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Modifying the Spectral Weights of Vibronic Transitions via Strong Coupling to Surface Plasmons
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Development of Lipid-Coated Semiconductor Nanosensors for Recording of Membrane Potential in Neurons
In the past decade, optical imaging methods have significantly improved our understanding of the information processing principles in the brain. Although many promising tools have been designed, sensors of membrane potential are lagging behind the rest. Semiconductor nanoparticles are an attractive alternative to classical voltage indicators, such as voltage-sensitive dyes and proteins. Such nanoparticles exhibit high sensitivity to external electric fields via the quantum-confine Stark effect. Here we report the development of semiconductor voltage-sensitive nanorods (vsNRs) that self-insert into the neuronal membrane. To facilitate interaction of the nanorods with the membrane, we functionalized their surface with the lipid mixture derived from brain extract. We describe a workflow to detect and process the photoluminescent signal of vsNRs after widefield time-lapse recordings. We also present data indicating that vsNRs are feasible for sensing membrane potential in neurons at a single-particle level. This shows the potential of vsNRs for the detection of neuronal activity with unprecedentedly high spatial and temporal resolution.
Nanoscale Infrared Spectroscopy and Imaging of Catalytic Reactions in Cu 2 O Crystals
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Damage-free vibrational spectroscopy of biological materials in the electron microscope
Vibrational spectroscopy in the electron microscope would be transformative in the study of biological samples, provided that radiation damage could be prevented. However, electron beams typically create high-energy excitations that severely accelerate sample degradation. Here this major difficulty is overcome using an ‘aloof’ electron beam, positioned tens of nanometres away from the sample: high-energy excitations are suppressed, while vibrational modes of energies o1 eV can be ‘safely’ investigated. To demonstrate the potential of aloof spectroscopy, we record electron energy loss spectra from biogenic guanine crystals in their native state, resolving their characteristic C–H, N–H and C=O vibrational signatures with no observable radiation damage. Furthermore, the technique opens up the possibility of non-damaging compositional analyses of organic functional groups, including non-crystalline biological materials, at a spatial resolution of ~10nm, simultaneously combined with imaging in the electron microscope.
Magnetic hyperbolic optical metamaterials
Strongly anisotropic media where the principal components of electric permittivity or magnetic permeability tensors have opposite signs are termed as hyperbolic media. Such media support propagating electromagnetic waves with extremely large wave vectors exhibiting unique optical properties. However, in all artificial and natural optical materials studied to date, the hyperbolic dispersion originates solely from the electric response. This then restricts material functionality to one polarization of light and inhibits free-space impedance matching. Such restrictions can be overcome in media having components of opposite signs for both electric and magnetic tensors. Here we present the experimental demonstration of the magnetic hyperbolic dispersion in three-dimensional metamaterials. We also measure metamaterial isofrequency contours and reveal the topological phase transition between the elliptic and hyperbolic dispersion. In the hyperbolic regime, we demonstrate the strong enhancement of thermal emission, which becomes directional, coherent and polarized. These findings show the possibilities for realizing efficient impedance-matched hyperbolic media for unpolarized light.
Direct observation of narrow mid-infrared plasmon linewidths of single metal oxide nanocrystals
Infrared-responsive doped metal oxide nanocrystals are an emerging class of plasmonic materials whose localized surface plasmon resonances (LSPR) can be resonant with molecular vibrations. This presents a distinctive opportunity to manipulate light-matter interactions to redirect chemical or spectroscopic outcomes through the strong local electric fields they generate. Here we report a technique for measuring single nanocrystal absorption spectra of doped metal oxide nanocrystals, revealing significant spectral inhomogeneity in their mid-infrared LSPRs. Our analysis suggests dopant incorporation is heterogeneous beyond expectation based on a statistical distribution of dopants. The broad ensemble linewidths typically observed in these materials result primarily from sam ple heterogeneity and not from strong electronic damping associated with lossy plasmonic materials. In fact, single nanocrystal spectra reveal linewidths as narrow as 600 cm -1 in aluminium-doped zinc oxide, a value less than half the ensemble linewidth and markedly less than homogeneous linewidths of gold nanospheres.
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS 2 and MoSe 2 ) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS 2 .
Observation of possible topological in-gap surface states in the Kondo insulator SmB 6 by photoemission
SmB 6 , a well-known Kondo insulator, exhibits a transport anomaly at low temperature. This anomaly is usually attributed to states within the hybridization gap. Recent theoretical work and transport measurements suggest that these in-gap states could be ascribed to topological surface states, which would make SmB6 the first realization of topological Kondo insulator. Here by performing angle-resolved photoemission spectroscopy experiments, we directly observe several dispersive states within the hybridization gap of SmB 6 . These states show negligible k z dependence, which indicates their surface origin. Furthermore, we perform photoemission circular dichroism experiments, which suggest that the in-gap states possess chirality of the orbital angular momentum. These states vanish simultaneously with the hybridization gap at around 150 K. Together, these observations suggest the possible topological origin of the in-gap states.
A highly conspicuous mineralized composite photonic architecture in the translucent shell of the blue-rayed limpet
Many species rely on diverse selections of entirely organic photonic structures for the manipulation of light and the display of striking colours. Here we report the discovery of a mineralized hierarchical photonic architecture embedded within the translucent shell of the blue-rayed limpet Patella pellucida . The bright colour of the limpet’s stripes originates from light interference in a periodically layered zig-zag architecture of crystallographically co-oriented calcite lamellae. Beneath the photonic multilayer, a disordered array of light-absorbing particles provides contrast for the blue colour. This unique mineralized manifestation of a synergy of two distinct optical elements at specific locations within the continuum of the limpet’s translucent protective shell ensures the vivid shine of the blue stripes, which can be perceived under water from a wide range of viewing angles. The stripes’ reflection band coincides with the spectral range of minimal light absorption in sea water, raising intriguing questions regarding their functional significance.
Phased-array sources based on nonlinear metamaterial nanocavities
Coherent superposition of light from subwavelength sources is an attractive prospect for the manipulation of the direction, shape and polarization of optical beams. This phenomenon constitutes the basis of phased arrays, commonly used at microwave and radio frequencies. Here we propose a new concept for phased-array sources at infrared frequencies based on metamaterial nanocavities coupled to a highly nonlinear semiconductor heterostructure. Optical pumping of the nanocavity induces a localized, phase-locked, nonlinear resonant polarization that acts as a source feed for a higher-order resonance of the nanocavity. Varying the nanocavity design enables the production of beams with arbitrary shape and polarization. As an example, we demonstrate two second harmonic phased-array sources that perform two optical functions at the second harmonic wavelength (~5 μm): a beam splitter and a polarizing beam splitter. As a result, proper design of the nanocavity and nonlinear heterostructure will enable such phased arrays to span most of the infrared spectrum.
Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots
In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. We report ultra-fast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects of electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices.
Observation of a Hot-Phonon Bottleneck in Lead-Iodide Perovskites
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Polarization control in an X-ray free-electron laser
X-ray free-electron lasers are unique sources of high-brightness coherent radiation. However, existing devices supply only linearly polarized light, precluding studies of chiral dynamics. A device called the Delta undulator has been installed at the Linac Coherent Light Source (LCLS) to provide tunable polarization. With a reverse tapered planar undulator line to pre-microbunch the beam and the novel technique of beam diverting, hundreds of microjoules of circularly polarized X-ray pulses are produced at 500–1,200 eV. These X-ray pulses are tens of femtoseconds long, have a degree of circular polarization of 0.98 –0.04 +0.02 at 707 eV and may be scanned in energy. We also present a new two-colour X-ray pump–X-ray probe operating mode for the LCLS. As a result, energy differences of ΔE/E = 2.4% are supported, and the second pulse can be adjusted to any elliptical polarization. In this mode, the pointing, timing, intensity and wavelength of the two pulses can be modified.