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

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.