Compressed Sensing for Multidimensional Spectroscopy Experiments
Open accessAbstract
Compressed sensing is a processing method that significantly reduces the number of measurements needed to accurately resolve signals in many fields of science and engineering. We develop a two-dimensional variant of compressed sensing for multidimensional spectroscopy and apply it to experimental data. For the model system of atomic rubidium vapor, we find that compressed sensing provides an order-of-magnitude (about 10-fold) improvement in spectral resolution along each dimension, as compared to a conventional discrete Fourier transform, using the same data set. More attractive is that compressed sensing allows for random undersampling of the experimental data, down to less than 5% of the experimental data set, with essentially no loss in spectral resolution. We believe that by combining powerful resolution with ease of use, compressed sensing can be a powerful tool for the analysis and interpretation of ultrafast spectroscopy data.
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Claims other papers make about this one
Each is checked against this paper’s own text: does it say what the citing paper says it does?
Non-equilibrium exchanges between system and environment may lead to generation of long-lived quantum coherence in the system.
“This and other non-equilibrium exchanges between system and environment can have considerable influence on the system dynamics [28-35], influence the direction of energy transfer [28] and may even lead to the generation of long-lived quantum coherence in the system [28, 36-38].”
From Vibrations, quanta and biology (2013) · cites this paper as [38]
Self-check
Percentages, sums and reported differences re-computed from the paper’s own numbers.
The self-check needs the paper’s full text.
Cites
Donoho, D. L. (2006) · IEEE Transactions on Information Theory · doi:10.1109/tit.2006.871582 · Cited by 23,994 · see citing works
Donoho, D. L. (2004) · Cited by 16,703 · see citing works
Candes, E. J., Romberg, J., & Tao, T. (2006) · IEEE Transactions on Information Theory · doi:10.1109/tit.2005.862083 · Cited by 15,639 · see citing works
An Introduction To Compressive Sampling
Candes, E. J., & Wakin, M. B. (2008) · IEEE Signal Processing Magazine · doi:10.1109/msp.2007.914731 · Cited by 10,017 · see citing works
Sparse MRI: The application of compressed sensing for rapid MR imaging
Lustig, M., Donoho, D., & Pauly, J. M. (2007) · Magnetic Resonance in Medicine · doi:10.1002/mrm.21391 · Cited by 6,952 · see citing works
Compressive Sensing [Lecture Notes]
Baraniuk, R. G. (2007) · IEEE Signal Processing Magazine · doi:10.1109/msp.2007.4286571 · Cited by 4,203 · see citing works
Probing the Pareto Frontier for Basis Pursuit Solutions
van den Berg, E., & Friedlander, M. P. (2008) · SIAM Journal on Scientific Computing · doi:10.1137/080714488 · Cited by 1,940 · see citing works
Application of Fourier Transform Spectroscopy to Magnetic Resonance
Ernst, R. R., & Anderson, W. A. (1966) · Review of Scientific Instruments · doi:10.1063/1.1719961 · Cited by 1,698 · see citing works
Two-dimensional spectroscopy of electronic couplings in photosynthesis
Brixner, T., Stenger, J., Vaswani, H. M., Cho, M., Blankenship, R. E., & Fleming, G. R. (2005) · Nature · doi:10.1038/nature03429 · Cited by 1,241 · see citing works
Two-Dimensional Femtosecond Spectroscopy
Jonas, D. M. (2003) · Annual Review of Physical Chemistry · doi:10.1146/annurev.physchem.54.011002.103907 · Cited by 1,198 · see citing works
Image reconstruction from incomplete and noisy data
Gull, S. F., & Daniell, G. J. (1978) · Nature · doi:10.1038/272686a0 · Cited by 963 · see citing works
Coherent 2D IR Spectroscopy: Molecular Structure and Dynamics in Solution
Khalil, M., Demirdöven, N., & Tokmakoff, A. (2003) · The Journal of Physical Chemistry A · doi:10.1021/jp0219247 · Cited by 703 · see citing works
Phase-stabilized two-dimensional electronic spectroscopy
Brixner, T., Mančal, T., Stiopkin, I. V., & Fleming, G. R. (2004) · The Journal of Chemical Physics · doi:10.1063/1.1776112 · Cited by 524 · see citing works
Faster STORM using compressed sensing
Zhu, L., Zhang, W., Elnatan, D., et al. (2012) · Nature Methods · doi:10.1038/nmeth.1978 · Cited by 521 · see citing works
Femtosecond Phase-Coherent Two-Dimensional Spectroscopy
Tian, P., Keusters, D., Suzaki, Y., & Warren, W. S. (2003) · Science · doi:10.1126/science.1083433 · Cited by 499 · see citing works
Tekavec, P. F., Lott, G. A., & Marcus, A. H. (2007) · The Journal of Chemical Physics · doi:10.1063/1.2800560 · Cited by 363 · see citing works
Self-citationAndrade, X., Alberdi‐Rodriguez, J., Strubbe, D. A., Oliveira, M. J. T., Nogueira, F., Castro, A., Muguerza, J., Arruabarrena, A., Louie, S. G., Aspuru‐Guzik, A., et al. (2012) · Journal of Physics Condensed Matter · doi:10.1088/0953-8984/24/23/233202 · Cited by 282 · see citing works
Self-citationEfficient Measurement of Quantum Dynamics via Compressive Sensing
Shabani, A., Kosut, R. L., Mohseni, M., RABITZ, H. A., Broome, M. A., de Almeida, M. P., Fedrizzi, A., & White, A. G. (2011) · Physical Review Letters · doi:10.1103/physrevlett.106.100401 · Cited by 229 · see citing works
Zhang, Z., Piątkowski, Ł., Bakker, H. J., et al. (2011) · Nature Chemistry · doi:10.1038/nchem.1158 · Cited by 226 · see citing works
Picosecond dynamics of a membrane protein revealed by 2D IR
Mukherjee, P., Kass, I., Arkin, I. T., et al. (2006) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0508833103 · Cited by 210 · see citing works
NMR data processing using iterative thresholding and minimum l1-norm reconstruction
Stern, A. S., Donoho, D. L., & Hoch, J. C. (2007) · Journal of Magnetic Resonance · doi:10.1016/j.jmr.2007.07.008 · Cited by 149 · see citing works
Lott, G. A., Perdomo‐Ortiz, A., Utterback, J. K., Widom, J. R., Aspuru‐Guzik, A., & Marcus, A. H. (2011) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1017308108 · Cited by 134 · see citing works
Self-citationCoherently Controlled Ultrafast Four-Wave Mixing Spectroscopy
Vaughan, J. C., Hornung, T., Stone, K. W., & Nelson, K. A. (2007) · The Journal of Physical Chemistry A · doi:10.1021/jp0662911 · Cited by 119 · see citing works
Linear prediction spectral analysis of NMR data
Koehl, P. (1999) · Progress in Nuclear Magnetic Resonance Spectroscopy · doi:10.1016/s0079-6565(99)00002-3 · Cited by 113 · see citing works
Perdomo‐Ortiz, A., Widom, J. R., Lott, G. A., Aspuru‐Guzik, A., & Marcus, A. H. (2012) · The Journal of Physical Chemistry B · doi:10.1021/jp305916x · Cited by 107 · see citing works
Self-citationTidal surge in the M2 proton channel, sensed by 2D IR spectroscopy
Ghosh, A., Qiu, J. X., DeGrado, W. F., et al. (2011) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1103027108 · Cited by 102 · see citing works
Application of the linear prediction method to NMR spectroscopy
Led, J. J., & Gesmar, H. (1991) · Chemical Reviews · doi:10.1021/cr00007a007 · Cited by 95 · see citing works
Sparse sampling methods in multidimensional NMR
Mobli, M., Maciejewski, M. W., Schuyler, A. D., et al. (2012) · Physical Chemistry Chemical Physics · doi:10.1039/c2cp40174f · Cited by 87 · see citing works
Quantum state and process tomography of energy transfer systems via ultrafast spectroscopy
Yuen-Zhou, J. Y., Krich, J. J., Mohseni, M., & Aspuru‐Guzik, A. (2011) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1110642108 · Cited by 75 · see citing works
Self-citationYuen-Zhou, J. Y., & Aspuru‐Guzik, A. (2011) · The Journal of Chemical Physics · doi:10.1063/1.3569694 · Cited by 61 · see citing works
Self-citationShrot, Y., & Frydman, L. (2011) · Journal of Magnetic Resonance · doi:10.1016/j.jmr.2011.01.017 · Cited by 60 · see citing works
Application of compressed sensing to the simulation of atomic systems
Andrade, X., Sanders, J. N., & Aspuru‐Guzik, A. (2012) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1209890109 · Cited by 54 · see citing works
Self-citationLPZ spectral analysis using linear prediction and the z transform
Tang, J., & Norris, J. R. (1986) · The Journal of Chemical Physics · doi:10.1063/1.450638 · Cited by 42 · see citing works
Multidimensional ultrafast spectroscopy
Hochstrasser, R. M. (2007) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0706002104 · Cited by 35 · see citing works
Computation of Two-Dimensional Spectra Assisted by Compressed Sampling
Almeida, J., Prior, J., & Plenio, M. B. (2012) · The Journal of Physical Chemistry Letters · doi:10.1021/jz3009369 · Cited by 24 · see citing works
Introduction to the Issue on Compressive Sensing
Chartrand, R., Baraniuk, R. G., Eldar, Y. C., et al. (2010) · IEEE Journal of Selected Topics in Signal Processing · doi:10.1109/jstsp.2010.2043892 · Cited by 19 · see citing works
Flagged first, then by citations
Research works printed but not linked: 12
- [1]R. M. Hochstrasser, Proc. Natl. Acad. Sci. 104 , 14189 (2007)
- [2]P. Hamm and R. M. Hochstrasser, in Ultrafast infrared and Raman spectroscopy , edited by M. D. Fayer (Marcel Dekker, 2001) pp. 273-347
- [8]J. Yuen-Zhou, J. J. Krich, M. Mohseni, and A. AspuruGuzik, Proc. Natl. Acad. Sci. 108 , 17615 (2011)
- [9]E. Candes, J. Romberg, and T. Tao, IEEE Trans. Inf. Theory 52 , 489 (2006)
- [10]D. Donoho, IEEE Trans. Inf. Theory 52 , 1289 (2006), ISSN 0018-9448
- [14]X. Andrade, J. N. Sanders, and A. Aspuru-Guzik, arXiv:1205.6485(2012) · arXiv
- [16]Y. Shrot and L. Frydman, Journal of Magnetic Resonance 209 , 352 (2011)
- [17]J. Almeida, J. Prior, and M. B. Plenio, arXiv:1207.2404(2012) · arXiv
- [21]R. Baraniuk, IEEE Signal Process. Mag. 24 , 118 (2007), ISSN 1053-5888
- [22]E. Candes and M. Wakin, IEEE Signal Process. Mag. 25 , 21 (2008), ISSN 1053-5888
- IEEE J. Sel. Topics Signal Process. 4 , 241 (2010), ISSN 1932-4553
- [24]G. A. Lott, A. Perdomo-Ortiz, J. K. Utterback, J. R. Widom, A. Aspuru-Guzik, and A. H. Marcus, Proc. Natl. Acad. Sci. 108 , 16521 (2011)
Cited by
Sorted by citations
Vibrations, quanta and biology
Huelga, S. F., & Plenio, M. B. (2013) · Contemporary Physics · doi:10.1080/00405000.2013.829687 · Cited by 568 · see citing works
Room-temperature ultrafast nonlinear spectroscopy of a single molecule
Liebel, M., Toninelli, C., & van Hulst, N. F. (2018) · Nature Photonics · doi:10.1038/s41566-017-0056-5 · Cited by 84 · see citing works
Computation of Two-Dimensional Spectra Assisted by Compressed Sampling
Almeida, J., Prior, J., & Plenio, M. B. (2012) · The Journal of Physical Chemistry Letters · doi:10.1021/jz3009369 · Cited by 24 · see citing works
- Authors
- Sanders, J. N., Saikin, S. K., Mostame, S., Andrade, X., Widom, J. R., Marcus, A. H., & Aspuru-Guzik, A.
- Affiliations
- Harvard University (US)
- University of Oregon (US)
- Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States
- ORCID
- Venue
- The Journal of Physical Chemistry Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-09-11
- Volume
- 3
- Issue
- 18
- Pages
- 2697-2702
- ISSN
- 1948-7185 (ISSN-L)
- OpenAlex
- W2120659202
- Cited by
- 83
- References
- 36
- Citations by year
- 2026: 4 · 2025: 3 · 2024: 4 · 2023: 21 · 2022: 4 · 2021: 5 · 2020: 3 · 2019: 5 · 2018: 4 · 2017: 9 · 2016: 7 · 2015: 6 · 2014: 2 · 2013: 5 · 2012: 1
- FWCI
- 4.43
- Type
- journal article
- Language
- en
- Open access
- green
- nrs.harvard.edu
- Licence
- cc-by
- Locations
- The Journal of Physical Chemistry Letters (publishedVersion)
- PubMed (publishedVersion)
- Digital Access to Scholarship at Harvard (DASH) (Harvard University) (submittedVersion, cc-by)
- Topics
- Physical Sciences › Engineering › Computational Mechanics › Sparse and Compressive Sensing Techniques
- Physical Sciences › Mathematics › Applied Mathematics › Mathematical Analysis and Transform Methods
- Physical Sciences › Chemistry › Spectroscopy › Spectroscopy and Laser Applications
- Keywords
- compressed sensing, multidimensional spectroscopy, spectral resolution, undersampling, rubidium vapor, ultrafast spectroscopy
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
