Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule

被引：39

作者：

Barillot, T. ^{[1
]}

Alexander, O. ^{[1
]}

Cooper, B. ^{[1
,2
]}

Driver, T. ^{[1
,3
,4
]}

Garratt, D. ^{[1
]}

Li, S. ^{[5
]}

Al Haddad, A. ^{[6
,7
]}

Sanchez-Gonzalez, A. ^{[1
]}

Agaker, M. ^{[8
,9
]}

Arrell, C. ^{[7
]}

Bearpark, M. J. ^{[10
]}

Berrah, N. ^{[11
]}

Bostedt, C. ^{[6
,7
,12
]}

Bozek, J. ^{[13
]}

Brahms, C. ^{[1
]}

Bucksbaum, P. H. ^{[3
]}

Clark, A. ^{[14
]}

Doumy, G. ^{[6
]}

Feifel, R. ^{[15
]}

Frasinski, L. J. ^{[1
]}

Jarosch, S. ^{[1
]}

Johnson, A. S. ^{[1
]}

Kjellsson, L. ^{[8
]}

Kumagai, Y. ^{[6
]}

Larsen, E. W. ^{[1
]}

Matia-Hernando, P. ^{[1
]}

Robb, M. ^{[10
]}

Rubensson, J-E ^{[8
]}

Ruberti, M. ^{[1
]}

Sathe, C. ^{[9
]}

Squibb, R. J. ^{[15
]}

Tan, A. ^{[1
]}

Tisch, J. W. G. ^{[1
]}

Vacher, M. ^{[10
,17
]}

Walke, D. J. ^{[1
]}

Wolf, T. J. A. ^{[3
]}

Wood, D. ^{[1
]}

Zhaunerchyk, V ^{[15
]}

Walter, P. ^{[4
]}

Osipov, T. ^{[4
]}

Marinelli, A. ^{[5
]}

Maxwell, T. J. ^{[5
]}

Coffee, R. ^{[4
]}

Lutman, A. A. ^{[5
]}

Averbukh, V ^{[1
]}

Ueda, K. ^{[18
,19
]}

Cryan, J. P. ^{[3
,4
]}

Marangos, J. P. ^{[1
]}

Kolorenc, P. ^{[16
]}

机构：

[1] Imperial Coll London, Blackett Lab, Quantum Opt & Laser Sci Grp, London SW7 2BW, England

[2] UCL, Dept Phys & Astron, Atom Mol Opt & Positron Phys Grp, Gower St, London WC1E 6BT, England

[3] SLAC Natl Accelerator Lab, Stanford PULSE Inst, Menlo Pk, CA 94025 USA

[4] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA

[5] SLAC Natl Accelerator Lab, Accelerator Directorate, Menlo Pk, CA 94025 USA

[6] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA

[7] Paul Scherrer Inst, CH-5232 Villigen, Switzerland

[8] Uppsala Univ, Dept Phys & Astron, Box 516, S-75120 Uppsala, Sweden

[9] Lund Univ, MAX IV Lab, Box 118, SE-22100 Lund, Sweden

[10] Imperial Coll London, Dept Chem, Mol Sci Res Hub, London W12 0BZ, England

[11] Univ Connecticut, Dept Phys, Storrs, CT 06268 USA

[12] Ecole Polytech Fed Lausanne EPFL, LUXS Lab Ultrafast Xray Sci, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland

[13] Orme Merisiers, Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France

[14] Ecole Polytech Fed Lausanne, Lab Mol Nanodynam, CH-1015 Lausanne, Switzerland

[15] Univ Gothenburg, Dept Phys, Origovagen 6B, S-41258 Gothenburg, Sweden

[16] Charles Univ Prague, Fac Math & Phys, Inst Theoret Phys, V Holesovickach 2, Prague 18000, Czech Republic

[17] Univ Nantes, CNRS, CEISAM UMR 6230, F-44000 Nantes, France

[18] Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Sendai, Miyagi 9808577, Japan

[19] Tohoku Univ, Dept Chem, Aoba Ku, 6-3 Aramaki Aza Aoba, Sendai, Miyagi 9808578, Japan

来源：

PHYSICAL REVIEW X | 2021年 / 11卷 / 03期

基金：

英国工程与自然科学研究理事会; 瑞典研究理事会;

关键词：

SURFACE-HOPPING PROGRAM; CHARGE MIGRATION; NEWTON-X; ATTOSECOND; SPECTROSCOPY; FEMTOSECOND;

D O I：

10.1103/PhysRevX.11.031048

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

The possibility of suddenly ionized molecules undergoing extremely fast electron hole (or hole) dynamics prior to significant structural change was first recognized more than 20 years ago and termed charge migration. The accurate probing of ultrafast electron hole dynamics requires measurements that have both sufficient temporal resolution and can detect the localization of a specific hole within the molecule. We report an investigation of the dynamics of inner valence hole states in isopropanol where we use an x-ray pump-x-ray probe experiment, with site and state-specific probing of a transient hole state localized near the oxygen atom in the molecule, together with an ab initio theoretical treatment. We record the signature of transient hole dynamics and make the first tentative observation of dynamics driven by frustrated Auger-Meitner transitions. We verify that the effective hole lifetime is consistent with our theoretical prediction. This state-specific measurement paves the way to widespread application for observations of transient hole dynamics localized in space and time in molecules and thus to charge transfer phenomena that are fundamental in chemical and material physics.

引用

页数：15

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