Noncollinear wave mixing of attosecond XUV and few-cycle optical laser pulses in gas-phase atoms: Toward multidimensional spectroscopy involving XUV excitations

被引:53
作者
Cao, Wei [1 ,2 ,3 ]
Warrick, Erika R. [1 ,2 ]
Fidler, Ashley [1 ,2 ]
Neumark, Daniel M. [1 ,2 ]
Leone, Stephen R. [1 ,2 ,3 ]
机构
[1] Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA
[2] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[3] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA
关键词
RESOLVED 4-WAVE-MIXING SPECTROSCOPY; HIGH HARMONIC-GENERATION; RAMAN-SCATTERING; IODINE VAPOR; FEMTOSECOND; DYNAMICS; STATES; MOLECULES;
D O I
10.1103/PhysRevA.94.053846
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
Ultrafast nonlinear spectroscopy, which records transient wave-mixing signals in a medium, is a powerful tool to access microscopic information using light sources in the radio-frequency and optical regimes. The extension of this technique towards the extreme ultraviolet (XUV) or even x-ray regimes holds the promise to uncover rich structural or dynamical information with even higher spatial or temporal resolution. Here, we demonstrate noncollinear wave mixing between weak XUV attosecond pulses and a strong near-infrared (NIR) few-cycle laser pulse in gas phase atoms (one photon of XUV and two photons of NIR). In the noncollinear geometry the attosecond and either one or two NIR pulses interact with argon atoms. Nonlinear XUV signals are generated in a spatially resolved fashion as required by phase matching. Different transition pathways can be identified from these background-free nonlinear signals according to the specific phase-matching conditions. Time-resolved measurements of the spatially gated XUV signals reveal electronic coherences of Rydberg wave packets prepared by a single XUV photon or XUV-NIR two-photon excitation, depending on the applied pulse sequences. These measurements open possible applications of tabletop multidimensional spectroscopy to the study of dynamics associated with valence or core excitation with XUV photons.
引用
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页数:7
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