Optical Spectra of p-Doped PEDOT Nano-Aggregates Provide Insight into the Material Disorder

Highly doped Poly(3,4-ethylenedioxythiophene) or PEDOT is a conductive polymer with a wide range of applications in energy conversion due to its ease of processing, optical properties and high conductivity. The latter is influenced by processing conditions, including formulation, annealing, and solvent treatment of the polymer, which also affects the polymer arrangement. Here we show that the analysis of the optical spectra of PEDOT domains reveals the nature and magnitude of the structural disorder in the material. In particular, the optical spectra of objects on individual domains can be used for the elucidation of the molecular disorder in oligomer arrangement which is a key factor affecting the conductivity

Toward Real-Time Monitoring and Control of Single Nanoparticle Properties with a Microbubble Resonator Spectrometer

Optical microresonators have widespread application at the frontiers of nanophotonic technology, driven by their ability to confine light to the nanoscale and enhance light-matter interactions. Microresonators form the heart of a recently developed method for single-particle photothermal absorption spectroscopy, whereby the microresonators act as microscale thermometers to detect the heat dissipated by optically pumped, nonluminescent nanoscopic targets. However, translation of this technology to chemically dynamic systems requires a platform that is mechanically stable, solution compatible, and visibly transparent. We report microbubble absorption spectrometers as a versatile platform that meets these requirements. Microbubbles integrate a two-port microfluidic device within a whispering gallery mode microresonator, allowing for the facile exchange of chemical reagents within the resonator\u27s interior while maintaining a solution-free environment on its exterior. We first leverage these qualities to investigate the photoactivated etching of single gold nanorods by ferric chloride, providing a method for rapid acquisition of spatial and morphological information about nanoparticles as they undergo chemical reactions. We then demonstrate the ability to control nanorod orientation within a microbubble through optically exerted torque, a promising route toward the construction of hybrid photonic-plasmonic systems. Critically, the reported platform advances microresonator spectrometer technology by permitting room-temperature, aqueous experimental conditions, which may be used for time-resolved single-particle experiments on non-emissive, nanoscale analytes engaged in catalytically and biologically relevant chemical dynamics

Active Control of Plasmonic–Photonic Interactions in a Microbubble Cavity

Active control of light–matter interactions using nanophotonic structures is critical for new modalities for solar energy production, cavity quantum electrodynamics (QED), and sensing, particularly at the single-particle level, where it underpins the creation of tunable nanophotonic networks. Coupled plasmonic–photonic systems show great promise toward these goals because of their subwavelength spatial confinement and ultrahigh-quality factors inherited from their respective components. Here, we present a microfluidic approach using microbubble whispering-gallery mode cavities to actively control plasmonic–photonic interactions at the single-particle level. By changing the solvent in the interior of the microbubble, control can be exerted on the interior dielectric constant and, thus, on the spatial overlap between the photonic and plasmonic modes. Qualitative agreement between experiment and simulation reveals the competing roles mode overlap and mode volume play in altering coupling strengths.journal articl

A graceful multiversal link of particle physics to cosmology

In this paper we work out a multiverse scenario whose physical characteristics enable us to advance the following the conjecture that whereas the physics of particles and fields is confined to live in the realm of the whole multiverse formed by finite-time single universes, that for our observable universe must be confined just in one of the infinite number of universes of the multiverse when such a universe is consistently referred to an infinite cosmic time. If this conjecture is adopted then some current fundamental problems that appear when one tries to make compatible particle physics and cosmology- such as that for the cosmological constant, the arrow of time and the existence of a finite proper size of the event horizon- can be solved.Comment: 10 pages, LaTe

Optical monitoring of polymerizations in droplets with high temporal dynamic range

The ability to optically monitor a chemical reaction and generate an in situ readout is an important enabling technology, with applications ranging from the monitoring of reactions in flow, to the critical assessment step for combinatorial screening, to mechanistic studies on single reactant and catalyst molecules. Ideally, such a method would be applicable to many polymers and not require only a specific monomer for readout. It should also be applicable if the reactions are carried out in microdroplet chemical reactors, which offer a route to massive scalability in combinatorial searches. We describe a convenient optical method for monitoring polymerization reactions, fluorescence polarization anisotropy monitoring, and show that it can be applied in a robotically generated microdroplet. Further, we compare our method to an established optical reaction monitoring scheme, the use of Aggregation-Induced Emission (AIE) dyes, and find the two monitoring schemes offer sensitivity to different temporal regimes of the polymerization, meaning that the combination of the two provides an increased temporal dynamic range. Anisotropy is sensitive at early times, suggesting it will be useful for detecting new polymerization “hits” in searches for new reactivity, while the AIE dye responds at longer times, suggesting it will be useful for detecting reactions capable of reaching higher molecular weights

A search for pre-substellar cores and proto-brown dwarf candidates in Taurus: multiwavelength analysis in the B213-L1495 clouds

In an attempt to study whether the formation of brown dwarfs (BDs) takes place as a scaled-down version of low-mass stars, we conducted IRAM30m/MAMBO-II observations at 1.2 mm in a sample of 12 proto-BD candidates selected from Spitzer/IRAC data in the B213-L1495 clouds in Taurus. Subsequent observations with the CSO at 350 micron, VLA at 3.6 and 6 cm, and IRAM30m/EMIR in the 12CO(1-0), 13CO(1-0), and N2H+(1-0) transitions were carried out toward the two most promising Spitzer/IRAC source(s), J042118 and J041757. J042118 is associated with a compact (<10 arcsec or <1400 AU) and faint source at 350 micron, while J041757 is associated with a partially resolved (~16 arcsec or ~2000 AU) and stronger source emitting at centimetre wavelengths with a flat spectral index. The corresponding masses of the dust condensations are ~1 and ~5 Mjup for J042118 and J041757, respectively. In addition, about 40 arcsec to the northeast of J041757 we detect a strong and extended submillimetre source, J041757-NE, which is not associated with NIR/FIR emission down to our detection limits, but is clearly detected in 13CO and N2H+ at ~7 km/s, and for which we estimated a total mass of ~100 Mjup, close to the mass required to be gravitationally bound. In summary, our observational strategy has allowed us to find in B213-L1495 two proto-BD candidates and one pre-substellar core candidate, whose properties seem to be consistent with a scaled-down version of low-mass stars.Comment: MNRAS, 424, 2778; corrected typos, mass estimate refined in Section 3.2.1 and Section 5.3; conclusions unchange

The role of experimental noise in a hybrid classical-molecular computer to solve combinatorial optimization problems

Chemical and molecular-based computers may be promising alternatives to modern silicon-based computers. In particular, hybrid systems, where tasks are split between a chemical medium and traditional silicon components, may provide access and demonstration of chemical advantages such as scalability, low power dissipation, and genuine randomness. This work describes the development of a hybrid classical-molecular computer (HCMC) featuring an electrochemical reaction on top of an array of discrete electrodes with a fluorescent readout. The chemical medium, optical readout, and electrode interface combined with a classical computer generate a feedback loop to solve several canonical optimization problems in computer science such as number partitioning and prime factorization. Importantly, the HCMC makes constructive use of experimental noise in the optical readout, a milestone for molecular systems, to solve these optimization problems, as opposed to in silico random number generation. Specifically, we show calculations stranded in local minima can consistently converge on a global minimum in the presence of experimental noise. Scalability of the hybrid computer is demonstrated by expanding the number of variables from 4 to 7, increasing the number of possible solutions by 1 order of magnitude. This work provides a stepping stone to fully molecular approaches to solving complex computational problems using chemistry

Airships: A New Horizon for Science

The "Airships: A New Horizon for Science" study at the Keck Institute for Space Studies investigated the potential of a variety of airships currently operable or under development to serve as observatories and science instrumentation platforms for a range of space, atmospheric, and Earth science. The participants represent a diverse cross-section of the aerospace sector, NASA, and academia. Over the last two decades, there has been wide interest in developing a high altitude, stratospheric lighter-than-air (LTA) airship that could maneuver and remain in a desired geographic position (i.e., "station-keeping") for weeks, months or even years. Our study found considerable scientific value in both low altitude (< 40 kft) and high altitude (> 60 kft) airships across a wide spectrum of space, atmospheric, and Earth science programs. Over the course of the study period, we identified stratospheric tethered aerostats as a viable alternative to airships where station-keeping was valued over maneuverability. By opening up the sky and Earth's stratospheric horizon in affordable ways with long-term flexibility, airships allow us to push technology and science forward in a project-rich environment that complements existing space observatories as well as aircraft and high-altitude balloon missions.Comment: This low resolution version of the report is 8.6 MB. For the high resolution version see: http://kiss.caltech.edu/study/airship