Organic molecule exciton-polaritons in photonic lattices are a versatile platform to emulate unconventional phases of matter at ambient temperatures, including protected interface modes in topological insulators. Here, we investigate bosonic condensation in the most prototypical higher-order topological lattice: a 2D-version of the Su-Schrieffer-Heeger model. Under strong optical pumping, we observe bosonic condensation into both 0D and 1D topologically protected modes.
View Article and Find Full Text PDFEmitter dephasing is one of the key issues in the performance of solid-state single-photon sources. Among the various sources of dephasing, acoustic phonons play a central role in adding decoherence to the single-photon emission. Here, we demonstrate that it is possible to tune and engineer the coherence of photons emitted from a single WSe_{2} monolayer quantum dot via selectively coupling it to a spectral cavity resonance.
View Article and Find Full Text PDFBosonic condensation and lasing of exciton polaritons in microcavities is a fascinating solid-state phenomenon. It provides a versatile platform to study out-of-equilibrium many-body physics and has recently appeared at the forefront of quantum technologies. Here, we study the photon statistics via the second-order temporal correlation function of polariton lasing emerging from an optical microcavity with an embedded atomically thin MoSe_{2} crystal.
View Article and Find Full Text PDFStructures of membrane proteins determined by X-ray crystallography and, increasingly, by cryo-electron microscopy often fail to resolve the structural details of unstable or reactive small molecular ligands in their physiological sites. This work demonstrates that C chemical shifts measured by magic-angle spinning (MAS) solid-state NMR (SSNMR) provide unique information on the conformation of a labile ligand in the physiological site of a functional protein in its native membrane, by exploiting freeze-trapping to stabilise the complex. We examine the ribose conformation of ATP in a high affinity complex with Na,K-ATPase (NKA), an enzyme that rapidly hydrolyses ATP to ADP and inorganic phosphate under physiological conditions.
View Article and Find Full Text PDFSolid-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 WSe coupled to a tunable optical cavity in a liquid-helium-free cryostat without the further need for active stabilization.
View Article and Find Full Text PDFSpontaneous Brillouin scattering in bulk crystalline solids is governed by the intrinsic selection rules locking the relative polarization of the excitation laser and the Brillouin signal. In this work, we independently manipulate the polarization of the two by employing polarization-sensitive optical resonances in elliptical micropillars to induce a wavelength-dependent rotation of the polarization states. Consequently, a polarization-based filtering technique allows us to measure acoustic phonons with frequencies difficult to access with standard Brillouin and Raman spectroscopies.
View Article and Find Full Text PDFUltrahigh-frequency acoustic-phonon resonators usually require atomically flat interfaces to avoid phonon scattering and dephasing, leading to expensive fabrication processes, such as molecular beam epitaxy. Mesoporous thin films are based on inexpensive wet chemical fabrication techniques that lead to relatively flat interfaces regardless the presence of nanopores. Here, we report mesoporous titanium dioxide-based acoustic resonators with resonances up to 90 GHz, and quality factors from 3 to 7.
View Article and Find Full Text PDFThe excitonic fine structure plays a key role for the quantum light generated by semiconductor quantum dots, both for entangled photon pairs and single photons. Controlling the excitonic fine structure has been demonstrated using electric, magnetic, or strain fields, but not for quantum dots in optical cavities, a key requirement to obtain high source efficiency and near-unity photon indistinguishability. Here, we demonstrate the control of the fine structure splitting for quantum dots embedded in micropillar cavities.
View Article and Find Full Text PDFEngineering the properties of quantum materials via strong light-matter coupling is a compelling research direction with a multiplicity of modern applications. Those range from modifying charge transport in organic molecules, steering particle correlation and interactions, and even controlling chemical reactions. Here, we study the modification of the material properties via strong coupling and demonstrate an effective inversion of the excitonic band-ordering in a monolayer of WSe with spin-forbidden, optically dark ground state.
View Article and Find Full Text PDFThe emergence of spatial and temporal coherence of light emitted from solid-state systems is a fundamental phenomenon intrinsically aligned with the control of light-matter coupling. It is canonical for laser oscillation, emerges in the superradiance of collective emitters, and has been investigated in bosonic condensates of thermalized light, as well as exciton-polaritons. Our room temperature experiments show the strong light-matter coupling between microcavity photons and excitons in atomically thin WSe.
View Article and Find Full Text PDFSpin labels based on cinobufagin, a specific inhibitor of the Na,K-ATPase, have proved valuable tools to characterize the binding site of cardiotonic steroids (CTSs), which also constitutes the extracellular cation pathway. Because existing literature suggests variations in the physiological responses caused by binding of different CTSs, we extended the original set of spin-labeled inhibitors to the more potent bufalin derivatives. Positioning of the spin labels within the Na,K-ATPase site was defined and visualized by molecular docking.
View Article and Find Full Text PDFBrillouin spectroscopy emerges as a promising non-invasive tool for nanoscale imaging and sensing. One-dimensional semiconductor superlattice structures are eminently used for selectively enhancing the generation or detection of phonons at few GHz. While commercially available Brillouin spectrometers provide high-resolution spectra, they consist of complex experimental techniques and are not suitable for semiconductor cavities operating at a wide range of optical wavelengths.
View Article and Find Full Text PDFLight states composed of multiple entangled photons-such as cluster states-are essential for developing and scaling-up quantum computing networks. Photonic cluster states can be obtained from single-photon sources and entangling gates, but so far this has only been done with probabilistic sources constrained to intrinsically low efficiencies, and an increasing hardware overhead. Here, we report the resource-efficient generation of polarization-encoded, individually-addressable photons in linear cluster states occupying a single spatial mode.
View Article and Find Full Text PDFPhilos Trans A Math Phys Eng Sci
December 2020
Conical metallic tapers represent an intriguing subclass of metallic nanostructures, as their plasmonic properties show interesting characteristics in strong correlation to their geometrical properties. This is important for possible applications such as in the field of scanning optical microscopy, as favourable plasmonic resonance behaviour can be tailored by optimizing structural parameters like surface roughness or opening angle. Here, we review our recent studies, where single-crystalline gold tapers were investigated experimentally by means of electron energy-loss and cathodoluminescence spectroscopy techniques inside electron microscopes, supported by theoretical finite-difference time-domain calculations.
View Article and Find Full Text PDFThree-dimensional plasmonic gold tapers are widely used structures in nano-optics for achieving imaging at the nanometer scale, enhanced spectroscopy, confined light sources, and ultrafast photoelectron emission. To understand their radiation properties further, especially in the proximity of the apex at the nanoscale, we employ cathodoluminescence spectroscopy with high spatial and energy resolution. The plasmon-induced radiation in the visible spectral range from three-dimensional gold tapers with opening angles of 13° and 47° is investigated under local electron excitation.
View Article and Find Full Text PDFThe coherent exchange of optical near fields between two neighbouring dipoles plays an essential role in the optical properties, quantum dynamics and thus the function of many naturally occurring and artificial nanosystems. These interactions are challenging to quantify experimentally. They extend over only a few nanometres and depend sensitively on the detuning, dephasing and relative orientation (that is, the vectorial properties) of the coupled dipoles.
View Article and Find Full Text PDFThe information obtained from crystallized complexes of the Na ,K -ATPase with cardiotonic steroids (CTS) is not sufficient to explain differences in the inhibitory properties of CTS such as stereoselectivity of CTS binding or effect of glycosylation on the preference to enzyme isoforms. The uncertainty is related to the spatial organization of the hydrophilic cavity at the entrance of the CTS-binding site. Therefore, there is a need to supplement the crystallographic description with data obtained in aqueous solution, where molecules have significant degree of flexibility.
View Article and Find Full Text PDFRecent experiments demonstrated that GaAs/AlAs based micropillar cavities are promising systems for quantum optomechanics, allowing the simultaneous three-dimensional confinement of near-infrared photons and acoustic phonons in the 18-100 GHz range. Here, we investigate through numerical simulations the optomechanical properties of this new platform. We evidence how the Poisson's ratio and semiconductor/vacuum boundary conditions lead to very distinct features in the mechanical and optical three-dimensional confinement.
View Article and Find Full Text PDFWe investigate different dynamic mechanisms, reflection and phase matching, of surface plasmons in a three-dimensional single-crystalline gold taper excited by relativistic electrons. Plasmonic modes of gold tapers with various opening angles from 5° to 47° are studied both experimentally and theoretically, by means of electron energy-loss spectroscopy and finite-difference time-domain numerical calculations, respectively. Distinct resonances along the taper shaft are observed in tapers independent of opening angles.
View Article and Find Full Text PDFCardiotonic steroids (CTS) are clinically important drugs for the treatment of heart failure owing to their potent inhibition of cardiac Na(+), K(+)-ATPase (NKA). Bufadienolides constitute one of the two major classes of CTS, but little is known about how they interact with NKA. We report a remarkable stereoselectivity of NKA inhibition by native 3β-hydroxy bufalin over the 3α-isomer, yet replacing the 3β-hydroxy group with larger polar groups in the same configuration enhances inhibitory potency.
View Article and Find Full Text PDFThis paper addresses the question of long-range interactions between the intramembranous cation binding sites and the cytoplasmic nucleotide binding site of the ubiquitous ion-transporting Na,K-ATPase using (13)C cross-polarization magic-angle spinning (CP-MAS) solid-state nuclear magnetic resonance. High-affinity ATP binding is induced by the presence of Na(+) as well as of Na-like substances such as Tris(+), and these ions are equally efficient promoters of nucleotide binding. CP-MAS analysis of bound ATP with Na,K-ATPase purified from pig kidney membranes reveals subtle differences in the nucleotide interactions within the nucleotide site depending on whether Na(+) or Tris(+) is used to induce binding.
View Article and Find Full Text PDFWe investigate the optical modes in three-dimensional single-crystalline gold tapers by means of electron energy-loss spectroscopy. At the very proximity to the apex, a broad-band excitation at all photon energies from 0.75 to 2 eV, which is the onset for interband transitions, is detected.
View Article and Find Full Text PDFTransitions between conformational substates of membrane proteins can be driven by torsional librations in the protein that may be coupled to librational fluctuations of the lipid chains. Here, librational motion of spin-labeled lipid chains in membranous Na,K-ATPase is investigated by spin-echo electron paramagnetic resonance. Lipids at the protein interface are targeted by using negatively charged spin-labeled fatty acids that display selectivity of interaction with the Na,K-ATPase.
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