Effects of Floquet Engineering on the Coherent Exciton Dynamics in Monolayer WS2.

Coherent optical manipulation of electronic bandstructures via Floquet Engineering is a promising means to control quantum systems on an ultrafast time scale. However, the ultrafast switching on/off of the driving field comes with questions regarding the limits of the Floquet formalism (which is defined for an infinite periodic drive) through the switching process and to what extent the transient changes can be driven adiabatically. Experimentally addressing these questions has been difficult, in large part due to the absence of an established technique to measure coherent dynamics through the duration of the pulse. Here, using multidimensional coherent spectroscopy we explicitly excite, control, and probe a coherent superposition of excitons in the K and K' valleys in monolayer WS2. With a circularly polarized, red-detuned pump pulse, the degeneracy of the K and K' excitons can be lifted, and the phase of the coherence rotated. We directly measure phase rotations greater than π during the 100 fs driving pulse and show that this can be described by a combination of the AC-Stark shift of excitons in one valley and the Bloch-Siegert shift of excitons in the opposite valley. Despite showing a smooth evolution of the phase that directly follows the intensity envelope of the nonresonant pump pulse, the process is not perfectly adiabatic. By measuring the magnitude of the macroscopic coherence as it evolves before, during, and after the nonresonant pump pulse we show that there is additional decoherence caused by power broadening in the presence of the nonresonant pump. This nonadiabaticity arises as a result of interactions with the otherwise adiabatic Floquet states and may be a problem for many applications, such as manipulating qubits in quantum information processing; however, these measurements also suggest ways such effects can be minimized or eliminated.

Interactions between Fermi polarons in monolayer WS2.

Interactions between quasiparticles are of fundamental importance and ultimately determine the macroscopic properties of quantum matter. A famous example is the phenomenon of superconductivity, which arises from attractive electron-electron interactions that are mediated by phonons or even other more exotic fluctuations in the material. Here we introduce mobile exciton impurities into a two-dimensional electron gas and investigate the interactions between the resulting Fermi polaron quasiparticles. We employ multi-dimensional coherent spectroscopy on monolayer WS2, which provides an ideal platform for determining the nature of polaron-polaron interactions due to the underlying trion fine structure and the valley specific optical selection rules. At low electron doping densities, we find that the dominant interactions are between polaron states that are dressed by the same Fermi sea. In the absence of bound polaron pairs (bipolarons), we show using a minimal microscopic model that these interactions originate from a phase-space filling effect, where excitons compete for the same electrons. We furthermore reveal the existence of a bipolaron bound state with remarkably large binding energy, involving excitons in different valleys cooperatively bound to the same electron. Our work lays the foundation for probing and understanding strong electron correlation effects in two-dimensional layered structures such as moiré superlattices.

Photothermal release and recovery of mesenchymal stem cells from substrates functionalized with gold nanorods.

Mesenchymal stem cell therapies show great promise in regenerative medicine. However, to generate clinically relevant numbers of these stem cells, significant in vitro expansion of the cells is required before transplantation into the affected wound or defect. The current gold standard protocol for recovering in vitro cultured cells involves treatment with enzymes such as trypsin which can affect the cell phenotype and ability to interact with the environment. Alternative enzyme free methods of adherent cell recovery have been investigated, but none match the convenience and performance of enzymatic detachment. In this work we have developed a synthetically simple, low cost cell culture substrate functionalized with gold nanorods that can support cell proliferation and detachment. When these nanorods are irradiated with biocompatible low intensity near infrared radiation (785 nm, 560 mWcm-2) they generate localized surface plasmon resonance induced nanoscale heating effects which trigger detachment of adherent mesenchymal stem cells. Through simulations and thermometry experiments we show that this localized heating is concentrated at the cell-nanorod interface, and that the stem cells detached using this technique show either similar or improved multipotency, viability and ability to differentiate into clinically desirable osteo and adipocytes, compared to enzymatically harvested cells. This proof-of-principle work shows that photothermally mediated cell detachment is a promising method for recovering mesenchymal stem cells from in vitro culture substrates, and paves the way for further studies to scale up this process and facilitate its clinical translation. STATEMENT OF SIGNIFICANCE: New non-enzymatic methods of harvesting adherent cells without damaging or killing them are highly desirable in fields such as regenerative medicine. Here, we present a synthetically simple, non-toxic, infra-red induced method of harvesting mesenchymal stem cells from gold nanorod functionalized substrates. The detached cells retain their ability to differentiate into therapeutically valuable osteo and adipocytes. This work represents a significant improvement on similar cell harvesting studies due to: its simplicity; the use of clinically valuable stem cells as oppose to immortalized cell lines; and the extensive cellular characterization performed. Understanding, not just if cells live or die but how they proliferate and differentiate after photothermal detachment will be essential for the translation of this and similar techniques into commercial devices.

Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.

Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in materials. Here, by confining coherent excitons at the 2D quantum limit, we first observed molecular aggregation-enabled 'supertransport' of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured high effective exciton diffusion coefficient of ~346.9 cm2/s at room temperature. This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (~1.2 nm thick) with high crystallinity (J-type aggregation) and minimal interfacial states, showed superradiant emission from Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalised over ~135 molecules, which is significantly larger than the values (a few molecules) observed for other organic thin films. In addition, the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other optoelectronic devices.

Active sorting of orbital angular momentum states of light with a cascaded tunable resonator.

The orbital angular momentum (OAM) of light has been shown to be useful in diverse fields ranging from astronomy and optical trapping to optical communications and data storage. However, one of the primary impediments preventing such applications from widespread adoption is the lack of a straightforward and dynamic method to sort incident OAM states without altering the states. Here, we report a technique that can dynamically filter individual OAM states and preserve the incident OAM states for subsequent processing. Although the working principle of this technique is based on resonance, the device operation is not limited to a particular wavelength. OAM states with different wavelengths can resonate in the resonator without any additional modulation other than changing the length of the cavity. Consequently, we are able to demonstrate a reconfigurable OAM sorter that is constructed by cascading such optical resonators. This approach does not require specially designed components and is readily amenable to integration into potential applications.

Toward broadband, dynamic structuring of a complex plasmonic field.

The ability to tailor a coherent surface plasmon polariton (SPP) field is an important step toward many new opportunities for a broad range of nanophotonic applications. Previously, both scanning a converging SPP spot and designing SPP profiles using an ensemble of spots have been demonstrated. SPPs, however, are normally excited by intense, coherent light sources, that is, lasers. Hence, interference between adjacent spots is inevitable and will affect the overall SPP field distributions. We report a reconfigurable and wavelength-independent platform for generating a tailored two-dimensional (2D) SPP field distribution by considering the coherent field as a whole rather than as individual spots. With this new approach, the inherent constraints in a 2D coherent field distribution are revealed. Our design approach works not only for SPP waves but also for other 2D wave systems such as surface acoustic waves.

Luminescence of a Transition Metal Complex Inside a Metamaterial Nanocavity.

Modification of the local density of optical states using metallic nanostructures leads to enhancement in the number of emitted quanta and photocatalytic turnover of luminescent materials. In this work, the fabrication of a metamaterial is presented that consists of a nanowire separated from a metallic mirror by a polymer thin film doped with a luminescent organometallic iridium(III) complex. The large spin-orbit coupling of the heavy metal atom results in an excited state with significant magnetic-dipole character. The nanostructured architecture supports two distinct optical modes and their assignment achieved with the assistance of numerical simulations. The simulations show that one mode is characterized by strong confinement of the electric field and the other by strong confinement of the magnetic field. These modes elicit drastic changes in the emitter's photophysical properties, including dominant nanocavity-derived modes observable in the emission spectra along with significant increases in emission intensity and the total decay rate. A combination of simulations and momentum-resolved spectroscopy helps explain the mechanism of the different interactions of each optical mode supported by the metamaterial with the excited state of the emitter.

Collective excitation of plasmonic hot-spots for enhanced hot charge carrier transfer in metal/semiconductor contacts.

We show how a combination of near- and far-field coupling of the localised surface plasmon resonances in aluminium nanoparticles deposited on TiO2 films greatly enhances the visible light photocatalytic activity of the semiconductor material. We demonstrate two orders of magnitude enhancement in the rate of decomposition of methylene blue under visible light illumination when the surface of TiO2 films is decorated with gratings of Al nanoparticle dimers.

Tunable optical antennas enabled by the phase transition in vanadium dioxide.

Optical antennas, subwavelength metallic structures resonating at visible frequencies, are a relatively new branch of antenna technology being applied in science, technology and medicine. Dynamically tuning the resonances of these antennas would increase their range of application and offer potential increases in plasmonic device efficiencies. Silver nanoantenna arrays were fabricated on a thin film of the phase change material vanadium dioxide (VO(2)) and the resonant wavelength of these arrays was modulated by increasing the temperature of the substrate above the critical temperature (approximately 68 °C). Depending on the array, wavelength modulation of up to 110 nm was observed.