Echo Spectroscopy in multi-level quantum-mechanical rotors

TL;DR

This paper demonstrates how rotational echo spectroscopy in multi-level molecules depends on pulse delay and intensity, enabling controlled spectroscopic analysis of complex molecular rotational states.

Contribution

It introduces a method to control and analyze multi-level molecular rotations using rotational echo spectroscopy with tailored pulse parameters.

Findings

Rotational echo response varies with pulse delay in multi-level systems.

Controlling second pulse intensity enables selective rotational echo detection.

Theoretical and experimental results align to validate the approach.

Abstract

The rotational echo response of molecules is found to strongly depend on the delay between the two ultrashort laser pulses, as opposed to two-level systems. We study this dependence experimentally and theoretically and show that by judicious control of the 2nd pulse intensity, 'rotational echo spectroscopy' in a multi-level molecular system becomes possible.