arXiv subjects

P. A. D. Gonçalves

Publications and source records attributed to P. A. D. Gonçalves.

At least 19 recordsLinked to original sources

arXiv2026

Surface quantum response of plasmonic heterodimers: revealing the hidden nonlocality

We probe the quantum response of plasmonic heterodimers with extended (plane waves) and localized (point dipoles and electron beams) sources. Implementing the surface-response formalism based on Feibelman parameters, we explore nanosphere heterodimers where one particle is characterized by electron spill-in, while the other by spill-out. We identify situations where the two quantum surface corrections that act in opposite spectral-shift directions can cancel out, producing mesoscopic spectra that do not differ from the predictions of the local-response approximation. This picture changes dramatically once localized sources are implemented, allowing one to selectively probe the quantum response of the particles independently. Such probing occurs in terms of higher-order modes in the case of electron beams, or for the complete modal landscape in the case of point dipole sources. This description offers a new insight into the mechanisms governing light--matter interactions in extreme plasmonic architectures, and opens new perspectives for the understanding and tailoring of plasmonic--quantum emitter architectures.

physics.optics↗

arXiv2026

Probe- and Substrate-Dependent Visibility of Mie Resonances in Silicon Nanospheres

Silicon nanospheres are high-quality optical resonators and promising building blocks for Mie-tronic devices. While the Mie resonances of an isolated sphere are well understood, practical implementations require substrates that inevitably modify the measured optical response. Here, we investigate how substrates alter the observable spectrum of individual nanospheres, focusing on three fundamentally different cases: a thin silicon nitride membrane, that emulates a free-standing particle, bulk silicon, which is common in experiments, and gold, where mirror charges lead to hybrid optical modes. Cathodoluminescence and dark-field spectroscopy, combined with electrodynamic simulations, show that the measured resonances are not intrinsic to the particle but depend strongly on the environment and the excitation mechanism. We find that substrate-induced effects and probe-specific selection rules can suppress, enhance, or even invert the spectral signatures of electric and magnetic modes. These results provide practical guidelines for interpreting and designing substrate-supported dielectric resonators for Mie-tronic applications.

physics.optics↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2025

Roadmap on Nonlocality in Photonic Materials and Metamaterials

Photonic technologies continue to drive the quest for new optical materials with unprecedented responses. A major frontier in this field is the exploration of nonlocal (spatially dispersive) materials, going beyond the local, wavevector-independent assumption traditionally made in optical material modeling. On one end, the growing interest in plasmonic, polaritonic and quantum materials has revealed naturally occurring nonlocalities, emphasizing the need for more accurate models to predict and design their optical responses. This has major implications also for topological, nonreciprocal, and time-varying systems based on these material platforms. Beyond natural materials, artificially structured materials--metamaterials and metasurfaces--can provide even stronger and engineered nonlocal effects, emerging from long-range interactions or multipolar effects. This is a rapidly expanding area in the field of photonic metamaterials, with open frontiers yet to be explored. In the case of metasurfaces, in particular, nonlocality engineering has become a powerful tool for designing strongly wavevector-dependent responses, enabling enhanced wavefront control, spatial compression, multifunctional devices, and wave-based computing. Furthermore, nonlocality and related concepts play a critical role in defining the ultimate limits of what is possible in optics, photonics, and wave physics. This Roadmap aims to survey the most exciting developments in nonlocal photonic materials, highlight new opportunities and open challenges, and chart new pathways that will drive this emerging field forward--toward new scientific discoveries and technological advancements.

cond-mat.mes-hall↗

arXiv2024

Rydberg-atom manipulation through strong interaction with free electrons

Optically trapped Rydberg atoms are a suitable platform to explore quantum many-body physics mediated by long-range atom--atom interactions that can be engineered through externally applied light fields. However, this approach is limited to dipole-allowed transitions and a spatial resolution of the order of the optical wavelength. Here, we theoretically investigate the interaction between free electrons and individual Rydberg atoms as an approach to induce nondipolar transitions with subnanometer spatial precision and a substantial degree of control over the final atomic states. We observe unity-order excitation probabilities produced by a single electron for suitably chosen combinations of electron energies and electron-beam distance to the atom. We further discuss electron--atom entanglement in combination with lateral shaping of the electron followed by postselection. Our results support free electrons as powerful tools to manipulate Rydberg atoms in previously inaccessible ways.

physics.atom-ph↗

arXiv2024

Probing Plexciton Emission from 2D Materials on Gold Nanotrenches

Probing strongly coupled quasiparticle excitations at their intrinsic length scales offers unique insights into their properties and facilitates the design of devices with novel functionalities. In this work, we investigate the formation and emission characteristics of plexcitons, arising from the interaction between surface plasmons in narrow gold nanotrenches and excitons in monolayer WSe2. We study this strong plasmon-exciton coupling in both the far-field and the near-field. Specifically, we observe a Rabi splitting in the far-field reflection spectra of about 80 meV under ambient conditions, consistent with our theoretical modeling. Using a custom-designed near-field probe, we find that plexciton emission originates predominantly from the lower-frequency branch, which we can directly probe and map the local field distribution. We precisely determine the plexciton extension, similar to the trench width, with nanometric precision via collecting spectra at controlled probe locations. Our work opens exciting prospects for nanoscale mapping and engineering of plexcitons in complex nanostructures with potential applications in nanophotonic devices, optoelectronics, and quantum electrodynamics in nanoscale cavities.

cond-mat.mes-hall↗

arXiv2024

Quantum effects in the interaction of low-energy electrons with light

The interaction between free electrons and nanoscale optical fields has emerged as a unique platform to investigate ultrafast processes in matter and explore fundamental quantum phenomena. In particular, optically modulated electrons are employed in ultrafast electron microscopy as noninvasive probes that push the limits of spatiotemporal and spectral resolution down to the picometer--attosecond--microelectronvolt range. Electron kinetic energies well above the involved photon energies are commonly employed, rendering the electron--light coupling efficiency low and, thus, only providing limited access to the wealth of quantum nonlinear phenomena underlying the dynamical response of nanostructures. Here, we theoretically investigate electron--light interactions when photons and electrons have comparable energies, revealing strong quantum and recoil effects that include a nonvanishing coupling of surface-scattered electrons to plane waves of light, inelastic electron backscattering from localized optical fields, and strong electron--light coupling under grazing electron diffraction by an illuminated crystal surface. Our results open new vistas in electron--light--matter interactions with promising applications in ultrafast electron microscopy.

cond-mat.mes-hall↗

arXiv2023

Multi-plasmon effects and plasmon satellites in photoemission from nanostructures

Plasmons can be excited during photoemission and produce spectral photoelectron features that yield information on the nanoscale optical response of the probed materials. However, these so-called plasmon satellites have so far been observed only for planar surfaces, while their potential for the characterization of nanostructures remains unexplored. Here, we theoretically demonstrate that core-level photoemission from nanostructures can display spectrally narrow plasmonic features, reaching relatively high probabilities similar to the direct peak. Using a nonperturbative quantum-mechanical framework, we find a dramatic effect of nanostructure morphology and dimensionality as well as universal scaling laws for the plasmon-satellite probabilities. In addition, we introduce a pump--probe scheme in which plasmons are optically excited prior to photoemission, leading to plasmon losses and gains in the photoemission spectra and granting us access to the ultrafast dynamics of the sampled nanostructure. These results emphasize the potential of plasmon satellites to explore multi-plasmon effects and ultrafast electron--plasmon dynamics in metal-based nanoparticles and two-dimensional nanoislands.

cond-mat.mes-hall↗

arXiv2023

Interrogating Quantum Nonlocal Effects in Nanoplasmonics through Electron-Beam Spectroscopy

A rigorous account of quantum nonlocal effects is paramount for understanding the optical response of metal nanostructures and for designing plasmonic devices at the nanoscale. Here, we present a scheme for retrieving the quantum surface response of metals, encapsulated in the Feibelman $d$-parameters, from electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) measurements. We theoretically demonstrate that quantum nonlocal effects have a dramatic impact on EELS and CL spectra, in the guise of spectral shifts and nonlocal damping, when either the system size or the inverse wave vector in extended structures approach the nanometer scale. Our concept capitalizes on the unparalleled ability of free-electrons to supply deeply subwavelength near-fields and, thus, probe the optical response of metals at length scales in which quantum-mechanical effects are apparent. These results pave the way for a widespread use of the $d$-parameter formalism, thereby facilitating a rigorous yet practical inclusion of nonclassical effects in nanoplasmonics.

cond-mat.mes-hall↗

arXiv2023

Gain-compensated cavities for the dynamic control of light-matter interactions

We propose an efficient approach for actively controlling the Rabi oscillations in emitter-cavity hybrids based on the presence of an element with optical gain. Inspired by recent developments in parity-time ($\mathcal{PT}$)-symmetry photonics, we show that nano- or micro-cavities where intrinsic losses are partially or fully compensated by an externally controllable amount of gain offer unique capabilities for manipulating the dynamics of emitters. In particular, one can drastically modify the dynamics of the system, increase the overall occupation numbers, enhance the longevity of the Rabi oscillations, and even decelerate them to the point where their experimental observation becomes less challenging. Furthermore, we show that there is a specific gain value that leads to an exceptional point, where both emitter and cavity occupation oscillate practically in phase, with occupation numbers that can significantly exceed unity. By revisiting a recently-introduced Rabi-visibility measure, we provide robust guidelines for quantifying the coupling strength and achieving strong-coupling with adaptable Rabi frequency via loss compensation.

physics.optics↗

arXiv2022

Quantum-phase two-dimensional materials

The modification of electronic band structures and the subsequent tuning of electrical, optical, and thermal material properties is a central theme in the engineering and fundamental understanding of solid-state systems. In this scenario, atomically thin materials offer an appealing platform because they are extremely susceptible to electric and magnetic gating, as well as to interlayer hybridization in stacked configurations, providing the means to customize and actively modulate their response functions. Here, we introduce a radically different approach to material engineering relying on the self-interaction that electrons in a two-dimensional material experience when an electrically neutral structure is placed in its vicinity. Employing rigorous theoretical methods, we show that electrons in a semiconductor atomic monolayer acquire a quantum phase resulting from the image potential induced by the presence of a neighboring periodic array of conducting ribbons, which in turn produces strong modifications in the optical, electrical, and thermal properties of the monolayer, specifically giving rise to the emergence of interband optical absorption, plasmon hybridization, and metal-insulator transitions. Beyond its fundamental interest, material engineering based on the quantum phase induced by noncontact neighboring structures represents a disruptive approach to tailor the properties of atomic layers for application in nanodevices.

cond-mat.mtrl-sci↗

arXiv2021

Extremely confined gap plasmon modes: when nonlocality matters

Historically, the field of plasmonics has been relying on the framework of classical electrodynamics, with the local-response approximation of material response being applied even when dealing with nanoscale metallic structures. However, when approaching the atomic-scale confinement of the electromagnetic radiation, mesoscopic effects are anticipated to become observable, e.g., those associated with the nonlocal electrodynamic surface response of the electron gas. We investigate nonlocal effects in propagating gap surface plasmon modes in ultrathin metal--dielectric--metal planar waveguides, exploiting monocrystalline gold flakes separated by atomic-layer-deposited aluminum oxide. We use scanning near-field optical microscopy to directly access the near-field of such confined gap plasmon modes and measure their dispersion relation (via their complex-valued propagation constants). We compare our experimental findings with the predictions of the generalized nonlocal optical response theory to unveil signatures of nonlocal damping, which becomes appreciable for smaller dielectric gaps.

cond-mat.mes-hall↗

arXiv2021

Polaritons in two-dimensional parabolic waveguides

The suite of highly confined polaritons supported by two-dimensional (2D) materials constitutes a versatile platform for nano-optics, offering the means to channel light on deep-subwavelength scales. Graphene, in particular, has attracted considerable interest due to its ability to support long-lived plasmons that can be actively tuned via electrical gating. While the excellent optoelectronic properties of graphene are widely exploited in plasmonics, its mechanical flexibility remains relatively underexplored in the same context. Here, we present a semi-analytical formalism to describe plasmons and other polaritons supported in waveguides formed by bending a 2D material into a parabolic shape. Specifically, for graphene parabolas, our theory reveals that the already large field confinement associated with graphene plasmons can be substantially increased by bending an otherwise flat graphene sheet into a parabola shape, thereby forming a plasmonic waveguide without introducing potentially lossy edge terminations via patterning. Further, we show that the high field confinement associated with such channel polaritons in 2D parabolic waveguides can enhance the spontaneous emission rate of a quantum emitter near the parabola vertex. Our findings apply generally to 2D polaritons in atomically thin materials deposited onto grooves or wedges prepared on a substrate or freely suspended in a quasi-parabolic (catenary) shape. We envision that both the optoelectronic and mechanical flexibility of 2D materials can be harnessed in tandem to produce 2D channel polaritons with versatile properties that can be applied to a wide range of nano-optics functionalities, including subwavelength polaritonic circuitry and bright single-photon sources.

cond-mat.mes-hall↗

arXiv2021

Quantum Nanophotonics in Two-Dimensional Materials

The field of 2D materials-based nanophotonics has been growing at a rapid pace, triggered by the ability to design nanophotonic systems with in situ control, unprecedented degrees of freedom, and to build material heterostructures from bottom up with atomic precision. A wide palette of polaritonic classes have been identified, comprising ultra confined optical fields, even approaching characteristic length scales of a single atom. These advances have been a real boost for the emerging field of quantum nanophotonics, where the quantum mechanical nature of the electrons and-or polaritons and their interactions become relevant. Examples include, quantum nonlocal effects, ultrastrong light matter interactions, Cherenkov radiation, access to forbidden transitions, hydrodynamic effects, single plasmon nonlinearities, polaritonic quantization, topological effects etc. In addition to these intrinsic quantum nanophotonic phenomena, the 2D material system can also be used as a sensitive probe for the quantum properties of the material that carries the nanophotonics modes, or quantum materials in its vicinity. Here, polaritons act as a probe for otherwise invisible excitations, e.g. in superconductors, or as a new tool to monitor the existence of Berry curvature in topological materials and superlattice effects in twisted 2D materials.

physics.optics↗

arXiv2021

Quantum Surface-Response of Metals Revealed by Acoustic Graphene Plasmons

A quantitative understanding of the electromagnetic response of materials is essential for the precise engineering of maximal, versatile, and controllable light--matter interactions. Material surfaces, in particular, are prominent platforms for enhancing electromagnetic interactions and for tailoring chemical processes. However, at the deep nanoscale, the electromagnetic response of electron systems is significantly impacted by quantum surface-response at material interfaces, which is challenging to probe using standard optical techniques. Here, we show how ultra-confined acoustic graphene plasmons (AGPs) in graphene--dielectric--metal structures can be used to probe the quantum surface-response functions of nearby metals, here encoded through the so-called Feibelman $d$-parameters. Based on our theoretical formalism, we introduce a concrete proposal for experimentally inferring the low-frequency quantum response of metals from quantum shifts of the AGPs' dispersion, and demonstrate that the high field confinement of AGPs can resolve intrinsically quantum mechanical electronic length-scales with subnanometer resolution. Our findings reveal a promising scheme to probe the quantum response of metals, and further suggest the utilization of AGPs as plasmon rulers with ångström-scale accuracy.

cond-mat.mes-hall↗

arXiv2021

Surface-response functions obtained from equilibrium electron-density profiles

Surface-response functions are one of the most promising routes for bridging the gap between fully quantum-mechanical calculations and phenomenological models in quantum nanoplasmonics. Within all the currently available recipes for obtaining such response functions, \emph{ab initio} calculations remain one of the most predominant, wherein the surface-response function are retrieved via the metal's non-equilibrium response to an external perturbation. Here, we present a complementary approach where one of the most appealing surface-response functions, namely the Feibelman $d$-parameters, yield a finite contribution even in the case where they are calculated directly from the equilibrium properties described under the local-response approximation (LRA), but with a spatially varying equilibrium electron density. Using model calculations that mimic both spill-in and spill-out of the equilibrium electron density, we show that the obtained $d$-parameters are in qualitative agreement with more elaborate, but also more computationally demanding, \emph{ab initio} methods. The analytical work presented here illustrates how microscopic surface-response functions can emerge out of entirely local electrodynamic considerations.

cond-mat.mes-hall↗

arXiv2021

Harnessing Ultraconfined Graphene Plasmons to Probe the Electrodynamics of Superconductors

We show that the Higgs mode of a superconductor, which is usually challenging to observe by far-field optics, can be made clearly visible using near-field optics by harnessing ultraconfined graphene plasmons. As near-field sources we investigate two examples: graphene plasmons and quantum emitters. In both cases the coupling to the Higgs mode is clearly visible. In the case of the graphene plasmons, the coupling is signaled by a clear anticrossing stemming from the interaction of graphene plasmons with the Higgs mode of the superconductor. In the case of the quantum emitters, the Higgs mode is observable through the Purcell effect. When combining the superconductor, graphene, and the quantum emitters, a number of experimental knobs become available for unveiling and studying the electrodynamics of superconductors.

cond-mat.mes-hall↗

arXiv2020

Optical response of noble metal nanostructures: Quantum surface effects in crystallographic facets

Noble metal nanostructures are ubiquitous elements in nano-optics, supporting plasmon modes that can focus light down to length scales commensurate with nonlocal effects associated with quantum confinement and spatial dispersion in the underlying electron gas. Nonlocal effects are naturally more prominent for crystalline noble metals, which potentially offer lower intrinsic loss than their amorphous counterparts, and with particular crystal facets giving rise to distinct electronic surface states. Here, we employ a quantum-mechanical model to describe nonclassical effects impacting the optical response of crystalline noble-metal films and demonstrate that these can be well-captured using a set of surface-response functions known as Feibelman $d$-parameters. In particular, we characterize the $d$-parameters associated with the (111) and (100) crystal facets of gold, silver, and copper, emphasizing the importance of surface effects arising due to electron wave function spill-out and the surface-projected band gap emerging from atomic-layer corrugation. We then show that the extracted $d$-parameters can be straightforwardly applied to describe the optical response of various nanoscale metal morphologies of interest, including metallic ultra-thin films, graphene-metal heterostructures hosting extremely confined acoustic graphene plasmons, and crystallographic faceted metallic nanoparticles supporting localized surface plasmons. The tabulated $d$-parameters reported here can circumvent computationally expensive first-principles atomistic simulations to describe microscopic nonlocal effects in the optical response of mesoscopic crystalline metal surfaces, which are becoming widely available with increasing control over morphology down to atomic length scales for state-of-the-art experiments in nano-optics.

cond-mat.mes-hall↗