arXiv subjects

Martin Silies

Publications and source records attributed to Martin Silies.

5 recordsLinked to original sources

arXiv2025

Ultrafast transition from coherent to incoherent polariton nonlinearities in a hybrid 1L-WS2/plasmon structure

Exciton polaritons based on atomically thin semiconductors are essential building blocks of quantum optoelectronic devices. Their properties are governed by an ultrafast and oscillatory energy transfer between their excitonic and photonic constituents, resulting in the formation of polaritonic quasiparticles with pronounced nonlinearities induced by the excitonic component. In metallic nanoresonators, dissipation phenomena limit the polariton lifetime to a few ten femtoseconds, so short that the role of these polaritons for the nonlinearities of such hybrids is yet unexplored. Here, we use ultrafast two-dimensional electronic spectroscopy (2DES) to uncover coherent polariton dynamics in a hybrid monolayer (1L) WS2/plasmonic nanostructure. With respect to an uncoupled WS2 flake, we observe an over 20-fold, polarization-dependent enhancement of the optical nonlinearity and a rapid evolution of the 2DES spectra within ~70 fs. We relate these dynamics to a transition from coherent polaritons to incoherent excitations, unravel the microscopic optical nonlinearities, and show the potential of coherent polaritons for ultrafast all-optical switching.

cond-mat.mes-hall↗

arXiv2023

In-situ spontaneous emission control of MoSe$_2$-WSe$_2$ interlayer excitons with near-unity quantum yield

Optical resonators are a powerful platform to control the spontaneous emission dynamics of excitons in solid-state nanostructures. Here, we study a MoSe$_2$-WSe$_2$ van-der-Waals heterostructure that is integrated in a widely tunable open optical microcavity to gain insights into fundamental optical properties of the emergent interlayer charge-transfer excitons. First, we utilize an ultra-low quality factor open planar vertical cavity and investigate the modification of the excitonic lifetime as on- and off-resonant conditions are met with consecutive longitudinal modes. Time-resolved photoluminescence measurements reveal that the interlayer exciton lifetime can thus be periodically tuned with an amplitude of 110 ps. The resulting oscillations of the interlayer exciton lifetime allows us to extract a 0.5 ns free-space radiative lifetime and a quantum efficiency as high as 81 \%. We subsequently engineer the local density of optical states by introducing a spatially confined and fully spectrally tunable Tamm-plasmon resonance. The dramatic redistribution of the local optical modes in this setting allows us to encounter a profound inhibition of spontaneous emission of the interlayer excitons by a factor of 3.2. We expect that specifically engineering the inhibition of radiation from moiré excitons is a powerful tool to steer their thermalization, and eventually their condensation into coherent condensate phases.

cond-mat.mtrl-sci↗

arXiv2023

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.

cond-mat.mes-hall↗

arXiv2023

Ultra-bright single photon source based on an atomically thin material

Solid-state single photon sources are central building blocks in quantum communication networks and on-chip quantum information processing. Atomically thin crystals were established as possible candidates to emit non-classical states of light, however, the performance of monolayer-based single photon sources has so far been lacking behind state-of-the-art devices based on volume crystals. Here, we implement a single photon source based on an atomically thin sheet of WSe2 coupled to a spectrally tunable optical cavity. It is characterized by a high single photon purity with a $g^{(2)}(0)$ value as low as $4.7 \pm 0.7 \%$ and a record-high first lens brightness of linearly polarized photons as large as $65 \pm 4 \%$. Interestingly, the high performance of our devices allows us to observe genuine quantum interference phenomena in a Hong-Ou-Mandel experiment. Our results demonstrate that open cavities and two-dimensional materials constitute an excellent platform for ultra-bright quantum light sources: the unique properties of such two-dimensional materials and the versatility of open cavities open an inspiring avenue for novel quantum optoelectronic devices.

quant-ph↗

arXiv2019

Bridging Microscopic Nonlinear Polarizations toward Far-Field Second Harmonic Radiation

Since the first observation of second harmonic generation (SHG), there have been extensive studies on this nonlinear phenomenon not only to clarify its physical origin but also to realize unconventional functionalities. Nonetheless, a widely accepted model of SHG with rigorous experimental verification that describes the contributions of different underlying microscopic mechanisms is still under debate. Here, we examine second harmonic far-field radiation patterns over a wide angle from metallic structures with different resonances, to reveal the structure-dependent contributions from distinct nonlinear polarizations. By comparing the measured SHG radiation patterns of 82 antennas with different SHG models, we demonstrate the critical role of the surface-parallel and bulk nonlinear polarizations in the far-field SHG patterns, and thus show that the common belief of the dominant contribution of the surface-normal component in SHG should be corrected. A virtual multi-resonator SHG model inside a single physical resonator is introduced to explain and control the interplay between different nonlinear polarizations and their structure-dependent excitations. Our findings offer a new strategy for the design of highly efficient and directional nonlinear metamaterials.

physics.optics↗