Ultrafast relaxation of photoexcited superfluid He nanodroplets

被引：31

作者：

Mudrich, M. ^{[1
]}

LaForge, A. C. ^{[2
,3
]}

Ciavardini, A. ^{[4
,18
]}

O'Keeffe, P. ^{[4
]}

Callegari, C. ^{[5
]}

Coreno, M. ^{[4
]}

Demidovich, A. ^{[5
]}

Devetta, M. ^{[6
,19
]}

Di Fraia, M. ^{[5
]}

Drabbels, M. ^{[7
]}

Finetti, P. ^{[5
]}

Gessner, O. ^{[8
]}

Grazioli, C. ^{[20
]}

Hernando, A. ^{[9
,10
]}

Neumark, D. M. ^{[8
,11
]}

Ovcharenko, Y. ^{[12
,21
]}

Piseri, P. ^{[6
]}

Plekan, O. ^{[5
]}

Prince, K. C. ^{[5
]}

Richter, R. ^{[5
]}

Ziemkiewicz, M. P. ^{[8
,11
]}

Moeller, T. ^{[12
]}

Eloranta, J. ^{[13
]}

Pi, M. ^{[14
,15
]}

Barranco, M. ^{[14
,15
,16
,17
]}

Stienkemeier, F. ^{[2
]}

机构：

[1] Aarhus Univ, Dept Phys & Astron, DK-8000 Aarhus C, Denmark

[2] Univ Freiburg, Inst Phys, D-79104 Freiburg, Germany

[3] Univ Connecticut, Dept Phys, Storrs, CT 06269 USA

[4] CNR ISM, Area Ric Roma 1, I-00015 Monterotondo Scale, Italy

[5] Elettra Sincrotrone Trieste SCpA, I-34149 Trieste, Italy

[6] Univ Milan, Dipartimento Fis, I-20133 Milan, Italy

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

[8] Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA

[9] EPFL Innovat Pk, Kido Dynam, Bat C, CH-1015 Lausanne, Switzerland

[10] IFISC CSIC UIB, Inst Fis Interdisciplinar & Sistemas Complejos, Campus Univ Illes Balears, Palma De Mallorca 07122, Spain

[11] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[12] TU Berlin, Inst Opt & Atomare Phys, D-10623 Berlin, Germany

[13] Calif State Univ Northridge, Dept Chem & Biochem, Northridge, CA 91330 USA

[14] Univ Barcelona, Fac Fis, Dept FQA, E-08028 Barcelona, Spain

[15] Univ Barcelona, IN2, E-08028 Barcelona, Spain

[16] CNRS, UMR 5589, IRSAMC, Lab Collis Agregats Reactivite, F-31062 Toulouse 09, France

[17] Univ Paul Sabatier Toulouse 3, F-31062 Toulouse 09, France

[18] Cer ERIC Basovizza, I-34149 Trieste, Italy

[19] CNR, IFN, I-20133 Milan, Italy

[20] CNR IOM, Ist Officina Mat, Area Sci Pk Basovizza, I-34149 Trieste, Italy

[21] European XFEL, D-22869 Schenefeld, Germany

来源：

NATURE COMMUNICATIONS | 2020年 / 11卷 / 01期

基金：

瑞士国家科学基金会; 美国国家科学基金会;

关键词：

LIQUID-HELIUM; EXCITED-STATES; DYNAMICS; ATOMS; CLUSTERS; PHOTOELECTRON; CONFIGURATION; EXCITATIONS; DESORPTION; MOLECULES;

D O I：

10.1038/s41467-019-13681-6

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

The relaxation of photoexcited nanosystems is a fundamental process of light-matter interaction. Depending on the couplings of the internal degrees of freedom, relaxation can be ultrafast, converting electronic energy in a few fs, or slow, if the energy is trapped in a metastable state that decouples from its environment. Here, we study helium nanodroplets excited resonantly by femtosecond extreme-ultraviolet (XUV) pulses from a seeded free-electron laser. Despite their superfluid nature, we find that helium nanodroplets in the lowest electronically excited states undergo ultrafast relaxation. By comparing experimental photoelectron spectra with time-dependent density functional theory simulations, we unravel the full relaxation pathway: Following an ultrafast interband transition, a void nanometer-sized bubble forms around the localized excitation (He*) within 1 ps. Subsequently, the bubble collapses and releases metastable He* at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses.

引用

页数：7

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