Structural studies of complex liquids  Page description

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Details of project

  
Identifier
83529
Type K
Principal investigator Pusztai, László
Title in Hungarian Komplex folyadékok szerkezetvizsgálata
Title in English Structural studies of complex liquids
Keywords in Hungarian folyadék; szerkezet; diffrakció; EXAFS; számítógépes szimuláció;
Keywords in English liquid; structure; diffraction; EXAFS; computer simulation
Discipline
Physical Chemistry and Theoretical Chemistry (Council of Physical Sciences)100 %
Ortelius classification: Physical chemistry
Panel Chemistry 1
Department or equivalent Complex Fluids Department (Wigner Research Centre for Physics)
Participants Harsányi, Ildikó
Jóvári, Pál
Mile, Viktória
Pothoczki, Szilvia
Szakályné Dr. Gereben, Orsolya
Temleitner, László
Starting date 2011-02-01
Closing date 2015-12-31
Funding (in million HUF) 15.206
FTE (full time equivalent) 12.73
state closed project
Summary in Hungarian
Átfogó vizsgálatokat kívánunk végezni a komplex molekuláris folyadékok szerkezetét illetően, kezdve a tiszta víz különböző termodinamikai állapotain, az alkáli- és alkáliföldfém-halogenidek (pl. a számos biológiai folyamatban kulcsfontosságú kalcium-klorid) vizes oldatán keresztül fontos szerves anyagok (alkoholok, aminosavak) vizes oldatáig. Minden egyes említett folyadékban számos, a szerkezetre vonatkozó alapkérdés tisztázatlan mind a mai napig: Hogyan jellemezhetjük a molekulák kölcsönös orientációit? Miként befolyásolja ezt a molekulaszerkezet, illetve annak kismértékű megváltoztatása? Hogyan érthetjük meg az ionok és az oldott molekulák hidrátburkának viselkedését? Milyen mértékben alkalmazhatók a szerkezet leírására a jelenleg használatos klasszikus kölcsönhatási potenciálok?
Az általunk megvalósítandó megközelítés, melynek során (többek között) a fenti kérdésekre keresünk megnyugtató választ, magában foglalja a röntgen- és neutrondiffrakció, valamint a röntgen-abszorpció (ezen belül elsősorban az EXAFS) kísérleti módszereket. Olyan, több tízezer részecskét tartalmazó szerkezeti modelleket fogunk készíteni a Reverse Monte Carlo (RMC) számítógépes eljárás segítségével, amelyek az összes felsorolt kísérleti eredménnyel (hibán belül) konzisztensek lesznek. Végül megkíséreljük a széles körben alkalmazott (Monte Carlo és molekuláris dinamikai) számítógépes szimulációkból kapott szerkezeti információt is szerkezeti modelljeinkbe integrálni, felhasználva a pályázók által frissen kidolgozott eljárást. Magától értetődően e szerkezetek megbízhatóbbak lesznek a vizsgált molekuláris folyadékok jelenleg ismert összes szerkezeti modelljénél.
Summary
We wish to carry out comprehensive investigations concerning the structure of molecular liquids, starting from the various themodynamic states of pure water, via aqueous solutions of alkaline earth halides (including calcium chloride; calcium ions in solution have vital roles in quite a few biological processes) to aqueous solutions of important organic compounds (such as alcohols and amino acids). In every single liquid mentioned previously there are a number of problems concerning their structure that need to be clarified urgently: How can we characterise the mutual orientations of molecules? How are these orientations influenced by (small changes of) the molecular structure? How can we understand the behaviour of the hydration spheres of ions and larger molecules? To what extent can we rely on structural information provided by computer simulations using classical interatomic potentials?
Our approach, by which we seek answers to (among others) the above questions, will involve X-ray and neutron diffraction, as well as X-ray absorption (mainly extended X-ray absorption fine structure, EXAFS) experiments. Structural models, containing tens of thousands of particles, will be prepared by using the Reverse Monte Carlo (RMC) modelling technique, so that a single (set of) model(s) will be consistent with results of all experiments listed above. Finally, we will make an attempt for integrating structural information obtained via widely spread (Monte Carlo and molecular dynamics) computer simulation techniques into our structural models (for this purpose, we will apply a procedure introduced recently by the proposers). Clearly, such models will be superior to all existing models of the structure of molecular liquids.




 

Final report

  
Results in Hungarian
Molekuláris folyadékok és amorf szilárd anyagok mikroszkópikus szerkezetét tanulmányoztuk neutron- és röntgendiffrakciós kísérleti módszerekkel, illetve az azokat követő Reverse Monte Carlo (RMC) számítógépes modellezési eljárással. Az amorf anyagokra minden esetben alkalmaztunk EXAFS eredményeket is, így többször akár 6-7 kísérleti adatsorral konzisztens szerkezeteket állítottunk elő. A vizsgált folyadékok között találjuk a tiszta vizet, egyszerű tiszta alkoholokat (metanol, etanol, propanol) valamint ezek vízzel alkotott keverékeit, továbbá egyszerű sók (pl. LiCl, CsCl) tömény vizes oldatait. A felsorolt rendszerekre molekuláris dinamikai (MD) számítógépes szimulációkat is végeztünk: ezen összetett megközelítéssel (diffrakció+MD+RMC) elsősorban az említett folyadékokban kialakuló hidrogénkötéses hálózatokat jellemeztük. Az asszociáló folyadékok tanulmányozásán kívül folytattuk, majd egy nagyobb lélegzetű műben összegeztük a tetraéder alakú molekulákat tartalmazó folyadékok (pl. széntetraklorid, kloroform) szerkezetét illető vizsgálatainkat: bemutattuk a kíséleti és számítógépes módszerek azon kombinációját, amelyekkel a molekulák kölcsönös elhelyezkedése (azaz az 'orientációs korrelációk') a lehető legrészletesebben jellemezhetők.
Results in English
We have studied the microscopic structure of molecular liquids and amorphous solids by neutron and X-ray diffraction experiments and subsequently, by Reverse Monte Carlo (RMC) computer modeling methods. For amorphous materials EXAFS results have always been applied, too, so that in several cases, it was possible to prepare structures that were consistent with 6 to 7 experimental datasets. Among others, we have investigated the structures of pure water, pure low alcohols (methanol, ethanol and propanol), as well as their mixtures with water, and concentrated aqueous solutions of simple salts (e.g., LiCl, CsCl). For the systems just listed, molecular dynamics (MD) computer simulations have also been conducted: via this complex approach (diffraction+MD+RMC) primarily the hydrogen bonded networks present in these liquids have been characterized. Apart from studying associating liquids, we have followed on and later, in the framework of a comprehensive review article, summarized our investigations concerning liquids that contain molecules with a tetrahedral shape (e.g., carbon tetrachloride or chloroform): we have presented a combination of experimental and computer-based methods by which the mutual arrangements of molecules (i.e., the 'orientational correlations') may be characterized to minute details.
Full text https://www.otka-palyazat.hu/download.php?type=zarobeszamolo&projektid=83529
Decision
Yes





 

List of publications

  
Orsolya Gereben, László Pusztai: Extension of the invariant environment refinement technique + reverse Monte Carlo method of structural modelling for interpreting experimental structure factors: ..., J. Chem. Phys. 135, 084111/1-7, 2011
Orsolya Gereben, László Pusztai: System size and trajectory length dependence of the static structure factor and the diffusion coefficient as calculated from molecular dynamics simulations: ..., J. Mol. Liq. 161, pp. 36-40, 2011
Orsolya Gereben, László Pusztai: On the accurate calculation of the dielectric constant from molecular dynamics simulations: the case of SPC/E and SWM4-DP water, Chem. Phys. Letts. 507, 8083, 2011
Aleksander Vrhovsek, Orsolya Gereben, Andrej Jamnik, László Pusztai: Hydrogen bonding and molecular aggregates in liquid methanol, ethanol and propanol, J. Phys. Chem. B 115, pp. 13473-13488, 2011
Ildikó Harsányi, László Temleitner, Brigitte Beuneu, László Pusztai: Neutron and X-ray diffraction measurements on highly concentrated aqueous LiCl solutions, J. Mol. Liq. 165, pp. 94-100, 2012
Ildikó Harsányi, Philippe A. Bopp., Aleksander Vrhovsek, László Pusztai: On the hydration structure of LiCl aqueous solutions: a Reverse Monte Carlo based combination of diffraction data and Molecular Dynamics simulations, J. Mol. Liq. 158, pp. 61-67, 2011
Szilvia Pothoczki, László Temleitner, László Pusztai: Detailed intermolecular structure of molecular liquids containing slightly distorted tetrahedral molecules with C3v symmetry: chloroform, bromoform and methyl-iodide, J. Chem. Phys. 134, 044521/1-8, 2011
Ohara K, Temleitner L, Sugimoto K, Kohara S, Matsunaga T, Pusztai L, Itou M, Ohsumi H, Kojima R, Yamada N, Usuki T, Fujiwara A, Takata M: he roles of the Ge-Te core network and the Sb-Te pseudo network during rapid nucleation-dominated crystallization of amorphous Ge2Sb2Te5, Advanced Functional Materials; 22, 2251-2257, DOI: 10.1002/adfm.201102940, 2012
Gereben O, Kohara S, Pusztai L: The liquid structure of some food aromas: joint X-ray diffraction, all-atom Molecular Dynamics and Reverse Monte Carlo investigations of dimethyl sulfide, dimethyl disulf, Journal of Molecular Liquids; 169, 63-73, 2012
Antipas GSE, Temleitner L, Karalis K, Kohara S, Pusztai L, Xenidis A: A containerless study of short-range order in high-temperature Fe-Si-Al-Ca-Mg-Cr-Cu-Ni oxide systems, Journal of Molecular Structure 1019, 151-158, 2012
Steinczinger Zs, Pusztai L: An independent, general method for checking consistency between diffraction data and partial radial distribution functions derived from them: the example of liquid water, Condensed Matter Physics 15, 23606:1-6, 2012
Gereben O, Pusztai L: Molecular Conformations and the Liquid Structure in Bis(methylthio)methane and Diethyl Sulfide: Diffraction Experiments vs Molecular Dynamics Simulations, J. Phys. Chem. B, 116, pp. 9114-9121, 2012
Mile V, Gereben O, Kohara S, Pusztai L: On the Structure of Aqueous Cesium Fluoride and Cesium Iodide Solutions: Diffraction Experiments, Molecular Dynamics Simulations and Reverse Monte Carlo Modeling, J. Phys. Chem. B, 116, pp. 9758-9767, 2012
Gereben O, Pusztai L: RMC_POT, a computer code for Reverse Monte Carlo modeling the structure of disordered systems containing molecules of arbitrary complexity, Journal of Computational Chemistry, 2012
Temleitner L, Pusztai L, Rubio-Arroyo MF, Aguilar-Lopez S, Klimova T, Pizio O: Microscopic and mesoscopic structural features of an activated carbon sample, prepared from sorghum via activation by phosphoric acid, Materials Research Bulletin, 47, pp. 4409-4413, 2012
Harsányi I, Pusztai L: Hydration structure in concentrated aqueous lithium chloride solutions: A reverse Monte Carlo based combination of molecular dynamics simulations and diffraction data, J. Chem. Phys. 137, 204503/1-9, 2012
Pothoczki Sz, Temleitner L, Pusztai L: Determination of molecular orientational correlations in disordered systems from diffraction data, Advances in Chemical Physics; 150, pp. 143-168, 2012
Voleska I, Akola J, Jóvári P, Gutwirth J, Wagner T, Yannopoulos SN, Jones RO: Structure, electronic, and vibrational properties of glassy Ga11Ge11Te78: Experimentally constrained density functional study, Phys Rev B; 86, 094108/1-9, 2012
Kaban I, Jóvári P, Wang R-P, Luther-Davies B, Mattern N, Eckert J: Structural investigations of Ge5AsxSe95-x and Ge15AsxSe85-x glasses using x-ray diffraction and extended x-ray fine structure spectroscopy, J Phys.: Condensed Matter; 24, 385802:1-7, 2012
Chrissanthopoulos A, Jóvári P, Kaban I, Gruner S, Kavetskyy T, Borc J, Wang W, Ren J, Chen G, Yannopoulos SN: Structure of AgI-doped Ge–In–S glasses: Experiment, reverse Monte Carlo modelling, and density functional calculation, J Solid State Chem; 192, 7-15, 2012
Amir Hossein Taghvaei, Mihai Stoica, Mohsen Samadi Khoshkhoo, Ivan Kaban, Jozef Bednarčik, Pál Jóvári, Kamal Janghorban, Jürgen Eckert: DSC, XRD and TEM characterization of glassy Co40Fe22Ta8B30 alloy with very high thermal stability, Materials Letters, Volume 93, Pages 322-325, 2013
P. Jóvári, Y. Sutou, I. Kaban, Y. Saito, J. Koike: Fourfold coordinated Te atoms in amorphous GeCu2Te3 phase change material, Scripta Materialia, Volume 68, Issue 2, Pages 122-125, 2013
Ohara K, Temleitner L, Sugimoto K, Kohara S, Matsunaga T, Pusztai L, Itou M, Ohsumi H, Kojima R, Yamada N, Usuki T, Fujiwara A, Takata M: he roles of the Ge-Te core network and the Sb-Te pseudo network during rapid nucleation-dominated crystallization of amorphous Ge2Sb2Te5, Advanced Functional Materials; 22, 2251-2257, DOI: 10.1002/adfm.201102940, 2012
Steinczinger Zs, Pusztai L: An independent, general method for checking consistency between diffraction data and partial radial distribution functions derived from them: the example of liquid water, Condensed Matter Physics 15, 23606:1-6, 2012
Antipas GSE, Temleitner L, Karalis K, Pusztai L, Xenidis A: Atomic order and cluster energetics of a 17 wt% Si-based glass versus the liquid phase, JOURNAL OF PHYSICS-CONDENSED MATTER 25:(45) Paper 454206. 7 p. , 2013
Charpentier F, Starecki F, Doualan JL, Jóvári P, Camy P, Troles J, Belin S, Bureau B, Nazabal V: Mid-IR luminescence of Dy3+ and Pr3+ doped Ga5Ge20Sb10S(Se)65 buUR - glasses and fibers, MATERIALS LETTERS 101: pp. 21-24., 2013
Gereben O, Pusztai L: Conformational analysis of bis(methylthio)methane and diethyl sulfide molecules in the liquid phase: reverse Monte Carlo studies using classical interatomic potential fun, JOURNAL OF PHYSICS-CONDENSED MATTER 25:(45) Paper 454201. 13 p., 2013
Gereben O, Pusztai L: The liquid structure of tetrachloroethene: Molecular dynamics simulations and reverse Monte Carlo modeling with interatomic potentials, JOURNAL OF CHEMICAL PHYSICS 139:(16) Paper 164509. 10 p., 2013
Harsanyi I, Pusztai L, Jovari P, Beuneu B: Acidic properties of aqueous phosphoric acid solutions: a microscopic view, JOURNAL OF PHYSICS-CONDENSED MATTER 25:(45) Paper 454215. 5 p., 2013
Jóvári P, Piarristeguy A, Escalier R, Kaban I, Bednarčik J, Pradel A: Short range order and stability of amorphous GexTe 100-x alloys (12 ≤ x ≤ 44.6), JOURNAL OF PHYSICS-CONDENSED MATTER 25:(19) Paper 195401. , 2013
Kaban I, Jóvári P, Kokotin V, Shuleshova O, Beuneu B, Saksl K, Mattern N, Eckert J, Greer AL: Local atomic arrangements and their topology in Ni-Zr and Cu-Zr glassy and crystalline alloys, ACTA MATERIALIA 61:(7) pp. 2509-2520. , 2013
Pothoczki S, Temleitner L, Pardo LC, Cuello GJ, Rovira-Esteva M, Tamarit JL: Comparison of the atomic level structure of the plastic crystalline and liquid phases of CBr2Cl2: Neutron diffraction and reverse Monte Carlo modelling, JOURNAL OF PHYSICS-CONDENSED MATTER 25:(45) Paper 454216. 14 p. , 2013
Rátkai L, Kaban I, Wágner T, Kolář J, Valková S, Voleská I, Beuneu B, Jóvári P: Silver environment and covalent network rearrangement in GeS3-Ag glasses, JOURNAL OF PHYSICS-CONDENSED MATTER 25:(45) Paper 454210. , 2013
Shimakura H, Kawakita Y, Ohara K, Pusztai L, Wakisaka Y, Takeda S: Inter-molecular correlations in liquid Se2Br2, JOURNAL OF PHYSICS-CONDENSED MATTER 25:(45) Paper 454221. 8 p., 2013
Steinczinger Z, Pusztai L: Comparison of the TIP4P-2005, SWM4-DP and BK3 interaction potentials of liquid water with respect to their consistency with neutron and X-ray diffraction data of pure wat, CONDENSED MATTER PHYSICS 16:(4) Paper 43604. 8 p., 2013
Temleitner L, Pusztai L: The origin of diffuse scattering in crystalline carbon tetraiodide, JOURNAL OF PHYSICS-CONDENSED MATTER 25:(45) Paper 454209. 6 p., 2013
Karalis K , Temleitner L , Antipas GSE , Pusztai L , Xenidis A: Experimentally constrained atomic order probing of a Si-Al composite glass, PHILOSOPHICAL MAGAZINE 94:(8) pp. 792-800. , 2014
Kohara S , Tajiri H , Song CH , Ohara K , Temleitner L , Sugimito K , Fujiwara A , Pusztai L , Usuki T , Hosokawa S , Benino Y , Kitamura N , Fukumi K: Anomalous x-ray scattering studies of functional disordered materials, JOURNAL OF PHYSICS-CONFERENCE SERIES 502:(1) Paper 012014. 6 p. , 2014
Pothoczki S , Temleitner L , Pusztai L: The structure of PX3 (X = Cl, Br, I) molecular liquids from X-ray diffraction, molecular dynamics simulations, and reverse Monte Carlo modeling, JOURNAL OF CHEMICAL PHYSICS 140:(5) Paper 054504. 9 p. , 2014
Temleitner L.: Structure determination of liquid carbon tetrabromide via a combination of x-ray and neutron diffraction data and Reverse Monte Carlo modelling, JOURNAL OF MOLECULAR LIQUIDS 197: pp. 204-210. , 2014
Kaban I , Jóvári P , Waske A , Stoica M , Bednarčik J , Beuneu B , Mattern N , Eckert J: Atomic structure and magnetic properties of Fe-Nb-B metallic glasses, JOURNAL OF ALLOYS AND COMPOUNDS 586:(Suppl1) pp. S189-S193. , 2014
Jóvári P , Lucas P , Yang Z , Bureau B , Kaban I , Beuneu B , Bednarčik J: Short-Range Order in Ge-As-Te Glasses, JOURNAL OF THE AMERICAN CERAMIC SOCIETY 97:(5) pp. 1625-1632., 2014
Akola J , Jovari P , Kaban I , Voleska I , Kolar J , Wagner T , Jones RO: Structure, electronic, and vibrational properties of amorphous AsS2 and AgAsS2: Experimentally constrained density functional study, PHYSICAL REVIEW B CONDENSED MATTER AND MATERIALS PHYSICS 89:(6) Paper 064202. 9 p. , 2014
Gereben O, Pusztai L: Understanding the structure of molecular liquids via combinations of molecular dynamics simulations and Reverse Monte Carlo modeling: Handling information deficiency, Journal of Non-Crystalline Solids 407, pp. 213–219, 2015
Gereben O, Pusztai L: Investigation of the Structure of Ethanol/Water Mixtures by Molecular Dynamics Simulation I: Analyses Concerning the Hydrogen-Bonded Pairs, Journal of Physical Chemistry B; 119, pp 3070–3084, 2015
Gereben O: Ring structure analysis of ethanol–water mixtures, J. Mol. Liq. 211, Pages 812-820, 2015
Gereben O: Lacunarity analysis of atomic configurations: Application to ethanol-water mixtures, Phys. Rev. E 92, 033305, 2015
Sanchez V, Noya EG, Temleitner L, Pusztai L: Reverse Monte Carlo modeling: the two distinct routes of calculating the experimental structure factor, Journal of Molecular Liquids; 207, pp. 211-215, 2015
Galicia-Andres E, Pusztai L, Temleitner L, Pizio O: Microscopic structure of methanol–water mixtures: Synchrotron X-ray diffraction experiments and molecular dynamics simulations over the entire composition range, Journal of Molecular Liquids; 209, pp. 586-595, 2015
Galicia-Andres E, Dominguez H, Pusztai L, Pizio O: Composition dependence of thermodynamic, dynamic and dielectric properties of water–methanol model mixtures. Molecular dynamics simulation results with the OPLS-AA model for methanol, J. Mol. Liq. Volume 212, Pages 70-78, 2015
Galicia-Andres E, Dominguez H, Pusztai L, Pizio O: On the composition dependence of thermodynamic, dynamic and dielectric properties of water-methanol model mixtures. Molecular dynamics simulation results, Condensed Matter Physics, vol. 18, No. 4, p. 43602, 2015
Pothoczki Sz, Temleitner L, Pusztai L: Structure of Neat Liquids Consisting of (Perfect and Nearly) Tetrahedral Molecules, Chemical Reviews; 115, No. 24, pp 13308–13361, 2015
A. A. Piarristeguy, M. Micoulaut, R. Escalier, P. Jóvári, I. Kaban, J. van Eijk, J. Luckas, S. Ravindren, P. Boolchand and A. Pradel: Structural singularities in GexTe100−x films, J. Chem. Phys. 143, 074502, 2015
I. Pethes, I. Kaban, R-P Wang, B. Luther-Davies, P. Jóvári: Short range order in Ge-As-Se glasses, Journal of Alloys and Compounds 623, 454, 2015
I. Pethes, R. Chahal, V. Nazabal, C. Prestipino, A. Trapananti, C. Pantalei, B. Beuneu, B. Bureau, P. Jóvári: Short range order in Ge-Ga-Se glasses, J. Alloys and Compounds 651, 578-584, 2015
I. Kaban, P. Jóvári, B. Escher, D. T. Tran, G. Svensson, M.A. Webb, T. Regier, V. Kokotin, B. Beuneu, T. Gemming, J. Eckert: Atomic structure and formation of CuZr-Al bulk metallic glasses and composites, Acta Materialia, 100, 369-376, 2015




 

Events of the project

  
2013-03-13 14:29:08
Résztvevők változása
2013-01-22 14:36:12
Kutatóhely váltás
A kutatás helye megváltozott. Korábbi kutatóhely: SZFI - Neutronfizikai Osztály (MTA Wigner Fizikai Kutatóközpont), Új kutatóhely: SZFI - Komplex Folyadékok Osztály (MTA Wigner Fizikai Kutatóközpont).



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