient approximation (meta-GGA) specifically targeting the cavity-dependent XC interaction in strongly coupled light–matter systems. This novel approximation is built upon a new semilocal polarizability approximation, which draws from the jellium-with-a-gap model, and can be extended to a “global hybrid” variant that goes beyond the isotropic model from previous approximations. The polarizability model yields significantly improved dispersion coefficients and benchmark calculations with the cavity-dependent XC functional demonstrate improved agreement with QED Hartree–Fock (QED-HF) reference energies. Application to the regioselectivity of brominated nitrobenzene intermediates reveals the functional’s capacity to capture cavity-induced energetic shifts. In conclusion, our results advance the Jacob’s ladder of functionals for QEDFT and provide a practical tool for modeling polaritonic chemistry.
Cavity-modified molecular dipole switching dynamics
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.
Circuit QED Pulse Control Interface
The Circuit Quantum Electrodynamics (Circuit QED) Pulse Control Interface provides a robust platform for designing and testing control signals in transmon-cavity systems. Utilizing a PyQt5-based drag-and-drop GUI, this tool facilitates the implementation of two key protocols: Selective Number-dependent Arbitrary Phase (SNAP)-Displacement and Echoed Conditional Displacement (ECD). It offers real-time pulse visualization and supports CSV exports and imports for integrating custom signals, thereby enhancing circuit QED experimental workflows. Simulations performed using QuTiP confirm the high fidelity of quantum state preparations and the effectiveness of the implemented controls. Future developments will focus on interfacing the tool with hardware and enhancing signal generation accuracy.
Chiral flat-band optical cavity with atomically thin mirrors
A fundamental requirement for photonic technologies is the ability to control the confinement and propagation of light. Widely used platforms include two-dimensional (2D) optical microcavities in which electromagnetic waves are confined in either metallic or distributed Bragg reflectors. Recently, transition metal dichalcogenides hosting tightly bound excitons with high optical quality have emerged as promising atomically thin mirrors. In this work, we propose and experimentally demonstrate a subwavelength 2D nanocavity using two atomically thin mirrors with degenerate resonances. Angle-resolved measurements show a flat band, which sets this system apart from conventional photonic cavities. We demonstrate how the excitonic nature of the mirrors enables the formation of chiral and tunable optical modes upon the application of an external magnetic field. Moreover, we show the electrical tunability of the confined mode. Our work demonstrates a mechanism for confining light with high-quality excitonic materials, opening perspectives for spin-photon interfaces, and chiral cavity electrodynamics.
The constructive method for massive particles in QED
The constructive method of determining amplitudes from on-shell pole structure has been shown to be promising for calculating amplitudes in a more efficient way. However, challenges have been encountered when a massless internal photon is involved in the gluing of three-point amplitudes with massive external particles. In this paper, we use the original on-shell method, old-fashioned perturbation theory, to shed light on the constructive method, and show that one can derive the Feynman amplitude by correctly identifying the residue even when there is an internal photon involved.
Perspective on Many-Body Methods for Molecular Polaritonic Systems
Recent advances in strong light–matter interactions have revealed a wealth of new physical phenomena in molecules embedded in optical cavities, including modified chemical reactivity, altered excitation spectra, and novel quantum correlations. To describe these effects from first-principles, the field of ab initio quantum electrodynamics (QED) has emerged as a compelling extension of quantum chemistry that treats electronic and photonic degrees of freedom on equal footing. In this Perspective, we review the growing landscape of many-body QED methods, including Hartree–Fock, density functional theory (QEDFT), time-dependent DFT (QED-TDDFT), configuration interaction (QED-CI), complete active space (QED-CASSCF), coupled cluster (QED-CC), quantum Monte Carlo (QED-QMC), and density matrix renormalization group (QED-DMRG), highlighting recent developments and implementations. We further explore real-time methods, gradient and Hessian formalisms, and the integration of nonadiabatic nuclear dynamics. Applications range from benchmark simulations of polaritonic chemistry to quantum simulations on emerging quantum hardware. We conclude by outlining future directions for theory development and interdisciplinary efforts at the interface of quantum chemistry, condensed matter, and quantum optics.
When do molecular polaritons behave like optical filters?
This review outlines several linear optical effects featured by molecular polaritons arising in the collective strong light–matter coupling regime. Under weak laser irradiation and when the single-molecule light–matter coupling can be neglected (often in the limit when the number of molecules per photon mode is large), we show that the excited-state molecular dynamics under collective strong coupling can be exactly replicated without the cavity using a shaped (or “filtered”) laser, whose field amplitude is enhanced by the cavity quality factor, shining on the bare molecules. As a consequence, the absorption within a cavity can be understood as the overlap between the polariton transmission and the bare molecular absorption, suggesting that polaritons act in part as optical filters. This framework demystifies and provides a straightforward explanation for a large class of experiments and theoretical models in molecular polaritonics, highlighting that the same effects can be achieved without the cavity with shaped laser pulses. With a few modifications, this simple conceptual picture can also be adapted to understand the incoherent nonlinear response of polaritonic systems. This review establishes a clear distinction between polaritonic phenomena that can be fully explained through classical linear optics and those that require a quantum electrodynamics approach. It also highlights the need to differentiate between effects that necessitate polaritons (i.e., hybrid light–matter states) and those that can occur in the weak coupling regime. Here, we further discuss that certain quantum optical effects like fluorescence can be partially described as optical filtering, whereas some others like cavity-induced Raman scattering go beyond this. Further exploration in these areas is needed to uncover novel polaritonic phenomena beyond optical filtering.
Theory predicts 2D chiral polaritons based on achiral Fabry–Pérot cavities using apparent circular dichroism
Abstract Realizing polariton states with high levels of chirality offers exciting prospects for quantum information, sensing, and lasing applications. Such chirality must emanate from either the involved optical resonators or the quantum emitters. Here, we theoretically demonstrate a rare opportunity for realizing polaritons with so-called 2D chirality by strong coupling of the optical modes of (high finesse) achiral Fabry–Pérot cavities with samples exhibiting “apparent circular dichroism” (ACD). ACD is a phenomenon resulting from an interference between linear birefringence and dichroic interactions. By introducing a quantum electrodynamical theory of ACD, we identify the design rules based on which 2D chiral polaritons can be produced, and their chirality can be optimized.
Ab Initio Polariton Transport Dynamics with the Classical Path Approximation
We present an ab initio framework for simulating polariton transport dynamics based on the classical path approximation (CPA). The quantum dynamics of polariton transport involves simulating many electronic degrees of freedom, making a fully ab initio dynamics simulation computationally expensive. We demonstrate that the CPA, which removes the need for excited-state nuclear gradients, is well-suited for polaritonic systems because collective light–matter coupling leads to vanishing excited-state forces. Benchmark comparisons between CPA and full evaluation of the excited-state forces show excellent agreement for polariton transport results in model light–matter systems such as polariton group velocities and mean-squared displacements. Ab initio simulations of polariton transport using CPA reproduce key physical trends that are observed in experiments with BODIPY molecules. Our work establishes the CPA as a highly efficient tool for ab initio investigations of transport and energy flow in hybrid light–matter systems.
A precise electron EDM constraint on CP-odd heavy-quark Yukawas
CP-odd Higgs couplings to bottom and charm quarks arise in many extensions of the standard model and are of potential interest for electroweak baryogenesis. These couplings induce a contribution to the electron EDM. The experimental limit on the latter then leads to a strong bound on the CP-odd Higgs couplings. We point out that this bound receives large QCD corrections, even though it arises from a leptonic observable. We calculate the contribution of CP-odd Higgs couplings to the bottom and charm quarks in renormalisation-group improved perturbation theory at next-to-leading order in the strong interaction, thereby reducing the uncertainty to a few percent.
Photon Frequency Conversion in High-Q Superconducting Resonators: Axion Electrodynamics, QED, and Nonlinear Meissner Radiation
High-Q superconducting resonators have been proposed and developed as detectors of light-by-light scattering mediated by the hypothesized axion or virtual electron–positron pairs in quantum electrodynamics: the Euler–Heisenberg (EH) interaction. Photon frequency and mode conversion is central to the scheme for detecting such rare events. Superconducting resonators are nonlinear devices. The Meissner screening currents that confine the electromagnetic fields to the vacuum region of a superconducting RF cavity are nonlinear functions of the EM field at the vacuum–superconducting interface, and as a result can generate source currents and frequency conversion of microwave photons in the cavity. In this report we consider photon frequency and mode conversion in superconducting resonators with high quality factors from Meissner currents in single- and dual-cavity setups proposed for axion and QED searches based on light-by-light scattering. In a single cavity with two pump modes, photon frequency conversion by the Meissner screening current dominates photon generation by the EH interaction for cavities with Q≲1012. The Meissner currents also generate background photons that limit the operation of the resonator for axion detection in three-mode, single-cavity setups. We also consider the leakage of photons from pump modes into the signal mode for both axion- and EH-mediated light-by-light scattering. Photon frequency conversion by the EH interaction can compete with Meissner and leakage radiation in ultra-high-Q cavities that are beyond the current state of the art. Meissner radiation and leakage backgrounds can be suppressed in dual-cavity setups with appropriate choices for pump and spectator modes, as well as the single-cavity setup proposed for heterodyne detection of galactic axion dark matter.