Anomalously reduced homogeneous broadening of two-dimensional electronic spectroscopy at high temperature by detailed balance

TL;DR

This paper predicts that under electromagnetically induced transparency, the homogeneous broadening in two-dimensional electronic spectroscopy can be reduced at higher temperatures due to detailed balance, contrary to typical expectations.

Contribution

It introduces the concept that detailed balance can lead to reduced homogeneous broadening in 2DES at high temperatures under EIT conditions, challenging conventional understanding.

Findings

Homogeneous broadening can decrease with increasing temperature under EIT.

Long-lasting off-diagonal peaks are observed in 2DES due to this effect.

Theoretical prediction of anomalous broadening behavior in quantum systems.

Abstract

Dissipation and decoherence of quantum systems in thermal environments is important to various spectroscopies. It is generally believed that dissipation can broaden the line shape of spectroscopies, and thus stronger system-bath interaction can result in more significant homogeneous broadening of two-dimensional electronic spectroscopy (2DES). Here we show that the case can be the opposite in the regime of electromagnetically induced transparency (EIT). We predict that assisted by EIT, the homogeneous broadening of the 2DES at a higher temperature can be significantly reduced due to the detailed balance. This anomalous effect is due to the long-lasting off-diagonal peaks in 2DES.