Dutch Institute for Fundamental Energy Research

OBJECTIVE: To address the problem of volume conduction and active reference electrodes in the assessment of functional connectivity, we propose a novel measure to quantify phase synchronization, the phase lag index (PLI), and compare its performance to the well-known phase coherence (PC), and to the imaginary component of coherency (IC). METHODS: The PLI is a measure of the asymmetry of the distribution of phase differences between two signals. The performance of PLI, PC, and IC was examined in (i) a model of 64 globally coupled oscillators, (ii) an EEG with an absence seizure, (iii) an EEG data set of 15 Alzheimer patients and 13 control subjects, and (iv) two MEG data sets. RESULTS: PLI and PC were more sensitive than IC to increasing levels of true synchronization in the model. PC and IC were influenced stronger than PLI by spurious correlations because of common sources. All measures detected changes in synchronization during the absence seizure. In contrast to PC, PLI and IC were barely changed by the choice of different montages. PLI and IC were superior to PC in detecting changes in beta band connectivity in AD patients. Finally, PLI and IC revealed a different spatial pattern of functional connectivity in MEG data than PC. CONCLUSION: The PLI performed at least as well as the PC in detecting true changes in synchronization in model and real data but, at the same token and like-wise the IC, it was much less affected by the influence of common sources and active reference electrodes.

<p>Journal of Physics D: Applied Physics published the first Plasma Roadmap in 2012 consisting of the individual perspectives of 16 leading experts in the various sub-fields of low temperature plasma science and technology. The 2017 Plasma Roadmap is the first update of a planned series of periodic updates of the Plasma Roadmap. The continuously growing interdisciplinary nature of the low temperature plasma field and its equally broad range of applications are making it increasingly difficult to identify major challenges that encompass all of the many sub-fields and applications. This intellectual diversity is ultimately a strength of the field. The current state of the art for the 19 sub-fields addressed in this roadmap demonstrates the enviable track record of the low temperature plasma field in the development of plasmas as an enabling technology for a vast range of technologies that underpin our modern society. At the same time, the many important scientific and technological challenges shared in this roadmap show that the path forward is not only scientifically rich but has the potential to make wide and far reaching contributions to many societal challenges.</p>

In the literature, it is well established that subjects are able to jump higher in a countermovement jump (CMJ) than in a squat jump (SJ). The purpose of this study was to estimate the relative contribution of the time available for force development and the storage and reutilization of elastic energy to the enhancement of performance in CMJ compared with SJ. Six male volleyball players performed CMJ and SJ. Kinematics, kinetics, and muscle electrical activity (EMG) from six muscles of the lower extremity were monitored. It was found that even when the body position at the start of push-off was the same in SJ as in CMJ, jump height was on average 3.4 cm greater in CMJ. The possibility that nonoptimal coordination in SJ explained the difference in jump height was ruled out: there were no signs of movement disintegration in SJ, and toe-off position was the same in SJ as in CMJ. The greater jump height in CMJ was attributed to the fact that the countermovement allowed the subjects to attain greater joint moments at the start of push-off. As a consequence, joint moments were greater over the first part of the range of joint extension in CMJ, so that more work could be produced than in SJ. To explain this finding, measured and manipulated kinematics and electromyographic activity were used as input for a model of the musculoskeletal system. According to simulation results, storage and reutilization of elastic energy could be ruled out as explanation for the enhancement of performance in CMJ over that in SJ. The crucial contribution of the countermovement seemed to be that it allowed the muscles to build up a high level of active state (fraction of attached cross-bridges) and force before the start of shortening, so that they were able to produce more work over the first part of their shortening distance.

Water electrolysis is the most promising method for efficient production of high purity hydrogen (and oxygen), while the required power input for the electrolysis process can be provided by renewable sources (e.g. solar or wind). The thus produced hydrogen can be used either directly as a fuel or as a reducing agent in chemical processes, such as in Fischer–Tropsch synthesis. Water splitting can be realized both at low temperatures (typically below 100 °C) and at high temperatures (steam water electrolysis at 500–1000 °C), while different ionic agents can be electrochemically transferred during the electrolysis process (OH−, H+, O2−). Singular requirements apply in each of the electrolysis technologies (alkaline, polymer electrolyte membrane and solid oxide electrolysis) for ensuring high electrocatalytic activity and long-term stability. The aim of the present article is to provide a brief overview on the effect of the nature and structure of the catalyst–electrode materials on the electrolyzer's performance. Past findings and recent progress in the development of efficient anode and cathode materials appropriate for large-scale water electrolysis are presented. The current trends, limitations and perspectives for future developments are summarized for the diverse electrolysis technologies of water splitting, while the case of CO2/H2O co-electrolysis (for synthesis gas production) is also discussed.

Conjugated polymers have been extensively studied for application in organic solar cells. In designing new polymers, particular attention has been given to tuning the absorption spectrum, molecular energy levels, crystallinity, and charge carrier mobility to enhance performance. As a result, the power conversion efficiencies (PCEs) of solar cells based on conjugated polymers as electron donor and fullerene derivatives as electron acceptor have exceeded 10% in single-junction and 11% in multijunction devices. Despite these efforts, it is notoriously difficult to establish thorough structure-property relationships that will be required to further optimize existing high-performance polymers to their intrinsic limits. In this Account, we highlight progress on the development and our understanding of diketopyrrolopyrrole (DPP) based conjugated polymers for polymer solar cells. The DPP moiety is strongly electron withdrawing and its polar nature enhances the tendency of DPP-based polymers to crystallize. As a result, DPP-based conjugated polymers often exhibit an advantageously broad and tunable optical absorption, up to 1000 nm, and high mobilities for holes and electrons, which can result in high photocurrents and good fill factors in solar cells. Here we focus on the structural modifications applied to DPP polymers and rationalize and explain the relationships between chemical structure and organic photovoltaic performance. The DPP polymers can be tuned via their aromatic substituents, their alkyl side chains, and the nature of the π-conjugated segment linking the units along the polymer chain. We show that these building blocks work together in determining the molecular conformation, the optical properties, the charge carrier mobility, and the solubility of the polymer. We identify the latter as a decisive parameter for DPP-based organic solar cells because it regulates the diameter of the semicrystalline DPP polymer fibers that form in the photovoltaic blends with fullerenes via solution processing. The width of these fibers and the photon energy loss, defined as the energy difference between optical band gap and open-circuit voltage, together govern to a large extent the quantum efficiency for charge generation in these blends and thereby the power conversion efficiency of the photovoltaic devices. Lowering the photon energy loss and maintaining a high quantum yield for charge generation is identified as a major pathway to enhance the performance of organic solar cells. This can be achieved by controlling the structural purity of the materials and further control over morphology formation. We hope that this Account contributes to improved design strategies of DPP polymers that are required to realize new breakthroughs in organic solar cell performance in the future.

Abstract The 2022 Roadmap is the next update in the series of Plasma Roadmaps published by Journal of Physics D with the intent to identify important outstanding challenges in the field of low-temperature plasma (LTP) physics and technology. The format of the Roadmap is the same as the previous Roadmaps representing the visions of 41 leading experts representing 21 countries and five continents in the various sub-fields of LTP science and technology. In recognition of the evolution in the field, several new topics have been introduced or given more prominence. These new topics and emphasis highlight increased interests in plasma-enabled additive manufacturing, soft materials, electrification of chemical conversions, plasma propulsion, extreme plasma regimes, plasmas in hypersonics, data-driven plasma science and technology and the contribution of LTP to combat COVID-19. In the last few decades, LTP science and technology has made a tremendously positive impact on our society. It is our hope that this roadmap will help continue this excellent track record over the next 5–10 years.

Abstract Organic photodetectors (OPDs) have gained increasing interest as they offer cost‐effective fabrication methods using low temperature processes, making them particularly attractive for large area image detectors on lightweight flexible plastic substrates. Moreover, their photophysical and optoelectronic properties can be tuned both at a material and device level. Visible‐light OPDs are proposed for use in indirect‐conversion X‐ray detectors, fingerprint scanners, and intelligent surfaces for gesture recognition. Near‐infrared OPDs find applications in biomedical imaging and optical communications. For most applications, minimizing the OPD dark current density ( J d ) is crucial to improve important figures of merits such as the signal‐to‐noise ratio, the linear dynamic range, and the specific detectivity ( D *). Here, a quantitative analysis of the intrinsic dark current processes shows that charge injection from the electrodes is the dominant contribution to J d in OPDs. J d reduction is typically addressed by fine‐tuning the active layer energetics and stratification or by using charge blocking layers. Yet, most experimental J d values are higher than the calculated intrinsic limit. Possible reasons for this deviation are discussed, including extrinsic defects in the photoactive layer and the presence of trap states. This provides the reader with guidelines to improve the OPD performances in view of imaging applications.

Metal nanoparticle arrays that support surface lattice resonances have emerged as an exciting platform for manipulating light–matter interactions at the nanoscale and enabling a diverse range of applications. Their recent prominence can be attributed to a combination of desirable photonic and plasmonic attributes: high electromagnetic field enhancements extended over large volumes with long-lived lifetimes. This Review will describe the design rules for achieving high-quality optical responses from metal nanoparticle arrays, nanofabrication advances that have enabled their production, and the theory that inspired their experimental realization. Rich fundamental insights will focus on weak and strong coupling with molecular excitons, as well as semiconductor excitons and the lattice resonances. Applications related to nanoscale lasing, solid-state lighting, and optical devices will be discussed. Finally, prospects and future open questions will be described.

Abstract Density functional theory (DFT) simulations of the oxygen evolution reaction (OER) are considered essential for understanding the limitations of water splitting. Most DFT calculations of the OER use an acidic reaction mechanism and the standard hydrogen electrode (SHE) as reference electrode. However, experimental studies are usually carried out under alkaline conditions using the reversible hydrogen electrode (RHE) as reference electrode. The difference between the conditions in experiment and calculations is then usually taken into account by applying a pH-dependent correction factor to the latter. As, however, the OER reaction mechanisms under acidic and under alkaline conditions are quite different, it is not clear a priori whether a simple correction factor can account for this difference. We derive in this paper step by step the theory to simulate the OER based on the alkaline reaction mechanism and explain the OER process with this mechanism and the RHE as reference electrode. We compare the mechanisms for alkaline and acidic OER catalysis and highlight the roles of the RHE and the SHE. Our detailed analysis validates current OER simulations in the literature and explains the differences in OER calculations with acidic and alkaline mechanisms.

Diketopyrrolopyrrole-based conjugated polymers bridged with thiazole units and different donors have been designed for polymer solar cells. Quantum efficiencies above 50% have been achieved with energy loss between optical band gap and open-circuit voltage below 0.6 eV.

The use of nanoplasmonics to control light and heat close to the thermodynamic limit enables exciting opportunities in the field of plasmonic catalysis. The decay of plasmonic excitations creates highly nonequilibrium distributions of hot carriers that can initiate or catalyze reactions through both thermal and nonthermal pathways. In this Perspective, we present the current understanding in the field of plasmonic catalysis, capturing vibrant debates in the literature, and discuss future avenues of exploration to overcome critical bottlenecks. Our Perspective spans first-principles theory and computation of correlated and far-from-equilibrium light-matter interactions, synthesis of new nanoplasmonic hybrids, and new steady-state and ultrafast spectroscopic probes of interactions in plasmonic catalysis, recognizing the key contributions of each discipline in realizing the promise of plasmonic catalysis. We conclude with our vision for fundamental and technological advances in the field of plasmon-driven chemical reactions in the coming years.

Hydrogen gas is rapidly approaching a global breakthrough as a carbon-free energy vector. In such a hydrogen economy, safety sensors for hydrogen leak detection will be an indispensable element along the entire value chain, from the site of hydrogen production to the point of consumption, due to the high flammability of hydrogen-air mixtures. To stimulate and guide the development of such sensors, industrial and governmental stakeholders have defined sets of strict performance targets, which are yet to be entirely fulfilled. In this Perspective, we summarize recent efforts and discuss research strategies for the development of hydrogen sensors that aim at meeting the set performance goals. In the first part, we describe the state-of-the-art for fast and selective hydrogen sensors at the research level, and we identify nanostructured Pd transducer materials as the common denominator in the best performing solutions. As a consequence, in the second part, we introduce the fundamentals of the Pd-hydrogen interaction to lay the foundation for a detailed discussion of key strategies and Pd-based material design rules necessary for the development of next generation high-performance nanostructured Pd-based hydrogen sensors that are on par with even the most stringent and challenging performance targets.

Light absorption and scattering of plasmonic metal nanoparticles can lead to non-equilibrium charge carriers, intense electromagnetic near-fields, and heat generation, with promising applications in a vast range of fields, from chemical and physical sensing to nanomedicine and photocatalysis for the sustainable production of fuels and chemicals. Disentangling the relative contribution of thermal and non-thermal contributions in plasmon-driven processes is, however, difficult. Nanoscale temperature measurements are technically challenging, and macroscale experiments are often characterized by collective heating effects, which tend to make the actual temperature increase unpredictable. This work is intended to help the reader experimentally detect and quantify photothermal effects in plasmon-driven chemical reactions, to discriminate their contribution from that due to photochemical processes and to cast a critical eye on the current literature. To this aim, we review, and in some cases propose, seven simple experimental procedures that do not require the use of complex or expensive thermal microscopy techniques. These proposed procedures are adaptable to a wide range of experiments and fields of research where photothermal effects need to be assessed, such as plasmonic-assisted chemistry, heterogeneous catalysis, photovoltaics, biosensing, and enhanced molecular spectroscopy.

The performance of organic semiconductors in optoelectronic devices depends on the functional properties of the individual molecules and their mutual orientations when they are in the solid state. The effect of H‐ and J‐aggregation on the photophysical properties and photovoltaic behavior of four electronically identical but structurally different thiophene–pyridine–diketopyrrolopyrrole molecules is studied. By introducing and changing the position of two hexyl side chains on the two peripheral thiophene units of these molecules, their aggregation in thin films between H‐type and J‐type is effectively tuned, as evidenced from the characteristics of optical absorption, fluorescence, and excited state lifetime. The two derivatives that assemble into J‐type aggregates exhibit a significantly enhanced photovoltaic performance, up to an order of magnitude, compared to the two molecules that form H‐type aggregates. The reasons for this remarkably different behavior are discussed.

The influence of different iron carbides on the activity and selectivity of iron-based Fischer–Tropsch catalysts has been studied. Different iron carbide phases are obtained by the pretreatment of a binary Fe/SiO2 model catalyst (prepared by coprecipitation method) to different gas atmospheres (syngas, CO, or H2). The phase structures, compositions, and particle sizes of the catalysts are characterized systematically by XRD, XAFS, MES, and TEM. It is found that in the syngas-treated catalyst only χ-Fe5C2 carbide is formed. In the CO-treated catalyst, Fe7C3 and χ-Fe5C2 with a bimodal particle size distribution are formed, while the H2-treated catalyst exhibits the bimodal size distributed ε-Fe2C and χ-Fe5C2 after a Fischer–Tropsch synthesis (FTS) reaction. The intrinsic FTS activity is calculated and assigned to each corresponding iron carbide based on the phase composition and the particle size. It is identified that Fe7C3 has the highest intrinsic activity (TOF = 4.59 × 10–2 s–1) among the three candidate carbides (ε-Fe2C, Fe7C3, and χ-Fe5C2) in typical medium-temperature Fischer–Tropsch (MTFT) conditions (260–300 °C, 2–3 MPa, and H2/CO = 2). Moreover, FTS over ε-Fe2C leads to the lowest methane selectivity.

BACKGROUND: Despite major advances in pharmacological treatment of chronic heart failure (CHF), a number of patients still suffer from dyspnoea, fatigue, diminished exercise capacity and poor quality of life. It is in this context that exercise training is being intensively evaluated for any additional benefit in the treatment of CHF. AIMS: To determine the effect of exercise training in patients with CHF on cardiac performance, exercise capacity and health-related quality of life. A meta-analysis was performed to obtain this goal. METHODS AND RESULTS: After including 35 randomised controlled trials, the methodological quality of each study was assessed, summary effect sizes (SESs) and the concomitant 95% confidence intervals (95% CI) were calculated for each outcome. Quantitative analysis showed statistically significant SESs, at rest, for diastolic blood pressure and end-diastolic volume. During maximal exercise, significant SESs were found for systolic blood pressure, heart rate, cardiac output, peak oxygen uptake, anaerobic threshold and 6-min walking test. The Minnesota Living with Heart Failure Questionnaire improved by an average of 9.7 points. CONCLUSIONS: Exercise training has clinically important effects on exercise capacity and HRQL, and may have small positive effects on cardiac performance during exercise.

Physiotherapy is an established component of stroke rehabilitation but uncertainties remain about the most appropriate intensity of therapy input. We conducted a systematic review of the randomised trials of physiotherapy after stroke where qualitatively similar therapy regimens were provided at different levels of intensity. A heterogeneous group of seven randomised trials (597 patients) was identified. Dichotomous outcomes (death or the combined poor outcome of death or deterioration) were analysed by use of the odds ratio and 95% confidence interval. Patients subjected to more intensive physiotherapy input showed a non-significant reduction in case fatality (odds ratio 0.60; 95% CI 0.33-1.09) and a significant reduction (OR 0.54; 95% CI 0.34-0.85; p < 0.01) in the combined poor outcome of death or deterioration by the end of follow-up. Two statistical techniques were used to identify patterns within the continuous data. Firstly, impairment and disability scores were converted to a standardised measure of 0-100 and the weighted mean difference (WMD) between the scores in the intensive and conventional physiotherapy groups were then calculated. Modest improvements were observed in both the impairment (WMD+5; 95% CI-1-11) and disability scores (WMD+5; 95% CI 0-10) recorded at the initial review (median 3 months post-stroke), but not at the final review (median 1 year post-stroke). Secondly, Fisher's inverse chi-squared test was used to combine the p values from individual trials; this confirmed the above findings (p < 0.05 at initial review; p > 0.05 at final review). More intensive physiotherapy input was associated with a reduction in the combined poor outcome of death or deterioration and may enhance the rate of recovery. These observations warrant further investigation.

Understanding and controlling the formation of nanoparticles at the surface of functional oxide supports is critical for tuning activity and stability for catalytic and energy conversion applications. Here, we use a latest generation environmental transmission electron microscope to follow the exsolution of individual nanoparticles at the surface of perovskite oxides, with ultrahigh spatial and temporal resolution. Qualitative and quantitative analysis of the data reveals the atomic scale processes that underpin the formation of the socketed, strain-inducing interface that confers exsolved particles their exceptional stability and reactivity. This insight also enabled us to discover that the shape of exsolved particles can be controlled by changing the atmosphere in which exsolution is carried out, and additionally, this could also produce intriguing heterostructures consisting of metal–metal oxide coupled nanoparticles. Our results not only provide insight into the in situ formation of nanoparticles but also demonstrate the tailoring of nanostructures and nanointerfaces.

Power‐to‐gas is a storage technology aiming to convert surplus electricity from renewable energy sources like wind and solar power into gaseous fuels compatible with the current network infrastructure. Results of CO 2 dissociation in a vortex‐stabilized microwave plasma reactor are presented. The microwave field, residence time, quenching, and vortex configuration were varied to investigate their influence on energy‐ and conversion efficiency of CO 2 dissociation. Significant deterioration of the energy efficiency is observed at forward vortex plasmas upon increasing pressure in the range of 100 mbar towards atmospheric pressure, which is mitigated by using a reverse vortex flow configuration of the plasma reactor. Data from optical emission shows that under all conditions covered by the experiments the gas temperature is in excess of 4000 K, suggesting a predominant thermal dissociation. Different strategies are proposed to enhance energy and conversion efficiencies of plasma‐driven dissociation of CO 2 .

Water is a ubiquitous solvent in chemistry and life. It is therefore no surprise that the aqueous solubility of compounds has a key role in various domains, including but not limited to drug discovery, paint, coating, and battery materials design. Measurement and prediction of aqueous solubility is a complex and prevailing challenge in chemistry. For the latter, different data-driven prediction models have recently been developed to augment the physics-based modeling approaches. To construct accurate data-driven estimation models, it is essential that the underlying experimental calibration data used by these models is of high fidelity and quality. Existing solubility datasets show variance in the chemical space of compounds covered, measurement methods, experimental conditions, but also in the non-standard representations, size, and accessibility of data. To address this problem, we generated a new database of compounds, AqSolDB, by merging a total of nine different aqueous solubility datasets, curating the merged data, standardizing and validating the compound representation formats, marking with reliability labels, and providing 2D descriptors of compounds as a Supplementary Resource.