Ultrafast Coherent Exciton Couplings and Many-Body Interactions in Monolayer WS2.

Transition metal dichalcogenides (TMDs) are quantum confined systems with interesting optoelectronic properties, governed by Coulomb interactions in the monolayer (1L) limit, where strongly bound excitons provide a sensitive probe for many-body interactions. Here, we use two-dimensional electronic spectroscopy (2DES) to investigate many-body interactions and their dynamics in 1L-WS2 at room temperature and with sub-10 fs time resolution. Our data reveal coherent interactions between the strongly detuned A and B exciton states in 1L-WS2. Pronounced ultrafast oscillations of the transient optical response of the B exciton are the signature of a coherent 50 meV coupling and coherent population oscillations between the two exciton states. Supported by microscopic semiconductor Bloch equation simulations, these coherent dynamics are rationalized in terms of Dexter-like interactions. Our work sheds light on the role of coherent exciton couplings and many-body interactions in the ultrafast temporal evolution of spin and valley states in TMDs.

Plasmon mediated coherent population oscillations in molecular aggregates.

The strong coherent coupling of quantum emitters to vacuum fluctuations of the light field offers opportunities for manipulating the optical and transport properties of nanomaterials, with potential applications ranging from ultrasensitive all-optical switching to creating polariton condensates. Often, ubiquitous decoherence processes at ambient conditions limit these couplings to such short time scales that the quantum dynamics of the interacting system remains elusive. Prominent examples are strongly coupled exciton-plasmon systems, which, so far, have mostly been investigated by linear optical spectroscopy. Here, we use ultrafast two-dimensional electronic spectroscopy to probe the quantum dynamics of J-aggregate excitons collectively coupled to the spatially structured plasmonic fields of a gold nanoslit array. We observe rich coherent Rabi oscillation dynamics reflecting a plasmon-driven coherent exciton population transfer over mesoscopic distances at room temperature. This opens up new opportunities to manipulate the coherent transport of matter excitations by coupling to vacuum fields.

Monolayer-Based Single-Photon Source in a Liquid-Helium-Free Open Cavity Featuring 65% Brightness and Quantum Coherence.

Solid-state single-photon sources are central building blocks in quantum information processing. Atomically thin crystals have emerged as sources of nonclassical light; however, they perform below the state-of-the-art devices based on volume crystals. Here, we implement a bright single-photon source based on an atomically thin sheet of WSe2 coupled to a tunable optical cavity in a liquid-helium-free cryostat without the further need for active stabilization. Its performance is characterized by high single-photon purity (g(2)(0) = 4.7 ± 0.7%) and record-high, first-lens brightness of linearly polarized photons of 65 ± 4%, representing a decisive step toward real-world quantum applications. The high performance of our devices allows us to observe two-photon interference in a Hong-Ou-Mandel experiment with 2% visibility limited by the emitter coherence time and setup resolution. Our results thus demonstrate that the combination of the unique properties of two-dimensional materials and versatile open cavities emerges as an inspiring avenue for novel quantum optoelectronic devices.

Ultrafast Coupling of Optical Near Fields to Low-Energy Electrons Probed in a Point-Projection Microscope.

We report the first observation of the coupling of strong optical near fields to wavepackets of free, 100 eV electrons with <50 fs temporal resolution in an ultrafast point-projection microscope. Optical near fields are created by excitation of a thin, nanometer-sized Yagi-Uda antenna, with 20 fs near-infrared laser pulses. Phase matching between electrons and near fields is achieved due to strong spatial confinement of the antenna near field. Energy-resolved projection images of the antenna are recorded in an optical pump-electron probe scheme. We show that the phase modulation of the electron by transverse-field components results in a transient electron deflection while longitudinal near-field components broaden the kinetic energy distribution. This low-energy electron near-field coupling is used here to characterize the chirp of the ultrafast electron wavepackets, acquired upon propagation from the electron emitter to the sample. Our results bring direct mapping of different vectorial components of highly localized optical near fields into reach.

Plasmon-Enhanced Exciton Delocalization in Squaraine-Type Molecular Aggregates.

Enlarging exciton coherence lengths in molecular aggregates is critical for enhancing the collective optical and transport properties of molecular thin film nanostructures or devices. We demonstrate that the exciton coherence length of squaraine aggregates can be increased from 10 to 24 molecular units at room temperature when preparing the aggregated thin film on a metallic rather than a dielectric substrate. Two-dimensional electronic spectroscopy measurements reveal a much lower degree of inhomogeneous line broadening for aggregates on a gold film, pointing to a reduced disorder. The result is corroborated by simulations based on a Frenkel exciton model including exciton-plasmon coupling effects. The simulation shows that localized, energetically nearly resonant excitons on spatially well separated segments can be radiatively coupled via delocalized surface plasmon polariton modes at a planar molecule-gold interface. Such plasmon-enhanced delocalization of the exciton wave function is of high importance for improving the coherent transport properties of molecular aggregates on the nanoscale. Additionally, it may help tailor the collective optical response of organic materials for quantum optical applications.

Steering second-harmonic radiation through local excitations of plasmon.

We propose an approach of steering the second harmonic (SH) emission from a single plasmonic structure, through local excitations of plasmon. The proposed idea is confirmed experimentally, by adjusting the incident beam position at the fundamental frequency, on a single plasmonic antenna. A significant directivity change ( ± 52°) for the SH emission is observed with submicrometer adjustment ( ± 250 nm) of the excitation beam position, over broadband SH frequencies. Providing a simple method of controlling the directivity of frequency-converted light, our approach paves the way to new design strategy for nonlinear optical devices with various nonlinear wavefronts.

Suppression of Radiative Damping and Enhancement of Second Harmonic Generation in Bull's Eye Nanoresonators.

We report a drastic increase of the damping time of plasmonic eigenmodes in resonant bull's eye (BE) nanoresonators to more than 35 fs. This is achieved by tailoring the groove depth of the resonator and by coupling the confined plasmonic field in the aperture to an extended resonator mode such that spatial coherence is preserved over distances of more than 10 µm. Experimentally, this is demonstrated by probing the plasmon dynamics at the field level using broadband spectral interferometry. The nanoresonator allows us to efficiently concentrate the incident field inside the central aperture of the BE and to tailor its local optical nonlinearity by varying the aperture geometry. By replacing the central circular hole with an annular ring structure, we obtain 50-times higher second harmonic generation efficiency, allowing us to demonstrate the efficient concentration of long-lived plasmonic modes inside nanoapertures by interferometric frequency-resolved autocorrelation. Such a light concentration in a nanoresonator with high quality factor has high potential for sensing and coherent control of light-matter interactions on the nanoscale.

Toward plasmonics with nanometer precision: nonlinear optics of helium-ion milled gold nanoantennas.

Plasmonic nanoantennas are versatile tools for coherently controlling and directing light on the nanoscale. For these antennas, current fabrication techniques such as electron beam lithography (EBL) or focused ion beam (FIB) milling with Ga(+)-ions routinely achieve feature sizes in the 10 nm range. However, they suffer increasingly from inherent limitations when a precision of single nanometers down to atomic length scales is required, where exciting quantum mechanical effects are expected to affect the nanoantenna optics. Here, we demonstrate that a combined approach of Ga(+)-FIB and milling-based He(+)-ion lithography (HIL) for the fabrication of nanoantennas offers to readily overcome some of these limitations. Gold bowtie antennas with 6 nm gap size were fabricated with single-nanometer accuracy and high reproducibility. Using third harmonic (TH) spectroscopy, we find a substantial enhancement of the nonlinear emission intensity of single HIL-antennas compared to those produced by state-of-the-art gallium-based milling. Moreover, HIL-antennas show a vastly improved polarization contrast. This superior nonlinear performance of HIL-derived plasmonic structures is an excellent testimonial to the application of He(+)-ion beam milling for ultrahigh precision nanofabrication, which in turn can be viewed as a stepping stone to mastering quantum optical investigations in the near-field.