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David J. Masiello

Publications and source records attributed to David J. Masiello.

At least 19 recordsLinked to original sources

Unified light-matter metric of molecular and nanophotonic chirality

Signatures of a material object's broken inversion symmetry within its intrinsic excitations and associated optical fields have largely evaded characterization from a perspective that evenly accounts for the inseparability between matter and field dynamics. Here, we formulate a complex-valued pseudoscalar chirality metric that is derived from the coupled electromagnetic and material governing equations, and demonstrate its resolution of the excitational chirality exhibited by the eigenmodes and eigenfields of a family of structurally chiral objects, including those with chirally connected enantiomeric states.

physics.optics↗

Conservation of Pseudoangular Momentum in the Radiative Emission and Optical Excitation of Valley-Polarized Surface Lattice Resonances

Surface lattice resonances (SLRs) are collective polaritonic excitations in nanoparticle arrays, with band-edge states enabling symmetry-based control of radiation including scattering, photoluminescence, conventional and polariton lasing, and condensation. Here, we show that the integer pseudoangular momentum (PAM) of valley-polarized SLRs in parity-broken hexagonal arrays of honeycomb and kagome arrangements is directly encoded in the phase and polarization structure of their emitted electromagnetic fields. The effects of parity-symmetry breaking on SLR PAM and the localized surface plasmon angular momentum associated with the individual nanoparticles composing the array are investigated, and an explicit link between these quantities is established. Leveraging electromagnetic reciprocity, we further propose a structured optical field possessing the same array symmetries and integer PAM as the underlying SLRs and demonstrate theoretically and numerically that it selectively couples to valley-polarized SLRs with matching quantized PAM. Our results establish PAM-resolved light-matter interactions involving lattice resonances as providing new opportunities for symmetry-selective nanophotonic control, chiral light generation, and angular-momentum-engineered metasurfaces.

physics.optics↗

Probing Plasmonic Oscillations in 2D Moiré Nanocrystal Superlattices by Low-Loss EELS

Electron energy loss spectroscopy (EELS) has been established as a powerful analytical technique for investigating the oxidation state, band structure, and dielectric properties of materials with exceptional spatial resolution. Inspired by twisted 2D materials, we utilize low-loss EELS to examine the plasmonic excitations in 2D moiré Au nanocrystal superlattices (NCSLs) formed by liquid-air interface self-assembly using a double-dipping method. This approach produces stacked hexagonal layers that can be twisted, forming moiré patterns in NCSLs whose twist angles are precisely measured via scanning transmission electron microscopy (STEM). Low-loss EELS effectively mitigates challenges arising from fabrication-induced non-uniformity and reveals a blue shift in plasmonic excitation when comparing single-layer, double-layer, and twisted configurations. This sharply contrasts with the optical spectroscopy measurements, which show an overall red shift relative to the EELS data. The high spatial resolution of STEM-EELS further demonstrates that twist-induced symmetry breaking strongly influences plasmonic behavior. Coupled dipole modeling explains the observed discrepancies: the electron beam excites out-of-plane polarization modes unavailable to optical probes, while optical measurements average over ensembles. Our findings highlight that EELS provides complementary information to optical spectroscopy for understanding how structural arrangements at the nanoscale influence collective electronic properties, advancing the design of plasmonic metamaterials.

cond-mat.mtrl-sci↗

Strongly coupled photonic molecules as doubly-coupled oscillators

In this work, we present a field-theoretic model of strongly coupled photonic molecules composed of interacting dielectric cavities in a closed, perfect-electric-conductor domain. Within this setting, we treat the resulting inter-mode couplings non-perturbatively. We demonstrate the predictive power of this framework by showing that supermode eigenfrequencies, field profiles, and mode volumes can be obtained directly from the isolated-cavity modes and dielectric environment, without electromagnetic simulations of the composite structure or numerical fitting. While our model affirms the phenomenological approach of modeling coupled cavity modes as simple coordinate-coupled oscillators in the weak coupling regime, we show that this intuition remarkably breaks down for strong coupling. Instead, we demonstrate that strongly coupled cavity modes are analogous to harmonic oscillators we term as \emph{doubly} coupled, with interactions via electric and magnetic fields appearing as independent coordinate-coordinate and momentum-momentum couplings, respectively. We show that this distinction is not merely cosmetic, but gives rise to observable properties while providing deep insights into the physical mechanism behind previously observed phenomena, such as coupling induced frequency shifts. Finally, we illustrate that the complex interplay of these dual couplings suggests the possibility to realize exotic phenomena that typically only occur in the ultrastrong coupling regime, here predicted to emerge for comparably modest mode splittings within a regime we term pseudo-ultrastrong coupling.

physics.optics↗

Substrate matters: Coupled phonon modes of a spherical particle on a substrate probed with EELS

Using vibrational electron energy loss spectroscopy (vib-EELS) combined with numerical modeling, we investigate the physical mechanisms governing the phonon coupling between a spherical particle sustaining multipolar surface phonon modes and an underlying thin film. Depending upon their dielectric composition, a variety of hybrid phonon modes arise in the EEL spectrum due to the interaction between polarization charges in the particle and film. Mirror charge effects and phonon mode hybridization are the active mechanisms acting on dielectric and metallic-type films, respectively. Processes beyond dipole-dipole interactions are required to describe the sphere-film coupling.

cond-mat.mtrl-sci↗

Conservation of optical chirality in nanoscale light-matter interactions: A study of the Born-Kuhn model system

Optical chirality density is a measure of the local handedness of electromagnetic fields. Like energy density, it may be absorbed or scattered through the interaction between light and matter. Here, we utilize the conservation of optical chirality to connect the parity and time-reversal symmetries of the intrinsic excitational eigenmodes of a material to those of their associated electromagnetic eigenfields as dictated by Maxwell's equations. To make this connection explicit, we theoretically examine the Born-Kuhn (BK) system, composed of a pair of plasmonic nanorods of variable separation, as a prototypical material model that is both geometrically chiral in its static structure and truly excitationally chiral in its eigenexcitations and eigenfields. By relaying optical chirality metrics of the BK eigenfields back to their underlying sourcing material degrees of freedom, we derive a unique mechanical chirality measure that is related to, but distinct from, other pseudoscalar metrics recently discussed in the literature. Beyond analysis in the absence of sources, we further derive optical chiral extinction, scattering, and absorption cross sections under external drive and discuss their rigorous connection to more common circular dichroism measurements as well as their limitations in comparison to eigenfield chirality metrics. Lastly, we investigate the conversion of achiral linearly polarized light into chiral elliptically polarized light through interaction with the BK system, illustrating the conservation of optical chirality in the interaction between light and matter through an analytically tractable example.

physics.optics↗

Strategy for Direct Detection of Chiral Phonons with Phase-Structured Free Electrons

Chiral phonons possessing valley pseudo angular momentum (PAM) underlie a diversity of quantum phenomena of fundamental and applied importance, but are challenging to probe directly. We show that deficiencies of typical momentum-resolved electron energy loss measurements that make it impossible to distinguish the PAM of chiral phonons can be overcome by introducing pinwheel free electron states with well-defined PAM. Transitions between such states generate 2D periodic arrays of in-plane field vortices with polarization textures tailored to selectively couple to desired chiral mode symmetries.

cond-mat.mtrl-sci↗

Inelastic scattering of transversely structured free electrons from nanophotonic targets: Theory and computation

Recent advancements in abilities to create and manipulate the electron's transverse wave function within the transmission electron microscope (TEM) and scanning TEM (STEM) have enabled vectorially-resolved electron energy loss (EEL) and gain (EEG) measurements of nanoscale and quantum material responses using pre- and post-selected free electron states. This newfound capability is prompting renewed theoretical interest in quantum mechanical treatments of inelastic electron scattering observables and the information they contain. Here, we present a quantum mechanical treatment of the inelastic scattering of free electrons between pre- and post-selected transverse states with fully-retarded electron-sample interactions for both spontaneous EEL and continuous-wave laser-stimulated EEG measurements. General expressions for the state-resolved energy loss and gain rates are recast in forms amenable to numerical calculation using the method of coupled dipoles. We numerically implement our theory within the $e$-DDA code, and use it to investigate specific examples that highlight its versatility regarding the number, size, geometry, and material composition of the target specimen, as well as its ability to describe matter-wave diffraction from finite nanoscopic targets.

cond-mat.mes-hall↗

Probing the Polarization of Low-Energy Excitations in 2D Materials from Atomic Crystals to Nanophotonic Arrays using Momentum-Resolved Electron Energy Loss Spectroscopy

Spectroscopies utilizing free electron beams as probes offer detailed information on the reciprocal-space excitations of 2D materials such as graphene and transition metal dichalcogenide monolayers. Yet, despite the attention paid to such quantum materials, less consideration has been given to the electron-beam characterization of 2D periodic nanostructures such as photonic crystals, metasurfaces, and plasmon arrays, which can exhibit the same lattice and excitation symmetries as their atomic analogs albeit at drastically different length, momentum, and energy scales. Due to their lack of covalent bonding and influence of retarded electromagnetic interactions, important physical distinctions arise that complicate interpretation of scattering signals. Here we present a fully-retarded theoretical framework for describing the inelastic scattering of wide field electron beams from 2D materials and apply it to investigate the complementarity in sample excitation information gained in the measurement of a honeycomb plasmon array versus angle-resolved optical spectroscopy in comparison to single monolayer graphene.

cond-mat.mtrl-sci↗

A composite electrodynamic mechanism to reconcile spatiotemporally resolved exciton transport in quantum dot superlattices

Quantum dot (QD) solids are promising optoelectronic materials; further advancing their device functionality depends on understanding their energy transport mechanisms. The commonly invoked near-field Förster resonance energy transfer (FRET) theory often underestimates the exciton hopping rate in QD solids, yet no consensus exists on the underlying cause. In response, we use time-resolved ultrafast stimulated emission depletion (TRUSTED) microscopy, an ultrafast transformation of stimulated emission depletion (STED) microscopy to spatiotemporally resolve exciton diffusion in tellurium-doped CdSe-core/CdS-shell QD superlattices. We measure the concomitant time-resolved exciton energy decay due to excitons sampling a heterogeneous energetic landscape within the superlattice. The heterogeneity is quantified by single-particle emission spectroscopy. This powerful multimodal set of observables provides sufficient constraints on a kinetic Monte Carlo simulation of exciton transport to elucidate a composite transport mechanism that includes both near-field FRET and previously-neglected far-field emission/reabsorption contributions. Uncovering this mechanism offers a much-needed unified framework in which to characterize transport in QD solids and additional principles for device design.

cond-mat.mes-hall↗

Optical Polarization Analogs in Inelastic Free Electron Scattering

Advances in the ability to manipulate free electron phase profiles within the electron microscope have spurred development of quantum-mechanical descriptions of electron energy loss (EEL) processes involving transitions between phase-shaped transverse states. Here, we elucidate an underlying connection between two ostensibly distinct optical polarization analogs identified in EEL experiments as manifestations of the same conserved scattering flux. Our work introduces a procedure for probing general tensorial target characteristics including global mode symmetries and local polarization.

cond-mat.mes-hall↗

Near-Field Enhancement of Optical Second Harmonic Generation in Hybrid Gold-Lithium Niobate Nanostructures

Nanophotonics research has focused recently on the ability of non-linear optical processes to mediate and transform optical signals in a myriad of novel devices, including optical modulators, transducers, color filters, photodetectors, photon sources, and ultrafast optical switches. The inherent weakness of optical nonlinearities at smaller scales has, however, hindered the realization of efficient miniaturized devices, and strategies for enhancing both device efficiencies and synthesis throughput via nanoengineering remain limited. Here, we demonstrate a novel mechanism by which second harmonic generation, a prototypical non-linear optical phenomenon, from individual lithium niobate particles can be significantly enhanced through nonradiative coupling to the localized surface plasmon resonances of embedded gold nanoparticles. A joint experimental and theoretical investigation of single mesoporous lithium niobate particles coated with aispersed layer of $\sim$10-nm diameter gold nanoparticles shows that a $\sim$32-fold enhancement of second harmonic generation can be achieved without introducing finely tailored radiative nanoantennas to mediate photon transfer to or from the non-linear material. This work highlights the limitations of current strategies for enhancing non-linear optical phenomena and proposes a route through which a new class of subwavelength nonlinear optical platforms can be designed to maximize non-linear efficiencies through near-field energy exchange.

physics.optics↗

Resolving resonance effects in the theory of single particle photothermal imaging

Photothermal spectroscopy and microscopy provides a route to measure the spectral and spatial properties of individual nanoscopic absorbers, independent from scattering, extinction, and emission. The approach relies upon use of two light sources, one that resonantly excites and heats the target and its surrounding environment and a second off-resonant probe that scatters from the resulting volume of thermally modified refractive index. Over the past twenty years, considerable effort has been extended to apply photothermal methods to detect, spatially resolve, and perform absorption spectroscopy on single non-emissive molecules and other absorbers like plasmonic nanoparticles at room temperature conditions. Companion theoretical models have been developed to interpret these experimental advances, yet it is not clear how they are related to each other nor how the effects of lock-in detection modify the theory. For larger target systems that host their own intrinsic scattering resonances as well as for background media that do not instantaneously thermalize with the absorbing target, additional dependencies arise that are yet to be explored theoretically. The aim of this Perspective is to overview the theory of photothermal spectroscopy and microscopy and present a unifying theoretical approach that recovers past models in certain limits while explicitly including the effects of target scattering resonances, thermal and optical retardation, and lock-in detection. Focus is made on plasmonic particles to interpret the photothermal signal, yet all results are applicable equally to individual molecules or nanoparticle absorbers. Consequently, we expect this review to provide a useful foundation for the understanding of photothermal measurements independent of target identity.

physics.optics↗

Wavelength-dependent photothermal imaging probes nanoscale temperature differences among sub-diffraction coupled plasmonic nanorods

While the thermal and electromagnetic properties of plasmonic nanostructures are well understood, nanoscale thermometry still presents an experimental and theoretical challenge. Plasmonic structures can confine electromagnetic energy at the nanoscale, resulting in local, inhomogeneous, controllable heating. But reading out the temperature with nanoscale precision using optical techniques poses a difficult challenge. Here we report on the optical thermometry of individual gold nanorod trimers that exhibit multiple wavelength-dependent plasmon modes resulting in measurably different local temperature distributions. Specifically, we demonstrate how photothermal microscopy encodes different wavelength-dependent temperature profiles in the asymmetry of the photothermal image point spread function. These point spread function asymmetries are interpreted through companion numerical simulations of the photothermal images to reveal how differing thermal gradients within the nanorod trimer can be controlled by exciting its hybridized plasmonic modes. We also find that hybrid plasmon modes that are optically dark can be excited by our focused laser beam illumination geometry at certain beam positions, thereby providing an additional route to modify thermal profiles at the nanoscale beyond wide-field illumination. Taken together these findings demonstrate an all-optical thermometry technique to actively create and measure thermal gradients at the nanoscale below the diffraction limit.

physics.optics↗

Exact $k$-body representation of the Jaynes-Cummings interaction in the dressed basis: Insight into many-body phenomena with light

Analog quantum simulation - the technique of using one experimentally well-controlled physical system to mimic the behavior of another - has quickly emerged as one of the most promising near term strategies for studying strongly correlated quantum many-body systems. In particular, systems of interacting photons, realizable in solid-state cavity and circuit QED frameworks, for example, hold tremendous promise for the study of nonequilibrium many-body phenomena due to the capability to locally create and destroy photons. These systems are typically modeled using a Jaynes-Cummings-Hubbard (JCH) Hamiltonian, named due to similarities with the Bose-Hubbard (BH) model. Here, we present a non-perturbative procedure for transforming the JC Hamiltonian into a dressed operator representation that, in its most general form, admits an infinite sum of bosonic $k$-body terms where $k$ is bound only by the number of excitations in the system. We closely examine this result in both the dispersive and resonant coupling regimes, finding rapid convergence in the former and contributions from $k\gg1$ in the latter. Through extension to a two-site JCH system, we demonstrate that this approach facilitates close inspection of the analogy between the JCH and BH models and its breakdown for resonant light-matter coupling. Finally, we use this framework to survey the many-body character of a two-site JCH for general system parameters, identifying four unique quantum phases and the parameter regimes in which they are realized, thus highlighting phenomena realizable with finite JCH-based quantum simulators beyond the BH model. More broadly, this work is intended to serve as a clear mathematical exposition of bosonic many-body interactions underlying JC-type systems, often postulated through analogy to Kerr-like nonlinear susceptibilities or by matching coefficients to obtain the appropriate eigenvalue spectrum.

quant-ph↗

Active tuning of hybridized modes in a heterogeneous photonic molecule

From fundamental discovery to practical application, advances in the optical and quantum sciences rely upon precise control of light-matter interactions. Systems of coupled optical cavities are ubiquitous in these efforts, yet design and active modification of the hybridized mode properties remains challenging. In this Letter, we demonstrate the ability to thermally control the degree of hybridization in a heterogeneous photonic molecule composed of a ring resonator strongly coupled to a nanobeam photonic crystal cavity. Combining theory and experiment, we show that the composition of the resulting super-modes can be actively tailored and we derive temperature-dependent analytic expressions for the super-mode profiles, frequencies, and volumes. This work illustrates the potential for actively tunable, designer photonic properties using heterogeneous optical cavity devices.

physics.optics↗

Direct Observation of Infrared Plasmonic Fano Antiresonances by a Nanoscale Electron Probe

In this Letter, we exploit recent breakthroughs in monochromated aberration-corrected scanning transmission electron microscopy (STEM) to resolve infrared plasmonic Fano antiresonances in individual nanofabricated disk-rod dimers. Using a combination of electron energy-loss spectroscopy (EELS) and theoretical modeling, we investigate and characterize a subspace of the weak coupling regime between quasi-discrete and quasi-continuum localized surface plasmon resonances where infrared plasmonic Fano antiresonances appear. This work illustrates the capability of STEM instrumentation to experimentally observe nanoscale plasmonic responses that were previously the domain only of higher resolution infrared spectroscopies.

cond-mat.mes-hall↗

On the linear response and scattering of an interacting molecule-metal system

A many-body Green's function approach to the microscopic theory of plasmon-enhanced spectroscopy is presented within the context of localized surface-plasmon resonance spectroscopy and applied to investigate the coupling between quantum-molecular and classical-plasmonic resonances in monolayer-coated silver nanoparticles. Electronic propagators or Green's functions, accounting for the repeated polarization interaction between a single molecule and its image in a nearby nanoscale metal, are explicitly computed and used to construct the linear-response properties of the combined molecule-metal system to an external electromagnetic perturbation. Shifting and finite lifetime of states appear rigorously and automatically within our approach and reveal an intricate coupling between molecule and metal not fully described by previous theories. Self-consistent incorporation of this quantum-molecular response into the continuum-electromagnetic scattering of the molecule-metal target is exploited to compute the localized surface-plasmon resonance wavelength shift with respect to the bare metal from first principles.

physics.chem-ph↗