Orbital Density Reconstruction for Molecules

被引：79

作者：

Dauth, M. ^{[1
]}

Koerzdoerfer, T. ^{[1
]}

Kuemmel, S. ^{[1
]}

Ziroff, J. ^{[2
,3
]}

Wiessner, M. ^{[2
,3
]}

Schoell, A. ^{[2
,3
]}

Reinert, F. ^{[2
,3
]}

Arita, M. ^{[4
,5
]}

Shimada, K. ^{[4
,5
]}

机构：

[1] Univ Bayreuth, D-95440 Bayreuth, Germany

[2] Univ Wurzburg, Rontgen Res Ctr Complex Mat Syst RCCM, D-97074 Wurzburg, Germany

[3] KIT, Gemeinschaftslab Nanoanalyt, D-76021 Karlsruhe, Germany

[4] Hiroshima Univ, Hiroshima Synchrotron Radiat Ctr, Hiroshima 7398526, Japan

[5] Hiroshima Univ, Grad Sch Sci, Hiroshima 7398526, Japan

来源：

PHYSICAL REVIEW LETTERS | 2011年 / 107卷 / 19期

关键词：

D O I：

10.1103/PhysRevLett.107.193002

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

The experimental imaging of electronic orbitals has allowed one to gain a fascinating picture of quantum effects. We here show that the energetically high-lying orbitals that are accessible to experimental visualization in general differ, depending on which approach is used to calculate the orbitals. Therefore, orbital imaging faces the fundamental question of which orbitals are the ones that are visualized. Combining angular-resolved photoemission experiments with first-principles calculations, we show that the orbitals from self-interaction-free Kohn-Sham density functional theory are the ones best suited for the orbital-based interpretation of photoemission.

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页数：5

相关论文

共 24 条

[1] Interpretation of the Kohn-Sham orbital energies as approximate vertical ionization potentials [J].

Chong, DP ;

Gritsenko, OV ;

Baerends, EJ .

JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (05) :1760-1772

[2] Valence electronic structure of gas-phase 3,4,9,10-perylene tetracarboxylic acid dianhydride: Experiment and theory [J].

Dori, Navit ;

Menon, Mahesh ;

Kilian, Lennart ;

Sokolowski, Moritz ;

Kronik, Leeor ;

Umbach, Eberhard .

PHYSICAL REVIEW B, 2006, 73 (19)

[3] ASSESSMENT OF KOHN-SHAM DENSITY-FUNCTIONAL ORBITALS AS APPROXIMATE DYSON ORBITALS FOR THE CALCULATION OF ELECTRON-MOMENTUM-SPECTROSCOPY SCATTERING CROSS-SECTIONS [J].

DUFFY, P ;

CHONG, DP ;

CASIDA, ME ;

SALAHUB, DR .

PHYSICAL REVIEW A, 1994, 50 (06) :4707-4728

[4] Normal-incidence x-ray standing-wave determination of the adsorption geometry of PTCDA on Ag(111): Comparison of the ordered room-temperature and disordered low-temperature phases [J].

Hauschild, A. ;

Temirov, R. ;

Soubatch, S. ;

Bauer, O. ;

Schoell, A. ;

Cowie, B. C. C. ;

Lee, T. -L. ;

Tautz, F. S. ;

Sokolowski, M. .

PHYSICAL REVIEW B, 2010, 81 (12)

[5]

Hufner S., 2003, PHOTOELECTRON SPECTR, P10

[6] Tomographic imaging of molecular orbitals [J].

Itatani, J ;

Levesque, J ;

Zeidler, D ;

Niikura, H ;

Pépin, H ;

Kieffer, JC ;

Corkum, PB ;

Villeneuve, DM .

NATURE, 2004, 432 (7019) :867-871

[7] PROOF THAT DELTA-E-DELTA-NI=EPSILON-I IN DENSITY-FUNCTIONAL THEORY [J].

JANAK, JF .

PHYSICAL REVIEW B, 1978, 18 (12) :7165-7168

[8] Quantitative analysis of photoelectron angular distribution of single-domain organic monolayer film: NTCDA on GeS(001) [J].

Kera, S ;

Tanaka, S ;

Yamane, H ;

Yoshimura, D ;

Okudaira, KK ;

Seki, K ;

Ueno, N .

CHEMICAL PHYSICS, 2006, 325 (01) :113-120

[9] Single-particle and quasiparticle interpretation of Kohn-Sham and generalized Kohn-Sham eigenvalues for hybrid functionals [J].

Koerzdoerfer, T. ;

Kuemmel, S. .

PHYSICAL REVIEW B, 2010, 82 (15)

[10] When to trust photoelectron spectra from Kohn-Sham eigenvalues: The case of organic semiconductors (vol 79, 201205, 2009) [J].

Koerzdoerfer, T. ;

Kuemmel, S. ;

Marom, N. ;

Kronik, L. .

PHYSICAL REVIEW B, 2010, 82 (12)