Attosecond Pump-Probe Spectroscopy of Charge Dynamics in Tryptophan

被引:78
|
作者
Lara-Astias, Manuel [1 ]
Galli, Mara [2 ,3 ]
Trabattoni, Andrea [4 ]
Palacios, Alicia [1 ]
Ayuso, David [1 ]
Frassetto, Fabio [5 ]
Poletto, Luca [5 ]
De Camillis, Simone [6 ]
Greenwood, Jason [6 ]
Decleva, Piero [7 ]
Tavernelli, Ivano [8 ]
Calegari, Francesca [2 ,4 ,9 ]
Nisoli, Mauro [2 ,3 ]
Martin, Fernando [1 ,10 ,11 ]
机构
[1] Univ Autonoma Madrid, Dept Quim, Modulo 13, E-28049 Madrid, Spain
[2] CNR, IFN, Inst Photon & Nanotechnol, I-20133 Milan, Italy
[3] Politecn Milan, Dipartimento Fis, I-20133 Milan, Italy
[4] DESY, Ctr Free Electron Laser Sci CFEL, D-22607 Hamburg, Germany
[5] CNR, IFN, Inst Photon & Nanotechnol, I-35131 Padua, Italy
[6] Queens Univ, Sch Maths & Phys, Belfast BT7 1NN, Antrim, North Ireland
[7] Univ Trieste, Dipartimento Sci Chim & Farmaceut, I-34127 Trieste, Italy
[8] Zurich Res Lab, IBM Res GmbH, CH-8803 Ruschlikon, Switzerland
[9] Hamburg Univ, Dept Phys, D-20355 Hamburg, Germany
[10] Inst Madrileno Estudios Avanzados Nanociencia, Madrid 28049, Spain
[11] Univ Autonoma Madrid, Condensed Matter Phys Ctr IFIMAC, E-28049 Madrid, Spain
来源
基金
欧洲研究理事会; 英国工程与自然科学研究理事会;
关键词
DENSITY-FUNCTIONAL THEORY; REAL-TIME OBSERVATION; MOLECULAR PHOTOIONIZATION; ELECTRON CORRELATION; MIGRATION; PULSES; PSEUDOPOTENTIALS; PROTEINS; GLYCINE;
D O I
10.1021/acs.jpclett.8b01786
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Attosecond pump-probe experiments performed in small molecules have allowed tracking charge dynamics in the natural time scale of electron motion. That this is also possible in biologically relevant molecules is still a matter of debate, because the large number of available nuclear degrees of freedom might destroy the coherent charge dynamics induced by the attosecond pulse. Here we investigate extreme ultraviolet-induced charge dynamics in the amino acid tryptophan. We find that, although nuclear motion and nonadiabatic effects introduce some decoherence in the moving electron wave packet, these do not significantly modify the coherence induced by the attosecond pulse during the early stages of the dynamics, at least for molecules in their equilibrium geometry. Our conclusions are based on elaborate theoretical calculations and the experimental observation of sub-4 fs dynamics, which can only be reasonably assigned to electronic motion. Hence, attosecond pump-probe spectroscopy appears as a promising approach to induce and image charge dynamics in complex molecules.
引用
收藏
页码:4570 / 4577
页数:15
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