arXiv subjects

F. Javier García de Abajo

Publications and source records attributed to F. Javier García de Abajo.

At least 109 records · Page 6Linked to original sources

arXiv2019

Magnetically Activated Rotational Vacuum Friction

We predict the existence of a torque acting on an isotropic neutral nanosphere activated by a static magnetic field when the particle temperature differs from the surrounding vacuum. This phenomenon originates in time-reversal symmetry breaking of the particle interaction with the vacuum electromagnetic field. We present a rigorous quantum treatment of photons and particle excitations that leads to a nonzero torque even in a motionless particle. We also find that the dynamical evolution of the particle temperature and rotation frequency follow an exotic dynamics, including spontaneous changes in the rotation direction. Magnetically activated thermal vacuum torques open a unique avenue for the investigation of the effect of time-reversal symmetry-breaking in thermal and Casimir physics.

cond-mat.mes-hall↗

arXiv2019

Plasmonics in Atomically-Thin Crystalline Silver Films

Light-matter interaction at the atomic scale rules fundamental phenomena such as photoemission and lasing, while enabling basic everyday technologies, including photovoltaics and optical communications. In this context, plasmons --the collective electron oscillations in conducting materials-- are important because they allow manipulating optical fields at the nanoscale. The advent of graphene and other two-dimensional crystals has pushed plasmons down to genuinely atomic dimensions, displaying appealing properties such as a large electrical tunability. However, plasmons in these materials are either too broad or lying at low frequencies, well below the technologically relevant near-infrared regime. Here we demonstrate sharp near-infrared plasmons in lithographically-patterned wafer-scale atomically-thin silver crystalline films. Our measured optical spectra reveal narrow plasmons (quality factor $\sim4$), further supported by a low sheet resistance comparable to bulk metal in few-atomic-layer silver films down to seven Ag(111) monolayers. Good crystal quality and plasmon narrowness are obtained despite the addition of a thin passivating dielectric, which renders our samples resilient to ambient conditions. The observation of spectrally sharp and strongly confined plasmons in atomically thin silver holds great potential for electro-optical modulation and optical sensing applications.

cond-mat.mes-hall↗

arXiv2019

Tailored nanoscale plasmon-enhanced vibrational electron spectroscopy

Vibrational optical spectroscopies can be enhanced by surface plasmons to reach molecular-sized limits of detection and characterization. The level of enhancement strongly depends on microscopic details of the sample that are generally missed by macroscopic techniques. Here we investigate phonons in h-BN by coupling them to silver-nanowire plasmons, whose energy is tuned by modifying the nanowire length. Specifically, we use electron beam milling to accurately and iteratively change the nanowire length, followed by electron energy-loss spectroscopy to reveal the plasmon-enhanced vibrational features of h-BN. This allows us to investigate otherwise hidden bulk phonons and observe strong plasmon-phonon coupling. The new milling-and-spectroscopy technique holds great potential for resolving vibrational features in material nanostructures.

cond-mat.mes-hall↗

arXiv2019

Circular Dichroism in Rotating Particles

Light interaction with rotating nanostructures gives rise to phenemona as varied as optical torques and quantum friction. Here we reveal that circular dichroism of rotating optically-isotropic particles has an unexpectedly strong dependence on their internal geometry. In particular, nanorings and nanocrosses exhibit a splitting of $2Ω$ in the particle optical resonances, while compact particles display weak circular dichroism at low rotation frequency $Ω$, but a strong circular dichroism at high $Ω$. We base our findings on a quantum-mechanical description of the polarizability of rotating particles, which has not been rigorously addressed so far. Specifically, we use the random-phase approximation and populate the particle electronic states according to the principle that they are thermally equilibrated in the rotating frame. We further provide insight into the rotational superradience effect and the ensuing optical gain, originating in population inversion as regarded from the lab frame, in which the particle is out of equilibrium. Surprisingly, we find the optical frequency cutoff for superradiance to deviate from the rotation frequency $Ω$. Our results unveil a rich, unexplored phenomenology of light interaction with rotating objects.

cond-mat.mes-hall↗

arXiv2019

Nonlinear atom-plasmon interactions enabled by nanostructured graphene

Electrically tunable graphene plasmons are anticipated to enable strong light-matter interactions with resonant quantum emitters. However, plasmon resonances in graphene are typically limited to infrared frequencies, below those of optical excitations in robust quantum light sources and many biologically interesting molecules. Here we propose to utilize near fields generated by the plasmon-assisted nonlinear optical response of nanostructured graphene to resonantly couple with proximal quantum emitters operating in the near-infrared. We show that the nonlinear near-field produced by a graphene nanodisk can strongly excite and coherently control quantum states in two- and three-level atomic systems when the third harmonic of its plasmon resonance is tuned to a particular electronic transition. In the present scheme, emitter and plasmon resonances are nondegenerate, circumventing strong enhancement of spontaneous emission. We envision potential applications for the proposed nonlinear plasmonic coupling scheme in sensing and temporal quantum control.

cond-mat.mes-hall↗

arXiv2019

Tunable plasmons in ultrathin metal films

The physics of electrons, photons, and their plasmonic interactions changes greatly when one or more dimensions are reduced down to the nanometer scale. For example, graphene shows unique electrical, optical, and plasmonic properties, which are tunable through gating or chemical doping. Similarly, ultrathin metal films (UTMFs) down to atomic thickness can possess new quantum optical effects, peculiar dielectric properties, and predicted strong plasmons. However, truly two-dimensional plasmonics in metals has so far elusive because of the difficulty in producing large areas of sufficiently thin continuous films. Thanks to a deposition technique that allows percolation even at 1 nm thickness, we demonstrate plasmons in few-nanometer gold UTMFs, with clear evidence of new dispersion regimes and large electrical tunability. Resonance peaks at 1.5-5 micrometer wavelengths are shifted by hundreds of nanometers and amplitude-modulated by tens of per cent through gating using relatively low voltages. The results suggest ways to use metals in plasmonic applications, such as electro-optic modulation, bio-sensing, and smart windows.

cond-mat.mes-hall↗

arXiv2019

Imaging the Renner-Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS$_2$) in the B$^1$B$_2$ excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS$_2$ molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the B$^1$B$_2$ excited state in neutral CS$_2$, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS$_2$, which is known to appear as a two-center scatterer.

physics.chem-ph↗

arXiv2019

Plasmon generation through electron tunneling in twisted double-layer graphene and metal-insulator-graphene systems

The generation of highly-confined plasmons through far-field optical illumination appears to be impractical for technological applications due to their large energy-momentum mismatch with external light. Electrical generation of plasmons offers a possible solution to this problem, although its performance depends on a careful choice of material and geometrical parameters. Here we theoretically investigate graphene-based structures and show in particular the very different performance between (i) two layers of graphene separated by a dielectric and (ii) metal$|$insulator$|$graphene sandwiches as generators of propagating plasmons assisted by inelastic electron tunneling. For double-layer graphene, we study the dependence on the relative tilt angle between the two sheets and show that the plasmon generation efficiency for $4^\circ$ twist angle drops to $\sim20$\% of its maximum for perfect stacking. For metal$|$insulator$|$graphene sandwiches, the inelastic tunneling efficiency drops by several orders of magnitude relative to double-layer graphene, regardless of doping level, metal$|$graphene separation, choice of metal, and direction of tunneling (metal to or from graphene), a result that we attribute to the small fraction of the surface-projected metal Brillouin zone covered by the graphene Dirac cone. Our results reveal a reasonable tolerance to graphene lattice misalignment and a poor performance of structures involving metals, thus supporting the use of double-layer graphene as an optimum choice for electrical plasmon generation in tunneling devices.

cond-mat.mes-hall↗

arXiv2019

Fundamental Limits to the Coupling between Light and 2D Polaritons by Small Scatterers

Polaritonic modes in two-dimensional van der Waals materials display short in-plane wavelengths compared with light in free space. As interesting as this may look from both fundamental and applied viewpoints, such large confinement is accompanied by poor in/out optical coupling, which severely limits the application of polaritons in practical devices. Here, we quantify the coupling strength between light and 2D polaritons in both homogeneous and anisotropic films using accurate rigorous analytical methods. In particular, we obtain universal expressions for the cross sections associated with photon-polariton coupling by point and line defects, as well as with polariton extinction and scattering processes. Additionally, we find closed-form constraints that limit the maximum possible values of these cross sections. Specifically, the maximum photon-to-plasmon conversion efficiency in graphene is $\sim10^{-6}$ and $\sim10^{-4}$ for point and line scatterers sitting at its surface, respectively, when the plasmon and photon energies are comparable in magnitude. We further show that Mie resonators placed at an optimum distance from the film can boost light-to-polariton coupling to order unity. Our results bear fundamental interest for the development of 2D polaritonics and the design of applications based on these excitations.

cond-mat.mes-hall↗

arXiv2019

Quantum Effects in the Acoustic Plasmons of Atomically-Thin Heterostructures

Recent advances in nanofabrication technology now enable unprecedented control over 2D heterostructures, in which single- or few-atom thick materials with synergetic opto-electronic properties can be combined to develop next-generation nanophotonic devices. Precise control of light can be achieved at the interface between 2D metal and dielectric layers, where surface plasmon polaritons strongly confine electromagnetic energy. Here we reveal quantum and finite-size effects in hybrid systems consisting of graphene and few-atomic-layer noble metals, based on a quantum description that captures the electronic band structure of these materials. These phenomena are found to play an important role in the metal screening of the plasmonic fields, determining the extent to which they propagate in the graphene layer. In particular, we find that a monoatomic metal layer is capable of pushing graphene plasmons toward the intraband transition region, rendering them acoustic, while the addition of more metal layers only produces minor changes in the dispersion but strongly affects the lifetime. We further find that a quantum approach is required to correctly account for the sizable Landau damping associated with single-particle excitations in the metal. We anticipate that these results will aid in the design of future platforms for extreme light-matter interaction on the nanoscale.

cond-mat.mtrl-sci↗

arXiv2018

Tracking ultrafast hot-electron diffusion in space and time by ultrafast thermo-modulation microscopy

The ultrafast response of metals to light is governed by intriguing non-equilibrium dynamics involving the interplay of excited electrons and phonons. The coupling between them gives rise to nonlinear diffusion behavior on ultrashort timescales. Here, we use scanning ultrafast thermo-modulation microscopy to image the spatio-temporal hot-electron diffusion in a thin gold film. By tracking local transient reflectivity with 20 nm and 0.25 ps resolution, we reveal two distinct diffusion regimes, consisting of an initial rapid diffusion during the first few picoseconds after optical excitation, followed by about 100-fold slower diffusion at longer times. We simulate the thermo-optical response of the gold film with a comprehensive three-dimensional model, and identify the two regimes as hot-electron and phonon-limited thermal diffusion, respectively.

physics.optics↗

arXiv2018

Efficient orbital angular momentum transfer between plasmons and free electrons

Free electrons can efficiently absorb or emit plasmons excited in a thin conductor, giving rise to multiple energy peaks in the transmitted electron spectra separated by multiples of the plasmon energy. When the plasmons are chiral, this can also give rise to transfer of orbital angular momentum (OAM). Here, we show that large amounts of OAM can be efficiently transferred between chiral plasmons supported by a thin film and free electrons traversing it. Under realistic conditions, our predictive simulations reveal efficient absorption of $\ell\gg1$ chiral plasmons of vorticity $m\gg1$, resulting in an OAM transfer $\ell m\hbar\gg\hbar$. Our work supports the use of chiral plasmons sustained by externally illuminated thin films as a way of generating high-vorticity electrons, resulting in a remarkably large fraction of kinetic energy associated with motion along the azimuthal direction, perpendicular to the incident beam.

cond-mat.mes-hall↗

arXiv2018

Photothermal Engineering of Graphene Plasmons

Nanoscale photothermal sources find important applications in theranostics, imaging, and catalysis. In this context, graphene offers a unique suite of optical, electrical, and thermal properties, which we exploit to show self-consistent active photothermal modulation of its nanoscale response. In particular, we predict the existence of plasmons confined to the optical landscape tailored by continuous-wave external-light pumping of homogeneous graphene. This result relies on the high electron temperatures achievable in optically pumped clean graphene while its lattice remains near ambient temperature. Our study opens a new avenue toward the active optical control of the nanophotonic response in graphene with potential application in photothermal devices.

cond-mat.mtrl-sci↗

arXiv2018

Efficient Electrical Detection of Mid-Infrared Graphene Plasmons at Room Temperature

Optical excitation and subsequent decay of graphene plasmons can produce a significant increase in charge-carrier temperature. An efficient method to convert this temperature elevation into a measurable electrical signal at room temperature can enable important mid-infrared applications such as thermal sensing and imaging in ubiquitous mobile devices. However, as appealing as this goal might be, it is still unrealized due to the modest thermoelectric coefficient and weak temperature-dependence of carrier transport in graphene. Here, we demonstrate mid-infrared graphene detectors consisting of arrays of plasmonic resonators interconnected by quasi one-dimensional nanoribbons. Localized barriers associated with disorder in the nanoribbons produce a dramatic temperature dependence of carrier transport, thus enabling the electrical detection of plasmon decay in the nearby graphene resonators. We further realize a device with a subwavelength footprint of 5*5 um2 operating at 12.2 um, an external responsivity of 16 mA/W, a low noise-equivalent power of 1.3 nW/Hz1/2 at room temperature, and an operational frequency potentially beyond gigahertz. Importantly, our device is fabricated using large-scale graphene and possesses a simple two-terminal geometry, representing an essential step toward the realization of on-chip graphene mid-infrared detector arrays.

cond-mat.mes-hall↗

arXiv2018

Electrical Detection of Single Graphene Plasmons

Plasmons --the collective oscillations of electrons in conducting materials-- play a pivotal role in nanophotonics because of their ability to couple electronic and photonic degrees of freedom. In particular, plasmons in graphene --the atomically thin carbon material-- offer strong spatial confinement and long lifetimes, accompanied by extraordinary optoelectronic properties derived from its peculiar electronic band structure. Understandably, this material has generated great expectations for its application to enhanced integrated devices. However, an efficient scheme for detecting graphene plasmons remains a challenge. Here we show that extremely compact graphene nanostructures are capable of realizing on-chip electrical detection of single plasmons. Specifically, we predict a twofold increase in the electrical current across a graphene nanostructure junction caused by the excitation of a single plasmon. This effect, which is due to the increase in electron temperature following plasmon decay, should persist during a picosecond time interval characteristic of electron-gas relaxation. We further show that a broad spectral detection range is accessible either by electrically doping the junction or by varying the size of the nanostructure. The proposed graphene plasmometer could find application as a basic component of future optics-free integrated nanoplasmonic devices.

cond-mat.mtrl-sci↗

arXiv2018

Molecular Sensing with Tunable Graphene Plasmons

We study the potential of graphene plasmons for spectrometer-free sensing based on surface-enhanced infrared absorption and Raman scattering. The large electrical tunability of these excitations enables an accurate identification of infrared molecular resonances by recording broadband absorption or inelastic scattering, replacing wavelength-resolved light collection by a signal integrated over photon energy as a function of the graphene doping level. The high quality factor of graphene plasmons plays a central role in the proposed detection techniques, which we show to be capable of providing label-free identification of the molecular vibration fingerprints. We find an enhancement of the absorption and inelastic scattering cross-sections by 3-4 orders of magnitude for molecules in close proximity to doped graphene nanodisks under currently feasible conditions. Our results pave the way for the development of novel cost-effective sensors capable of identifying spectral signatures of molecules without using spectrometers and laser sources.

cond-mat.mes-hall↗

arXiv2018

Analytical Modeling of Graphene Plasmons

The two-dimensionality of graphene and other layered materials can be exploited to simplify the theoretical description of their plasmonic and polaritonic modes. We present an analytical theory that allows us to simulate these excitations in terms of plasmon wave functions (PWFs). Closed-form expressions are offered for their associated extinction spectra, involving only two real parameters for each plasmon mode and graphene morphology, which we calculate and tabulate once and for all. Classical and quantum-mechanical formulations of this PWF formalism are introduced, in excellent mutual agreement for armchaired islands with $>10\,$nm characteristic size. Examples of application are presented to predict both plasmon-induced transparency in interacting nanoribbons and excellent sensing capabilities through the response to the dielectric environment. We argue that the PWF formalism has general applicability and allows us to analytically describe a wide range of 2D polaritonic behavior, thus facilitating their use for the design of actual devices.

cond-mat.mes-hall↗

arXiv2017

How To Identify Plasmons from the Optical Response of Nanostructures

A promising trend in plasmonics involves shrinking the size of plasmon-supporting structures down to a few nanometers, thus enabling control over light-matter interaction at extreme-subwavelength scales. In this limit, quantum mechanical effects, such as nonlocal screening and size quantization, strongly affect the plasmonic response, rendering it substantially different from classical predictions. For very small clusters and molecules, collective plasmonic modes are hard to distinguish from other excitations such as single-electron transitions. Using rigorous quantum mechanical computational techniques for a wide variety of physical systems, we describe how an optical resonance of a nanostructure can be classified as either plasmonic or nonplasmonic. More precisely, we define a universal metric for such classification, the generalized plasmonicity index (GPI), which can be straightforwardly implemented in any computational electronic-structure method or classical electromagnetic approach to discriminate plasmons from single-particle excitations and photonic modes. Using the GPI, we investigate the plasmonicity of optical resonances in a wide range of systems including: the emergence of plasmonic behavior in small jellium spheres as the size and the number of electrons increase; atomic-scale metallic clusters as a function of the number of atoms; and nanostructured graphene as a function of size and doping down to the molecular plasmons in polycyclic aromatic hydrocarbons. Our study provides a rigorous foundation for the further development of ultrasmall nanostructures based on molecular plasmonics

cond-mat.mes-hall↗