000222274 001__ 222274
000222274 005__ 20181203024415.0
000222274 0247_ $$2doi$$a10.1021/acs.jctc.6b00145
000222274 022__ $$a1549-9618
000222274 02470 $$2ISI$$a000381320200046
000222274 037__ $$aARTICLE
000222274 245__ $$aFirst-Principles Photoemission Spectroscopy of DNA and RNA Nucleobases from Koopmans-Compliant Functionals
000222274 260__ $$bAmer Chemical Soc$$c2016$$aWashington
000222274 269__ $$a2016
000222274 300__ $$a11
000222274 336__ $$aJournal Articles
000222274 520__ $$aThe need to interpret ultraviolet photoemission data strongly motivates the refinement of first-principles techniques that are able to accurately predict spectral properties. In this work, we employ Koopmans-compliant functionals, constructed to enforce piecewise linearity in approximate density functionals, to calculate the structural and electronic properties of DNA and RNA nucleobases. Our results show that not only ionization potentials and electron affinities are accurately predicted with mean absolute errors of <0.1 eV, but also that calculated photoemission spectra are in excellent agreement with experimental ultraviolet photo emission spectra. In particular, the role and contribution of different tautomers to the photoemission spectra are highlighted and discussed in detail. The structural properties of nucleobases are also investigated, showing an improved description with respect to local and semilocal density-functional theory. Methodologically, our results further consolidate the role of Koopmans-compliant functionals in providing, through orbital-density-dependent potentials, accurate electronic and spectral properties.
000222274 700__ $$aNguyen, Linh Ngoc
000222274 700__ $$0246485$$g220405$$uEcole Polytech Fed Lausanne, Theory & Simulat Mat THEOS, CH-1015 Lausanne, Switzerland$$aBorghi, Giovanni
000222274 700__ $$aFerretti, Andrea
000222274 700__ $$uEcole Polytech Fed Lausanne, Theory & Simulat Mat THEOS, CH-1015 Lausanne, Switzerland$$aMarzari, Nicola$$g210230$$0246415
000222274 773__ $$j12$$tJournal Of Chemical Theory And Computation$$k8$$q3948-3958
000222274 909C0 $$xU12411$$0252461$$pTHEOS
000222274 909CO $$pSTI$$particle$$ooai:infoscience.tind.io:222274
000222274 917Z8 $$x210230
000222274 937__ $$aEPFL-ARTICLE-222274
000222274 973__ $$rREVIEWED$$sPUBLISHED$$aEPFL
000222274 980__ $$aARTICLE