Nowadays, the accurate and full temporal characterization of ultrabroadband few-cycle laser pulses with pulse durations below 7 fs is of great importance in fields of science that investigate ultrafast dynamic processes. There are several indirect methods that use nonlinear optical signals to retrieve the complex electric field of femtosecond lasers. However, the precise characterization of few-cycle femtosecond laser sources with an ultrabroadband spectrum presents additional difficulties, such as reabsorption of nonlinear signals, partial phase matching, and spatiotemporal mismatches. In this work, we combine the dispersion scan (d-scan) method with atomically thin WS2 flakes to overcome these difficulties and fully characterize ultrabroadband laser pulses with a pulse duration of 6.9 fs and a spectrum that ranges from 650 to 1050 nm. Two-dimensional WS2 acts as a remarkably efficient nonlinear medium that offers a broad transparency range and allows for achieving relaxed phase-matching conditions due to its atomic thickness. Using mono- and trilayers of WS2, we acquire d-scan traces by measuring the second-harmonic generation (SHG) signal, originated via laser-WS2 interaction, as a function of optical dispersion (i.e., glass thickness) and wavelength. Our retrieval algorithm extracts a pulse duration at full-width half-maximum of 6.9 fs and the same spectral phase function irrespective of the number of layers. We benchmark and validate our results obtained using WS2 by comparing them with those obtained using a 10-μm-thick BBO crystal. Our findings show that atomically thin media can be an interesting alternative to micrometer-thick bulk crystals to characterize ultrabroadband femtosecond laser pulses using SHG-d-scan with an error below 100 as (attoseconds).

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.

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.

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.

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.

We observe that the asymmetric transmission (AT) through photonic systems with a resonant chiral response is strongly related to the far-field properties of eigenmodes of the system. This understanding can be used to predict the AT for any resonant system from its complex eigenmodes. We find that the resonant chiral phenomenon of AT is related to, and is bounded by, the nonresonant scattering properties of the system. Using the principle of reciprocity, we determine a fundamental limit to the maximum AT possible for a single mode in any chiral resonator. We propose and follow a design route for a highly chiral dielectric photonic crystal structure that reaches this fundamental limit for AT.