• Seidl, M.: Mehr Elfenbeinturm. – Nachrichten aus der Chemie 64, 1094–1095 (2016); doi:10.1002/nadc.20164052677, PDF-Datei Volltext.

    Wiederabdruck: Mehr Elfenbeintürme braucht das Land. – Quart Nr. 2/2017, 41–42 (2017).

    Zum Inhalt: Das Nützlichkeitsdenken hat sämtliche Lebensbereiche erfasst. Alles wird an seinem Zweck oder seinem Verwertungspotenzial gemessen. Wie geht es dabei der Grundlagenforschung? Besteht ihr Sinn allein in ihrem (sozio-)ökonomischen Nutzen?

  • Seidl, M.; Amann-Winkel, K.; Bernard, J.; Loerting, T.: Eine Substanz, zwei Flüssigkeiten. – Nachrichten aus der Chemie 63, 111–115 (2015); doi:10.1002/nadc.201590041, PDF-Datei Volltext.

    Zum Inhalt: Immer noch wird kontrovers diskutiert, warum ausgerechnet Wasser das Molekül des Lebens ist und es sich im Vergleich mit anderen Flüssigkeiten so anomal verhält.

  • Seidl, M.: Wasser: Philosophie der Anomalie. – science.orf.at, 24.02.2012; Volltext.

    Zum Inhalt: Wasser weist zahlreiche ungewöhnliche Eigenschaften auf und verblüfft durch die große Vielfalt an Eisformen. Aktuelle Forschungsprojekte tragen wesentlich zur Lösung der Rätsel von Wasser bei. Offene Fragen bleiben dennoch – und diese betreffen auch die Philosophie, erklärt der Chemiker Markus Seidl in einem Gastbeitrag.

  • Lemke, S.; Handle, P. H.; Plaga, L. J.; Stern, J. N.; Seidl, M.; Fuentes-Landete, V.; Amann-Winkel, K.; Köster, K. W.; Gainaru, C.; Loerting, T.; Böhmer, R.: Relaxation dynamics and transformation kinetics of deeply supercooled water: Temperature, pressure, doping, and proton/deuteron isotope effects. – Journal of Chemical Physics 147, 034506 (2017); doi:10.1063/1.4993790.

    Abstract: Above its glass transition, the equilibrated high-density amorphous ice (HDA) transforms to the low-density pendant (LDA). The temperature dependence of the transformation is monitored at ambient pressure using dielectric spectroscopy and at elevated pressures using dilatometry. It is found that near the glass transition temperature of deuterated samples, the transformation kinetics is 300 times slower than the structural relaxation, while for protonated samples, the time scale separation is at least 30 000 and insensitive to doping. The kinetics of the HDA to LDA transformation lacks a proton/deuteron isotope effect, revealing that this process is dominated by the restructuring of the oxygen network. The x-ray diffraction experiments performed on samples at intermediate transition stages reflect a linear combination of the LDA and HDA patterns implying a macroscopic phase separation, instead of a local intermixing of the two amorphous states.

  • Handle, P. H.; Seidl, M.; Fuentes-Landete, V.; Loerting, T.: Ex situ studies of unannealed high-density amorphous ice annealed at 0.1 and 0.2 GPa: Includes response to "Comment on: 'Relaxation time of high-density amorphous ice'" by G.P. Johari. – Thermochimica Acta 636, 11–22 (2016); doi:10.1016/j.tca.2016.04.012.

    Abstract: In earlier work [P. H. Handle, M. Seidl and T. Loerting, Phys. Rev. Lett., 2012, 108, 225901] we reported on the relaxation time and extrapolated glass transition temperatures Tg of high-density amorphous ice (HDA) kept under a pressure of 0.1 and 0.2 GPa. Our ex situ strategy of obtaining these properties and the interpretation of our observations was recently assessed and questioned by Johari [Thermochimica Acta, 2014, 589, 76–84]. Here we reply to the criticism, describe all our measurement and data analysis procedures in detail to reconfirm our earlier interpretation and conclusions. In addition to the more detailed analysis of relaxation times τR we also present an analysis of crystallization times τX. The comparison between the two reveals it is possible to significantly relax unannealed HDA (uHDA) at 0.1 and 0.2 GPa prior to its full crystallization.

  • Stern, J.; Seidl, M.; Gainaru, C.; Fuentes-Landete, V.; Amann-Winkel, K.; Handle, P. H.; Köster, K. W.; Nelson, H.; Böhmer, R.; Loerting, T.: Experimental evidence for two distinct deeply supercooled liquid states of water – Response to "Comment on 'Water's second glass transition'", by G. P. Johari, Thermochim. Acta (2015). – Thermochimica Acta 617, 200–207 (2015); doi:10.1016/j.tca.2015.08.030.

    Abstract: Recently, our earlier data which led us to conclude that deeply supercooled water displays a second glass transition (Amann-Winkel et al., 2013) was reinterpreted (Johari, 2015). In particular, the increase in heat capacity observed for high-density amorphous ice (HDA) samples at 116 K was reinterpreted to indicate sub-Tg features of low-density amorphous ice's (LDA's) glass transition. We reply to the criticism in detail and report an experiment triggered by the comment on our work. This experiment unequivocally confirms our original interpretation of the observations and reinforces the case for water's second glass transition, its polyamorphism, and the observation of two distinct ultraviscous states of water differing by about 25% in density.

  • Köster, K. W.; Fuentes-Landete, V.; Raidt, A.; Seidl, M.; Gainaru, C.; Loerting, T.; Böhmer, R.: Dynamics enhanced by HCl doping triggers full Pauling entropy release at the ice XII–XIV transition. – Nature Communications 6, 7349 (2015); doi:10.1038/ncomms8349.

    Abstract: The pressure–temperature phase diagram of ice displays a perplexing variety of structurally distinct phases. In the century-long history of scientific research on ice, the proton-ordered ice phases numbered XIII through XV were discovered only recently. Despite considerable effort, none of the transitions leading from the low-temperature ordered ices VIII, IX, XI, XIII, XIV and XV to their high-temperature disordered counterparts were experimentally found to display the full Pauling entropy. Here we report calorimetric measurements on suitably high-pressure-treated, hydrogen chloride-doped ice XIV that demonstrate just this at the transition to ice XII. Dielectric spectroscopy on undoped and on variously doped ice XII crystals reveals that addition of hydrogen chloride, the agent triggering complete proton order in ice XIV, enhances the precursor dynamics strongest. These discoveries provide new insights into the puzzling observation that different dopants trigger the formation of different proton-ordered ice phases.

  • Seidl, M.; Fayter, A.; Stern, J. N.; Zifferer, G.; Loerting, T.: Shrinking water's no man's land by lifting its low-temperature boundary. – Physical Review B 91, 144201 (2015); doi:10.1103/PhysRevB.91.144201.

    Abstract: Investigation of the properties and phase behavior of non-crystalline water is hampered by rapid crystallization in the so-called "no-man's land". We here show that it is possible to shrink the no-man's land by lifting its low-temperature boundary, i.e., the pressure-dependent crystallization temperature Tx(p). In particular, we investigate two types of high-density amorphous ice (HDA) in the pressure range of 0.10–0.50 GPa and show that the commonly studied unannealed state, uHDA, is up to 11 K less stable against crystallization than a pressure-annealed state called eHDA. We interpret this finding based on our previously established microscopic picture of uHDA and eHDA, respectively [M. Seidl et al., Phys. Rev. B 88, 174105 (2013)]. In this picture the glassy uHDA matrix contains ice Ih-like nanocrystals, which simply grow upon heating uHDA at pressures ≤0.20 GPa. By contrast, they experience a polymorphic phase transition followed by subsequent crystal growth at higher pressures. In comparison, upon heating purely glassy eHDA, ice nuclei of a critical size have to form in the first step of crystallization, resulting in a lifted Tx(p). Accordingly, utilizing eHDA enables the study of amorphous ice at significantly higher temperatures at which we regard it to be in the ultraviscous liquid state. This will boost experiments aiming at investigating the proposed liquid-liquid phase transition.

  • Jehser, M.; Seidl, M.; Rauer, C.; Loerting, T.; Zifferer, G.: Simulation of high-density water: Its glass transition for various water models. – Journal of Chemical Physics 140, 134504 (2014); doi:10.1063/1.4869861.

    Abstract: High-density amorphous water is simulated by use of isothermal-isobaric molecular dynamics at a pressure of 0.3 GPa making use of several water models (SPC/E, TIP3P, TIP4P variants, and TIP5P). Heating/cooling cycles are performed in the temperature range 80–280 K and quantities like density, total energy, and mobility are analysed. Raw data as well as the glass transition temperatures Tg observed in our studies depend on the water model used as well as on the treatment of intramolecular bonds and angles. However, a clear-cut evidence for the occurrence of a glass-to-liquid transition is found in all cases. Thus, all models indicate that high-density amorphous ice found experimentally may be a low-temperature proxy of an ultraviscous high-density liquid.

  • Seidl, M.; Amann-Winkel, K.; Handle, P. H.; Zifferer, G.; Loerting, T.: From parallel to single crystallization kinetics in high-density amorphous ice. – Physical Review B 88, 174105 (2013); doi:10.1103/PhysRevB.88.174105.

    Abstract: The isobaric transformation behavior of unannealed (uHDA) and expanded (eHDA) high-density amorphous ice at pressures up to 0.20 GPa is compared using powder x-ray diffraction and dilatometry. eHDA shows high thermal stability and crystallizes to a single ice phase only, whereas uHDA shows much lower thermal stability and always crystallizes to a mixture of ice phases. Unexpectedly, at low temperatures hexagonal ice grows first from uHDA, whereas this phase never crystallizes from eHDA. This leads us to conclude that hidden structural order in the form of nanocrystalline domains is present in uHDA, which triggers growth of hexagonal ice. By contrast, these ordered domains are absent in eHDA, which appears to be a homogeneous material and, thus, could be considered as a candidate for the low-temperature proxy of the proposed high-density liquid phase of water. The present work provides the basis for further experimental studies aiming at investigating this possibility since it establishes that the well-studied uHDA is not the right material to be studied in this context, whereas the more recently discovered eHDA is.

  • Amann-Winkel, K.; Gainaru, C.; Handle, P. H.; Seidl, M.; Nelson, H.; Böhmer, R.; Loerting, T.: Water's second glass transition. – Proceedings of the National Academy of Sciences of the United States of America 110, 17720–17725 (2013); doi:10.1073/pnas.1311718110.

    Abstract: The glassy states of water are of common interest as the majority of H2O in space is in the glassy state and especially because a proper description of this phenomenon is considered to be the key to our understanding why liquid water shows exceptional properties, different from all other liquids. The occurrence of water's calorimetric glass transition of low-density amorphous ice at 136 K has been discussed controversially for many years because its calorimetric signature is very feeble. Here, we report that high-density amorphous ice at ambient pressure shows a distinct calorimetric glass transitions at 116 K and present evidence that this second glass transition involves liquid-like translational mobility of water molecules. This "double Tg scenario" is related to the coexistence of two liquid phases. The calorimetric signature of the second glass transition is much less feeble, with a heat capacity increase at Tg,2 about five times as large as at Tg,1. By using broadband-dielectric spectroscopy we resolve loss peaks yielding relaxation times near 100 s at 126 K for low-density amorphous ice and at 110 K for high-density amorphous ice as signatures of these two distinct glass transitions. Temperature-dependent dielectric data and heating-rate-dependent calorimetric data allow us to construct the relaxation map for the two distinct phases of water and to extract fragility indices m = 14 for the low-density and m = 20–25 for the high-density liquid. Thus, low-density liquid is classified as the strongest of all liquids known ("superstrong"), and also high-density liquid is classified as a strong liquid.

  • Bernard, J.; Seidl, M.; Mayer, E.; Loerting, T.: Formation and stability of bulk carbonic acid (H2CO3) by protonation of tropospheric calcite. – ChemPhysChem 13, 3087–3091 (2012); doi:10.1002/cphc.201200422.

    Description: In this paper it is shown that H2CO3 may form in the atmosphere from mineral dust in the presence of acid and remain stable there for long periods even in the presence of rather high relative humidity.

  • Handle, P. H.; Seidl, M.; Loerting, T.: Relaxation time of high-density amorphous ice. – Physical Review Letters 108, 225901 (2012); doi:10.1103/PhysRevLett.108.225901.

    Abstract: Amorphous water plays a fundamental role in astrophysics, cryoelectron microscopy, hydration of matter, and our understanding of anomalous liquid water properties. Yet, the characteristics of the relaxation processes taking place in high-density amorphous ice (HDA) are unknown. We here reveal that the relaxation processes in HDA at 110–135 K at 0.1–0.2 GPa are of collective and global nature, resembling the alpha relaxation in glassy material. Measured relaxation times suggest liquid-like relaxation characteristics in the vicinity of the crystallization temperature at 145 K. By carefully relaxing pressurized HDA for several hours at 135 K, we produce a state that is closer to the ideal glass state than all HDA states discussed so far in literature.

  • Seidl, M.; Karsai, F.; Loerting, T.; Zifferer, G.: Note: Molecular dynamics studies of high-density amorphous ice: Influence of long-range Coulomb interactions. – Journal of Chemical Physics 136, 026101 (2012); doi:10.1063/1.3676058.

    Abstract: Making use of isothermal-isobaric molecular dynamics high-density amorphousice is simulated at a pressure of 0.3 GPa. Heating/cooling cycles are performed in the temperature range 80 K–300 K. Analysis of quantities like density, total energy, and mobility give clear evidence for a glass-to-liquid transition. However, raw data as well as the observed glass transition temperatures Tg are not only dependent on the force field used but in addition on the treatment of Coulomb interactions (group based cut-off or long-range terms by Ewald summation). Nevertheless, all models indicate that high-density amorphousices may indeed be low-temperature proxies of ultraviscous high-density liquids.

  • Seidl, M.; Elsaesser, M. S.; Winkel, K.; Zifferer, G.; Mayer, E.; Loerting, T.: Volumetric study consistent with a glass-to-liquid transition in amorphous ices under pressure. – Physical Review B 83, 100201 (2011); doi:10.1103/PhysRevB.83.100201.

    Abstract: Dilatometry experiments on low- and high-density amorphous ices up to 0.30 GPa are presented together with powder x-ray diffraction data. Repeated isobaric heating and cooling cycles reveal three competing processes: irreversible (micro)structural relaxation, reversible relaxation, and (irreversible) crystallization. The third and subsequent heating runs produce identical curves, i.e., irreversible relaxation is absent. We interpret the deviation from linear expansivity in these curves as the onset temperature of the volumetric glass-to-liquid transition (Tg, onset) and report its dependence on pressure.

  • Winkel, K.; Seidl, M.; Loerting, T.; Bove, L. E.; Imberti, S.; Molinero, V.; Bruni, F.; Mancinelli, R.; Ricci, M. A.: Structural study of low concentration LiCl aqueous solutions in the liquid, supercooled, and hyperquenched glassy states. – Journal of Chemical Physics 134, 024515 (2011); doi:10.1063/1.3528000.

    Abstract: Neutron diffraction experiments on a solution of LiCl in water (R = 40) at ambient conditions and in the supercooled and hyperquenched states are reported and analyzed within the empirical potential structure refinement framework. Evidence for the modifications of the microscopic structure of the solvent in the presence of such a small amount of salt is found at all investigated thermodynamic states. On the other hand, it is evident that the structure of the hyperquenched salty sample is similar to that of pure low density amorphous water, although all the peaks of the radial distribution functions are broader in the present case. Changes upon supercooling or hyperquenching of the ion's hydration shells and contacts are of limited size and evidence for segregation phenomena at these states does not clearly show up, although the presence of water separated contacts between ion of the same sign is intriguing.

  • Bernard, J.; Seidl, M.; Kohl, I.; Liedl, K. R.; Mayer, E.; Gálvez, Ó; Grothe, H.; Loerting, T.: Spectroscopic observation of matrix-isolated carbonic acid trapped from the gas phase. – Angewandte Chemie International Edition 50, 1939–1943 (2011); doi:10.1002/anie.201004729.

    Description: Carbonic acid molecules were trapped from the gas phase in a solid noble-gas matrix at <10 K and studied by IR spectroscopy. The 2H and 13C isotopologues were also examined. Gas-phase carbonic acid is thought to exist as a 1:10:1 mixture of two monomeric conformers and the cyclic dimer (H2CO3)2. This data is vital in the search for gas-phase carbonic acid in astrophysical environments.

  • Bernard, J.; Seidl, M.; Kohl, I.; Liedl, K. R.; Mayer, E.; Gálvez, Ó; Grothe, H.; Loerting, T.: Spektroskopische Beobachtung von matrixisolierter Kohlensäure, abgeschieden aus der Gasphase. – Angewandte Chemie 123, 1981–1985 (2011); doi:10.1002/ange.201004729.

    Zum Inhalt: Kohlensäuremoleküle wurden aus der Gasphase in einer festen Edelgasmatrix bei <10 K eingefangen und IR-spektroskopisch untersucht. Auch die 2H- und 13C-Isotopologe wurden vermessen, und daraus konnte das Vorliegen einer 1:10:1-Mischung von zwei Monomerkonformationen und dem ringförmigen Dimer (H2CO3)2 gefolgert werden. Diese Daten sind wertvoll, um gasförmige Kohlensäure im Weltraum aufzuspüren.

  • Seidl, M.; Loerting, T.; Zifferer, G.: High-density amorphous ice: Molecular dynamics simulations of the glass transition at 0.3 GPa. – Journal of Chemical Physics 131, 114502 (2009); doi:10.1063/1.3224857.

    Abstract: Based on several force fields (COMPASS, modified TIP3P and SPC/E) high-density amorphousice is simulated by use of isothermal-isobaric molecular dynamics at a pressure of p ≈ 0.3 GPa in the temperature range from 70 to 300 K. Starting at low temperature a large number of heating/cooling cycles are performed and several characteristic properties (density, total energy, and mobility) are traced as functions of temperature. While the first cycles are showing irreversible structural relaxation effects data points from further cycles are reproducible and give clear evidence for the existence of a glass-to-liquid transition. Although, the observed transition temperatures Tg are dependent on the actual force field used and slightly dependent on the method adopted the results indicate that high-density amorphousices may indeed be low-temperature structural proxies of ultraviscous high-density liquids.

  • Seidl, M.; Loerting, T.; Zifferer, G.: Molecular dynamics simulations on the glass-to-liquid transition in high density amorphous ice. – Zeitschrift für Physikalische Chemie 223, 1047–1062 (2009); special issue dedicated to Prof. Alfons Geiger on the occasion of his 65th birthday; doi:10.1524/zpch.2009.6057.

    Abstract: It is an open question whether high density amorphous (HDA) ice is a glassy material structurally related to an ultraviscous high density liquid (HDL) or a nanocrystalline material unrelated to a liquid. In order to shed light on this question we have performed molecular dynamics simulations on a HDA model system at a pressure of p ≈ 0.3 GPa using the COMPASS force field. After removing the irreversible structural relaxation effect by initial isobaric heating/cooling cycles, we observe a deviation from linearity in the density vs. temperature plot in the range 170 ± 15 K in subsequent cycles, which we attribute to the glass-transition temperature Tg. This assignment of Tg is corroborated by two independent methods, namely from a rapid increase in the diffusion coefficient at ≈169 K and a deviation from linearity at ≈174 K in an enthalpy versus temperature plot. The structure of the model system is in good agreement with the experimentally determined structure of HDA. We, thus, suggest that HDA may indeed be a low temperature structural proxy of an ultraviscous liquid HDL.

  • Seidl, M.; Etinski, M.; Uiberacker, C.; Jakubetz, W.: Pulse-train control of branching processes: Elimination of background- and intruder state population. – Journal of Chemical Physics 129, 234305 (2008); doi:10.1063/1.3041380.

    Abstract: The authors introduce and describe pulse train control (PTC) of population branching in strongly coupled processes as a novel control tool for the separation of competing multiphoton processes. Control strategies are presented based on the different responses of processes with different photonicities and/or different frequency detunings to the pulse-to-pulse time delay and the pulse-to-pulse phase shift in pulse trains. The control efficiency is further enhanced by the property of pulse trains that complete population transfer can be obtained over an extended frequency range that replaces the resonance frequency of simple pulses. The possibility to freely tune the frequency assists the separation of the competing processes and reduces the number of subpulses required for full control. As a sample application, PTC of leaking multiphoton resonances is demonstrated by numerical simulations. In model systems exhibiting sizable background (intruder) state population if excited with single pulses, PTC leading to complete accumulation of population in the target state and elimination of background population is readily achieved. The analysis of the results reveals different mechanisms of control and provides clues on the mechanisms of the leaking process itself. In an alternative setup, pulse trains can be used as a phase-sensitive tool for level switching. By changing only the pulse-to-pulse phase shift of a train with otherwise unchanged parameters, population can be transferred to any of two different target states in a near-quantitative manner.

  • Winkel, K.; Bauer, M.; Mayer, E.; Seidl, M.; Elsaesser, M. S.; Loerting, T.: Structural transitions in amorphous H2O and D2O: The effect of temperature. – Journal of Physics: Condensed Matter 20, 494212 (2008); doi:10.1088/0953-8984/20/49/494212.

    Abstract: We have recently observed amorphous-amorphous transitions incurred upon decompressing very high density amorphous ice (VHDA) at 140 K from 1.1 to <0.02 GPa in a piston-cylinder setup by monitoring the piston displacement as a function of pressure and by taking powder x-ray diffractograms of quench-recovered samples (Winkel et al 2008 J. Chem. Phys. 128 044510). Here we study the effect of changing the temperature from 77 to 160 K during decompression from 1.1 to <0.02 GPa, and the effect of substituting D2O for H2O at 140 and 143 K. At 77 K all structural transitions are arrested and six-coordinated VHDA is quench recovered. At 125–136 K the continuous transition to five-coordinated expanded high density amorphous ice (eHDA) takes place. At 139–140 K, both the continuous transition to eHDA and the quasi-discontinuous transition to four-coordinated LDA are observed, i.e. VHDA → eHDA → LDA. At 142–144 K, crystallization to mixtures of cubic ice Ic and ice IX is observed prior to the quasi-discontinuous transition, i.e. VHDA → eHDA → ice Ic/ice IX. At 160 K ice Ic is recovered, which most likely transforms from a high-pressure ice (HPI) such as ice V, i.e. VHDA → HPI → ice Ic. Exchanging D2O for H2O at 140 K does not significantly affect the amorphous-amorphous transitions: both the decompression curves and the powder x-ray diffractograms are unaffected within the experimental resolution. However, at 143 K D2O-VHDA can be decompressed according to the sequence VHDA → eHDA → LDA, i.e. crystallization can be suppressed at ≈3 K higher temperatures.

  • Seidl, M.; Uiberacker, C.; Jakubetz, W.: Pulse-train control of multiphoton transitions in anharmonic progressions: Resonance loci and resonance ridges. – Chemical Physics 349, 296–307 (2008); special issue dedicated to the 65th birthday of Prof. Hans Lischka; doi:10.1016/j.chemphys.2008.02.058.

    Abstract: The properties of pulse-train induced multiphoton excitation in anharmonic progressions and the accumulation of population in a specific rung state are investigated by means of numerical simulations. It is shown how and under which conditions resonant π-pulses and multiple-π pulses can be split into trains of fractional π-pulses driving the same transition. Standardized train forms are considered with sub-pulses of equal (gaussian) shapes and equal, but tunable pulse-to-pulse delays and pulse-to-pulse phase shifts. The increased number of tuning parameters together with the handle on the number of sub-pulses gives rise to a remarkable variability in the control of state-specific population transfer, where simple zero-order estimates assist the determination of the parameters. Each π- or multiple-π pulse is replaced by a resonance locus in parameter space representing an infinite set of π-trains. The loci span extended frequency ranges that increase with increasing sub-pulse number. Their projection onto the frequency-field strength plane gives rise to elliptically shaped closed curves, termed resonance ridges, which replace the singular points mapped out by simple π- and multiple-π pulses. In the subspace of pulse-to-pulse delays and pulse-to-pulse phase shifts the resonance loci are characterized by phase recurrence relations, whose number and complexity increases with increasing numbers of sub-pulses. Our results indicate that pulse trains may be a powerful tool for the control of parallel or branching multiphoton transitions and for the elimination of background and intruder state population.

  • Seidl, M.; Fayter, A.; Stern, J. N.; Amann-Winkel, K.; Bauer, M.; Loerting, T.: High-performance dilatometry under extreme conditions. – In: Proceedings of the 6th Zwick Academia Day 2015; published by Zwick GmbH & Co. KG, Ulm 2015.

    Abstract: Equations of state describe the pressure-volume-temperature surface of the thermodynamically stable phases of a given material. However, the thermodynamically (most) stable phase might not be observed experimentally due to kinetic reasons. Instead metastable phases could be obtained, which is in fact a very common and technologically important phenomenon. Here we describe how to use a material testing machine from Zwick as a high-performance dilatometer. In conjunction with a custom-made piston cylinder setup it enables the study of phase diagrams as well as metastable phases and instable states, i. e., the experimental representation of equations of state, via both isobaric and isothermal experiments up to pressures of ∼2 GPa and down to temperatures of ∼79 K. In particular, we consider amorphous, metastable solid states of water (i. e., amorphous ices) as well as crystalline ice phases to exemplify our apparatus' performance in detail.

  • Fuentes-Landete, V.; Mitterdorfer, C.; Handle, P. H.; Ruiz, G. N.; Bernard, J.; Bogdan, A.; Seidl, M.; Amann-Winkel, K.; Stern, J.; Fuhrmann, S.; Loerting, T.: Crystalline and amorphous solid phases of water. – In: Debenedetti, P. G.; Ricci, M. A.; Bruni, F. (Eds.): Proceedings of the International School of Physics "Enrico Fermi", Volume 187: Water: Fundamentals as the Basis for Understanding the Environment and Promoting Technology; Amsterdam: IOS and Bologna: SIF 2015, 173–208; doi:10.3254/978-1-61499-507-4-173.

    Abstract: Water is one of the most abundant molecules on Earth, of paramount importance to our daily lives and is of great relevance in astrophysics. Nevertheless its physical and chemical properties, which are often called anomalies, are not fully understood by now. Investigations in recent decades have shown that water exists in several crystalline forms – a phenomenon known as polymorphism – and in three amorphous forms – a phenomenon known as polyamorphism. In this article we review the crystalline ice phases and outline possibilities for future experimental discoveries of ice polymorphs. We then provide an overview about the current knowledge on polyamorphism and finally go into more detail about the question whether or not the amorphous ices are linked by glass-to-liquid transitions to deeply supercooled liquids, which has been a major focus in our research group over the last years.

  • Loerting, T.; Fuentes-Landete, V.; Handle, P. H.; Seidl, M.; Amann-Winkel, K.; Gainaru, C.; Böhmer, R.: The glass transition in high-density amorphous ice. – Journal of Non-Crystalline Solids 407, 423–430 (2015); doi:10.1016/j.jnoncrysol.2014.09.003.

    Abstract: There has been a long controversy regarding the glass transition in low-density amorphous ice (LDA). The central question is whether or not it transforms to an ultraviscous liquid state above 136 K at ambient pressure prior to crystallization. Currently, the most widespread interpretation of the experimental findings is in terms of a transformation to a superstrong liquid above 136 K. In the last decade some work has also been devoted to the study of the glass transition in high-density amorphous ice (HDA) which is in the focus of the present review. At ambient pressure HDA is metastable against both ice I and LDA, whereas at >0.2 GPa HDA is no longer metastable against LDA, but merely against high-pressure forms of crystalline ice. The first experimental observation interpreted as the glass transition of HDA was made using in situ methods by Mishima, who reported a glass transition temperature Tg of 160 K at 0.40 GPa. Soon thereafter Andersson and Inaba reported a much lower glass transition temperature of 122 K at 1.0 GPa. Based on the pressure dependence of HDA's Tg measured in Innsbruck, we suggest that they were in fact probing the distinct glass transition of very high-density amorphous ice (VHDA). Very recently the glass transition in HDA was also observed at ambient pressure at 116 K. That is, LDA and HDA show two distinct glass transitions, clearly separated by about 20 K at ambient pressure. In summary, this suggests that three glass transition lines can be defined in the p–T plane for LDA, HDA, and VHDA.

  • Loerting, T.; Winkel, K.; Seidl, M.; Bauer, M.; Mitterdorfer, C.; Handle, P. H.; Salzmann, C. G.; Mayer, E.; Finney, J. L.; Bowron, D. T.: How many amorphous ices are there? – Physical Chemistry Chemical Physics 13, 8783–8794 (2011); doi:10.1039/c0cp02600j.

    Abstract: Many acronyms are used in the literature for describing different kinds of amorphous ice, mainly because many different preparation routes and many different sample histories need to be distinguished. We here introduce these amorphous ices and discuss the question of how many of these forms are of relevance in the context of polyamorphism. We employ the criterion of reversible transitions between amorphous "states" in finite intervals of pressure and temperature to discriminate between independent metastable amorphous "states" and between "substates" of the same amorphous "state". We argue that the experimental evidence suggests we should consider there to be three polyamorphic "states" of ice, namely low-(LDA), high-(HDA) and very high-density amorphous ice (VHDA). In addition to the realization of reversible transitions between them, they differ in terms of their properties, e.g., compressibility, or number of "interstitial" water molecules. Thus they cannot be regarded as structurally relaxed variants of each other and so we suggest considering them as three distinct megabasins in an energy landscape visualization.

  • Seidl, M.: Peinlich, Rezension zu Ernst Peter Fischer, "Noch wichtiger als das Wissen ist die Phantasie" – Die 50 besten Erkenntnisse der Wissenschaft von Galilei bis Einstein. – Nachrichten aus der Chemie 64, 1206 (2016); PDF-Datei Volltext.

  • Seidl, M.: Beschwörung ist zu wenig, Rezension zu Peter Atkins, Die wundersame Welt der Chemie. – Nachrichten aus der Chemie 64, 1204–1205 (2016); PDF-Datei Volltext.

  • Seidl, M.: Amorphes Eis: Glasig oder nanokristallin? – Kolloquium des Instituts für Anorganische und Angewandte Chemie der Universität Hamburg, Einladung durch Dr. Frank Hoffmann, Hamburg, Deutschland, 29.05.2017.
  • Seidl, M.: High-performance dilatometry under extreme conditions. – 6th Zwick Academia Day 2015, Zürich, Schweiz, 02.06.2015.
  • Seidl, M.: Crystallization behavior of amorphous ices prepared via different routes. – Fritz-Haber-Institut der Max-Planck-Gesellschaft, Berlin, Deutschland, 01.04.2014.
  • Seidl, M.; Dalal, S. S.; Ediger, M. D.: Crystallization kinetics of tris-naphthylbenzene isomers. – 15. Österreichische Chemietage, Graz, Österreich, 23.–26.09.2013.
  • Seidl, M.; Amann-Winkel, K.; Handle, P. H.; Zifferer, G.; Loerting, T.: Crystallization studies demonstrate hidden structural order in amorphous ice. – 7th International Discussion Meeting on Relaxations in Complex Systems, Barcelona, Spanien, 21.–26.07.2013.
  • Seidl, M.; Handle, P. H.; Winkel, K.; Zifferer, G.; Mayer, E.; Loerting, T.: On the (non)crystallinity of high-density amorphous ice. – Gordon-Kenan Research Seminar on Water and Aqueous Solutions, Holderness, New Hampshire, Vereinigte Staaten, 11.–12.08.2012.
  • Seidl, M.; Winkel, K.; Handle, P. H.; Zifferer, G.; Mayer, E.; Loerting, T.: Amorphous ices and their glassy nature. – Arbeitsgruppen-Seminar von Prof. Mark D. Ediger, University of Wisconsin-Madison, Madison, Wisconsin, Vereinigte Staaten, 08.02.2012.
  • Seidl, M.; Winkel, K.; Handle, P. H.; Zifferer, G.; Mayer, E.; Loerting, T.: Presence and absence of crystallization nuclei in high-density amorphous ice. – Workshop on Phase Transformations and Novel Materials, Obergurgl, Österreich, 03.–05.11.2011.
  • Seidl, M.; Winkel, K.; Loerting, T.; Mayer, E.; Karsai, F.; Zifferer, G.: Are amorphous ices connected to liquid states? Answers from experimental and in silico studies. – Bunsentagung 2011, Berlin, Deutschland, 02.–04.06.2011.
  • Seidl, M.; Elsaesser, M. S.; Winkel, K.; Handle, P. H.; Zifferer, G.; Mayer, E.; Loerting, T.: Kristallisationsverhalten und Glasübergang von amorphem Eis unter Druck. – 1. Eis- und Clathrat-Treffen, Odenwald, Deutschland, 05.–07.10.2010.
  • Seidl, M.; Elsaesser, M. S.; Zifferer, G.; Mayer, E.; Loerting, T.: The volumetric glass transition and crystallization behavior of high-density amorphous ice (HDA). – 10th International Workshop on Non-Crystalline Solids, Barcelona, Spanien, 21.–23.04.2010.
  • Seidl, M.: Repräsentation des Stoffes Wasser in Molekulardynamik-Simulationen. – StipendiatInnenwochenende der Österreichischen Akademie der Wissenschaften, Wien, Österreich, 26.–27.02.2010.
  • Fuentes Landete, V.; Köster, K. W.; Raidt, A.; Seidl, M.; Gainaru, C.; Loerting, T.; Böhmer, R.: Dynamics enhanced by HCl doping triggers full Pauling entropy release at the ice XII–XIV transition – 16. Österreichische Chemietage, Innsbruck, Österreich, 21.–24.09.2015.
  • Jehser, M.; Seidl, M.; Loerting, T.; Zifferer, G.: Studies of amorphous ice by molecular dynamics simulations – 16. Österreichische Chemietage, Innsbruck, Österreich, 21.–24.09.2015.
  • Fuentes Landete, V.; Köster, K. W.; Raidt, A.; Seidl, M.; Gainaru, C.; Loerting, T.; Böhmer, R.: Dynamics enhanced by HCl doping triggers full Pauling entropy release at the ice XII–XIV transition – Roma Tre Workshop on Water under Extreme Conditions, Rom, Italien, 10.–12.06.2015.
  • Seidl, M.; Handle, P. H.; Amann-Winkel, K.; Zifferer, G.; Loerting, T.: How stable is high-density amorphous ice against crystallization? – WATER 2014: Metastability and nucleation in water, Les Houches, Frankreich, 01.–06.06.2014.
  • Jehser, M.; Seidl, M.; Loerting, T.; Zifferer, G.: Atomistic molecular dynamics simulations of amorphous ice. – Bunsentagung 2014, Hamburg, Deutschland, 29.–31.05.2014.
  • Seidl, M.; Handle, P. H.; Amann-Winkel, K.; Zifferer, G.; Loerting, T.: Dynamical and thermodynamical properties of amorphous ice: B. Experimental advancements. – 15. Österreichische Chemietage, Graz, Österreich, 23.–26.09.2013.
  • Seidl, M.; Jehser, M.; Rauer, C.; Loerting, T.; Zifferer, G.: Simulation of high-density water: Its glass transition for various water models. – 7th International Discussion Meeting on Relaxations in Complex Systems, Barcelona, Spanien, 21.–26.07.2013.
  • Seidl, M.; Dalal, S. S.; Ediger, M. D.: Diffusion-controlled and diffusionless crystal growth of tris-naphthylbenzene isomers. – 7th International Discussion Meeting on Relaxations in Complex Systems, Barcelona, Spanien, 21.–26.07.2013.
  • Seidl, M.; Handle, P. H.; Winkel, K.; Elsaesser, M. S.; Zifferer, G.; Mayer, E.; Loerting, T.: The glass-to-liquid transition of high-density amorphous ice, revealed from τ(T), V(T) and Cp(T). – Gordon Research Conference on Water and Aqueous Solutions, Holderness, New Hampshire, Vereinigte Staaten, 12.–17.08.2012.
  • Seidl, M.; Karsai, F.; Loerting, T.; Zifferer, G.: Molecular dynamics studies of amorphous ices. – 14. Österreichische Chemietage, Linz, Österreich, 26.–29.09.2011.
  • Handle, P. H.; Seidl, M.; Mayer, E.; Loerting, T.: Structural relaxation times in high-density amorphous ice (HDA). – 8th Liquid Matter Conference, Wien, Österreich, 06.–10.09.2011.
  • Seidl, M.; Winkel, K.; Handle, P. H.; Zifferer, G.; Mayer, E.; Loerting, T.: Presence and absence of crystallization nuclei in high-density amorphous ice. – 8th Liquid Matter Conference, Wien, Österreich, 06.–10.09.2011.
  • Seidl, M.; Karsai, F.; Loerting, T.; Zifferer, G.: Quantities affecting the glass transition temperature of amorphous ices in molecular dynamics. – 8th Liquid Matter Conference, Wien, Österreich, 06.–10.09.2011.
  • Winkel, K.; Handle, P.; Elsaesser, M. S.; Seidl, S.; Mayer, E.; Loerting, T.: Amorphous ices – the glassy states of water. – Passion for Knowledge, Donostia-San Sebastián, Spanien, 27.09.–01.10.2010.
  • Seidl, M.; Zifferer, G.; Loerting, T.: Das Wesen amorpher Eisformen. – StipendiatInnenwochenende der Österreichischen Akademie der Wissenschaften, Wien, Österreich, 26.–27.02.2010.
  • Seidl, M.; Elsaesser, M. S.; Handle, P.; Zifferer, G.; Mayer, E.; Loerting, T.: Volumetric glass-to-liquid transition in amorphous ices. – XVIII International Conference on Horizons in Hydrogen Bond Research, Paris, Frankreich, 14.–18.09.2009.
  • Bernard, J.; Winkel, K.; Seidl, M.; Hage, W.; Loerting, T.; Price, S. L.; Mayer, E.: Retention of hydrogen-bond motif in solid H2CO3: Crystallization of two polymorphs from two amorphous forms. – XVIII International Conference on Horizons in Hydrogen Bond Research, Paris, Frankreich, 14.–18.09.2009.
  • Seidl, M.; Elsaesser, M. S.; Mayer, E.; Loerting, T.; Zifferer, G.: The volumetric glass-to-liquid transition in high density amorphous ice (HDA). – Bunsentagung 2009, Köln, Deutschland, 21.–23.05.2009.
  • Seidl, M.; Elsaesser, M. S.; Mayer, E.; Loerting, T.; Zifferer, G.: Simulation and experiment: The volumetric glass-to-liquid transition in high density amorphous ice (HDA). – 2. GÖCH-Symposium Physikalische Chemie, Innsbruck, Österreich, 23.–24.02.2009.
  • Elsaesser, M. S.; Seidl, M.; Kohl, I.; Mayer, E.; Loerting, T.: The volumetric glass-to-liquid transition at high pressures: Glycerol and low density amorphous ice (LDA). – 2. GÖCH-Symposium Physikalische Chemie, Innsbruck, Österreich, 23.–24.02.2009.
  • Winkel, K.; Bernard, J.; Seidl, M.; Hage, W.; Loerting, T.; Price, S. L.; Mayer, E.: Crystallization of amorphous carbonic acid studied by FT-IR spectroscopy: Evidence for amorphous polymorphism. – 58. Jahrestagung der Österreichischen Physikalischen Gesellschaft, Leoben, Österreich, 22.–26.09.2008.
  • Elsaesser, M. S.; Seidl, M.; Kohl, I.; Mayer, E.; Loerting, T.: The volumetric glass→liquid transition at high pressures: Glycerol and low density amorphous ice (LDA). – 7th Liquid Matter Conference, Lund, Schweden, 27.06.–01.07.2008.

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