TY  - JOUR
A1  - Kenfack, A.
A1  - Banerjee, Shiladitya
A1  - Paulus, Beate
T1  - Probing electron correlation in molecules via quantum fluxes
JF  - Physical review : A, Atomic, molecular, and optical physics
N2  - We present quantum simulations of a vibrating hydrogen molecule H-2 and address the issue of electron correlation. After appropriately setting the frame and the observer plane, we were able to determine precisely the number of electrons and nuclei which actually flow by evaluating electronic and nuclear fluxes. This calculation is repeated for three levels of quantum chemistry, for which we account for no correlation, Hartree-Fock, static correlation, and dynamic correlation. Exciting each of these systems with the same amount of energy, we show that the electron correlation can be revealed with the knowledge of quantum fluxes. This is evidenced by a clear sensitivity of these fluxes to electron correlation. In particular, we find that this correlation remarkably enhances more electronic yield than the nuclear one. It turns out that less electrons accompany the nuclei in Hartree-Fock than in the correlation cases.
Y1  - 2012
U6  - https://doi.org/10.1103/PhysRevA.85.032501
SN  - 1050-2947
VL  - 85
IS  - 3
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Lindic, Tilen
A1  - Sinha, Shreya
A1  - Mattsson, Stefan
A1  - Paulus, Beate
T1  - Prediction of a model crystal structure for Ni2F5 by first-principles calculations
JF  - Zeitschrift für Naturforschung : B, Chemical sciences
N2  - Electrochemical fluorination in anhydrous HF, also known as the Simons process, is a widely used industrial method for fluorination of organic compounds. Its mechanism, being not so well understood, has long been debated and is believed to involve higher valent nickel fluorides formed on the nickel-plated anode during the process. One of these is speculated to be Ni2F5, which was previously reported in the literature and assigned via infrared spectroscopy, but its crystal structure is not yet known. We have identified known crystal structures of compounds with similar stoichiometries as Ni2F5 and utilized them as a starting point for our periodic DFT investigations, applying the PBE+U method. Ni2F5 as the most stable polymorph was found to be of the same crystal structure as another mixed valent fluoride, Cr2F5. The calculated lattice parameters are a = 7.24 angstrom, b = 7.40 angstrom, c = 7.08 angstrom and beta = 118.9 degrees with an antiferromagnetic ordering of the nickel magnetic moments.
KW  - crystal structure prediction
KW  - DFT
KW  - Ni2F5
Y1  - 2022
U6  - https://doi.org/10.1515/znb-2022-0072
SN  - 0932-0776
SN  - 1865-7117
VL  - 77
IS  - 6
SP  - 469
EP  - 473
PB  - De Gruyter
CY  - Berlin
ER  - 
TY  - JOUR
A1  - Wirth, Jonas
A1  - Schacht, Julia
A1  - Saalfrank, Peter
A1  - Paulus, Beate
T1  - Fluorination of the Hydroxylated alpha-Al2O3 (0001) and Its Implications for Water Adsorption: A Theoretical Study
JF  - The journal of physical chemistry : C, Nanomaterials and interfaces
N2  - Fluorination of the hydroxylated alpha-Al2O3 (0001) surface is studied using periodic density functional theory calculations. On the basis of a hypothetical reaction substituting surface hydroxyl groups with fluorine atoms, we find surface fluorination to be strongly exergonic but kinetically hindered. Fluorinated surface areas turn out to be rather hydrophobic as compared to hydroxylated areas, suggesting fluorination as a potential route for tuning oxide surface properties such as hydrophilicity.
Y1  - 2016
U6  - https://doi.org/10.1021/acs.jpcc.5b10975
SN  - 1932-7447
VL  - 120
SP  - 9713
EP  - 9718
PB  - American Chemical Society
CY  - Washington
ER  -