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1. Evidence of a liquid–liquid phase transition in H$$_2$$O and D$$_2$$O from path-integral molecular dynamics simulations

   https://doi.org/10.1038/s41598-022-09525-x  

   Eltareb, Ali ; Lopez, Gustavo E. ; Giovambattista, Nicolas ( April 2022 , Scientific Reports)

   We perform path-integral molecular dynamics (PIMD), ring-polymer MD (RPMD), and classical MD simulations of H$$_2$$${}_2$O and D$$_2$$${}_2$O using the q-TIP4P/F water model over a wide range of temperatures and pressures. The density$$\rho (T)$$$\rho \left(T\right)$, isothermal compressibility$$\kappa _T(T)$$${\kappa }_T\left(T\right)$, and self-diffusion coefficientsD(T) of H$$_2$$${}_2$O and D$$_2$$${}_2$O are in excellent agreement with available experimental data; the isobaric heat capacity$$C_P(T)$$$C_P\left(T\right)$obtained from PIMD and MD simulations agree qualitatively well with the experiments. Some of these thermodynamic properties exhibit anomalous maxima upon isobaric cooling, consistent with recent experiments and with the possibility that H$$_2$$${}_2$O and D$$_2$$${}_2$O exhibit a liquid-liquid critical point (LLCP) at low temperatures and positive pressures. The data from PIMD/MD for H$$_2$$${}_2$O and D$$_2$$${}_2$O can be fitted remarkably well using the Two-State-Equation-of-State (TSEOS). Using the TSEOS, we estimate that the LLCP for q-TIP4P/F H$$_2$$${}_2$O, from PIMD simulations, is located at$$P_c = 167 \pm 9$$$P_c=167\pm 9$ MPa,$$T_c = 159 \pm 6$$$T_c=159\pm 6$ K, and$$\rho _c = 1.02 \pm 0.01$$${\rho }_c=1.02\pm 0.01$ g/cm$$^3$$${}^3$. Isotope substitution effects are important; the LLCP location in q-TIP4P/F D$$_2$$${}_2$O is estimated to be$$P_c = 176 \pm 4$$$P_c=176\pm 4$ MPa,$$T_c = 177 \pm 2$$$T_c=177\pm 2$ K, and$$\rho _c = 1.13 \pm 0.01$$${\rho }_c=1.13\pm 0.01$ g/cm$$^3$$${}^3$. Interestingly, for the water model studied, differences in the LLCP location from PIMD and MD simulations suggest that nuclear quantum effects (i.e., atoms delocalization) play an important role in the thermodynamics of water around the LLCP (from the MD simulations of q-TIP4P/F water,$$P_c = 203 \pm 4$$$P_c=203\pm 4$ MPa,$$T_c = 175 \pm 2$$$T_c=175\pm 2$ K, and$$\rho _c = 1.03 \pm 0.01$$${\rho }_c=1.03\pm 0.01$ g/cm$$^3$$${}^3$). Overall, our results strongly support the LLPT scenario to explain water anomalous behavior, independently of the fundamental differences between classical MD and PIMD techniques. The reported values of$$T_c$$$T_c$for D$$_2$$${}_2$O and, particularly, H$$_2$$${}_2$O suggest that improved water models are needed for the study of supercooled water.

    

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2. Roaming pathways and survival probability in real-time collisional dynamics of cold and controlled bialkali molecules

   https://doi.org/10.1038/s41598-021-90004-0  

   Kłos, Jacek ; Guan, Qingze ; Li, Hui ; Li, Ming ; Tiesinga, Eite ; Kotochigova, Svetlana ( May 2021 , Scientific Reports)

   Perfectly controlled molecules are at the forefront of the quest to explore chemical reactivity at ultra low temperatures. Here, we investigate for the first time the formation of the long-lived intermediates in the time-dependent scattering of cold bialkali$$^{23}\hbox {Na}^{87}$$${}^{23}{\text{Na}}^{87}$Rb molecules with and without the presence of infrared trapping light. During the nearly 50 nanoseconds mean collision time of the intermediate complex, we observe unconventional roaming when for a few tens of picoseconds either NaRb or$$\hbox {Na}_2$$${\text{Na}}_2$and$$\hbox {Rb}_2$$${\text{Rb}}_2$molecules with large relative separation are formed before returning to the four-atom complex. We also determine the likelihood of molecular loss when the trapping laser is present during the collision. We find that at a wavelength of 1064 nm the$$\hbox {Na}_2\hbox {Rb}_2$$${\text{Na}}_2{\text{Rb}}_2$complex is quickly destroyed and thus that the$$^{23}\hbox {Na}^{87}$$${}^{23}{\text{Na}}^{87}$Rb molecules are rapidly lost.

    

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3. Local structure elucidation of tungsten-substituted vanadium dioxide (V$$_{1-x}$$W$$_x$$O$$_2$$)

   https://doi.org/10.1038/s41598-022-18575-0  

   Wilson, Catrina E. ; Gibson, Amanda E. ; Cuillier, Paul M. ; Li, Cheng-Han ; Crosby, Patrice H. N. ; Trigg, Edward B. ; Najmr, Stan ; Murray, Christopher B. ; Jinschek, Joerg R. ; Doan-Nguyen, Vicky ( August 2022 , Scientific Reports)

   Initially, vanadium dioxide seems to be an ideal first-order phase transition case study due to its deceptively simple structure and composition, but upon closer inspection there are nuances to the driving mechanism of the metal-insulator transition (MIT) that are still unexplained. In this study, a local structure analysis across a bulk powder tungsten-substitution series is utilized to tease out the nuances of this first-order phase transition. A comparison of the average structure to the local structure using synchrotron x-ray diffraction and total scattering pair-distribution function methods, respectively, is discussed as well as comparison to bright field transmission electron microscopy imaging through a similar temperature-series as the local structure characterization. Extended x-ray absorption fine structure fitting of thin film data across the substitution-series is also presented and compared to bulk. Machine learning technique, non-negative matrix factorization, is applied to analyze the total scattering data. The bulk MIT is probed through magnetic susceptibility as well as differential scanning calorimetry. The findings indicate the local transition temperature ($$T_c$$$T_c$) is less than the average$$T_c$$$T_c$supporting the Peierls-Mott MIT mechanism, and demonstrate that in bulk powder and thin-films, increasing tungsten-substitution instigates local V-oxidation through the phase pathway VO$$_2\, \rightarrow$$${}_2\to$V$$_6$$${}_6$O$$_{13} \, \rightarrow$$${}_{13}\to$V$$_2$$${}_2$O$$_5$$${}_5$.

    

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4. Two coupled chains are simpler than one: field-induced chirality in a frustrated spin ladder

   https://doi.org/10.1038/s41598-020-72215-z  

   Pikulski, Marek ; Shiroka, Toni ; Casola, Francesco ; Reyes, Arneil P. ; Kuhns, Philip L. ; Wang, Shuang ; Ott, Hans-Rudolf ; Mesot, Joël ( September 2020 , Scientific Reports)

   Although the frustrated (zigzag) spin chain is the Drosophila of frustrated magnetism, our understanding of a pair of coupled zigzag chains (frustrated spin ladder) in a magnetic field is still lacking. We address this problem through nuclear magnetic resonance (NMR) experiments on BiCu$$_2$$${}_2$PO$$_6$$${}_6$in magnetic fields up to 45 T, revealing a field-induced spiral magnetic structure. Conjointly, we present advanced numerical calculations showing that even a moderate rung coupling dramatically simplifies the phase diagram below half-saturation magnetization by stabilizing a field-induced chiral phase. Surprisingly for a one-dimensional model, this phase and its response to Dzyaloshinskii-Moriya (DM) interactions adhere to classical expectations. While explaining the behavior at the highest accessible magnetic fields, our results imply a different origin for the solitonic phases occurring at lower fields in BiCu$$_2$$${}_2$PO$$_6$$${}_6$. An exciting possibility is that the known, DM-mediated coupling between chirality and crystal lattice may give rise to a new kind of spin-Peierls instability.

    

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5. Positron pair interactions in a nearly free-electron metal

   https://doi.org/10.1140/epjd/s10053-022-00406-6  

   Mills, Jr., Allen Paine ; Fuentes-Garcia, Melina ( June 2022 , The European Physical Journal D)

   The electric field surrounding a single positron in a metal is screened by an increase in the local electron density which, in the case of nearly free-electron metals (like Al, Na, etc.), has a radial distribution similar to that of the electron in positronium (Ps). In such metals, a singlet pair of positrons would experience an attractive interaction and at low enough electron densities could possibly form a bound state that is held together by exchange and correlation energies, thus forming structures analogous to that of the positronium molecule (Ps$$_2$$${}_2$), with binding energies of a few tenths of an eV. Such di-positrons could be prevalent at positron densities of around 10$$^{18}$$${}^{18}$cm$$^{-3}$$${}^{-3}$and, if so, would be evident from an apparent broadening of the sharp step at the Fermi surface in measurements of the electron momentum distribution by the angular correlation of the 2$$\gamma $$$\gamma$annihilation radiation. Even if di-positrons are not directly formed in a metal, optical spectroscopy of Ps$$_2$$${}_2$formed in vacuum via pairs of positrons simultaneously being emitted from the surface could be applied to the direct measurement of the momentum distribution of Cooper pairs. If they exist, di-positrons in metals would yield interesting information about electron and positron interactions and at very high densities might allow the study of a di-positron Bose–Einstein condensate immersed in an electron gas.

    

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