Impact of Transforming Interface Geometry on Edge States in Valley Photonic Crystals.

We investigate how altering the interface geometry from a zigzag to a glide plane interface between two topologically distinct valley Hall emulating photonic crystals (VPC), profoundly affects edge states. We experimentally observe a transition from gapless to gapped edge states, accompanied by the occurrence of slow light within the Brillouin zone, rather than at its edge. We numerically simulate the propagation and measure the transmittance of the modified edge states through a specially designed valley-conserving defect. The robustness to backscattering gradually decreases, suggesting a disruption of valley-dependent transport. We demonstrate the significance of interface geometry to gapless edge states in a VPC.

Ultrafast Time Dynamics of Plasmonic Fractional Orbital Angular Momentum.

The creation and manipulation of optical vortices, both in free space and in two-dimensional systems such as surface plasmon polaritons (SPPs), has attracted widespread attention in nano-optics due to their robust topological structure. Coupled with strong spatial confinement in the case of SPPs, these plasmonic vortices and their underlying orbital angular momentum (OAM) have promise in novel light-matter interactions on the nanoscale with applications ranging from on-chip particle manipulation to tailored control of plasmonic quasiparticles. Until now, predominantly integer OAM values have been investigated. Here, we measure and analyze the time evolution of fractional OAM SPPs using time-resolved two-photon photoemission electron microscopy and near-field optical microscopy. We experimentally show the field's complex rotational dynamics and observe the beating of integer OAM eigenmodes at fractional OAM excitations. With our ability to access the ultrafast time dynamics of the electric field, we can follow the buildup of the plasmonic fractional OAM during the interference of the converging surface plasmons. By adiabatically increasing the phase discontinuity at the excitation boundary, we track the total OAM, leading to plateaus around integer OAM values that arise from the interplay between intrinsic and extrinsic OAM.

Breakdown of Spin-to-Helicity Locking at the Nanoscale in Topological Photonic Crystal Edge States.

We measure the local near-field spin in topological edge state waveguides that emulate the quantum spin Hall effect. We reveal a highly structured spin density distribution that is not linked to a unique pseudospin value. From experimental near-field real-space maps and numerical calculations, we confirm that this local structure is essential in understanding the properties of optical edge states and light-matter interactions. The global spin is reduced by a factor of 30 in the near field and, for certain frequencies, flipped compared to the pseudospin measured in the far field. We experimentally reveal the influence of higher-order Bloch harmonics in spin inhomogeneity, leading to a breakdown in the coupling between local helicity and global spin.

Simultaneous Characterization of Two Ultrashort Optical Pulses at Different Frequencies Using a WS2 Monolayer.

The precise characterization of ultrashort laser pulses has been of interest to the scientific community for many years. Frequency-resolved optical gating (FROG) has been extensively used to retrieve the temporal and spectral field distributions of ultrashort laser pulses. In this work, we exploit the high, broad-band nonlinear optical response of a WS2 monolayer to simultaneously characterize two ultrashort laser pulses with different frequencies. The relaxed phase-matching conditions in a WS2 monolayer enable the simultaneous acquisition of the spectra resulting from both four-wave mixing (FWM) and sum-frequency generation (SFG) nonlinear processes while varying the time delay between the two ultrashort pulses. Next, we introduce an adjusted double-blind FROG algorithm, based on iterative fast Fourier transforms between two FROG traces, to extract the intensity distribution and phase of two ultrashort pulses from the combination of their FWM and SFG FROG traces. Using this algorithm, we find an agreement between the computed and observed FROG traces for both the FWM and SFG processes. Exploiting the broad-band nonlinear response of a WS2 monolayer, we additionally characterize one of the pulses using a second-harmonic generation (SHG) FROG trace to validate the pulse shapes extracted from the combination of the FWM and SFG FROG traces. The retrieved pulse shape from the SHG FROG agrees well with the pulse shape retrieved from our nondegenerate cross-correlation FROG measurement. In addition to the nonlinear parametric processes, we also observe a nonlinearly generated photoluminescence (PL) signal emitted from the WS2 monolayer. Because of its nonlinear origin, the PL signal can also be used to obtain complementary autocorrelation and cross-correlation traces.

Morphology-induced spectral modification of self-assembled WS2 pyramids.

Due to their intriguing optical properties, including stable and chiral excitons, two-dimensional transition metal dichalcogenides (2D-TMDs) hold the promise of applications in nanophotonics. Chemical vapor deposition (CVD) techniques offer a platform to fabricate and design nanostructures with diverse geometries. However, the more exotic the grown nanogeometry, the less is known about its optical response. WS2 nanostructures with geometries ranging from monolayers to hollow pyramids have been created. The hollow pyramids exhibit a strongly reduced photoluminescence with respect to horizontally layered tungsten disulphide, facilitating the study of their clear Raman signal in more detail. Excited resonantly, the hollow pyramids exhibit a great number of higher-order phononic resonances. In contrast to monolayers, the spectral features of the optical response of the pyramids are position dependent. Differences in peak intensity, peak ratio and spectral peak positions reveal local variations in the atomic arrangement of the hollow pyramid crater and sides. The position-dependent optical response of hollow WS2 pyramids is characterized and attributed to growth-induced nanogeometry. Thereby the first steps are taken towards producing tunable nanophotonic devices with applications ranging from opto-electronics to non-linear optics.

Radiationless anapole states in on-chip photonics.

High-index nanoparticles are known to support radiationless states called anapoles, where dipolar and toroidal moments interfere to inhibit scattering to the far field. In order to exploit the striking properties arising from these interference conditions in photonic integrated circuits, the particles must be driven in-plane via integrated waveguides. Here, we address the excitation of electric anapole states in silicon disks when excited on-chip at telecom wavelengths. In contrast to normal illumination, we find that the anapole condition-identified by a strong reduction of the scattering-does not overlap with the near-field energy maximum, an observation attributed to retardation effects. We experimentally verify the two distinct spectral regions in individual disks illuminated in-plane from closely placed waveguide terminations via far-field and near-field measurements. Our finding has important consequences concerning the use of anapole states and interference effects of other Mie-type resonances in high-index nanoparticles for building complex photonic integrated circuitry.

Effective pair-interaction of phase singularities in random waves.

In two-dimensional random waves, phase singularities are point-like dislocations with a behavior reminiscent of interacting particles. This-qualitative-consideration stems from the spatial arrangement of these entities, which finds its hallmark in a pair correlation reminiscent of a liquid-like system. Starting from their pair correlation function, we derive an effective pair-interaction for phase singularities in random waves by using a reverse Monte Carlo method. This study initiates a new, to the best of our knowledge, approach for the treatment of singularities in random waves and can be generalized to topological defects in any system.

Nonlinear Optical Response of a WS2 Monolayer at Room Temperature upon Multicolor Laser Excitation.

Currently, the nonlinear optical properties of 2D materials are attracting the attention of an ever-increasing number of research groups due to their large potential for applications in a broad range of scientific disciplines. Here, we investigate the interplay between nonlinear photoluminescence (PL) and several degenerate and nondegenerate nonlinear optical processes of a WS2 monolayer at room temperature. We illuminate the sample using two femtosecond laser pulses at frequencies ω1 and ω2 with photon energies below the optical bandgap. As a result, the sample emits light that shows characteristic spectral peaks of the second-harmonic generation, sum-frequency generation, and four-wave mixing. In addition, we find that both resonant and off-resonant nonlinear excitation via frequency mixing contributes to the (nonlinear) PL emission at the A-exciton frequency. The PL exhibits a clear correlation with the observed nonlinear effects, which we attribute to the generation of excitons via degenerate and nondegenerate multiphoton absorption. Our work illustrates a further step toward understanding the fundamental relation between parametric and nonparametric nondegenerate optical mechanisms in transition-metal dichalcogenides. In turn, such understanding has great potential to expand the range of applicability of nonlinear optical processes of 2D materials in different fields of science and technology, where nonlinear mechanisms are typically limited to degenerate processes.

Direct quantification of topological protection in symmetry-protected photonic edge states at telecom wavelengths.

Topological on-chip photonics based on tailored photonic crystals (PhCs) that emulate quantum valley-Hall effects has recently gained widespread interest owing to its promise of robust unidirectional transport of classical and quantum information. We present a direct quantitative evaluation of topological photonic edge eigenstates and their transport properties in the telecom wavelength range using phase-resolved near-field optical microscopy. Experimentally visualizing the detailed sub-wavelength structure of these modes propagating along the interface between two topologically non-trivial mirror-symmetric lattices allows us to map their dispersion relation and differentiate between the contributions of several higher-order Bloch harmonics. Selective probing of forward- and backward-propagating modes as defined by their phase velocities enables direct quantification of topological robustness. Studying near-field propagation in controlled defects allows us to extract upper limits of topological protection in on-chip photonic systems in comparison with conventional PhC waveguides. We find that protected edge states are two orders of magnitude more robust than modes of conventional PhC waveguides. This direct experimental quantification of topological robustness comprises a crucial step toward the application of topologically protected guiding in integrated photonics, allowing for unprecedented error-free photonic quantum networks.

Vertically-oriented MoS2 nanosheets for nonlinear optical devices.

Transition metal dichalcogenides such as MoS2 represent promising candidates for building blocks of ultra-thin nanophotonic devices. For such applications, vertically-oriented MoS2 (v-MoS2) nanosheets could be advantageous as compared to conventional horizontal MoS2 (h-MoS2) given that their inherent broken symmetry would favor an enhanced nonlinear response. However, the current lack of a controllable and reproducible fabrication strategy for v-MoS2 limits the exploration of this potential. Here we present a systematic study of the growth of v-MoS2 nanosheets based on the sulfurization of a pre-deposited Mo-metal seed layer. We demonstrate that the sulfurization process at high temperatures is driven by the diffusion of sulfur from the vapor-solid interface to the Mo seed layer. Furthermore, we verify an enhanced nonlinear response in the resulting v-MoS2 nanostructures as compared to their horizontal counterparts. Our results represent a stepping stone towards the fabrication of low-dimensional TMD-based nanostructures for versatile nonlinear nanophotonic devices.

Nanoscale Optical Addressing of Valley Pseudospins through Transverse Optical Spin.

Valley pseudospin has emerged as a good quantum number to encode information, analogous to spin in spintronics. Two-dimensional transition metal dichalcogenides (2D TMDCs) recently attracted enormous attention for their easy access to the valley pseudospin through valley-dependent optical transitions. Different ways have been reported to read out the valley pseudospin state. For practical applications, on-chip access to and manipulation of valley pseudospins is paramount, not only to read out but especially to initiate the valley pseudospin state. Here, we experimentally demonstrate the selective on-chip, optical near-field initiation of valley pseudospins at room temperature. We exploit a nanowire optical waveguide, such that the local transverse optical spin of its guided modes selectively excites a specific valley pseudospin. Furthermore, spin-momentum locking of the transverse optical spin enables us to flip valley pseudospins with the opposite propagation direction. Thus, we open up ways to realize integrated hybrid opto-valleytronic devices.

Poynting singularities in the transverse flow-field of random vector waves.

In order to utilize the full potential of tailored flows of electromagnetic energy at the nanoscale, we need to understand its general behavior given by its generic representation of interfering random waves. For applications in on-chip photonics as well as particle trapping, it is important to discern between the topological features in the flow-field of the commonly investigated cases of fully vectorial light fields and their 2D equivalents. We demonstrate the distinct difference between these cases in both the allowed topology of the flow-field and the spatial distribution of its singularities, given by their pair correlation function g(r). Specifically, we show that a random field confined to a 2D plane has a divergence-free flow-field and exhibits a liquid-like correlation, whereas its freely propagating counterpart has no clear correlation and features a transverse flow-field with the full range of possible 2D topologies around its singularities.

Direct observation of topological edge states in silicon photonic crystals: Spin, dispersion, and chiral routing.

Topological protection in photonics offers new prospects for guiding and manipulating classical and quantum information. The mechanism of spin-orbit coupling promises the emergence of edge states that are helical, exhibiting unidirectional propagation that is topologically protected against back scattering. We directly observe the topological states of a photonic analog of electronic materials exhibiting the quantum spin Hall effect, living at the interface between two silicon photonic crystals with different topological order. Through the far-field radiation that is inherent to the states' existence, we characterize their properties, including linear dispersion and low loss. We find that the edge state pseudospin is encoded in unique circular far-field polarization and linked to unidirectional propagation, thus revealing a signature of the underlying photonic spin-orbit coupling. We use this connection to selectively excite different edge states with polarized light and directly visualize their routing along sharp chiral waveguide junctions.

Circular Dichroism Measurement of Single Metal Nanoparticles Using Photothermal Imaging.

Circular dichroism (CD) spectroscopy is a powerful optical technique for the study of chiral materials and molecules. It gives access to an enantioselective signal based on the differential absorption of right and left circularly polarized light, usually obtained through polarization analysis of the light transmitted through a sample of interest. CD is routinely used to determine the secondary structure of proteins and their conformational state. However, CD signals are weak, limiting the use of this powerful technique to ensembles of many molecules. Here, we experimentally realize the concept of photothermal circular dichroism, a technique that combines the enantioselective signal from circular dichroism with the high sensitivity of photothermal microscopy, achieving a superior signal-to-noise ratio to detect chiral nano-objects. As a proof of principle, we studied the chiral response of single plasmonic nanostructures with CD in the visible range, demonstrating a signal-to-noise ratio better than 40 with only 30 ms integration time for these nanostructures. The high signal-to-noise ratio allows us to quantify the CD signal for individual nanoparticles. We show that we can distinguish relative absorption differences for right circularly and left circularly polarized light as small as gmin = 4 × 10-3 for a 30 ms integration time with our current experimental settings. The enhanced sensitivity of our technique extends CD studies to individual nano-objects and opens CD spectroscopy to numbers of molecules much lower than those in conventional experiments.

A full vectorial mapping of nanophotonic light fields.

Light is a union of electric and magnetic fields, and nowhere is the complex relationship between these fields more evident than in the near fields of nanophotonic structures. There, complicated electric and magnetic fields varying over subwavelength scales are generally present, which results in photonic phenomena such as extraordinary optical momentum, superchiral fields, and a complex spatial evolution of optical singularities. An understanding of such phenomena requires nanoscale measurements of the complete optical field vector. Although the sensitivity of near-field scanning optical microscopy to the complete electromagnetic field was recently demonstrated, a separation of different components required a priori knowledge of the sample. Here, we introduce a robust algorithm that can disentangle all six electric and magnetic field components from a single near-field measurement without any numerical modeling of the structure. As examples, we unravel the fields of two prototypical nanophotonic structures: a photonic crystal waveguide and a plasmonic nanowire. These results pave the way for new studies of complex photonic phenomena at the nanoscale and for the design of structures that optimize their optical behavior.

Label-Free Optical Detection of DNA Translocations through Plasmonic Nanopores.

Solid-state nanopores are single-molecule sensors that hold great potential for rapid protein and nucleic-acid analysis. Despite their many opportunities, the conventional ionic current detection scheme that is at the heart of the sensor suffers inherent limitations. This scheme intrinsically couples signal strength to the driving voltage, requires the use of high-concentration electrolytes, suffers from capacitive noise, and impairs high-density sensor integration. Here, we propose a fundamentally different detection scheme based on the enhanced light transmission through a plasmonic nanopore. We demonstrate that translocations of single DNA molecules can be optically detected, without the need of any labeling, in the transmitted light intensity through an inverted-bowtie plasmonic nanopore. Characterization and the cross-correlation of the optical signals with their electrical counterparts verify the plasmonic basis of the optical signal. We demonstrate DNA translocation event detection in a regime of driving voltages and buffer conditions where traditional ionic current sensing fails. This label-free optical detection scheme offers opportunities to probe native DNA-protein interactions at physiological conditions.

Screening and fluctuation of the topological charge in random wave fields.

Vortices, phase singularities, and topological defects of any kind often reflect information that is crucial for understanding physical systems in which such entities arise. With near-field experiments supported by numerical calculations, we determine the fluctuations of the topological charge for phase singularities in isotropic random waves as a function of the size R of the observation window. We demonstrate that for two-dimensional fields such fluctuations increase with a superlinear scaling law, consistent with a R log R behavior. Additionally, we show that such scaling remains valid in the presence of anisotropy.

Electromagnetic Helicity in Complex Media.

Optical helicity density is usually discussed for monochromatic electromagnetic fields in free space. It plays an important role in the interaction with chiral molecules or nanoparticles. Here we introduce the optical helicity density in a dispersive isotropic medium. Our definition is consistent with biorthogonal Maxwell electromagnetism in optical media and the Brillouin energy density as well as with the recently introduced canonical momentum and spin of light in dispersive media. We consider a number of examples, including electromagnetic waves in dielectrics, negative-index materials, and metals, as well as interactions of light in a medium with chiral and magnetoelectric molecules.

Nanoscale chiral valley-photon interface through optical spin-orbit coupling.

The emergence of two-dimensional transition metal dichalcogenide materials has sparked intense activity in valleytronics, as their valley information can be encoded and detected with the spin angular momentum of light. We demonstrate the valley-dependent directional coupling of light using a plasmonic nanowire-tungsten disulfide (WS2) layers system. We show that the valley pseudospin in WS2 couples to transverse optical spin of the same handedness with a directional coupling efficiency of 90 ± 1%. Our results provide a platform for controlling, detecting, and processing valley and spin information with precise optical control at the nanoscale.