arXiv - PHYS - Chemical Physics最新文献_第2页

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 用球形谐振器测量的沼气混合物 $CH_{4}$ + $N_{2}$ + $CO_{2}$ + $CO$ 在 $T$ = (273、300 和 325) K 条件下从 $p$ = (1-12) MPa 产生的声速

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-17 DOI: arxiv-2409.10962

Daniel Lozano-Martín, José J. Segovia, M. Carmen Martín, Teresa Fernández-Vicente, D. del Campo

{"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}

引用次数: 0

Volumetric behaviour of (carbon dioxide + hydrocarbon) mixtures at high pressures 二氧化碳+碳氢化合物）混合物在高压下的体积特性

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-17 DOI: arxiv-2409.10973

Johnny Zambrano, Franklin V. Gómez-Soto, Daniel Lozano-Martín, M. Carmen Martín, José J. Segovia

{"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}

引用次数: 0

Duality of particle-hole and particle-particle theories for strongly correlated electronic systems 强相关电子系统的粒子-空穴和粒子-粒子理论的二重性

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-17 DOI: arxiv-2409.11284

Aleksandra Tucholska, Yang Guo, Katarzyna Pernal

{"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}

引用次数: 0

Updated determination of the molar gas constant $R$ by acoustic measurements in argon at UVa-CEM 通过 UVa-CEM 在氩气中的声学测量更新确定摩尔气体常数 $R$

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-16 DOI: arxiv-2409.10140

J J Segovia, D Lozano-Martín, M C Martín, C R Chamorro, M A Villamañán, E Pérez, C García Izquierdo, D del Campo

{"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}

引用次数: 0

Smart Resetting: An Energy-Efficient Strategy for Stochastic Search Processes 智能重置：随机搜索过程的节能策略

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-16 DOI: arxiv-2409.10108

Ofir Tal-Friedman, Tommer D. Keidar, Shlomi Reuveni, Yael Roichman

{"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}

引用次数: 0

Integrating Experiment with Theory to Determine the Structure of Electrode-Electrolyte Interfaces 将实验与理论相结合，确定电极-电解质界面的结构

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-16 DOI: arxiv-2409.10008

Lalith Krishna Samanth Bonagiri, Amir Farokh Payam, Narayana R. Aluru, Yingjie Zhang

{"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}

引用次数: 0

Efficient polarizable QM/MM using the direct reaction field Hamiltonian with electrostatic potential fitted multipole operators 使用带静电势拟合多极算子的直接反应场哈密顿的高效可极化 QM/MM

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-16 DOI: arxiv-2409.10483

Thomas P. Fay, Nicolas Ferré, Miquel Huix-Rotllant

{"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}

引用次数: 0

How to do impactful research in artificial intelligence for chemistry and materials science 如何在化学和材料科学领域开展有影响力的人工智能研究

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-16 DOI: arxiv-2409.10304

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

引用次数: 0

Research evolution of metal organic frameworks: A scientometric approach with human-in-the-loop 金属有机框架的研究演变：以人为本的科学计量学方法

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-16 DOI: arxiv-2409.10776

Xintong Zhao, Kyle Langlois, Jacob Furst, Yuan An, Xiaohua Hu, Diego Gomez Gualdron, Fernando Uribe-Romo, Jane Greenberg

引用次数: 0

Orientational effects in alkanone, alkanal or dialkyl carbonate + alkane mixtures and in alkanone + alkanone or + dialkyl carbonate systems 烷酮、烷醛或碳酸二烷基酯 + 烷烃混合物以及烷酮 + 烷酮或 + 碳酸二烷基酯体系中的定向效应

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-16 DOI: arxiv-2409.10149

Fernando Hevia, Juan Antonio González, Cristina Alonso Tristán, Isaías García de la Fuente, Luis Felipe Sanz

{"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}

引用次数: 0