Ultrafast Four-Dimensional Coherent Spectroscopy by Projection Reconstruction.

Multidimensional coherent spectroscopy provides insights into the vibronic structure and dynamics of complex systems. In general, the higher the dimensionality, the better the spectral discrimination and the more information that may be extracted about the system. A major impediment to widespread implementation of these methods, however, is that the acquisition time generally increases exponentially with dimensionality, prohibiting practical implementation. We demonstrate the use of nonuniform sampling based on the projection-slice theorem and inverse Radon transform within the context of a fifth-order, 4D technique (GAMERS) designed to correlate the vibrational contributions to different electronic states. Projection-reconstruction (PRO GAMERS) greatly reduces the data sampling requirements without sacrificing frequency resolution. The sensitivity of this technique is demonstrated to surpass conventional uniform sampling by orders of magnitude. The incorporation of projection-reconstruction into multidimensional coherent spectroscopy opens up the possibility to study the structure of complex chemical, biological, and physical systems with unprecedented detail.

[1]  Ray Freeman,et al.  Projection-reconstruction technique for speeding up multidimensional NMR spectroscopy. , 2004, Journal of the American Chemical Society.

[2]  Elad Harel,et al.  Isolated Ground-State Vibrational Coherence Measured by Fifth-Order Single-Shot Two-Dimensional Electronic Spectroscopy. , 2016, The journal of physical chemistry letters.

[3]  E. Harel.  Four-dimensional coherent electronic Raman spectroscopy. , 2017, The Journal of chemical physics.

[4]  Bahram Javidi,et al.  An overview of compressive sensing techniques applied in holography , 2013 .

[5]  Graham R. Fleming,et al.  Two-dimensional spectroscopy of electronic couplings in photosynthesis , 2005, Nature.

[6]  Tobias Brixner,et al.  Inherently phase-stable coherent two-dimensional spectroscopy using only conventional optics. , 2008, Optics letters.

[7]  Brian E. Coggins,et al.  PR-CALC: A Program for the Reconstruction of NMR Spectra from Projections , 2006, Journal of biomolecular NMR.

[8]  Carlos R. Baiz,et al.  Studying Protein-Protein Binding through T-Jump Induced Dissociation: Transient 2D IR Spectroscopy of Insulin Dimer. , 2016, The journal of physical chemistry. B.

[9]  D. Jonas.  Two-dimensional femtosecond spectroscopy. , 2003, Annual review of physical chemistry.

[10]  Elad Harel,et al.  Enhanced-Resolution Single-Shot 2DFT Spectroscopy by Spatial Spectral Interferometry. , 2015, The journal of physical chemistry letters.

[11]  Jasper Knoester,et al.  Two-dimensional spectroscopy of a molecular dimer unveils the effects of vibronic coupling on exciton coherences. , 2014, Nature chemistry.

[12]  Gregory S. Engel,et al.  Quantum coherence spectroscopy reveals complex dynamics in bacterial light-harvesting complex 2 (LH2) , 2012, Proceedings of the National Academy of Sciences.

[13]  E. Harel,et al.  Two-dimensional spectroscopy can distinguish between decoherence and dephasing of zero-quantum coherences. , 2012, The journal of physical chemistry. A.

[14]  Kurt Wüthrich,et al.  The use of cross-sections and of projections in two-dimensional NMR spectroscopy , 1978 .

[15]  Richard D. Schaller,et al.  Measurement of electronic splitting in PbS quantum dots by two-dimensional nonlinear spectroscopy , 2012 .

[16]  G. Cerullo,et al.  Two-Dimensional Electronic Spectroscopy Unravels sub-100 fs Electron and Hole Relaxation Dynamics in Cd-Chalcogenide Nanostructures , 2017, The journal of physical chemistry letters.

[17]  B. Dietzek,et al.  Appearance of intramolecular high-frequency vibrations in two-dimensional, time-integrated three-pulse photon echo data. , 2007, Physical chemistry chemical physics : PCCP.

[18]  Elad Harel,et al.  Quantum coherence selective 2D Raman–2D electronic spectroscopy , 2017, Nature Communications.

[19]  G. Bodenhausen,et al.  Principles of nuclear magnetic resonance in one and two dimensions , 1987 .

[20]  Tak W. Kee,et al.  Vibrational coherence probes the mechanism of ultrafast electron transfer in polymer–fullerene blends , 2014, Nature Communications.

[21]  T. Mančal,et al.  Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems , 2007, Nature.

[22]  R. Freeman,et al.  Projection-reconstruction of three-dimensional NMR spectra. , 2003, Journal of the American Chemical Society.

[23]  G. Engel,et al.  Engineering Coherence Among Excited States in Synthetic Heterodimer Systems , 2013, Science.

[24]  Elad Harel,et al.  Stable and high-power few cycle supercontinuum for 2D ultrabroadband electronic spectroscopy. , 2015, Optics letters.

[25]  Daniel B. Turner,et al.  Ultrabroadband two-quantum two-dimensional electronic spectroscopy , 2016 .

[26]  S. Frick,et al.  Compressed Sensing , 2014, Computer Vision, A Reference Guide.

[27]  Richard A. Mathies,et al.  Excited‐state structure and electronic dephasing time of Nile blue from absolute resonance Raman intensities , 1992 .

[28]  M. Zanni,et al.  Fully absorptive 3D IR spectroscopy using a dual mid-infrared pulse shaper. , 2013, The Journal of chemical physics.

[29]  William K. Peters,et al.  Electronic resonance with anticorrelated pigment vibrations drives photosynthetic energy transfer outside the adiabatic framework , 2012, Proceedings of the National Academy of Sciences.

[30]  Martin T Zanni,et al.  Broadband 2D electronic spectrometer using white light and pulse shaping: noise and signal evaluation at 1 and 100 kHz. , 2017, Optics express.

[31]  E. Harel,et al.  Mapping the Vibronic Structure of a Molecule by Few-Cycle Continuum Two-Dimensional Spectroscopy in a Single Pulse. , 2014, The journal of physical chemistry letters.

[32]  Andrew F Fidler,et al.  Real-time mapping of electronic structure with single-shot two-dimensional electronic spectroscopy , 2010, Proceedings of the National Academy of Sciences.

[33]  S. Hyberts,et al.  Poisson-gap sampling and forward maximum entropy reconstruction for enhancing the resolution and sensitivity of protein NMR data. , 2010, Journal of the American Chemical Society.

[34]  Mark W Maciejewski,et al.  Nonuniform sampling and maximum entropy reconstruction in multidimensional NMR. , 2014, Accounts of chemical research.

[35]  Andrew F Fidler,et al.  Single-shot gradient-assisted photon echo electronic spectroscopy. , 2011, The journal of physical chemistry. A.

[36]  E. van Veldhoven,et al.  Time-resolved optical spectroscopy with multiple population dimensions: a general method for resolving dynamic heterogeneity. , 2007, Chemphyschem : a European journal of chemical physics and physical chemistry.

[37]  Daniel B. Turner,et al.  Two-Quantum 2D FT Electronic Spectroscopy of Biexcitons in GaAs Quantum Wells , 2009, Science.

[38]  J. Skilling,et al.  Exponential sampling, an alternative method for sampling in two-dimensional NMR experiments , 1987 .

[39]  Andrew J. Musser,et al.  Evidence for conical intersection dynamics mediating ultrafast singlet exciton fission , 2015, Nature Physics.

[40]  Elad Harel,et al.  Mapping multidimensional electronic structure and ultrafast dynamics with single-element detection and compressive sensing , 2016, Nature Communications.

[41]  Zhenkun Guo,et al.  Multidimensional resonance Raman spectroscopy by six-wave mixing in the deep UV. , 2014, The Journal of chemical physics.

[42]  Yuan Feng,et al.  General noise suppression scheme with reference detection in heterodyne nonlinear spectroscopy. , 2017, Optics express.

[43]  Xavier Andrade,et al.  Compressed Sensing for Multidimensional Spectroscopy Experiments. , 2012, The journal of physical chemistry letters.

[44]  Graham R Fleming,et al.  Phase-stabilized two-dimensional electronic spectroscopy. , 2004, The Journal of chemical physics.

[45]  E. Harel,et al.  Single-shot ultrabroadband two-dimensional electronic spectroscopy of the light-harvesting complex LH2. , 2011, Optics letters.

[46]  G. Engel,et al.  Controlling quantum-beating signals in 2D electronic spectra by packing synthetic heterodimers on single-walled carbon nanotubes. , 2017, Nature chemistry.