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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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NASA NTRS1986

Optical and transient capacitance study of EL2 in the absence and presence of other midgap levels

A high-resolution optical study was carried out on GaAs crystals grown by horizontal Bridgman and liquid-encapsulated-Czochralski methods. An excellent correlation was found between the intensity of the 1.039-eV no-phonon line and the characteristic absorption of EL2, the major deep donor level in GaAs. A correlation was also found between the characteristic optical absorption of EL2 and its concentration as determined by junction capacitance measurements. The presence of EL0, another midgap level contained in heavily oxygen-doped crystals at concentration always less than those of EL2, had no effect on the optical spectra, but altered the capacitance measurements. Accordingly, an accurate calibration for the determination of EL2 by optical absorption was obtained from capacitance measurements on crystals containing only EL2; in this way the uncertainties introduced by other midgap levels were eliminated.

Skowronski, M.↗
NASA NTRS1989

OTS 1809+314 and the gamma-ray burst GB 790325b

Deep CCD images of the field containing the recurring Optical Transient Source (OTS) 1809+314 recently discovered on archival plates of the Sonneberg Observatory are presented. At the position of OTS 1809+314 no optical counterpart brighter than V = 24.0-24.5, r(Gunn) = 22.0-22.5, and I = 22.0-22.5 is found. In the zero proper motion limit our observations place severe constraints on possible quiescent counterparts. There is no compelling evidence to suggest an association between the historical optical transient source and the gamma-ray burst GB 790325b located about 5 arcmin to the east of OTS 1809+314.

Hartmann, Dieter↗
NASA NTRS1999

An Unusual Supernova in the Error Box of the Gamma-Ray Burst of 25 April 1998

The discovery of afterglows associated with gamma-ray bursts at X-ray, optical and radio wavelengths and the measurement of the redshifts of some of these events has established that gamma-ray bursts lie at extreme distances, making them the most powerful photon-emitters known in the Universe. Here we report the discovery of transient optical emission in the error box of the gamma-ray burst GRB980425, the light curve of which was very different from that of previous optical afterglows associated with gamma-ray bursts. The optical transient is located in a spiral arm of the galaxy ESO 184-GS2, which has a redshift velocity of only 2,550 km/ s. Its optical spectrum and location indicate that it is a very luminous supernova, which has been identified as SN1998bw. If this supernova and GRB980425 are indeed associated, the energy radiated in gamma-rays is at least four orders of magnitude less than in other gamma-ray bursts, although its appearance was otherwise unremarkable: this indicates that very different mechanisms can give rise to gamma-ray bursts. But independent of this association, the supernova is itself unusual, exhibiting an unusual light curve at radio wavelengths that requires that the gas emitting the radio photons be expanding relativistically.

Galama , T. J.↗
DOE OSTI2024

Photodriven electron-transfer dynamics in a series of heteroleptic Cu(I)–anthraquinone dyads

Solar fuels catalysis is a promising route to efficiently harvesting, storing, and utilizing abundant solar energy. To achieve this promise, however, molecular systems must be designed with sustainable components that can balance numerous photophysical and chemical processes. To that end, here we report on the structural and photophysical characterization of a series of Cu(I)–anthraquinone-based electron donor–acceptor dyads. The dyads utilized a heteroleptic Cu(I) bis-diimine architecture with a copper(I) bis-phenanthroline chromophore donor and anthraquinone electron acceptor. We characterized the structures of the complexes using x-ray crystallography and density functional theory calculations and the photophysical properties via resonance Raman and optical transient absorption spectroscopy. The calculations and resonance Raman spectroscopy revealed that excitation of the Cu(I) metal-to-ligand charge-transfer (MLCT) transition transfers the electron to a delocalized ligand orbital. The optical transient absorption spectroscopy demonstrated that each dyad formed the oxidized copper–reduced anthraquinone charge-separated state. Unlike most Cu(I) bis-phenanthroline complexes where increasingly bulky substituents on the phenanthroline ligands lead to longer MLCT excited-state lifetimes, here, we observe a decrease in the long-lived charge-separated state lifetime with increasing steric bulk. The charge-separated state lifetimes were best explained in the context of electron-transfer theory rather than with the energy gap law, which is typical for MLCT excited states, despite the complete conjugation between the phenanthroline and anthraquinone moieties.

14 SOLAR ENERGY↗
NASA NTRSDate not supplied

Quality Assurance of ISS LIS lightning Data

Optical lighting detection from space has been ongoing since 1995 from the Optical Transient detector (1995-2000), then later by the Lightning Imaging Sensors (LIS) on the Tropical Rainfall Measuring Mission (TRMM) satellite (1997-2015) and the International Space Station (ISS) (ISS 2017-present). A rapid readout (2 ms) 128x128 pixel CCD (Charge-coupled Device) array detects optical transients from lightning (events) and transmits the observations to ground. Ground processing determines whether individual events are likely due to lightning or noise. Likely lightning events are then grouped into groups, flashes, and areas and their location on the earth are determined. The lightning data are saved in orbit files; each file containing the time, location, and intensity of the lightning events, groups, flashes, and areas detected during one orbit. Even after this processing anomalies may exist in some of the orbits. A manual quality assurance (QA) procedure is performed monthly to assess the data and omit orbits with obvious anomalies from the dataset. These files are not included in the final dataset that has undergone QA. The manual QA was developed during the OTD mission to identify artifacts that made it through ground processing algorithms. The manual QA process was continued for the TRMM and ISS LIS missions. Many anomalies have been identified and software updates now address many of them. However, some anomalies still occur in the processed datasets. The manual QA process examines the data for obvious issues in the lightning files that passed through the processing algorithms. These files are considered anomalous and are not included in the final QA dataset. Some issues that may cause an orbit to be considered anomalous include: obvious noise (excess events that make it through the processing), suspect geolocation, and excessive missing data packets. As an example, one way noise manifests is as “streaks” in lightning climatology plots. These streaks are especially apparent in low lightning rate regions (eg., over oceans). Since there is no method at present to extract these anomalies during processing, orbit files with significant anomalies are identified and removed from the final QA ISS LIS dataset. The final QA dataset can be obtained files from the Global Hydrometeorological Resource Center (GHRC). This presentation will provide examples of the various anomalies and examine how often the various anomalies occur and how much data is lost due to the omission of the anomalous orbits. Comparisons with OTD and TRMM LIS will also be examined.

ISS↗
DOE OSTI2020

The Zwicky Transient Facility Bright Transient Survey. II. A Public Statistical Sample for Exploring Supernova Demographics

Here we present a public catalog of transients from the Zwicky Transient Facility (ZTF) Bright Transient Survey, a magnitude-limited ( m < 19 mag in either the g or r filter) survey for extragalactic transients in the ZTF public stream. We introduce cuts on survey coverage, sky visibility around peak light, and other properties unconnected to the nature of the transient, and show that the resulting statistical sample is spectroscopically 97% complete at <18 mag, 93% complete at <18.5 mag, and 75% complete at <19 mag. We summarize the fundamental properties of this population, identifying distinct duration–luminosity correlations in a variety of supernova (SN) classes and associating the majority of fast optical transients with well-established spectroscopic SN types (primarily SN Ibn and II/IIb). We measure the Type Ia SN and core-collapse (CC) SN rates and luminosity functions, which show good consistency with recent work. About 7% of CC SNe explode in very low-luminosity galaxies ( M i > –16 mag), 10% in red-sequence galaxies, and 1% in massive ellipticals. We find no significant difference in the luminosity or color distributions between the host galaxies of SNe Type II and SNe Type Ib/c, suggesting that line-driven wind stripping does not play a major role in the loss of the hydrogen envelope from their progenitors. Future large-scale classification efforts with ZTF and other wide-area surveys will provide high-quality measurements of the rates, properties, and environments of all known types of optical transients and limits on the existence of theoretically predicted but as yet unobserved explosions.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2004

The GOES-R Lightning Mapper Sensor

The Lightning Mapper Sensor on GOES-R builds on previous measurements of lightning from low earth orbit by the OTD (Optical Transient Detector) and LIS (Lightning Imaging Sensor) sensors. Unlike observations from low earth orbit, the GOES-R platform will allow continuous monitoring of lightning activity over the Continental United States and southern Canada, Central and South America, and portions of the Atlantic and Pacific Oceans. The LMS will detect total (cloud-to-ground and intracloud) lightning at storm scale resolution (approx. 8 km) using a highly sensitive Charge Coupled Device (CCD) detector array. Discrimination between lightning optical transients and a bright sunlit background scene is accomplished by employing spectral, spatial, and temporal filtering along with a background subtraction technique. The result is 24 hour detection capability of total lightning. These total lightning observations can be made available to users within about 20 seconds. Research indicates a number of ways that total lightning observations from LMS could benefit operational activities, including 1) potential increases in lead times and reduced false alarms for severe thunderstorm and tornado Warnings, 2) improved routing of &rail around thunderstorms, 3) support for spacecraft launches and landings, 4) improved ability to monitor tropical cyclone intensity, 5) ability to monitor thunderstorm intensification/weakening during radar outages or where radar coverage is poor, 6) better identification of deep convection for the initialization of numerical prediction models, 7) improved forest fire forecasts, 8) identification of convective initiation, 9) identification of heavy convective snowfall, and 10) enhanced temporal resolution of storm evolution (1 minute) than is available from radar observations. Total lightning data has been used in an operational environment since July 2003 at the Huntsville, Alabama National Weather Service office. Total lightning measurements are obtained by the North Alabama Lightning Mapping Array (LMA) and have successfully been used in warning decisions. Every 2 minutes, total lightning counts in 2 km by 2 km horizontal, 1 km vertical grids are available to forecasters on an AWIPS (Advanced Weather Interactive Processing System) workstation. Experience with the LMA total lightning data is used to illustrate the potential use of LMS data that would be available to forecasters across the US. This abstract is for submission as a presentation to the National Weather Association Annual Meeting to be held 16-21 October 2004 in Portland, OR. This abstract will be published in the conference proceedings.

Buechler, Dennis↗
NASA NTRS2008

Pre-Launch Algorithms and Risk Reduction in Support of the Geostationary Lightning Mapper for GOES-R and Beyond

The Geostationary Lightning Mapper (GLM) is a single channel, near-IR optical transient event detector, used to detect, locate and measure total lightning activity over the full-disk as part of a 3-axis stabilized, geostationary weather satellite system. The next generation NOAA Geostationary Operational Environmental Satellite (GOES-R) series with a planned launch in 2014 will carry a GLM that will provide continuous day and night observations of lightning from the west coast of Africa (GOES-E) to New Zealand (GOES-W) when the constellation is fully operational.The mission objectives for the GLM are to 1) provide continuous,full-disk lightning measurements for storm warning and Nowcasting, 2) provide early warning of tornadic activity, and 3) accumulate a long-term database to track decadal changes of lightning. The GLM owes its heritage to the NASA Lightning Imaging Sensor (1997-Present) and the Optical Transient Detector (1995-2000), which were developed for the Earth Observing System and have produced a combined 13 year data record of global lightning activity. Instrument formulation studies were completed in March 2007 and the implementation phase to develop a prototype model and up to four flight units is expected to begin in latter part of the year. In parallel with the instrument development, a GOES-R Risk Reduction Team and Algorithm Working Group Lightning Applications Team have begun to develop the Level 2B algorithms and applications. Proxy total lightning data from the NASA Lightning Imaging Sensor on the Tropical Rainfall Measuring Mission (TRMM) sate]lite and regional test beds (e.g., Lightning Mapping Arrays in North Alabama and the Washington DC Metropolitan area) are being used to develop the pre-launch algorithms and applications, and also improve our knowledge of thunderstorm initiation and evolution. Real time lightning mapping data provided to selected National Weather Service forecast offices in Southern and Eastern Region are also improving our understanding of the application of these data in the severe storm warning process and help to accelerate the development of the pre-launch algorithms and Nowcasting applications. Abstract for the 3 rd Conference on Meteorological

Goodman, Steven↗
NASA NTRS2008

Pre-Launch Algorithms and Risk Reduction in Support of the Geostationary Lightning Mapper for GOES-R and Beyond

The Geostationary Lightning Mapper (GLM) is a single channel, near-IR optical transient event detector, used to detect, locate and measure total lightning activity over the full-disk as part of a 3-axis stabilized, geostationary weather satellite system. The next generation NOAA Geostationary Operational Environmental Satellite (GOES-R) series with a planned launch in 2014 will carry a GLM that will provide continuous day and night observations of lightning from the west coast of Africa (GOES-E) to New Zealand (GOES-W) when the constellation is fully operational. The mission objectives for the GLM are to 1) provide continuous,full-disk lightning measurements for storm warning and Nowcasting, 2) provide early warning of tornado activity, and 3) accumulate a long-term database to track decadal changes of lightning. The GLM owes its heritage to the NASA Lightning Imaging Sensor (1997-Present) and the Optical Transient Detector (1995-2000), which were developed for the Earth Observing System and have produced a combined 13 year data record of global lightning activity. Instrument formulation studies were completed in March 2007 and the implementation phase to develop a prototype model and up to four flight units is expected to begin in latter part of the year. In parallel with the instrument development, a GOES-R Risk Reduction Team and Algorithm Working Group Lightning Applications Team have begun to develop the Level 2B algorithms and applications. Proxy total lightning data from the NASA Lightning Imaging Sensor on the Tropical Rainfall Measuring Mission (TRMM) satellite and regional test beds (e.g., Lightning Mapping Arrays in North Alabama and the Washington DC Metropolitan area) are being used to develop the pre-launch algorithms and applications, and also improve our knowledge of thunderstorm initiation and evolution. Real time lightning mapping data provided to selected National Weather Service forecast offices in Southern and Eastern Region are also improving our understanding of the application of these data in the severe storm warning process and help to accelerate the development of the pre-launch algorithms and Nowcasting applications.

Goodman, Steven↗
DOE OSTI2024

Overview of the distributed image processing infrastructure to produce the Legacy Survey of Space and Time

The Vera C. Rubin Observatory is preparing to execute the most ambitious astronomical survey ever attempted, the Legacy Survey of Space and Time (LSST). Currently the final phase of construction is under way in the Chilean Andes, with the Observatory’s ten-year science mission scheduled to begin in 2025. Rubin’s 8.4-meter telescope will nightly scan the southern hemisphere collecting imagery in the wavelength range 320–1050 nm covering the entire observable sky every 4 nights using a 3.2 gigapixel camera, the largest imaging device ever built for astronomy. Automated detection and classification of celestial objects will be performed by sophisticated algorithms on high-resolution images to progressively produce an astronomical catalog eventually composed of 20 billion galaxies and 17 billion stars and their associated physical properties. In this article we present an overview of the system currently being constructed to perform data distribution as well as the annual campaigns which reprocess the entire image dataset collected since the beginning of the survey. These processing campaigns will utilize computing and storage resources provided by three Rubin data facilities (one in the US and two in Europe). Each year a Data Release will be produced and disseminated to science collaborations for use in studies comprising four main science pillars: probing dark matter and dark energy, taking inventory of solar system objects, exploring the transient optical sky and mapping the Milky Way. Also presented is the method by which we leverage some of the common tools and best practices used for management of large-scale distributed data processing projects in the high energy physics and astronomy communities. We also demonstrate how these tools and practices are utilized within the Rubin project in order to overcome the specific challenges faced by the Observatory.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

SN 2018ijp: the explosion of a stripped-envelope star within a dense H-rich shell?

In this work, we discuss the outcomes of the follow-up campaign of SN 2018ijp, discovered as part of the Zwicky Transient Facility survey for optical transients. Its first spectrum shows similarities to broad-lined Type Ic supernovae around maximum light, whereas later spectra display strong signatures of interaction between rapidly expanding ejecta and a dense H-rich circumstellar medium, coinciding with a second peak in the photometric evolution of the transient. This evolution, along with the results of modeling of the first light-curve peak, suggests a scenario where a stripped star exploded within a dense circumstellar medium. The two main phases in the evolution of the transient could be interpreted as a first phase dominated by radioactive decays, and a later interaction-dominated phase where the ejecta collide with a pre-existing shell. We therefore discuss SN 2018jp within the context of a massive star depleted of its outer layers exploding within a dense H-rich circumstellar medium.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Thermal transport in nanoporous holey silicon membranes investigated with optically induced transient thermal gratings

In this study, we use transient thermal gratings—a non-contact, laser-based thermal metrology technique with intrinsically high accuracy—to investigate room-temperature phonon-mediated thermal transport in two nanoporous holey silicon membranes with limiting dimensions of 120 nm and 250 nm, respectively. We compare the experimental results with ab initio calculations of phonon-mediated thermal transport according to the phonon Boltzmann transport equation (BTE) using two different computational techniques. We find that the calculations conducted within the Casimir framework, i.e., based on the BTE with the bulk phonon dispersion and diffuse scattering from surfaces, are in quantitative agreement with the experimental data and thus conclude that this framework is adequate for describing phonon-mediated thermal transport in silicon nanostructures with feature sizes of the order of 100 nm.

Duncan, Ryan A. (ORCID:0000000328318099)↗
NASA NTRS1984

The explosive transient camera (ETC) - An instrument for identification of gamma ray burst optical counterparts

The ETC is a wide-field (3-steradian) electronic camera array which can detect coincident optical flashes with durations of 0.1 to 100 sec. Each array element is a 20 x 30 deg FOV, cooled CCD detector. An optical transient (possibly associated with a gamma ray burst) as faint as B = +11 (1 sec duration) can be detected with an S/N of not less than 20, and its position determined to an accuracy of + or - 10 arcsec. Candidate events 1000 times fainter than the archived event (plate taken in 1928) reported for the November 19, 1978 gamma ray burst by Schaefer (1981) should be detectable in real time. A prototype camera was tested in April 1982 to establish sky background levels and spurious event rejection schemes; a 1/2-ster test version of the ETC was planned for operation in early 1984; expansion to the full 3-ster complement of 16 detectors at each of two sites was planned for the 1984-1985 period.

Ricker, G. R.↗
DOE OSTI2022

The Nascent Milliquasar VT J154843.06+220812.6: Tidal Disruption Event or Extreme Accretion State Change?

We present a detailed multiwavelength follow-up of the nuclear radio flare VT J154843.06+220812.6, hereafter VT J1548. VT J1548 was selected as a ~1 mJy radio flare in 3 GHz observations from the Very Large Array Sky Survey. It is located in the nucleus of a low-mass ($\mathrm{log}{M}_{\mathrm{BH}}/{M}_{\odot }\sim 6$) host galaxy with weak or no past active galactic nuclei (AGN) activity. VT J1548 is associated with a slow rising (multiple year), bright mid-IR flare in the Wide-field Infrared Survey Explorer survey, peaking at ~10%L edd. . No associated optical transient is detected, although we cannot rule out a short, early optical flare given the limited data available. Constant late-time (~3 yr post-flare) X-ray emission is detected at ~10 42 erg s –1 . The radio spectral energy distribution is consistent with synchrotron emission from an outflow incident on an asymmetric medium. A follow-up, optical spectrum shows transient, bright, high-ionization coronal line emission ([Fe xi] λ6375, [Fe xi] λ7894, [S xii] λ7612). Transient broad Hα is also detected but without corresponding broad Hβ emission, suggesting high nuclear extinction. We interpret this event as either a tidal disruption event or an extreme flare of an AGN, in both cases obscured by a dusty torus. Although these individual properties have been observed in previous transients, the combination is unprecedented. This event highlights the importance of searches across all wave bands for assembling a sample of nuclear flares that spans the range of observable properties and possible triggers.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

The host galaxies of 106 rapidly evolving transients discovered by the Dark Energy Survey

Rapidly evolving transients (RETs), also termed fast blue optical transients, are a recently discovered group of astrophysical events that display rapid luminosity evolution. RETs typically rise to peak in less than 10 d and fade within 30, a time-scale unlikely to be compatible with the decay of Nickel-56 that drives conventional supernovae (SNe). Their peak luminosity spans a range of -15 < Mg < -22.5, with some events observed at redshifts greater than 1. Their evolution on fast time-scales has hindered high-quality follow-up observations, and thus their origin and explosion/emission mechanism remains unexplained. In this paper, we present the largest sample of RETs to date, comprising 106 objects discovered by the Dark Energy Survey, and perform the most comprehensive analysis of RET host galaxies. Using deep-stacked photometry and emission lines from OzDES spectroscopy, we derive stellar masses and star formation rates (SFRs) for 49 host galaxies, and metallicities ([O/H]) for 37. Here, we find that RETs explode exclusively in star-forming galaxies and are thus likely associated with massive stars. Comparing RET hosts to samples of host galaxies of other explosive transients as well as field galaxies, we find that RETs prefer galaxies with high specific SFRs ($\langle$log(sSFR)$\rangle$ ~ -9.6), indicating a link to young stellar populations, similar to stripped-envelope SNe. RET hosts appear to show a lack of chemical enrichment, their metallicities akin to long-duration gamma-ray bursts and superluminous SN host galaxies ($\langle$12+ log (O/H)$\rangle$ ~ 9.4). There are no clear relationships between mass or SFR of the host galaxies and the peak magnitudes or decline rates of the transients themselves.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. In this paper, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron–phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron–phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Mapping the Ultrafast Mechanistic Pathways of Co Photocatalysts in Pure Water through Time‐Resolved X‐ray Spectroscopy

Abstract Nanosecond time‐resolved X‐ray (tr‐XAS) and optical transient absorption spectroscopy (OTA) are applied to study 3 multimolecular photocatalytic systems with [Ru(bpy) 3 ] 2+ photoabsorber, ascorbic acid electron donor and Co catalysts with methylene ( 1 ), hydroxomethylene ( 2 ) and methyl ( 3 ) amine substituents in pure water. OTA and tr‐XAS of 1 and 2 show that the favored catalytic pathway involves reductive quenching of the excited photosensitizer and electron transfer to the catalyst to form a Co II square pyramidal intermediate with a bonded aqua molecule followed by a Co I square planar derivative that decays within ≈8 μs. By contrast, a Co I square pyramidal intermediate with a longer decay lifetime of ≈35 μs is formed from an analogous Co II geometry for 3 in H 2 O. These results highlight the protonation of Co I to form the elusive hydride species to be the rate limiting step and show that the catalytic rate can be enhanced through hydrogen containing pendant amines that act as H−H bond formation proton relays.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Tracking the Light-Induced Excited-State Dynamics and Structural Configurations of an Extraordinarily Long-Lived Metastable State at Room Temperature

Time-resolved X-ray (Tr-XAS) and optical transient absorption (OTA) spectroscopy in the pico-microsecond time scale coupled with Density Functional theory calculations are applied to study the light-induced spin crossover processes of a Fe-based macrocyclic complex in solution. Tr-XAS analysis after light illumination shows the formation of a seven-coordinated high spin quintet metastable state which relaxes to a six-coordinated high spin configuration before decaying to ground state. Kinetic analysis of the macrocyclic complex reveals an unprecedented long-lived decay lifetime of ~42.6 µs. Comparative studies with a non-macrocyclic counterpart illustrate a significantly shortened ~568-old decay lifetime of ~75 ns, and highlight the importance of the ligand arrangement in stabilizing the reactivity of the excited state. Lastly, OTA analysis shows the seven-coordinated high spin state to be formed within ~6.2 ps. Finally, these findings provide a complete understanding of the spin crossover reaction and relaxation pathways of the macrocyclic complex, and reveal the importance of a flexible coordination environment for their rational design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗