Sparse optimization of two-dimensional terahertz spectroscopy

Wang, Z.; Da, H.; Disa, A. S.; Pullerits, T.; Liu, A.; Schlawin, Frank

doi:10.1063/5.0276901

Sparse optimization of two-dimensional terahertz spectroscopy

Journal Article · Wed Sep 10 00:00:00 EDT 2025 · APL Photonics

DOI:https://doi.org/10.1063/5.0276901· OSTI ID:2589804

^[1]; ^[2]; ^[3]; ^[4]; ^[5]; ^[6]

Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany); Univ. of Hamburg (Germany); Stockholm Univ. (Sweden)
CNPC Research Institute of Safety and Environment Technology, Beijing (China)
Cornell Univ., Ithaca, NY (United States)
Lund Univ. (Sweden)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany); Univ. of Hamburg (Germany)

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 2589804

Report Number(s):: BNL--228998-2025-JAAM

Journal Information:: APL Photonics, Journal Name: APL Photonics Journal Issue: 9 Vol. 10; ISSN 2378-0967

Publisher:: AIP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

References (43)

Direct Visualization of Confinement and Many‐Body Correlation Effects in 2D Spectroscopy of Quantum Dots Amarotti, Edoardo; Wang, Zhengjun; Hedse, Albin Advanced Optical Materials, Vol. 12, Issue 15 https://doi.org/10.1002/adom.202302968	journal	February 2024
Accelerated Nuclear Magnetic Resonance Spectroscopy with Deep Learning Qu, Xiaobo; Huang, Yihui; Lu, Hengfa Angewandte Chemie International Edition, Vol. 59, Issue 26 https://doi.org/10.1002/anie.201908162	journal	April 2020
Stable signal recovery from incomplete and inaccurate measurements Candès, Emmanuel J.; Romberg, Justin K.; Tao, Terence Communications on Pure and Applied Mathematics, Vol. 59, Issue 8, p. 1207-1223 https://doi.org/10.1002/cpa.20124	journal	January 2006
An Exact Expression for Multidimensional Spectroscopy of a Spin‐Boson Hamiltonian Liu, Albert Advanced Quantum Technologies, Vol. 7, Issue 3 https://doi.org/10.1002/qute.202300399	journal	February 2024
High resolution sparse estimation of exponentially decaying N-dimensional signals Swärd, Johan; Adalbjörnsson, Stefan I.; Jakobsson, Andreas Signal Processing, Vol. 128 https://doi.org/10.1016/j.sigpro.2016.04.002	journal	November 2016
Coherent Two-Dimensional and Broadband Electronic Spectroscopies Biswas, Somnath; Kim, JunWoo; Zhang, Xinzi Chemical Reviews, Vol. 122, Issue 3 https://doi.org/10.1021/acs.chemrev.1c00623	journal	January 2022
Compressed Sensing for Reconstructing Coherent Multidimensional Spectra Wang, Zhengjun; Lei, Shiwen; Karki, Khadga Jung The Journal of Physical Chemistry A, Vol. 124, Issue 9 https://doi.org/10.1021/acs.jpca.9b11681	journal	February 2020
Simultaneous Existence of Confined and Delocalized Vibrational Modes in Colloidal Quantum Dots Liu, Albert; Almeida, Diogo B.; Bae, Wan-Ki The Journal of Physical Chemistry Letters, Vol. 10, Issue 20 https://doi.org/10.1021/acs.jpclett.9b02474	journal	September 2019
Coherent Two-Dimensional Optical Spectroscopy Cho, Minhaeng Chemical Reviews, Vol. 108, Issue 4 https://doi.org/10.1021/cr078377b	journal	April 2008
Compressed Sensing for Multidimensional Spectroscopy Experiments Sanders, Jacob N.; Saikin, Semion K.; Mostame, Sarah The Journal of Physical Chemistry Letters, Vol. 3, Issue 18 https://doi.org/10.1021/jz300988p	journal	September 2012
Accelerated 2D-IR Using Compressed Sensing Dunbar, Josef A.; Osborne, Derek G.; Anna, Jessica M. The Journal of Physical Chemistry Letters, Vol. 4, Issue 15 https://doi.org/10.1021/jz401281r	journal	July 2013
Two-dimensional spectroscopy of electronic couplings in photosynthesis Brixner, Tobias; Stenger, Jens; Vaswani, Harsha M. Nature, Vol. 434, Issue 7033 https://doi.org/10.1038/nature03429	journal	March 2005
Watching hydrogen-bond dynamics in a β-turn by transient two-dimensional infrared spectroscopy Kolano, Christoph; Helbing, Jan; Kozinski, Mariusz Nature, Vol. 444, Issue 7118 https://doi.org/10.1038/nature05352	journal	November 2006
Using coherence to enhance function in chemical and biophysical systems Scholes, Gregory D.; Fleming, Graham R.; Chen, Lin X. Nature, Vol. 543, Issue 7647 https://doi.org/10.1038/nature21425	journal	March 2017
Vibronic coherence in oxygenic photosynthesis Fuller, Franklin D.; Pan, Jie; Gelzinis, Andrius Nature Chemistry, Vol. 6, Issue 8 https://doi.org/10.1038/nchem.2005	journal	July 2014
Extreme terahertz magnon multiplication induced by resonant magnetic pulse pairs Huang, C.; Luo, L.; Mootz, M. Nature Communications, Vol. 15, Issue 1 https://doi.org/10.1038/s41467-024-47471-6	journal	April 2024
Multidimensional terahertz probes of quantum materials Liu, Albert npj Quantum Materials, Vol. 10, Issue 1 https://doi.org/10.1038/s41535-025-00741-y	journal	February 2025
Quantum coherence tomography of light-controlled superconductivity Luo, L.; Mootz, M.; Kang, J. H. Nature Physics https://doi.org/10.1038/s41567-022-01827-1	journal	December 2022
Terahertz field-induced nonlinear coupling of two magnon modes in an antiferromagnet Zhang, Zhuquan; Gao, Frank Y.; Curtis, Jonathan B. Nature Physics https://doi.org/10.1038/s41567-024-02386-3	journal	January 2024
Probing inhomogeneous cuprate superconductivity by terahertz Josephson echo spectroscopy Liu, A.; Pavićević, D.; Michael, M. H. Nature Physics, Vol. 20, Issue 11 https://doi.org/10.1038/s41567-024-02643-5	journal	September 2024
Invited Article: Single-shot THz detection techniques optimized for multidimensional THz spectroscopy Teo, Stephanie M.; Ofori-Okai, Benjamin K.; Werley, Christopher A. Review of Scientific Instruments, Vol. 86, Issue 5 https://doi.org/10.1063/1.4921389	journal	May 2015
Optimizing sparse sampling for 2D electronic spectroscopy Roeding, Sebastian; Klimovich, Nikita; Brixner, Tobias The Journal of Chemical Physics, Vol. 146, Issue 8 https://doi.org/10.1063/1.4976309	journal	February 2017
Optical multidimensional coherent spectroscopy Cundiff, Steven T.; Mukamel, Shaul Physics Today, Vol. 66, Issue 7 https://doi.org/10.1063/pt.3.2047	journal	July 2013
Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase Lu, Jian; Zhang, Yaqing; Hwang, Harold Y. Proceedings of the National Academy of Sciences, Vol. 113, Issue 42 https://doi.org/10.1073/pnas.1609558113	journal	October 2016
Josephson plasmonics in layered superconductors Laplace, Y.; Cavalleri, A. Advances in Physics: X, Vol. 1, Issue 3 https://doi.org/10.1080/23746149.2016.1212671	journal	May 2016
Perspective: multi-dimensional coherent spectroscopy of perovskite nanocrystals Liu, Albert; Almeida, Diogo B.; Padilha, Lazaro A. Journal of Physics: Materials, Vol. 5, Issue 2 https://doi.org/10.1088/2515-7639/ac4fa5	journal	February 2022
Spectral broadening and ultrafast dynamics of a nitrogen-vacancy center ensemble in diamond Liu, Albert; Cundiff, Steven T.; Almeida, Diogo B. Materials for Quantum Technology, Vol. 1, Issue 2 https://doi.org/10.1088/2633-4356/abf330	journal	May 2021
Accelerating Ultrafast Spectroscopy with Compressive Sensing Adhikari, Sushovit; Cortes, Cristian L.; Wen, Xiewen Physical Review Applied, Vol. 15, Issue 2 https://doi.org/10.1103/physrevapplied.15.024032	journal	February 2021
Mapping LiNbO3 Phonon-Polariton Nonlinearities with 2D THz-THz-Raman Spectroscopy Lin, Haw-Wei; Mead, Griffin; Blake, Geoffrey A. Physical Review Letters, Vol. 129, Issue 20 https://doi.org/10.1103/physrevlett.129.207401	journal	November 2022
Origin of Terahertz Soft-Mode Nonlinearities in Ferroelectric Perovskites Pal, Shovon; Strkalj, Nives; Yang, Chia-Jung Physical Review X, Vol. 11, Issue 2 https://doi.org/10.1103/physrevx.11.021023	journal	April 2021
Electrodynamics of correlated electron materials Basov, D. N.; Averitt, Richard D.; van der Marel, Dirk Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/revmodphys.83.471	journal	June 2011
A Systematic Review of Compressive Sensing: Concepts, Implementations and Applications Rani, Meenu; Dhok, S. B.; Deshmukh, R. B. IEEE Access, Vol. 6 https://doi.org/10.1109/access.2018.2793851	journal	January 2018
An Introduction To Compressive Sampling Candes, E. J.; Wakin, M. B. IEEE Signal Processing Magazine, Vol. 25, Issue 2 https://doi.org/10.1109/msp.2007.914731	journal	March 2008
Compressed sensing Donoho, D. L. IEEE Transactions on Information Theory, Vol. 52, Issue 4 https://doi.org/10.1109/tit.2006.871582	journal	April 2006
Coherence in Energy Transfer and Photosynthesis Chenu, Aurélia; Scholes, Gregory D. Annual Review of Physical Chemistry, Vol. 66, Issue 1 https://doi.org/10.1146/annurev-physchem-040214-121713	journal	April 2015
T WO -D IMENSIONAL F EMTOSECOND S PECTROSCOPY Jonas, David M. Annual Review of Physical Chemistry, Vol. 54, Issue 1 https://doi.org/10.1146/annurev.physchem.54.011002.103907	journal	October 2003
Compressed sensing MRI: a review from signal processing perspective Ye, Jong Chul BMC Biomedical Engineering, Vol. 1, Issue 1 https://doi.org/10.1186/s42490-019-0006-z	journal	March 2019
Off-axis imaging with off-axis parabolic mirrors Liu, Albert Applied Optics, Vol. 62, Issue 32 https://doi.org/10.1364/ao.505675	journal	November 2023
Nonlinear light–matter interaction at terahertz frequencies Nicoletti, Daniele; Cavalleri, Andrea Advances in Optics and Photonics, Vol. 8, Issue 3 https://doi.org/10.1364/aop.8.000401	journal	January 2016
Resonance lineshapes in two-dimensional Fourier transform spectroscopy Siemens, Mark E.; Moody, Galan; Li, Hebin Optics Express, Vol. 18, Issue 17 https://doi.org/10.1364/oe.18.017699	journal	January 2010
Excitation-dependent features and artifacts in 2-D terahertz spectroscopy Liu, Albert; Disa, Ankit Optics Express, Vol. 32, Issue 16 https://doi.org/10.1364/oe.529152	journal	July 2024
High-speed two-dimensional terahertz spectroscopy with echelon-based shot-to-shot balanced detection Gao, Frank Y.; Zhang, Zhuquan; Liu, Zi-Jie Optics Letters, Vol. 47, Issue 14 https://doi.org/10.1364/ol.462624	journal	July 2022
Organic Crystals for THz Photonics Jazbinsek, Mojca; Puc, Uros; Abina, Andreja Applied Sciences, Vol. 9, Issue 5 https://doi.org/10.3390/app9050882	journal	March 2019

Similar Records

Multidimensional terahertz probes of quantum materials

Journal Article · Sun Feb 09 19:00:00 EST 2025 · npj Quantum Materials · OSTI ID:2513513

Principles of two-dimensional terahertz spectroscopy of collective excitations: The case of Josephson plasmons in layered superconductors

Journal Article · Thu Sep 19 20:00:00 EDT 2024 · Physical Review. B · OSTI ID:2514345

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY

Sparse optimization of two-dimensional terahertz spectroscopy

Citation Formats

References (43)

Similar Records

Related Subjects