Complex Optical Response Research Articles

Disentangling optical effects in 3D spiral-like, chiral plasmonic assemblies templated by a dark conglomerate liquid crystal.

Chiral thin films showing electronic and plasmonic circular dichroism (CD) are intensively explored for optoelectronic applications. The most studied chiral organic films are the composites exhibiting a helical geometry, which often causes entanglement of circular optical properties with unwanted linear optical effects (linearly polarized absorption or refraction). This entanglement limits tunability and often translates to a complex optical response. This paper describes chiral films based on dark conglomerate, sponge-like, liquid crystal films, which go beyond the usual helical type geometry, waiving the problem of linear contributions to chiroptical electronic and plasmonic properties. First, we show that purely organic films exhibit high electronic CD and circular birefringence, as studied in detail using Mueller matrix polarimetry. Analogous linear properties are two orders of magnitude lower, highlighting the benefits of using the bi-isotropic dark conglomerate liquid crystal for chiroptical purposes. Next, we show that the liquid crystal can act as a template to guide the assembly of chemically compatible gold nanoparticles into 3D spiral-like assemblies. The Mueller matrix polarimetry measurements confirm that these composites exhibit both electronic and plasmonic circular dichroisms, while nanoparticle presence is not compromising the beneficial optical properties of the matrix.

Analysis of mechanically tunable metasurfaces for identifying multiple strains

We present design and analysis of a mechanically tunable metasurface under multiple strains, which consists of an array of low aspect ratio bilayer Si-TiO2 nanopillars embedded in a flexible substrate. Based on the generalized Snell's law, active control of the transmitted light is analyzed under uniaxial, biaxial and shear strains. A bidirectional solution between complex external strain and optical response is developed. Far-field refracted light spot coordinates are used to determine the strain state the metasurface is under and to estimate the arrangement parameters of the meta-atoms. Finite-difference time-domain simulations and preliminary proof-of-concept experiments validate the accuracy of the bidirectional solution model. Our analysis demonstrates the promise of such tunable metasurfaces for multi-strain detection, beam steering and optical sensing.

Experimental demonstration of inverse-designed silicon integrated photonic power splitters

Abstract The on-chip optical power splitter is a common and important device in photonic integrated circuits (PICs). To achieve a low insertion loss and high uniformity while splitting the guided light, multi-mode interferometer-based structures utilizing a self-imaging principle are widely used mainly in the form of a 1 × 2 configuration. Recently, an inverse design method for nanophotonic devices has emerged to overcome the limited capability of the conventional design methods and make it possible to explore the vast number of design parameters. Because of the non-intuitive shape of inverse-designed structures, they allow us to discover interesting and complex optical responses which are almost impossible to find with conventional design methods. Here, we report two kinds of inverse-designed 1 × 4 optical power splitters composed of silicon bars of different lengths, which are fabricated with a standard CMOS-compatible process. The particle swarm optimization method was used to minimize the insertion loss and divide the power evenly into each output port with finite-difference time-domain method simulation. The first optical power splitter has a compact size of 8.14 × 12 μm2 and the second optical power splitter has an even more compact size of 6.0 × 7.2 μm2. With the inverse designed structures, we fabricated the chip with a CMOS-compatible fabrication process. Experimental verification of the structures is provided and good agreement with the numerical results is obtained. The first 1 × 4 optical power splitter has a low insertion loss of less than 0.76 dB and uniformity of less than 0.84 dB, and the second more compact optical power splitter has a low insertion loss of less than 1.08 dB and uniformity of less than 0.81 dB. As the complexity of on-chip photonic systems has steadily increased, the inverse design of photonic structures holds great potential to be an essential part of advanced design tools.

Deconvoluting the Optical Response of Biocompatible Photonic Pigments.

To unlock the widespread use of block copolymers as photonic pigments, there is an urgent need to consider their environmental impact (cf. microplastic pollution). Here we show how an inverse photonic glass architecture can enable the use of biocompatible bottlebrush block copolymers (BBCPs), which otherwise lack the refractive index contrast needed for a strong photonic response. A library of photonic pigments is produced from poly(norbornene‐graft‐polycaprolactone)‐block‐poly(norbornene‐graft‐polyethylene glycol), with the color tuned via either the BBCP molecular weight or the processing temperature upon microparticle fabrication. The structure–optic relationship between the 3D porous morphology of the microparticles and their complex optical response is revealed by both an analytical scattering model and 3D finite‐difference time domain (FDTD) simulations. Combined, this allows for strategies to enhance the color purity to be proposed and realized with our biocompatible BBCP system.

Deconvoluting the Optical Response of Biocompatible Photonic Pigments.

To unlock the widespread use of block copolymers as photonic pigments, there is an urgent need to consider their environmental impact (cf. microplastic pollution). Here we show how an inverse photonic glass architecture can enable the use of biocompatible bottlebrush block copolymers (BBCPs), which otherwise lack the refractive index contrast needed for a strong photonic response. A library of photonic pigments is produced from poly(norbornene-graft-polycaprolactone)-block-poly(norbornene-graft-polyethylene glycol), with the color tuned via either the BBCP molecular weight or the processing temperature upon microparticle fabrication. The structure-optic relationship between the 3D porous morphology of the microparticles and their complex optical response is revealed by both an analytical scattering model and 3D finite-difference time domain (FDTD) simulations. Combined, this allows for strategies to enhance the color purity to be proposed and realized with our biocompatible BBCP system.

Effective two-level approximation of a multilevel system driven by coherent and incoherent fields

The numerical simulation of multiple scattering in dense ensembles is the mostly adopted solution to predict their complex optical response. While the scalar- and vectorial-light-mediated interactions are accurately taken into account, the computational complexity still limits current simulations to the low saturation regime and ignores the internal structure of atoms. Here, we propose to go beyond these restrictions, at constant computational cost, by describing a multilevel system by an effective two-level system that best reproduces the coherent and total scattering properties in any saturation regime. The correspondence of our model is evaluated for different experimentally realistic conditions such as the modification of the driving field polarization, the presence of stray magnetic fields, or an incoherent resonant electromagnetic field background. The trust interval of the model is quantified for the ${\mathrm{D}}_{2}$ line of $^{87}\mathrm{Rb}$ atoms, but it could be generalized to any closed transition of a multilevel quantum system.

Enhanced Light Absorption in All‐Polymer Biomimetic Photonic Structures by Near‐Zero‐Index Organic Matter

AbstractNatural photosynthetic photonic nanostructures can show sophisticated light–matter interactions including enhanced light absorption by slow light even for highly pigmented systems. Beyond fundamental biology aspects, these natural nanostructures are very attractive as blueprints for advanced photonic devices. But the soft‐matter biomimetic implementations of such nanostructures is challenging due to the low refractive index contrast of most organic photonic structures. Excitonic organic materials with near‐zero index (NZI) optical properties allow overcoming these bottlenecks. Here, it is demonstrated that the combination of NZI thin films with photonic multilayers like the ones found in nature enables broadband tunable strong reflectance as well as slow light absorption enhancement and tailored photoluminescence properties in the full VIS spectrum. Moreover, it is shown that this complex optical response is tunable, paving the way toward the development of active devices based on all‐polymer and near‐zero index materials photonic structures.

Structural and oxide-based colours on laser textured copper

Laser texturing to create colours has recently attracted significant interest due to the rapid and non-contact nature of the technique. The complex optical response of femtosecond laser-textured copper surfaces, producing a palette of perceived colours with varying amounts of angle dependence, is presented. The colours depend on the line spacing used in the laser raster-scanning process. Grazing angle Fourier transform Infrared spectroscopy (FTIR) and Raman microscopy show increased oxide content with larger total accumulated fluence and increased pulse overlap. The increased oxide content coincides with a greater angle independence of the colours compared to colours obtained at larger line spacings. All samples have a similar sinusoidal periodic microstructure, with amplitudes ranging from 400 nm for the smallest line spacings (∼1 µm) to 100 nm for the largest line spacings (∼20 µm), and are decorated with nanoparticles. The angle dependence of the colours is quantified using reflectance measurements, which show a shift in reflectance peak with observation angle. The overall complex colour of the surfaces is attributed to a combination of copper oxides and structural colours driven by underlying nanoparticles, be they metal or metal-oxide, and sinusoidal gratings with a pitch of approximately 1 µm.

Gated Photoreactivity of Pyrene Copolymers in Multiresponsive Cross-Linked starPEG-Hydrogels.

The synthesis and manufacturing of multiresponsive polymer hydrogels using simple components is a notable challenge. Pyrene is an excimer-forming fluorophore mostly used as microenvironmental probe and for the localization of molecules in close proximity in artificial and biomaterials. Here we make use of the solvophobic preaggregation and photolysis properties of pyrene to construct multiresponsive hydrogels. We synthesize poly(ethylene glycol) (PEG) hydrogels from well-defined pyrene-substituted macro-cross-linkers and elucidate their intricate intra- and intermolecular excimer formation pathways. We find that controlling the water content of the hydrogels through the degree of swelling acts as a gating stimulus governing the photoinduced solvolysis of pyrenylmethyl esters from their poly(methacrylate) backbone. This allows the implementation of a simple transient photolithography process. We thus demonstrate that multiresponsive soft materials with complex optical and mechanical responses can be obtained with comparatively little synthetic effort.

Field-resolved detection of the temporal response of a single plasmonic antenna in the mid-infrared

Unveiling the spatial and temporal dynamics of a light pulse interacting with nanosized objects is of extreme importance to widen our understanding of how photons interact with matter at the nanoscale and trigger physical and photochemical phenomena. An ideal platform to study light–matter interactions with an unprecedented spatial resolution is represented by plasmonics, which enables an extreme confinement of optical energy into sub-wavelength volumes. The ability to resolve and control the dynamics of this energy confinement on the time scale of a single optical cycle is at the ultimate frontier towards a full control of nanoscale phenomena. Here, we resolve in the time domain the linear behavior of a single germanium plasmonic antenna in the mid-infrared by measuring the complex optical field response in amplitude and phase with sub-optical-cycle precision, with the promise to extend the observation of light–matter interactions in the time domain to single quantum objects. Accessing this fundamental information opens a plethora of opportunities in a variety of research areas based on plasmon-mediated photonic processes and their coherent control, such as plasmon-enhanced chemical reactions and energy harvesting.

Correlated electronic structure and optical response of rare-earth based semiconductors

The coexistence of Mott localized $f$ states with wide conduction and valence bands in $f$-electron semiconductors results, quite generically, in a complex optical response with the nature of the absorption edge difficult to resolve both experimentally and theoretically. Here, we combine a dynamical mean-field theory approach to localized $4f$ shells with an improved description of band gaps by a semilocal exchange-correlation potential to calculate the optical properties of the light rare-earth fluorosulfides $Ln\mathrm{SF}$ ($Ln=\mathrm{Pr}$, Nd, Sm, Gd) from first principles. In agreement with experiment, we find the absorption edge in SmSF to stem from $\mathrm{S}\text{\ensuremath{-}}3p$ to $\mathrm{Sm}\text{\ensuremath{-}}4f$ transitions, while the Gd compound behaves as an ordinary $p\text{\ensuremath{-}}d$ gap semiconductor. In the unexplored PrSF and NdSF systems we predict a rather unique occurrence of strongly hybridized $4f\text{\ensuremath{-}}5d$ states at the bottom of the conduction band. The nature of the absorption edge results in a characteristic anisotropy of the optical conductivity in each system, which may be used as a fingerprint of the relative energetic positions of different states.

Universal Design Rules for Flory–Huggins Polymer Photonic Vapor Sensors

AbstractMultilayered photonic sensors that rely on polymer‐solvent Flory–Huggins interactions are drawing increasing interest owing to their broad‐band selectivity, even among mixtures, without the need for chemical targeting. Moreover, these sensors provide simple colorimetric responses, and easy, quick fabrication both on laboratory and industrial scales. However, complex optical responses and slow response times are limiting their development. In this work, the behavior of different photonic sensor architectures is analyzed to speed up response time and define a strategy to simplify their spectral behavior. To this end, the effect of interfaces, materials order, and thickness on the diffusion kinetics of a single reference analyte in the multilayered sensors is studied to design the optimal structure.

Signatures of complex optical response in Casimir interactions of type I and II Weyl semimetals

The Casimir interaction, induced by electromagnetic fluctuations between objects, is strongly dependent upon the electronic and optical properties of the materials making up the objects. Here we investigate this ubiquitous interaction between semi-infinite spaces of topologically nontrivial Weyl semimetals. A comprehensive examination of all components of the bulk conductivity tensor and the surface conductivity due to the Fermi arc states in real and imaginary frequency domains is presented using the Kubo formalism for materials with different degree of tilting of their linear energy cones. The Casimir energy is calculated using a generalized Lifshitz approach, for which electromagnetic boundary conditions for anisotropic materials were derived and used. We find that the interaction between Weyl semimetals is metallic-like and its magnitude and characteristic distance dependence can be modified by the degree of tilting and chemical potential. The nontrivial topology plays a secondary role in the interaction and thermal fluctuations are expected to have similar effects as in metallic systems.

Merging Top‐Down and Bottom‐Up Approaches to Fabricate Artificial Photonic Nanomaterials with a Deterministic Electric and Magnetic Response

AbstractArtificial photonic nanomaterials made from densely packed scatterers are frequently realized either by top‐down or bottom‐up techniques. While top‐down techniques offer unprecedented control over achievable geometries for the scatterers, by trend they suffer from being limited to planar and periodic structures. In contrast, materials fabricated with bottom‐up techniques do not suffer from such disadvantages but, unfortunately, they offer only little control on achievable geometries for the scatterers. To overcome these limitations, a nanofabrication strategy is introduced that merges both approaches. A large number of scatterers are fabricated with a tailored optical response by fast character projection electron‐beam lithography and are embedded into a membrane. By peeling‐off this membrane from the substrate, scrambling, and densifying it, a bulk material comprising densely packed and randomly arranged scatterers is obtained. The fabrication of an isotropic material from these scatterers with a strong electric and magnetic response is demonstrated. The approach of this study unlocks novel opportunities to fabricate nanomaterials with a complex optical response in the bulk but also on top of arbitrarily shaped surfaces.

Mueller matrix polarimetry of bianisotropic materials [Invited

Mueller matrix polarimetry is a powerful optical technique for characterization of both anisotropic and bianisotropic materials. This review emphasizes methods for the interpretation of measured Mueller matrices, from the meanings of matrix symmetries, to ab initio calculations of Mueller matrices that begin with Maxwell’s equations operating on materials with permittivity, permeability, and magnetoelectric constitutive tensors. We present an overview of polarimetry measurements in crystals as well as metamaterials that have optically responsive features on the order of the wavelength of visible light. Examples of the full measurement of the constitutive tensors of bianisotropic media from the analysis of their Mueller matrices, collected in either transmission or reflection, are illustrated for natural crystals, polycrystals, and nanofabricated metamaterials. Experimental and theoretical research into the complex optical responses of bianisotropic materials with polarized light is best expressed in terms of the Mueller matrix, as it offers an unambiguous and mathematically robust platform for analysis of light–matter interactions.

Anomalous interaction of spatial solitons in nematic liquid crystals.

We study experimentally the interaction of mutually incoherent bright spatial solitons in dye-doped nematic liquid crystals (LCs). The dye-induced light absorption results in a complex nonlinear optical response of the LC having spatially nonlocal focusing and defocusing contributions. The competition between both nonlinearities leads to the separation-dependent soliton interaction with repulsion of distant and attraction of closely placed solitons.

Ultrafast time-resolved investigations of excitons and biexcitons at room temperature in layered WS2

Strong light-matter interactions in layered transition metal dichalcogenides (TMDs) open up vivid possibilities for novel excitonic quasiparticle-based devices. The optical properties of TMDs are dominated mostly by the tightly bound excitons and more complex quasiparticles, the biexcitons. Instead of physically exfoliated monolayers, the solvent-mediated chemical exfoliation of these 2D crystals is a cost-effective, large-scale production method suitable for substantial practical implications. Here, we explore the ultrafast excitonic phenomena in layered WS2 (mono-to-quad) dispersion using broadband (350–750 nm) femtosecond pump-probe spectroscopy at room temperature (300 K) which are inaccessible to the steady-state absorption or emission spectroscopy. The transient absorption spectra (TAS) suggest that the mono-to-quad layered dispersion of WS2 has similar spectral features as monolayer WS2 in terms of saturation absorptions (SA) and excited state absorptions (ESA). Similar to monolayer TMDs, we are able to identify excitons and biexcitons in multi-layered 2D stratum of WS2 as well as calculate the biexciton binding energies ( 69 meV and 66 meV), which are in excellent agreement with earlier theoretical predictions. Furthermore, using many-body physics, we demonstrate that the excitons in layered WS2 behave like Wannier–Mott excitons and explain their origins via first-principles calculations. Our detailed time-resolved investigation provides ultrafast radiative and non-radiative lifetimes of the excitons and biexcitons in layered WS2. Indeed, our results unravel the complex optical response of layered TMDs, which should lead to numerous technological applications for developing excitonic quasiparticle-based valleytronic devices and ultrafast biexciton lasers at room temperature.

Measurement of complex optical susceptibility for individual carbon nanotubes by elliptically polarized light excitation

The complex optical susceptibility is the most fundamental parameter characterizing light-matter interactions and determining optical applications in any material. In one-dimensional (1D) materials, all conventional techniques to measure the complex susceptibility become invalid. Here we report a methodology to measure the complex optical susceptibility of individual 1D materials by an elliptical-polarization-based optical homodyne detection. This method is based on the accurate manipulation of interference between incident left- (right-) handed elliptically polarized light and the scattering light, which results in the opposite (same) contribution of the real and imaginary susceptibility in two sets of spectra. We successfully demonstrate its application in determining complex susceptibility of individual chirality-defined carbon nanotubes in a broad optical spectral range (1.6–2.7 eV) and under different environments (suspended and in device). This full characterization of the complex optical responses should accelerate applications of various 1D nanomaterials in future photonic, optoelectronic, photovoltaic, and bio-imaging devices.

The Dual Functional Reflecting Iris of the Zebrafish.

Many marine organisms have evolved a reflective iris to prevent unfocused light from reaching the retina. The fish iris has a dual function, both to camouflage the eye and serving as a light barrier. Yet, the physical mechanism that enables this dual functionality and the benefits of using a reflective iris have remained unclear. Using synchrotron microfocused diffraction, cryo‐scanning electron microscopy imaging, and optical analyses on zebrafish at different stages of development, it is shown that the complex optical response of the iris is facilitated by the development of high‐order organization of multilayered guanine‐based crystal reflectors and pigments. It is further demonstrated how the efficient light reflector is established during development to allow the optical functionality of the eye, already at early developmental stages.

Nanoparticle heterodimers: The role of size and interparticle gap distance on the optical response

Composite plasmonic nanostructures with controlled size, shape and relative arrangement is a subject of significant current research interest. Much of this is stimulated by the prospects by generating enormous near-field enhancements of the surface and interparticle gap regions for potential applications in surface-enhanced spectroscopies. In this manuscript, using time-dependent density functional theory (TDDFT) calculations, we investigate how the optical response in size matched homodimers and size mismatched heterodimers composed of Aluminum modify while varying the size and interparticle gap distances in the sub-nanometer range. Both systems show interesting optical response evolution. In particular, the size mismatched heterodimers show even more complex optical response evolution due to a symmetry-breaking in the system.