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All-optical nanoscopic spatial control of molecular reaction yields on nanoparticles

Molecular adsorbate reactions on nanoparticles play a fundamental role in areas such as nano-photocatalysis, atmospheric, and astrochemistry. They can be induced, enhanced, and controlled by field localization and enhancement on the nanoparticle surface. In particular, the ability to perform highly controlled near-field-mediated reactions is key to deepening our understanding of surface photoactivity on nanosystems. Here, using reaction nanoscopy, we experimentally demonstrate all-optical nanoscopic control of surface reaction yields by tailoring the near fields on nanoparticles with waveform-controlled linear and bicircular two-color laser pulses, respectively. We observe site-selective proton emission from the dissociative ionization of adsorbate molecules on Si O 2 nanoparticles as a function of the polarization and relative phase of the two-color pulses. The angularly resolved close-to-uniform mapping between the surface reaction yields and the measured ion momentum enables the observation and spatial control of molecular reactions on the nanoparticle surface with nanoscopic resolution. The experimental results are modeled and reproduced qualitatively by classical trajectory Monte Carlo simulations. Our work paves the way toward reliable all-optical control of photocatalytic chemical reactions on nanoscale surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The double-nucleus galaxy IRAS 02580-1136 - A merging system

CCD imaging, infrared photometry, and optical spectroscopy lead to the conclusion that IRAS 02580-1136 consists of two colliding galaxies and is possibly an ongoing merger. Visually, the IRAS source displays two distinct brightness concentrations. These two nuclei, referred to as A and B, have a projected linear separation of 7 kpc and a radial-velocity difference of 180 km/s. Nucleus A belongs to a bulgelike structure and has an optical spectrum typical of a Seyfert 2. It is argued that it harbors a 99 percent dust-obscured low-luminosity Seyfert I source that powers most of the far-infrared radiation. Nucleus B is either a galactic bulge or a low-luminosity elliptical with a heavily reddened compact H II region at its center.

Heisler, Charlene A.↗

Compact single-shot electro-optic detection system for THz pulses with femtosecond time resolution at MHz repetition rates

Electro-optical detection has proven to be a valuable technique to study temporal profiles of THz pulses with pulse durations down to femtoseconds. As the Coulomb field around a relativistic electron bunch resembles the current profile, electro-optical detection can be exploited for non-invasive bunch length measurements at accelerators. We have developed a very compact and robust electro-optical detection system based on spectral decoding for single-shot longitudinal bunch profile monitoring at the European X-ray Free Electron Laser (XFEL) for electron bunch lengths down to 200 fs (rms). Apart from the GaP crystal and the corresponding laser optics at the electron beamline, all components are housed in 19 in. chassis for rack mount and remote operation inside the accelerator tunnel. An advanced laser synchronization scheme based on radio-frequency down-conversion has been developed for locking a custom-made Yb-fiber laser to the radio-frequency of the European XFEL accelerator. In order to cope with the high bunch repetition rate of the superconducting accelerator, a novel linear array detector has been employed for spectral measurements of the Yb-fiber laser pulses at frame rates of up to 2.26 MHz. In this paper, we describe all sub-systems of the electro-optical detection system as well as the measurement procedure in detail and discuss the first measurement results of longitudinal bunch profiles of around 400 fs (rms) with an arrival-time jitter of 35 fs (rms).

47 OTHER INSTRUMENTATION↗

Integrated Modeling for the Next Generation Space Telescope "Yardstick" Concept

The so-called NASA "Yardstick" design concept for the Next Generation Space Telescope presents unique challenges for systems-level analysis. Simulations that integrate controls, optics, thermal, and structural models are required to evaluate baseline performance, study design sensitivities, and perform design optimization. An integrated modeling approach was chosen using a combination of commercial off-the-shelf and "in-house" developed codes. The resulting capability provides a foundation for linear and non-linear analysis, using both the time and frequency-domain methods. It readily allows various combinations of design parameters and environmental loads to be evaluated directly in terms of key science-related metrics, in this case the scalar RMS (root mean square) line-of-sight and RMS wavefront errors. This presentation first addresses the development of the component, or discipline, models for the Yardstick design. It will then proceed to present the integration of the component models, using linear-systems approaches, in order to support two of the most critical baseline performance analyses: jitter and thermal-elastic stability of the optical telescope assembly (OTA). The results of the jitter analysis indicate that disturbances from the reaction wheels coupled with the lightly-damped and highly-flexible structure present significant challenges to the baseline line-of-sight control architecture. Vibration isolation will be required to meet jitter error requirements. The results of the thermal-elastic analysis indicate that the mirror segment displacements due to ground-to-orbit cool-down of the telescope are within the expected capture range of the segment rigid-body control actuators. This means we will be able to align and phase the primary mirror. However, the results for the analysis of the thermal transient response following an attitude maneuver (slew) show that this telescope design is not sufficiently stable, passively, to meet the wavefront error requirements. Structural re-design is one possibility; alternatively, active thermal control of the OTA may be considered. The Yardstick integrated models were successfully used to demonstrate the feasibility of two thermal control strategies.

Mosier, Gary E.↗

324GHz CMOS VCO Using Linear Superimposition Technique

Terahertz (frequencies ranged from 300GHz to 3THz) imaging and spectroscopic systems have drawn increasing attention recently due to their unique capabilities in detecting and possibly analyzing concealed objects. The generation of terahertz signals is nonetheless nontrivial and traditionally accomplished by using either free-electron radiation, optical lasers, Gunn diodes or fundamental oscillation by using III-V based HBT/HEMT technology[1-3]... We have substantially extended the operation range of deep-scaled CMOS by using a linear superimposition method, in which we have realized a 324GHz VCO in 90nm digital CMOS with 4GHz tuning range under 1V supply voltage. This may also pave the way for ultra-high data rate wireless communications beyond that of IEEE 802.15.3c and reach data rates comparable to that of fiber optical communications, such as OC768 (40Gbps) and beyond.

voltage controlled oscillators (VCO)↗

Use of Photoelastic Modulators for High-accuracy Spectropolarimetric Imaging of Aerosols

Passive multiangular, multispectral, and polarimetric sensing approaches each have unique strengths for the measurement of tropospheric aerosol column abundances and microphysical properties. Current spaceborne multispectral and multiangular aerosols sensors operate at approximately 1 km resolution. Under NASA's Instrument Incubator Program, we are developing an electro-optic imaging approach that will enable adding high-accuracy polarimetry to such observations. To achieve a degree of linear polarization (DOLP) uncertainty of 0.5%, our approach temporally modulates the linear-polarization component of incoming light at a rapid rate, enabling each detector within a focal-plane array, combined with polarization analyzers, to measure the relative proportions of the linear Stokes components Q or U to the total intensity. Our system uses tandem photoelastic modulators (PEMs) within a high-reflectance, low diattenuation camera design. The two PEMs vibrate at slightly different resonant frequencies, leading to modulation of the polarized light at a heterodyne frequency of ~25 Hz. High-speed (1 kHz) readout of the detector arrays samples the output waveforms from which Q/I and U/I are derived. We report on experimental and theoretical analyses of PEM and optical system performance, along with plans for developing ruggedized PEMs capable of withstanding launch and on-orbit stresses.

photoelastics↗

Absorbed dose measurements on LDEF and comparisons with predictions

The radiation environment on LDEF was monitored by cumulative absorbed dose measurements made with TLDs at different locations and shielding depths. The TLDs were included in four experiments: A0015(a) Biostack, P0004 Seeds in Space and P0006 Linear Energy Transfer Spectrum Measurements at the trailing edge (west side) of the satellite; M0004 Fiber Optics Data Link at the leading edge (east side); and A0015(b) Biostack at the Earth side. The shielding depths varied between 0.48 and 15.4 g/cm2, Al equivalent. Both the directional dependence of trapped protons incident on the satellite and the shielding thickness were reflected in absorbed dose values. The trapped proton anisotropy was measured by TLDs at the east and west sides of LDEF. At the east side doses ranged from 2.10 to 2.58 Gy under shielding of 2.90 to 1.37 g/cm2 (M0004) while on the west side doses ranged from 2.66 to 6.48 Gy under shielding of 15.4 to 0.48 g/cm2 (P0006). The west side doses were more than a factor of two higher, where the vertical shielding thicknesses to space were equal. Other west side doses of 3.04 to 4.49 Gy under shielding of 11.7 to 3.85 g/cm2 (A0015(a)) and 2.91 to 6.64 Gy under shielding of 11.1 to 0.48 g/cm2 (P0004) generally agreed with the P0006 results. The Earth side doses of 2.41 to 3.93 Gy under shielding of 10.0 to 1.66 g cm2 (A0015(b)) were intermediate between the east side and west side doses. Calculations utilizing a model of trapped proton spectra were performed by Watts et al. (1993) and comparisons of dose measurement and calculations may be found in a companion paper (Armstrong et al., 1996).

Flight Experiment↗

Polarimetric Retrievals of Surface and Cirrus Clouds Properties in the Region Affected by the Deepwater Horizon Oil Spill

In 2010, the Goddard Institute for Space Studies (GISS) Research Scanning Polarimeter (RSP) performed several aerial surveys over the region affected by the oil spill caused by the explosion of the Deepwater Horizon offshore platform. The instrument was deployed on the NASA Langley B200 aircraft together with the High Spectral Resolution Lidar (HSRL), which provides information on the distribution of the aerosol layers beneath the aircraft, including an accurate estimate of aerosol optical depth. This work illustrates the merits of polarization measurements in detecting variations of ocean surface properties linked to the presence of an oil slick. In particular, we make use of the degree of linear polarization in the glint region, which is severely affected by variations in the refractive index but insensitive to the waviness of the water surface. Alterations in the surface optical properties are therefore expected to directly affect the polarization response of the RSP channel at 2264 nm, where both molecular and aerosol scattering are negligible and virtually all of the observed signal is generated via Fresnel reflection at the surface. The glint profile at this wavelength is fitted with a model which can optimally estimate refractive index, wind speed and direction, together with aircraft attitude variations affecting the viewing geometry. The retrieved refractive index markedly increases over oil-contaminated waters, while the apparent wind speed is significantly lower than in adjacent uncontaminated areas, suggesting that the slick dampens high-frequency components of the ocean wave spectrum. The constraint on surface reflectance provided by the short-wave infrared channels is a cornerstone of established procedures to retrieve atmospheric aerosol microphysical parameters based on the inversion of the RSP multispectral measurements. This retrieval, which benefits from the ancillary information provided by the HSRL, was in this specific case hampered by prohibitive variability in atmospheric conditions (very inhomogeneous aerosol distribution and cloud cover). Although the results presented for the surface are essentially unaffected, we discuss the results obtained by typing algorithms in sorting the complex mix of aerosol types, and show evidence of oriented ice in cirrus clouds present in the area. In this context, polarization measurements at 1880 nm were used to infer ice habit and cirrus optical depth, which was found in the subvisual/threshold-visible regime, confirming the utility of the aforementioned RSP channel for the remote sensing of even thin cold clouds.

Polarization↗

MOPITT Mechanisms 16 Years In-Orbit Operation on TERRA

The 16th anniversary of the launch of NASA's Terra Spacecraft was marked on December 18, 2015, with the Measurements of Pollution in the Troposphere (MOPITT) instrument being a successful contributor to the NASA EOS flagship. MOPITT has been enabled by a large suite of mechanisms, allowing the instrument to perform long-duration monitoring of atmospheric carbon monoxide, providing global measurements of this important greenhouse gas for 16 years. Mechanisms have been successfully employed for scanning, cooling of detectors, and to optically modulate the gas path length within the instrument by means of pressure and gas cell length variation. The instrument utilizes these devices to perform correlation spectroscopy, enabling measurements with vertical resolution from the nadir view, and has thereby furthered understanding of source and global transport effects of carbon monoxide. Given the design requirement for a 5.25-year lifetime, the stability and performance of the majority of mechanisms have far surpassed design goals. With 16 continuously operating mechanisms in service on MOPITT, including 12 rotating mechanisms and 4 with linear drive elements, the instrument was an ambitious undertaking. The long life requirements combined with demands for cleanliness and optical stability made for difficult design choices including that of the selection of new lubrication processes. Observations and lessons learned with regards to many aspects of the mechanisms and associated monitoring devices are discussed here. Mechanism behaviors are described, including anomalies, long-term drive current/power, fill pressure, vibration and cold-tip temperature trends. The effectiveness of particular lubrication formulations and the screening method implemented is discussed in relation to continuous rotating mechanisms and stepper motors, which have exceeded 15 billon rotations and 2.5 billion steps respectively. Aspects of gas cell hermeticity, optical cleanliness, heater problems and SEU effects on accelerometers are also discussed.

Gibson, Andrew S.↗

Experimental Characterization of Photoemission from Plasmonic Nanogroove Arrays

Metal photocathodes are an important source of high-brightness electron beams, ubiquitous in the operation of both large-scale accelerators and table-top microscopes. When the surface of a metal is nanoengineered with patterns on the order of the optical wavelength, it can lead to the excitation and confinement of surface-plasmon-polariton waves that drive nonlinear photoemission. In this work, we aim to evaluate gold plasmonic nanogrooves as a concept for producing bright electron beams for accelerators via nonlinear photoemission. Here, we do this by first comparing their optical properties to numerical calculations from first principles to confirm our ability to fabricate these nanoscale structures. Their nonlinear photoemission yield is found by measuring emitted photocurrent as the intensity of their driving laser is varied. Finally, the mean transverse energy of this electron source is found using the solenoid-scan technique. Our data demonstrate the ability of these cathodes to provide a tenfold enhancement in the efficiency of photoemission over flat metals driven with a linear process. We find that these cathodes are robust and capable of reaching sustained average currents over 100 nA at optical intensities larger than 2 GW cm –2 with no degradation of performance. The emittance of the generated beam is found to be highly asymmetric, a fact we can explain with calculations involving the also asymmetric roughness of the patterned surface. These results demonstrate the use of nanoengineered surfaces as enhanced photocathodes, providing a robust air-stable source of high-average-current electron beams hopefully with great potential for industrial and scientific applications.

47 OTHER INSTRUMENTATION↗

Microwave Oscillators Based on Nonlinear WGM Resonators

Optical oscillators that exploit resonantly enhanced four-wave mixing in nonlinear whispering-gallery-mode (WGM) resonators are under investigation for potential utility as low-power, ultra-miniature sources of stable, spectrally pure microwave signals. There are numerous potential uses for such oscillators in radar systems, communication systems, and scientific instrumentation. The resonator in an oscillator of this type is made of a crystalline material that exhibits cubic Kerr nonlinearity, which supports the four-photon parametric process also known as four-wave mixing. The oscillator can be characterized as all-optical in the sense that the entire process of generation of the microwave signal takes place within the WGM resonator. The resonantly enhanced four-wave mixing yields coherent, phase-modulated optical signals at frequencies governed by the resonator structure. The frequency of the phase-modulation signal, which is in the microwave range, equals the difference between the frequencies of the optical signals; hence, this frequency is also governed by the resonator structure. Hence, further, the microwave signal is stable and can be used as a reference signal. The figure schematically depicts the apparatus used in a proof-of-principle experiment. Linearly polarized pump light was generated by an yttrium aluminum garnet laser at a wavelength of 1.32 microns. By use of a 90:10 fiber-optic splitter and optical fibers, some of the laser light was sent into a delay line and some was transmitted to one face of glass coupling prism, that, in turn, coupled the laser light into a crystalline CaF2 WGM disk resonator that had a resonance quality factor (Q) of 6x10(exp 9). The output light of the resonator was collected via another face of the coupling prism and a single-mode optical fiber, which transmitted the light to a 50:50 fiber-optic splitter. One output of this splitter was sent to a slow photodiode to obtain a DC signal for locking the laser to a particular resonator mode. The other output of this splitter was combined with the delayed laser signal in another 50:50 fiber-optic splitter used as a combiner. The output.of the combiner was fed to a fast photodiode that demodulated light and generated microwave signal. In this optical configuration, the resonator was incorporated into one arm of a Mach-Zehnder interferometer, which was necessary for the following reasons: It was found that when the output of the resonator was sent directly to a fast photodiode, the output of the photodiode did not include a measurable microwave signal. However, when the resonator was placed in an arm of the interferometer and the delay in the other arm was set at the correct value, the microwave signal appeared. Such behavior is distinctly characteristic of phase-modulated light. The phase-modulation signal had a frequency of about 8 GHz, corresponding to the free spectral range of the resonator. The spectral width of this microwave signal was less than 200 Hz. The threshold pump power for generating the microwave signal was about 1 mW. It would be possible to reduce the threshold power by several orders of magnitude if resonators could be made from crystalline materials in dimensions comparable to those of micro-resonators heretofore made from fused silica.

Maleki, Lute↗

The solar vector magnetograph of the Okayama Astrophysical Observatory

The vector magnetograph of the Okayama Astrophysical Observatory is fed to the 65 cm solar coude telescope with a 10 m Littrow spectrograph. The polarimeter put at the telescope focus analyzes the incident polarization. Photomultipliers (PMT) at the exit of the spectrograph pick up the modulated light signals and send them to the electronic controller. The controller analyzes frequency and phase of the signal. The analyzer of the polarimeter is a combination of a single wave plate rotating at 40 Hz and a Wallaston prism. Incident linear and circular polarizations are modified at four times and twice the rotation frequency, respectively. Two compensators minimize the instrumental polarization, mainly caused by the two tilt mirrors in the optical path of the telescope. The four photomultipliers placed on the wings of the FeI 5250A line give maps of intensity, longitudinal field and transverse field. The main outputs, maps of intensity, and net linear and circular polarizations in the neighboring continuum are obtained by the other two monitor PMTs.

Makita, M.↗

Pseudoslit Spectrometer

The pseudoslit spectrometer is a conceptual optoelectronic instrument that would offer some of the advantages, without the disadvantages, of prior linear-variable etalon (LVE) spectrometers and prior slit spectrometers. The pseudoslit spectrometer is so named because it would not include a slit, but the combined effects of its optical components would include a spatial filtering effect approximately equivalent to that of a slit. Like a prior LVE spectrometer, the pseudoslit spectrometer would include an LVE (essentially, a wedge-like narrowband- pass filter, the pass wavelength of which varies linearly with position in one dimension) in a focal plane covering an imaging planar array of photodetectors. However, the pseudoslit spectrometer would be more efficient because unlike a prior LVE spectrometer, the pseudoslit spectrometer would not have to be scanned across an entire field of view to obtain the spectrum of an object of interest that may occupy only a small portion of the field of view. Like a prior slit spectrometer, the pseudoslit spectrometer could acquire the entire spectrum of such a small object without need for scanning. However, the pseudoslit spectrometer would be optically and mechanically simpler: it would have fewer components and, hence, would pose less of a problem of alignment of components and would be less vulnerable to misalignment.

Reuter, Dennis C.↗

Rational Design of Methylated Triazine‐Based Linear Conjugated Polymers for Efficient CO 2 Photoreduction with Water

The development of semiconducting conjugated polymers for photoredox catalysis holds great promise for sustainable utilization of solar energy. In this work, a new family of porous methylated triazine‐based linear conjugated polymers is reported that enable efficient photoreduction of carbon dioxide (CO 2 ) with water (H 2 O) vapor, in the absence of any additional photosensitizer, sacrificial agents or cocatalysts. It is demonstrated that the key lies in the generation of methylated triazine linkages through a facile condensation reaction between benzamidine and acetic anhydride, which impedes the formation of conventional triazine‐based frameworks. It is also shown that regulating conjugated linear backbones with different lengths of electron‐donated benzyl units provides a facile means to modulate their optical properties and the exciton dissociation, thereby affording more long‐lived photogenerated charge carriers and boosting charge separation and transfer. A high‐performance carbon monoxide (CO) production rate of 218.9 µmol g −1 h −1 is achieved with ≈ 100% CO selectivity, which is accompanied by exceptional H 2 O oxidation to oxygen (O 2 ). It anticipates this new study will advance synthetic approaches toward polymeric semiconductors and facilitate new possibilities for triazine‐based conjugated polymers with promising potential in artificial photocatalysis.

36 MATERIALS SCIENCE↗

The Simons Observatory: A fully remote controlled calibration system with a sparse wire grid for cosmic microwave background telescopes

For cosmic microwave background (CMB) polarization observations, calibration of detector polarization angles is essential. We have developed a fully remote controlled calibration system with a sparse wire grid that reflects linearly polarized light along the wire direction. The new feature is a remote-controlled system for regular calibration, which has not been possible in sparse wire grid calibrators in past experiments. The remote control can be achieved by two electric linear actuators that load or unload the sparse wire grid into a position centered on the optical axis of a telescope between the calibration time and CMB observation. Furthermore, the sparse wire grid can be rotated by using a motor. A rotary encoder and a gravity sensor are installed on the sparse wire grid to monitor the wire direction. They allow us to achieve detector polarization angle calibration with an expected systematic error of 0.08°. The calibration system will be installed in small-aperture telescopes at Simons Observatory.

47 OTHER INSTRUMENTATION↗

Computing nuclear response functions with time-dependent coupled-cluster theory

We compute nuclear response functions by solving the time-dependent 𝐴-body Schrödinger equation, recording the time-dependent transition moment and extracting spectral information via Fourier transforms. The solution of the time-dependent many-body problem accounts for correlations on top of the mean field by taking advantage of a time-dependent formulation of coupled-cluster theory. As a validation, we focus on electric dipole transitions in 4 He and 16 O and compare moments of the response function distribution to the results of an equivalent static framework, finding negligible discrepancies. We investigate how proton and neutron densities evolve in time, and we see the traditional picture of soft and giant dipole resonances as collective oscillations of protons and neutrons emerging from our calculations in 16 O and 24 O. Furthermore, this method also allows us to investigate the behavior of the nucleus in the presence of a strong electric field. In that regime, the behavior of the system becomes chaotic. Qualitatively, the spectral information obtained in this limit is in line with previous time-dependent mean-field results.

Ab initio calculations↗

ARM shortwave spectrometers to study the clear-cloud transition zone and mixing processes

The proposed research is a collaborative effort between NASA/Goddard Space Flight Center and the Hebrew University of Jerusalem. While the NASA team focused on analyzing ground-based hyper-spectral radiance observations to understand cloud edge properties and their connection to mixing processes, the Hebrew University team tackled the problem through cloud modeling activities. By approximating the shortwave spectra in the cloud-clear transition zone as a linear combination of purely clear and purely cloudy spectra we can characterize the variations of cloud optical thickness and cloud droplet effective radius in the transition zone. When applying this method to the measurements of a ground-based shortwave spectroradiometer at the ARM’s SGP site, representing continental conditions, and MAGIC field campaign between Log Angeles, California and Honolulu, Hawaii, representing maritime scenarios, we found that cloud optical depth consistently decreases in both cases, but droplet size decreases much more substantially for the continental regime, suggesting different mixing processes for the continental and maritime conditions. The investigation and measurements of radiation clouds were coupled with a unique cloud modeling. A novel spectral bin microphysics was developed and implemented to the System of Atmospheric Modeling (SAM). In order to resolve cloud transition zones with high spatial gradients of microphysical variables a unique high resolution (10 m) was used in simulations. The model calculates droplet size distributions in each grid point. The model output was transferred to the NASA/GSFC team for utilization in radiative calculations and testing of both radiative algorithm and model representation.

54 ENVIRONMENTAL SCIENCES↗