Mapping multidimensional electronic structure and ultrafast dynamics with single-element detection and compressive sensing

Nature Communications
Austin P SpencerElad Harel

Abstract

Compressive sensing allows signals to be efficiently captured by exploiting their inherent sparsity. Here we implement sparse sampling to capture the electronic structure and ultrafast dynamics of molecular systems using phase-resolved 2D coherent spectroscopy. Until now, 2D spectroscopy has been hampered by its reliance on array detectors that operate in limited spectral regions. Combining spatial encoding of the nonlinear optical response and rapid signal modulation allows retrieval of state-resolved correlation maps in a photosynthetic protein and carbocyanine dye. We report complete Hadamard reconstruction of the signals and compression factors as high as 10, in good agreement with array-detected spectra. Single-point array reconstruction by spatial encoding (SPARSE) Spectroscopy reduces acquisition times by about an order of magnitude, with further speed improvements enabled by fast scanning of a digital micromirror device. We envision unprecedented applications for coherent spectroscopy using frequency combs and super-continua in diverse spectral regions.

References

Mar 3, 1999·Proceedings of the National Academy of Sciences of the United States of America·P HammR M Hochstrasser
Mar 11, 2003·Annual Review of Physical Chemistry·David M Jonas
Aug 31, 2004·The Journal of Chemical Physics·Tobias BrixnerGraham R Fleming
Mar 21, 2006·Optics Letters·Sang-Hee ShimMartin T Zanni
Oct 31, 2007·Magnetic Resonance in Medicine : Official Journal of the Society of Magnetic Resonance in Medicine·Michael LustigJohn M Pauly
Dec 11, 2007·The Journal of Chemical Physics·Patrick F TekavecAndrew H Marcus
Mar 28, 2008·Chemical Reviews·Minhaeng Cho
Jul 31, 2008·The Journal of Physical Chemistry. B·Junrong Zheng, M D Fayer
Jul 10, 2010·Proceedings of the National Academy of Sciences of the United States of America·Gitt PanitchayangkoonGregory S Engel
Sep 3, 2010·Proceedings of the National Academy of Sciences of the United States of America·Elad HarelGregory S Engel
Nov 13, 2010·The Journal of Physical Chemistry. a·Cathy Y Wong, Gregory D Scholes
Mar 12, 2011·The Journal of Physical Chemistry. B·Kirill A Velizhanin, Andrei Piryatinski
Nov 25, 2011·The Journal of Chemical Physics·Xiaojun CaiSteven Baldelli
Apr 24, 2012·Nature Methods·Lei ZhuBo Huang
Aug 15, 2012·Proceedings of the National Academy of Sciences of the United States of America·Xavier AndradeAlán Aspuru-Guzik
Jan 8, 2013·Applied Optics·Yair RivensonBahram Javidi
Jul 24, 2014·Nature Communications·Alberto PeruzzoJeremy L O'Brien
Aug 12, 2015·The Journal of Physical Chemistry Letters·Austin P SpencerElad Harel
Aug 19, 2015·The Journal of Physical Chemistry Letters·Boris Spokoyny, Elad Harel
Sep 20, 2012·The Journal of Physical Chemistry Letters·Jacob N SandersAlán Aspuru-Guzik
Mar 25, 2015·ACS Central Science·Jacob N SandersAlán Aspuru-Guzik

❮ Previous
Next ❯

Citations

Aug 16, 2016·ACS Photonics·Joshua S OstranderMartin T Zanni
Mar 3, 2017·The Journal of Chemical Physics·Sebastian RoedingTobias Brixner
Jul 15, 2016·Applied Optics·David J StarlingGregory A Howland
Jun 9, 2018·Sensors·Ashkan Ghanbarzadeh-DagheyanJose Martinez Lorenzo
Feb 13, 2018·The Journal of Physical Chemistry Letters·William O HutsonElad Harel
Jul 19, 2017·Analytical Chemistry·N L P AndrewsH-P Loock
Feb 12, 2020·The Journal of Physical Chemistry. a·Zhengjun WangTönu Pullerits

❮ Previous
Next ❯

Methods Mentioned

BETA
X-ray

Software Mentioned

MAGIC
SPARSE
GRAPES

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.

© 2021 Meta ULC. All rights reserved