Investigation of attosecond ionization dynamics in gases and solids with intense few-cycle laser pulses

Abstract

Interaction of intense light fields with dielectric materials has fascinated scientists since the invention of pulsed lasers in the early sixties. Despite the many decades of research, the interest in the field keeps growing because of the potential technological applications of optical (meta-) materials and the prospects of light-controlled peta-Hertz electronics as well as the improving understanding of the fundamental processes behind light-matter interactions. The progress in the short-pulse laser technology that delivered ever-shorter light pulses was echoed by the discoveries of different progressively shorter time scales in the cycle of excitation and energy/charge relaxation in transparent solids, many parts of which are now well understood. The ultimate challenge lies in recovering the earliest stages of the dynamics which are linked to optical-field-ionization that proceeds within a fraction of an optical cycle. One of the complications of advancing the attosecond science to the bulk media is the problem of inducing and detecting a synchronized attosecond response. The charged particles spectroscopy, well developed in gaseous media during last decade and capable of reaching an attosecond temporal resolution cannot be used as an experimental tool for investigation since direct detection of charged particles is impossible in the volume of a solid material.<br />However, solids are the natural place where electronic processes on the sub-femtosecond or attosecond time scale are expected. Very recently several methods for measuring attosecond dynamics in condensed media have been proposed utilizing optical fields in the transparency range of the material.<br />In this thesis a method, suggested in our scientific group is presented.<br />It is an all-optical method based on the detection of optical harmonics originating from ultrafast modulation of a free electron current due to ionization in the field of intense few-cycle laser pulses. This technique will allow retrieving the temporal dynamics of ionization in transparent solids. It can also be considered as an all-optical alternative to the methods of attosecond metrology based on the detection of charged particles. The experiments on the optical-field-ionization in solids are discussed along with the description of the main technologies used in generation and characterization of few-cycle near-IR laser pulses. Characterization of ultra-broadband ultra-short pulses is a separate important problem. A new bandwidth unlimited pulse measurement technique based on quasi-linear temporal phase modulation in a gas weakly ionized by a long pump pulse is presented in this thesis.<br />The most direct way to investigate the electron dynamics in different systems with a high temporal resolution is to employ time-resolved spectroscopy where the initiating and probing optical events are substantially shorter then the characteristic time of the process under investigation. The substantial progress in the development of XUV technologies and attosecond science in the recent years resulted in a remarkable success in studying ionization dynamics in atoms and molecules with a sub-femtosecond time resolution. The closing part of this thesis is dedicated to the time- and energy-resolved measurements of Auger decay in Krypton and Xenon using attosecond XUV-pump-IR-probe spectroscopic technique.<br />