Abstract:Nanoplatelets are strongly anisotropic colloidal nanocrystals confined in only one direction. Perfect thickness control and large lateral dimensions enable a large exciton coherence area that exhibits a high oscillator strength. Here we investigate experimentally the existence of a strong plasmon−exciton coupling regime in a system consisting of a layer of nanoplatelets on top of a gold planar surface. We performed reflectivity measurements to extract geometrical and optical parameters of the system, and we us… Show more
“…2e,h) describes well the experimental data 𝑠3(q,w) (Fig. 2d,g), particularly peak positions, linewidths and the saddle point at the CBP resonance, demonstrating that spatially Fourier transformed spectral polariton interferometry can be interpreted analogously to momentum-and frequencyresolved surface plasmon resonance spectroscopy employing, for example, the classical Kretschmann-Raether configuration 27,[29][30][31][32] .…”
Phonon polaritons (PPs) in van der Waals (vdW) materials can strongly enhance light-matter interactions at mid-infrared frequencies, owing to their extreme infrared field confinement and long lifetimes. PPs thus bear potential for achieving vibrational strong coupling (VSC) with molecules. Although the onset of VSC has recently been observed spectroscopically with PP nanoresonators, no experiments so far have resolved VSC in real space and with propagating modes in unstructured layers. Here, we demonstrate by real-space nanoimaging that VSC can be achieved between propagating PPs in thin vdW crystals (specifically h-BN) and molecular vibrations in adjacent thin molecular layers. To that end, we performed near-field polariton interferometry, showing that VSC leads to the formation of a propagating hybrid mode with a pronounced anti-crossing region in its dispersion, in which propagation with negative group velocity is found. Numerical calculations predict VSC for nanometer-thin molecular layers and PPs in few-layer vdW materials, which could make propagating PPs a promising platform for ultra-sensitive on-chip spectroscopy and strong coupling experiments.
Main textPhonon polaritons (PPs) -light coupled to lattice vibrations -in van der Waals (vdW) crystals open up new possibilities for infrared nanophotonics, owing to their strong infrared field confinement, picosecond-long lifetimes 1-7 and tunability via thickness and dielectric environment [8][9][10][11] . Since PPs in many vdW materials spectrally coincide with molecular vibrational resonances, which abound the mid-infrared spectral range, PP are thus promising candidates for achieving vibrational strong coupling (VSC) for developing ultrasensitive infrared spectroscopy
“…2e,h) describes well the experimental data 𝑠3(q,w) (Fig. 2d,g), particularly peak positions, linewidths and the saddle point at the CBP resonance, demonstrating that spatially Fourier transformed spectral polariton interferometry can be interpreted analogously to momentum-and frequencyresolved surface plasmon resonance spectroscopy employing, for example, the classical Kretschmann-Raether configuration 27,[29][30][31][32] .…”
Phonon polaritons (PPs) in van der Waals (vdW) materials can strongly enhance light-matter interactions at mid-infrared frequencies, owing to their extreme infrared field confinement and long lifetimes. PPs thus bear potential for achieving vibrational strong coupling (VSC) with molecules. Although the onset of VSC has recently been observed spectroscopically with PP nanoresonators, no experiments so far have resolved VSC in real space and with propagating modes in unstructured layers. Here, we demonstrate by real-space nanoimaging that VSC can be achieved between propagating PPs in thin vdW crystals (specifically h-BN) and molecular vibrations in adjacent thin molecular layers. To that end, we performed near-field polariton interferometry, showing that VSC leads to the formation of a propagating hybrid mode with a pronounced anti-crossing region in its dispersion, in which propagation with negative group velocity is found. Numerical calculations predict VSC for nanometer-thin molecular layers and PPs in few-layer vdW materials, which could make propagating PPs a promising platform for ultra-sensitive on-chip spectroscopy and strong coupling experiments.
Main textPhonon polaritons (PPs) -light coupled to lattice vibrations -in van der Waals (vdW) crystals open up new possibilities for infrared nanophotonics, owing to their strong infrared field confinement, picosecond-long lifetimes 1-7 and tunability via thickness and dielectric environment [8][9][10][11] . Since PPs in many vdW materials spectrally coincide with molecular vibrational resonances, which abound the mid-infrared spectral range, PP are thus promising candidates for achieving vibrational strong coupling (VSC) for developing ultrasensitive infrared spectroscopy
“…The exceptionally narrow absorption and fluorescence line widths of NPLs (compared to their spherical cousins colloidal quantum dots) and their exceptionally large oscillator strengths make these semiconducting NPLs promising candidates for achieving a strong light–matter coupling. Indeed NPLs have recently been incorporated into resonant photonic structures. ,, Challenges for integrating colloidal NPLs into optical cavities include complex sample preparation or the use of plasmonic structures with a relatively low Q -factor. , Importantly, the fundamental photophysical properties of the polariton states in the NPL–cavity hybrid system have not been carefully investigated.…”
We demonstrate the formation of CdSe nanoplatelet (NPL) exciton-polaritons in a distributed bragg reflector (DBR) cavity. The molecule-cavity hybrid system is in the strong coupling regime with an 83 meV Rabi splitting, characterized from angle-resolved reflectance and photoluminescence measurements. Mixed quantum-classical dynamics simulations are used to investigate the polariton photophysics of the hybrid system by treating the electronic and photonic degrees of freedom (DOF) quantum mechanically, and the nuclear phononic DOF classically. Our numerical simulations of the angle-resolved photoluminescence (PL) agree extremely well with the experimental data, providing a fundamental explanation of the asymmetric intensity distribution of the upper and lower polariton branches. Our results also provide mechanistic insights into the importance of phonon-assisted non-adiabatic transitions among polariton states which are reflected in the various features of the PL spectra. This work proves the feasibility of coupling nanoplatelet electronic states with the photon states of a dielectric cavity to form a hybrid system and provides a new platform for investigating cavity-mediated physical and chemical processes.
“…We note that the spectral position of reflection minima and the actual polaritonic modes of a system can be different due to the interference of spectrally closely spaced modes (particularly in weakly coupled systems [36,37]). For that reason, we determine the eigenfrequencies of the modes (ω (j) + and ω (j) − for the filled cavity, and ω (j) cav for the bare cavity), which correspond to the poles of the reflection coefficient obtained from the TM calculation [38] (dashed lines in Fig. 3a and b, for details see Supplementary Information S2.1 and S2.2).…”
Strong coupling between molecular vibrations and microcavity modes has been demonstratedto modify physical and chemical properties of the molecular material. Here, we study the much less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities, we demonstrate the evolution from weak to ultrastrong phonon-photon coupling when the hBN thickness is increased from a few nanometers to a fully filled cavity. Remarkably, strong coupling is achieved for hBN layers as thin as 10 nm. Further, the ultrastrong coupling in fully filled cavities yields a cavity polariton dispersion matching that of phonon polaritons in bulk hBN, highlighting that the maximum light-matter coupling in microcavities is limited to the coupling strength between photons and the bulk material. The tunable cavity phonon polaritons could become a versatile platform for studying how the coupling strength between photons and phonons may modify the properties of polar crystals.
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