@misc{KarKoerzdoerfer2020, author = {Kar, Manaswita and K{\"o}rzd{\"o}rfer, Thomas}, title = {Computational high throughput screening of inorganic cation based halide perovskites for perovskite only tandem solar cells}, series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, number = {5}, issn = {1866-8372}, doi = {10.25932/publishup-51683}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-516831}, pages = {11}, year = {2020}, abstract = {We search for homovalent alternatives for A, B, and X-ions in ABX(3) type inorganic halide perovskites suitable for tandem solar cell applications. We replace the conventional A-site organic cation CH3NH3, by 3 inorganic cations, Cs, K, and Rb, and the B site consists of metals; Cd, Hg, Ge, Pb, and Sn This work is built on our previous high throughput screening of hybrid perovskite materials (Kar et al 2018 J. Chem. Phys. 149, 214701). By performing a systematic screening study using Density Functional Theory (DFT) methods, we found 11 suitable candidates; 2 Cs-based, 3 K-based and 6 Rb-based that are suitable for tandem solar cell applications.}, language = {en} } @article{BalischewskiChoiBehrensetal.2021, author = {Balischewski, Christian and Choi, Hyung-Seok and Behrens, Karsten and Beqiraj, Alkit and K{\"o}rzd{\"o}rfer, Thomas and Gessner, Andre and Wedel, Armin and Taubert, Andreas}, title = {Metal sulfide nanoparticle synthesis with ionic liquids state of the art and future perspectives}, series = {ChemistryOpen}, volume = {10}, journal = {ChemistryOpen}, number = {2}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2191-1363}, doi = {10.1002/open.202000357}, pages = {272 -- 295}, year = {2021}, abstract = {Metal sulfides are among the most promising materials for a wide variety of technologically relevant applications ranging from energy to environment and beyond. Incidentally, ionic liquids (ILs) have been among the top research subjects for the same applications and also for inorganic materials synthesis. As a result, the exploitation of the peculiar properties of ILs for metal sulfide synthesis could provide attractive new avenues for the generation of new, highly specific metal sulfides for numerous applications. This article therefore describes current developments in metal sulfide nano-particle synthesis as exemplified by a number of highlight examples. Moreover, the article demonstrates how ILs have been used in metal sulfide synthesis and discusses the benefits of using ILs over more traditional approaches. Finally, the article demonstrates some technological challenges and how ILs could be used to further advance the production and specific property engineering of metal sulfide nanomaterials, again based on a number of selected examples.}, language = {en} } @article{KarKoerzdoerfer2020, author = {Kar, Manaswita and K{\"o}rzd{\"o}rfer, Thomas}, title = {Computational high throughput screening of inorganic cation based halide perovskites for perovskite only tandem solar cells}, series = {Materials Research Express}, volume = {7}, journal = {Materials Research Express}, number = {5}, publisher = {IOP Publ. Ltd.}, address = {Bristol}, issn = {2053-1591}, doi = {10.1088/2053-1591/ab8c0d}, pages = {1 -- 10}, year = {2020}, abstract = {We search for homovalent alternatives for A, B, and X-ions in ABX(3) type inorganic halide perovskites suitable for tandem solar cell applications. We replace the conventional A-site organic cation CH3NH3, by 3 inorganic cations, Cs, K, and Rb, and the B site consists of metals; Cd, Hg, Ge, Pb, and Sn This work is built on our previous high throughput screening of hybrid perovskite materials (Kar et al 2018 J. Chem. Phys. 149, 214701). By performing a systematic screening study using Density Functional Theory (DFT) methods, we found 11 suitable candidates; 2 Cs-based, 3 K-based and 6 Rb-based that are suitable for tandem solar cell applications.}, language = {en} } @article{XiongWłodarczykGallandietal.2018, author = {Xiong, Tao and Włodarczyk, Radosław Stanisław and Gallandi, Lukas and K{\"o}rzd{\"o}rfer, Thomas and Saalfrank, Peter}, title = {Vibrationally resolved photoelectron spectra of lower diamondoids}, series = {The journal of chemical physics : bridges a gap between journals of physics and journals of chemistry}, volume = {148}, journal = {The journal of chemical physics : bridges a gap between journals of physics and journals of chemistry}, number = {4}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0021-9606}, doi = {10.1063/1.5012131}, pages = {9}, year = {2018}, abstract = {Vibrationally resolved lowest-energy bands of the photoelectron spectra (PES) of adamantane, diamantane, and urotropine were simulated by a time-dependent correlation function approach within the harmonic approximation. Geometries and normal modes for neutral and cationic molecules were obtained from B3LYP hybrid density functional theory (DFT). It is shown that the simulated spectra reproduce the experimentally observed vibrational finestructure (or its absence) quite well. Origins of the finestructure are discussed and related to recurrences of autocorrelation functions and dominant vibrations. Remaining quantitative and qualitative errors of the DFT-derived PES spectra refer to (i) an overall redshift by ∼0.5 eV and (ii) the absence of satellites in the high-energy region of the spectra. The former error is shown to be due to the neglect of many-body corrections to ordinary Kohn-Sham methods, while the latter has been argued to be due to electron-nuclear couplings beyond the Born-Oppenheimer approximation [Gali et al., Nat. Commun. 7, 11327 (2016)].}, language = {en} } @article{AbouserieZehbeMetzneretal.2017, author = {Abouserie, Ahed and Zehbe, Kerstin and Metzner, Philipp and Kelling, Alexandra and G{\"u}nter, Christina and Schilde, Uwe and Strauch, Peter and K{\"o}rzd{\"o}rfer, Thomas and Taubert, Andreas}, title = {Alkylpyridinium Tetrahalidometallate Ionic Liquids and Ionic Liquid Crystals: Insights into the Origin of Their Phase Behavior}, series = {European journal of inorganic chemistry : a journal of ChemPubSoc Europe}, journal = {European journal of inorganic chemistry : a journal of ChemPubSoc Europe}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1434-1948}, doi = {10.1002/ejic.201700826}, pages = {5640 -- 5649}, year = {2017}, abstract = {Six N-alkylpyridinium salts [CnPy](2)[MCl4] (n = 4 or 12 and M = Co, Cu, Zn) were synthesized, and their structure and thermal properties were studied. The [C4Py](2)[MCl4] compounds are monoclinic and crystallize in the space group P2(1)/n. The crystals of the longer chain analogues [C12Py](2)[MCl4] are triclinic and crystallize in the space group P (1) over bar. Above the melting temperature, all compounds are ionic liquids (ILs). The derivatives with the longer C12 chain exhibit liquid crystallinity and the shorter chain compounds only show a melting transition. Consistent with single-crystal analysis, electron paramagnetic resonance spectroscopy suggests that the [CuCl4](2-) ions in the Cu-based ILs have a distorted tetrahedral geometry.}, language = {en} } @article{AbouserieZehbeMetzneretal.2017, author = {Abouserie, Ahed and Zehbe, Kerstin and Metzner, Philipp and Kelling, Alexandra and G{\"u}nter, Christina and Schilde, Uwe and Strauch, Peter and K{\"o}rzd{\"o}rfer, Thomas and Taubert, Andreas}, title = {Alkylpyridinium Tetrahalidometallate Ionic Liquids and Ionic Liquid Crystals: Insights into the Origin of Their Phase Behavior}, series = {European journal of inorganic chemistry : a journal of ChemPubSoc Europe}, journal = {European journal of inorganic chemistry : a journal of ChemPubSoc Europe}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1434-1948}, doi = {10.1002/ejic.201700826}, pages = {5640 -- 5649}, year = {2017}, abstract = {Six N-alkylpyridinium salts [CnPy](2)[MCl4] (n = 4 or 12 and M = Co, Cu, Zn) were synthesized, and their structure and thermal properties were studied. The [C4Py](2)[MCl4] compounds are monoclinic and crystallize in the space group P2(1)/n. The crystals of the longer chain analogues [C12Py](2)[MCl4] are triclinic and crystallize in the space group P (1) over bar. Above the melting temperature, all compounds are ionic liquids (ILs). The derivatives with the longer C12 chain exhibit liquid crystallinity and the shorter chain compounds only show a melting transition. Consistent with single-crystal analysis, electron paramagnetic resonance spectroscopy suggests that the [CuCl4](2-) ions in the Cu-based ILs have a distorted tetrahedral geometry.}, language = {en} } @article{KnightWangGallandietal.2016, author = {Knight, Joseph W. and Wang, Xiaopeng and Gallandi, Lukas and Dolgounitcheva, Olga and Ren, Xinguo and Ortiz, J. Vincent and Rinke, Patrick and K{\"o}rzd{\"o}rfer, Thomas and Marom, Noa}, title = {Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules III: A Benchmark of GW Methods}, series = {Journal of chemical theory and computation}, volume = {12}, journal = {Journal of chemical theory and computation}, publisher = {American Chemical Society}, address = {Washington}, issn = {1549-9618}, doi = {10.1021/acs.jctc.5b00871}, pages = {615 -- 626}, year = {2016}, abstract = {The performance of different GW methods is assessed for a set of 24 organic acceptors. Errors are evaluated with respect to coupled cluster singles, doubles, and perturbative triples [CCSD(T)] reference data for the vertical ionization potentials (IPs) and electron affinities (EAs), extrapolated to the complete basis set limit. Additional comparisons are made to experimental data, where available. We consider fully self-consistent GW (scGW), partial self-consistency in the Green's function (scGW0), non-self-consistent G0W0 based on several mean-field starting points, and a "beyond GW" second-order screened exchange (SOSEX) correction to G0W0. We also describe the implementation of the self-consistent Coulomb hole with screened exchange method (COHSEX), which serves as one of the mean-field starting points. The best performers overall are G0W0+SOSEX and G0W0 based on an IP-tuned long-range corrected hybrid functional with the former being more accurate for EAs and the latter for IPs. Both provide a balanced treatment of localized vs delocalized states and valence spectra in good agreement with photoemission spectroscopy (PES) experiments.}, language = {en} } @article{GallandiMaromRinkeetal.2016, author = {Gallandi, Lukas and Marom, Noa and Rinke, Patrick and K{\"o}rzd{\"o}rfer, Thomas}, title = {Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules II: Non-Empirically Tuned Long-Range Corrected Hybrid Functionals}, series = {Journal of chemical theory and computation}, volume = {12}, journal = {Journal of chemical theory and computation}, publisher = {American Chemical Society}, address = {Washington}, issn = {1549-9618}, doi = {10.1021/acs.jctc.5b00873}, pages = {605 -- 614}, year = {2016}, abstract = {The performance of non-empirically tuned long-range corrected hybrid functionals for the prediction of vertical ionization potentials (IPs) and electron affinities (EAs) is assessed for a set of 24 organic acceptor molecules. Basis set extrapolated coupled cluster singles, doubles, and perturbative triples [CCSD(T)] calculations serve as a reference for this study. Compared to standard exchange-correlation functionals, tuned long-range corrected hybrid functionals produce highly reliable results for vertical IPs and EAs, yielding mean absolute errors on par with computationally more demanding GW calculations. In particular, it is demonstrated that long-range corrected hybrid functionals serve as ideal starting points for non-self-consistent GW calculations.}, language = {en} } @article{BoisKoerzdoerfer2016, author = {Bois, Juliana and K{\"o}rzd{\"o}rfer, Thomas}, title = {0 How Bond Length Alternation and Thermal Disorder Affect the Optical Excitation Energies of pi-Conjugated Chains: A Combined Density Functional Theory and Molecular Dynamics Study}, series = {Journal of chemical theory and computation}, volume = {12}, journal = {Journal of chemical theory and computation}, publisher = {American Chemical Society}, address = {Washington}, issn = {1549-9618}, doi = {10.1021/acs.jctc.5b01070}, pages = {1872 -- 1882}, year = {2016}, abstract = {We dissect the sources of error leading to inaccuracies in the description of the geometry and optical excitation energies of pi-conjugated polymers. While the ground-state bond length alternation is shown to be badly reproduced by standard functionals, the recently adapted functionals PBEh* and omega PBE* as well as the double hybrid functional XYGJ-OS manage to replicate results obtained at the CCSD(T) level. By analysis of the bond length alternation in the excited state, a sensitive dependence of the exciton localization on the long-range behavior of the functional and the amount of Hartree-Fock exchange present is shown. Introducing thermal disorder through molecular dynamics simulations allows the consideration of a range of thermally accessible configurations of each oligomer, including trans to cis rotations, which break the conjugation of the backbone. Thermal disorder has a considerable effect when combined with functionals that overestimate the delocalization of the excitation, such as B3LYP. For functionals with a larger amount of exact exchange such as our PBEh* and omega PBE*, however, the effect is small, as excitations are often localized enough to fit between twists in the chain.}, language = {en} } @article{SunRynoZhongetal.2016, author = {Sun, Haitao and Ryno, Sean and Zhong, Cheng and Ravva, Mahesh Kumar and Sun, Zhenrong and K{\"o}rzd{\"o}rfer, Thomas and Bredas, Jean-Luc}, title = {Ionization Energies, Electron Affinities, and Polarization Energies of Organic Molecular Crystals: Quantitative Estimations from a Polarizable Continuum Model (PCM)-Tuned Range-Separated Density Functional Approach}, series = {Journal of chemical theory and computation}, volume = {12}, journal = {Journal of chemical theory and computation}, publisher = {American Chemical Society}, address = {Washington}, issn = {1549-9618}, doi = {10.1021/acs.jctc.6b00225}, pages = {2906 -- 2916}, year = {2016}, abstract = {We propose a new methodology for the first principles description of the electronic properties relevant for charge transport in organic molecular crystals. This methodology, which is based on the combination of a nonempirical, optimally tuned range separated hybrid functional with the polarizable continuum model, is applied to a series of eight representative molecular semiconductor crystals. We show that it provides ionization energies, electron affinities, and transport gaps in very good agreement with experimental values, as well as with the results of many-body perturbation theory-within the GW approximation at a fraction of the computational cost. Hence, this approach represents an easily applicable and computationally efficient tool to estimate the gas-to crystal phase shifts of the frontier-orbital quasiparticle energies in organic electronic materials.}, language = {en} }