| 1. |
- Zhai, Panlong, et al.
(author)
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Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting
- 2021
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In: Nature Communications. - : Springer Nature. - 2041-1723. ; 12:1
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Journal article (peer-reviewed)abstract
- Rational design of single atom catalyst is critical for efficient sustainable energy conversion. However, the atomic-level control of active sites is essential for electrocatalytic materials in alkaline electrolyte. Moreover, well-defined surface structures lead to in-depth understanding of catalytic mechanisms. Herein, we report a single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets (Ru-1/D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru-1/D-NiFe LDH delivers an ultralow overpotential of 18mV at 10mAcm(-2) for hydrogen evolution reaction, surpassing the commercial Pt/C catalyst. Density functional theory calculations reveal that Ru-1/D-NiFe LDH optimizes the adsorption energies of intermediates for hydrogen evolution reaction and promotes the O-O coupling at a Ru-O active site for oxygen evolution reaction. The Ru-1/D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts. Rational design of single atom catalyst is critical for efficient sustainable energy conversion. Single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets achieve superior HER and OER performance in alkaline media.
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| 2. |
- Zhang, Yanting, et al.
(author)
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Two-Dimensional Defective Boron-Doped Niobic Acid Nanosheets for Robust Nitrogen Photofixation
- 2021
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In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:11, s. 17820-17830
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Journal article (peer-reviewed)abstract
- Direct nitrogen photofixation is a feasible solution toward sustainable production of ammonia under mild conditions. However, the generation of active sites for solar-dirven nitrogen fixation not only limits the fundamental understanding of the relationship among light absorption, charge transfer, and catalytic efficiency but also influences the photocatalytic activity. Herein, we report two-dimensional boron-doped niobic acid nanosheets with oxygen vacancies (B-V-o-HNbO3 NSs) for efficient N-2 photofixation in the absence of any scavengers and cocatalysts. Impressively, B-V-o-HNbO3 NS as a model catalyst achieves the enhanced ammonia evolution rate of 170 mu mol g(cat)(-1) h(-1) in pure water under visible-light irradiation. The doublet coupling representing (NH4+)-N-15 in an isotopic labeling experiment and in situ infrared spectra confirm the reliable ammonia generation. The experimental analysis and density functional theory (DFT) calculations indicate that the strong synergy of boron dopant and oxygen vacancy regulates band structure of niobic acid, facilitates photogenerated charge transfer, reduces free energy barriers, accelerates reaction kinetics, and promotes the high rates of ammonia evolution. This work provides a general strategy to design active photocatalysts toward solar N-2 conversion.
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| 3. |
- Kristan, Matej, et al.
(author)
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The Visual Object Tracking VOT2015 challenge results
- 2015
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In: Proceedings 2015 IEEE International Conference on Computer Vision Workshops ICCVW 2015. - : IEEE. - 9780769557205 ; , s. 564-586
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Conference paper (peer-reviewed)abstract
- The Visual Object Tracking challenge 2015, VOT2015, aims at comparing short-term single-object visual trackers that do not apply pre-learned models of object appearance. Results of 62 trackers are presented. The number of tested trackers makes VOT 2015 the largest benchmark on short-term tracking to date. For each participating tracker, a short description is provided in the appendix. Features of the VOT2015 challenge that go beyond its VOT2014 predecessor are: (i) a new VOT2015 dataset twice as large as in VOT2014 with full annotation of targets by rotated bounding boxes and per-frame attribute, (ii) extensions of the VOT2014 evaluation methodology by introduction of a new performance measure. The dataset, the evaluation kit as well as the results are publicly available at the challenge website(1).
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| 4. |
- Kristan, Matej, et al.
(author)
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The Visual Object Tracking VOT2016 Challenge Results
- 2016
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In: COMPUTER VISION - ECCV 2016 WORKSHOPS, PT II. - Cham : SPRINGER INT PUBLISHING AG. - 9783319488813 - 9783319488806 ; , s. 777-823
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Conference paper (peer-reviewed)abstract
- The Visual Object Tracking challenge VOT2016 aims at comparing short-term single-object visual trackers that do not apply pre-learned models of object appearance. Results of 70 trackers are presented, with a large number of trackers being published at major computer vision conferences and journals in the recent years. The number of tested state-of-the-art trackers makes the VOT 2016 the largest and most challenging benchmark on short-term tracking to date. For each participating tracker, a short description is provided in the Appendix. The VOT2016 goes beyond its predecessors by (i) introducing a new semi-automatic ground truth bounding box annotation methodology and (ii) extending the evaluation system with the no-reset experiment.
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| 5. |
- Chi, Chaodan, et al.
(author)
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Si-based InGaAs photodetectors on heterogeneous integrated substrate
- 2021
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In: Science China: Physics, Mechanics and Astronomy. - : Springer Science and Business Media LLC. - 1674-7348 .- 1869-1927. ; 64:6
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Journal article (peer-reviewed)abstract
- In this paper, InGaAs p-i-n photodetectors (PDs) on an InP/SiO2/Si (InPOI) substrate fabricated by ion-slicing technology are demonstrated and compared with the identical device on a commercial InP substrate. The quality of epitaxial layers on the InPOI substrate is similar to that on the InP substrate. The photo responsivities of both devices measured at 1.55 µm are comparable, which are about 0.808–0.828 A W−1. Although the dark current of PD on the InPOI substrate is twice as high as that of PD on the InP substrate at 300 K, the peak detectivities of both PDs are comparable. In general, the overall performance of the InPOI-based PD is comparable to the InP-based PD, demonstrating that the ion-slicing technology is a promising route to enable the high-quality Si-based InP platform for the full photonic integration on a Si substrate.
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| 6. |
- Yu, ChaoQing, et al.
(author)
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Managing nitrogen to restore water quality in China
- 2019
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In: Nature. - : Nature Publishing Group. - 0028-0836 .- 1476-4687. ; 567:7749, s. 516-520
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Journal article (peer-reviewed)abstract
- The nitrogen cycle has been radically changed by human activities(1). China consumes nearly one third of the world's nitrogen fertilizers. The excessive application of fertilizers(2,3) and increased nitrogen discharge from livestock, domestic and industrial sources have resulted in pervasive water pollution. Quantifying a nitrogen 'boundary'(4) in heterogeneous environments is important for the effective management of local water quality. Here we use a combination of water-quality observations and simulated nitrogen discharge from agricultural and other sources to estimate spatial patterns of nitrogen discharge into water bodies across China from 1955 to 2014. We find that the critical surface-water quality standard (1.0 milligrams of nitrogen per litre) was being exceeded in most provinces by the mid-1980s, and that current rates of anthropogenic nitrogen discharge (14.5 +/- 3.1 megatonnes of nitrogen per year) to fresh water are about 2.7 times the estimated 'safe' nitrogen discharge threshold (5.2 +/- 0.7 megatonnes of nitrogen per year). Current efforts to reduce pollution through wastewater treatment and by improving cropland nitrogen management can partially remedy this situation. Domestic wastewater treatment has helped to reduce net discharge by 0.7 +/- 0.1 megatonnes in 2014, but at high monetary and energy costs. Improved cropland nitrogen management could remove another 2.3 +/- 0.3 megatonnes of nitrogen per year-about 25 per cent of the excess discharge to fresh water. Successfully restoring a clean water environment in China will further require transformational changes to boost the national nutrient recycling rate from its current average of 36 per cent to about 87 per cent, which is a level typical of traditional Chinese agriculture. Although ambitious, such a high level of nitrogen recycling is technologically achievable at an estimated capital cost of approximately 100 billion US dollars and operating costs of 18-29 billion US dollars per year, and could provide co-benefits such as recycled wastewater for crop irrigation and improved environmental quality and ecosystem services.
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| 7. |
- Zhang, Xiaomeng, et al.
(author)
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Engineering Single-Atomic Ni-N-4-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting
- 2021
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 143:49, s. 20657-20669
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Journal article (peer-reviewed)abstract
- Direct photoelectrochemical (PEC) water splitting is a promising solution for solar energy conversion; however, there is a pressing bottleneck to address the intrinsic charge transport for the enhancement of PEC performance. Herein, a versatile coupling strategy was developed to engineer atomically dispersed Ni-N-4 sites coordinated with an axial direction oxygen atom (Ni-N-4-O) incorporated between oxygen evolution cocatalyst (OEC) and semiconductor photoanode, boosting the photogenerated electron-hole separation and thus improving PEC activity. This state-ofthe-art OEC/Ni-N-4-O/BiVO4 photoanode exhibits a record high photo-current density of 6.0 mA cm(-2) at 1.23 V versus reversible hydrogen electrode (vs RHE), over approximately 3.97 times larger than that of BiVO4, achieving outstanding long-term photostability. From X- ray absorption fine structure analysis and density functional theory calculations, the enhanced PEC performance is attributed to the construction of single-atomic Ni-N-4-O moiety in OEC/BiVO4, facilitating the holes transfer, decreasing the free energy barriers, and accelerating the reaction kinetics. This work enables us to develop an effective pathway to design and fabricate efficient and stable photoanodes for feasible PEC water splitting application.
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| 8. |
- Du, Mengqi, et al.
(author)
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High-resolution wavefront sensing and aberration analysis of multi-spectral extreme ultraviolet beams
- 2023
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In: Optica. - : Optica Publishing Group. - 2334-2536. ; 10:2, s. 255-263
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Journal article (peer-reviewed)abstract
- Coherent multi-spectral extreme ultraviolet beams have great potential for providing high spatial and temporal resolution for microscopy and spectroscopy applications. But due to the limitations of short-wavelength optics and the broad bandwidth, it remains a challenge to perform quantitative, high-resolution beam characterization. Here we present a wavefront sensing solution based on multiplexed ptychography, with which we show spectrally resolved, high-resolution beam reconstructions. Furthermore, using these high-fidelity quantitative wavefront measurements, we investigate aberration transfer mechanisms in the high-harmonic-generation process, where we present and explain harmonic-order-dependent astigmatism inheritance from the fundamental wavefront. This ptychographic wavefront sensing concept thus enables detailed studies of the high-harmonic-generation process, such as spatiotemporal effects in attosecond pulse formation.
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| 9. |
- Fu, Xiaozhi, 1990, et al.
(author)
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Recent Advances on Sorting Methods of High-Throughput Droplet-Based Microfluidics in Enzyme Directed Evolution
- 2021
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In: Frontiers in Chemistry. - : Frontiers Media SA. - 2296-2646. ; 9
-
Research review (peer-reviewed)abstract
- Droplet-based microfluidics has been widely applied in enzyme directed evolution (DE), in either cell or cell-free system, due to its low cost and high throughput. As the isolation principles are based on the labeled or label-free characteristics in the droplets, sorting method contributes mostly to the efficiency of the whole system. Fluorescence-activated droplet sorting (FADS) is the mostly applied labeled method but faces challenges of target enzyme scope. Label-free sorting methods show potential to greatly broaden the microfluidic application range. Here, we review the developments of droplet sorting methods through a comprehensive literature survey, including labeled detections [FADS and absorbance-activated droplet sorting (AADS)] and label-free detections [electrochemical-based droplet sorting (ECDS), mass-activated droplet sorting (MADS), Raman-activated droplet sorting (RADS), and nuclear magnetic resonance-based droplet sorting (NMR-DS)]. We highlight recent cases in the last 5 years in which novel enzymes or highly efficient variants are generated by microfluidic DE. In addition, the advantages and challenges of different sorting methods are briefly discussed to provide an outlook for future applications in enzyme DE.
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| 10. |
- Kaplow, Irene M., et al.
(author)
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Relating enhancer genetic variation across mammals to complex phenotypes using machine learning
- 2023
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In: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 380:6643
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Journal article (peer-reviewed)abstract
- Protein-coding differences between species often fail to explain phenotypic diversity, suggesting the involvement of genomic elements that regulate gene expression such as enhancers. Identifying associations between enhancers and phenotypes is challenging because enhancer activity can be tissue-dependent and functionally conserved despite low sequence conservation. We developed the Tissue-Aware Conservation Inference Toolkit (TACIT) to associate candidate enhancers with species' phenotypes using predictions from machine learning models trained on specific tissues. Applying TACIT to associate motor cortex and parvalbumin-positive interneuron enhancers with neurological phenotypes revealed dozens of enhancer-phenotype associations, including brain size-associated enhancers that interact with genes implicated in microcephaly or macrocephaly. TACIT provides a foundation for identifying enhancers associated with the evolution of any convergently evolved phenotype in any large group of species with aligned genomes.
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| 11. |
- Lin, Jiajie, et al.
(author)
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Wafer-scale heterogeneous integration InP on trenched Si with a bubble-free interface
- 2020
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In: APL Materials. - : AIP Publishing. - 2166-532X. ; 8:5
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Journal article (peer-reviewed)abstract
- Heterogeneous integration of compound semiconductors on a Si platform leads to advanced device applications in the field of Si photonics and high frequency electronics. However, the unavoidable bubbles formed at the bonding interface are detrimental for achieving a high yield of dissimilar semiconductor integration by the direct wafer bonding technology. In this work, lateral outgassing surface trenches (LOTs) are introduced to efficiently inhibit the bubbles. It is found that the chemical reactions in InP-Si bonding are similar to those in Si-Si bonding, and the generated gas can escape via the LOTs. The outgassing efficiency is dominated by LOTs' spacing, and moreover, the relationship between bubble formation and the LOT's structure is well described by a thermodynamic model. With the method explored in this work, a 2-in. bubble-free crystalline InP thin film integrated on the Si substrate with LOTs is obtained by the ion-slicing and wafer bonding technology. The quantum well active region grown on this Si-based InP film shows a superior photoemission efficiency, and it is found to be 65% as compared to its bulk counterpart.
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| 12. |
- Waterton, John C., et al.
(author)
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Repeatability and reproducibility of longitudinal relaxation rate in 12 small-animal MRI systems
- 2019
-
In: Magnetic Resonance Imaging. - : Elsevier BV. - 1873-5894 .- 0730-725X. ; 59, s. 121-129
-
Journal article (peer-reviewed)abstract
- Background: Many translational MR biomarkers derive from measurements of the water proton longitudinal relaxation rate R 1 , but evidence for between-site reproducibility of R 1 in small-animal MRI is lacking. Objective: To assess R 1 repeatability and multi-site reproducibility in phantoms for preclinical MRI. Methods: R 1 was measured by saturation recovery in 2% agarose phantoms with five nickel chloride concentrations in 12 magnets at 5 field strengths in 11 centres on two different occasions within 1–13 days. R 1 was analysed in three different regions of interest, giving 360 measurements in total. Root-mean-square repeatability and reproducibility coefficients of variation (CoV) were calculated. Propagation of reproducibility errors into 21 translational MR measurements and biomarkers was estimated. Relaxivities were calculated. Dynamic signal stability was also measured. Results: CoV for day-to-day repeatability (N = 180 regions of interest) was 2.34% and for between-centre reproducibility (N = 9 centres) was 1.43%. Mostly, these do not propagate to biologically significant between-centre error, although a few R 1 -based MR biomarkers were found to be quite sensitive even to such small errors in R 1 , notably in myocardial fibrosis, in white matter, and in oxygen-enhanced MRI. The relaxivity of aqueous Ni 2+ in 2% agarose varied between 0.66 s −1 mM −1 at 3 T and 0.94 s −1 mM −1 at 11.7T. Interpretation: While several factors affect the reproducibility of R 1 -based MR biomarkers measured preclinically, between-centre propagation of errors arising from intrinsic equipment irreproducibility should in most cases be small. However, in a few specific cases exceptional efforts might be required to ensure R 1 -reproducibility.
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| 13. |
- Yilimulati, Mihebai, et al.
(author)
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Regulation of Photosynthesis in Bloom-Forming Cyanobacteria with the Simplest β-Diketone
- 2021
-
In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 55:20, s. 14173-14184
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Journal article (peer-reviewed)abstract
- Selective inhibition of photosynthesis is a fundamental strategy to solve the global challenge caused by harmful cyanobacterial blooms. However, there is a lack of specificity of the currently used cyanocides, because most of them act on cyanobacteria by generating nontargeted oxidative stress. Here, for the first time, we find that the simplest β-diketone, acetylacetone, is a promising specific cyanocide, which acts on Microcystis aeruginosa through targeted binding on bound iron species in the photosynthetic electron transport chain, rather than by oxidizing the components of the photosynthetic apparatus. The targeted binding approach outperforms the general oxidation mechanism in terms of specificity and eco-safety. Given the essential role of photosynthesis in both natural and artificial systems, this finding not only provides a unique solution for the selective control of cyanobacteria but also sheds new light on the ways to modulate photosynthesis.
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| 14. |
- Zhang, Yu, et al.
(author)
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Photochemical conversion of tin-oxo cage compounds studied using hard x-ray photoelectron spectroscopy
- 2017
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In: Journal of Micro/Nanolithography. - 1932-5150 .- 1932-5134. ; 16:2
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Journal article (peer-reviewed)abstract
- Molecular inorganic materials are currently considered photoresists for extreme ultraviolet lithography (EUVL). Their high EUV absorption cross section and small building block size potentially allow high sensitivity and resolution as well as low line-edge roughness. The photochemical reaction mechanisms that allow these kinds of materials to function as photoresists, however, are still poorly understood. We discuss photochemical reactions upon deep UV (DUV) irradiation of a model negative-tone EUV photoresist material, namely the well-defined molecular tin-oxo cage compound [(SnBu)12O14(OH)6](OH)2, which is spin-coated to thin layers of 20 nm. The core electronic structures (Sn 3d, O 1s, and C 1s) of unexposed and DUV exposed films were then investigated using synchrotron radiation-based hard x-ray photoelectron spectroscopy. Different chemical oxidation states and concentrations of atoms and atom types in the unexposed and exposed films were found. We observed that the exposure in a nitrogen atmosphere prevented the oxidation but still led to carbon loss, albeit with a smaller conversion. Finally, a mechanistic hypothesis for the basic DUV photoreactions in molecular tin-oxo cages is proposed.
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| 15. |
- Zhang, Yu, et al.
(author)
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Photochemical conversion of tin-oxo cage compounds studied using hard x-ray photoelectron spectroscopy
- 2017
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In: ADVANCES IN PATTERNING MATERIALS AND PROCESSES XXXIV. - : SPIE. - 9781510607446 - 9781510607439
-
Conference paper (peer-reviewed)abstract
- Several metal-containing molecular inorganic materials are currently considered as photoresists for extreme ultraviolet lithography (EUVL). This is primarily due to their high EUV absorption cross section and small building block size, properties which potentially allow both high sensitivity and resolution as well as low line-edge roughness. The photochemical reaction mechanisms that allow these kinds of materials to function as photoresists, however, are still poorly understood. As a step in this direction, we here discuss photochemical reactions upon deep UV (DUV) irradiation of a model negative-tone EUV photoresist material, namely the well-defined molecular tin-oxo cage compound [(SnR)12O14(OH)6]X2 (R = organic group; X = anion) which is spin coated to thin layers of 20 nm. The core electronic structure (Sn 3d, O 1s and C 1s) of fresh and DUV exposed films were then investigated using synchrotron radiationbased hard X-ray photoelectron spectroscopy (HAXPES). This method provides information about the structure and chemical state of the respective atoms in the material. We performed a comparative HAXPES study of the composition of the tin-oxo cage compound [(SnR)12O14(OH)6](OH)2, either fresh directly after spin-coated vs. DUV-exposed materials under either ambient condition or under a dry N2 atmosphere. Different chemical oxidation states and concentrations of atoms and atom types in the fresh and exposed films were found. We further found that the chemistry resulting from exposure in air and N2 is strikingly different, clearly illustrating the influence of film-gas interactions on the (photo)chemical processes that eventually determine the photoresist. Finally, a mechanistic hypothesis for the basic DUV photoreactions in molecular tin-oxo cages is proposed.
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