Daniel Lozano-Martín, José J. Segovia, M. Carmen Martín, Teresa Fernández-Vicente, D. del Campo
The present work aims to measure speeds of sound $c$ in a biogas mixture of $CH_{4}$ + $N_{2}$ + $CO_{2}$ + $CO$, at $p$ = (1-12) MPa and $T$ = (273, 300 and 325) K, using a spherical acoustical resonator. The results are fitted to the virial acoustic equation of state, and the virial acoustic coefficients are obtained, $beta_{a}$ and $gamma_{a}$ and extrapolated to zero pressure, determining the adiabatic coefficient as perfect gas, $gamma^{pg}$, and the isobaric and isochoric heat capacities as perfect gas, $C_{p}^{pg}$ and $C_{V}^{pg}$, respectively. The speeds of sound are acquired with a mean expanded relative uncertainty of 165 parts in $10^{6}$ ($k$ = 2) and are compared with the results predicted by the reference equation of state for this kind of mixture (natural gas-like mixtures), EoS GERG-2008. Relative deviations between experimental data and values estimated by this model were less than 700 parts in $10^{6}$ at $T$ = 325 K, and below 400 parts in $10^{6}$, and within measurement uncertainty of at $T$ = 300 K, although appreciably higher at isotherm $T$ = 273 K at the highest pressure data for this work, and even reaching values above 3 400 parts in $10^{6}$.
{"title":"Speeds of sound for a biogas mixture $CH_{4}$ + $N_{2}$ + $CO_{2}$ + $CO$ from $p$ = (1-12) MPa at $T$ = (273, 300 and 325) K measured with a spherical resonator","authors":"Daniel Lozano-Martín, José J. Segovia, M. Carmen Martín, Teresa Fernández-Vicente, D. del Campo","doi":"arxiv-2409.10962","DOIUrl":"https://doi.org/arxiv-2409.10962","url":null,"abstract":"The present work aims to measure speeds of sound $c$ in a biogas mixture of\u0000$CH_{4}$ + $N_{2}$ + $CO_{2}$ + $CO$, at $p$ = (1-12) MPa and $T$ = (273, 300\u0000and 325) K, using a spherical acoustical resonator. The results are fitted to\u0000the virial acoustic equation of state, and the virial acoustic coefficients are\u0000obtained, $beta_{a}$ and $gamma_{a}$ and extrapolated to zero pressure,\u0000determining the adiabatic coefficient as perfect gas, $gamma^{pg}$, and the\u0000isobaric and isochoric heat capacities as perfect gas, $C_{p}^{pg}$ and\u0000$C_{V}^{pg}$, respectively. The speeds of sound are acquired with a mean\u0000expanded relative uncertainty of 165 parts in $10^{6}$ ($k$ = 2) and are\u0000compared with the results predicted by the reference equation of state for this\u0000kind of mixture (natural gas-like mixtures), EoS GERG-2008. Relative deviations\u0000between experimental data and values estimated by this model were less than 700\u0000parts in $10^{6}$ at $T$ = 325 K, and below 400 parts in $10^{6}$, and within\u0000measurement uncertainty of at $T$ = 300 K, although appreciably higher at\u0000isotherm $T$ = 273 K at the highest pressure data for this work, and even\u0000reaching values above 3 400 parts in $10^{6}$.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142258129","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}
Johnny Zambrano, Franklin V. Gómez-Soto, Daniel Lozano-Martín, M. Carmen Martín, José J. Segovia
The interest of oil industry in increasing heavy oil production has promoted the use of enhanced oil recovery techniques such as $CO_{2}$ injection, which produce a decrease of oil viscosity and displacement of heavy oil from reservoir to surface. The design of these processes requires accurate data of densities, viscosities or surface tensions of ($CO_{2}$ + hydrocarbon) mixtures in order to simulate the behaviour of these mixtures in the reservoir. An automated Anton Paar DMA HPM vibrating-tube densimeter was used to measure densities of this kind of mixtures, and a new mixture injection system, by means of two syringe pumps, was developed for the densimeter. The equipment operates at high pressure, which is controlled through a back pressure valve and a variable volume cylinder with a stepper motor. The estimated standard uncertainty of the density is $mathrm{pm0.9 kg cdot m^{-3}}$ at temperatures below 373.15 K and pressure range (0.1-140) MPa.In this paper, the densities of the mixtures ($CO_{2}$ + $n$-decane), ($CO_{2}$ + $n$-dodecane) and ($CO_{2}$ + squalane) are reported at $T$ = (283.15-393.15) K and $p$ = (10-100) MPa.
{"title":"Volumetric behaviour of (carbon dioxide + hydrocarbon) mixtures at high pressures","authors":"Johnny Zambrano, Franklin V. Gómez-Soto, Daniel Lozano-Martín, M. Carmen Martín, José J. Segovia","doi":"arxiv-2409.10973","DOIUrl":"https://doi.org/arxiv-2409.10973","url":null,"abstract":"The interest of oil industry in increasing heavy oil production has promoted\u0000the use of enhanced oil recovery techniques such as $CO_{2}$ injection, which\u0000produce a decrease of oil viscosity and displacement of heavy oil from\u0000reservoir to surface. The design of these processes requires accurate data of\u0000densities, viscosities or surface tensions of ($CO_{2}$ + hydrocarbon) mixtures\u0000in order to simulate the behaviour of these mixtures in the reservoir. An\u0000automated Anton Paar DMA HPM vibrating-tube densimeter was used to measure\u0000densities of this kind of mixtures, and a new mixture injection system, by\u0000means of two syringe pumps, was developed for the densimeter. The equipment\u0000operates at high pressure, which is controlled through a back pressure valve\u0000and a variable volume cylinder with a stepper motor. The estimated standard\u0000uncertainty of the density is $mathrm{pm0.9 kg cdot m^{-3}}$ at\u0000temperatures below 373.15 K and pressure range (0.1-140) MPa.In this paper, the\u0000densities of the mixtures ($CO_{2}$ + $n$-decane), ($CO_{2}$ + $n$-dodecane)\u0000and ($CO_{2}$ + squalane) are reported at $T$ = (283.15-393.15) K and $p$ =\u0000(10-100) MPa.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269439","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}
We propose a novel approach to electron correlation for multireference systems. It is based on particle-hole (ph) and particle-particle (pp) theories in the second-order, developed in the random phase approximation (RPA) framework for multireference wavefunctions. We show a formal correspondence (duality), between contributions to the correlation energy in the ph and pp pictures. It allows us to describe correlation energy by rigorously combining pp and ph terms, avoiding correlation double counting. The multireference ph, pp, and the combined correlation methods are applied to ground and excited states of systems in the intermediate and strong correlation regimes and compared with the multireference second-order perturbation method (MRPT2). It is shown that the pp approximation fails to describe dissociation of multiple bonds. The ph-pp combined method is overall superior to both ph and pp alone. It parallels good accuracy of the second-order perturbation theory for ground states and singlet excitation energies. For the singlet-triplet gaps of biradicals its accuracy is significantly better. This is impressive, taking into account that it relies only on one- and two-body density matrices, while MRPT2 methods typically require density matrices up to the four-body.
{"title":"Duality of particle-hole and particle-particle theories for strongly correlated electronic systems","authors":"Aleksandra Tucholska, Yang Guo, Katarzyna Pernal","doi":"arxiv-2409.11284","DOIUrl":"https://doi.org/arxiv-2409.11284","url":null,"abstract":"We propose a novel approach to electron correlation for multireference\u0000systems. It is based on particle-hole (ph) and particle-particle (pp) theories\u0000in the second-order, developed in the random phase approximation (RPA)\u0000framework for multireference wavefunctions. We show a formal correspondence\u0000(duality), between contributions to the correlation energy in the ph and pp\u0000pictures. It allows us to describe correlation energy by rigorously combining\u0000pp and ph terms, avoiding correlation double counting. The multireference ph,\u0000pp, and the combined correlation methods are applied to ground and excited\u0000states of systems in the intermediate and strong correlation regimes and\u0000compared with the multireference second-order perturbation method (MRPT2). It\u0000is shown that the pp approximation fails to describe dissociation of multiple\u0000bonds. The ph-pp combined method is overall superior to both ph and pp alone.\u0000It parallels good accuracy of the second-order perturbation theory for ground\u0000states and singlet excitation energies. For the singlet-triplet gaps of\u0000biradicals its accuracy is significantly better. This is impressive, taking\u0000into account that it relies only on one- and two-body density matrices, while\u0000MRPT2 methods typically require density matrices up to the four-body.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142258127","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}
J J Segovia, D Lozano-Martín, M C Martín, C R Chamorro, M A Villamañán, E Pérez, C García Izquierdo, D del Campo
A new determination of the molar gas constant was performed from measurements of the speed of sound in argon at the triple point of water and extrapolation to zero pressure. A new resonant cavity was used. This is a triaxial ellipsoid whose walls are gold-coated steel and which is divided into two identical halves that are bolted and sealed with an O-ring. Microwave and electroacoustic traducers are located in the northern and southern parts of the cavity, respectively, so that measurements of microwave and acoustic frequencies are carried out in the same experiment. Measurements were taken at pressures from 600 kPa to 60 kPa and at 273.16 K. The internal equivalent radius of the cavity was accurately determined by microwave measurements and the first four radial symmetric acoustic modes were simultaneously measured and used to calculate the speed of sound. The improvements made using the new cavity have reduced by half the main contributions to the uncertainty due to the radius determination using microwave measurements which amounts to 4.7 parts in $10^{6}$ and the acoustic measurements, 4.4 parts in $10^{6}$, where the main contribution (3.7 parts in $10^{6}$) is the relative excess half-widths associated with the limit of our acoustic model, compared with our previous measurements. As a result of all the improvements with the new cavity and the measurements performed, we determined the molar gas constant $R$ = (8.314 449 $pm$ 0.000 056) J/(K mol) which corresponds to a relative standard uncertainty of 6.7 parts in $10^{6}$. The value reported in this paper lies -1.3 parts in $10^{6}$ below the recommended value of CODATA 2014, although still within the range consistent with it.
{"title":"Updated determination of the molar gas constant $R$ by acoustic measurements in argon at UVa-CEM","authors":"J J Segovia, D Lozano-Martín, M C Martín, C R Chamorro, M A Villamañán, E Pérez, C García Izquierdo, D del Campo","doi":"arxiv-2409.10140","DOIUrl":"https://doi.org/arxiv-2409.10140","url":null,"abstract":"A new determination of the molar gas constant was performed from measurements\u0000of the speed of sound in argon at the triple point of water and extrapolation\u0000to zero pressure. A new resonant cavity was used. This is a triaxial ellipsoid\u0000whose walls are gold-coated steel and which is divided into two identical\u0000halves that are bolted and sealed with an O-ring. Microwave and electroacoustic\u0000traducers are located in the northern and southern parts of the cavity,\u0000respectively, so that measurements of microwave and acoustic frequencies are\u0000carried out in the same experiment. Measurements were taken at pressures from\u0000600 kPa to 60 kPa and at 273.16 K. The internal equivalent radius of the cavity\u0000was accurately determined by microwave measurements and the first four radial\u0000symmetric acoustic modes were simultaneously measured and used to calculate the\u0000speed of sound. The improvements made using the new cavity have reduced by half\u0000the main contributions to the uncertainty due to the radius determination using\u0000microwave measurements which amounts to 4.7 parts in $10^{6}$ and the acoustic\u0000measurements, 4.4 parts in $10^{6}$, where the main contribution (3.7 parts in\u0000$10^{6}$) is the relative excess half-widths associated with the limit of our\u0000acoustic model, compared with our previous measurements. As a result of all the\u0000improvements with the new cavity and the measurements performed, we determined\u0000the molar gas constant $R$ = (8.314 449 $pm$ 0.000 056) J/(K mol) which\u0000corresponds to a relative standard uncertainty of 6.7 parts in $10^{6}$. The\u0000value reported in this paper lies -1.3 parts in $10^{6}$ below the recommended\u0000value of CODATA 2014, although still within the range consistent with it.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269442","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}
Ofir Tal-Friedman, Tommer D. Keidar, Shlomi Reuveni, Yael Roichman
Stochastic resetting, a method for accelerating target search in random processes, often incurs temporal and energetic costs. For a diffusing particle, a lower bound exists for the energetic cost of reaching the target, which is attained at low resetting rates and equals the direct linear transportation cost against fluid drag. Here, we study ``smart resetting," a strategy that aims to beat this lower bound. By strategically resetting the particle only when this benefits its progress toward the target, smart resetting leverages information to minimize energy consumption. We analytically calculate the energetic cost per mean first passage time and show that smart resetting consistently reduces the energetic cost compared to regular resetting. Surprisingly, smart resting achieves the minimum energy cost previously established for regular resetting, irrespective of the resetting rate. Yet, it fails to reduce this cost further. We extend our findings in two ways: first, by examining nonlinear energetic cost functions, and second, by considering smart resetting of drift-diffusion processes.
{"title":"Smart Resetting: An Energy-Efficient Strategy for Stochastic Search Processes","authors":"Ofir Tal-Friedman, Tommer D. Keidar, Shlomi Reuveni, Yael Roichman","doi":"arxiv-2409.10108","DOIUrl":"https://doi.org/arxiv-2409.10108","url":null,"abstract":"Stochastic resetting, a method for accelerating target search in random\u0000processes, often incurs temporal and energetic costs. For a diffusing particle,\u0000a lower bound exists for the energetic cost of reaching the target, which is\u0000attained at low resetting rates and equals the direct linear transportation\u0000cost against fluid drag. Here, we study ``smart resetting,\" a strategy that\u0000aims to beat this lower bound. By strategically resetting the particle only\u0000when this benefits its progress toward the target, smart resetting leverages\u0000information to minimize energy consumption. We analytically calculate the\u0000energetic cost per mean first passage time and show that smart resetting\u0000consistently reduces the energetic cost compared to regular resetting.\u0000Surprisingly, smart resting achieves the minimum energy cost previously\u0000established for regular resetting, irrespective of the resetting rate. Yet, it\u0000fails to reduce this cost further. We extend our findings in two ways: first,\u0000by examining nonlinear energetic cost functions, and second, by considering\u0000smart resetting of drift-diffusion processes.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142258191","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}
Lalith Krishna Samanth Bonagiri, Amir Farokh Payam, Narayana R. Aluru, Yingjie Zhang
Electrode-electrolyte interfaces are crucial for electrochemical energy conversion and storage. At these interfaces, the liquid electrolytes form electrical double layers (EDLs). However, despite more than a century of active research, the fundamental structure of EDLs remains elusive to date. Experimental characterization and theoretical calculations have both provided insights, yet each method by itself only offers incomplete or inexact information of the multifaceted EDL structure. Here we provide a survey of the mainstream approaches for EDL quantification, with a particular focus on the emerging 3D atomic force microscopy (3D-AFM) imaging which provides real-space atomic-scale EDL structures. To overcome the existing limits of EDL characterization methods, we propose a new approach to integrate 3D-AFM with classical molecular dynamics (MD) simulation, to enable realistic, precise, and high-throughput determination and prediction of EDL structures. As examples of real-world application, we will discuss the feasibility of using this joint experiment-theory method to unravel the EDL structure at various carbon-based electrodes for supercapacitors, batteries, and electrocatalysis. Looking forward, we believe 3D-AFM, future versions of scanning probe microscopy, and their integration with theory offer promising platforms to profile liquid structures in many electrochemical systems.
{"title":"Integrating Experiment with Theory to Determine the Structure of Electrode-Electrolyte Interfaces","authors":"Lalith Krishna Samanth Bonagiri, Amir Farokh Payam, Narayana R. Aluru, Yingjie Zhang","doi":"arxiv-2409.10008","DOIUrl":"https://doi.org/arxiv-2409.10008","url":null,"abstract":"Electrode-electrolyte interfaces are crucial for electrochemical energy\u0000conversion and storage. At these interfaces, the liquid electrolytes form\u0000electrical double layers (EDLs). However, despite more than a century of active\u0000research, the fundamental structure of EDLs remains elusive to date.\u0000Experimental characterization and theoretical calculations have both provided\u0000insights, yet each method by itself only offers incomplete or inexact\u0000information of the multifaceted EDL structure. Here we provide a survey of the\u0000mainstream approaches for EDL quantification, with a particular focus on the\u0000emerging 3D atomic force microscopy (3D-AFM) imaging which provides real-space\u0000atomic-scale EDL structures. To overcome the existing limits of EDL\u0000characterization methods, we propose a new approach to integrate 3D-AFM with\u0000classical molecular dynamics (MD) simulation, to enable realistic, precise, and\u0000high-throughput determination and prediction of EDL structures. As examples of\u0000real-world application, we will discuss the feasibility of using this joint\u0000experiment-theory method to unravel the EDL structure at various carbon-based\u0000electrodes for supercapacitors, batteries, and electrocatalysis. Looking\u0000forward, we believe 3D-AFM, future versions of scanning probe microscopy, and\u0000their integration with theory offer promising platforms to profile liquid\u0000structures in many electrochemical systems.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142258134","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}
Thomas P. Fay, Nicolas Ferré, Miquel Huix-Rotllant
Electronic polarization and dispersion are decisive actors in determining interaction energies between molecules. These interactions have a particularly profound effect on excitation energies of molecules in complex environments, especially when the excitation involves a significant degree of charge reorganisation. The direct reaction field (DRF) approach, which has seen a recent revival of interest, provides a powerful framework for describing these interactions in quantum mechanics/molecular mechanics (QM/MM) models of systems, where a small subsystem of interest is described using quantum chemical methods and the remainder is treated with a simple MM force field. In this paper we show how the DRF approach can be combined with the electrostatic potential fitted (ESPF) multipole operator description of the QM region charge density, which reduces the scaling $mathcal{O}(N_mathrm{MM}^3)$ of the method with MM system to $mathcal{O}(N_mathrm{MM}^2)$. We also show how the DRF approach can be combined with fluctuating charge descriptions of the polarizable environment, as well as previously used atom-centred dipole-polarizability based models. We further show that the ESPF-DRF method provides an accurate description of molecular interactions in both ground and excited electronic states of the QM system and apply it to predict the gas to aqueous solution solvatochromic shifts in the UV/visible absorption spectrum of acrolein.
电子极化和色散是决定分子间相互作用能量的决定性因素。这些相互作用对分子在复杂环境中的激发能量具有特别重要的影响，尤其是当激发涉及到很大程度的电荷重组时。直接反应场（DRF）方法近来重新受到关注，它为描述量子力学/分子力学（QM/MM）系统模型中的这些相互作用提供了一个强大的框架，其中一小部分感兴趣的子系统使用量子化学方法进行描述，其余部分则使用简单的 MM 力场进行处理。在本文中，我们展示了 DRF 方法如何与静电势拟合（ESPF）多极算子描述的 QM 区域带电强度相结合，从而将方法与 MM 系统的缩放 $/mathcal{O}(N_mathrm{MM}^3)$降低到 $/mathcal{O}(N_mathrm{MM}^2)$。我们还展示了 DRF 方法如何与可极化环境的波动电荷描述以及之前使用的基于原子-中心-偶极子-可极化性的模型相结合。我们进一步证明了 ESPF-DRF 方法能准确描述 QM 系统基态和激发态电子中的分子相互作用，并将其用于预测丙烯醛紫外/可见吸收光谱中气体到水溶液溶解的色移。
{"title":"Efficient polarizable QM/MM using the direct reaction field Hamiltonian with electrostatic potential fitted multipole operators","authors":"Thomas P. Fay, Nicolas Ferré, Miquel Huix-Rotllant","doi":"arxiv-2409.10483","DOIUrl":"https://doi.org/arxiv-2409.10483","url":null,"abstract":"Electronic polarization and dispersion are decisive actors in determining\u0000interaction energies between molecules. These interactions have a particularly\u0000profound effect on excitation energies of molecules in complex environments,\u0000especially when the excitation involves a significant degree of charge\u0000reorganisation. The direct reaction field (DRF) approach, which has seen a\u0000recent revival of interest, provides a powerful framework for describing these\u0000interactions in quantum mechanics/molecular mechanics (QM/MM) models of\u0000systems, where a small subsystem of interest is described using quantum\u0000chemical methods and the remainder is treated with a simple MM force field. In\u0000this paper we show how the DRF approach can be combined with the electrostatic\u0000potential fitted (ESPF) multipole operator description of the QM region charge\u0000density, which reduces the scaling $mathcal{O}(N_mathrm{MM}^3)$ of the method\u0000with MM system to $mathcal{O}(N_mathrm{MM}^2)$. We also show how the DRF\u0000approach can be combined with fluctuating charge descriptions of the\u0000polarizable environment, as well as previously used atom-centred\u0000dipole-polarizability based models. We further show that the ESPF-DRF method\u0000provides an accurate description of molecular interactions in both ground and\u0000excited electronic states of the QM system and apply it to predict the gas to\u0000aqueous solution solvatochromic shifts in the UV/visible absorption spectrum of\u0000acrolein.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269441","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}
Austin Cheng, Cher Tian Ser, Marta Skreta, Andrés Guzmán-Cordero, Luca Thiede, Andreas Burger, Abdulrahman Aldossary, Shi Xuan Leong, Sergio Pablo-García, Felix Strieth-Kalthoff, Alán Aspuru-Guzik
Machine learning has been pervasively touching many fields of science. Chemistry and materials science are no exception. While machine learning has been making a great impact, it is still not reaching its full potential or maturity. In this perspective, we first outline current applications across a diversity of problems in chemistry. Then, we discuss how machine learning researchers view and approach problems in the field. Finally, we provide our considerations for maximizing impact when researching machine learning for chemistry.
{"title":"How to do impactful research in artificial intelligence for chemistry and materials science","authors":"Austin Cheng, Cher Tian Ser, Marta Skreta, Andrés Guzmán-Cordero, Luca Thiede, Andreas Burger, Abdulrahman Aldossary, Shi Xuan Leong, Sergio Pablo-García, Felix Strieth-Kalthoff, Alán Aspuru-Guzik","doi":"arxiv-2409.10304","DOIUrl":"https://doi.org/arxiv-2409.10304","url":null,"abstract":"Machine learning has been pervasively touching many fields of science.\u0000Chemistry and materials science are no exception. While machine learning has\u0000been making a great impact, it is still not reaching its full potential or\u0000maturity. In this perspective, we first outline current applications across a\u0000diversity of problems in chemistry. Then, we discuss how machine learning\u0000researchers view and approach problems in the field. Finally, we provide our\u0000considerations for maximizing impact when researching machine learning for\u0000chemistry.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142258137","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}
Xintong Zhao, Kyle Langlois, Jacob Furst, Yuan An, Xiaohua Hu, Diego Gomez Gualdron, Fernando Uribe-Romo, Jane Greenberg
This paper reports on a scientometric analysis bolstered by human in the loop, domain experts, to examine the field of metal organic frameworks (MOFs) research. Scientometric analyses reveal the intellectual landscape of a field. The study engaged MOF scientists in the design and review of our research workflow. MOF materials are an essential component in next generation renewable energy storage and biomedical technologies. The research approach demonstrates how engaging experts, via human in the loop processes, can help develop a comprehensive view of a field research trends, influential works, and specialized topics.
{"title":"Research evolution of metal organic frameworks: A scientometric approach with human-in-the-loop","authors":"Xintong Zhao, Kyle Langlois, Jacob Furst, Yuan An, Xiaohua Hu, Diego Gomez Gualdron, Fernando Uribe-Romo, Jane Greenberg","doi":"arxiv-2409.10776","DOIUrl":"https://doi.org/arxiv-2409.10776","url":null,"abstract":"This paper reports on a scientometric analysis bolstered by human in the\u0000loop, domain experts, to examine the field of metal organic frameworks (MOFs)\u0000research. Scientometric analyses reveal the intellectual landscape of a field.\u0000The study engaged MOF scientists in the design and review of our research\u0000workflow. MOF materials are an essential component in next generation renewable\u0000energy storage and biomedical technologies. The research approach demonstrates\u0000how engaging experts, via human in the loop processes, can help develop a\u0000comprehensive view of a field research trends, influential works, and\u0000specialized topics.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269440","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}
Fernando Hevia, Juan Antonio González, Cristina Alonso Tristán, Isaías García de la Fuente, Luis Felipe Sanz
Interactions and structure of alkanone, or alkanal or dialkyl carbonate + alkane mixtures, or of 2-alkanone+ 2-alkanone, or of ketone + dialkyl carbonate systems have been investigated by means of a set of thermodynamic properties and by the application of the Flory model. The properties considered are excess molar quantities: enthalpies, $H_{text{m}}^{text{E}}$, volumes, $V_{text{m}}^{text{E}}$, or isobaric heat capacities, $C_{p text{m}}^{text{E}}$, and liquid-liquid equilibria. Experimental data show that alkane mixtures are characterized by rather strong dipolar interactions. In the case of systems containing ketones with the same number of C atoms and a given alkane, dipolar interactions become weaker in the sequence: aromatic > cyclic > linear. In addition, the mentioned interactions become also weaker in the order: dialkyl carbonate > linear alkanone > linear alkanal. This is an important result, as carbonates show lower effective dipole moments than the other compounds, and it suggests that the group size may be relevant when evaluating thermodynamic properties of liquid mixtures. Results on $H_{text{m}}^{text{E}}$ from the Flory model show that orientational effects (i.e., non-random mixing) are rather similar for systems with linear, cyclic or aromatic ketones or alkanals and alkanes. In contrast, orientational effects become weaker in dialkyl carbonate + alkane mixtures. The behaviour of 2-alkanone + 2-alkanone systems and of mixtures of longer 2-alkanones or cyclohexanone with dialkyl carbonate is close to random mixing. Larger orientational effects are encountered in solutions of carbonates and shorter 2-alkanones.
{"title":"Orientational effects in alkanone, alkanal or dialkyl carbonate + alkane mixtures and in alkanone + alkanone or + dialkyl carbonate systems","authors":"Fernando Hevia, Juan Antonio González, Cristina Alonso Tristán, Isaías García de la Fuente, Luis Felipe Sanz","doi":"arxiv-2409.10149","DOIUrl":"https://doi.org/arxiv-2409.10149","url":null,"abstract":"Interactions and structure of alkanone, or alkanal or dialkyl carbonate +\u0000alkane mixtures, or of 2-alkanone+ 2-alkanone, or of ketone + dialkyl carbonate\u0000systems have been investigated by means of a set of thermodynamic properties\u0000and by the application of the Flory model. The properties considered are excess\u0000molar quantities: enthalpies, $H_{text{m}}^{text{E}}$, volumes,\u0000$V_{text{m}}^{text{E}}$, or isobaric heat capacities, $C_{p\u0000text{m}}^{text{E}}$, and liquid-liquid equilibria. Experimental data show\u0000that alkane mixtures are characterized by rather strong dipolar interactions.\u0000In the case of systems containing ketones with the same number of C atoms and a\u0000given alkane, dipolar interactions become weaker in the sequence: aromatic >\u0000cyclic > linear. In addition, the mentioned interactions become also weaker in\u0000the order: dialkyl carbonate > linear alkanone > linear alkanal. This is an\u0000important result, as carbonates show lower effective dipole moments than the\u0000other compounds, and it suggests that the group size may be relevant when\u0000evaluating thermodynamic properties of liquid mixtures. Results on\u0000$H_{text{m}}^{text{E}}$ from the Flory model show that orientational effects\u0000(i.e., non-random mixing) are rather similar for systems with linear, cyclic or\u0000aromatic ketones or alkanals and alkanes. In contrast, orientational effects\u0000become weaker in dialkyl carbonate + alkane mixtures. The behaviour of\u00002-alkanone + 2-alkanone systems and of mixtures of longer 2-alkanones or\u0000cyclohexanone with dialkyl carbonate is close to random mixing. Larger\u0000orientational effects are encountered in solutions of carbonates and shorter\u00002-alkanones.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269225","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：