Skip to main content
U.S. flag

An official website of the United States government

Dot gov

The .gov means it’s official.
Federal government websites often end in .gov or .mil. Before sharing sensitive information, make sure you’re on a federal government site.


The site is secure.
The https:// ensures that you are connecting to the official website and that any information you provide is encrypted and transmitted securely.

Single-scan acquisition of multiple multidimensional spectra



Travis M. Autry, Galan Moody, James M. Fraser, Corey A. McDonald, Richard P. Mirin, Kevin L. Silverman


Multidimensional coherent spectroscopy is a powerful tool for understanding the ultrafast dynamics of complex quantum systems. To fully characterize the nonlinear optical response of a system, multiple pulse sequences must be recorded and quantitatively compared. We present a new single-scan method that enables rapid and parallel acquisition of all unique pulse sequences corresponding to first- and third-order degenerate wave-mixing processes. Signals are recorded with shot-noise limited detection, enabling acquisition times of ∼2 minutes with ∼100 zs phase stability and ∼8 orders of dynamic range, in a collinear geometry, on a single-pixel detector. We demonstrate this method using quantum well excitons, and quantitative analysis reveals new insights into the bosonic nature of excitons. This scheme may enable rapid and scalable analysis of unique chemical signatures, metrology of optical susceptibilities, nonperturbative coherent control, and the implementation of quantum information protocols using multidimensional spectroscopy.


Spectroscopy, Nonlinear Optics
Created May 29, 2019, Updated July 9, 2019