Quantum process tomography by 2D fluorescence spectroscopy

Pachón, Leonardo A.; Marcus, Andrew H.; Aspuru-Guzik, Alán

doi:10.1063/1.4919954

Title: Quantum process tomography by 2D fluorescence spectroscopy

Abstract

Reconstruction of the dynamics (quantum process tomography) of the single-exciton manifold in energy transfer systems is proposed here on the basis of two-dimensional fluorescence spectroscopy (2D-FS) with phase-modulation. The quantum-process-tomography protocol introduced here benefits from, e.g., the sensitivity enhancement ascribed to 2D-FS. Although the isotropically averaged spectroscopic signals depend on the quantum yield parameter Γ of the doubly excited-exciton manifold, it is shown that the reconstruction of the dynamics is insensitive to this parameter. Finally, applications to foundational and applied problems, as well as further extensions, are discussed.

Authors:

Pachón, Leonardo A. ^[1]; Marcus, Andrew H. ^[2];

^[3]

Univ. de Antioquia UdeA, Medellín, (Colombia) Grupo de Física Atómica y Molecular, Inst. de Física, Facultad de Ciencias Exactas y Naturales; Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology
Univ. of Oregon, Eugene, OR (United States). Dept. of Chemistry and Biochemistry, Oregon Center for Optics, and Inst. of Molecular Biology
Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology

Publication Date:: Mon May 18 00:00:00 EDT 2015

Research Org.:: Energy Frontier Research Centers (EFRC), Washington D.C. (United States). Center for Excitonics (CE)

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

OSTI Identifier:: 1370896

Alternate Identifier(s):: OSTI ID: 1228176

Grant/Contract Number:: SC0001088

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 142; Journal Issue: 21; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (photovoltaic); solid state lighting; photosynthesis (natural and artificial); charge transport; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats


                    Pachón, Leonardo A., Marcus, Andrew H., and Aspuru-Guzik, Alán. Quantum process tomography by 2D fluorescence spectroscopy.  United States: N. p., 2015. 
Web.  doi:10.1063/1.4919954.

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                    Pachón, Leonardo A., Marcus, Andrew H., & Aspuru-Guzik, Alán. Quantum process tomography by 2D fluorescence spectroscopy.  United States.  https://doi.org/10.1063/1.4919954

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                    Pachón, Leonardo A., Marcus, Andrew H., and Aspuru-Guzik, Alán. Mon .  
"Quantum process tomography by 2D fluorescence spectroscopy".  United States.  https://doi.org/10.1063/1.4919954.  https://www.osti.gov/servlets/purl/1370896.

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@article{osti_1370896,

  title        = {Quantum process tomography by 2D fluorescence spectroscopy},

  author       = {Pachón, Leonardo A. and Marcus, Andrew H. and Aspuru-Guzik, Alán},

  abstractNote = {Reconstruction of the dynamics (quantum process tomography) of the single-exciton manifold in energy transfer systems is proposed here on the basis of two-dimensional fluorescence spectroscopy (2D-FS) with phase-modulation. The quantum-process-tomography protocol introduced here benefits from, e.g., the sensitivity enhancement ascribed to 2D-FS. Although the isotropically averaged spectroscopic signals depend on the quantum yield parameter Γ of the doubly excited-exciton manifold, it is shown that the reconstruction of the dynamics is insensitive to this parameter. Finally, applications to foundational and applied problems, as well as further extensions, are discussed.},

  doi          = {10.1063/1.4919954},

  journal      = {Journal of Chemical Physics},

  number       = 21,

  volume       = 142,

  place        = {United States},

  year         = {Mon May 18 00:00:00 EDT 2015},

  month        = {Mon May 18 00:00:00 EDT 2015}

}

Copy to clipboard

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Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods
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Title: Quantum process tomography by 2D fluorescence spectroscopy

Abstract

Citation Formats

Direct experimental determination of spectral densities of molecular complexes journal, November 2014

Coherent Exciton Dynamics in Supramolecular Light-Harvesting Nanotubes Revealed by Ultrafast Quantum Process Tomography journal, April 2014

Two-dimensional electronic spectroscopy of an excitonically coupled dimer journal, July 2006

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Temperature-Dependent Conformations of a Membrane Supported Zinc Porphyrin Tweezer by 2D Fluorescence Spectroscopy journal, March 2013

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Direct Characterization of Quantum Dynamics journal, October 2006

Experimental realization of direct characterization of quantum dynamics journal, April 2007

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Solution conformation of 2-aminopurine dinucleotide determined by ultraviolet two-dimensional fluorescence spectroscopy journal, February 2013

Experimental Characterization of Quantum Dynamics Through Many-Body Interactions journal, February 2013

Conformation of self-assembled porphyrin dimers in liposome vesicles by phase-modulation 2D fluorescence spectroscopy journal, September 2011

Nonclassical phase-space trajectories for the damped harmonic quantum oscillator journal, October 2010

Measuring protein concentration with entangled photons journal, June 2012

Selective and Efficient Quantum Process Tomography with Single Photons journal, March 2010

Quantum state and process tomography of energy transfer systems via ultrafast spectroscopy journal, October 2011

Conformation and Electronic Population Transfer in Membrane-Supported Self-Assembled Porphyrin Dimers by 2D Fluorescence Spectroscopy journal, August 2012

Coherent one-photon phase control in closed and open quantum systems: A general master equation approach journal, January 2013

The failure of the quantum regression hypothesis journal, April 1986

Efficient Measurement of Quantum Dynamics via Compressive Sensing journal, March 2011

50 years of DNA ‘Breathing’: Reflections on old and new approaches [For special issue of biopolymers on 50 years of nucleic acids research] journal, July 2013

Wave packet interferometry and quantum state reconstruction by acousto-optic phase modulation journal, November 2006

Incoherent excitation of thermally equilibrated open quantum systems journal, February 2013

Selective and Efficient Estimation of Parameters for Quantum Process Tomography journal, May 2008

Coherence Dynamics in Photosynthesis: Protein Protection of Excitonic Coherence journal, June 2007

Mechanisms in environmentally assisted one-photon phase control journal, October 2013

Semiclassical propagation of Wigner functions journal, June 2010

There is No Quantum Regression Theorem journal, July 1996

Quantum driven dissipative parametric oscillator in a blackbody radiation field journal, January 2014

Microscopic Theory of Exciton Annihilation: Application to the LH2 Antenna System journal, November 2001

Prescription for experimental determination of the dynamics of a quantum black box journal, November 1997

Ultrafast Spectroscopy: Quantum information and wavepackets book, September 2014

Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation journal, December 2007

Quantum process tomography of excitonic dimers from two-dimensional electronic spectroscopy. I. General theory and application to homodimers journal, April 2011

Entangled Photon-Pair Two-Dimensional Fluorescence Spectroscopy (EPP-2DFS) journal, September 2013

Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods journal, June 2018

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting journal, October 2019

Quantum coherences reveal excited-state dynamics in biophysical systems journal, June 2019

Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport journal, January 2020

Secular versus nonsecular Redfield dynamics and Fano coherences in incoherent excitation: An experimental proposal journal, January 2018

Single-scan acquisition of multiple multidimensional spectra journal, January 2019

Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods book, June 2018

Secular vs. Non-secular Redfield Dynamics and Fano Coherences in Incoherent Excitation: An Experimental Proposal text, January 2017

Direct experimental determination of spectral densities of molecular complexes
journal, November 2014

Coherent Exciton Dynamics in Supramolecular Light-Harvesting Nanotubes Revealed by Ultrafast Quantum Process Tomography
journal, April 2014

Two-dimensional electronic spectroscopy of an excitonically coupled dimer
journal, July 2006

Completely positive linear maps on complex matrices
journal, June 1975

Temperature-Dependent Conformations of a Membrane Supported Zinc Porphyrin Tweezer by 2D Fluorescence Spectroscopy
journal, March 2013

Two-Dimensional Optical Spectroscopy
book, January 2009

Direct Characterization of Quantum Dynamics
journal, October 2006

Experimental realization of direct characterization of quantum dynamics
journal, April 2007

Time-Domain Scars: Resolving the Spectral Form Factor in Phase Space
journal, April 2009

Solution conformation of 2-aminopurine dinucleotide determined by ultraviolet two-dimensional fluorescence spectroscopy
journal, February 2013

Experimental Characterization of Quantum Dynamics Through Many-Body Interactions
journal, February 2013

Conformation of self-assembled porphyrin dimers in liposome vesicles by phase-modulation 2D fluorescence spectroscopy
journal, September 2011

Nonclassical phase-space trajectories for the damped harmonic quantum oscillator
journal, October 2010

Measuring protein concentration with entangled photons
journal, June 2012

Selective and Efficient Quantum Process Tomography with Single Photons
journal, March 2010

Quantum state and process tomography of energy transfer systems via ultrafast spectroscopy
journal, October 2011

Conformation and Electronic Population Transfer in Membrane-Supported Self-Assembled Porphyrin Dimers by 2D Fluorescence Spectroscopy
journal, August 2012

Coherent one-photon phase control in closed and open quantum systems: A general master equation approach
journal, January 2013

The failure of the quantum regression hypothesis
journal, April 1986

Efficient Measurement of Quantum Dynamics via Compressive Sensing
journal, March 2011

50 years of DNA ‘Breathing’: Reflections on old and new approaches [For special issue of biopolymers on 50 years of nucleic acids research]
journal, July 2013

Wave packet interferometry and quantum state reconstruction by acousto-optic phase modulation
journal, November 2006

Incoherent excitation of thermally equilibrated open quantum systems
journal, February 2013

Selective and Efficient Estimation of Parameters for Quantum Process Tomography
journal, May 2008

Coherence Dynamics in Photosynthesis: Protein Protection of Excitonic Coherence
journal, June 2007

Mechanisms in environmentally assisted one-photon phase control
journal, October 2013

Semiclassical propagation of Wigner functions
journal, June 2010

There is No Quantum Regression Theorem
journal, July 1996

Quantum driven dissipative parametric oscillator in a blackbody radiation field
journal, January 2014

Microscopic Theory of Exciton Annihilation: Application to the LH2 Antenna System
journal, November 2001

Prescription for experimental determination of the dynamics of a quantum black box
journal, November 1997

Ultrafast Spectroscopy: Quantum information and wavepackets
book, September 2014

Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation
journal, December 2007

Quantum process tomography of excitonic dimers from two-dimensional electronic spectroscopy. I. General theory and application to homodimers
journal, April 2011

Entangled Photon-Pair Two-Dimensional Fluorescence Spectroscopy (EPP-2DFS)
journal, September 2013

Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods
journal, June 2018

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting
journal, October 2019

Quantum coherences reveal excited-state dynamics in biophysical systems
journal, June 2019

Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport
journal, January 2020

Secular versus nonsecular Redfield dynamics and Fano coherences in incoherent excitation: An experimental proposal
journal, January 2018

Single-scan acquisition of multiple multidimensional spectra
journal, January 2019

Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods
book, June 2018

Secular vs. Non-secular Redfield Dynamics and Fano Coherences in Incoherent Excitation: An Experimental Proposal
text, January 2017