International Reviews in Physical Chemistry最新文献

{"title":"15N NMR Studies of tautomerism","authors":"E. Kolehmainen, B. Ośmiałowski","doi":"10.1080/0144235X.2012.734157","DOIUrl":"https://doi.org/10.1080/0144235X.2012.734157","url":null,"abstract":"The literature related to 15N NMR studies of tautomerism is updated and discussed. The 15N NMR data show that the technique is applicable for both liquid and solid state (both crystalline and amorphous) materials. Modern computational methods combined with experimental NMR data can aid in the chemical shift assignments especially in case of crystalline materials (so-called NMR crystallography). This review article is divided into chapters based on the different classes of compounds and a brief description of experimental and computational NMR techniques is also included.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"11 1","pages":"567 - 629"},"PeriodicalIF":6.1,"publicationDate":"2012-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89140701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Energy transfer of highly vibrationally excited molecules studied by crossed molecular beam/time-sliced velocity map ion imaging","authors":"H. Hsu, Ming-Tsang Tsai, Y. Dyakov, C. Ni","doi":"10.1080/0144235X.2012.673282","DOIUrl":"https://doi.org/10.1080/0144235X.2012.673282","url":null,"abstract":"Energy transfer of highly vibrationally excited molecules has been studied extensively under bulk conditions in the past 40 years. On the other hand, in 1973 Fisk and co-workers reported the first experimental results of collisional energy transfer of highly vibrationally excited KBr using cross-molecular beams. Surprisingly, it is the only crossed molecular beam experiment about the energy transfer of highly vibrationally excited molecules. No other similar crossed molecular beam experiments have been reported in the following four decades. Recently we have studied the energy transfer of highly vibrationally excited molecules using crossed molecular beams/time-of-flight mass spectrometer in combination with time-sliced velocity map ion imaging techniques. Energy transfer probability density functions were accurately obtained and details of energy transfer mechanisms were evidenced from the cross-molecular beam scatterings. This paper reviews our recent work of energy transfer of highly vibrationally excited molecules. The effects of long-lived complex, initial translational energy, initial rotational temperature, vibrational motions, alkylation, attractive potential and electronic state on the energy transfer and supercollisions were discussed, and comparisons to theoretical calculations and experiments conducted under bulk conditions were made.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"15 1","pages":"201 - 233"},"PeriodicalIF":6.1,"publicationDate":"2012-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"90468011","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Coulomb-crystallised molecular ions in traps: methods, applications, prospects","authors":"S. Willitsch","doi":"10.1080/0144235X.2012.667221","DOIUrl":"https://doi.org/10.1080/0144235X.2012.667221","url":null,"abstract":"Translationally cold, spatially localised molecular ions prepared by sympathetic cooling with laser-cooled atomic ions in ion traps have recently found a wide range of applications in both chemistry and physics. The very low temperatures of the ions (down to millikelvins), their tight localisation in the trap and the ability to control and manipulate single isolated molecules on the quantum level offer intriguing possibilities for new experiments in the realms of cold chemistry, precision molecular spectroscopy, mass spectrometry and quantum technology. The present article gives an overview of the basic experimental methods, current topics and recent developments in this field.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"30 1","pages":"175 - 199"},"PeriodicalIF":6.1,"publicationDate":"2012-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"72659421","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Atomistic simulations of reactive processes in the gas- and condensed-phase","authors":"Pierre-André Cazade, Jing Huang, Juvenal Yosa, J. J. Szymczak, M. Meuwly","doi":"10.1080/0144235X.2012.694694","DOIUrl":"https://doi.org/10.1080/0144235X.2012.694694","url":null,"abstract":"This review focuses on force-field-based approaches to investigate – through computer simulations – reactive processes in chemical and biological systems. Both, reactions in the gas-phase and in condensed-phase environments are discussed and opportunities and the potential for further developments are pointed out. Where available, results are compared with alternative methods and the advantages and drawbacks of the methods are compared. Particular applications include vibrationally and electronically induced (photo)dissociation of small molecules, proton transfer in the gas- and condensed phase and ligand un- and re-binding in proteins.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"7 1","pages":"235 - 264"},"PeriodicalIF":6.1,"publicationDate":"2012-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"88323940","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Quantum dynamics of complex-forming bimolecular reactions","authors":"Hua Guo","doi":"10.1080/0144235X.2011.649999","DOIUrl":"https://doi.org/10.1080/0144235X.2011.649999","url":null,"abstract":"Many gas-phase chemical reactions proceed via reaction intermediates, supported by potential wells. The characteristics of such complex-forming reactions differ drastically from those for direct reactions that involve barriers. For example, the reaction path for a complex-forming reaction is often barrierless, which results in weak and sometimes negative temperature dependence for its rate constant. The product angular and internal distributions of such reactions also bear clear signatures. Specifically, the angular distribution (i.e. differential cross-section) of a complex-forming reaction is often dominated by scattering in the forward and backward directions, and the product rotational state distribution usually peaks near the highest accessible rotational state, while vibrational state distribution often decays monotonically. While the quantum dynamics of direct reactions is well established, our understanding of complex-forming reactions is still far from complete. Given the importance of such reactions in interstellar, atmospheric and combustion chemistry, much research effort has recently been devoted to understand their dynamics. In this review, we survey the recent progress in the quantum dynamics of several prototypical complex-forming reactions, particularly those involving three or four atoms. We will focus on methodological advances in quantum scattering theory, quasi-classical trajectory methods and statistical models.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"60 1","pages":"1 - 68"},"PeriodicalIF":6.1,"publicationDate":"2012-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"84787772","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Modelling of the separation performance and electrokinetic properties of nanofiltration membranes","authors":"Xiao-lin Wang, Yanyan Fang, Cong-Hui Tu, B. Bruggen","doi":"10.1080/0144235X.2012.659049","DOIUrl":"https://doi.org/10.1080/0144235X.2012.659049","url":null,"abstract":"Nanofiltration (NF) has been developed and commercialised over the past decades as a promising liquid separation technology. Recent insights in separation and purification mechanisms related to NF underlined its potential applications for liquid mixtures. During the last years, substantial progress has been made in mathematical modelling of NF, which resulted from a better understanding of separation mechanisms and physico-chemical interactions. The NF separation mechanism is known to be largely related to steric and electrostatic partitioning effects. This combination of effects requires an in-depth analysis of interactions to predict the separation and electrokinetic performance of NF membranes. The mathematical models used to describe the NF process include the following: the nonequilibrium thermodynamic model, structure models and semi-empirical models. This article reviews the origins and general ideas of the above models, as well as their applications to the prediction of separation performance and description of the electrokinetic properties for NF membranes.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"8 1","pages":"111 - 130"},"PeriodicalIF":6.1,"publicationDate":"2012-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89106345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ionisation-induced site switching dynamics in solvated aromatic clusters: phenol–(rare gas) n clusters as prototypical example","authors":"M. Fujii, O. Dopfer","doi":"10.1080/0144235X.2012.656013","DOIUrl":"https://doi.org/10.1080/0144235X.2012.656013","url":null,"abstract":"The ionisation-induced π → H site switching reaction in clusters of phenol solvated by rare gas ligands, PhOH–Rg n (Rg = Ar and Kr, n = 1–3), is characterised by electron impact infrared (EI–IR) photodissociation as well as nanosecond and picosecond time-resolved UV–UV–IR spectroscopy. The EI–IR spectra of the PhOH+–Rg dimers demonstrate that the H-bound isomer is the most stable structure in the ground electronic state of the cation, in which the Rg atom forms a hydrogen bond to the OH group of PhOH+. The π-bound structure, in which the Rg ligand is attached to the aromatic ring, is also weakly detected as a less stable structure in the EI–IR spectrum. The IR spectra of the PhOH+–Rg dimers change drastically, when the cluster cations are generated by resonance-enhanced multiphoton ionisation (REMPI). The metastable π-bound structure becomes the major species and dominates the population. The picosecond time-resolved REMPI–IR spectra clearly demonstrate the initial population of the π-bound structure by ionisation, the subsequent π → H site switching to the H-bound site, and the eventual formation of an π/H equilibrium population by the H → π back reaction. Classically, this intermolecular π ↔ H structural rearrangment corresponds to a pendular motion of Rg atom around PhOH+. The π → H switching dynamics is sensitively affected by the addition of one or more Rg ligands with respect to the reaction mechanism and the rate constants. In larger PhOH+–Rg n clusters (n ≥ 2), the initially populated π-bound structure is completely converted into the H-bound structure by a one-way single-step reaction with a single exponential decay on the picosecond timescale. This principal change in the reaction mechanism is rationalised by efficient intermolecular vibrational energy redistribution from the reaction coordinate to modes of the available spectator ligand(s), which completely quenches the H → π back reaction for n ≥ 2. Structures, energetics and dynamics of this π-H site switching, along with a quantum chemical description based on wavepacket dynamics are discussed. Significantly, these spectroscopic experiments for PhOH+–Rg n represent the first time-resolved studies of intermolecular rearrangment reactions in molecular clusters.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"278 2","pages":"131 - 173"},"PeriodicalIF":6.1,"publicationDate":"2012-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1080/0144235X.2012.656013","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"72456237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Collisional depolarisation of rotational angular momentum: influence of the potential energy surface on the collision dynamics?","authors":"Grant Paterson, M. Costen, K. McKendrick","doi":"10.1080/0144235X.2012.659046","DOIUrl":"https://doi.org/10.1080/0144235X.2012.659046","url":null,"abstract":"We review recent progress in the loss or transfer of the polarisation of angular momentum in collisions of small free radicals with a thermal bath of closed-shell partners. Our primary theme is the connection between the observed behaviour and the nature of the underlying potential energy surfaces (PESs). We consider the systems NO(A2Σ+) + He and Ar; OH(A2Σ+) + He and Ar; OH(X2Π) + He, Ar and Xe; NO(X2Π) + Ar and CN(A2Π) + Ar, which vary both kinematically and in the strength of any attractive interaction. They are chosen because reliable theoretical PESs have been predicted; QS or QCT scattering calculations have been carried out; and they have been studied by recently developed experimental methods sensitive to polarisation. The efficiency of elastic depolarisation depends intimately on the competition with other, inelastic outcomes. It is generally found to be inefficient for systems dominated by impulsive forces, which promote instead changes of state. This is exacerbated by kinematic effects, in particular for the light He collision partner. Moderately attractive PESs support more efficient elastic depolarisation for low rotational levels, but this drops off rapidly with increasing rotation. Persistent elastic depolarisation across all rotational levels is a feature of deeply attractive, strongly anisotropic PESs. The 2Σ+-rare gas systems are characterised by a single controlling PES and are well described by a spin-spectator model. The 2Π-rare gas systems require two PESs, expressible as 2 A′ and 2 A′′ adiabatic surfaces or their diabatic sum and difference, V sum and V diff. Propensities rules reflecting the symmetries of these surfaces help to explain much of the detailed behaviour.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"5 1","pages":"109 - 69"},"PeriodicalIF":6.1,"publicationDate":"2012-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"81843471","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Statistical mechanics theory of molecular recognition and pharmaceutical design","authors":"N. Yoshida, Yasuomi Kiyota, S. Phongphanphanee, Y. Maruyama, T. Imai, F. Hirata","doi":"10.1080/0144235X.2011.648755","DOIUrl":"https://doi.org/10.1080/0144235X.2011.648755","url":null,"abstract":"Molecular recognition (MR) is an essential elementary process allowing biomolecules to perform their function. MR can be defined as a molecular process in which one or several guest molecules are bound with a high probability at a particular site such as a cleft or a cavity, of a host molecule in a particular orientation. It is a thermodynamic process which is characterised by the difference of the free energies between two states of a host–guest system, bound and unbound. The process features an extremely heterogeneous atomic-environment around binding sites, which has turned away challenges by the conventional statistical mechanics of liquids, e.g. a mean field theory. We have been developing a new theory for MR in biomolecular systems, based on the statistical mechanics of liquids, or the 3D-reference interaction site model (RISM)/RISM theory. The theory has demonstrated its amazing capability of predicting the process from the first principle. In this article, we review our recent works on MR concerning protein and deoxyribonucleic acid. Some applications of the method to drug design are also presented.","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"14 5","pages":"445 - 478"},"PeriodicalIF":6.1,"publicationDate":"2011-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1080/0144235X.2011.648755","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"72471310","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Towards controlling molecular motions in fluorescence microscopy and optical trapping: a spatiotemporal approach.","authors":"Arijit Kumar De, Debabrata Goswami","doi":"10.1080/0144235X.2011.603237","DOIUrl":"10.1080/0144235X.2011.603237","url":null,"abstract":"<p><p>This account reviews some recent studies pursued in our group on several control experiments with important applications in (one-photon) confocal and two-photon fluorescence laser-scanning microscopy and optical trapping with laser tweezers. We explore the simultaneous control of internal and external (i.e. centre-of-mass motion) degrees of freedom, which require the coupling of various control parameters to result in the spatiotemporal control. Of particular interest to us is the implementation of such control schemes in living systems. A live cell is a system of a large number of different molecules which combine and interact to generate complex structures and functions. These combinations and interactions of molecules need to be choreographed perfectly in time and space to achieve intended intra-cellular functions. Spatiotemporal control promises to be a versatile tool for dynamical control of spatially manipulated bio-molecules.</p>","PeriodicalId":54932,"journal":{"name":"International Reviews in Physical Chemistry","volume":"30 3","pages":"275-299"},"PeriodicalIF":2.5,"publicationDate":"2011-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3695459/pdf/emss-53304.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"31546415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}