ALBERT

Description: Electron solvation dynamics in photoexcited anion clusters of I-(D2O)n=4-6 and I-(H2O)4-6 were probed by using femtosecond photoelectron spectroscopy (FPES). An ultrafast pump pulse excited the anion to the cluster analog of the charge-transfer-to-solvent state seen for I- in aqueous solution. Evolution of this state was monitored by time-resolved photoelectron spectroscopy using an ultrafast probe pulse. The excited n = 4 clusters showed simple population decay, but in the n = 5 and 6 clusters the solvent molecules rearranged to stabilize and localize the excess electron, showing characteristics associated with electron solvation dynamics in bulk water. Comparison of the FPES of I-(D2O)n with I-(H2O)n indicates more rapid solvation in the H2O clusters.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Lehr -- Zanni -- Frischkorn -- Weinkauf -- Neumark -- New York, N.Y. -- Science. 1999 Apr 23;284(5414):635-8.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Berkeley, CA 94720, USA and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/10213684" target="_blank"〉PubMed〈/a〉

Description: The degree of electronic and nuclear coupling in the Cl + H2 reaction has become a vexing problem in chemical dynamics. We report slow electron velocity-map imaging (SEVI) spectra of ClH2- and ClD2-. These spectra probe the reactant valley of the neutral reaction potential energy surface, where nonadiabatic transitions responsible for reactivity of the Cl excited spin-orbit state with H2 would occur. The SEVI spectra reveal progressions in low-frequency Cl.H2 bending and stretching modes, and are compared to simulations with and without nonadiabatic couplings between the Cl spin-orbit states. Although nonadiabatic effects are small, their inclusion improves agreement with experiment. This comparison validates the theoretical treatment, especially of the nonadiabatic effects, in this critical region of the Cl + H2 reaction, and suggests strongly that these effects are minor.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Garand, Etienne -- Zhou, Jia -- Manolopoulos, David E -- Alexander, Millard H -- Neumark, Daniel M -- New York, N.Y. -- Science. 2008 Jan 4;319(5859):72-5. doi: 10.1126/science.1150602.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Berkeley, CA 94720, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/18174436" target="_blank"〉PubMed〈/a〉

Description: The conclusion by Turi et al. (Reports, 5 August 2005, p. 914) that all experimental spectral and energetic data on water-cluster anions point toward surface-bound electrons is overstated. Comparison of experimental vertical detachment energies with their calculated values for (H2O)n- clusters with surface-bound and internalized electrons supports previous arguments that both types of clusters exist.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Verlet, J R R -- Bragg, A E -- Kammrath, A -- Cheshnovsky, O -- Neumark, D M -- New York, N.Y. -- Science. 2005 Dec 16;310(5755):1769; author reply 1769.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Berkeley, CA 94720, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/16357246" target="_blank"〉PubMed〈/a〉

Description: The electronic relaxation dynamics of size-selected (H2O)n-/(D2O)n[25 〈/= n 〈/= 50] clusters have been studied with time-resolved photoelectron imaging. The excess electron (ec-) was excited through the ec-(p)〈--ec-(s) transition with an ultrafast laser pulse, with subsequent evolution of the excited state monitored with photodetachment and photoelectron imaging. All clusters exhibited p-state population decay with concomitant s-state repopulation (internal conversion) on time scales ranging from 180 to 130 femtoseconds for (H2O)n- and 400 to 225 femtoseconds for (D2O)n-; the lifetimes decrease with increasing cluster sizes. Our results support the "nonadiabatic relaxation" mechanism for the bulk hydrated electron (eaq-), which invokes a 50-femtosecond eaq-(p)--〉eaq-(s(dagger)) internal conversion lifetime.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Bragg, A E -- Verlet, J R R -- Kammrath, A -- Cheshnovsky, O -- Neumark, D M -- New York, N.Y. -- Science. 2004 Oct 22;306(5696):669-71. Epub 2004 Sep 16.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Berkeley, CA 94720, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/15375222" target="_blank"〉PubMed〈/a〉

Description: Anionic water clusters have long been studied to infer properties of the bulk hydrated electron. We used photoelectron imaging to characterize a class of (H2O)n- and (D2O)n- cluster anions (n 〈/= 200 molecules) with vertical binding energies that are significantly lower than those previously recorded. The data are consistent with a structure in which the excess electron is bound to the surface of the cluster. This result implies that the excess electron in previously observed water-cluster anions, with higher vertical binding energies, was internally solvated. Thus, the properties of those clusters could be extrapolated to those of the bulk hydrated electron.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Verlet, J R R -- Bragg, A E -- Kammrath, A -- Cheshnovsky, O -- Neumark, D M -- New York, N.Y. -- Science. 2005 Jan 7;307(5706):93-6. Epub 2004 Dec 16.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Berkeley, CA 94720, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/15604360" target="_blank"〉PubMed〈/a〉

Description: The protonated water dimer is a prototypical system for the study of proton transfer in aqueous solution. We report infrared photodissociation spectra of cooled H+(H2O)2 [and D+(D2O2] ions, measured between 620 and 1900 wave numbers (cm-1). The experiment directly probes the shared proton region of the potential energy surface and reveals three strong bands below 1600 cm-1 and one at 1740 cm-1 (for H5O2+). From a comparison to multidimensional quantum calculations, the three lower energy bands were assigned to stretching and bending fundamentals involving the O...H+...O moiety, and the highest energy band was assigned to a terminal water bend. These results highlight the importance of intermode coupling in shared proton systems.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Asmis, Knut R -- Pivonka, Nicholas L -- Santambrogio, Gabriele -- Brummer, Mathias -- Kaposta, Cristina -- Neumark, Daniel M -- Woste, Ludger -- New York, N.Y. -- Science. 2003 Feb 28;299(5611):1375-7. Epub 2003 Feb 6.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Institut fur Experimentalphysik, Freie Universitat Berlin, Arnimallee 14, D 14195 Berlin, Germany. asmis@physik.fu-berlin.de〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/12574498" target="_blank"〉PubMed〈/a〉

Description: The transition state region of the F + H(2) reaction has been studied by photoelectron spectroscopy of FH(2)(-). New para and normal FH(2)(-)photoelectron spectra have been measured in refined experiments and are compared here with exact three-dimensional quantum reactive scattering simulations that use an accurate new ab initio potential energy surface for F + H(2). The detailed agreement that is obtained between this fully ab initio theory and experiment is unprecedented for the F + H(2) reaction and suggests that the transition state region of the F + H(2) potential energy surface has finally been understood quantitatively.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Manolopoulos, D E -- Stark, K -- Werner, H J -- Arnold, D W -- Bradforth, S E -- Neumark, D M -- New York, N.Y. -- Science. 1993 Dec 17;262(5141):1852-5.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/17829631" target="_blank"〉PubMed〈/a〉

Description: The relaxation dynamics of the photoexcited hydrated electron have been subject to conflicting interpretations. Here, we report time-resolved photoelectron spectra of hydrated electrons in a liquid microjet with the aim of clarifying ambiguities from previous experiments. A sequence of three ultrashort laser pulses (~100 femtosecond duration) successively created hydrated electrons by charge-transfer-to-solvent excitation of dissolved anions, electronically excited these electrons via the s--〉p transition, and then ejected them into vacuum. Two distinct transient signals were observed. One was assigned to the initially excited p-state with a lifetime of ~75 femtoseconds, and the other, with a lifetime of ~400 femtoseconds, was attributed to s-state electrons just after internal conversion in a nonequilibrated solvent environment. These assignments support the nonadiabatic relaxation model.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Elkins, Madeline H -- Williams, Holly L -- Shreve, Alexander T -- Neumark, Daniel M -- New York, N.Y. -- Science. 2013 Dec 20;342(6165):1496-9. doi: 10.1126/science.1246291.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Berkeley, CA 94720, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/24357314" target="_blank"〉PubMed〈/a〉

Description: Helium nanodroplets are considered ideal model systems to explore quantum hydrodynamics in self-contained, isolated superfluids. However, exploring the dynamic properties of individual droplets is experimentally challenging. In this work, we used single-shot femtosecond x-ray coherent diffractive imaging to investigate the rotation of single, isolated superfluid helium-4 droplets containing ~10(8) to 10(11) atoms. The formation of quantum vortex lattices inside the droplets is confirmed by observing characteristic Bragg patterns from xenon clusters trapped in the vortex cores. The vortex densities are up to five orders of magnitude larger than those observed in bulk liquid helium. The droplets exhibit large centrifugal deformations but retain axially symmetric shapes at angular velocities well beyond the stability range of viscous classical droplets.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Gomez, Luis F -- Ferguson, Ken R -- Cryan, James P -- Bacellar, Camila -- Tanyag, Rico Mayro P -- Jones, Curtis -- Schorb, Sebastian -- Anielski, Denis -- Belkacem, Ali -- Bernando, Charles -- Boll, Rebecca -- Bozek, John -- Carron, Sebastian -- Chen, Gang -- Delmas, Tjark -- Englert, Lars -- Epp, Sascha W -- Erk, Benjamin -- Foucar, Lutz -- Hartmann, Robert -- Hexemer, Alexander -- Huth, Martin -- Kwok, Justin -- Leone, Stephen R -- Ma, Jonathan H S -- Maia, Filipe R N C -- Malmerberg, Erik -- Marchesini, Stefano -- Neumark, Daniel M -- Poon, Billy -- Prell, James -- Rolles, Daniel -- Rudek, Benedikt -- Rudenko, Artem -- Seifrid, Martin -- Siefermann, Katrin R -- Sturm, Felix P -- Swiggers, Michele -- Ullrich, Joachim -- Weise, Fabian -- Zwart, Petrus -- Bostedt, Christoph -- Gessner, Oliver -- Vilesov, Andrey F -- New York, N.Y. -- Science. 2014 Aug 22;345(6199):906-9. doi: 10.1126/science.1252395.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of Southern California (USC), Los Angeles, CA 90089, USA. ; Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. ; Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA 94720, USA. ; Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA 94720, USA. Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA. ; Max-Planck-Institut fur Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany. Max Planck Advanced Study Group at the Center for Free-Electron Laser Science (CFEL), Notkestrasse 85, 22607 Hamburg, Germany. ; Department of Physics and Astronomy, USC, Los Angeles, CA 90089, USA. ; Max-Planck-Institut fur Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany. Max Planck Advanced Study Group at the Center for Free-Electron Laser Science (CFEL), Notkestrasse 85, 22607 Hamburg, Germany. Deutsches Elektronen-Synchrotron (DESY), Notkestrasse 85, 22607 Hamburg, Germany. ; Advanced Light Source, LBNL, Berkeley, CA 94720, USA. ; CFEL, DESY, Notkestrasse 85, 22607 Hamburg, Germany. ; Max-Planck-Institut fur Extraterrestrische Physik, Giessenbachstrasse, 85741 Garching, Germany. ; Max Planck Advanced Study Group at the Center for Free-Electron Laser Science (CFEL), Notkestrasse 85, 22607 Hamburg, Germany. Max-Planck-Institut fur Medizinische Forschung, Jahnstrasse 29, 69120 Heidelberg, Germany. ; PNSensor GmbH, Otto-Hahn-Ring 6, 81739 Munchen, Germany. ; Mork Family Department of Chemical Engineering and Materials Science, USC, Los Angeles, CA 90089, USA. ; Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA 94720, USA. Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA. Department of Physics, University of California Berkeley, Berkeley, CA 94720, USA. ; Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA 94720, USA. Department of Physics, The Chinese University of Hong Kong, Hong Kong, China. ; National Energy Research Scientific Computing Center, LBNL, Berkeley, CA 94720, USA. ; Physical Biosciences Division, LBNL, Berkeley, CA 94720, USA. Department of Plant and Microbial Biology, University of Calfornia Berkeley, Berkeley, CA 94720, USA. ; Advanced Light Source, LBNL, Berkeley, CA 94720, USA. Department of Physics, University of California Davis, Davis, CA 95616, USA. ; Physical Biosciences Division, LBNL, Berkeley, CA 94720, USA. ; Department of Chemistry, University of California Berkeley, Berkeley, CA 94720, USA. ; Max Planck Advanced Study Group at the Center for Free-Electron Laser Science (CFEL), Notkestrasse 85, 22607 Hamburg, Germany. Deutsches Elektronen-Synchrotron (DESY), Notkestrasse 85, 22607 Hamburg, Germany. Max-Planck-Institut fur Medizinische Forschung, Jahnstrasse 29, 69120 Heidelberg, Germany. ; Max-Planck-Institut fur Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany. Max Planck Advanced Study Group at the Center for Free-Electron Laser Science (CFEL), Notkestrasse 85, 22607 Hamburg, Germany. James R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA. ; Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. PULSE Institute, Stanford University and SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. bostedt@slac.stanford.edu ogessner@lbl.gov vilesov@usc.edu. ; Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA 94720, USA. bostedt@slac.stanford.edu ogessner@lbl.gov vilesov@usc.edu. ; Department of Chemistry, University of Southern California (USC), Los Angeles, CA 90089, USA. Department of Physics and Astronomy, USC, Los Angeles, CA 90089, USA. bostedt@slac.stanford.edu ogessner@lbl.gov vilesov@usc.edu.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/25146284" target="_blank"〉PubMed〈/a〉

Description: Electron transfer from valence to conduction band states in semiconductors is the basis of modern electronics. Here, attosecond extreme ultraviolet (XUV) spectroscopy is used to resolve this process in silicon in real time. Electrons injected into the conduction band by few-cycle laser pulses alter the silicon XUV absorption spectrum in sharp steps synchronized with the laser electric field oscillations. The observed ~450-attosecond step rise time provides an upper limit for the carrier-induced band-gap reduction and the electron-electron scattering time in the conduction band. This electronic response is separated from the subsequent band-gap modifications due to lattice motion, which occurs on a time scale of 60 +/- 10 femtoseconds, characteristic of the fastest optical phonon. Quantum dynamical simulations interpret the carrier injection step as light-field-induced electron tunneling.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Schultze, Martin -- Ramasesha, Krupa -- Pemmaraju, C D -- Sato, S A -- Whitmore, D -- Gandman, A -- Prell, James S -- Borja, L J -- Prendergast, D -- Yabana, K -- Neumark, Daniel M -- Leone, Stephen R -- New York, N.Y. -- Science. 2014 Dec 12;346(6215):1348-52. doi: 10.1126/science.1260311.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Berkeley, CA 94720, USA. Fakultat fur Physik, Ludwig-Maximilians-Universitat, Am Coulombwall 1, D-85748 Garching, Germany. martin.schultze@mpq.mpg.de dneumark@berkeley.edu srl@berkeley.edu. ; Department of Chemistry, University of California, Berkeley, CA 94720, USA. ; The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. ; Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8571, Japan. ; Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8571, Japan. Center for Computational Sciences, University of Tsukuba, Tsukuba 305-8577, Japan. ; Department of Chemistry, University of California, Berkeley, CA 94720, USA. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. martin.schultze@mpq.mpg.de dneumark@berkeley.edu srl@berkeley.edu. ; Department of Chemistry, University of California, Berkeley, CA 94720, USA. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. Department of Physics, University of California, Berkeley, CA 94720, USA. martin.schultze@mpq.mpg.de dneumark@berkeley.edu srl@berkeley.edu.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/25504716" target="_blank"〉PubMed〈/a〉