Strongly correlated multielectron bunches from interaction with quantum light.

Strongly correlated electron systems are a cornerstone of modern physics, being responsible for groundbreaking phenomena from superconducting magnets to quantum computing. In most cases, correlations in electrons arise exclusively because of Coulomb interactions. In this work, we reveal that free electrons interacting simultaneously with a light field can become highly correlated via mechanisms beyond Coulomb interactions. In the case of two electrons, the resulting Pearson correlation coefficient for the joint probability distribution of the output electron energies is enhanced by more than 13 orders of magnitude compared to that of electrons interacting with the light field in succession (one after another). These highly correlated electrons are the result of momentum and energy exchange between the participating electrons via the external quantum light field. Our findings pave the way to the creation and control of highly correlated free electrons for applications including quantum information and ultrafast imaging.

Intense Squeezed Light from Lasers with Sharply Nonlinear Gain at Optical Frequencies.

Nonclassical states of light, such as number-squeezed light, with fluctuations below the classical shot noise level, have important uses in metrology, communication, quantum information processing, and quantum simulation. However, generating these nonclassical states of light, especially with high intensity and a high degree of squeezing, is challenging. To address this problem, we introduce a new concept which uses gain to generate intense sub-Poissonian light at optical frequencies. It exploits a strongly nonlinear gain for photons which arises from a combination of frequency-dependent gain and Kerr nonlinearity. In this laser architecture, the interaction between the gain medium and Kerr nonlinearity suppresses the spontaneous emission at high photon number states, leading to a strong "negative feedback" that suppresses photon-number fluctuations. We discuss realistic implementations of this concept based on the use of solid-state gain media in laser cavities with Kerr nonlinear materials, showing how 90% squeezing of photon number fluctuations below the shot noise level can be realized.

Lossless Monochromator in an Ultrafast Electron Microscope Using Near-Field THz Radiation.

The ability to form monoenergetic electron beams is vital for high-resolution electron spectroscopy and imaging. Such capabilities are commonly achieved using an electron monochromator, which energy filters a dispersed electron beam, thus reducing the electron flux to yield down to meV energy resolution. This reduction in flux hinders the use of monochromators in many applications, such as ultrafast transmission electron microscopes (UTEMs). Here, we develop and demonstrate a mechanism for electron energy monochromation that does not reduce the flux-a lossless monochromator. The mechanism is based on the interaction of free-electron pulses with single-cycle THz near fields, created by nonlinear conversion of an optical laser pulse near the electron beam path inside a UTEM. Our experiment reduces the electron energy spread by a factor of up to 2.9 without compromising the beam flux. Moreover, as the electron-THz interaction takes place over an extended region of many tens of microns in free space, the realized technique is highly robust-granting uniform monochromation over a wide area, larger than the electron beam diameter. We further demonstrate the wide tunability of our method by monochromating the electron beam at multiple primary electron energies from 60 to 200 keV, studying the effect of various electron and THz parameters on its performance. Our findings have direct applications in the fast-growing field of ultrafast electron microscopy, allowing time- and energy-resolved studies of exciton physics, phononic vibrational resonances, charge transport effects, and optical excitations in the mid IR to the far IR.

Biasing the quantum vacuum to control macroscopic probability distributions.

Quantum field theory suggests that electromagnetic fields naturally fluctuate, and these fluctuations can be harnessed as a source of perfect randomness. Many potential applications of randomness rely on controllable probability distributions. We show that vacuum-level bias fields injected into multistable optical systems enable a controllable source of quantum randomness, and we demonstrated this concept in an optical parametric oscillator (OPO). By injecting bias pulses with less than one photon on average, we controlled the probabilities of the two possible OPO output states. The potential of our approach for sensing sub-photon-level fields was demonstrated by reconstructing the temporal shape of fields below the single-photon level. Our results provide a platform to study quantum dynamics in nonlinear driven-dissipative systems and point toward applications in probabilistic computing and weak field sensing.

Ultrafast Electron Microscopy of Nanoscale Charge Dynamics in Semiconductors.

The ultrafast dynamics of charge carriers in solids plays a pivotal role in emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, the investigation and direct visualization of such nonequilibrium phenomena remains as a long-standing challenge, owing to the nanometer-femtosecond spatiotemporal scales at which the charge carriers evolve. Here, we propose and demonstrate an interaction mechanism enabling nanoscale imaging of the femtosecond dynamics of charge carriers in solids. This imaging modality, which we name charge dynamics electron microscopy (CDEM), exploits the strong interaction of free-electron pulses with terahertz (THz) near fields produced by the moving charges in an ultrafast scanning transmission electron microscope. The measured free-electron energy at different spatiotemporal coordinates allows us to directly retrieve the THz near-field amplitude and phase, from which we reconstruct movies of the generated charges by comparison to microscopic theory. The CDEM technique thus allows us to investigate previously inaccessible spatiotemporal regimes of charge dynamics in solids, providing insight into the photo-Dember effect and showing oscillations of photogenerated electron-hole distributions inside a semiconductor. Our work facilitates the exploration of a wide range of previously inaccessible charge-transport phenomena in condensed matter using ultrafast electron microscopy.

Creating large Fock states and massively squeezed states in optics using systems with nonlinear bound states in the continuum.

The quantization of the electromagnetic field leads directly to the existence of quantum mechanical states, called Fock states, with an exact integer number of photons. Despite these fundamental states being long-understood, and despite their many potential applications, generating them is largely an open problem. For example, at optical frequencies, it is challenging to deterministically generate Fock states of order two and beyond. Here, we predict the existence of an effect in nonlinear optics, which enables the deterministic generation of large Fock states at arbitrary frequencies. The effect, which we call an n-photon bound state in the continuum, is one in which a photonic resonance (such as a cavity mode) becomes lossless when a precise number of photons n is inside the resonance. Based on analytical theory and numerical simulations, we show that these bound states enable a remarkable phenomenon in which a coherent state of light, when injected into a system supporting this bound state, can spontaneously evolve into a Fock state of a controllable photon number. This effect is also directly applicable for creating (highly) squeezed states of light, whose photon number fluctuations are (far) below the value expected from classical physics (i.e., shot noise). We suggest several examples of systems to experimentally realize the effects predicted here in nonlinear nanophotonic systems, showing examples of generating both optical Fock states with large n (n >  10), as well as more macroscopic photonic states with very large squeezing, with over 90% less noise (10 dB) than the classical value associated with shot noise.

Quantum sensing of strongly coupled light-matter systems using free electrons.

Strong coupling in light-matter systems is a central concept in cavity quantum electrodynamics and is essential for many quantum technologies. Especially in the optical range, full control of highly connected multi-qubit systems necessitates quantum coherent probes with nanometric spatial resolution, which are currently inaccessible. Here, we propose the use of free electrons as high-resolution quantum sensors for strongly coupled light-matter systems. Shaping the free-electron wave packet enables the measurement of the quantum state of the entire hybrid systems. We specifically show how quantum interference of the free-electron wave packet gives rise to a quantum-enhanced sensing protocol for the position and dipole orientation of a subnanometer emitter inside a cavity. Our results showcase the great versatility and applicability of quantum interactions between free electrons and strongly coupled cavities, relying on the unique properties of free electrons as strongly interacting flying qubits with miniscule dimensions.

A framework for scintillation in nanophotonics.

Bombardment of materials by high-energy particles often leads to light emission in a process known as scintillation. Scintillation has widespread applications in medical imaging, x-ray nondestructive inspection, electron microscopy, and high-energy particle detectors. Most research focuses on finding materials with brighter, faster, and more controlled scintillation. We developed a unified theory of nanophotonic scintillators that accounts for the key aspects of scintillation: energy loss by high-energy particles, and light emission by non-equilibrium electrons in nanostructured optical systems. We then devised an approach based on integrating nanophotonic structures into scintillators to enhance their emission, obtaining nearly an order-of-magnitude enhancement in both electron-induced and x-ray-induced scintillation. Our framework should enable the development of a new class of brighter, faster, and higher-resolution scintillators with tailored and optimized performance.

Superradiance and Subradiance due to Quantum Interference of Entangled Free Electrons.

When multiple quantum emitters radiate, their emission rate may be enhanced or suppressed due to collective interference in a process known as super- or subradiance. Such processes are well known to occur also in light emission from free electrons, known as coherent cathodoluminescence. Unlike atomic systems, free electrons have an unbounded energy spectrum, and, thus, all their emission mechanisms rely on electron recoil, in addition to the classical properties of the dielectric medium. To date, all experimental and theoretical studies of super- and subradiance from free electrons assumed only classical correlations between particles. However, dependence on quantum correlations, such as entanglement between free electrons, has not been studied. Recent advances in coherent shaping of free-electron wave functions motivate the investigation of such quantum regimes of super- and subradiance. In this Letter, we show how a pair of coincident path-entangled electrons can demonstrate either super- or subradiant light emission, depending on the two-particle wave function. By choosing different free-electron Bell states, the spectrum and emission pattern of the light can be reshaped, in a manner that cannot be accounted for by a classical mixed state. We show these results for light emission in any optical medium and discuss their generalization to many-body quantum states. Our findings suggest that light emission can be sensitive to the explicit quantum state of the emitting matter wave and possibly serve as a nondestructive measurement scheme for measuring the quantum state of many-body systems.

Casimir Light in Dispersive Nanophotonics.

Time-varying optical media, whose dielectric properties are actively modulated in time, introduce a host of novel effects in the classical propagation of light, and are of intense current interest. In the quantum domain, time-dependent media can be used to convert vacuum fluctuations (virtual photons) into pairs of real photons. We refer to these processes broadly as "dynamical vacuum effects" (DVEs). Despite interest for their potential applications as sources of quantum light, DVEs are generally very weak, presenting many opportunities for enhancement through modern techniques in nanophotonics, such as using media which support excitations such as plasmon and phonon polaritons. Here, we present a theory of weakly modulated DVEs in arbitrary nanostructured, dispersive, and dissipative systems. A key element of our framework is the simultaneous incorporation of time-modulation and "dispersion" through time-translation-breaking linear response theory. As an example, we use our approach to propose a highly efficient scheme for generating entangled surface polaritons based on time-modulation of the optical phonon frequency of a polar insulator.

Toward Atomic-Resolution Quantum Measurements with Coherently Shaped Free Electrons.

Free electrons provide a powerful tool for probing material properties at atomic resolution. Recent advances in ultrafast electron microscopy enable the manipulation of free-electron wave functions using laser pulses. It would be of great importance if one could combine the spatial resolution of electron microscopes with the ability of laser pulses to probe coherent phenomena in quantum systems. To this end, we propose a novel concept that leverages free electrons that are coherently shaped by laser pulses to measure quantum coherence in materials. We develop the quantum theory of interactions between shaped electrons and arbitrary qubit states in materials, and show how the postinteraction electron energy spectrum enables measuring the qubit state (on the Bloch sphere) and the decoherence or relaxation times (T_{2}/T_{1}). Finally, we describe how such electrons can detect and quantify superradiance from multiple qubits. Our scheme can be implemented in ultrafast transmission electron microscopes (UTEM), opening the way toward the full characterization of the state of quantum systems at atomic resolution.

Creating heralded hyper-entangled photons using Rydberg atoms.

Entangled photon pairs are a fundamental component for testing the foundations of quantum mechanics, and for modern quantum technologies such as teleportation and secured communication. Current state-of-the-art sources are based on nonlinear processes that are limited in their efficiency and wavelength tunability. This motivates the exploration of physical mechanisms for entangled photon generation, with a special interest in mechanisms that can be heralded, preferably at telecommunications wavelengths. Here we present a mechanism for the generation of heralded entangled photons from Rydberg atom cavity quantum electrodynamics (cavity QED). We propose a scheme to demonstrate the mechanism and quantify its expected performance. The heralding of the process enables non-destructive detection of the photon pairs. The entangled photons are produced by exciting a rubidium atom to a Rydberg state, from where the atom decays via two-photon emission (TPE). A Rydberg blockade helps to excite a single Rydberg excitation while the input light field is more efficiently collectively absorbed by all the atoms. The TPE rate is significantly enhanced by a designed photonic cavity, whose many resonances also translate into high-dimensional entanglement. The resulting high-dimensionally entangled photons are entangled in more than one degree of freedom: in all of their spectral components, in addition to the polarization-forming a hyper-entangled state, which is particularly interesting in high information capacity quantum communication. We characterize the photon comb states by analyzing the Hong-Ou-Mandel interference and propose proof-of-concept experiments.

The coherence of light is fundamentally tied to the quantum coherence of the emitting particle.

Coherent emission of light by free charged particles is believed to be successfully captured by classical electromagnetism in all experimental settings. However, recent advances triggered fundamental questions regarding the role of the particle wave function in these processes. Here, we find that even in seemingly classical experimental regimes, light emission is fundamentally tied to the quantum coherence and correlations of the emitting particle. We use quantum electrodynamics to show how the particle's momentum uncertainty determines the optical coherence of the emitted light. We find that the temporal duration of Cherenkov radiation, envisioned for almost a century as a shock wave of light, is limited by underlying entanglement between the particle and light. Our findings enable new capabilities in electron microscopy for measuring quantum correlations of shaped electrons. Last, we propose new Cherenkov detection schemes, whereby measuring spectral photon autocorrelations can unveil the wave function structure of any charged high-energy particle.

Control of quantum electrodynamical processes by shaping electron wavepackets.

Fundamental quantum electrodynamical (QED) processes, such as spontaneous emission and electron-photon scattering, encompass phenomena that underlie much of modern science and technology. Conventionally, calculations in QED and other field theories treat incoming particles as single-momentum states, omitting the possibility that coherent superposition states, i.e., shaped wavepackets, can alter fundamental scattering processes. Here, we show that free electron waveshaping can be used to design interferences between two or more pathways in a QED process, enabling precise control over the rate of that process. As an example, we show that free electron waveshaping modifies both spatial and spectral characteristics of bremsstrahlung emission, leading for instance to enhancements in directionality and monochromaticity. The ability to tailor general QED processes opens up additional avenues of control in phenomena ranging from optical excitation (e.g., plasmon and phonon emission) in electron microscopy to free electron lasing in the quantum regime.

The quantum-optical nature of high harmonic generation.

High harmonic generation (HHG) is an extremely nonlinear effect generating coherent broadband radiation and pulse durations reaching attosecond timescales. Conventional models of HHG that treat the driving and emitted fields classically are usually very successful but inherently cannot capture the quantum-optical nature of the process. Although prior work considered quantum HHG, it remains unknown in what conditions the spectral and statistical properties of the radiation depart considerably from the known phenomenology of HHG. The discovery of such conditions could lead to novel sources of attosecond light having squeezing and entanglement. Here, we present a fully-quantum theory of extreme nonlinear optics, predicting quantum effects that alter both the spectrum and photon statistics of HHG, thus departing from all previous approaches. We predict the emission of shifted frequency combs and identify spectral features arising from the breakdown of the dipole approximation for the emission. Our results show that each frequency component of HHG can be bunched and squeezed and that each emitted photon is a superposition of all frequencies in the spectrum, i.e., each photon is a comb. Our general approach is applicable to a wide range of nonlinear optical processes, paving the way towards novel quantum phenomena in extreme nonlinear optics.

Monochromatic X-ray Source Based on Scattering from a Magnetic Nanoundulator.

We present a novel design for an ultracompact, passive light source capable of generating ultraviolet and X-ray radiation, based on the interaction of free electrons with the magnetic near-field of a ferromagnet. Our design is motivated by recent advances in the fabrication of nanostructures, which allow the confinement of large magnetic fields at the surface of ferromagnetic nanogratings. Using ab initio simulations and a complementary analytical theory, we show that highly directional, tunable, monochromatic radiation at high frequencies could be produced from relatively low-energy electrons within a tabletop design. The output frequency is tunable in the extreme ultraviolet to hard X-ray range via electron kinetic energies from 1 keV to 5 MeV and nanograting periods from 1 µm to 5 nm. The proposed radiation source can achieve the tunability and monochromaticity of current free-electron-driven sources (free-electron lasers, synchrotrons, and laser-driven undulators), yet with a significantly reduced scale, cost, and complexity. Our design could help realize the next generation of tabletop or on-chip X-ray sources.

Plasmon-emitter interactions at the nanoscale.

Plasmon-emitter interactions are of central importance in modern nanoplasmonics and are generally maximal at short emitter-surface separations. However, when the separation falls below 10-20 nm, the classical theory deteriorates progressively due to its neglect of quantum effects such as nonlocality, electronic spill-out, and Landau damping. Here we show how this neglect can be remedied in a unified theoretical treatment of mesoscopic electrodynamics incorporating Feibelman [Formula: see text]-parameters. Our approach incorporates nonclassical resonance shifts and surface-enabled Landau damping-a nonlocal damping effect-which have a dramatic impact on the amplitude and spectral distribution of plasmon-emitter interactions. We consider a broad array of plasmon-emitter interactions ranging from dipolar and multipolar spontaneous emission enhancement, to plasmon-assisted energy transfer and enhancement of two-photon transitions. The formalism gives a complete account of both plasmons and plasmon-emitter interactions at the nanoscale, constituting a simple yet rigorous platform to include nonclassical effects in plasmon-enabled nanophotonic phenomena.

Uncured-Labeled Meat Products Produced Using Plant-Derived Nitrates and Nitrites: Chemistry, Safety, and Regulatory Considerations.

Consumers often malign conventional curing agents while concomitantly accepting the natural forms of the same constituents in numerous food products. This paradox ostensibly exceeds all other food-related controversies to date and likely contributes to the rapid expansion of meat products that utilize natural nitrate derivatives. While there is high demand for these products, a fundamental lack of understanding regarding the safety and chemical implications of curing agents, whether derived from synthetic or natural sources, continues to persist. This manuscript elucidates the variations among curing preparations with particular emphasis pertaining to the associated safety, chemical, and regulatory ramifications encompassing these product categories.