arXiv subjects

Thomas Christensen

Publications and source records attributed to Thomas Christensen.

At least 37 records · Page 2Linked to original sources

arXiv2020

Control of quantum electrodynamical processes by shaping electron wavepackets

Fundamental quantum electrodynamical (QED) processes such as spontaneous emission and electron-photon scattering encompass a wealth of phenomena that form one of the cornerstones of modern science and technology. Conventionally, calculations in QED and in other field theories assume that incoming particles are single-momentum states. The possibility that coherent superposition states, i.e. "shaped wavepackets", will alter the result of fundamental scattering processes is thereby neglected, and is instead assumed to sum to an incoherent (statistical) distribution in the incoming momentum. Here, we show that free-electron wave-shaping can be used to engineer quantum interferences that alter the results of scattering processes in QED. Specifically, the interference of two or more pathways in a QED process (such as photon emission) enables precise control over the rate of that process. As an example, we apply our concept to Bremsstrahlung, a ubiquitous phenomenon that occurs, for instance, in X-ray sources for state-of-the-art medical imaging, security scanning, materials analysis, and astrophysics. We show that free electron wave-shaping can be used to tailor both the spatial and the spectral distribution of emitted photons, enhancing their directionality and monochromaticity, and adding more degrees of freedom that make emission processes like Bremsstrahlung more versatile. The ability to tailor the spatiotemporal attributes of photon emission via quantum interference provides a new degree of freedom in shaping radiation across the entire electromagnetic spectrum. More broadly, the ability to tailor general QED processes through the shaping of free electrons opens up new avenues of control in processes ranging from optical excitation processes (e.g., plasmon and phonon emission) in electron microscopy to free electron lasing in the quantum regime.

quant-ph↗

arXiv2019

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↗

arXiv2019

Maximal Spontaneous Photon Emission and Energy Loss from Free Electrons

Free electron radiation such as Cerenkov, Smith--Purcell, and transition radiation can be greatly affected by structured optical environments, as has been demonstrated in a variety of polaritonic, photonic-crystal, and metamaterial systems. However, the amount of radiation that can ultimately be extracted from free electrons near an arbitrary material structure has remained elusive. Here we derive a fundamental upper limit to the spontaneous photon emission and energy loss of free electrons, regardless of geometry, which illuminates the effects of material properties and electron velocities. We obtain experimental evidence for our theory with quantitative measurements of Smith--Purcell radiation. Our framework allows us to make two predictions. One is a new regime of radiation operation---at subwavelength separations, slower (nonrelativistic) electrons can achieve stronger radiation than fast (relativistic) electrons. The second is a divergence of the emission probability in the limit of lossless materials. We further reveal that such divergences can be approached by coupling free electrons to photonic bound states in the continuum (BICs). Our findings suggest that compact and efficient free-electron radiation sources from microwaves to the soft X-ray regime may be achievable without requiring ultrahigh accelerating voltages.

physics.optics↗

arXiv2019

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↗

arXiv2019

A General Theoretical and Experimental Framework for Nanoscale Electromagnetism

Local, bulk response functions, e.g permittivity, and the macroscopic Maxwell equations completely specify the classical electromagnetic problem, which features only wavelength $λ$ and geometric scales. The above neglect of intrinsic electronic length scales $L_{\text{e}}$ leads to an eventual breakdown in the nanoscopic limit. Here, we present a general theoretical and experimental framework for treating nanoscale electromagnetic phenomena. The framework features surface-response functions---known as the Feibelman $d$-parameters---which reintroduce the missing electronic length scales. As a part of our framework, we establish an experimental procedure to measure these complex, dispersive surface response functions, enabled by quasi-normal-mode perturbation theory and observations of pronounced nonclassical effects---spectral shifts in excess of 30% and the breakdown of Kreibig-like broadening---in a quintessential multiscale architecture: film-coupled nanoresonators, with feature-sizes comparable to both $L_{\text{e}}$ and $λ$.

physics.optics↗

arXiv2018

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↗

arXiv2018

Dynamics and Spin-Valley Locking Effects in Monolayer Transition Metal Dichalcogenides

Transition metal dichalcogenides have been the primary materials of interest in the field of valleytronics for their potential in information storage, yet the limiting factor has been achieving long valley decoherence times. We explore the dynamics of four monolayer TMDCs (MoS$_2$, MoSe$_2$, WS$_2$, WSe$_2$) using ab initio calculations to describe electron-electron and electron-phonon interactions. By comparing calculations which both omit and include relativistic effects, we isolate the impact of spin-resolved spin-orbit coupling on transport properties. In our work, we find that spin-orbit coupling increases carrier lifetimes at the valence band edge by an order of magnitude due to spin-valley locking, with a proportional increase in the hole mobility at room temperature. At temperatures of 50~K, we find intervalley scattering times on the order of 100 ps, with a maximum value ~140 ps in WSe$_2$. Finally, we calculate excited-carrier generation profiles which indicate that direct transitions dominate across optical energies, even for WSe$_2$ which has an indirect band gap. Our results highlight the intriguing interplay between spin and valley degrees of freedom critical for valleytronic applications. Further, our work points towards interesting quantum properties on-demand in transition metal dichalcogenides that could be leveraged via driving spin, valley and phonon degrees of freedom.

cond-mat.mes-hall↗

arXiv2018

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↗

arXiv2018

Magnetically-defined topological edge plasmons in edgeless electron gas

Topological materials bear gapped excitations in bulk yet protected gapless excitations at boundaries. Magnetoplasmons (MPs), as high-frequency density excitations of two-dimensional electron gas (2DEG) in a perpendicular magnetic field, embody a prototype of band topology for bosons. The time-reversal-breaking magnetic field opens a topological gap for bulk MPs up to the cyclotron frequency; topologically-protected edge magnetoplasmons (EMPs) bridge the bulk gap and propagate unidirectionally along system's boundaries. However, all the EMPs known to date adhere to physical edges where the electron density terminates abruptly. This restriction has made device application extremely difficult. Here we demonstrate a new class of topological edge plasmons -- domain-boundary magnetoplasmons (DBMPs), within a uniform edgeless 2DEG. Such DBMPs arise at the domain boundaries of an engineered sign-changing magnetic field and are protected by the difference of gap Chern numbers (+/-1) across the magnetic domains. They propagate unidirectionally along the domain boundaries and are immune to domain defects. Moreover, they exhibit wide tunability in the microwave frequency range under an applied magnetic field or gate voltage. Our study opens a new direction to realize high-speed reconfigurable topological devices.

cond-mat.mtrl-sci↗

arXiv2017

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↗

arXiv2017

Limits to the Optical Response of Graphene and 2D Materials

2D materials provide a platform for strong light--matter interactions, creating wide-ranging design opportunities via new-material discoveries and new methods for geometrical structuring. We derive general upper bounds to the strength of such light--matter interactions, given only the optical conductivity of the material, including spatial nonlocality, and otherwise independent of shape and configuration. Our material figure of merit shows that highly doped graphene is an optimal material at infrared frequencies, whereas single-atomic-layer silver is optimal in the visible. For quantities ranging from absorption and scattering to near-field spontaneous-emission enhancements and radiative heat transfer, we consider canonical geometrical structures and show that in certain cases the bounds can be approached, while in others there may be significant opportunity for design improvement. The bounds can encourage systematic improvements in the design of ultrathin broadband absorbers, 2D antennas, and near-field energy harvesters.

physics.optics↗

arXiv2017

Infrared Topological Plasmons in Graphene

We propose a two-dimensional plasmonic platform - periodically patterned monolayer graphene - which hosts topological one-way edge states operable up to infrared frequencies. We classify the band topology of this plasmonic system under time-reversal-symmetry breaking induced by a static magnetic field. At finite doping, the system supports topologically nontrivial bandgaps with mid-gap frequencies up to tens of terahertz. By the bulk-edge correspondence, these bandgaps host topologically protected one-way edge plasmons, which are immune to backscattering from structural defects and subject only to intrinsic material and radiation loss. Our findings reveal a promising approach to engineer topologically robust chiral plasmonic devices and demonstrate a realistic example of high-frequency topological edge state.

cond-mat.mes-hall↗

arXiv2016

Low-loss Plasmonic Dielectric Nanoresonators

Material losses in metals are a central bottleneck in plasmonics for many applications. Here we propose and theoretically demonstrate that metal losses can be successfully mitigated with dielectric particles on metallic films, giving rise to hybrid dielectric--metal resonances. In the far field, they yield strong and efficient scattering, beyond even the theoretical limits of all-metal and all-dielectric structures. In the near field, they offer high-Purcell-factor (${>}5000$), high-quantum-efficiency (${>}90\%$), and highly directional emission at visible and infrared wavelengths. Their quality factors can be readily tailored from plasmonic-like (${\sim}10$) to dielectric-like (${\sim}10^3$), with wide control over the individual resonant coupling to photon, plasmon, and dissipative channels. Compared with conventional plasmonic nanostructures, such resonances show robustness against detrimental nonlocal effects and provide higher field enhancement at extreme nanoscopic sizes and spacings. These hybrid resonances equip plasmonics with high efficiency, which has been the predominant goal since the field's inception.

physics.optics↗

arXiv2016

Quantum corrections in nanoplasmonics: shape, scale, and material

The classical treatment of plasmonics is insufficient at the nanometer-scale due to quantum mechanical surface phenomena. Here, an extension to the classical paradigm is reported which rigorously remedies this deficiency through the incorporation of first-principles surface response functions - the Feibelman d-parameters - in general geometries. Several analytical results for the leading-order plasmonic quantum corrections are obtained in a first-principles setting; particularly, a clear separation of the roles of shape, scale, and material is established. The utility of the formalism is illustrated by the derivation of a modified sum-rule for complementary structures, a rigorous reformulation of Kreibig's phenomenological damping prescription, and an account of the small-scale resonance-shifting of simple and noble metal nanostructures. These insights open the technological design space and deepen our fundamental understanding of nanoplasmonics beyond the classical regime.

cond-mat.mes-hall↗

arXiv2015

Kerr nonlinearity and plasmonic bistability in graphene nanoribbons

We theoretically examine the role of Kerr nonlinearities for graphene plasmonics in nanostructures, specifically in nanoribbons. The nonlinear Kerr interaction is included semiclassically in the intraband approximation. The resulting electromagnetic problem is solved numerically by self-consistent iteration with linear steps using a real-space discretization. We derive a simple approximation for the resonance shifts in general graphene nanostructures, and obtain excellent agreement with numerics for moderately high field strengths. Near plasmonic resonances the nonlinearities are strongly enhanced due to field enhancement, and the total nonlinearity is significantly affected by the field inhomogeneity of the plasmonic excitation. Finally, we discuss the emergence of a plasmonic bistability which exists for frequencies redshifted relative to the linear resonance. Our results offer new insights into the role of nonlinear interaction in nanostructured graphene and paves the way for experimental investigation.

cond-mat.mes-hall↗

arXiv2015

Multipole plasmons and their disappearance in few-nanometer silver nanoparticles

In electron energy-loss spectroscopy (EELS) of individual silver nanoparticles encapsulated in silicon nitride, we observe besides the usual dipole resonance an additional surface plasmon (SP) resonance corresponding to higher angular momenta. We even observe both resonances for nanoparticle radii as small as 4 nm, where previously only the dipole resonance was assumed to play a role. Electron beams positioned outside of the particles mostly excite the dipole mode, but the higher-order resonance can even dominate the dipole peak when exciting at the particle surface, the usual choice for maximal EELS signal. This allows us to study the radius dependence of both resonances separately. For particles smaller than 4 nm, the higher-order SP mode disappears, in agreement with generalized nonlocal optical response (GNOR) theory, while the dipole resonance blueshift exceeds GNOR predictions. Unlike in optical spectra, multipole surface plasmons are important in EELS spectra even of ultra-small metallic nanoparticles.

physics.optics↗

arXiv2014

Localized plasmons in graphene-coated nanospheres

We present an analytical derivation of the electromagnetic response of a spherical object coated by a conductive film, here exemplified by a graphene coating. Applying the framework of Mie-Lorenz theory augmented to account for a conductive boundary condition, we derive the multipole scattering coefficients, modified essentially through the inclusion of an additive correction in numerator and denominator. By reductionist means, starting from the retarded response, we offer simple results in the quasistatic regime by analyzing the multipolar polarizability and associated dispersion equation for the localized plasmons. We consider graphene coatings of both dielectric and conducting spheres, where in the former case the graphene coating introduces the plasmons and in the latter case modifies in interesting ways the existing ones. Finally, we discuss our analytical results in the context of extinction cross-section and local density of states. Recent demonstrations of fabricated spherical graphene nanostructures make our study directly relevant to experiments.

cond-mat.mes-hall↗

arXiv2014

Plasmonic eigenmodes in individual and bow-tie graphene nanotriangles

Serving as a new two-dimensional plasmonic material, graphene has stimulated an intensive study of its optical properties which benefit from the unique electronic band structure of the underlying honeycomb lattice of carbon atoms. In classical electrodynamics, nanostructured graphene is commonly modeled by the computationally demanding problem of a three-dimensional conducting film of atomic-scale thickness. Here, we propose an efficient alternative two-dimensional electrostatic approach where all the calculation procedures are restricted to the plane of the graphene sheet. To explore possible quantum effects, we perform tight-binding calculations, adopting a random-phase approximation. We investigate the multiple plasmon modes in triangles of graphene, treating the optical response classically as well as quantum mechanically in the case of both armchair and zigzag edge termination of the underlying atomic lattice. Compared to the classical plasmonic spectrum which is "blind" to the edge termination, we find that the quantum plasmon frequencies exhibit blueshifts in the case of armchair edge termination, while redshifts are found for zigzag edges. Furthermore, we find spectral features in the zigzag case which are associated with electronic edge states not present for armchair termination. Merging pairs of such triangles into dimers, the plasmon hybridization leads to energy splitting in accordance with plasmon-hybridization theory, with a lower energy for the antisymmetric modes and a smaller splitting for modes with less confinement to the gap region. The hybridization appears strongest in classical calculations while the splitting is lower for armchair edges and even more reduced for zigzag edges. Our various results illustrate a surprising phenomenon: Even 20 nm large graphene structures clearly exhibit quantum plasmonic features due to atomic-scale details in the edge termination.

cond-mat.mes-hall↗