Ana Luiza Costa Silva, Rafael Schio Wengenroth Silva, Lucas Augusto Moisés, Adenilson José Chiquito, Marcio Peron Franco de Godoy, Fabian Hartmann, Victor Lopez-Richard
Gas and moisture sensing devices leveraging the resistive switching effect in transition metal oxide memristors promise to revolutionize next-generation, nano-scaled, cost-effective, and environmentally sustainable sensor solutions. These sensors encode readouts in resistance state changes based on gas concentration, yet their nonlinear current-voltage characteristics offer richer dynamics, capturing detailed information about REDOX reactions and surface kinetics. Traditional vertical devices fail to fully exploit this complexity. This study demonstrates planar resistive switching devices, moving beyond the Butler-Volmer model. A systematic investigation of the electrochemical processes in Na-doped ZnO with lateral planar contacts reveals intricate patterns resulting from REDOX reactions on the device surface. When combined with advanced algorithms for pattern recognition, allow the analysis of complex switching patterns, including crossings, loop directions, and resistance values, providing unprecedented insights for next-generation complex sensors.
{"title":"Memory traces ruled by surface-biased REDOX reactions","authors":"Ana Luiza Costa Silva, Rafael Schio Wengenroth Silva, Lucas Augusto Moisés, Adenilson José Chiquito, Marcio Peron Franco de Godoy, Fabian Hartmann, Victor Lopez-Richard","doi":"arxiv-2409.07299","DOIUrl":"https://doi.org/arxiv-2409.07299","url":null,"abstract":"Gas and moisture sensing devices leveraging the resistive switching effect in\u0000transition metal oxide memristors promise to revolutionize next-generation,\u0000nano-scaled, cost-effective, and environmentally sustainable sensor solutions.\u0000These sensors encode readouts in resistance state changes based on gas\u0000concentration, yet their nonlinear current-voltage characteristics offer richer\u0000dynamics, capturing detailed information about REDOX reactions and surface\u0000kinetics. Traditional vertical devices fail to fully exploit this complexity.\u0000This study demonstrates planar resistive switching devices, moving beyond the\u0000Butler-Volmer model. A systematic investigation of the electrochemical\u0000processes in Na-doped ZnO with lateral planar contacts reveals intricate\u0000patterns resulting from REDOX reactions on the device surface. When combined\u0000with advanced algorithms for pattern recognition, allow the analysis of complex\u0000switching patterns, including crossings, loop directions, and resistance\u0000values, providing unprecedented insights for next-generation complex sensors.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190253","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Daniel Lozano-Martín, M. Carmen Martín, César R. Chamorro, Dirk Tuma, José Juan Segovia
Speed of sound is one of the thermodynamic properties that can be measured with least uncertainty and is of great interest in developing equations of state. Moreover, accurate models are needed by the H2 industry to design the transport and storage stages of hydrogen blends in the natural gas network. This research aims to provide accurate data for ($CH_{4}$ + $H_{2}$) mixtures of nominal (5, 10, and 50) mol-% of hydrogen, in the $p$ = (0.5 up to 20) MPa pressure range and with temperatures $T$ = (273.16, 300, 325, 350, and 375) K. Using an acoustic spherical resonator, speed of sound was determined with an overall relative expanded ($k$ = 2) uncertainty of 220 parts in $10^{6}$ (0.022%). Data were compared to reference equations of state for natural gas-like mixtures, such as AGA8-DC92 and GERG-2008. Average absolute deviations below 0.095% and percentage deviations between 0.029% and up to 0.30%, respectively, were obtained. Additionally, results were fitted to the acoustic virial equation of state and adiabatic coefficients, molar isochoric heat capacities and molar isobaric heat capacities as perfect-gas, together with second and third acoustic virial coefficients were estimated. Density second virial coefficients were also obtained.
{"title":"Speed of sound for three binary ($CH_{4}$ + $H_{2}$) mixtures from $p$ = (0.5 up to 20) MPa at $T$ = (273.16 to 375) K","authors":"Daniel Lozano-Martín, M. Carmen Martín, César R. Chamorro, Dirk Tuma, José Juan Segovia","doi":"arxiv-2409.07130","DOIUrl":"https://doi.org/arxiv-2409.07130","url":null,"abstract":"Speed of sound is one of the thermodynamic properties that can be measured\u0000with least uncertainty and is of great interest in developing equations of\u0000state. Moreover, accurate models are needed by the H2 industry to design the\u0000transport and storage stages of hydrogen blends in the natural gas network.\u0000This research aims to provide accurate data for ($CH_{4}$ + $H_{2}$) mixtures\u0000of nominal (5, 10, and 50) mol-% of hydrogen, in the $p$ = (0.5 up to 20) MPa\u0000pressure range and with temperatures $T$ = (273.16, 300, 325, 350, and 375) K.\u0000Using an acoustic spherical resonator, speed of sound was determined with an\u0000overall relative expanded ($k$ = 2) uncertainty of 220 parts in $10^{6}$\u0000(0.022%). Data were compared to reference equations of state for natural\u0000gas-like mixtures, such as AGA8-DC92 and GERG-2008. Average absolute deviations\u0000below 0.095% and percentage deviations between 0.029% and up to 0.30%,\u0000respectively, were obtained. Additionally, results were fitted to the acoustic\u0000virial equation of state and adiabatic coefficients, molar isochoric heat\u0000capacities and molar isobaric heat capacities as perfect-gas, together with\u0000second and third acoustic virial coefficients were estimated. Density second\u0000virial coefficients were also obtained.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190249","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Explicitly utilizing the sparsity of the electronic structure problem, fragmentation methods have been heavily researched for decades with great success, pushing the limits of ab initio quantum chemistry ever further. Recently, this set of methods was expanded to include a fundamentally different approach called excitonic renormalization, providing promising initial results. It builds a supersystem Hamiltonian in a second-quantized-like representation from transition-density tensors of isolated fragments, contracted with biorthogonalized molecular integrals. This makes the method fully modular in terms of the quantum chemical methods applied to each fragment and enables massive truncation of the state-space required. Proof-of-principle tests have previously shown that solving for the ground state of an excitonically renormalized Hamiltonian can efficiently scale to hundreds of fragments, but the ad hoc approach that was used to build the Hamiltonian in those tests was not scalable to larger fragments. On the other hand, initial tests of the originally proposed fully modular Hamiltonian build, presented here, have shown the accuracy to be poor on account of its non-Hermitian character. In this study we bridge the gap between these with an operator expansion that is shown to converge rapidly, tending towards a Hermitian Hamiltonian while retaining the modularity, yielding an accurate, scalable method. The accuracy of the Hamiltonian is tested here for a beryllium dimer. At distances near the equilibrium point and longer, the zeroth-order method is comparable to CCSD(T), and the first-order method to FCI. Deviations occurring at shorter bond distances are discussed along with approaches to scaling up to larger fragments.
{"title":"Series Expansion of a Scalable Hermitian Excitonic Renormalization Method","authors":"Marco Bauer, Andreas Dreuw, Anthony D. Dutoi","doi":"arxiv-2409.07628","DOIUrl":"https://doi.org/arxiv-2409.07628","url":null,"abstract":"Explicitly utilizing the sparsity of the electronic structure problem,\u0000fragmentation methods have been heavily researched for decades with great\u0000success, pushing the limits of ab initio quantum chemistry ever further.\u0000Recently, this set of methods was expanded to include a fundamentally different\u0000approach called excitonic renormalization, providing promising initial results.\u0000It builds a supersystem Hamiltonian in a second-quantized-like representation\u0000from transition-density tensors of isolated fragments, contracted with\u0000biorthogonalized molecular integrals. This makes the method fully modular in\u0000terms of the quantum chemical methods applied to each fragment and enables\u0000massive truncation of the state-space required. Proof-of-principle tests have\u0000previously shown that solving for the ground state of an excitonically\u0000renormalized Hamiltonian can efficiently scale to hundreds of fragments, but\u0000the ad hoc approach that was used to build the Hamiltonian in those tests was\u0000not scalable to larger fragments. On the other hand, initial tests of the\u0000originally proposed fully modular Hamiltonian build, presented here, have shown\u0000the accuracy to be poor on account of its non-Hermitian character. In this\u0000study we bridge the gap between these with an operator expansion that is shown\u0000to converge rapidly, tending towards a Hermitian Hamiltonian while retaining\u0000the modularity, yielding an accurate, scalable method. The accuracy of the\u0000Hamiltonian is tested here for a beryllium dimer. At distances near the\u0000equilibrium point and longer, the zeroth-order method is comparable to CCSD(T),\u0000and the first-order method to FCI. Deviations occurring at shorter bond\u0000distances are discussed along with approaches to scaling up to larger\u0000fragments.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Daniel Lozano-Martín, David Vega-Maza, M. Carmen Martín, Dirk Tuma, César R. Chamorro
Continuing our study on ($CO_{2}$ + $O_{2}$) mixtures, this work reports new experimental($p$, $rho$, $T$) data for two oxygen-rich mixtures with mole fractions $x$($O_{2}$) = (0.50 and 0.75) mol/mol, in the temperature range $T$ = (250-375) K and pressure range $p$ = (0.5-20) MPa, using a single-sinker densimeter. Experimental density data were compared to two well-established equation-of-state models: EOS-CG and GERG-2008. In the $p$, $T$-range investigated, the EOS-CG gave a better reproduction for the equimolar mixture $x$($O_{2}$) = 0.5, whereas the GERG-2008 performed significantly better for the oxygen-rich mixture $x$($O_{2}$) = 0.75. The EOS-CG generally overestimates the density, while the GERG-2008 underestimates it. This complete set of new experimental data, together with previous measurements, is used to calculate the virial coefficients $B$($T$, $x$) and $C$($T$, $x$), as well as the second interaction virial coefficient $B_{12}$($T$) for the ($CO_{2}$ + $O_{2}$) system.
{"title":"Thermodynamic characterization of the ($CO_{2}$ + $O_{2}$) binary system for the development of models for CCS processes: Accurate experimental ($p$, $ρ$, $T$) data and virial coefficients","authors":"Daniel Lozano-Martín, David Vega-Maza, M. Carmen Martín, Dirk Tuma, César R. Chamorro","doi":"arxiv-2409.06312","DOIUrl":"https://doi.org/arxiv-2409.06312","url":null,"abstract":"Continuing our study on ($CO_{2}$ + $O_{2}$) mixtures, this work reports new\u0000experimental($p$, $rho$, $T$) data for two oxygen-rich mixtures with mole\u0000fractions $x$($O_{2}$) = (0.50 and 0.75) mol/mol, in the temperature range $T$\u0000= (250-375) K and pressure range $p$ = (0.5-20) MPa, using a single-sinker\u0000densimeter. Experimental density data were compared to two well-established\u0000equation-of-state models: EOS-CG and GERG-2008. In the $p$, $T$-range\u0000investigated, the EOS-CG gave a better reproduction for the equimolar mixture\u0000$x$($O_{2}$) = 0.5, whereas the GERG-2008 performed significantly better for\u0000the oxygen-rich mixture $x$($O_{2}$) = 0.75. The EOS-CG generally overestimates\u0000the density, while the GERG-2008 underestimates it. This complete set of new\u0000experimental data, together with previous measurements, is used to calculate\u0000the virial coefficients $B$($T$, $x$) and $C$($T$, $x$), as well as the second\u0000interaction virial coefficient $B_{12}$($T$) for the ($CO_{2}$ + $O_{2}$)\u0000system.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190287","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Juan Antonio González, Fernando Hevia, Luis Felipe Sanz, Daniel Lozano-Martín, Isaías García de la Fuente, José Carlos Cobos
The CH$_3$(CH$_2$)$_u$COO(CH$_3$)$_v$CH$_3$ + n-alkane mixtures have been investigated on the basis of an experimental database containing effective dipole moments of esters, and excess molar functions of the systems: enthalpies ($H_{text{m}}^{text{E}}$), volumes ($V_{text{m}}^{text{E}}$), isobaric heat capacities ($C_{ptext{m}}^{text{E}}$) and isochoric internal energies ($U_{Vtext{m}}^{text{E}}$) and by means of the application of the Flory model and the Kirkwood-Buff formalism. The situation of the mixtures within the $G_{text{m}}^{text{E}}$ (excess molar Gibbs energy) vs. $H_{text{m}}^{text{E}}$ diagram has also been briefly considered. Results indicate that dispersive interactions are dominant and that steric effects can explain some differences between solutions containing heptane and isomeric esters. Proximity and orientational effects are also discussed in diester + hexane mixtures. In the case of systems with a given alkane and different isomeric polar compounds, orientational effects become weaker in the order: n-alkanone > dialkyl carbonate > n-alkanoate. Results from the Kirkwood-Buff formalism indicate that the number of ester-ester interactions decreases in systems with alkyl ethanoates when the alkyl size increases and that preferential solvation between polar molecules decreases as follows: dialkyl carbonate > n-alkanone > n-alkanoate.
{"title":"Orientational and steric effects in linear alkanoates + N-Alkane mixtures","authors":"Juan Antonio González, Fernando Hevia, Luis Felipe Sanz, Daniel Lozano-Martín, Isaías García de la Fuente, José Carlos Cobos","doi":"arxiv-2409.06347","DOIUrl":"https://doi.org/arxiv-2409.06347","url":null,"abstract":"The CH$_3$(CH$_2$)$_u$COO(CH$_3$)$_v$CH$_3$ + n-alkane mixtures have been\u0000investigated on the basis of an experimental database containing effective\u0000dipole moments of esters, and excess molar functions of the systems: enthalpies\u0000($H_{text{m}}^{text{E}}$), volumes ($V_{text{m}}^{text{E}}$), isobaric heat\u0000capacities ($C_{ptext{m}}^{text{E}}$) and isochoric internal energies\u0000($U_{Vtext{m}}^{text{E}}$) and by means of the application of the Flory model\u0000and the Kirkwood-Buff formalism. The situation of the mixtures within the\u0000$G_{text{m}}^{text{E}}$ (excess molar Gibbs energy) vs.\u0000$H_{text{m}}^{text{E}}$ diagram has also been briefly considered. Results\u0000indicate that dispersive interactions are dominant and that steric effects can\u0000explain some differences between solutions containing heptane and isomeric\u0000esters. Proximity and orientational effects are also discussed in diester +\u0000hexane mixtures. In the case of systems with a given alkane and different\u0000isomeric polar compounds, orientational effects become weaker in the order:\u0000n-alkanone > dialkyl carbonate > n-alkanoate. Results from the Kirkwood-Buff\u0000formalism indicate that the number of ester-ester interactions decreases in\u0000systems with alkyl ethanoates when the alkyl size increases and that\u0000preferential solvation between polar molecules decreases as follows: dialkyl\u0000carbonate > n-alkanone > n-alkanoate.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190286","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Scientific groups are struggling to adapt their codes to quickly-developing GPU-based HPC platforms. The domain of distributed coupled cluster (CC) calculations is not an exception. Moreover, our applications to tiny QED effects require higher-order CC which include thousands of tensor contractions, which makes automatic treatment imperative. The challenge is to allow efficient implementation by capturing key symmetries of the problem, while retaining the abstraction from the hardware. We present the tensor programming framework tenpi, which seeks to find this balance. It features a python library user interface, global optimization of intermediates, a visualization module and Fortran code generator that bridges the DIRAC package for relativistic molecular calculations to tensor contraction libraries. tenpi brings higher-order CC functionality to the massively parallel module of DIRAC. The architecture and design decision schemes are accompanied by benchmarks and by first production calculations on Summit, Frontier and LUMI along with state-of-the-art of tensor contraction software.
{"title":"Generating coupled cluster code for modern distributed memory tensor software","authors":"Jan Brandejs, Johann Pototschnig, Trond Saue","doi":"arxiv-2409.06759","DOIUrl":"https://doi.org/arxiv-2409.06759","url":null,"abstract":"Scientific groups are struggling to adapt their codes to quickly-developing\u0000GPU-based HPC platforms. The domain of distributed coupled cluster (CC)\u0000calculations is not an exception. Moreover, our applications to tiny QED\u0000effects require higher-order CC which include thousands of tensor contractions,\u0000which makes automatic treatment imperative. The challenge is to allow efficient\u0000implementation by capturing key symmetries of the problem, while retaining the\u0000abstraction from the hardware. We present the tensor programming framework\u0000tenpi, which seeks to find this balance. It features a python library user\u0000interface, global optimization of intermediates, a visualization module and\u0000Fortran code generator that bridges the DIRAC package for relativistic\u0000molecular calculations to tensor contraction libraries. tenpi brings\u0000higher-order CC functionality to the massively parallel module of DIRAC. The\u0000architecture and design decision schemes are accompanied by benchmarks and by\u0000first production calculations on Summit, Frontier and LUMI along with\u0000state-of-the-art of tensor contraction software.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Simranjot K. Sapra, Mononita Das, M. Wasim Raja, Jeng-Kuei Chang, Rajendra S. Dhaka
We design a full cell configuration having Na$_{3}$V$_{2}$(PO$_{4}$)$_{3}$ as cathode and pre-sodiated hard carbon as an anode with Cellulosic Paper Separators and compare the electrochemical performance of these ceramic-impregnated polymer-coated cellulose paper separators with commercial glass fiber separator. Notably, the paper-based multilayer separators provide desirable characteristics such as excellent electrolyte wettability, thermal stability up to 200degree C, and ionic conductivity, which are essential for the efficient operation of SIBs. The cellulose separator is coated by a layer of polyvinylidene fluoride polymer, followed by a second layer of styrene butadiene rubber (SBR) polymer in which ferroelectric fillers BaTiO$_{3}$ are integrated, which interacts with the polymer hosts through Lewis acid-base interactions ion and improves the conduction mechanism for the Na$^{+}$ ions. The final lamination is performed by varying the SBR concentrations (0.5, 0.75, and 1.0 w/v%). The incorporated polymer matrices improve the flexibility, adhesion and dispersion of the nanoparticles and affinity of the electrolyte to the electrode. The morphology of the paper separators shows the uniform interconnected fibers with the porous structure. Interestingly, we find that the paper separator with 0.75 w/v% content of SBR exhibit decreased interfacial resistance and improved electrochemical performance, having retention of 62% and nearly 100% Coulombic efficiency up to 240 cycles, as compared to other concentrations. Moreover, we observe the energy density around 376 Wh kg$^{-1}$ (considering cathode weight), which found to be comparable to the commercially available glass fiber separator. Our results demonstrate the potential of these multilayer paper separators towards achieving sustainability and safety in energy storage systems.
{"title":"Flexible Trilayer Cellulosic Paper Separators engineered with BaTiO$_3$ ferroelectric fillers for High Energy Density Sodium-ion Batteries","authors":"Simranjot K. Sapra, Mononita Das, M. Wasim Raja, Jeng-Kuei Chang, Rajendra S. Dhaka","doi":"arxiv-2409.06743","DOIUrl":"https://doi.org/arxiv-2409.06743","url":null,"abstract":"We design a full cell configuration having Na$_{3}$V$_{2}$(PO$_{4}$)$_{3}$ as\u0000cathode and pre-sodiated hard carbon as an anode with Cellulosic Paper\u0000Separators and compare the electrochemical performance of these\u0000ceramic-impregnated polymer-coated cellulose paper separators with commercial\u0000glass fiber separator. Notably, the paper-based multilayer separators provide\u0000desirable characteristics such as excellent electrolyte wettability, thermal\u0000stability up to 200degree C, and ionic conductivity, which are essential for\u0000the efficient operation of SIBs. The cellulose separator is coated by a layer\u0000of polyvinylidene fluoride polymer, followed by a second layer of styrene\u0000butadiene rubber (SBR) polymer in which ferroelectric fillers BaTiO$_{3}$ are\u0000integrated, which interacts with the polymer hosts through Lewis acid-base\u0000interactions ion and improves the conduction mechanism for the Na$^{+}$ ions.\u0000The final lamination is performed by varying the SBR concentrations (0.5, 0.75,\u0000and 1.0 w/v%). The incorporated polymer matrices improve the flexibility,\u0000adhesion and dispersion of the nanoparticles and affinity of the electrolyte to\u0000the electrode. The morphology of the paper separators shows the uniform\u0000interconnected fibers with the porous structure. Interestingly, we find that\u0000the paper separator with 0.75 w/v% content of SBR exhibit decreased\u0000interfacial resistance and improved electrochemical performance, having\u0000retention of 62% and nearly 100% Coulombic efficiency up to 240 cycles, as\u0000compared to other concentrations. Moreover, we observe the energy density\u0000around 376 Wh kg$^{-1}$ (considering cathode weight), which found to be\u0000comparable to the commercially available glass fiber separator. Our results\u0000demonstrate the potential of these multilayer paper separators towards\u0000achieving sustainability and safety in energy storage systems.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Elspeth K. H. Lee, Shang-Min Tsai, Julianne I. Moses, John M. C. Plane, Channon Visscher, Stephen J. Klippenstein
Due to the detection of phosphine PH3 in the Solar System gas giants Jupiter and Saturn, PH3 has long been suggested to be detectable in exosolar substellar atmospheres too. However, to date, a direct detection of phosphine has proven to be elusive in exoplanet atmosphere surveys. We construct an updated phosphorus-hydrogen-oxygen (PHO) photochemical network suitable for simulation of gas giant hydrogen-dominated atmospheres. Using this network, we examine PHO photochemistry in hot Jupiter and warm Neptune exoplanet atmospheres at Solar and enriched metallicities. Our results show for HD 189733b-like hot Jupiters that HOPO, PO and P2 are typically the dominant P carriers at pressures important for transit and emission spectra, rather than PH3. For GJ1214b-like warm Neptune atmospheres our results suggest that at Solar metallicity PH3 is dominant in the absence of photochemistry, but is generally not in high abundance for all other chemical environments. At 10 and 100 times Solar, small oxygenated phosphorus molecules such as HOPO and PO dominate for both thermochemical and photochemical simulations. The network is able to reproduce well the observed PH3 abundances on Jupiter and Saturn. Despite progress in improving the accuracy of the PHO network, large portions of the reaction rate data remain with approximate, uncertain or missing values, which could change the conclusions of the current study significantly. Improving understanding of the kinetics of phosphorus-bearing chemical reactions will be a key undertaking for astronomers aiming to detect phosphine and other phosphorus species in both rocky and gaseous exoplanetary atmospheres in the near future.
{"title":"A photochemical PHO network for hydrogen-dominated exoplanet atmospheres","authors":"Elspeth K. H. Lee, Shang-Min Tsai, Julianne I. Moses, John M. C. Plane, Channon Visscher, Stephen J. Klippenstein","doi":"arxiv-2409.06802","DOIUrl":"https://doi.org/arxiv-2409.06802","url":null,"abstract":"Due to the detection of phosphine PH3 in the Solar System gas giants Jupiter\u0000and Saturn, PH3 has long been suggested to be detectable in exosolar substellar\u0000atmospheres too. However, to date, a direct detection of phosphine has proven\u0000to be elusive in exoplanet atmosphere surveys. We construct an updated\u0000phosphorus-hydrogen-oxygen (PHO) photochemical network suitable for simulation\u0000of gas giant hydrogen-dominated atmospheres. Using this network, we examine PHO\u0000photochemistry in hot Jupiter and warm Neptune exoplanet atmospheres at Solar\u0000and enriched metallicities. Our results show for HD 189733b-like hot Jupiters\u0000that HOPO, PO and P2 are typically the dominant P carriers at pressures\u0000important for transit and emission spectra, rather than PH3. For GJ1214b-like\u0000warm Neptune atmospheres our results suggest that at Solar metallicity PH3 is\u0000dominant in the absence of photochemistry, but is generally not in high\u0000abundance for all other chemical environments. At 10 and 100 times Solar, small\u0000oxygenated phosphorus molecules such as HOPO and PO dominate for both\u0000thermochemical and photochemical simulations. The network is able to reproduce\u0000well the observed PH3 abundances on Jupiter and Saturn. Despite progress in\u0000improving the accuracy of the PHO network, large portions of the reaction rate\u0000data remain with approximate, uncertain or missing values, which could change\u0000the conclusions of the current study significantly. Improving understanding of\u0000the kinetics of phosphorus-bearing chemical reactions will be a key undertaking\u0000for astronomers aiming to detect phosphine and other phosphorus species in both\u0000rocky and gaseous exoplanetary atmospheres in the near future.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
I study the influence of temperature and the crack-tip velocity of the bond breaking at the crack tip in rubber-like materials. The bond breaking is considered as a stress-aided thermally activated process and result in an effective crack propagation energy which increases strongly with decreasing temperature or increasing crack-tip speed. This effect is particular important for adhesive (interfacial) crack propagation but less important for cohesive crack propagation owing to the much larger bond-breaking energies in the latter case. For adhesive cracks the theory results are consistent with adhesion measurements for silicone (PDMS) rubber in contact with silica glass surfaces. For cohesive cracks the theory agree well with experimental results PDMS films chemically bound to silinized glass.
{"title":"Influence of temperature and crack-tip speed on crack propagation in elastic solids","authors":"B. N. J. Persson","doi":"arxiv-2409.06182","DOIUrl":"https://doi.org/arxiv-2409.06182","url":null,"abstract":"I study the influence of temperature and the crack-tip velocity of the bond\u0000breaking at the crack tip in rubber-like materials. The bond breaking is\u0000considered as a stress-aided thermally activated process and result in an\u0000effective crack propagation energy which increases strongly with decreasing\u0000temperature or increasing crack-tip speed. This effect is particular important\u0000for adhesive (interfacial) crack propagation but less important for cohesive\u0000crack propagation owing to the much larger bond-breaking energies in the latter\u0000case. For adhesive cracks the theory results are consistent with adhesion\u0000measurements for silicone (PDMS) rubber in contact with silica glass surfaces.\u0000For cohesive cracks the theory agree well with experimental results PDMS films\u0000chemically bound to silinized glass.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190289","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Carlo Kleine, Marc-Oliver Winghart, Zhuang-Yan Zhang, Maria Richter, Maria Ekimova, Sebastian Eckert, Marc J. J. Vrakking, Erik T. J. Nibbering, Arnaud Rouzee, Edward R. Grant
Air-lasing from single ionized N$_2^+$ molecules induced by laser filamentation in air has been intensively investigated and the mechanisms responsible for lasing are currently highly debated. We use ultrafast nitrogen K-edge spectroscopy to follow the strong field ionization and fragmentation dynamics of N$_2$ upon interaction with an ultrashort 800 nm laser pulse. Using probe pulses generated by extreme high-order harmonic generation, we observe transitions indicative of the formation of the electronic ground X$^2Sigma_{g}^{+}$, first excited A$^2Pi_u$ and second excited B$^2Sigma^+_u$ states of N$_2^+$ on femtosecond time scales, from which we can quantitatively determine the time-dependent electronic state population distribution dynamics of N$_2^+$. Our results show a remarkably low population of the A$^2Pi_u$ state, and nearly equal populations of the X$^2Sigma_{g}^{+}$ and B$^2Sigma^+_u$ states. In addition, we observe fragmentation of N$_2^+$ into N and N$^+$ on a time scale of several tens of picoseconds that we assign to significant collisional dynamics in the plasma, resulting in dissociative excitation of N$_2^+$.
{"title":"Electronic State Population Dynamics upon Ultrafast Strong Field Ionization and Fragmentation of Molecular Nitrogen","authors":"Carlo Kleine, Marc-Oliver Winghart, Zhuang-Yan Zhang, Maria Richter, Maria Ekimova, Sebastian Eckert, Marc J. J. Vrakking, Erik T. J. Nibbering, Arnaud Rouzee, Edward R. Grant","doi":"arxiv-2409.06757","DOIUrl":"https://doi.org/arxiv-2409.06757","url":null,"abstract":"Air-lasing from single ionized N$_2^+$ molecules induced by laser\u0000filamentation in air has been intensively investigated and the mechanisms\u0000responsible for lasing are currently highly debated. We use ultrafast nitrogen\u0000K-edge spectroscopy to follow the strong field ionization and fragmentation\u0000dynamics of N$_2$ upon interaction with an ultrashort 800 nm laser pulse. Using\u0000probe pulses generated by extreme high-order harmonic generation, we observe\u0000transitions indicative of the formation of the electronic ground\u0000X$^2Sigma_{g}^{+}$, first excited A$^2Pi_u$ and second excited\u0000B$^2Sigma^+_u$ states of N$_2^+$ on femtosecond time scales, from which we can\u0000quantitatively determine the time-dependent electronic state population\u0000distribution dynamics of N$_2^+$. Our results show a remarkably low population\u0000of the A$^2Pi_u$ state, and nearly equal populations of the\u0000X$^2Sigma_{g}^{+}$ and B$^2Sigma^+_u$ states. In addition, we observe\u0000fragmentation of N$_2^+$ into N and N$^+$ on a time scale of several tens of\u0000picoseconds that we assign to significant collisional dynamics in the plasma,\u0000resulting in dissociative excitation of N$_2^+$.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190255","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：