Molecular orbital tomography from multi-channel harmonic emission in N2

被引:19
作者
Diveki, Z. [1 ]
Guichard, R. [2 ,3 ]
Caillat, J. [2 ,3 ]
Camper, A. [1 ]
Haessler, S. [4 ]
Auguste, T. [1 ]
Ruchon, T. [1 ]
Carre, B. [1 ]
Maquet, A. [2 ]
Taieb, R. [2 ,3 ]
Salieres, P. [1 ]
机构
[1] CEA Saclay, IRAMIS, Serv Photons Atomes & Mol, F-91191 Gif Sur Yvette, France
[2] Univ Paris 06, Lab Chim Phys Mat & Rayonnement, UMR 7614, F-75231 Paris 05, France
[3] LCPMR, CNRS, UMR 7614, Paris, France
[4] Vienna Univ Technol, Photon Inst, A-1040 Vienna, Austria
基金
欧盟第七框架计划;
关键词
High-order harmonic generation; Strong field physics; Molecules; MULTIELECTRON DYNAMICS; GENERATION; IONIZATION; RADIATION; SOFT;
D O I
10.1016/j.chemphys.2012.03.021
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
High-order harmonic generation in aligned molecules can be used as an ultrafast probe of molecular structure and dynamics. By characterizing the emitted signal, one can retrieve information about electronic and nuclear dynamics at the attosecond timescale. In this paper, we discuss the theoretical and experimental aspects of molecular orbital tomography in N-2 and investigate the influence of multi-channel ionization on the orbital imaging. By analyzing the harmonics' spectral phase as a function of the driving laser intensity, we address two distinct cases, which in principle allow the orbital reconstruction. First, the contributions from two molecular orbitals could be disentangled in the real and imaginary parts of the measured dipole, allowing to reconstruct both orbitals. Second, by decreasing the driving laser intensity, the transition from a multi-channel to a single-channel ionization regime is shown. The latter approach paves the way towards the generalization of tomography to more complex systems. (c) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:121 / 129
页数:9
相关论文
共 82 条
[1]  
Ammosov M. V., 1986, Soviet Physics - JETP, V64, P1191
[2]   On the dipole, velocity and acceleration forms in high-order harmonic generation from a single atom or molecule [J].
Baggesen, Jan Conrad ;
Madsen, Lars Bojer .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 2011, 44 (11)
[3]   Probing proton dynamics in molecules on an attosecond time scale [J].
Baker, S ;
Robinson, JS ;
Haworth, CA ;
Teng, H ;
Smith, RA ;
Chirila, CC ;
Lein, M ;
Tisch, JWG ;
Marangos, JP .
SCIENCE, 2006, 312 (5772) :424-427
[4]   Coherent control of attosecond emission from aligned molecules [J].
Boutu, W. ;
Haessler, S. ;
Merdji, H. ;
Breger, P. ;
Waters, G. ;
Stankiewicz, M. ;
Frasinski, L. J. ;
Taieb, R. ;
Caillat, J. ;
Maquet, A. ;
Monchicourt, P. ;
Carre, B. ;
Salieres, P. .
NATURE PHYSICS, 2008, 4 (07) :545-549
[5]   PLASMA PERSPECTIVE ON STRONG-FIELD MULTIPHOTON IONIZATION [J].
CORKUM, PB .
PHYSICAL REVIEW LETTERS, 1993, 71 (13) :1994-1997
[6]   Spectrally resolved multi-channel contributions to the harmonic emission in N2 [J].
Diveki, Z. ;
Camper, A. ;
Haessler, S. ;
Auguste, T. ;
Ruchon, T. ;
Carre, B. ;
Salieres, P. ;
Guichard, R. ;
Caillat, J. ;
Maquet, A. ;
Taieb, R. .
NEW JOURNAL OF PHYSICS, 2012, 14
[7]  
Diveki Z., UNPUB
[8]   Time-resolved atomic inner-shell spectroscopy [J].
Drescher, M ;
Hentschel, M ;
Kienberger, R ;
Uiberacker, M ;
Yakovlev, V ;
Scrinzi, A ;
Westerwalbesloh, T ;
Kleineberg, U ;
Heinzmann, U ;
Krausz, F .
NATURE, 2002, 419 (6909) :803-807
[9]   Relation of high harmonic spectra to electronic structure in N2 [J].
Farrell, J. P. ;
McFarland, B. K. ;
Guehr, M. ;
Bucksbaum, P. H. .
CHEMICAL PHYSICS, 2009, 366 (1-3) :15-21
[10]   Strong Field Ionization to Multiple Electronic States in Water [J].
Farrell, Joseph P. ;
Petretti, Simon ;
Foerster, Johann ;
McFarland, Brian K. ;
Spector, Limor S. ;
Vanne, Yulian V. ;
Decleva, Piero ;
Bucksbaum, Philip H. ;
Saenz, Alejandro ;
Guehr, Markus .
PHYSICAL REVIEW LETTERS, 2011, 107 (08)