Change search
ReferencesLink to record
Permanent link

Direct link
K- and L-edge X-ray absorption spectrum calculations of closed-shell carbon, silicon, germanium, and sulfur compounds using damped four-component density functional response theory
2016 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, no 19, 13591-13603 p.Article in journal (Refereed) Published
Abstract [en]

X-ray absorption spectra of carbon, silicon, germanium, and sulfur compounds have been investigated by means of damped four-component density functional response theory. It is demonstrated that a reliable description of relativistic effects is obtained at both K- and L-edges. Notably, an excellent agreement with experimental results is obtained for L2,3-spectra - with spin-orbit effects well accounted for - also in cases when the experimental intensity ratio deviates from the statistical one of 2:1. The theoretical results are consistent with calculations using standard response theory as well as recently reported real-time propagation methods in time-dependent density functional theory, and the virtues of different approaches are discussed. As compared to silane and silicon tetrachloride, an anomalous error in the absolute energy is reported for the L2,3-spectrum of silicon tetrafluoride, amounting to an additional spectral shift of ∼1 eV. This anomaly is also observed for other exchange-correlation functionals, but it is seen neither at other silicon edges nor at the carbon K-edge of fluorine derivatives of ethene. Considering the series of molecules SiH4-XFX with X = 1, 2, 3, 4, a gradual divergence from interpolated experimental ionization potentials is observed at the level of Kohn-Sham density functional theory (DFT), and to a smaller extent with the use of Hartree-Fock. This anomalous error is thus attributed partly to difficulties in correctly emulating the electronic structure effects imposed by the very electronegative fluorines, and partly due to inconsistencies in the spurious electron self-repulsion in DFT. Substitution with one, or possibly two, fluorine atoms is estimated to yield small enough errors to allow for reliable interpretations and predictions of L2,3-spectra of more complex and extended silicon-based systems. © the Owner Societies 2016.

Place, publisher, year, edition, pages
2016. Vol. 18, no 19, 13591-13603 p.
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-198704DOI: 10.1039/c6cp00561fScopusID: 2-s2.0-84971351134OAI: oai:DiVA.org:kth-198704DiVA: diva2:1059138
Note

References: Norman, P., (2011) Phys. Chem. Chem. Phys., 13, p. 20519; Ekström, U., Norman, P., Carravetta, V., Ågren, H., (2006) Phys. Rev. Lett., 97, p. 143001; Ekström, U., Norman, P., (2006) Phys. Rev. A: At., Mol., Opt. Phys., 74, p. 042722; Norman, P., Bishop, D.M., Jensen, H.J.Aa., Oddershede, J., (2001) J. Chem. Phys., 115, p. 10323; Norman, P., Bishop, D.M., Jensen, H.J.Aa., Oddershede, J., (2005) J. Chem. Phys., 123, p. 194103; Fransson, T., Zhovtobriukh, I., Coriani, S., Wikfeldt, K.T., Norman, P., Pettersson, L.G.M., (2016) Phys. Chem. Chem. Phys., 18, p. 566; Schwarz, W.H.E., (1975) J. Chem. Phys., 11, p. 217; Fronzoni, G., Stener, M., Decleva, P., Wang, F., Ziegler, T., Van Lenthe, E., Baerends, E.J., (2005) Chem. Phys. Lett., 416, p. 56; Maganas, D., Roemelt, M., Weyhermüller, T., Blume, R., Hävecker, M., Knop-Gerick, A., DeBeer, S., Neese, F., (2014) Phys. Chem. Chem. Phys., 16, p. 264; Josefsson, I., Kunnus, K., Schreck, S., Föhlisch, A., De Groot, F., Wernet, Ph., Odelius, M., (2012) J. Phys. Chem. Lett., 3, p. 3565; Pinjari, R.V., Delcey, M.G., Guo, M., Odelius, M., Lundberg, M., (2014) J. Chem. Phys., 141, p. 124116; Engel, N., Bokarev, S.I., Suljoti, E., Garcia-Diez, R., Lange, K.M., Atak, K., Golnak, R., Aziz, E.F., (2014) J. Phys. Chem. B, 118, p. 1555; Grell, G., Bokarev, S.I., Winter, B., Seidel, R., Aziz, E.F., Aziz, S.G., Kühn, O., (2015) J. Chem. Phys., 143, p. 074104; Krüger, P., Natoli, C.R., (2004) Phys. Rev. B: Condens. Matter Mater. Phys., 70, p. 245120; Ikeno, H., De Groot, F.M.F., Stavitski, E., Tanaka, I., (2009) J. Phys.: Condens. Matter, 21, p. 104208; Roemelt, M., Maganas, D., DeBeer, S., Neese, F., (2013) J. Chem. Phys., 138, p. 204101; Ogasawara, K., Iwata, T., Koyama, Y., Ishii, T., Tanaka, I., Adachi, H., (2001) Phys. Rev. B: Condens. Matter Mater. Phys., 94, p. 115413; Ikeno, H., Tanaka, I., Koyama, Y., Mizogichi, T., Ogasawara, K., (2005) Phys. Rev. B: Condens. Matter Mater. Phys., 72, p. 075123; Ikeno, H., Mizoguchi, T., Tanaka, I., (2011) Phys. Rev. B: Condens. Matter Mater. Phys., 83, p. 155107; Vinson, J., Rehr, J.J., Kas, J.J., Shirley, E.L., (2011) Phys. Rev. B: Condens. Matter Mater. Phys., 83, p. 115106; Laskowski, R., Blaha, P., (2010) Phys. Rev. B: Condens. Matter Mater. Phys., 82, p. 205104; Shirley, E.L., (2005) J. Electron Spectrosc. Relat. Phenom., 144-147, p. 1187; Gilmore, K., Vinson, J., Shirley, E.L., Prendergast, D., Pemmaraju, C.D., Kas, J.J., Vila, F.D., Rehr, J.J., (2015) Comput. Phys. Commun., 197, p. 109; Haverkort, M.W., Zwierzycki, M., Andersen, O.K., (2012) Phys. Rev. B: Condens. Matter Mater. Phys., 85, p. 165113; Ekström, U., Norman, P., Carravetta, V., (2006) Phys. Rev. A: At., Mol., Opt. Phys., 73, p. 022501; Villaume, S., Ekström, U., Ottosson, H., Norman, P., (2010) Phys. Chem. Chem. Phys., 12, p. 5596; Mangoine, G., Sambi, M., Nardi, M.V., Casarin, M., (2014) Phys. Chem. Chem. Phys., 16, p. 19852; Mangione, G., Pandolfo, L., Sambi, M., Ligorio, G., Nardi, M.V., Cossaro, A., Floreano, L., Casarin, M., (2015) Eur. J. Inorg. Chem., p. 2707; Repisky, M., Konecny, L., Kadek, M., Komorovsky, S., Malkin, O.L., Malkin, V.G., Ruud, K., (2015) J. Chem. Theory Comput., 11, p. 980; Kadek, M., Konecny, L., Gao, B., Repisky, M., Ruud, K., (2015) Phys. Chem. Chem. Phys., 17, p. 22566; Coriani, S., Fransson, T., Christiansen, O., Norman, P., (2012) J. Chem. Theory Comput., 8, p. 1616; Fransson, T., Coriani, S., Christiansen, O., Norman, P., (2013) J. Chem. Phys., 138, p. 124311; Kauczor, J., Norman, P., Christiansen, O., Coriani, S., (2013) J. Chem. Phys., 139, p. 211102; Vahlberg, C., Linares, M., Villaume, S., Norman, P., Uvdal, K., (2011) J. Phys. Chem. C, 115, p. 165; Villaume, S., Saue, T., Norman, P., (2010) J. Chem. Phys., 133, p. 064105; Fransson, T., Saue, T., Norman, P., (2016) J. Chem. Theory Comput.; Friedrich, H., Sonntag, B., Rabe, P., Butscher, W., Schwarz, W.H.E., (1979) Chem. Phys. Lett., 64, p. 360; Bozek, J.D., Tan, K.H., Bancroft, G.M., (1987) Chem. Phys. Lett., 138, p. 33; Ferrett, T.A., Piancastelli, M.N., Lindle, D.W., Heimann, P.A., Shirley, D.A., (1988) Phys. Rev. A: At., Mol., Opt. Phys., 38, p. 701; Cooper, G., Ibuki, T., Brion, C.E., (1990) Chem. Phys., 140, p. 147; Bozek, J.D., Bancroft, G.M., Tan, K.H., (1990) Chem. Phys., 145, p. 131; Guo, X., Cooper, G., Chan, W.-F., Burton, G.R., Brion, C.E., (1992) Chem. Phys., 161, p. 471; Cooper, G., Burton, G.R., Chan, W.F., Brion, C.E., (1995) Chem. Phys., 196, p. 293; Chen, J.-M., Klauser, R., Yang, S.-C., Wen, C.-R., (1995) J. Phys. Chem. Lett., 246, p. 285; Püttner, R., Domke, M., Lentz, D., Kaindl, G., (1997) Phys. Rev. A: At., Mol., Opt. Phys., 56, p. 1228; Püttner, R., Domke, M., Kaindl, G., (1998) Phys. Rev. A: At., Mol., Opt. Phys., 57, p. 297; Miron, C., Guillemin, R., Leclercq, N., Morin, P., Simon, M., (1998) J. Electron Spectrosc. Relat. Phenom., 93, p. 95; Cooper, L., Shpinkova, L.G., Holland, D.M.P., Shaw, D.A., (2001) Chem. Phys., 270, p. 363; Sutherland, D.G.J., Bancroft, G.M., Bozek, J.D., Tan, K.H., (1992) Chem. Phys. Lett., 199, p. 341; Bodeur, S., Nenner, I., Millié, P., (1986) Phys. Rev. A: At., Mol., Opt. Phys., 34, p. 2986; Bodeur, S., Millié, P., Nenner, I., (1990) Phys. Rev. A: At., Mol., Opt. Phys., 41, p. 252; Ishikawa, H., Fujima, K., Adachi, H., Miyauchi, E., Fujii, T., (1991) J. Chem. Phys., 94, p. 6740; Chong, D.P., Segala, M., Takahata, Y., Baerends, E.J., (2008) Int. J. Quantum Chem., 108, p. 1358; Toffoli, D., Stener, M., Decleva, P., (2006) Phys. Rev. A: At., Mol., Opt. Phys., 73, p. 042704; Boyd, R.W., (2008) Nonlinear Optics, , Academic Press, San Diego, 3rd edn; Kauczor, J., Jørgensen, P., Norman, P., (2011) J. Chem. Theory Comput., 7, p. 1610; Kauczor, J., Norman, P., (2014) J. Chem. Theory Comput., 10, p. 2449; Casida, M.E., Time-dependent density-functional response theory for molecules (1995) Recent Advances in Density Functional Methods Part i, , ed. D. Chong, World Scientific, Singapore; Davidson, E.R., (1975) J. Comput. Phys., 17, p. 87; Wenzel, J., Wormit, M., Dreuw, A., (2014) J. Comput. Chem., 35, p. 1900; Peng, B., Lestrange, P.J., Goings, J.J., Caricato, M., Li, X., (2015) J. Chem. Theory Comput., 11, p. 4146; Besley, N.A., Asmuruf, F.A., (2010) Phys. Chem. Chem. Phys., 12, p. 12024; Skowron, S.T., Besley, N.A., (2012) Theor. Chem. Acc., 131, p. 1267; Lestrange, P.J., Nguyen, P.D., Li, X., (2015) J. Chem. Theory Comput., 11, p. 2994; Besley, N.A., Peach, M.J.G., Tozer, D.J., (2009) Phys. Chem. Chem. Phys., 11, p. 10350; Tu, G., Carravetta, V., Vahtras, O., Ågren, H., (2007) J. Chem. Phys., 127, p. 174110; Tu, G., Rinkevicius, Z., Vahtras, O., Ågren, H., Ekström, U., Norman, P., Carravetta, V., (2007) Phys. Rev. A: At., Mol., Opt. Phys., 76, p. 022506; Yanai, T., Tew, D.P., Handy, N.C., (2004) Chem. Phys. Lett., 393, p. 51; Ab Initio, , http://www.diracprogram.org, DIRAC, a relativistic electronic structure program, Release DIRAC13 (2013), written by L. Visscher, H. J. A. Jensen, R. Bast and T. Saue, with contributions from V. Bakken, K. G. Dyall, S. Dubillard, U. Ekström, E. Eliav, T. Enevoldsen, E. Faßhauer, T. Fleig, O. Fossgaard, A. S. Gomes, T. Helgaker, J. K. Lærdahl, Y. S. Lee, J. Henriksson, M. Iliaš, Ch. R. Jacob, S. Knecht, S. Komorovský, O. Kullie, C. V. Larsen, H. S. Nataraj, Norman, G. Olejniczak, J. Olsen, Y. C. Park, J. K. Pedersen, M. Pernpointner, K. Ruud, Sałek, B. Schimmelpfennig, J. Sikkema, A. J. Thorvaldsen, J. Thyssen, J. van Stralen, S. Villaume, O. Visser, T. Winther and S. Yamamoto (see); Frisch, M.J., Trucks, G.W., Schlegel, H.B., Scuseria, G.E., Robb, M.A., Cheeseman, J.R., Montgomery, J.A., Jr., Pople, J.A., (2004) Gaussian 03, Revision E.01., , Gaussian, Inc., Wallingford CT; Becke, A.D., (1993) J. Chem. Phys., 98, p. 5648; Dunning, T.H., (1989) J. Chem. Phys., 90, p. 1007; Woon, D.E., Dunning, T.H., (1995) J. Chem. Phys., 103, p. 4572; Kendall, R.A., Dunning, T.H., Harrison, R.J., (1992) J. Chem. Phys., 96, p. 6796; Visscher, L., (1997) Theor. Chem. Acc., 98, p. 68; Ilias, M., Saue, T., (2007) J. Chem. Phys., 126, p. 064102; Lévy-Leblond, J.-M., (1967) Commun. Math. Phys., 6, p. 286; Dyall, K.G., (1994) J. Chem. Phys., 100, p. 2118; Van Lenthe, J.H., Zwaans, R., Van Dam, H.J.J., Guest, M.F., (2006) J. Comput. Chem., 27, p. 926; Leetmaa, M., Ljungberg, M.P., Lyubartsev, A., Nilsson, A., Pettersson, L.G.M., (2010) J. Electron Spectrosc. Relat. Phenom., 177, p. 135; Cukras, J., Coriani, S., Decleva, P., Christiansen, O., Norman, P., (2013) J. Chem. Phys., 139, p. 094103; Coriani, S., Christiansen, O., Fransson, T., Norman, P., (2012) Phys. Rev. A: At., Mol., Opt. Phys., 85, p. 022507; Wenzel, J., Holzer, A., Wormit, M., Dreuw, A., (2015) J. Chem. Phys., 142, p. 214104; Bernadotte, S., Atkins, A.J., Jacob, C.R., (2012) J. Chem. Phys., 137, p. 204106; List, N.H., Kauczor, J., Saue, T., Jensen, H.J.Aa., Norman, P., (2015) J. Chem. Phys., 142, p. 244111; Cardona, M., Ley, L., (1978) Photoemission in Solids I: General Principles, , ed., Springer-Verlag, Berlin; Takahashi, O., Tashiro, M., Ehara, M., Yamasaki, K., Ueda, K., (2011) Chem. Phys., 384, p. 28; Thomas, T.D., Miron, C., Wiesner, K., Morin, P., Carroll, T.X., Sæthre, L.J., (2002) Phys. Rev. Lett., 89, p. 22; Imamura, Y., Otsuka, T., Nakai, H., (2007) J. Comput. Chem., 28, p. 2067; Stanton, J.F., Gauss, J., (1999) J. Chem. Phys., 111, p. 8785; Coriani, S., Koch, H., (2015) J. Chem. Phys., 143, p. 181103; Baev, A., Gel'Mukhanov, F., Kimberg, V., Ågren, H., (2003) J. Phys. B: At., Mol. Opt. Phys., 36, p. 3761; Saidi, W.A., Norman, P., (2014) Carbon, 67, p. 17; McLaren, R., Clark, S.A.C., Ishii, I., Hitchcock, A.P., (1987) Phys. Rev. A: At., Mol., Opt. Phys., 36, p. 1683; Wen, A.T., Hitchcock, A.P., http://unicorn.mcmaster.ca/corex/cedb-title.html, Gas Phase Core Excitation DatabaseHudson, E., Shirley, D.A., Domke, M., Remmers, G., Puschmann, A., Mandel, T., Xue, C., Kaindl, G., (1993) Phys. Rev. A: At., Mol., Opt. Phys., 47, p. 361

Available from: 2016-12-22 Created: 2016-12-21 Last updated: 2016-12-22

Open Access in DiVA

No full text

Other links

Publisher's full textScopus

Search in DiVA

By author/editor
Norman, P.
In the same journal
Physical Chemistry, Chemical Physics - PCCP
Theoretical Chemistry

Search outside of DiVA

GoogleGoogle Scholar

Altmetric score

ReferencesLink to record
Permanent link

Direct link