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Abstract. The TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel 5 Precursor (S5-P) satellite provides methane (CH4) measurements with high accuracy and exceptional temporal and spatial resolution and sampling. TROPOMI CH4 measurements are highly valuable to constrain emissions inventories and for trend analysis, with strict requirements on the data quality. This study describes the improvements that we have implemented to retrieve CH4 from TROPOMI using the RemoTeC full-physics algorithm. The updated retrieval algorithm features a constant regularization scheme of the inversion that stabilizes the retrieval and yields less scatter in the data and includes a higher resolution surface altitude database. We have tested the impact of three state-of-the-art molecular spectroscopic databases (HITRAN 2008, HITRAN 2016 and Scientific Exploitation of Operational Missions – Improved Atmospheric Spectroscopy Databases SEOM-IAS) and found that SEOM-IAS provides the best fitting results. The most relevant update in the TROPOMI XCH4 data product is the implementation of an a posteriori correction fully independent of any reference data that is more accurate and corrects for the underestimation at low surface albedo scenes and the overestimation at high surface albedo scenes. After applying the correction, the albedo dependence is removed to a large extent in the TROPOMI versus satellite (Greenhouse gases Observing SATellite – GOSAT) and TROPOMI versus ground-based observations (Total Carbon Column Observing Network – TCCON) comparison, which is an independent verification of the correction scheme. We validate 2 years of TROPOMI CH4 data that show the good agreement of the updated TROPOMI CH4 with TCCON (−3.4 ± 5.6 ppb) and GOSAT (−10.3 ± 16.8 ppb) (mean bias and standard deviation). Low- and high-albedo scenes as well as snow-covered scenes are the most challenging for the CH4 retrieval algorithm, and although the a posteriori correction accounts for most of the bias, there is a need to further investigate the underlying cause.

Despite previous studies on the restoration of tactile sensation on the fingers and the hand, there are no examples of use of the routed sensory information to finely control the prosthesis hand in complex grasp and manipulation tasks. Here it is shown that force and slippage sensations can be elicited in an amputee subject by means of biologically-inspired slippage detection and encoding algorithms, supported by a stick-slip model of the performed grasp. A combination of cuff and intraneural electrodes was implanted for eleven weeks in a young woman with hand amputation, and was shown to provide close-to-natural force and slippage sensations, paramount for significantly improving the subject’s manipulative skills with the prosthesis. Evidence is provided about the improvement of the subject’s grasping and manipulation capabilities over time, thanks to neural feedback. The elicited tactile sensations enabled the successful fulfillment of fine grasp and manipulation tasks with increasing complexity. Grasp performance was quantitatively assessed by means of instrumented objects and a purposely developed metrics. Closed-loop control capabilities enabled by the neural feedback were compared to those achieved without feedback. Further, the work investigates whether the described amelioration of motor performance in dexterous tasks had as central neurophysiological correlates changes in motor cortex plasticity and whether such changes were of purely motor origin, or else the effect of a strong and persistent drive of the sensory feedback.

In situ synchrotron diffraction studies on the formation of the Zr-fumarate MOF give insight into the mechanism of modulated MOF syntheses. In a water-based synthesis, evidence for a coordination modulation mechanism was found.

No abstract

A novel porous coordination polymer (PCP), Zr-abdc, composed of Zr-based secondary building units (SBUs), [Zr 6 O 4 (OH) 4 ] 12+ , and 4,4Ј-azobenzenedicarboxylate (abdc 2-) linkers, has been synthesized by a modulated synthetic approach. In accord with the twelve-fold connecting SBU, Zrabdc has a topology similar to the PCP series UiO-66-UiO-68, which is proposed from single-crystal XRD and powder (P)XRD experiments. The linkers are strongly disordered, which made it impossible to determine the exact structure.

A Zr-based MOF of the PIZOF type, which consists of two independent and mutually interpenetrating UiO-type frameworks with [ZrO(OH)(OC)] nodes, does not only form with a PEPEP dicarboxylic acid (P = phenylene, E = ethynylene). Also dicarboxylic acids with the shorter PPPP and PEPP spacers were found to give PIZOFs, denoted PPPP-PIZOF and PEPP-PIZOF, respectively. Reducing the spacer length even further to a PEEP segment caused a switchover to the formation of a UiO framework. The hysteresis in the Ar sorption curve of PEPP-PIZOF-1 and the slightly too large amount of combustion residue from PPPP-PIZOF-1 suggest structural defects. These hint at a mismatch between the requirement of the optimal linker length for PIZOF formation and the lengths of the PEPP and PPPP dicarboxylates. Nevertheless, these dicarboxylates prefer the formation of a PIZOF over the formation of a UiO structure. PEPEP-PIZOF-2, PPPP-PIZOF-1, and PEPP-PIZOF-1 are stable in air up to 325, 350, and 300 °C, respectively, and have BET surface areas of 2350, 2020, and 1650 m g, respectively. PEPEP-PIZOFs, even those with very hydrophilic oligo(ethylene glycol) side chains on the linkers, are very stable in water and also during drying from a water-wetted state. On the contrary, PEPP-PIZOF-1 and PPPP-PIZOF-1 that had been exposed to water required exchange of water for ethanol before drying to mostly preserve the framework. The results emphasize the importance of differentiating between framework damage caused through hydrolysis in water and through drying from a water-wetted state. The sensitivity of PEPP-PIZOF-1 and PPPP-PIZOF-1 against drying from a water-wetted state may be the consequence of defects. The drying stability of water-wetted PEPEP-PIZOFs lets us suggest that reversible bending of the linkers contributes to the stability of the PEPEP-PIZOFs.

CdZnTe is a promising material for the current generation of free electron laser light sources and future laser-driven γ-ray sources which require detectors capable of high flux imaging at X-ray and γ-ray energies (> 10 keV). However, at high fluxes CdZnTe has been shown to polarise due to hole trapping, leading to poor performance. Novel Redlen CdZnTe material with improved hole transport properties has been designed for high flux applications. Small pixel CdZnTe detectors were fabricated by Redlen Technologies and flip-chip bonded to PIXIE ASICs. An XIA Digital Gamma Finder PIXIE-16 system was used to digitise each of the nine analogue signals with a timing resolution of 10 ns. Pulse shape analysis was used to extract the rise times and amplitude of signals. These were measured as a function of applied bias voltage and used to calculate the mobility (µ) and mobility-lifetime (µτ) of electrons and holes in the material for three identical detectors. The measured values of the transport properties of electrons in the high-flux-capable material was lower than previously reported for Redlen CdZnTe material (µ e τ e ∼ 1 × 10 −3 cm 2 V −1 and µ e ∼ 1000 cm 2 V −1 s −1 ) while the hole transport properties were found to have improved (µ h τ h ∼ 3 × 10 −4 cm 2 V −1 and µ h ∼ 100 cm 2 V −1 s −1 ).