High-resolution two-dimensional electronic spectroscopy reveals homogeneous line profiles in isolated nanoparticles

TL;DR

This study uses advanced two-dimensional electronic spectroscopy to analyze isolated nanoparticles, revealing homogeneous line profiles that improve understanding of molecule-environment interactions in nanoconfined systems.

Contribution

It demonstrates the application of high-resolution 2D spectroscopy to probe homogeneous linewidths in gas-phase clusters, providing new insights into system-bath interactions.

Findings

Homogeneous linewidths can be measured in low-density cluster experiments.

The results serve as benchmarks for theoretical models of molecule-cluster interactions.

The method offers a promising route for high-resolution molecular spectroscopy in nanoconfined systems.

Abstract

Doped clusters in the gas phase provide nanoconfined model systems for the study of system-bath interactions. To gain insight into interaction mechanisms between chromophores and their environment, the ensemble inhomogeneity has to be lifted and the homogeneous line profile must be accessed. However, such measurements are very challenging at the low particle densities and low signal levels in cluster beam experiments. Here, we dope cryogenic rare-gas clusters with phthalocyanine molecules and apply action-detected two-dimensional electronic spectroscopy to gain insight into the local molecule-cluster environment for solid and superfluid cluster species. The high-resolution homogeneous linewidth analysis provides a benchmark for the theoretical modelling of binding configurations and shows a promising route for high-resolution molecular two-dimensional spectroscopy.