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At least 1,765 records · Page 98
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Light-Driven Redox Activation of CO 2 - and H 2 -Activating Complexes in a Self-Assembled Triad

We report a self-assembled triad for artificial photosynthesis composed of a chromophore, carbon-dioxide reduction catalyst, and hydrogen oxidation complex, which is designed to operate without conventional sacrificial redox equivalents. Excitation of the zinc-porphyrin chromophore of the triad results in ultrafast charge transfer between a tungsten-alkylidyne donor and a rhenium diimine tricarbonyl acceptor, producing a charge-separated state that persists on the time scale of tens of nanoseconds and is thermodynamically capable of the primary dihydrogen and carbon dioxide binding steps for initiating the reverse water-gas shift reaction. The charge-transfer behavior of this system was probed using transient absorption spectroscopy in the visible, near-infrared, and mid-infrared spectral regions. Here, the behavior of the triad was compared with that of the zinc-porphyrin-rhenium-diimide dyad; the triad was found to have a significantly longer charge-separated lifetime than other previously reported porphyrin-rhenium diimine compounds.

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

Kinetic Control via Binding Sites within the Confined Space of Metal Metalloporphyrin‐Frameworks for Enhanced Shape‐Selectivity Catalysis

Abstract One striking feature of enzyme is its controllable ability to trap substrates via synergistic or cooperative binding in the enzymatic pocket, which renders the shape‐selectivity of product by the confined spatial environment. The success of shape‐selective catalysis relies on the ability of enzyme to tune the thermodynamics and kinetics for chemical reactions. In emulation of enzyme's ability, we showcase herein a targeting strategy with the substrate being anchored on the internal pore wall of metal‐organic frameworks (MOFs), taking full advantage of the sterically kinetic control to achieve shape‐selectivity for the reactions. For this purpose, a series of binding site‐accessible metal metalloporphyrin‐frameworks (MMPFs) have been investigated to shed light on the nature of enzyme‐mimic catalysis. They exhibit a different density of binding sites that are well arranged into the nanospace with corresponding distances of opposite binding sites. Such a structural specificity results in a facile switch in selectivity from an exclusive formation of the thermodynamically stable product to the kinetic product. Thus, the proposed targeting strategy, based on the combination of porous materials and binding events, paves a new way to develop highly efficient heterogeneous catalysts for shifting selectivity.

Zhang, Weijie↗
DOE OSTI2020

Degradation of impact toughness in cast stainless steels during long-term thermal aging

Cast austenitic stainless steels (CASSs) have been extensively used for the large components of nuclear reactor primary coolant systems. Since the cast steels inevitably contain degradable metastable phases and replacement of the large coolant system components is impractical, the thermal embrittlement of CASS components has been a serious concern in the extended-term operation of nuclear power plants. This study aimed to systematically measure and analyze the effect of long-term thermal aging on the Charpy impact toughness to provide a comprehensive understanding of thermal degradation behavior and a practical aging model to predict the degree of thermal degradation in the cast stainless steels. Additionally, the materials tested in the research include eight CASS alloys (two CF3s, one CF3M, three CF8s, and two CF8Ms) and two reference wrought materials (304L and 316L), in which the nominal δ-ferrite content ranges from ~2% to 33%. These stainless steels have been thermally aged at two light water reactor (LWR) temperatures (290 and 330 °C) and at two accelerated-aging temperatures (360 and 400 °C) for up to 30,000 h; these include both under-aged and over-aged conditions relative to the extended service lifetime (80 years). Charpy impact testing was performed for aged and non-aged specimens, and the impact (absorbed) energy parameters were correlated with a new aging parameter (A). Both the reduction of impact fracture toughness and the shift of ductile-brittle transition temperature were strongly dependent on the δ-ferrite content and degree of thermal aging. A linear relationship was found between the increasing rate of the index transition temperature T 41J and aging parameter A; base on which an empirical model was proposed for prediction of the transition temperature as a simple function of the aging parameter (A) and δ-ferrite content (F). Finally, the critical aging parameter for embrittlement (AC) was evaluated and compared with the existing δ-ferrite content criteria.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Ultrafast narrowband exciton routing within layered perovskite nanoplatelets enables low-loss luminescent solar concentrators

In luminescent solar concentrator (LSC) systems, broadband solar energy is absorbed, down-converted and waveguided to the panel edges where peripheral photovoltaic cells convert the concentrated light to electricity. Achieving a low-loss LSC requires reducing the reabsorption of emitted light within the absorbing medium while maintaining high photoluminescence quantum yield (PLQY). Here we employ layered hybrid metal halide perovskites—ensembles of two-dimensional perovskite domains—to fabricate low-loss large-area LSCs that fulfil this requirement. Here, we devised a facile synthetic route to obtain layered perovskite nanoplatelets (PNPLs) that possess a tunable number of layers within each platelet. Efficient ultrafast non-radiative exciton routing within each PNPL (0.1 ps –1 ) produces a large Stokes shift and a high PLQY simultaneously. Using this approach, we achieve an optical quantum efficiency of 26% and an internal concentration factor of 3.3 for LSCs with an area of 10 × 10 cm 2 , which represents a fourfold enhancement over the best previously reported perovskite LSCs.

42 ENGINEERING↗
DOE OSTI2025

Cobalt promotion of the InO x –TiO 2 heterojunction for dual photothermal reduction of CO 2

A series of cobalt-promoted indium–titanium composite oxides was synthesized using a microemulsion method. Their functional properties were investigated for the photothermal reduction of carbon dioxide. In this series, the indium content varied between 2.5 and 20%, while the cobalt percentage was kept constant at 4% throughout the series. In all cases, carbon monoxide formation occurred selectively through the reverse water gas shift reaction. The sample with 2.5% In maximized the synergistic use of the two energy sources, while the sample with 10% In showed the highest catalytic activity under both thermal and dual photo-thermo conditions. A physicochemical characterization was performed for all samples. The use of microscopy and X-ray absorption spectroscopy demonstrated that sub-nanometric indium entities, in combination with atomically dispersed cobalt oxide entities, achieved a balance between high thermal activity and significant synergy between light and heat in a catalytic process. The system with 10% indium is thus able to improve the thermal catalytic process through the use of light, providing an intensification procedure for the classic process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Illumination angle and layer thickness influence on the photo current generation in organic solar cells: A combined simulative and experimental study

In most future organic photovoltaic applications, such as fixed roof installations, facade or clothing integration, the solar cells will face the sun under varying angles. By a combined simulative and experimental study, we investigate the mutual interdependencies of the angle of light incidence, the absorber layer thickness and the photon harvesting efficiency within a typical organic photovoltaic device. For thin absorber layers, we find a steady decrease of the effective photocurrent towards increasing angles. For 90-140 nm thick absorber layers, however, we observe an effective photocurrent enhancement, exhibiting a maximum yield at angles of incidence of about 50°. Both effects mainly originate from the angle-dependent spatial broadening of the optical interference pattern inside the solar cell and a shift of the absorption maximum away from the metal electrode.

14 SOLAR ENERGY↗
DOE OSTI2016

Study of structural and optical properties of ZnAlQ{sub 5} (zinc aluminum quinolate) organic phosphor for OLED applications

The various composition of ZnAlQ{sub 5} such as Zn{sub 1.5}A{sub 10.5}Q{sub 5}, Zn{sub 1}Al{sub 1}Q{sub 5}, Zn{sub 0.5}Al{sub 1.5}Q{sub 5} organic phosphors were prepared via simple cost effective co-precipitation method. The FTIR, SEM, photoluminescence analysis of the prepared phosphors were reported. ZnQ{sub 2} and AlQ{sub 3} were also prepared by similar method and their properties were compared with different composition of ZnAlQ{sub 5}. The structural elucidation in the form of stretching frequencies of chemical bonds of the prepared phosphor was carried out using Fourier Transform Infrared Spectroscopy (FTIR). The stretching frequency analysis confirms the formation of prepared phosphor materials. The SEM analysis shows the surface morphological behavior of prepared phosphor materials. Greenish photoluminescence were observed at 505 to 510 nm for the different composition of ZnAlQ{sub 5},in which Zn{sub 1.5}Al{sub 0.5}Q{sub 5} shows maximum luminescence intensity at 505 nm. PL emission of ZnQ{sub 2} was observed at 515 nm, while for AlQ{sub 3} at 520 nm. The blue shift of 10 nm was observed in Zn{sub 1.5}A{sub 10.5}Q{sub 5} due to modification of energy level due to presence of Zn{sup 2+} and Al{sup 3+}. The enhancement in PL intensity was observed in Zn{sub 1.5}A{sub 10.5}Q{sub 5} compared to the other composition due to transfer of energy between Zn{sup 2+} and quinolate complex. Optical properties of the prepared materials were evaluated for possible applications in organic light emitting devices (OLED).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Probing ultrafast C–Br bond fission in the UV photochemistry of bromoform with core-to-valence transient absorption spectroscopy

UV pump–extreme UV (XUV) probe femtosecond transient absorption spectroscopy is used to study the 268 nm induced photodissociation dynamics of bromoform (CHBr3). Core-to-valence transitions at the Br(3d) absorption edge (∼70 eV) provide an atomic scale perspective of the reaction, sensitive to changes in the local valence electronic structure, with ultrafast time resolution. The XUV spectra track how the singly occupied molecular orbitals of transient electronic states develop throughout the C–Br bond fission, eventually forming radical Br and CHBr2 products. Complementary ab initio calculations of XUV spectral fingerprints are performed for transient atomic arrangements obtained from sampling excited-state molecular dynamics simulations. C–Br fission along an approximately CS symmetrical reaction pathway leads to a continuous change of electronic orbital characters and atomic arrangements. Two timescales dominate changes in the transient absorption spectra, reflecting the different characteristic motions of the light C and H atoms and the heavy Br atoms. Within the first 40 fs, distortion from C3v symmetry to form a quasiplanar CHBr2 by the displacement of the (light) CH moiety causes significant changes to the valence electronic structure. Displacement of the (heavy) Br atoms is delayed and requires up to ∼300 fs to form separate Br + CHBr2 products. We demonstrate that transitions between the valence-excited (initial) and valence + core-excited (final) state electronic configurations produced by XUV absorption are sensitive to the localization of valence orbitals during bond fission. The change in valence electron-core hole interaction provides a physical explanation for spectral shifts during the process of bond cleavage.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Temperature effects on the nanoscale thermoelastic response of a SiO2 membrane

We crossed two femtosecond extreme ultraviolet (EUV) pulses on a 100 nm thick amorphous membrane of SiO2, generating transient gratings (TGs) of light intensity with 84 nm spatial periodicity. The EUV TG excitation gave rise to the efficient generation of Lamb waves (LWs) and of a temperature grating, whose dynamics was studied at two different initial sample temperatures, 50 and 300 K. The short penetration depth of the EUV excitation pulses turned into a strong non-uniformity in the actual temperature as a function of the depth from the sample surface. At the lowest temperature, the LW frequencies presented a sizable shift in time due to the thermal equilibration along the membrane thickness. The analysis of the EUV TG waveforms allowed us to determine the decay time of the thermal grating and the sound attenuation coefficient, both found in reasonable agreement with the literature. The results show how EUV TG can provide information of non-equilibrium thermoelastic dynamics in thin membranes transparent to optical radiation.

Materials Science↗
DOE OSTI2019

Spatiotemporal light control with active metasurfaces

Optical metasurfaces have provided us with extraordinary ways to control light by spatially structuring materials. The space-time duality in Maxwell’s equations suggests that additional structuring of metasurfaces in the time domain can even further expand their impact on the field of optics. Advances toward this goal critically rely on the development of new materials and nanostructures that exhibit very large and fast changes in their optical properties in response to external stimuli. New physics is also emerging as ultrafast tuning of metasurfaces is becoming possible, including wavelength shifts that emulate the Doppler effect, Lorentz nonreciprocity, time-reversed optical behavior, and negative refraction. The large-scale manufacturing of dynamic flat optics has the potential to revolutionize many emerging technologies that require active wavefront shaping with lightweight, compact, and power-efficient components.

Science & Technology - Other Topics↗
DOE OSTI2021

Genome-Wide Transcription Factor DNA Binding Sites and Gene Regulatory Networks in Clostridium thermocellum

Clostridium thermocellum is a thermophilic bacterium recognized for its natural ability to effectively deconstruct cellulosic biomass. While there is a large body of studies on the genetic engineering of this bacterium and its physiology to-date, there is limited knowledge in the transcriptional regulation in this organism and thermophilic bacteria in general. The study herein is the first report of a large-scale application of DNA-affinity purification sequencing (DAP-seq) to transcription factors (TFs) from a bacterium. We applied DAP-seq to > 90 TFs in C. thermocellum and detected genome-wide binding sites for 11 of them. We then compiled and aligned DNA binding sequences from these TFs to deduce the primary DNA-binding sequence motifs for each TF. These binding motifs are further validated with electrophoretic mobility shift assay (EMSA) and are used to identify individual TFs’ regulatory targets in C. thermocellum . Our results led to the discovery of novel, uncharacterized TFs as well as homologues of previously studied TFs including RexA-, LexA-, and LacI-type TFs. We then used these data to reconstruct gene regulatory networks for the 11 TFs individually, which resulted in a global network encompassing the TFs with some interconnections. As gene regulation governs and constrains how bacteria behave, our findings shed light on the roles of TFs delineated by their regulons, and potentially provides a means to enable rational, advanced genetic engineering of C. thermocellum and other organisms alike toward a desired phenotype.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Genome-wide Transcription Factor DNA Binding Sites and Gene Regulatory Networks in Clostridium thermocellum

Clostridium thermocellum is a thermophilic bacterium recognized for its natural ability to effectively deconstruct cellulosic biomass. While there is a large body of studies on the genetic engineering of this bacterium and its physiology to-date, there is limited knowledge in the transcriptional regulation in this organism and thermophilic bacteria in general. The study herein is the first report of a high-throughput application of DNA-affinity purification sequencing (DAP-seq) to transcription factors (TFs) from a thermophile. We applied DAP-seq to >90 TFs in C. thermocellum and detected genome-wide binding sites for 11 of them. We then compiled and aligned DNA binding sequences from these TFs to deduce the primary DNA-binding sequence motifs for each TF. These binding motifs are further validated with electrophoretic mobility shift assay (EMSA) and are used to identify individual TFs’ regulatory targets in C. thermocellum. Our results led to the discovery of novel, uncharacterized TFs as well as homologues of previously studied TFs including RexA-, LexA- and LacI-type TFs. We then used these data to reconstruct gene regulatory networks for the 11 TFs individually, which resulted in a global network encompassing the TFs with some interconnections. As gene regulation governs and constrains how bacteria behave, our findings shed light on the roles of TFs delineated by their regulons, and potentially provides a means to enable rational, advanced genetic engineering of C. thermocellum and other organisms alike towards a desired phenotype.

09 BIOMASS FUELS↗
NASA NTRS1980

Single-mode laser studies: Design and performance of a fixed-wave length source and coupling of lasers to thin-film optical waveguides

A module developed for the generation of a stable single wavelength to be used for a fiber optic multiplexing scheme is described. The laser is driven with RZ pulses, and the temperature is stabilized thermoelectrically. The unit is capable of maintaining a fixed wavelength within about 6 A as the pulse duty cycle is changed between 0 and 100 percent. This is considered the most severe case, and much tighter tolerances are obtainable for constant input power coding schemes. Using a constricted double heterostructure laser, a wavelength shift of 0.083 A mA is obtained due to laser self-heating by a dc driving current. The thermoelectric unit is capable of maintaining a constant laser heat-sink temperature within 0.02 C. In addition, miniature lenses and couplers are described which allow efficient coupling of single wavelength modes of junction lasers to thin film optical waveguides. The design of the miniature cylinder lenses and the prism coupling techniques allow 2 mW of single wavelength mode junction laser light to b coupled into thin film waveguides using compact assemblies. Selective grating couplers are also studied.

Ladany, I.↗
NASA NTRS1993

Further ROSAT measurements of the period of 4U 1820-30

We have made two new observations of 4U 1820-30 with the ROSAT position sensitive proportional counter (PSPC). The measurements do not provide further evidence for a secular period decrease of this source. Instead, after inclusion of our new arrival time measurements the significance of the orbital period derivative drops (from 5.5 to 4.6 sigma), its best-fit value decreases (to P-dot/P =(-5.3 +/- 1.1) x 10(exp -8)/yr) and the formal probability that statistical fluctuations have caused the observed P-dot increases to 0.5% (from 0.003%). We detect light curve changes that are large enough to be the cause of some (or all) of the period changes seen in 4U 1820-30, but not large enough to explain the discrepancy of the observed period derivative with that theoretically predicted. We explore the possibility that the secular period change observed during 1976-1991 could have been dominated by random or systematic changes in the position and shape of an occulting bulge on the disk rim and conclude that phase shifts caused by this mechanism could in principle explain the discrepancy entirely.

Klis, M. Van Der↗
NASA NTRS2018

Hawkeye Ocean Color Instrument – Performance Summary

Hawkeye is an ocean color instrument that is part of the SeaHawk satellite developed for SOCON, the Sustained Ocean Color Observations using Nanosatellites program funded by the Gordon and Betty Moore Foundation and managed by the University of North Carolina – Wilmington (UNC-W). HawkEye has spectral characteristics similar to SeaWiFS, but with 8 times finer resolution and a smaller field of view more appropriate for lakes, rivers, and near-shore terrestrial environments. With a volume of only 10 X 10 X 10 cm (a CubeSat 1U), it can produce 8 bands of image data in a single pass, each with 1800 x 6000 pixels, with a resolution of 120 meters per pixel. This paper will present a short summary of instrument design, the spacecraft interface, and “lessons learned” during this effort. Scientists considering using linear arrays in a pushbroom mode for remote sensing will find this useful. Much of the discussion will center on optical performance, such as flat field calibration, polarization effects, stray light, out-of-band response, and exposure linearity. Images from field tests will be shown.The Hawkeye instrument is an ocean color measuring instrument designed to fly on the SeaHawk satellite developed for SOCON, the Sustained Ocean Color Observations using Nanosatellites program funded by the Gordon and Betty Moore Foundation and managed by the University of North Carolina – Wilmington (UNC-W). The Hawkeye instrument measures ocean color in 8 spectral bands, similar to SeaWiFS, except Band 7, which is shifted to a slightly lower wavelength to avoid the oxygen absorption feature that a wider band overlapped on SeaWiFS. The instrument is approximately 1/3rd the volume of the entire satellite, which is a 3U Cubesat manufactured by Clydespace in Glasgow, Scotland. The purpose of this instrument is to ascertain the quality of ocean color data possible with such a small, inexpensive instrument and bus. The nominal orbit is 540 km, and the nominal pixel geometric instantaneous field of view (GIFOV) 120 meters on a side. Each band will produce an image 1800 x 6000 pixels in size, for a total field of view of 216 X 720 km.2) DESIGN CONCEPTThe Hawkeye instrument uses linear arrays in pushbroom mode to collect data over a two dimensional area. The instrument has 4 linear CCD arrays, the Onsemi KLI-4104, to collect the 8 bands of data. Figure 1 illustrates the optical design for two bands, sharing a single array.

Hawkeye↗
DOE OSTI2020

Quantifying Uncertainties In Neutron-Alpha Scattering With Chiral Nucleon-Nucleon And Three-Nucleon Forces

We report that modern ab initio theory combined with high-quality nucleon-nucleon (NN) and three-nucleon (3N) interactions from chiral effective field theory (EFT) can provide a predictive description of low-energy light-nuclei reactions relevant for astrophysics and fusion-energy applications. However, the high cost of computations has so far impeded a complete analysis of the uncertainty budget of such calculations. Starting from NN potentials up to fifth order (N 4 LO) combined with leading-order 3N forces, we study how the order-by-order convergence of the chiral expansion and confidence intervals for the 3N contact and contact-plus-one-pion-exchange low-energy constants (c E and c D ) contribute to the overall uncertainty budget of many-body calculations of neutron- 4 He (n-α) elastic scattering. We compute structure and reaction observables for three-, four-, and five-nucleon systems within the ab initio frameworks of the no-core shell model and no-core shell model with continuum. Using a small set of design runs, we construct a Gaussian process model (GPM) that acts as a statistical emulator for the theory. With this, we gain insight into how uncertainties in the 3N low-energy constants propagate throughout the calculation and determine the Bayesian posterior distribution of these parameters with Markov-Chain Monte Carlo. We find rapidly converging n-α phase shifts with respect to the chiral order. With the adopted leading-order 3N force, calculations based on the NN interaction at N 4 LO of Entem, Machleidt, and Nosyk are unable to reproduce the experimental phase shifts in the 3/2 - channel within the estimated chiral truncation errors. Closer agreement with empirical data is found when using an older parametrization of the NN interaction at order N 3 LO, and the position and width of the P-wave resonances can be used to reduce the uncertainty of the 3N low-energy constants. The present results point to a lack of spin-orbit strength when the newer parametrization of the chiral NN force up to fifth order is combined with the leading-order 3N force. The inclusion of higher-order 3N-force terms may be required to recover the missing strength. GPMs can act as fast and accurate emulators of ab initio many-body calculations of low-energy scattering and reactions of light nuclei, opening the way to a robust quantification of theoretical uncertainties grounded in the description of the underlying chiral Hamiltonian.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI1989

Nuclear Safety [Vol. 30, No. 1, January-March 1989]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 International Conference on Thermal Reactor Safety: NUCSAFE 88 by A. P. Malinauskas and J. G. Pruett; ACCIDENT ANALYSIS: 18 Chernobyl Today: State of Research by A. Yu. Gagarinskii; CONTROL AND INSTRUMENTATION: 23 Problems Associated with Routine In-Plant Radioactive Effluent Monitoring Systems at U.S. Light-Water Reactors by Barry G. Wahlig, David M. Walker, Mahmoud R. Ghavi, and John M. Palms; DESIGN FEATURES: 34 Twentieth DOE/NRC Nuclear Air-Cleaning Conference by R. R. Bellamy, D. W. Moeller, and M. W. First, 46 Design Options for the Core Support Structure for Liquid-Metal-Cooled Reactor Plants by J. P. Burelbach, W. J. Kann, J. G. Saiveau, and R. W. Seidensticker; ENVIRONMENTAL EFFECTS: 53 The Radiological Consequences of the Chernobyl Accident by L. V. Konstantinov and A. J. González; WASTE AND SPENT FUEL MANAGEMENT: 70 Activities Related to Waste Management Compiled by E. G. Silver; OPERATING EXPERIENCES: 80 Fuel Performance Annual Report for 1986 by W. J. Bailey, 103 Safety Considerations Related to 12-Hour Shift Schedules by S. Gould, 105 Reactor Shutdown Experience Compiled by J. W. Cletcher, 108 Operating U.S. Power Reactors Compiled by E. G. Silver; RECENT DEVELOPMENTS: 130 General Administrative Activities Compiled by E. G. Silver, 140 Reports, Standards, and Safety Guides by D. S. Queener, 145 Status of Power-Reactor Licensing Activities Compiled by E. G. Silver, 153 Proposed Rule Changes as of Sept. 30, 1988; ANNOUNCEMENTS: 69 Northwestern University Short Course on Radiation Safety, 79 International Seminar on Fission Product Transport Processes in Reactor Accidents, 129 Harvard School of Public Health Offers Short Courses, 152 MIT Offers Summer Short Courses on Reactor Safety and Nodal Analysis, 152 Seminar on Use of PCs in Probabilistic Safety Analysis, 157 The Authors, 160 Indexes to Nuclear Safety, Volume 29.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Engineering of B800 bacteriochlorophyll binding site specificity in the Rhodobacter sphaeroides LH2 antenna

The light-harvesting 2 complex (LH2) of the purple phototrophic bacterium Rhodobacter sphaeroides is a highly efficient, light-harvesting antenna that allows growth under a wide-range of light intensities. In order to expand the spectral range of this antenna complex, we first used a series of competition assays to measure the capacity of the non-native pigments 3-acetyl chlorophyll (Chl) a , Chl d , Chl f or bacteriochlorophyll (BChl) b to replace native BChl a in the B800 binding site of LH2. We then adjusted the B800 site and systematically assessed the binding of non-native pigments. We find that Arg –10 of the LH2 β polypeptide plays a crucial role in binding specificity, by providing a hydrogen-bond to the 3-acetyl group of native and non-native pigments. Reconstituted LH2 complexes harbouring the series of (B)Chls were examined by transient absorption and steady-state fluorescence spectroscopies. Although slowed 10-fold to ~6 ps, energy transfer from Chl a to B850 BChl a remained highly efficient. We measured faster energy-transfer time constants for Chl d (3.5 ps) and Chl f (2.7 ps), which have red-shifted absorption maxima compared to Chl a . BChl b , red-shifted from the native BChl a , gave extremely rapid (≤0.1 ps) transfer. These results show that modified LH2 complexes, combined with engineered (B)Chl biosynthesis pathways in vivo , have potential for retaining high efficiency whilst acquiring increased spectral range.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗