The Early Era of Laser-Selective Chemistry 1960∼1985: Roots of Modern Quantum Control

Abstract

Physicists revolutionized the scientific world when they invented the laser in 1960. During the next two decades, fruitful interplay occurred between theoreticians and experimentalists seeking progress in laser-selective chemistry. In the Early Era, defined as 1960∼1985, scientists gradually realized the immense complexity of the problem of performing tailored manipulations at the molecular scale. However, their efforts opened the doors to a new, broader scientific field of research called quantum control which developed in the Modern Era, defined as 1985 to the present time. This Perspective aims to show that the roots of quantum control may be linked to endeavors to manipulate chemical reactions with lasers and thus reaches as far back as the invention of the laser in 1960. We will emphasize the role of advancing technology, the prescience in the questions raised by researchers, and the role of interdisciplinary research. The Perspective concludes with an assessment of what was achieved in the Early Era.

Generation of High-Lying Vibrational States in Carbon Dioxide through Coherent Ladder Climbing

“…Such reaction control via vibrational excitation has been progressing with the development of mid-IR light sources . The first demonstration was reported to increase the rate of cis–trans isomerization of HNO 2 using an incoherent thermal light source. − Since the advent of mid-IR laser sources, enabling multistep vibrational excitation, or vibrational ladder climbing (VLC), a number of demonstrations were reported such as isotope separation and bond dissociation. − Although most previous experiments were conducted in the gas phase, where the vibrational relaxation is relatively slow, the recent availability of high-energy ultrafast mid-IR lasers in a compact setup has opened a new avenue toward reaction control in the condensed phase.…”