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

Title: Using coherence to enhance function in chemical and biophysical systems

Journal Article · · Nature (London)
DOI:https://doi.org/10.1038/nature21425· OSTI ID:1464147
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [8];  [9];  [10];  [11];  [12];  [13];  [14];  [15];  [16];  [17];  [18];  [19]
  1. Princeton Univ., NJ (United States). Dept. of Chemistry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Biophysics and Integrated Bioimaging Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  4. Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology
  5. Univ. of Freiburg (Germany). Inst. of Physics
  6. Boston Univ., MA (United States). Dept. of Chemistry
  7. Univ. of Chicago, IL (United States). Dept. of Chemistry
  8. Vrije Univ., Amsterdam (Netherlands). Dept. of Physics and Astronomy
  9. National Inst. of Natural Sciences (NINS), Okazaki (Japan). Inst. for Molecular Science
  10. Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry and Biochemistry
  11. Univ. of Ottawa, ON (Canada). Dept. of Physics
  12. Michigan State Univ., East Lansing, MI (United States). Dept. of Chemistry
  13. Univ. of California, Irvine, CA (United States). Dept. of Chemistry and Dept. of Physics and Astronomy
  14. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics
  15. Univ. College London (United Kingdom). Dept. of Physics and Astronomy
  16. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  17. Temple Univ., Philadelphia, PA (United States). Dept. of Chemistry
  18. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  19. Columbia Univ., New York, NY (United States). Dept. of Chemistry

Coherence phenomena arise from interference, or the addition, of wave-like amplitudes with fixed phase differences. Although coherence has been shown to yield transformative ways for improving function, advances have been confined to pristine matter and coherence was considered fragile. However, recent evidence of coherence in chemical and biological systems suggests that the phenomena are robust and can survive in the face of disorder and noise. In this work, we survey the state of recent discoveries, present viewpoints that suggest that coherence can be used in complex chemical systems, and discuss the role of coherence as a design element in realizing function.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357
OSTI ID:
1464147
Journal Information:
Nature (London), Vol. 543, Issue 7647; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 415 works
Citation information provided by
Web of Science

References (116)

Charge Carriers in Hybrid Organic–Inorganic Lead Halide Perovskites Might Be Protected as Large Polarons journal November 2015
Coherently wired light-harvesting in photosynthetic marine algae at ambient temperature journal February 2010
Random Laser Action in Semiconductor Powder journal March 1999
Unraveling the Electronic Structure of Individual Photosynthetic Pigment-Protein Complexes journal July 1999
Electron Transport in Molecular Wire Junctions journal May 2003
The Role of Driving Energy and Delocalized States for Charge Separation in Organic Semiconductors journal February 2012
Ultrafast delocalization of excitation in synthetic light-harvesting nanorings journal January 2015
Impact of environmentally induced fluctuations on quantum mechanically mixed electronic and vibrational pigment states in photosynthetic energy transfer and 2D electronic spectra journal June 2015
Weak Localization and Coherent Backscattering of Photons in Disordered Media journal December 1985
Real-time observation of interfering crystal electrons in high-harmonic generation journal July 2015
Macroscopic coherence of a single exciton state in an organic quantum wire journal December 2005
Molecular Electronic Junction Transport: Some Pathways and Some Ideas book January 2011
Vibronic coherence in oxygenic photosynthesis journal July 2014
Theory on Rates of Excitation-Energy Transfer between Molecular Aggregates through Distributed Transition Dipoles with Application to the Antenna System in Bacterial Photosynthesis journal January 1999
Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature journal October 2009
Electronic resonance with anticorrelated pigment vibrations drives photosynthetic energy transfer outside the adiabatic framework journal December 2012
Vibronic Resonances Facilitate Excited-State Coherence in Light-Harvesting Proteins at Room Temperature journal October 2015
Proton-Coupled Electron Transfer journal November 2007
Measurement of qubits journal October 2001
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems journal April 2007
Quantum Transport on Disordered and Noisy Networks: An Interplay of Structural Complexity and Uncertainty journal March 2016
Light Absorption and Energy Transfer in the Antenna Complexes of Photosynthetic Organisms journal March 2016
Measurement of the Stokes parameters of light journal January 1977
Coherent Multidimensional Optical Probes for Electron Correlations and Exciton Dynamics: From NMR to X-rays journal April 2009
Valence-bond calculation of the electronic structure of benzene journal May 1974
Vibronic coupling in quantum wires: Applications to polydiacetylene journal August 2011
The physics and applications of random lasers journal May 2008
Charge migration induced by attosecond pulses in bio-relevant molecules journal June 2016
Coherence in Metal−Metal-to-Ligand-Charge-Transfer Excited States of a Dimetallic Complex Investigated by Ultrafast Transient Absorption Anisotropy journal April 2011
Observation of quantum interference in molecular charge transport journal March 2012
The semiclassical way to molecular spectroscopy journal December 1981
Two‐electron transfer reactions in polar solvents journal July 1996
A quantum circuit rule for interference effects in single-molecule electrical junctions journal March 2015
Non-adiabatic effects in thermochemistry, spectroscopy and kinetics: the general importance of all three Born–Oppenheimer breakdown corrections journal January 2015
What Is Moving in Hybrid Halide Perovskite Solar Cells? journal February 2016
Ultrafast Excited-State Dynamics of Copper(I) Complexes journal February 2015
Engineering nanometre-scale coherence in soft matter journal June 2016
Quantum coherence controls the charge separation in a prototypical artificial light-harvesting system journal March 2013
Quantum correlation among photons from a single quantum dot at room temperature journal August 2000
Classical and quantum transport in deterministic Hamiltonian ratchets journal October 2000
Single-molecule junctions beyond electronic transport journal June 2013
Cross-conjugation and quantum interference: a general correlation? journal January 2014
Optimally Designed Quantum Transport across Disordered Networks journal October 2013
Coherent Intrachain Energy Migration in a Conjugated Polymer at Room Temperature journal January 2009
Quantum information and computation journal March 2000
Long-range electron and excitation energy transfer in donor–bridge–acceptor systems journal September 2008
Environment-assisted quantum transport journal March 2009
The role of non-equilibrium vibrational structures in electronic coherence and recoherence in pigment–protein complexes journal January 2013
Proton-Coupled Electron Transfer in Solution, Proteins, and Electrochemistry journal November 2008
Slow Intramolecular Vibrational Relaxation Leads to Long-Lived Excited-State Wavepackets journal August 2016
Coherent ultrafast charge transfer in an organic photovoltaic blend journal May 2014
Probing wavepacket dynamics using ultrafast x-ray spectroscopy journal September 2015
Vibronic Coupling in J-Aggregates and Beyond: A Direct Means of Determining the Exciton Coherence Length from the Photoluminescence Spectrum journal May 2011
Transport and Entanglement book January 2010
Modern Aspects of the Jahn−Teller Effect Theory and Applications To Molecular Problems journal April 2001
Origin of Long-Lived Coherences in Light-Harvesting Complexes journal June 2012
Pericyclic Reaction Transition States: Passions and Punctilios, 1935-1995 journal February 1995
Room-temperature exciton coherence and dephasing in two-dimensional nanostructures journal January 2015
Quantum coherence and its interplay with protein environments in photosynthetic electronic energy transfer journal January 2010
Monitoring attosecond dynamics of coherent electron-nuclear wave packets by molecular high-order-harmonic generation journal August 2011
Excitons in nanoscale systems journal September 2006
Vibrational Modes and the Dynamic Solvent Effect in Electron and Proton Transfer journal May 1992
Exciton scattering and localization in branched dendrimeric structures journal August 2006
Superexchange-pathway model for long-distance electronic couplings journal October 1991
Long-Range Electron Tunneling journal February 2014
Proton-Coupled Electron Transfer journal April 2012
Concerted Proton−Electron Transfer in the Oxidation of Hydrogen-Bonded Phenols journal April 2006
Localization of Light journal May 1991
Retro-Diels−Alder Femtosecond Reaction Dynamics journal January 1996
T WO -D IMENSIONAL F EMTOSECOND S PECTROSCOPY journal October 2003
Fluctuating exciton localization in giant π-conjugated spoked-wheel macrocycles journal September 2013
On the Mechanism of Light Harvesting in Photosynthetic Purple Bacteria:  B800 to B850 Energy Transfer journal March 2000
Unified treatment of quantum coherent and incoherent hopping dynamics in electronic energy transfer: Reduced hierarchy equation approach journal June 2009
The Spectral Signatures of Frenkel Polarons in H- and J-Aggregates journal March 2010
Coherence in Energy Transfer and Photosynthesis journal April 2015
Screening in crystalline liquids protects energetic carriers in hybrid perovskites journal September 2016
Atomistic Study of Energy Funneling in the Light-Harvesting Complex of Green Sulfur Bacteria journal January 2014
Noise-induced quantum coherence drives photo-carrier generation dynamics at polymeric semiconductor heterojunctions journal January 2014
Tunneling Time for Electron Transfer Reactions journal June 2000
Procedure for Direct Measurement of General Quantum States Using Weak Measurement journal February 2012
Photovoltaic concepts inspired by coherence effects in photosynthetic systems journal December 2016
A straightforward introduction to continuous quantum measurement journal September 2006
Direct observation of ultrafast coherent exciton dynamics in helical π-stacks of self-assembled perylene bisimides journal October 2015
Superradiance and Exciton Delocalization in Bacterial Photosynthetic Light-Harvesting Systems journal September 1997
Spatial propagation of excitonic coherence enables ratcheted energy transfer journal October 2012
Long-lived quantum coherence in photosynthetic complexes at physiological temperature journal July 2010
Origin of long-lived oscillations in 2D-spectra of a quantum vibronic model: Electronic versus vibrational coherence journal December 2013
Quantum coherence in photosynthesis for efficient solar-energy conversion journal July 2014
Exciton–vibrational coupling in the dynamics and spectroscopy of Frenkel excitons in molecular aggregates journal March 2015
Vibrational coherence in the excited state dynamics of Cr(acac)3: probing the reaction coordinate for ultrafast intersystem crossing journal January 2010
What Makes the Photocatalytic CO 2 Reduction on N-Doped Ta 2 O 5 Efficient: Insights from Nonadiabatic Molecular Dynamics journal August 2015
Direct measurement of the quantum wavefunction journal June 2011
Extracting the Excitonic Hamiltonian of the Fenna-Matthews-Olson Complex Using Three-Dimensional Third-Order Electronic Spectroscopy journal April 2011
Multidimensional Attosecond Resonant X-Ray Spectroscopy of Molecules: Lessons from the Optical Regime journal April 2013
Quantum Coherence in Photosynthetic Light Harvesting journal March 2012
Computational design of donor-bridge-acceptor systems exhibiting pronounced quantum interference effects journal January 2016
Wavelike charge density fluctuations and van der Waals interactions at the nanoscale journal March 2016
Elucidation of the timescales and origins of quantum electronic coherence in LHCII journal March 2012
M ULTIDIMENSIONAL F EMTOSECOND C ORRELATION S PECTROSCOPIES OF E LECTRONIC AND V IBRATIONAL E XCITATIONS journal October 2000
Lessons from nature about solar light harvesting journal September 2011
E LECTRON T RANSMISSION T HROUGH M OLECULES AND M OLECULAR I NTERFACES journal October 2001
Biological charge transfer via flickering resonance journal June 2014
Semiclassical Path Integral Dynamics: Photosynthetic Energy Transfer with Realistic Environment Interactions journal May 2016
Non-classicality of the molecular vibrations assisting exciton energy transfer at room temperature journal January 2014
Perovskites: The Emergence of a New Era for Low-Cost, High-Efficiency Solar Cells journal October 2013
Proton-Coupled Electron Transfer text January 2007
Quantum coherence controls the charge separation in a prototypical artificial light harvesting system conference May 2013
Real-time Observation of interfering Crystal electroncs in high-harmonic Generation text January 2015
Proton-Coupled Electron Transfer journal October 1998
Spatial propagation of excitonic coherence enables ratcheted energy transfer text January 2011
Direct Measurement of the Quantum Wavefunction text January 2011
Optimally designed quantum transport across disordered networks text January 2012
Atomistic study of energy funneling in the light-harvesting complex of green sulfur bacteria text January 2013
Origin of long-lived oscillations in 2D-spectra of a Quantum Vibronic Model: Electronic vs Vibrational coherence text January 2013
The Role of Driving Energy and Delocalised States for Charge Separation in Organic Semiconductors text January 2013
A Straightforward Introduction to Continuous Quantum Measurement text January 2006

Cited By (100)

Molecular Semiconductors for Logic Operations: Dead‐End or Bright Future? journal January 2020
Effect of an underdamped vibration with both diagonal and off‐diagonal exciton–phonon interactions on excitation energy transfer journal December 2018
Strong Light–Matter Coupling as a New Tool for Molecular and Material Engineering: Quantum Approach journal September 2018
Multidimensional Vibrational Coherence Spectroscopy journal August 2018
Studying light-harvesting models with superconducting circuits journal March 2018
Coherent exciton-vibrational dynamics and energy transfer in conjugated organics journal June 2018
Coherence in carotenoid-to-chlorophyll energy transfer journal August 2018
Tensor network simulation of multi-environmental open quantum dynamics via machine learning and entanglement renormalisation journal March 2019
Spectroscopic disentanglement of the quantum states of highly excited Cu2 journal July 2019
Modelling the ultra-strongly coupled spin-boson model with unphysical modes journal August 2019
A molecular movie of ultrafast singlet fission journal September 2019
Vibronic coherence evolution in multidimensional ultrafast photochemical processes journal December 2019
Strong optical response and light emission from a monolayer molecular crystal journal December 2019
Efficient quantum simulation of photosynthetic light harvesting journal October 2018
Probing quantum features of photosynthetic organisms journal November 2018
Attosecond-fast internal photoemission journal January 2020
The ultrafast X-ray spectroscopic revolution in chemical dynamics journal May 2018
Quantum coherences reveal excited-state dynamics in biophysical systems journal June 2019
P band intermediate state (PBIS) tailors photoluminescence emission at confined nanoscale interface journal November 2019
Advances in polydiacetylene development for the design of side chain groups in smart material applications – a mini review journal January 2017
Tracing feed-back driven exciton dynamics in molecular aggregates journal January 2018
Turning the challenge of quantum biology on its head: biological control of quantum optical systems journal January 2019
Chimera: enabling hierarchy based multi-objective optimization for self-driving laboratories journal January 2018
Transient synchronisation and quantum coherence in a bio-inspired vibronic dimer journal January 2019
Vibrational coherence and quantum yield of retinal-chromophore-inspired molecular switches journal January 2020
Time-resolved spectra of I 2 in a krypton crystal by G-MCTDH simulations: nonadiabatic dynamics, dissipation and environment driven decoherence journal January 2020
Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport journal January 2020
Exciton dissociation and charge separation at donor–acceptor interfaces from quantum-classical dynamics simulations journal January 2020
A theory on the role of π-electrons of docosahexaenoic acid in brain function: The six methylene-interrupted double bonds and the precision of neural signaling journal May 2018
Molecular model of J-aggregated pseudoisocyanine fibers journal July 2018
Electronic interactions do not affect electronic decoherence in the pure-dephasing limit journal November 2018
Theoretical investigation of real-time charge dynamics in open systems coupled to bulk materials journal May 2019
Role of coherence in the plasmonic control of molecular absorption journal July 2019
Vibrational coherence transfer illuminates dark modes in models of the FeFe hydrogenase active site journal August 2019
Photoinduced anomalous Coulomb blockade and the role of triplet states in electron transport through an irradiated molecular transistor. II. Effects of electron-phonon coupling and vibrational relaxation journal August 2019
Non-equilibrium relaxation of hot states in organic semiconductors: Impact of mode-selective excitation on charge transfer journal August 2019
Space- and time-resolved UV-to-NIR surface spectroscopy and 2D nanoscopy at 1 MHz repetition rate journal November 2019
Quantum modeling of ultrafast photoinduced charge separation journal December 2017
The future of quantum biology journal November 2018
Quantum effects in biology: golden rule in enzymes, olfaction, photosynthesis and magnetodetection journal May 2017
The origins of quantum biology journal December 2018
Diagrammatic time-local master equation for open quantum systems journal January 2020
Coherence and decoherence in quantum absorption refrigerators journal July 2018
Signatures of Strong Vibronic Coupling Mediating Coherent Charge Transfer in Two-Dimensional Electronic Spectroscopy journal August 2019
Excitons in Carbonic Nanostructures journal November 2019
Excited State Structural Evolution of a GFP Single-Site Mutant Tracked by Tunable Femtosecond-Stimulated Raman Spectroscopy journal September 2018
The hierarchical and perturbative forms of stochastic Schrödinger equations and their applications to carrier dynamics in organic materials journal July 2018
Multidimensional Vibrational Coherence Spectroscopy book December 2018
Engineering the vibrational coherence of vision into a synthetic molecular device journal January 2018
Vibronic coherence contributes to photocurrent generation in organic semiconductor heterojunction diodes journal January 2020
Quantum coherence in ultrafast photo-driven charge separation journal January 2019
Before Förster. Initial excitation in photosynthetic light harvesting journal January 2019
Signatures of vibronic coupling in two-dimensional electronic-vibrational and vibrational-electronic spectroscopies journal September 2017
Probing quantum coherence in ultrafast molecular processes: An ab initio approach to open quantum systems journal May 2018
How nature designs light-harvesting antenna systems: design principles and functional realization in chlorophototrophic prokaryotes journal January 2018
Coherent multidimensional spectroscopy in the gas phase journal August 2019
Electronic structure in the transition metal block and its implications for light harvesting journal January 2019
A molecular movie of ultrafast singlet fission text January 2019
Chimera: Enabling Hierarchy Based Multi-Objective Optimization for Self-Driving Laboratories posted_content April 2018
Synergistic Approach of Ultrafast Spectroscopy and Molecular Simulations in the Characterization of Intramolecular Charge Transfer in Push-Pull Molecules journal January 2020
Studying light-harvesting models with superconducting circuits text January 2018
The highly excited-state manifold of guanine: calibration for nonlinear electronic spectroscopy simulations journal March 2018
Observing charge separation in nanoantennas via ultrafast point-projection electron microscopy journal August 2018
Vibrational coherences in manganese single-molecule magnets after ultrafast photoexcitation journal March 2020
A negative feedback loop based on proton-driven in situ formation of plasmonic molybdenum oxide nanosheets journal January 2018
Coherent wavepackets in the Fenna-Matthews-Olson complex are robust to excitonic-structure perturbations caused by mutagenesis journal January 2019
Monitoring polariton dynamics in the LHCII photosynthetic antenna in a microcavity by two-photon coincidence counting journal February 2018
Optimizing co-operative multi-environment dynamics in a dark-state-enhanced photosynthetic heat engine journal August 2018
Macroscopic coherence as an emergent property in molecular nanotubes journal January 2019
Certification and Quantification of Multilevel Quantum Coherence journal October 2018
Resonance Energy Transfer: From Fundamental Theory to Recent Applications journal July 2019
Disentangling Ultrafast Electronic and Structural Dynamics with X-Ray Lasers journal September 2018
Switching between H- and J-type electronic coupling in single conjugated polymer aggregates journal November 2017
A solvent–solute cooperative mechanism for symmetry-breaking charge transfer journal January 2020
Unveiling coupled electronic and vibrational motions of chromophores in condensed phases journal November 2019
Double-crossed polarization transient grating for distinction and characterization of coherences journal January 2018
A molecular movie of ultrafast singlet fission. text January 2019
Non-equilibrium relaxation of hot states in organic semiconductors: Impact of mode-selective excitation on charge transfer. text January 2019
Vibrational Coherences in Manganese Single-molecule Magnets after Ultrafast Photoexcitation posted_content December 2018
Multiscale modelling of photoinduced processes in composite systems journal April 2019
Chimera: Enabling Hierarchy Based Multi-Objective Optimization for Self-Driving Laboratories posted_content April 2018
Switching between H- and J-type electronic coupling in single conjugated polymer aggregates text January 2017
Electronic Couplings in (Bio-) Chemical Processes journal March 2018
Recent advances in multidimensional ultrafast spectroscopy journal January 2018
Studying Light-Harvesting Models with Superconducting Circuits text January 2017
Probing quantum features of photosynthetic organisms text January 2017
Theory for polariton-assisted remote energy transfer preprint January 2017
Coherence and decoherence in quantum absorption refrigerators text January 2018
Macroscopic coherence as an emergent property in molecular nanotubes text January 2018
Photoinduced Anomalous Coulomb Blockade and the Role of Triplet States in Electron Transport through an Irradiated Molecular Transistor II: Effects of Electron-Phonon Coupling and Vibrational Relaxation text January 2019
Two-Dimensional Electronic Spectroscopy Reveals Dynamics and Mechanisms of Solvent-Driven Inertial Relaxation in Polar BODIPY Dyes journal February 2018
Photoinduced Electron Transfer in Donor–Acceptor Complexes: Isotope Effect and Dynamic Symmetry Breaking journal October 2019
Evolution of the Fenna–Matthews–Olson Complex and Its Quantum Coherence Features. Which Led the Way? journal October 2017
Publisher Correction: Studying light-harvesting models with superconducting circuits journal June 2018
Simulation of Quantum Dynamics of Excitonic Systems at Finite Temperature: an efficient method based on Thermo Field Dynamics journal August 2017
Mechanistic insight into internal conversion process within Q-bands of chlorophyll a journal September 2017
Local protein solvation drives direct down-conversion in phycobiliprotein PC645 via incoherent vibronic transport journal March 2018
Spectroscopic disentanglement of the quantum states of highly excited Cu2 text January 2019
The light-harvesting complex 2 of allochromatium vinosum: B800 absorption band splitting and exciton relaxation text January 2019
Distribution of quantum entanglement: Principles and applications preprint January 2020