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Nicholas Rivera

Publications and source records attributed to Nicholas Rivera.

At least 55 records · Page 3Linked to original sources

Light emission is fundamentally tied to the quantum coherence of the emitting particle

Coherent emission of light by free charged particles is ubiquitous in many areas of physics and engineering, with the light's properties believed to be successfully captured by classical electromagnetism in all relevant experimental settings. The advent of interactions between light and free quantum matter waves brought about fundamental questions regarding the role of the particle wavefunction. Here we show that even in seemingly classical experimental regimes, light emission is fundamentally tied to quantum properties of the emitting particles, such as their quantum coherence and correlations. By employing quantum electrodynamics, we unveil the role of the particle's coherent momentum uncertainty, without which decoherence of light becomes dominant. As an example, we consider Cherenkov radiation, envisioned for almost a century as a shockwave of light. We find instead that the shockwave's duration is fundamentally bound from below by the particle's coherent momentum uncertainty due to the underlying entanglement between the particle and light. This quantum optical paradigm opens new capabilities in analytical electron microscopy, enabling the measurement of quantum correlations of shaped electron wavepackets. Our findings also have applications for Cherenkov detectors in particle physics. For example, by measuring spectral photon autocorrelations, one can unveil the particle's wavefunction size, shape and coherence. Such schemes are especially intriguing for many high-energy particles, where other techniques are not available.

quant-ph↗

Towards atomic-resolution quantum measurements with coherently-shaped free electrons

Free electrons provide a powerful tool to probe material properties at atomic-scale spatial resolution. Recent advances in ultrafast electron microscopy enable the manipulation of free electron wavefunctions using laser pulses. It would be of great importance if one could combine the spatial resolution of electron probes with the ability of laser pulses to probe coherent phenomena in quantum systems. To this end, we propose a novel technique that leverages free electrons that are coherently-shaped by laser pulses to measure quantum coherence in materials. Developing a quantum theory of electron-qubit interactions in materials, we show how the energy spectrum of laser-shaped electrons enables measuring the qubit Block-sphere state and decoherence time (T2). Finally, we present how such shaped electrons can detect and quantify superradiance from multiple qubits. Our scheme could be implemented in an ultrafast transmission electron microscope (UTEM), opening the way towards the full characterization of the state of quantum systems at atomic-scale resolution.

quant-ph↗

Light-matter interactions with photonic quasiparticles

Interactions between light and matter play an instrumental role in many fields of science, giving rise to important applications in spectroscopy, sensing, quantum information processing, and lasers. In most of these applications, light is considered in terms of electromagnetic plane waves that propagate at the speed of light in vacuum. As a result, light-matter interactions can usually be treated as very weak, and captured at the lowest order in quantum electrodynamics (QED). However, recent progress in coupling photons to material quasiparticles (e.g., plasmons, phonons, and excitons) forces us to generalize the way we picture the photon at the core of every light-matter interaction. In this new picture, the photon, now of partly matter-character, can have greatly different polarization and dispersion, and be confined to the scale of a few nanometers. Such photonic quasiparticles enable a wealth of light-matter interaction phenomena that could not have been observed before, both in interactions with bound electrons and with free electrons. This Review focuses on exciting theoretical and experimental developments in realizing new light-matter interactions with photonic quasiparticles. As just a few examples, we discuss how photonic quasiparticles enable room-temperature strong coupling, ultrafast "forbidden transitions" in atoms, and new applications of the Cherenkov effect, as well as breakthroughs in ultrafast electron microscopy and new concepts for compact X-ray sources.

physics.optics↗

On the Quantum-Optical Nature of High Harmonic Generation

High harmonic generation (HHG) is an extremely nonlinear effect, where a medium is driven by a strong laser field, generating coherent broadband radiation with photon energies ranging up to the X-ray and pulse durations reaching attosecond timescales. Conventional models of HHG treat the medium quantum mechanically, while the driving and emitted fields are treated classically. Such models are usually very successful, but inherently cannot capture the quantum-optical nature of the process. Despite prior works considering quantum HHG, it is still not known in what circumstances the spectral and statistical properties of the radiation considerably depart from the known phenomenology of HHG. Finding such regimes in HHG could lead to novel sources of attosecond light with intrinsically quantum statistics such as squeezing and entanglement. In this work, we present a fully quantum electrodynamical theory of extreme nonlinear optics with which we predict new quantum effects that alter both spectral and statistical properties of HHG. We predict the emission of shifted frequency combs resulting from transitions between perturbed states of the driven atom, and identify new spectral features that arise from the breakdown of the dipole approximation for the emission. Moreover, we find that each HHG emitted photon is a superposition of all frequencies in the spectrum - e.g., HHG creates single photon combs. We also describe how the HHG process changes in the single atom regime, and discuss how our various predictions can be tested experimentally. Our approach is also applicable to a wide range of nonlinear optical processes, paving the way toward novel quantum information techniques in the EUV and X-ray, and in ultrafast quantum optics.

physics.optics↗

Monochromatic X-ray source based on scattering from a magnetic nanoundulator

We present a novel design for an ultra-compact, 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-5 MeV and nanograting periods from 1 μm-5 nm. Our design reduces the scale, cost, and complexity of current free-electron-driven light schemes, bypassing the need for lengthy acceleration stages in conventional synchrotrons and free-electron lasers and driving lasers in other compact designs. Our design could help realize the next generation of tabletop or on-chip X-ray sources.

physics.optics↗

Plasmon-Emitter Interactions at the Nanoscale

Plasmon-emitter interactions are of paramount 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 progressively deteriorates due to its neglect of quantum mechanical effects such as nonlocality, electronic spill-out, and Landau damping. Here, we show how this neglect can be remedied by presenting a unified theoretical treatment of mesoscopic electrodynamics grounded on the framework of Feibelman $d$-parameters. Crucially, our technique naturally 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 presented here gives a complete account of both plasmons and plasmon-emitter interactions at the nanoscale, constituting a simple yet rigorous and general platform to incorporate nonclassical effects in plasmon-empowered nanophotonic phenomena.

cond-mat.mes-hall↗

Phonon polaritonics in two-dimensional materials

Extreme confinement of electromagnetic energy by phonon polaritons holds the promise of strong and new forms of control over the dynamics of matter. To bring such control to the atomic-scale limit, it is important to consider phonon polaritons in two-dimensional (2D) systems. Recent studies have pointed out that in 2D, splitting between longitudinal and transverse optical (LO and TO) phonons is absent at the $Γ$ point, even for polar materials. Does this lack of LO--TO splitting imply the absence of a phonon polariton in polar monolayers? Here, we derive a first-principles expression for the conductivity of a polar monolayer specified by the wavevector-dependent LO and TO phonon dispersions. In the long-wavelength (local) limit, we find a universal form for the conductivity in terms of the LO phonon frequency at the $Γ$ point, its lifetime, and the group velocity of the LO phonon. Our analysis reveals that the phonon polariton of 2D is simply the LO phonon of the 2D system. For the specific example of hexagonal boron nitride (hBN), we estimate the confinement and propagation losses of the LO phonons, finding that high confinement and reasonable propagation quality factors coincide in regions which may be difficult to detect with current near-field optical microscopy techniques. Finally, we study the interaction of external emitters with two-dimensional hBN nanostructures, finding extreme enhancement of spontaneous emission due to coupling with localized 2D phonon polaritons, and the possibility of multi-mode strong and ultra-strong coupling between an external emitter and hBN phonons. This may lead to the design of new hybrid states of electrons and phonons based on strong coupling.

cond-mat.mes-hall↗

Variational theory of non-relativistic quantum electrodynamics

The ability to achieve ultra-strong coupling between light and matter promises to bring about new means to control material properties, new concepts for manipulating light at the atomic scale, and fundamentally new insights into quantum electrodynamics (QED). Thus, there is a need to develop quantitative theories of QED phenomena in complex electronic and photonic systems. In this Letter, we develop a variational theory of general non-relativistic QED systems of coupled light and matter. Essential to our ansatz is the notion of an effective photonic vacuum whose modes are different than the modes in the absence of light-matter coupling. This variational formulation leads to a set of general equations that can describe the ground state of multi-electron systems coupled to many photonic modes in real space. As a first step towards a new ab initio approach to ground and excited state energies in QED, we apply our ansatz to describe a multi-level emitter coupled to many optical modes, a system with no analytical solution. We find a compact semi-analytical formula which describes ground and excited state energies to less than 1% error in all regimes of coupling parameters allowed by sum rules. Additionally, our formulation provides essentially a non-perturbative theory of Lamb shifts and Casimir-Polder forces, as well as suggesting new physical concepts such as the Casimir energy of a single atom in a cavity. Our method should give rise to highly accurate descriptions of phenomena in general QED systems, such as Casimir forces, Lamb shifts, spontaneous emission, and other fluctuational electrodynamical effects.

quant-ph↗

Extreme enhancement of spin relaxation mediated by surface magnon polaritons

Polaritons in metals, semimetals, semiconductors, and polar insulators, with their extreme confinement of electromagnetic energy, provide many promising opportunities for enhancing typically weak light-matter interactions such as multipolar radiation, multiphoton spontaneous emission, Raman scattering, and material nonlinearities. These highly confined polaritons are quasi-electrostatic in nature, with most of their energy residing in the electric field. As a result, these "electric" polaritons are far from optimized for enhancing emission of a magnetic nature, such as spin relaxation, which is typically many orders of magnitude slower than corresponding electric decays. Here, we propose using surface magnon polaritons in negative magnetic permeability materials such as MnF$_2$ and FeF$_2$ to strongly enhance spin-relaxation in nearby emitters in the THz spectral range. We find that these magnetic polaritons in 100 nm thin-films can be confined to lengths over 10,000 times smaller than the wavelength of a photon at the same frequency, allowing for a surprising twelve orders of magnitude enhancement in magnetic dipole transitions. This takes THz spin-flip transitions, which normally occur at timescales on the order of a year, and forces them to occur at sub-ms timescales. Our results suggest an interesting platform for polaritonics at THz frequencies, and more broadly, a new way to use polaritons to control light-matter interactions.

physics.optics↗

Ab initio calculation of phonon polaritons in silicon carbide and boron nitride

The ability to use photonic quasiparticles to control electromagnetic energy far below the diffraction limit is a defining paradigm in nanophotonics. An important recent development in this field is the measurement and manipulation of extremely confined phonon-polariton modes in polar dielectrics such as silicon carbide and hexagonal boron nitride, which pave the way for nanophotonics and extreme light-matter interactions in the mid-IR to THz frequency range. To further advance this promising field, it is of great interest to predict the optical response of recently discovered and yet-to-be-synthesized polaritonic materials alike. Here we develop a unified framework based on quantum linear response theory to calculate the spatially non-local dielectric function of a polar lattice in arbitrary dimensions. In the case of a three-dimensional bulk material, the spatially local limit of our calculation reproduces standard results for the dielectric response of a polar lattice. Using this framework, we provide ab initio calculations of the dielectric permittivity of important bulk polar dielectrics such as silicon carbide and hexagonal boron nitride in good agreement with experiments. From the ab initio theory, we are able to develop a microscopic understanding of which phonon modes contribute to each component of the dielectric function, as well as predict features in the dielectric function that are a result of weak TO phonons. This formalism also identifies regime(s) where quantum nonlocal effects may correct the phonon polariton dispersion, extremely relevant in recent atomic-scale experiments which confine electromagnetic fields to the scale of 1~nm. Finally, our work points the way towards first principles descriptions of the effect of interface phonons, phonon strong coupling, and chiral phonons on the properties of phonon polaritons.

physics.optics↗

Plasmonics in Argentene

Two-dimensional materials exhibit a fascinating range of electronic and photonic properties vital for nanophotonics, quantum optics and emerging quantum information technologies. Merging concepts from the fields of ab initio materials science and nanophotonics, there is now an opportunity to engineer new photonic materials whose optical, transport, and scattering properties are tailored to attain thermodynamic and quantum limits. Here, we present first-principles calculations predicting that Argentene, a single-crystalline hexagonal close-packed monolayer of Ag, can dramatically surpass the optical properties and electrical conductivity of conventional plasmonic materials. In the low-frequency limit, we show that the scattering rate and resistivity reduce by a factor of three compared to the bulk three-dimensional metal. Most importantly, the low scattering rate extends to optical frequencies in sharp contrast to e.g. graphene, whose scattering rate increase drastically in the near-infrared range due to optical-phonon scattering. Combined with an intrinsically high carrier density, this facilitates highly-confined surface plasmons extending to visible frequencies. We evaluate Argentene across three distinct figures of merit, spanning the spectrum of typical plasmonic applications; in each, Argentene outperforms the state-of-the-art. This unique combination of properties will make Argentene a valuable addition to the two-dimensional heterostructure toolkit for quantum electronic and photonic technologies.

physics.app-ph↗

Shaping Long-lived Electron Wavepackets for Customizable Optical Spectra

Electrons in atoms and molecules are versatile physical systems covering a vast range of light-matter interactions, enabling the physics of Rydberg states, photon-photon bound states, simulation of condensed matter Hamiltonians, and quantum sources of light. A limitation on the versatility of such electronic systems for optical interactions would appear to arise from the discrete nature of the electronic transitions and from the limited ionization energy, constraining the energy scale through which the rich physics of bound electrons can be accessed. In this work, we propose the concept of shaping spatially confined electron wavepackets as superpositions of extended states in the ionization continuum. These wavepackets enable customizable optical emission spectra transitions in the eV-keV range. We find that the specific shaping lengthens the diffraction lifetime of the wavepackets in exchange for increasing their spatial spreads. Finally, we study the spontaneous radiative transitions of these excited states, examining the influence of the wavepacket shape and size on the radiation rate of the excited state. We observe that the rate of radiative capture is primarily limited by the diffraction lifetime of the wavepacket. The approach proposed in this work could have applications towards developing designer emitters at tunable energy and length scales, potentially bringing the physics of Rydberg states to new energy scales and extending the range and versatility of emitters that can be developed using shaped electrons.

quant-ph↗

Controlling light emission with electron wave interference

It is a long standing question whether or not one can change the nature of spontaneous emission by a free electron through shaping the electron wavefunction. On one hand, shaping the electron wavefunction changes the respective charge and current densities of the electron. On the other hand, spontaneous emission of an electron is an incoherent process and can often be insensitive to the shape of the electron wavefunction. In this work, we arrive at an affirmative answer examining Bremsstrahlung radiation by free electron superposition states. We find that the radiation can be markedly different from an incoherent sum of the radiations of the two states because of interference of the radiation amplitudes from the two components of the superposition. The ability to control free electron spontaneous emission via interference may eventually result in a new degree of control over radiation over the entire electromagnetic spectrum in addition to the ability to deterministically introduce quantum behavior into normally classical light emission processes.

quant-ph↗

Tunable UV-Emitters through Graphene Plasmons

Control over the spontaneous emission of light through tailored optical environments remains a fundamental paradigm in nanophotonics. The use of highly-confined plasmons in materials such as graphene provides a promising platform to enhance transition rates in the IR-THz by many orders of magnitude. However, such enhancements involve near-field plasmon modes or other kinds of near-field coupling like quenching, and it is challenging to use these highly confined modes to harness light in the far-field due to the difficulty of plasmonic outcoupling. Here, we propose that through the use of radiative cascade chains in multi-level emitters, IR plasmons can be used to enhance far field spectra in the visible and UV range, even at energies greater than 10 eV. Combining Purcell-enhancement engineering, graphene plasmonics, and radiative cascade can result in a new type of UV emitter whose properties can be tuned by electrically doping graphene. Varying the distance between the emitter and the graphene surface can change the strength of the far-field emission lines by two orders of magnitude. We also find that the dependence of the far-field emission on the Fermi energy is potentially extremely sharp at the onset of interband transitions, allowing the Fermi energy to effectively serve as a "switch" for turning on and off certain plasmonic and far-field emissions.

physics.optics↗

Shaping Polaritons to Reshape Selection Rules

The discovery of orbital angular momentum (OAM) in light established a new degree of freedom by which to control not only its flow but also its interaction with matter. Here, we show that by shaping extremely sub-wavelength polariton modes, for example by imbuing plasmon and phonon polariton with OAM, we engineer which transitions are allowed or forbidden in electronic systems such as atoms, molecules, and artificial atoms. Crucial to the feasibility of these engineered selection rules is the access to conventionally forbidden transitions afforded by sub-wavelength polaritons. We also find that the position of the absorbing atom provides a surprisingly rich parameter for controlling which absorption processes dominate over others. Additional tunability can be achieved by altering the polaritonic properties of the substrate, for example by tuning the carrier density in graphene, potentially enabling electronic control over selection rules. Our findings are best suited to OAM-carrying polaritonic modes that can be created in graphene, monolayer conductors, thin metallic films, and thin films of polar dielectrics such as boron nitride. By building on these findings we foresee the complete engineering of spectroscopic selection rules through the many degrees of freedom in the shape of optical fields.

physics.optics↗

Ultra-light Å-scale Optimal Optical Reflectors

High-reflectance in many state-of-the-art optical devices is achieved with noble metals. However, metals are limited by losses, and for certain applications, by their high mass density. Using a combination of ab initio and optical transfer matrix calculations, we evaluate the behavior of graphene-based Å-scale metamaterials and find that they could act as nearly-perfect reflectors in the mid-long wave infrared (IR) range. The low density of states for electron-phonon scattering and interband excitations leads to unprecedented optical properties for graphene heterostructures, especially alternating atomic layers of graphene and hexagonal boron nitride, at wavelengths greater than $10~μ$m. At these wavelengths, these materials exhibit reflectivities exceeding 99.7% at a fraction of the weight of noble metals, as well as plasmonic mode confinement and quality factors that are greater by an order of magnitude compared to noble metals. These findings hold promise for ultra-compact optical components and waveguides for mid-IR applications. Moreover, unlike metals, the photonic properties of these heterostructures could be actively tuned via chemical and/or electrostatic doping, providing exciting possibilities for tunable devices.

cond-mat.mes-hall↗

All-angle negative refraction of highly squeezed plasmon and phonon polaritons in graphene-boron nitride heterostructures

A fundamental building block for nanophotonics is the ability to achieve negative refraction of polaritons, because this could enable the demonstration of many unique nanoscale applications such as deep-subwavelength imaging, superlens, and novel guiding. However, to achieve negative refraction of highly squeezed polaritons, such as plasmon polaritons in graphene and phonon polaritons in boron nitride (BN) with their wavelengths squeezed by a factor over 100, requires the ability to flip the sign of their group velocity at will, which is challenging. Here we reveal that the strong coupling between plasmon and phonon polaritons in graphene-BN heterostructures can be used to flip the sign of the group velocity of the resulting hybrid (plasmon-phonon-polariton) modes. We predict all-angle negative refraction between plasmon and phonon polaritons, and even more surprisingly, between hybrid graphene plasmons, and between hybrid phonon polaritons. Graphene-BN heterostructures thus provide a versatile platform for the design of nano-metasurfaces and nano-imaging elements.

physics.optics↗

A near-unity efficiency source of entangled guided waves

Surface phonon polaritons are hybrid modes of photons and optical phonons that can propagate on the surface of a polar dielectric. In this work, we show that the precise combination of confinement and bandwidth offered by surface phonon polaritons allows for the ability to create highly efficient sources of entangled light in the IR/THz. Specifically, phonon polaritons can cause emitters to preferentially decay by the emission of pairs of surface phonon polaritons, instead of the previously dominant single-photon emission. We show that such two-photon emission processes can occur on nanosecond time-scales and can be nearly two orders of magnitude faster than competing single-photon transitions, as opposed to being as much as eight to ten orders of magnitude slower in free space. Our results suggest a fundamentally new design strategy for quantum light sources in the IR/THz: ones that prefer to emit a relatively broad spectrum of entangled photons, potentially allowing for new sources of both single and multiple photons.

physics.optics↗