skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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:
 [1];  [2]; ORCiD logo [3]
  1. 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
  2. Univ. of Oregon, Eugene, OR (United States). Dept. of Chemistry and Biochemistry, Oregon Center for Optics, and Inst. of Molecular Biology
  3. Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology
Publication Date:
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) (SC-22)
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.
Pachón, Leonardo A., Marcus, Andrew H., & Aspuru-Guzik, Alán. Quantum process tomography by 2D fluorescence spectroscopy. United States. doi:10.1063/1.4919954.
Pachón, Leonardo A., Marcus, Andrew H., and Aspuru-Guzik, Alán. Mon . "Quantum process tomography by 2D fluorescence spectroscopy". United States. doi:10.1063/1.4919954. https://www.osti.gov/servlets/purl/1370896.
@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 = {2015},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 5 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

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

  • Pachón, Leonardo A.; Brumer, Paul
  • The Journal of Chemical Physics, Vol. 141, Issue 17
  • DOI: 10.1063/1.4900512

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

  • Yuen-Zhou, Joel; Arias, Dylan H.; Eisele, Dorthe M.
  • ACS Nano, Vol. 8, Issue 6
  • DOI: 10.1021/nn406107q

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

  • Widom, Julia R.; Lee, Wonbae; Perdomo-Ortiz, Alejandro
  • The Journal of Physical Chemistry A, Vol. 117, Issue 29
  • DOI: 10.1021/jp400394z

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

  • Lott, G. A.; Perdomo-Ortiz, A.; Utterback, J. K.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 40
  • DOI: 10.1073/pnas.1017308108

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


Measuring protein concentration with entangled photons
journal, June 2012

  • Crespi, Andrea; Lobino, Mirko; Matthews, Jonathan C. F.
  • Applied Physics Letters, Vol. 100, Issue 23
  • DOI: 10.1063/1.4724105

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

  • Schmiegelow, Christian Tomás; Larotonda, Miguel Antonio; Paz, Juan Pablo
  • Physical Review Letters, Vol. 104, Issue 12
  • DOI: 10.1103/PhysRevLett.104.123601

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

  • Yuen-Zhou, J.; Krich, J. J.; Mohseni, M.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 43
  • DOI: 10.1073/pnas.1110642108

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

  • Perdomo-Ortiz, Alejandro; Widom, Julia R.; Lott, Geoffrey A.
  • The Journal of Physical Chemistry B, Vol. 116, Issue 35
  • DOI: 10.1021/jp305916x

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

  • Pachón, Leonardo A.; Yu, Li; Brumer, Paul
  • Faraday Discussions, Vol. 163
  • DOI: 10.1039/c3fd20144a

The failure of the quantum regression hypothesis
journal, April 1986


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


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

  • Tekavec, Patrick F.; Dyke, Thomas R.; Marcus, Andrew H.
  • The Journal of Chemical Physics, Vol. 125, Issue 19
  • DOI: 10.1063/1.2386159

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

  • Pachón, Leonardo A.; Brumer, Paul
  • The Journal of Chemical Physics, Vol. 139, Issue 16
  • DOI: 10.1063/1.4825358

Semiclassical propagation of Wigner functions
journal, June 2010

  • Dittrich, T.; Gómez, E. A.; Pachón, L. A.
  • The Journal of Chemical Physics, Vol. 132, Issue 21
  • DOI: 10.1063/1.3425881

There is No Quantum Regression Theorem
journal, July 1996


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

  • Pachón, Leonardo A.; Brumer, Paul
  • Journal of Mathematical Physics, Vol. 55, Issue 1
  • DOI: 10.1063/1.4858915

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

  • Brüggemann, Ben; Herek, Jennifer L.; Sundström, Villy
  • The Journal of Physical Chemistry B, Vol. 105, Issue 46
  • DOI: 10.1021/jp012072y

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


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

  • Tekavec, Patrick F.; Lott, Geoffrey A.; Marcus, Andrew H.
  • The Journal of Chemical Physics, Vol. 127, Issue 21
  • DOI: 10.1063/1.2800560

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

  • Yuen-Zhou, Joel; Aspuru-Guzik, Alán
  • The Journal of Chemical Physics, Vol. 134, Issue 13
  • DOI: 10.1063/1.3569694

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

  • Raymer, M. G.; Marcus, Andrew H.; Widom, Julia R.
  • The Journal of Physical Chemistry B, Vol. 117, Issue 49
  • DOI: 10.1021/jp405829n

    Works referencing / citing this record:

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


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


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