Four-mode multi-selection in the dual phase control of a molecular ionization induced by Fourier-synthesized laser fields

Hideki Ohmura,Naoaki Saito,Tsuyoshi Yoshida

doi:10.1063/1.5082578

Abstract

Coherent laser fields have been used to maximize the rate of a photochemical reaction or provide control over a single targeted property or function of matter by tuning of single-laser or multi-laser parameters. However, there is a need for multi-functionality control, albeit with as few parameters as possible. Here, we report simultaneous control of molecular geometry (selection of molecular orientation) and electron dynamics (electron removal) with dual-phase control of Fourier-synthesized laser fields. Directionally asymmetric tunneling ionization induced by intense, nanosecond, three-color Fourier-synthesized laser fields led to four-mode selection with a combination of positive/negative orientation-selected and yield-enhanced/suppressed molecular ionization of carbonyl sulfide.

Highlights

Quantum control with a single laser parameter, such as the time delay between two laser pulses or the relative phase between two laser fields, is conceptually and technically simple,[3,4,5,6,7] but in most cases, it is limited to controlling single functionality
Asymmetric tunneling ionization induced by intense, nanosecond, three-color Fourier-synthesized laser fields led to four-mode selection with a combination of positive/negative orientation-selected and yield-enhanced/suppressed molecular ionization of carbonyl sulfide
In practical applications such as photoreaction control of molecules, molecules are randomly oriented in a gas or liquid, and light–matter interactions depend on the relative orientation between the molecular geometry and the direction of polarization of the irradiating light

Summary

Introduction

Quantum control with a single laser parameter, such as the time delay between two laser pulses or the relative phase between two laser fields, is conceptually and technically simple,[3,4,5,6,7] but in most cases, it is limited to controlling single functionality. Asymmetric tunneling ionization induced by intense, nanosecond, three-color Fourier-synthesized laser fields led to four-mode selection with a combination of positive/negative orientation-selected and yield-enhanced/suppressed molecular ionization of carbonyl sulfide. We report simultaneous control of molecular geometry (selection of molecular orientation) and electron dynamics (electron removal) by dual phase control of Fourier-synthesized laser fields.

Results

Conclusion