000229570 001__ 229570
000229570 005__ 20181203024743.0
000229570 0247_ $$2doi$$a10.1038/s41467-017-00069-7
000229570 022__ $$a2041-1723
000229570 02470 $$2ISI$$a000403876000002
000229570 037__ $$aARTICLE
000229570 245__ $$aProbing ultrafast pi pi*/n pi* internal conversion in organic chromophores via K-edge resonant absorption
000229570 260__ $$bNature Publishing Group$$c2017$$aLondon
000229570 269__ $$a2017
000229570 300__ $$a7
000229570 336__ $$aJournal Articles
000229570 520__ $$aMany photoinduced processes including photosynthesis and human vision happen in organic molecules and involve coupled femtosecond dynamics of nuclei and electrons. Organic molecules with heteroatoms often possess an important excited-state relaxation channel from an optically allowed pi pi* to a dark n pi* state. The pi pi*/n pi* internal conversion is difficult to investigate, as most spectroscopic methods are not exclusively sensitive to changes in the excited-state electronic structure. Here, we report achieving the required sensitivity by exploiting the element and site specificity of near-edge soft X-ray absorption spectroscopy. As a hole forms in the n orbital during pi pi*/n pi* internal conversion, the absorption spectrum at the heteroatom K-edge exhibits an additional resonance. We demonstrate the concept using the nucleobase thymine at the oxygen K-edge, and unambiguously show that pi pi*/n pi* internal conversion takes place within (60 +/- 30) fs. High-level-coupled cluster calculations confirm the method's impressive electronic structure sensitivity for excited-state investigations.
000229570 700__ $$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aWolf, T. J. A.
000229570 700__ $$uEcole Polytech Fed Lausanne, Lab Ultrafast Spect, CH-1015 Lausanne, Switzerland$$aMyhre, R. H.
000229570 700__ $$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aCryan, J. P.
000229570 700__ $$uUniv Trieste, Dipartimento Sci Chim Farmaceutiche, Piazzale Europa 1, I-34127 Trieste, Italy$$aCoriani, S.
000229570 700__ $$uUniv Gothenburg, Dept Phys, S-41296 Gothenburg, Sweden$$aSquibb, R. J.
000229570 700__ $$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aBattistoni, A.
000229570 700__ $$uUniv Connecticut, Dept Phys, 2152 Hillside Rd, Storrs, CT 06269 USA$$aBerrah, N.
000229570 700__ $$uSLAC Natl Accelerator Lab, Linac Coherent Light Source, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aBostedt, C.
000229570 700__ $$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aBucksbaum, P.
000229570 700__ $$aCoslovich, G.
000229570 700__ $$aFeifel, R.
000229570 700__ $$uSLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, 2575 Sand Hill Rd,Menlo Pk, Stanford, CA 94025 USA$$aGaffney, K. J.
000229570 700__ $$0246217$$g223637$$uEcole Polytech Fed Lausanne, Lab Ultrafast Spect, CH-1015 Lausanne, Switzerland$$aGrilj, J.
000229570 700__ $$uStanford Univ, Dept Chem, 333 Campus Dr, Stanford, CA 94305 USA$$aMartinez, T. J.
000229570 700__ $$uRIKEN, Laser Technol Lab, Wako, Saitama 3510198, Japan$$aMiyabe, S.
000229570 700__ $$aMoeller, S. P.
000229570 700__ $$uUppsala Univ, Dept Phys & Astron, Box 516, SE-75120 Uppsala, Sweden$$aMucke, M.
000229570 700__ $$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aNatan, A.
000229570 700__ $$aObaid, R.
000229570 700__ $$aOsipov, T.
000229570 700__ $$uElettra Sincrotrone Trieste, 5 AREA Sci Pk, I-34149 BasovizzaTrieste, Italy$$aPlekan, O.
000229570 700__ $$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aWang, S.
000229570 700__ $$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA$$aKoch, H.
000229570 700__ $$aGuehr, M.$$uStanford PULSE Inst, SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA
000229570 773__ $$j8$$tNature Communications$$q29
000229570 909C0 $$xU10862$$0252026$$pLSU
000229570 909CO $$pSB$$particle$$ooai:infoscience.tind.io:229570
000229570 917Z8 $$x122830
000229570 937__ $$aEPFL-ARTICLE-229570
000229570 973__ $$rREVIEWED$$sPUBLISHED$$aEPFL
000229570 980__ $$aARTICLE