Tri-comb spectroscopy

TL;DR

Tri-comb spectroscopy introduces a rapid, high-resolution, and compact method for multidimensional coherent spectroscopy using three frequency combs, enabling faster data acquisition and potential field applications.

Contribution

It presents a novel tri-comb spectroscopy technique that simplifies setup, accelerates data collection, and enhances resolution compared to traditional MDCS methods.

Findings

Generated multidimensional spectra with 365 ms data acquisition

Achieved comb resolution without mechanical moving parts

Demonstrated potential for field-deployable chemical sensing

Abstract

Multi-dimensional coherent spectroscopy (MDCS)1,2 is a powerful method for optical spectroscopy that has become an important tool for studying ultrafast dynamics in a wide range of systems. It is an optical analog of multidimensional nuclear magnetic resonance spectroscopy that enables the measurement of homogeneous linewidths in inhomogeneously broadened systems, many-body interactions, and coupling between excited resonances, all of which are not simultaneously accessible by any other linear or non-linear method. Current implementations of MDCS require a bulky apparatus and suffer from resolution and acquisition speed limitations that constrain their applications outside the laboratory3-5. Here we propose and demonstrate an approach to nonlinear coherent spectroscopy that utilizes three frequency combs with slightly different repetition rates. Unlike traditional nonlinear methods, tri-comb spectroscopy uses only a single photodetector and no mechanical moving elements to enable faster acquisition times, while also providing comb resolution. As a proof of concept, a multidimensional coherent spectrum with comb cross-diagonal resolution is generated using only 365 ms of data. These improvements make multidimensional coherent spectroscopy relevant for systems with narrow resonances (especially cold atomic and molecular systems). In addition the method has the potential to be field deployable for chemical sensing applications.