Photoelectron properties of DNA and RNA bases from many-body perturbation theory

被引:30
作者
Qian, Xiaofeng [1 ]
Umari, Paolo [2 ]
Marzari, Nicola [1 ,3 ]
机构
[1] MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA
[2] CNR IOM Democritos, Theory Elettra Grp, Basovizza Trieste, Italy
[3] Univ Oxford, Dept Mat, Oxford OX1 3PH, England
来源
PHYSICAL REVIEW B | 2011年 / 84卷 / 07期
关键词
SPACE-TIME METHOD; GREENS-FUNCTION; ELECTRON; SPECTROSCOPY; MOLECULES; TRANSPORT; ENERGIES; SPECTRA; THYMINE; SYSTEMS;
D O I
10.1103/PhysRevB.84.075103
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
The photoelectron properties of DNA and RNA bases are studied using many-body perturbation theory within the GW approximation, together with a recently developed Lanczos-chain approach. Calculated vertical ionization potentials, electron affinities, and total density of states are in good agreement with experimental values and photoemission spectra. The convergence benchmark demonstrates the importance of using an optimal polarizability basis in the GW calculations. A detailed analysis of the role of exchange and correlation in both many-body and density-functional theory calculations shows that while self-energy corrections are strongly orbital-dependent, they nevertheless remain almost constant for states that share the same bonding character. Finally, we report on the inverse lifetimes ofDNAandRNAbases that are found to depend linearly on quasiparticle energies for all deep valence states. In general, our G(0)W(0)-Lanczos approach provides an efficient yet accurate and fully converged description of quasiparticle properties of five DNA and RNA bases.
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页数:8
相关论文
共 42 条
[1]   First-principles GW calculations for fullerenes, porphyrins, phtalocyanine, and other molecules of interest for organic photovoltaic applications [J].
Blase, X. ;
Attaccalite, C. ;
Olevano, V. .
PHYSICAL REVIEW B, 2011, 83 (11)
[2]   Electronic Structure and Spectroscopy of Nucleic Acid Bases: Ionization Energies, Ionization-Induced Structural Changes, and Photoelectron Spectra [J].
Bravaya, Ksenia B. ;
Kostko, Oleg ;
Dolgikh, Stanislav ;
Landau, Arie ;
Ahmed, Musahid ;
Krylov, Anna I. .
JOURNAL OF PHYSICAL CHEMISTRY A, 2010, 114 (46) :12305-12317
[3]   Inelastic lifetimes of hot electrons in real metals [J].
Campillo, I ;
Pitarke, JM ;
Rubio, A ;
Zarate, E ;
Echenique, PM .
PHYSICAL REVIEW LETTERS, 1999, 83 (11) :2230-2233
[4]   Ionization spectroscopy of a DNA base: Vacuum-ultraviolet mass-analyzed threshold ionization spectroscopy of jet-cooled thymine [J].
Choi, KW ;
Lee, JH ;
Kim, SK .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (45) :15674-15675
[5]   STRUCTURE AND RELATIVE STABILITY OF DEOXYRIBOSE RADICALS IN A MODEL DNA BACKBONE - AB-INITIO MOLECULAR-ORBITAL CALCULATIONS [J].
COLSON, AO ;
SEVILLA, MD .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (11) :3867-3874
[6]   Koopmans' condition for density-functional theory [J].
Dabo, Ismaila ;
Ferretti, Andrea ;
Poilvert, Nicolas ;
Li, Yanli ;
Marzari, Nicola ;
Cococcioni, Matteo .
PHYSICAL REVIEW B, 2010, 82 (11)
[7]   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)
[8]   PHOTOELECTRON-SPECTROSCOPY OF SOME BIOLOGICAL MOLECULES [J].
DOUGHERTY, D ;
YOUNATHAN, ES ;
VOLL, R ;
ABDULNUR, S ;
MCGLYNN, SP .
JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, 1978, 13 (06) :379-393
[9]   First-principles GW calculations for DNA and RNA nucleobases [J].
Faber, Carina ;
Attaccalite, Claudio ;
Olevano, V. ;
Runge, E. ;
Blase, X. .
PHYSICAL REVIEW B, 2011, 83 (11)
[10]   QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials [J].
Giannozzi, Paolo ;
Baroni, Stefano ;
Bonini, Nicola ;
Calandra, Matteo ;
Car, Roberto ;
Cavazzoni, Carlo ;
Ceresoli, Davide ;
Chiarotti, Guido L. ;
Cococcioni, Matteo ;
Dabo, Ismaila ;
Dal Corso, Andrea ;
de Gironcoli, Stefano ;
Fabris, Stefano ;
Fratesi, Guido ;
Gebauer, Ralph ;
Gerstmann, Uwe ;
Gougoussis, Christos ;
Kokalj, Anton ;
Lazzeri, Michele ;
Martin-Samos, Layla ;
Marzari, Nicola ;
Mauri, Francesco ;
Mazzarello, Riccardo ;
Paolini, Stefano ;
Pasquarello, Alfredo ;
Paulatto, Lorenzo ;
Sbraccia, Carlo ;
Scandolo, Sandro ;
Sclauzero, Gabriele ;
Seitsonen, Ari P. ;
Smogunov, Alexander ;
Umari, Paolo ;
Wentzcovitch, Renata M. .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2009, 21 (39)