Enhancement of surface activity in CO oxidation on Pt(110) through spatiotemporal laser actuation

We explore the effect of spatiotemporally varying substrate temperature profiles on the dynamics and resulting reaction rate enhancement for the catalytic oxidation of CO on Pt(110). The catalytic surface is "addressed" by a focused laser beam whose motion is computer-controlled. The averaged reaction rate is observed to undergo a characteristic maximum as a function of the speed of this moving laser spot. Experiments as well as modelling are used to explore and rationalize the existence of such an optimal laser speed.Comment: 9 pages, 12 figures, submitted to Phys. Rev.

Guiding chemical pulses through geometry: Y-junctions

We study computationally and experimentally the propagation of chemical pulses in complex geometries.The reaction of interest, CO oxidation, takes place on single crystal Pt(110) surfaces that are microlithographically patterned; they are also addressable through a focused laser beam, manipulated through galvanometer mirrors, capable of locally altering the crystal temperature and thus affecting pulse propagation. We focus on sudden changes in the domain shape (corners in a Y-junction geometry) that can affect the pulse dynamics; we also show how brief, localized temperature perturbations can be used to control reactive pulse propagation.The computational results are corroborated through experimental studies in which the pulses are visualized using Reflection Anisotropy Microscopy.Comment: submitted to Phys. Rev.

Economical and environmental contributions of installing a solar heating system in an industrial process: Contribuições econômicas e ambientais da instalação de um sistema de aquecimento solar em um processo industrial

Aware of the harmful consequences of climate change, several industrial sectors search for alternatives to minimize the environmental impact of their production processes. The use of thermal solar collectors is a promising alternative for the heat supply in industrial processes, contributing to the reduction of fossil fuel consumption for this purpose and, consequently, mitigating the environmental impact caused by greenhouse gas emissions. The present research analyzes the contribution of a Solar Heating for Industrial Processes (SHIP) system in an industry’s environmental and economic spheres on the outskirts of Porto Alegre, south Brazil. A solar field of Linear Fresnel concentrating collectors is simulated in SAM software. The field has an aperture area of 352 m² and operates in the supply of saturated steam for a given industrial process. The results indicate that the SHIP system would be able to supply 729 GJth to the industrial process annually. It means a reduction of greenhouse gas emissions in the magnitude of tens of tons of CO2-equivalent each year, whose value increases as the operation of the conventional steam-generating boiler moves away from ideal (theoretical efficiency of 100%). Two methodologies are used to calculate LCOH, resulting in 52 and 54 U$D/MWhth values for the analyzed SHIP system. Compared with the heat supply through burning natural gas and mineral coal, a solar thermal heating system can be evaluated as an environmentally responsible and economically advantageous alternative for the industrial sector that decides on this investment

Transition of pulsed operation from Q-switching to continuous-wave mode-locking in a Yb:KLuW waveguide laser

We report on the diverse pulsed operation regimes of a femtosecond-laser-written Yb:KLuW channel waveguide laser emitting near 1040 nm. By the precise position tuning of a carbon-nanotube-coated saturable absorber (SA) mirror, the transition of the pulsed operation from Q-switching, Q-switched mode-locking and finally sub-GHz continuous-wave mode-locking are obtained based on the interplay of dispersion and mode area control. The Q-switched pulses exhibit typical fast SA Q-switched pulse characteristics depending on absorbed pump powers. In the Q-switched mode-locking, amplitude modulations of the mode-locked pulses on the Q-switched envelope are observed. The radio-frequency spectrum represents the coexistence of Q-switching and mode-locking signals. In the purely mode-locked operation, the waveguide laser generates 2.05-ps pulses at 0.5 GHz.National Research Foundation of Korea (2018H1A2AA1061480, 2019R1A2C3003504, 2020R1A4A2002828); Spanish Government (FIS2017-87970-R, MAT2016-75716-C2-1-R (AEI/FEDER,UE)); Junta de Castilla y León (SA287P18); Generalitat de Catalunya (2017SGR755)

Femtosecond-laser-written Tm:KLu(WO_4)_2 waveguide lasers

Depressed-index channel waveguides with a circular and photonic crystal cladding structures are prepared in a bulk monoclinic Tm:KLu(WO4)2 crystal by 3D direct femtosecond laser writing. The channel waveguide structures are characterized and laser operation is achieved using external mirrors. In the continuous-wave mode, the maximum output power of 46 mW is achieved at 1912 nm corresponding to a slope efficiency of 15.2% and a laser threshold of only 21 mW. Passive -switching of a waveguide with a circular cladding is realized using single-walled carbon nanotubes. Stable 7 nJ/50 ns pulses are achieved at a repetition rate of 1.48 MHz. This first demonstration of ∼2 μm fs-laser-written waveguide lasers based on monoclinic double tungstates is promising for further lasers of this type doped with Tm3+and Ho3+ ions .Ministerio de Economía y Competitividad (MINECO) (FIS2013-44174-P, FIS2015-71933-REDT, MAT2013-47395-C4-4-R, MAT2016-75716-C2-1-R, TEC 2014-55948-R); Departament d’Innovació, Universitats i Empresa, Generalitat de Catalunya (DIUE) (2014SGR1358); Junta de Castilla y León (UIC016, SA046U16); Institució Catalana de Recerca i Estudis Avançats (ICREA) Academia (2010ICREA-02); H2020 Marie Skłodowska-Curie Actions (MSCA) (657630); Government of the Russian Federation (074-U01); National Research Foundation of Korea (NRF) Korea of MSIP (2016R1A2A1A05005381)

The redshift distribution of dusty star forming galaxies from the SPT survey

We use the Atacama Large Millimeter/submillimeter Array (ALMA) in Cycle 1 to determine spectroscopic redshifts of high-redshift dusty star-forming galaxies (DSFGs) selected by their 1.4mm continuum emission in the South Pole Telescope (SPT) survey. We present ALMA 3mm spectral scans between 84-114GHz for 15 galaxies and targeted ALMA 1mm observations for an additional eight sources. Our observations yield 30 new line detections from CO, [CI] , [NII] , H_2O and NH_3. We further present APEX [CII] and CO mid-J observations for seven sources for which only a single line was detected in spectral-scan data from ALMA Cycle 0 or Cycle 1. We combine the new observations with previously published and new mm/submm line and photometric data of the SPT-selected DSFGs to study their redshift distribution. The combined data yield 39 spectroscopic redshifts from molecular lines, a success rate of >85%. Our sample represents the largest data set of its kind today and has the highest spectroscopic completeness among all redshift surveys of high-z DSFGs. The median of the redshift distribution is z=3.9+/-0.4, and the highest-redshift source in our sample is at z=5.8. We discuss how the selection of our sources affects the redshift distribution, focusing on source brightness, selection wavelength, and strong gravitational lensing. We correct for the effect of gravitational lensing and find the redshift distribution for 1.4mm-selected sources with a median redshift of z=3.1+/-0.3. Comparing to redshift distributions selected at shorter wavelengths from the literature, we show that selection wavelength affects the shape of the redshift distribution

Suppression of spatiotemporal chaos in the oscillatory CO oxidation on Pt(110) by focused laser light

Chemical turbulence in the oscillatory catalytic CO oxidation on Pt(110) is suppressed by means of focused laser light. The laser locally heats the platinum surface which leads to a local increase of the oscillation frequency, and to the formation of a pacemaker which emits target waves. These waves slowly entrain the medium and suppress the spatiotemporal chaos present in the absence of laser light. Our experimental results are confirmed by a detailed numerical analysis of one- and two-dimensional media using the Krischer-Eiswirth-Ertl model for CO oxidation on Pt110. Different control regimes are identified and the dispersion relation of the system is determined using the pacemaker as an externally tunable wave source

The Rest-Frame Submillimeter Spectrum of High-Redshift, Dusty, Star-Forming Galaxies

We present the average rest-frame spectrum of high-redshift dusty, star-forming galaxies from 250-770GHz. This spectrum was constructed by stacking ALMA 3mm spectra of 22 such sources discovered by the South Pole Telescope and spanning z=2.0-5.7. In addition to multiple bright spectral features of 12CO, [CI], and H2O, we also detect several faint transitions of 13CO, HCN, HNC, HCO+, and CN, and use the observed line strengths to characterize the typical properties of the interstellar medium of these high-redshift starburst galaxies. We find that the 13CO brightness in these objects is comparable to that of the only other z>2 star-forming galaxy in which 13CO has been observed. We show that the emission from the high-critical density molecules HCN, HNC, HCO+, and CN is consistent with a warm, dense medium with T_kin ~ 55K and n_H2 >~ 10^5.5 cm^-3. High molecular hydrogen densities are required to reproduce the observed line ratios, and we demonstrate that alternatives to purely collisional excitation are unlikely to be significant for the bulk of these systems. We quantify the average emission from several species with no individually detected transitions, and find emission from the hydride CH and the linear molecule CCH for the first time at high redshift, indicating that these molecules may be powerful probes of interstellar chemistry in high-redshift systems. These observations represent the first constraints on many molecular species with rest-frame transitions from 0.4-1.2mm in star-forming systems at high redshift, and will be invaluable in making effective use of ALMA in full science operations.Comment: 19 pages, 10 figures (2 in appendices); accepted for publication in Ap

Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) experiment: design, execution and science overview

We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of air masses that contain the emission products from seasonal boreal wildfires and how these air masses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada, based out of Halifax, Nova Scotia. Atmospheric ground-based and sonde measurements over Canada and the Azores associated with the planned July 2010 deployment of the ARA, which was postponed by 12 months due to UK-based flights related to the dispersal of material emitted by the Eyjafjallajökull volcano, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 involved the same atmospheric measurements, but included the ARA, special satellite observations and a more comprehensive ground-based measurement suite. The high-frequency aircraft data provided a comprehensive chemical snapshot of pyrogenic plumes from wildfires, corresponding to photochemical (and physical) ages ranging from 45 sr 10 days, largely by virtue of widespread fires over Northwestern Ontario. Airborne measurements reported a large number of emitted gases including semi-volatile species, some of which have not been been previously reported in pyrogenic plumes, with the corresponding emission ratios agreeing with previous work for common gases. Analysis of the NOy data shows evidence of net ozone production in pyrogenic plumes, controlled by aerosol abundance, which increases as a function of photochemical age. The coordinated ground-based and sonde data provided detailed but spatially limited information that put the aircraft data into context of the longer burning season in the boundary layer. Ground-based measurements of particulate matter smaller than 2.5 μm (PM2.5) over Halifax show that forest fires can on an episodic basis represent a substantial contribution to total surface PM2.5

Passively Q-switched femtosecond-laser-written thulium waveguide laser based on evanescent field interaction with carbon nanotubes

Surface channel waveguides (WGs) were fabricated in a monoclinic Tm3+:KLu(WO4)2 crystal by femtosecond direct laser writing (fs-DLW). The WGs consisted of a half-ring cladding with diameters of 50 and 60 μm located just beneath the crystal surface. They were characterized by confocal laser microscopy and -Raman spectroscopy, indicating a reduced crystallinity and stress-induced birefringence of the WG cladding. In continuous-wave (CW) mode, under Ti:sapphire laser pumping at 802 nm, the maximum output power reached 171.1 mW at 1847.4 nm, corresponding to a slope efficiency of 37.8% for the 60 μm diameter WG. The WG propagation loss was 0.7±0.3 dB/cm. The top surface of the WGs was spin-coated by a polymethyl methacrylate film containing randomly oriented (spaghetti-like) arc-discharge single-walled carbon nanotubes serving as a saturable absorber based on evanescent field coupling. Stable passively -switched (PQS) operation was achieved. The PQS 60 μm diameter WG laser generated a record output power of 150 mW at 1846.8 nm with =34.6%. The conversion efficiency with respect to the CW mode was 87.6%. The best pulse characteristics (energy/duration) were 105.6 nJ/98 ns at a repetition rate of 1.42 MHz.Ministerio de Economía y Competitividad (MINECO) (FIS2013-44174-P, FIS2015-71933-REDT, MAT2016-75716-C2-1-R (AEI/FEDER,UE), TEC2014-55948-R); Agència de Gestió d’Ajuts Universitaris i de Recerca (AGAUR) (2017SGR755); Consejería de Educación, Junta de Castilla y León (SA046U16, UIC016); Generalitat de Catalunya (2016FI_B00844, 2017FI_B100158, 2018 FI_B2 00123)