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At least 19 records

Use of Novel Light Sources and Melatonin Delivery Systems in the Maintenance of Temporal Organization of Physiological and Behavioral Circadian Rhythms

The synchronization of physiological and behavioral rhythms are controlled by an endogenous biological clock. It is generally accepted that environmental lighting is the strongest entrainer of this clock. The pineal gland is an important physiological transducer of environmental lighting via systemic melatonin secretion. We have used a novel light source using light emitting diode (LED) technology to entrain circadian rhythms in rats, and propose a novel percutaneous exogenous melatonin delivery system to entrain rat rhythms. We used 5 groups of Sprague-Dawley rats (175-350 g; N = 8/group) and showed normal entrainment of gross locomotor activity, feeding, and drinking circadian rhythms at light intensities varying from 80 lux to 0.1 lux (22.4 to 0.03 sq cm). To improve the delivery of melatonin across the skin stratum corneum it was formulated in a suitable vehicle in a transdermal drug delivery system. Various saturated and unsaturated fatty acids were used E, akin penetration enhancers. Our best vehicle formulation was achieved with a combination-of ethano1:water (60:40) along with 5% oleic acid as the enhancer. This formulation mixture was studied using Franz diffusion cell (0.636 sq cm diffusional area) and 1 cu cm dorsal skin isolated from Sprague Dawley rats. Our results showed that oleic acid in combination with the water ethanol mixture improved the flux of melatonin by more than 18 fold. The lag time for melatonin permeation was 2-3 hrs and the peak concentrations were achieved in 8-10 hrs. Our approaches in the future will involve the use of our transdermal melatonin delivery system and under the influence of LED light and microgravity.

Winget, C. M.↗

Detection of the keto-enol tautomerization in acetaldehyde, acetone, cyclohexanone, and methyl vinyl ketone with a novel VUV light source

The discovery of enols in combustion environments and our atmosphere has garnered increasing attention to the many unanswered questions surrounding enol chemistry. The scarcity of experimental data concerning these enols renders combustion and atmospheric models with a lack of constraining parameters, leading to varying computational predictions. Experimental detection is difficult because mass spectrometry, a powerful tool for probing a wide variety of species, cannot distinguish between enols and their thermodynamically favorable ketone isomers. A solution to this ambiguity is to use tunable vacuum ultraviolet (VUV) light from a synchrotron to identify the presence of the enol by its lower ionization energy compared to the isomer. We present a tabletop-scale VUV light source that implements highly cascaded harmonic generation, a new regime of cascaded nonlinear optics, to provide a set of spectral lines spaced by 1.2 eV. We demonstrate that the variety of photon energies available allows us to detect the keto-enol tautomerization of four aldehydes and ketones. By combining this novel VUV light source with an established microreactor, we first revisit the formation of vinyl alcohol from acetaldehyde and confirm that the observed isomerization is indeed unimolecular. Secondly, we observe the thermal tautomerization of acetone to propen-2-ol for the first time. Finally, we observe the thermal tautomerization of cyclohexanone to 1-cyclohexenol and methyl vinyl ketone to 2-hydroxybutadiene, where the results are in good agreement with those reported at a synchrotron. Furthermore, our measurements can be used to constrain models, inform future experimental studies of enol reactivity, and potentially enhance current understanding of combustion and environmental chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The 2022 magneto-optics roadmap

Abstract Magneto-optical (MO) effects, viz. magnetically induced changes in light intensity or polarization upon reflection from or transmission through a magnetic sample, were discovered over a century and a half ago. Initially they played a crucially relevant role in unveiling the fundamentals of electromagnetism and quantum mechanics. A more broad-based relevance and wide-spread use of MO methods, however, remained quite limited until the 1960s due to a lack of suitable, reliable and easy-to-operate light sources. The advent of Laser technology and the availability of other novel light sources led to an enormous expansion of MO measurement techniques and applications that continues to this day (see section 1). The here-assembled roadmap article is intended to provide a meaningful survey over many of the most relevant recent developments, advances, and emerging research directions in a rather condensed form, so that readers can easily access a significant overview about this very dynamic research field. While light source technology and other experimental developments were crucial in the establishment of today’s magneto-optics, progress also relies on an ever-increasing theoretical understanding of MO effects from a quantum mechanical perspective (see section 2), as well as using electromagnetic theory and modelling approaches (see section 3) to enable quantitatively reliable predictions for ever more complex materials, metamaterials, and device geometries. The latest advances in established MO methodologies and especially the utilization of the MO Kerr effect (MOKE) are presented in sections 4 (MOKE spectroscopy), 5 (higher order MOKE effects), 6 (MOKE microscopy), 8 (high sensitivity MOKE), 9 (generalized MO ellipsometry), and 20 (Cotton–Mouton effect in two-dimensional materials). In addition, MO effects are now being investigated and utilized in spectral ranges, to which they originally seemed completely foreign, as those of synchrotron radiation x-rays (see section 14 on three-dimensional magnetic characterization and section 16 on light beams carrying orbital angular momentum) and, very recently, the terahertz (THz) regime (see section 18 on THz MOKE and section 19 on THz ellipsometry for electron paramagnetic resonance detection). Magneto-optics also demonstrates its strength in a unique way when combined with femtosecond laser pulses (see section 10 on ultrafast MOKE and section 15 on magneto-optics using x-ray free electron lasers), facilitating the very active field of time-resolved MO spectroscopy that enables investigations of phenomena like spin relaxation of non-equilibrium photoexcited carriers, transient modifications of ferromagnetic order, and photo-induced dynamic phase transitions, to name a few. Recent progress in nanoscience and nanotechnology, which is intimately linked to the achieved impressive ability to reliably fabricate materials and functional structures at the nanoscale, now enables the exploitation of strongly enhanced MO effects induced by light–matter interaction at the nanoscale (see section 12 on magnetoplasmonics and section 13 on MO metasurfaces). MO effects are also at the very heart of powerful magnetic characterization techniques like Brillouin light scattering and time-resolved pump-probe measurements for the study of spin waves (see section 7), their interactions with acoustic waves (see section 11), and ultra-sensitive magnetic field sensing applications based on nitrogen-vacancy centres in diamond (see section 17). Despite our best attempt to represent the field of magneto-optics accurately and do justice to all its novel developments and its diversity, the research area is so extensive and active that there remains great latitude in deciding what to include in an article of this sort, which in turn means that some areas might not be adequately represented here. However, we feel that the 20 sections that form this 2022 magneto-optics roadmap article, each written by experts in the field and addressing a specific subject on only two pages, provide an accurate snapshot of where this research field stands today. Correspondingly, it should act as a valuable reference point and guideline for emerging research directions in modern magneto-optics, as well as illustrate the directions this research field might take in the foreseeable future.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Free electron lasers driven by plasma accelerators: status and near-term prospects

Owing to their ultra-high accelerating gradients, combined with injection inside micrometer-scale accelerating wakefield buckets, plasma-based accelerators hold great potential to drive a new generation of free-electron lasers (FELs). Indeed, the first demonstration of plasma-driven FEL gain was reported recently, representing a major milestone for the field. Several groups around the world are pursuing these novel light sources, with methodology varying in the use of wakefield driver (laser-driven or beam-driven), plasma structure, phase-space manipulation, beamline design, and undulator technology, among others. This paper presents our best attempt to provide a comprehensive overview of the global community efforts towards plasma-based FEL research and development.

47 OTHER INSTRUMENTATION↗

An ultra-compact x-ray free-electron laser

In the field of beam physics, two frontier topics have taken center stage due to their potential to enable new approaches to discovery in a wide swath of science. These areas are: advanced, high gradient acceleration techniques, and x-ray free electron lasers (XFELs). Further, there is intense interest in the marriage of these two fields, with the goal of producing a very compact XFEL. In this context, recent advances in high gradient radio-frequency cryogenic copper structure research have opened the door to the use of surface electric fields between 250 and 500 MV m -1 . Such an approach is foreseen to enable a new generation of photoinjectors with six-dimensional beam brightness beyond the current state-of-the-art by well over an order of magnitude. This advance is an essential ingredient enabling an ultra-compact XFEL (UC-XFEL). In addition, one may accelerate these bright beams to GeV scale in less than 10 m. Such an injector, when combined with inverse free electron laser-based bunching techniques can produce multi-kA beams with unprecedented beam quality, quantified by 50 nm-rad normalized emittances. The emittance, we note, is the effective area in transverse phase space (x, p x /m e c) or (y, p y /m e c) occupied by the beam distribution, and it is relevant to achievable beam sizes as well as setting a limit on FEL wavelength. These beams, when injected into innovative, short-period (1–10 mm) undulators uniquely enable UC-XFELs having footprints consistent with university-scale laboratories. We describe the architecture and predicted performance of this novel light source, which promises photon production per pulse of a few percent of existing XFEL sources. We review implementation issues including collective beam effects, compact x-ray optics systems, and other relevant technical challenges. To illustrate the potential of such a light source to fundamentally change the current paradigm of XFELs with their limited access, we examine possible applications in biology, chemistry, materials, atomic physics, industry, and medicine—including the imaging of virus particles—which may profit from this new model of performing XFEL science.

47 OTHER INSTRUMENTATION↗

Ultrafast Dynamics of Molecules on Surfaces Studied with Time-Resolved XUV Photoelectron Spectroscopy (Final Report)

In this project we set out to make technical advances in time-resolved photoemission from surfaces and study molecule-surface charge transfer processes. Combining a novel light source developed at Stony Brook with a new type of time-of-flight photoemission electron microscope (TOF k-mic) developed in Mainz, Germany, we achieved the former goal. Our light source, based on cavity-enhanced high harmonic generation at 61 MHz repetition rate, enables ultrafast time-resolved photoemission experiments to be conducted with orders of magnitude higher photocurrents than otherwise possible. Critically, this provides the high dynamic range necessary to study perturbatively excited samples, such that one can study the intrinsic dynamics of electrons and holes as they would occur in a device. Combining our light source with the TOF k-mic, we’ve achieved an overall improvement in data rate of time- and angle-resolved photoemission (tr-ARPES) of approximately four orders of magnitude over the previous state-of-the-art using kHz-repetition rate sources and conventional hemispherical electron analyzers. This new instrument is now being used in experiments on 2D materials and organic semiconductors.

74 ATOMIC AND MOLECULAR PHYSICS↗

Circadian Behavioral Study: LED vs Cool White Fluorescent - 0.1, 1, 10, 40, 80 lux

Currently, the light source most commonly used in animal habitat lighting is cool white fluorescent (CWF) light. It was the objective of this study to evaluate a novel LED light source for use in animal habitat lighting by comparing its effectiveness to CWF light in producing and maintaining a normal circadian entrainment. The LED and CWF lights had similar spectral power distributions. Sprague-Dawley rats (175-350 g) were kept individually in metabolic cages, under a strict lighting control: 4 days of acclimation at 12:12 LD, 14 days of 12:12 LD, 14 days of 24:0 LD (free-run), and finally 12:12 LD. Food and water were provided ad libitum. Three behavioral parameters were monitored continuously: gross locomotor activity, drinking, and feeding. Combined mean free run periods (tau) were (mean +/- SEM): 24.6 +/- 0.1 and 24.7 +/- 0.2 at 0.1 lux, 25.5 +/- 0.1 and 25.7 +/- 0.1 at 1.0 lux, 25.3 +/- 0.2 and 25.4 +/- 0.2 at 10 lux, 25.8 +/- 0.1 and 25.9 +/- 0.1 at 40 lux, and 25.9 +/- 0.1 and 25.9 +/- 0.1 at 80 lux, CWF and LED respectively. ANOVA found a significant effect (p < 0.05) due to light level, but no difference in tau between rats exposed to constant CWF light and rats exposed to constant LED light. This study has shown that LED light can produce the same entrainment pattern as a conventional CWT light at similar intensities (0.1, 1, 10, 40, and 80 lux). LED light sources may be a suitable replacement for conventional light sources used in animal habitat lighting while providing many mechanical and economical advantages.

Holley, Daniel C.↗

Manipulation of quantum dot emission with semiconductor metasurfaces exhibiting magnetic quadrupole resonances

Optical metasurfaces were suggested as a route for engineering advanced light sources with tailored emission properties. In particular, they provide a control over the emission directionality, which is essential for single-photon sources and LED applications. Here, we experimentally study light emission from a metasurface composed of III-V semiconductor Mie-resonant nanocylinders with integrated quantum dots (QDs). Specifically, we focus on the manipulation of the directionality of spontaneous emission from the QDs due to excitation of different magnetic quadrupole resonances in the nanocylinders. To this end, we perform both back focal plane imaging and momentum-resolved spectroscopy measurements of the emission. This allows for a comprehensive analysis of the effect of the different resonant nanocylinder modes on the emission characteristics of the metasurface. Our results show that the emission directionality can be manipulated by an interplay of the excited quadrupolar nanocylinder modes with the metasurface lattice modes and provide important insights for the design of novel smart light sources and new display concepts.

Vaskin, Aleksandr↗

Laboratory Studies of the Photochemistry of Peroxynitric Acid

Observations of odd hydrogen radicals at high SZA in the lower stratosphere have demonstrated that our understanding of the HO(x) chemistry is incomplete [Wennberg et al., 1994a; Salawitch et al., 1994; Wennberg et al., 1999]. In particular, the concentrations of the HO(x) radicals are significantly larger than expected under weak photolytic conditions. Donaldson et al. [1997] have speculated that excitation of overtones of the OH stretching frequency in molecules such as HNO3 and HO2NO2 may be significant sources of HO(x) under these conditions. Although weak, vibrationally mediated photolysis may be important because it occurs in the near IR and visible and can provide energy in excess of the dissociation energy (D(o)): HONO2 + hv yields OH + NO (D(o) approx. 600 nm) and HOONO2 + hv yields OH + NO3 (D(o) approx. 735 nm) HOONO2 + hv yields HO2 + NO2 (D(o) approx. 1250 nm). In this project we developed instrumentation to characterize the photodissociation yields of hydroxyl containing compounds in the visible and near IR. This effort has involved coupling a tunable photolysis optical parametric oscillator (OPO) laser system with precise determination of the hydroxyl radical. The OPO system [Wu et al., 1997] was developed with support from the NSF Major Research Instrumentation Fund in a proposal entitled "Development of Novel, Compact Light Sources for Advanced Spectroscopy in Atmospheric Science and Materials Research" (Geoffrey A. Blake, P.I. California Institute of Technology).

Wennberg, Paul O.↗

Experimental observation of polarization-resolved nonlinear Thomson scattering of elliptically polarized light

We report experimental results from a study of nonlinear Thomson scattering of elliptically polarized light. Polarization-resolved radiation patterns of the scattered light are measured as a function of the elliptical polarization state of the incident laser light. The relativistic electron trajectory in intense elliptically polarized fields leads to the formation of unique radiated polarization states, which are observed by our measurements and predicted by a theoretical model. The polarization of Thomson scattered light depends strongly on the intensity of the incident light due to nonlinearity. The results are relevant to high-field electrodynamics and to research and development of light sources with novel capabilities.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Comparison of Light Emitting Diodes (LED) and Fluorescent Light on Suppression of Pineal Melatonin in the Rat

To validate a novel LED array for use in animal habitat lighting by comparing its effectiveness to cool-white fluorescent (CWF) lighting in suppressing pineal gland melatonin. Male Sprague-Dawley rats, 175-200 g, were maintained under control conditions for 2 weeks (food and water ad lib, 12L: 12D CWF, 18 uW/square cm). Dark adapted animals (animals before lights on) were exposed to 5 min of LED or CWF light of similar spectral power distribution. Two groups of rats (LED vs. CWF) were compared at 5 light intensities (100, 40, 1, 1.0, and 0. 1 lux). A control group was placed into the exposure apparatus but not exposed to light. After exposure, pineal glands were rapidly removed and assayed for melatonin by RIA. Results. The dark-exposed control groups matched with the 5 intensity groups (100, 40, 10, 1.0, and 0.1 lux) showed mean + SEM pineal melatonin values of 1167 +/- 136, 1569 +/- 126, 353 +/- 34, 650 +/- 124, and 464 +/- 85, pg/ml respectively. The corresponding CWF exposure data were 393 1 41, 365 +34, 257 +/- 13, 218 +/- 42, and 239 +/- 71 pg/ml, respectively. Corresponding LED exposure data were 439 +/- 25, 462 +/- 50, 231 +/- 6, 164 +/- 12, and 158 +/- 12 pg/ml, respectively. Rats exposed to both experimental light conditions at all illuminances studied showed significant melatonin suppression (p less than 0.01, ANOVA). In no case was the melatonin suppression induced by LED illuminance significantly different from the melatonin suppression elicited by the same intensity of CWF light. The results show that a novel LED light source can suppress pineal melatonin equal to that of a conventional CWF light source.

Winget, Charles M.↗

An LED Approach for Measuring the Photocatalytic Breakdown of Crystal Violet Dye

A simple technique to assess the reactivity of photocatalytic coatings sprayed onto transmissive glass surfaces was developed. This new method uses ultraviolet (UV) gallium nitride (GaN) light-emitting diodes (LEDs) to drive a photocatalytic reaction (the photocatalytic breakdown of a UV-resistant dye applied to a surface coated with the semiconductor titanium dioxide); and then a combination of a stabilized white light LED and a spectrometer to track the dye degradation as a function of time. Simple, standardized evaluation techniques that assess photocatalytic materials over a variety of environmental conditions, including illumination level, are not generally available and are greatly needed prior to in situ application of photocatalytic technologies. To date, much research pertaining to this aspect of photocatalysis has been limited and has focused primarily on laboratory experiments using mercury lamps. Mercury lamp illumination levels are difficult to control over large ranges and are temporally modulated by line power, limiting their use in helping to understand and predict how photocatalytic materials will behave in natural environmental settings and conditions. The methodology described here, using steady-state LEDs and time series spectroradiometric techniques, is a novel approach to explore the effect of UV light on the photocatalytic degradation of a UV resistant dye (crystal violet). GaN UV LED arrays, centered around 365 nm with an adjustable DC power supply, are used to create a small, spatially uniform light field where the steady state light level can be varied over three to four orders of magnitude. For this study, a set of glass microscope slides was custom coated with a thinly sprayed layer of photocatalytic titanium dioxide. Crystal violet was then applied to these titanium-dioxide coated slides and to uncoated control slides. The slides were then illuminated at various light levels from the dye side of the slide by the UV LED array. To monitor dye degradation on the slides over time, a temperature-stabilized white light LED was used to illuminate the opposite side of the slides. As the dye degraded, the amount of light from the white light LED transmitted through the slide was monitored with a spectrometer and subsequently analyzed to determine and compare the rate of dye degradation for photocatalytically coated versus uncoated slide surfaces. The long-term stability of the spectrometer/white light LED combination, which required only a single reference spectra to be taken for a time series sequence of several hours, enabled accurate measurements of transmitted light over time. Time series transmission curves were generated and results demonstrated that over time the transmission increased much more rapidly on the coated slides than on the control slides. This experimental configuration and methodology for photocatalytic activity measurement minimizes many external variable effects and allows low light level studies to be performed. This study also compares the advantages of this novel LED light source design to traditional mercury lamp systems and non-LED lamp approaches that have conventionally been used. The methodology and experimental design research summarized in this abstract is partly funded by the Department of Homeland Security, Science and Technology Directorate, and by the NASA Stennis Space Center Innovative Partnerships Program.

Ryan, Robert E.↗

Demonstration of a diamond anvil cell platform at the Linac Coherent Light Source: capabilities and outlook

A novel X-ray free electron laser (XFEL) diffraction setup for use with diamond anvil cells (DACs) at the Linac Coherent Light Source (LCLS) is described. The new diamond window at the Matter at Extreme Conditions (MEC) instrument allows hard X-ray experiments on DACs to be performed in air. The platform is described along with alignment and calibration procedures, and details of the X-ray beam and diagnostics. Example data are presented, including a reversible XFEL-induced phase transition in CsPbI 3 . The DAC setup was commissioned at MEC, but is applicable to most LCLS instruments where the unique pulse structures available at LCLS offer access to new ultrafast experimental techniques at high pressure.

Linac Coherent Light Source (LCLS)↗

Demonstration of a diamond anvil cell platform at the Linac Coherent Light Source: Capabilities and Outlook

A novel x-ray free electron laser (XFEL) diffraction setup for use with diamond anvil cells (DACs) at the Linac Coherent Light Source (LCLS) is described. Using the new diamond window at the Matter at Extreme Conditions (MEC) instrument, it allows hard x-ray experiments on DACs to be performed in air. The platform is described along with alignment and calibration procedures and details of the x-ray beam and diagnostics. Example data are presented, including a reversible XFEL induced phase transition in CsPbI3. The DAC setup was commissioned at MEC, but is applicable to most LCLS instruments where the unique pulse structures available at LCLS offer access to new ultrafast experimental techniques at high pressure.

Diamond Anvil Cells, LCLS, XFEL, High-Pressure↗

A cantilevered liquid-nitrogen-cooled silicon mirror for the Advanced Light Source Upgrade

This paper presents a novel cantilevered liquid-nitrogen-cooled silicon mirror design for the first optic in a new soft X-ray beamline that is being developed as part of the Advanced Light Source Upgrade (ALS-U) (Lawrence Berkeley National Laboratory, USA). The beamline is optimized for photon energies between 400 and 1400 eV with full polarization control. Calculations indicate that, without correction, this design will achieve a Strehl ratio greater than 0.85 for the entire energy and polarization ranges of the beamline. With a correction achieved by moving the focus 7.5 mm upstream, the minimum Strehl ratio is 0.99. This design is currently the baseline plan for all new ALS-U insertion device beamlines.

47 OTHER INSTRUMENTATION↗

Characterization and Application of Artificial Light Sources for Nighttime Aerosol Optical Depth Retrievals using the Visible Infrared Imager Radiometer Suite Day/Night Band

Using nighttime observations from Visible Infrared Imager Radiometer Suite (VIIRS) Day/Night band (DNB), the characteristics of artificial light sources are evaluated as functions of observation conditions, and incremental improvements are documented on nighttime aerosol retrievals using VIIRS DNB data on a regional scale. We find that the standard deviation of instantaneous radiance for a given artificial light source is strongly dependent upon the satellite viewing angle but is weakly dependent on lunar fraction and lunar angle. Retrieval of nighttime aerosol optical thickness (AOT) based on the novel use of these artificial light sources is demonstrated for three selected regions (United States, Middle East and India) during 2015. Reason-able agreement is found between nighttime AOTs from the VIIRS DNB and temporally adjacent daytime AOTs from the AErosol RObotic NETwork (AERONET) as well as from coincident nighttime AOT retrievals from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), indicating the potential of this method to begin filling critical gaps in diurnal AOT information at both regional and global scales. Issues related to cloud, snow and ice contamination during the winter season, as well as data loss due to the misclassification of thick aerosol plumes as clouds, must be addressed to make the algorithm operationally robust.

Jianglong Zhang↗

Light-Emitting Diodes and Cool White Fluorescent Light Similarly Suppress Pineal Gland Melatonin and Maintain Retinal Function and Morphology in the Rat

Currently, the light sources most commonly used in animal habitat lighting are cool white fluorescent or incandescent lamps. We evaluated a novel light-emitting diode (LED) light source for use in animal habitat lighting by comparing its effectiveness to cool white fluorescent light (CWF) in suppressing pineal gland melatonin and maintaining normal retinal physiology and morphology in the rat. Results of pineal melatonin suppression experiments showed equal suppression of pineal melatonin concentrations for LED light and CWF light at five different light illuminances (100, 40, 10, 1 and 0.1 lux). There were no significant differences in melatonin suppression between LED and CWF light when compared to unexposed controls. Retinal physiology was evaluated using electroretinography. Results show no differences in a-wave implicit times and amplitudes or b-wave implicit times and amplitudes between 100-lux LED-exposed rats and 100-lux CWF-exposed rats. Results of retinal histology assessment show no differences in retinal thickness rod outer segment length and number of rod nuclei between rats exposed to 100-lux LED and 100-lux CWF for days. Furthermore, the retinal pigmented epithelium and rod outer segments of all eyes observed were in good condition and of normal thickness. This study indicates that LED light does not cause retinal damage and can suppress pineal melatonin at similar intensities as a conventional CWF light source. These data suggest that LED light sources may be suitable replacements for conventional light sources used in the lighting of rodent vivariums while providing many mechanical and economical advantages.

Holley, Daniel C.↗