DOE OSTI · 2589804
Sparse optimization of two-dimensional terahertz spectroscopy
Abstract
Two-dimensional terahertz spectroscopy (2DTS) is a low-frequency analog of two-dimensional optical spectroscopy that is rapidly maturing as a probe of a wide variety of condensed matter systems. However, a persistent problem with 2DTS is the long experimental acquisition times, which prevent its broader adoption. A potential solution, requiring no increase in experimental complexity, is signal reconstruction via compressive sensing. In this work, we apply the sparse exponential mode analysis (SEMA) technique to 2DTS of a cuprate superconductor. We benchmark the performance of the algorithm in reconstructing terahertz nonlinearities and find that SEMA reproduces the asymmetric photon echo line shapes at sampling rates as low as 10%, reaching the reconstruction noise floor at sampling rates beyond 20%–30%. The success of SEMA in reproducing such subtle, asymmetric line shapes confirms compressive sensing as a general method to accelerate 2DTS and multidimensional spectroscopies more broadly.
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Wang, Z. [Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany); Univ. of Hamburg (Germany); Stockholm Univ. (Sweden)] (ORCID:0000000275990382), Da, H. [CNPC Research Institute of Safety and Environment Technology, Beijing (China)] (ORCID:0000000313912837), Disa, A. S. [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000277623244), Pullerits, T. [Lund Univ. (Sweden)] (ORCID:0000000314285564), Liu, A. [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000167183719), Schlawin, Frank [Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany); Univ. of Hamburg (Germany)] (ORCID:0000000169775881). 2025-09-10. Sparse optimization of two-dimensional terahertz spectroscopy. https://doi.org/10.1063/5.0276901
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