1. |
- Kersell, Heath, et al.
(author)
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Some Future Perspectives in Ambient Pressure X-ray Spectroscopies : Atmospheric Pressure, Spatially Resolved and Multi-modal Experiments
- 2021
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In: Ambient Pressure Spectroscopy in Complex Chemical Environments. - Washington, DC : American Chemical Society. - 0097-6156 .- 1947-5918. - 9780841298125 - 9780841298118 ; 1396, s. 333-358
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Book chapter (peer-reviewed)abstract
- This chapter introduces a selection of novel and emerging concepts in ambient pressure X-ray spectroscopies. Technical considerations and first photoemission experiments performed in and above 1 bar pressure are described. Then, X-ray spectroscopy experiments that provide high lateral (microscopy) and depth (X-ray standing-waves) resolution in ambient environments are discussed. The final part of the chapter introduces recent developments in multimodal instrumentation, such as the combination of ambient pressure X-ray Photoelectron Spectroscopy with Infrared spectroscopy and X-ray scattering.
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2. |
- Baeumer, Christoph, et al.
(author)
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Tuning electrochemically driven surface transformation in atomically flat LaNiO3 thin films for enhanced water electrolysis
- 2021
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In: Nature Materials. - : Springer Science and Business Media LLC. - 1476-1122 .- 1476-4660. ; 20:5, s. 674-682
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Journal article (peer-reviewed)abstract
- Structure–activity relationships built on descriptors of bulk and bulk-terminated surfaces are the basis for the rational design of electrocatalysts. However, electrochemically driven surface transformations complicate the identification of such descriptors. Here we demonstrate how the as-prepared surface composition of (001)-terminated LaNiO3 epitaxial thin films dictates the surface transformation and the electrocatalytic activity for the oxygen evolution reaction. Specifically, the Ni termination (in the as-prepared state) is considerably more active than the La termination, with overpotential differences of up to 150 mV. A combined electrochemical, spectroscopic and density-functional theory investigation suggests that this activity trend originates from a thermodynamically stable, disordered NiO2 surface layer that forms during the operation of Ni-terminated surfaces, which is kinetically inaccessible when starting with a La termination. Our work thus demonstrates the tunability of surface transformation pathways by modifying a single atomic layer at the surface and that active surface phases only develop for select as-synthesized surface terminations.
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3. |
- Eren, Baran, et al.
(author)
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Contamination Issues in Ambient Pressure Experiments
- 2021
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In: Ambient Pressure Spectroscopy in Complex Chemical Environments. - Washington, DC : American Chemical Society. - 1947-5918 .- 0097-6156. - 9780841298118 - 9780841298125 ; 1396, s. 267-295
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Book chapter (peer-reviewed)abstract
- Contamination is the most common and arguably the most significant problem scientists are facing in experimental surface science research that is practiced in the presence of gases. It is fair to say that contamination problems are often worse with ambient pressures compared to conventional experiments in vacuum. It is one of the main reasons for poor reproducibility in this field and in relevant basic and applied research fields like heterogeneous catalysis and electrochemistry. Whilst some type of contaminants are more innocent and only hinder quantitative analysis, some are harmful as they change the outcome of the experiments. In this chapter, the potential sources of contamination are summarized and some solutions are suggested. Examples of commonly observed contaminants such as hydrocarbons, oxygenated hydrocarbons, and adsorbed species of traces gases are presented. The scope of this chapter is restricted to ambient pressure x-ray photoelectron spectroscopy and infrared reflection absorption spectroscopy studies on single crystal surfaces, but similar problems exist on other sample surfaces or with other techniques such as x-ray absorption spectroscopy and sum frequency generation spectroscopy.
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4. |
- Kalha, Curran, et al.
(author)
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Hard x-ray photoelectron spectroscopy : a snapshot of the state-of-the-art in 2020
- 2021
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In: Journal of Physics. - : Institute of Physics Publishing (IOPP). - 0953-8984 .- 1361-648X. ; 33:23
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Research review (peer-reviewed)abstract
- Hard x-ray photoelectron spectroscopy (HAXPES) is establishing itself as an essential technique for the characterisation of materials. The number of specialised photoelectron spectroscopy techniques making use of hard x-rays is steadily increasing and ever more complex experimental designs enable truly transformative insights into the chemical, electronic, magnetic, and structural nature of materials. This paper begins with a short historic perspective of HAXPES and spans from developments in the early days of photoelectron spectroscopy to provide an understanding of the origin and initial development of the technique to state-of-the-art instrumentation and experimental capabilities. The main motivation for and focus of this paper is to provide a picture of the technique in 2020, including a detailed overview of available experimental systems worldwide and insights into a range of specific measurement modi and approaches. We also aim to provide a glimpse into the future of the technique including possible developments and opportunities.
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5. |
- Shavorskiy, Andrey, et al.
(author)
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Time Resolved Ambient Pressure X-ray Photoelectron Spectroscopy
- 2021
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In: Ambient Pressure Spectroscopy in Complex Chemical Environments. - Washington, DC : American Chemical Society. - 0097-6156 .- 1947-5918. ; 1396, s. 219-248
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Book chapter (peer-reviewed)abstract
- This chapter describes basic principles and recent advances in time-resolved X-ray Photoelectron Spectroscopy with particular emphasis on studies conducted in complex reaction environments. Specifically, it discusses different ways for obtaining time information and achieving different time resolutions in tr-(AP)XPS experiment, covering timescales from fs to s. This includes experimental setups at the free-electron lasers as well as electron storage rings and high-harmonic generation light sources. A variety of perturbations such as optical, mechanical, gas composition, temperature, and pressure is discussed. A number of examples are described that demonstrate the power of tr-APXPS in studies combining various timescales and perturbation methods.
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