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This study is the first in a series of papers that aim to develop high-resolution emission databases for different anthropogenic sources in China. Here we focus on on-road transportation. Because of the increasing impact of on-road transportation on regional air quality, developing an accurate and high-resolution vehicle emission inventory is important for both the research community and air quality management. This work proposes a new inventory methodology to improve the spatial and temporal accuracy and resolution of vehicle emissions in China. We calculate, for the first time, the monthly vehicle emissions for 2008 in 2364 counties (an administrative unit one level lower than city) by developing a set of approaches to estimate vehicle stock and monthly emission factors at county-level, and technology distribution at provincial level. We then introduce allocation weights for the vehicle kilometers traveled to assign the county-level emissions onto 0.05° × 0.05° grids based on the China Digital Road-network Map (CDRM). The new methodology overcomes the common shortcomings of previous inventory methods, including neglecting the geographical differences between key parameters and using surrogates that are weakly related to vehicle activities to allocate vehicle emissions. The new method has great advantages over previous methods in depicting the spatial distribution characteristics of vehicle activities and emissions. This work provides a better understanding of the spatial representation of vehicle emissions in China and can benefit both air quality modeling and management with improved spatial accuracy.

Nuclear charge radii are sensitive probes of different aspects of the nucleon–nucleon interaction and the bulk properties of nuclear matter, providing a stringent test and challenge for nuclear theory. Experimental evidence suggested a new magic neutron number at N = 32 (refs. 1–3) in the calcium region, whereas the unexpectedly large increases in the charge radii4,5 open new questions about the evolution of nuclear size in neutron-rich systems. By combining the collinear resonance ionization spectroscopy method with β-decay detection, we were able to extend charge radii measurements of potassium isotopes beyond N = 32. Here we provide a charge radius measurement of 52K. It does not show a signature of magic behaviour at N = 32 in potassium. The results are interpreted with two state-of-the-art nuclear theories. The coupled cluster theory reproduces the odd–even variations in charge radii but not the notable increase beyond N = 28. This rise is well captured by Fayans nuclear density functional theory, which, however, overestimates the odd–even staggering effect in charge radii. These findings highlight our limited understanding of the nuclear size of neutron-rich systems, and expose problems that are present in some of the best current models of nuclear theory.The charge radii of potassium isotopes up to 52K are measured, and show no sign of magicity at 32 neutrons as previously suggested in calcium. The observations are interpreted with coupled cluster and density functional theory calculations.

Nuclear charge radii globally scale with atomic mass number A as A 1∕3 , and isotopes with an odd number of neutrons are usually slightly smaller in size than their even-neutron neighbours. This odd–even staggering, ubiquitous throughout the nuclear landscape 1 , varies with the number of protons and neutrons, and poses a substantial challenge for nuclear theory 2 – 4 . Here, we report measurements of the charge radii of short-lived copper isotopes up to the very exotic 78 Cu (with proton number Z = 29 and neutron number N = 49), produced at only 20 ions s –1 , using the collinear resonance ionization spectroscopy method at the Isotope Mass Separator On-Line Device facility (ISOLDE) at CERN. We observe an unexpected reduction in the odd–even staggering for isotopes approaching the N = 50 shell gap. To describe the data, we applied models based on nuclear density functional theory 5 , 6 and A -body valence-space in-medium similarity renormalization group theory 7 , 8 . Through these comparisons, we demonstrate a relation between the global behaviour of charge radii and the saturation density of nuclear matter, and show that the local charge radii variations, which reflect the many-body polarization effects, naturally emerge from A -body calculations fitted to properties of A ≤ 4 nuclei. Isotopes with an odd number of neutrons are usually slightly smaller in size than their even-neutron neighbours. In charge radii of short-lived copper isotopes, a reduction of this effect is observed when the neutron number approaches fifty.

Molecular spectroscopy offers opportunities for the exploration of the fundamental laws of nature and the search for new particle physics beyond the standard model 1 – 4 . Radioactive molecules—in which one or more of the atoms possesses a radioactive nucleus—can contain heavy and deformed nuclei, offering high sensitivity for investigating parity- and time-reversal-violation effects 5 , 6 . Radium monofluoride, RaF, is of particular interest because it is predicted to have an electronic structure appropriate for laser cooling 6 , thus paving the way for its use in high-precision spectroscopic studies. Furthermore, the effects of symmetry-violating nuclear moments are strongly enhanced 5 , 7 – 9 in molecules containing octupole-deformed radium isotopes 10 , 11 . However, the study of RaF has been impeded by the lack of stable isotopes of radium. Here we present an experimental approach to studying short-lived radioactive molecules, which allows us to measure molecules with lifetimes of just tens of milliseconds. Energetically low-lying electronic states were measured for different isotopically pure RaF molecules using collinear resonance ionisation at the ISOLDE ion-beam facility at CERN. Our results provide evidence of the existence of a suitable laser-cooling scheme for these molecules and represent a key step towards high-precision studies in these systems. Our findings will enable further studies of short-lived radioactive molecules for fundamental physics research. Measurements of low-energy electronic states of radium monofluoride validate predictions of the use of this short-lived radioactive molecule in exploring fundamental physics and provide evidence of its suitability for laser cooling.

In spite of the high-density and strongly correlated nature of the atomic nucleus, experimental and theoretical evidence suggests that around particular ‘magic’ numbers of nucleons, nuclear properties are governed by a single unpaired nucleon 1 , 2 . A microscopic understanding of the extent of this behaviour and its evolution in neutron-rich nuclei remains an open question in nuclear physics 3 – 5 . The indium isotopes are considered a textbook example of this phenomenon 6 , in which the constancy of their electromagnetic properties indicated that a single unpaired proton hole can provide the identity of a complex many-nucleon system 6 , 7 . Here we present precision laser spectroscopy measurements performed to investigate the validity of this simple single-particle picture. Observation of an abrupt change in the dipole moment at N  = 82 indicates that, whereas the single-particle picture indeed dominates at neutron magic number N  = 82 (refs.  2 , 8 ), it does not for previously studied isotopes. To investigate the microscopic origin of these observations, our work provides a combined effort with developments in two complementary nuclear many-body methods: ab initio valence-space in-medium similarity renormalization group and density functional theory (DFT). We find that the inclusion of time-symmetry-breaking mean fields is essential for a correct description of nuclear magnetic properties, which were previously poorly constrained. These experimental and theoretical findings are key to understanding how seemingly simple single-particle phenomena naturally emerge from complex interactions among protons and neutrons. Precision laser spectroscopy measurements of neutron-rich indium isotopes were performed to investigate the validity and identify limitations of theoretical descriptions of nuclei based on simple single-particle approaches.

We demonstrate that the pulsed-time structure and high-peak ion intensity provided by the laser-ablation process can be directly combined with the high resolution, high efficiency, and low background offered by collinear resonance ionization spectroscopy. This simple, versatile, and powerful method offers new and unique opportunities for high-precision studies of atomic and molecular structures, impacting fundamental and applied physics research. We show that even for ion beams possessing a relatively large energy spread, high-resolution hyperfine-structure measurements can be achieved by correcting the observed line shapes with the time-of-flight information of the resonantly ionized ions. This approach offers exceptional advantages for performing precision measurements on beams with large energy spreads and allows measurements of atomic parameters of previously inaccessible electronic states. The potential of this experimental method in multidisciplinary research is illustrated by performing, for the first time, hyperfine-structure measurements of selected states in the naturally occurring isotopes of indium,In113,115. Ab initio atomic-physics calculations have been performed to highlight the importance of our findings in the development of state-of-the-art atomic many-body methods, nuclear structure, and fundamental-physics studies.

Diesel trucks are major contributors of nitrogen oxides (NOx) and primary particulate matter smaller than 2.5 μm (PM2.5) in the transportation sector. However, there are more obstacles to existing estimations of diesel-truck emissions compared with those of cars. The obstacles include both inappropriate methodology and missing basic data in China. According to our research, a large number of trucks are conducting long-distance intercity or interprovincial transportation. Thus, the method used by most existing inventories, based on local registration number, is inappropriate. A road emission intensity-based (REIB) approach is introduced in this research instead of registration-population-based approach. To provide efficient data for the REIB approach, 1060 questionnaire responses and approximately 1.7 million valid seconds of onboard GPS monitoring data were collected in China. The estimated NOx and PM2.5 emissions from diesel freight trucks in China were 5.0 (4.8–7.2) million tonnes and 0.20 (0.17–0.22) million tonnes, respectively, in 2011. The province-based emission inventory is also established using the REIB approach. It was found that the driving conditions on different types of road have significant impacts on the emission levels of freight trucks. The largest differences among the emission factors (in g km−1) on different roads exceed 70 and 50% for NOx and PM2.5, respectively. A region with more intercity freeways or national roads tends to have more NOx emissions, while urban streets play a more important role in primary PM2.5 emissions from freight trucks. Compared with the inventory of the Ministry of Environment Protection, which allocates emissions according to local truck registration number and neglects interregional long-distance transport trips, the differences for NOx and PM2.5 are +28 and −57%, respectively. The REIB approach matches better with traffic statistical data on a provincial level. Furthermore, the different driving conditions on the different roads types are no longer overlooked with this approach.

With increasing demand for accurate calculation of isotope shifts of atomic systems for fundamental and nuclear structure research, an analytic energy derivative approach is presented in the relativistic coupled-cluster (CC) theory framework to determine the atomic field shift and mass shift (MS) factors. This approach allows the determination of expectation values of atomic operators, overcoming fundamental problems that are present in existing atomic physics methods, i.e. it satisfies the Hellmann-Feynman theorem, does not involve any non-terminating series, and is free from choice of any perturbative parameter. As a proof of concept, the developed analytic response relativistic CC theory has been applied to determine MS and field shift factors for different atomic states of indium. High-precision isotope-shift measurements of 104 − 127 In were performed in the 246.8 nm (5p 2P3/2 → 9s 2S1/2) and 246.0 nm (5p 2P1/2 → 8s 2S1/2) transitions to test our theoretical results. An excellent agreement between the theoretical and measured values is found, which is known to be challenging in multi-electron atoms. The calculated atomic factors allowed an accurate determination of the nuclear charge radii of the ground and isomeric states of the 104 − 127 In isotopes, providing an isotone-independent comparison of the absolute charge radii.

This work reports on the application of a novel electric field-ionization setup for high-resolution laser spectroscopy measurements on bunched fast atomic beams in a collinear geometry. In combination with multi-step resonant excitation to Rydberg states using pulsed lasers, the field ionization technique demonstrates increased sensitivity for isotope separation and measurement of atomic parameters over previous non-resonant laser ionization methods. The setup was tested at the Collinear Resonance Ionization Spectroscopy experiment at ISOLDE-CERN to perform high-resolution measurements of transitions in the indium atom from the 5s 2 5d 2 D 5 / 2 and 5s 2 5d 2 D 3 / 2 states to 5s 2 n p  2 P and 5s 2 n f 2 F Rydberg states, up to a principal quantum number of n = 72 . The extracted Rydberg level energies were used to re-evaluate the ionization potential of the indium atom to be 46 , 670.107 ( 4 ) cm - 1 . The nuclear magnetic dipole and nuclear electric quadrupole hyperfine structure constants and level isotope shifts of the 5s 2 5d 2 D 5 / 2 and 5s 2 5d 2 D 3 / 2 states were determined for 113 , 115 In. The results are compared to calculations using relativistic coupled-cluster theory. A good agreement is found with the ionization potential and isotope shifts, while disagreement of hyperfine structure constants indicates an increased importance of electron correlations in these excited atomic states. With the aim of further increasing the detection sensitivity for measurements on exotic isotopes, a systematic study of the field-ionization arrangement implemented in the work was performed at the same time and an improved design was simulated and is presented. The improved design offers increased background suppression independent of the distance from field ionization to ion detection.

One hundred and thirty-six bla OXA-51 -negative strains were identified from 1,067 Acinetobacter calcoaceticus – A. baumannii complex (ACB complex) isolates, which were collected during October 2010 to March 2013 from 15 general hospitals in 10 cities throughout Zhejiang Province, China. Seven of the 136 bla OXA-51 -negative ACB complex isolates were New Delhi metallo-β-lactamase-1 (NDM-1)-positive, among which three were identified as A. nosocomialis and four were identified as A. pittii strains using 16S–23S rRNA gene intergenic spacer (ITS) sequencing and partial RNA polymerase β-subunit ( rpoB ) sequencing. Pulsed-field gel electrophoresis (PFGE) and multilocus sequence typing (MLST) analysis showed that the seven NDM-positive isolates belonged to three clonal strains with three novel sequence types (STs). Polymerase chain reaction (PCR) assays and DNA sequence analysis of the carbapenemase and other β-lactamase genes indicated that all the isolates harbored the bla NDM-1 gene, and that only one strain of A. nosocomialis isolates harbored both bla NDM-1 and bla OXA-23 . All of them were positive for bla ADC , from which three novel bla ADC genes (designated as bla ADC-69 , bla ADC-70 , and bla ADC-71 ) were detected for the first time. The presence of IS Aba125 upstream of bla NDM-1 was identified through genetic environment analysis. Carbapenem resistance can be transferred from A. nosocomialis and A. pittii to Escherichia coli EC600 by the conjugation experiment. Plasmid analysis, DNA hybridization, and extraction experiments indicated that bla NDM-1 was located on a plasmid of approximately 50 kb. In conclusion, we characterized the dissemination of NDM-1-positive A. pittii strains in Zhejiang Province, China, and reported the NDM-producing A. nosocomialis for the first time.