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Register a new userUltrafast fluorescent decay induced by metal-mediated dipole-dipole interaction in two-dimensional molecular aggregates
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Two-dimensional molecular aggregate (2DMA), a thin sheet of strongly interacting dipole molecules self-assembled at close distance on an ordered lattice, is a fascinating fluorescent material. It is distinctively different from the single or colloidal dye molecules or quantum dots in most previous research. In this paper, we verify for the first time that when a 2DMA is placed at a nanometric distance from a metallic substrate, the strong and coherent interaction between the dipoles inside the 2DMA dominates its fluorescent decay at picosecond timescale. Our streak-camera lifetime measurement and interacting lattice-dipole calculation reveal that the metal-mediated dipole-dipole interaction shortens the fluorescent lifetime to about one half and increases the energy dissipation rate by ten times than expected from the noninteracting single-dipole picture. Our finding can enrich our understanding of nanoscale energy transfer in molecular excitonic systems and may designate a new direction for developing fast and efficient optoelectronic devices.
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Circular dichroism (CD) caused by the response of a chiral object to circularly polarized light has been well established, and the strong CD of plasmonic meta-molecules has also become of interest in recent years; however, their response if the light also has orbital angular momentum is unclear. In this paper, the dichroism of a plasmonic cuboid-protuberance chiral structure under the illumination of a light beam with both orbital and spin angular momentums is numerically investigated. Distinguished spectra are observed under the different momentums. The circular dichroism under the combination of vortex beam and light spin is enhanced. This phenomenon is attributed to the partial spatial excitation of the nanoparticle, and the strong dichroism is simultaneously caused because of the interaction of the induced electric and magnetic modes and other higher-order modes caused by the partial excitation of the vortex beam. This research provides further insight into chiral light-matter interactions and the dichroism of light with orbital angular momentum.
Two dimensional (2D) transition metal dichalcogenide (TMDC) materials, such as MoS2, WS2, MoSe2, and WSe2, have received extensive attention in the past decade due to their extraordinary physical properties. The unique properties make them become ideal materials for various electronic, photonic and optoelectronic devices. However, their performance is limited by the relatively weak light-matter interactions due to their atomically thin form factor. Resonant nanophotonic structures provide a viable way to address this issue and enhance light-matter interactions in 2D TMDCs. Here, we provide an overview of this research area, showcasing relevant applications, including exotic light emission, absorption and scattering features. We start by overviewing the concept of excitons in 1L-TMDC and the fundamental theory of cavity-enhanced emission, followed by a discussion on the recent progress of enhanced light emission, strong coupling and valleytronics. The atomically thin nature of 1L-TMDC enables a broad range of ways to tune its electric and optical properties. Thus, we continue by reviewing advances in TMDC-based tunable photonic devices. Next, we survey the recent progress in enhanced light absorption over narrow and broad bandwidths using 1L or few-layer TMDCs, and their applications for photovoltaics and photodetectors. We also review recent efforts of engineering light scattering, e.g., inducing Fano resonances, wavefront engineering in 1L or few-layer TMDCs by either integrating resonant structures, such as plasmonic/Mie resonant metasurfaces, or directly patterning monolayer/few layers TMDCs. We then overview the intriguing physical properties of different types of van der Waals heterostructures, and their applications in optoelectronic and photonic devices. Finally, we draw our opinion on potential opportunities and challenges in this rapidly developing field of research.
The interaction between quantum two-level systems is typically short-range in free space and most photonic environments. Here we show that diminishing momentum isosurfaces with equal frequencies can create a significantly extended range of interaction between distant quantum systems. The extended range is robust and does not rely on a specific location or orientation of the transition dipoles. A general relation between the interaction range and properties of the isosurface is described for structured photonic media. It provides a new way to mediate long-range quantum behavior.
The coupling of laser light to matter can exert sub-cycle coherent control over material properties, with optically induced currents and magnetism shown to be controllable on ultrafast femtosecond time scales. Here, by employing laser light consisting of both linear and circular pulses, we show that charge of specified spin and crystal momentum can be created with precision throughout the first Brillouin zone. Our hybrid pulses induce in a controlled way both adiabatic intraband motion as well as vertical interband excitation between valence and conduction bands, and require only a gapped spin split valley structure for their implementation. This scenario is commonly found in the 2d semi-conductors, and we demonstrate our approach with monolayer WSe$_2$. We thus establish a route from laser light to local control over excitations in reciprocal space, opening the way to the preparation of momenta specified excited states at ultrafast time scales.
Polaritonic devices exploit the coherent coupling between excitonic and photonic degrees of freedom to perform highly nonlinear operations with low input powers. Most of the current results exploit excitons in epitaxially grown quantum wells and require low temperature operation, while viable alternatives have yet to be found at room temperature. Here we show that large single-crystal flakes of two-dimensional layered perovskite are able to sustain strong polariton nonlinearities at room temperature with no need to be embedded in an optical cavity. In particular, exciton-exciton interaction energies are measured to be remarkably similar to the ones known for inorganic quantum wells at cryogenic temperatures, and more than one order of magnitude larger than alternative room temperature polariton devices reported so far. Thanks to their easy fabrication, large dipolar oscillator strengths and strong nonlinearities, these materials hold great promises to realize actual polariton devices at room temperature.
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