Chapter 1
Molecular Movies from Molecular Frame
Photoelectron Angular Distribution (MF-PAD)
Measurements
Arnaud Rouzée, Ymkje Huismans, Freek Kelkensberg, Aneta Smolkowska,
Julia H. Jungmann, Arjan Gijsbertsen, Wing Kiu Siu, Georg Gademann,
Axel Hundertmark, Per Johnsson, and Marc J.J. Vrakking
Abstract We discuss recent and on-going experiments, where molecular frame
photoelectron angular distributions (MFPADs) of high kinetic energy photoelectrons are measured in order to determine the time evolution of molecular structures
in the course of a photochemical event. These experiments include, on the one hand,
measurements where single XUV/X-ray photons, obtained from a free electron laser
(FEL) or by means of high-harmonic generation (HHG), are used to eject a high energy photoelectron, and, on the other hand, measurements where a large number of
mid-infrared photons are absorbed in the course of strong-field ionization. In the
former case, first results indicate a manifestation of the both the electronic orbital
and the molecular structure in the angle-resolved photoelectron distributions, while
in the latter case novel holographic structures are measured that suggest that both the
molecular structure and ultrafast electronic rearrangement processes can be studied
with a time-resolution that reaches down into the attosecond and few-femtosecond
domain.
1.1 Introduction
Much of our knowledge about matter on the nano-scale is based on studies of the
interaction of matter with light. Consequently, the invention of lasers in the infrared,
visible and ultra-violet parts of the wavelength spectrum has greatly benefitted our
understanding of chemical and physical processes. Using lasers, very insightful exA. Rouzée · A. Hundertmark · M.J.J. Vrakking (B)
Max-Born Institut, Max Born Straße 2A, 12489 Berlin, Germany
e-mail: marc.vrakking@mbi-berlin.de
A. Rouzée · Y. Huismans · F. Kelkensberg · A. Smolkowska · J.H. Jungmann · A. Gijsbertsen ·
W.K. Siu · G. Gademann · A. Hundertmark · M.J.J. Vrakking
FOM Institute AMOLF, Science Park 104, 1098 XG Amsterdam, The Netherlands
P. Johnsson
Department of Physics, Lund University, P.O. Box 118, 221 00 Lund, Sweden
R. de Nalda, L. Bañares (eds.), Ultrafast Phenomena in Molecular Sciences,
Springer Series in Chemical Physics 107, DOI 10.1007/978-3-319-02051-8_1,
© Springer International Publishing Switzerland 2014
1
Molecular Movies from Molecular Frame
Photoelectron Angular Distribution (MF-PAD)
Measurements
Arnaud Rouzée, Ymkje Huismans, Freek Kelkensberg, Aneta Smolkowska,
Julia H. Jungmann, Arjan Gijsbertsen, Wing Kiu Siu, Georg Gademann,
Axel Hundertmark, Per Johnsson, and Marc J.J. Vrakking
Abstract We discuss recent and on-going experiments, where molecular frame
photoelectron angular distributions (MFPADs) of high kinetic energy photoelectrons are measured in order to determine the time evolution of molecular structures
in the course of a photochemical event. These experiments include, on the one hand,
measurements where single XUV/X-ray photons, obtained from a free electron laser
(FEL) or by means of high-harmonic generation (HHG), are used to eject a high energy photoelectron, and, on the other hand, measurements where a large number of
mid-infrared photons are absorbed in the course of strong-field ionization. In the
former case, first results indicate a manifestation of the both the electronic orbital
and the molecular structure in the angle-resolved photoelectron distributions, while
in the latter case novel holographic structures are measured that suggest that both the
molecular structure and ultrafast electronic rearrangement processes can be studied
with a time-resolution that reaches down into the attosecond and few-femtosecond
domain.
1.1 Introduction
Much of our knowledge about matter on the nano-scale is based on studies of the
interaction of matter with light. Consequently, the invention of lasers in the infrared,
visible and ultra-violet parts of the wavelength spectrum has greatly benefitted our
understanding of chemical and physical processes. Using lasers, very insightful exA. Rouzée · A. Hundertmark · M.J.J. Vrakking (B)
Max-Born Institut, Max Born Straße 2A, 12489 Berlin, Germany
e-mail: marc.vrakking@mbi-berlin.de
A. Rouzée · Y. Huismans · F. Kelkensberg · A. Smolkowska · J.H. Jungmann · A. Gijsbertsen ·
W.K. Siu · G. Gademann · A. Hundertmark · M.J.J. Vrakking
FOM Institute AMOLF, Science Park 104, 1098 XG Amsterdam, The Netherlands
P. Johnsson
Department of Physics, Lund University, P.O. Box 118, 221 00 Lund, Sweden
R. de Nalda, L. Bañares (eds.), Ultrafast Phenomena in Molecular Sciences,
Springer Series in Chemical Physics 107, DOI 10.1007/978-3-319-02051-8_1,
© Springer International Publishing Switzerland 2014
1