Quantum Computation of Electronic Transitions Using a Variational Quantum Eigensolver
Abstract
We develop an extension of the variational quantum eigensolver (VQE) algorithm – multistate, contracted VQE (MC-VQE) – that allows for the efficient computation of the transition energies between the ground state and several low-lying excited states of a molecule, as well as the oscillator strengths associated with these transitions. Here, we numerically simulate MC-VQE by computing the absorption spectrum of an ab initio exciton model of an 18-chromophore light-harvesting complex from purple photosynthetic bacteria
- Authors:
-
- Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); QC Ware Corp., Palo Alto, CA (United States)
- Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Stanford Univ., Stanford, CA (United States); QC Ware Corp., Palo Alto, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1512808
- Alternate Identifier(s):
- OSTI ID: 1546400
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 23; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Parrish, Robert M., Hohenstein, Edward G., McMahon, Peter L., and Martínez, Todd J. Quantum Computation of Electronic Transitions Using a Variational Quantum Eigensolver. United States: N. p., 2019.
Web. doi:10.1103/PhysRevLett.122.230401.
Parrish, Robert M., Hohenstein, Edward G., McMahon, Peter L., & Martínez, Todd J. Quantum Computation of Electronic Transitions Using a Variational Quantum Eigensolver. United States. https://doi.org/10.1103/PhysRevLett.122.230401
Parrish, Robert M., Hohenstein, Edward G., McMahon, Peter L., and Martínez, Todd J. Wed .
"Quantum Computation of Electronic Transitions Using a Variational Quantum Eigensolver". United States. https://doi.org/10.1103/PhysRevLett.122.230401. https://www.osti.gov/servlets/purl/1512808.
@article{osti_1512808,
title = {Quantum Computation of Electronic Transitions Using a Variational Quantum Eigensolver},
author = {Parrish, Robert M. and Hohenstein, Edward G. and McMahon, Peter L. and Martínez, Todd J.},
abstractNote = {We develop an extension of the variational quantum eigensolver (VQE) algorithm – multistate, contracted VQE (MC-VQE) – that allows for the efficient computation of the transition energies between the ground state and several low-lying excited states of a molecule, as well as the oscillator strengths associated with these transitions. Here, we numerically simulate MC-VQE by computing the absorption spectrum of an ab initio exciton model of an 18-chromophore light-harvesting complex from purple photosynthetic bacteria},
doi = {10.1103/PhysRevLett.122.230401},
journal = {Physical Review Letters},
number = 23,
volume = 122,
place = {United States},
year = {Wed Jun 12 00:00:00 EDT 2019},
month = {Wed Jun 12 00:00:00 EDT 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 100 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Assessment of a long-range corrected hybrid functional
journal, December 2006
- Vydrov, Oleg A.; Scuseria, Gustavo E.
- The Journal of Chemical Physics, Vol. 125, Issue 23
An Ab Initio Exciton Model Including Charge-Transfer Excited States
journal, July 2017
- Li, Xin; Parrish, Robert M.; Liu, Fang
- Journal of Chemical Theory and Computation, Vol. 13, Issue 8
Dephasing-assisted transport: quantum networks and biomolecules
journal, November 2008
- Plenio, M. B.; Huelga, S. F.
- New Journal of Physics, Vol. 10, Issue 11
Tensor hypercontraction density fitting. I. Quartic scaling second- and third-order Møller-Plesset perturbation theory
journal, July 2012
- Hohenstein, Edward G.; Parrish, Robert M.; Martínez, Todd J.
- The Journal of Chemical Physics, Vol. 137, Issue 4
A long-range-corrected time-dependent density functional theory
journal, May 2004
- Tawada, Yoshihiro; Tsuneda, Takao; Yanagisawa, Susumu
- The Journal of Chemical Physics, Vol. 120, Issue 18
Molecular Electronic-Structure Theory
book, August 2000
- Helgaker, Trygve; Jørgensen, Poul; Olsen, Jeppe
Exact Two-Qubit Universal Quantum Circuit
journal, July 2003
- Zhang, Jun; Vala, Jiri; Sastry, Shankar
- Physical Review Letters, Vol. 91, Issue 2
Tensor hypercontraction. II. Least-squares renormalization
journal, December 2012
- Parrish, Robert M.; Hohenstein, Edward G.; Martínez, Todd J.
- The Journal of Chemical Physics, Vol. 137, Issue 22
Entanglement and entangling power of the dynamics in light-harvesting complexes
journal, June 2010
- Caruso, Filippo; Chin, Alex W.; Datta, Animesh
- Physical Review A, Vol. 81, Issue 6
A full coupled‐cluster singles and doubles model: The inclusion of disconnected triples
journal, February 1982
- Purvis, George D.; Bartlett, Rodney J.
- The Journal of Chemical Physics, Vol. 76, Issue 4
Many – Body Methods in Chemistry and Physics
book, January 2009
- Shavitt, Isaiah; Bartlett, Rodney J.
The Bravyi-Kitaev transformation for quantum computation of electronic structure
journal, December 2012
- Seeley, Jacob T.; Richard, Martin J.; Love, Peter J.
- The Journal of Chemical Physics, Vol. 137, Issue 22
Computation of Molecular Spectra on a Quantum Processor with an Error-Resilient Algorithm
journal, February 2018
- Colless, J. I.; Ramasesh, V. V.; Dahlen, D.
- Physical Review X, Vol. 8, Issue 1
Emulation of complex open quantum systems using superconducting qubits
journal, December 2016
- Mostame, Sarah; Huh, Joonsuk; Kreisbeck, Christoph
- Quantum Information Processing, Vol. 16, Issue 2
A variational eigenvalue solver on a photonic quantum processor
journal, July 2014
- Peruzzo, Alberto; McClean, Jarrod; Shadbolt, Peter
- Nature Communications, Vol. 5, Issue 1
Communication: An adaptive configuration interaction approach for strongly correlated electrons with tunable accuracy
journal, April 2016
- Schriber, Jeffrey B.; Evangelista, Francesco A.
- The Journal of Chemical Physics, Vol. 144, Issue 16
Heat-Bath Configuration Interaction: An Efficient Selected Configuration Interaction Algorithm Inspired by Heat-Bath Sampling
journal, August 2016
- Holmes, Adam A.; Tubman, Norm M.; Umrigar, C. J.
- Journal of Chemical Theory and Computation, Vol. 12, Issue 8
Electronic Absorption Spectra from MM and ab Initio QM/MM Molecular Dynamics: Environmental Effects on the Absorption Spectrum of Photoactive Yellow Protein
journal, September 2012
- Isborn, Christine M.; Götz, Andreas W.; Clark, Matthew A.
- Journal of Chemical Theory and Computation, Vol. 8, Issue 12
Atomistic non-adiabatic dynamics of the LH2 complex with a GPU-accelerated ab initio exciton model
journal, January 2017
- Sisto, Aaron; Stross, Clem; van der Kamp, Marc W.
- Physical Chemistry Chemical Physics, Vol. 19, Issue 23
Quantum Algorithm Providing Exponential Speed Increase for Finding Eigenvalues and Eigenvectors
journal, December 1999
- Abrams, Daniel S.; Lloyd, Seth
- Physical Review Letters, Vol. 83, Issue 24
Generalized Unitary Coupled Cluster Wave functions for Quantum Computation
journal, November 2018
- Lee, Joonho; Huggins, William J.; Head-Gordon, Martin
- Journal of Chemical Theory and Computation, Vol. 15, Issue 1
Communication: Approaching exact quantum chemistry by cluster analysis of full configuration interaction quantum Monte Carlo wave functions
journal, October 2018
- Deustua, J. Emiliano; Magoulas, Ilias; Shen, Jun
- The Journal of Chemical Physics, Vol. 149, Issue 15
On the Transformation of light into Heat in Solids. I
journal, January 1931
- Frenkel, J.
- Physical Review, Vol. 37, Issue 1
Density matrix formulation for quantum renormalization groups
journal, November 1992
- White, Steven R.
- Physical Review Letters, Vol. 69, Issue 19
The Density Matrix Renormalization Group in Quantum Chemistry
journal, May 2011
- Chan, Garnet Kin-Lic; Sharma, Sandeep
- Annual Review of Physical Chemistry, Vol. 62, Issue 1
Ab Initio Nonadiabatic Dynamics of Multichromophore Complexes: A Scalable Graphical-Processing-Unit-Accelerated Exciton Framework
journal, July 2014
- Sisto, Aaron; Glowacki, David R.; Martinez, Todd J.
- Accounts of Chemical Research, Vol. 47, Issue 9
Simulation of Many-Body Fermi Systems on a Universal Quantum Computer
journal, September 1997
- Abrams, Daniel S.; Lloyd, Seth
- Physical Review Letters, Vol. 79, Issue 13
Strategies for quantum computing molecular energies using the unitary coupled cluster ansatz
journal, October 2018
- Romero, Jonathan; Babbush, Ryan; McClean, Jarrod R.
- Quantum Science and Technology, Vol. 4, Issue 1
Adaptive Configuration Interaction for Computing Challenging Electronic Excited States with Tunable Accuracy
journal, October 2017
- Schriber, Jeffrey B.; Evangelista, Francesco A.
- Journal of Chemical Theory and Computation, Vol. 13, Issue 11
Gate-count estimates for performing quantum chemistry on small quantum computers
journal, August 2014
- Wecker, Dave; Bauer, Bela; Clark, Bryan K.
- Physical Review A, Vol. 90, Issue 2
Low-Scaling Quantum Chemistry Approach to Excited-State Properties via an ab Initio Exciton Model: Application to Excitation Energy Transfer in a Self-Assembled Nanotube
journal, October 2015
- Morrison, Adrian F.; Herbert, John M.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 21
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
Conical intersections and double excitations in time-dependent density functional theory
journal, March 2006
- Levine, Benjamin G.; Ko, Chaehyuk; Quenneville, Jason
- Molecular Physics, Vol. 104, Issue 5-7
Simulated Quantum Computation of Molecular Energies
journal, September 2005
- Aspuru-Guzik, A.
- Science, Vol. 309, Issue 5741
Fermion Monte Carlo without fixed nodes: A game of life, death, and annihilation in Slater determinant space
journal, January 2009
- Booth, George H.; Thom, Alex J. W.; Alavi, Ali
- The Journal of Chemical Physics, Vol. 131, Issue 5
Quantum simulator of an open quantum system using superconducting qubits: exciton transport in photosynthetic complexes
journal, October 2012
- Mostame, Sarah; Rebentrost, Patrick; Eisfeld, Alexander
- New Journal of Physics, Vol. 14, Issue 10
Studying light-harvesting models with superconducting circuits
journal, March 2018
- Potočnik, Anton; Bargerbos, Arno; Schröder, Florian A. Y. N.
- Nature Communications, Vol. 9, Issue 1
Quantum algorithms for fermionic simulations
journal, July 2001
- Ortiz, G.; Gubernatis, J. E.; Knill, E.
- Physical Review A, Vol. 64, Issue 2
Witnessing eigenstates for quantum simulation of Hamiltonian spectra
journal, January 2018
- Santagati, Raffaele; Wang, Jianwei; Gentile, Antonio A.
- Science Advances, Vol. 4, Issue 1
Barren plateaus in quantum neural network training landscapes
journal, November 2018
- McClean, Jarrod R.; Boixo, Sergio; Smelyanskiy, Vadim N.
- Nature Communications, Vol. 9, Issue 1
Optimal quantum circuits for general two-qubit gates
journal, March 2004
- Vatan, Farrokh; Williams, Colin
- Physical Review A, Vol. 69, Issue 3
Quantum Chemistry on Graphical Processing Units. 3. Analytical Energy Gradients, Geometry Optimization, and First Principles Molecular Dynamics
journal, August 2009
- Ufimtsev, Ivan S.; Martinez, Todd J.
- Journal of Chemical Theory and Computation, Vol. 5, Issue 10
The theory of variational hybrid quantum-classical algorithms
journal, February 2016
- McClean, Jarrod R.; Romero, Jonathan; Babbush, Ryan
- New Journal of Physics, Vol. 18, Issue 2
Fermionic Quantum Computation
journal, May 2002
- Bravyi, Sergey B.; Kitaev, Alexei Yu.
- Annals of Physics, Vol. 298, Issue 1
Density-Functional Theory for Time-Dependent Systems
journal, March 1984
- Runge, Erich; Gross, E. K. U.
- Physical Review Letters, Vol. 52, Issue 12
Studies in Configuration Interaction: The First-Row Diatomic Hydrides
journal, July 1969
- Bender, Charles F.; Davidson, Ernest R.
- Physical Review, Vol. 183, Issue 1
Hybrid quantum-classical hierarchy for mitigation of decoherence and determination of excited states
journal, April 2017
- McClean, Jarrod R.; Kimchi-Schwartz, Mollie E.; Carter, Jonathan
- Physical Review A, Vol. 95, Issue 4
Minimal universal two-qubit controlled-NOT-based circuits
journal, June 2004
- Shende, Vivek V.; Markov, Igor L.; Bullock, Stephen S.
- Physical Review A, Vol. 69, Issue 6
Ab Initio Implementation of the Frenkel–Davydov Exciton Model: A Naturally Parallelizable Approach to Computing Collective Excitations in Crystals and Aggregates
journal, November 2014
- Morrison, Adrian F.; You, Zhi-Qiang; Herbert, John M.
- Journal of Chemical Theory and Computation, Vol. 10, Issue 12
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Direct determination of effective Hamiltonians by wave-operator methods. II. Application to effective-spin interactions in -electron systems
journal, December 1983
- Maynau, D.; Durand, Ph.; Daudey, J. P.
- Physical Review A, Vol. 28, Issue 6
Communications: Survival of the fittest: Accelerating convergence in full configuration-interaction quantum Monte Carlo
journal, January 2010
- Cleland, Deidre; Booth, George H.; Alavi, Ali
- The Journal of Chemical Physics, Vol. 132, Issue 4
Highly efficient energy excitation transfer in light-harvesting complexes: The fundamental role of noise-assisted transport
journal, January 2009
- Caruso, F.; Chin, A. W.; Datta, A.
- The Journal of Chemical Physics, Vol. 131, Issue 10
Iterative perturbation calculations of ground and excited state energies from multiconfigurational zeroth‐order wavefunctions
journal, June 1973
- Huron, B.; Malrieu, J. P.; Rancurel, P.
- The Journal of Chemical Physics, Vol. 58, Issue 12
Dynamic Precision for Electron Repulsion Integral Evaluation on Graphical Processing Units (GPUs)
journal, March 2011
- Luehr, Nathan; Ufimtsev, Ivan S.; Martínez, Todd J.
- Journal of Chemical Theory and Computation, Vol. 7, Issue 4
On the Correlation Problem in Atomic and Molecular Systems. Calculation of Wavefunction Components in Ursell‐Type Expansion Using Quantum‐Field Theoretical Methods
journal, December 1966
- Čížek, Jiří
- The Journal of Chemical Physics, Vol. 45, Issue 11
Towards quantum chemistry on a quantum computer
journal, January 2010
- Lanyon, B. P.; Whitfield, J. D.; Gillett, G. G.
- Nature Chemistry, Vol. 2, Issue 2
Hardware-efficient variational quantum eigensolver for small molecules and quantum magnets
journal, September 2017
- Kandala, Abhinav; Mezzacapo, Antonio; Temme, Kristan
- Nature, Vol. 549, Issue 7671
Quantum Simulation of Electronic Structure with Linear Depth and Connectivity
journal, March 2018
- Kivlichan, Ian D.; McClean, Jarrod; Wiebe, Nathan
- Physical Review Letters, Vol. 120, Issue 11
Scalable Quantum Simulation of Molecular Energies
journal, July 2016
- O’Malley, P. J. J.; Babbush, R.; Kivlichan, I. D.
- Physical Review X, Vol. 6, Issue 3
Inhomogeneous Electron Gas
journal, March 1973
- Rajagopal, A. K.; Callaway, J.
- Physical Review B, Vol. 7, Issue 5
The theory of molecular excitons [Теория молекулярных экситонов]
journal, January 1964
- Davydov, A. S.
- Uspekhi Fizicheskih Nauk, Vol. 82, Issue 3
Studying light-harvesting models with superconducting circuits
text, January 2018
- Potočnik, Anton; Bargerbos, Arno; Schröder, Florian A. Y. N.
- ETH Zurich
Dephasing assisted transport: Quantum networks and biomolecules
text, January 2008
- Plenio, M. B.; Huelga, S. F.
- arXiv
Highly efficient energy excitation transfer in light-harvesting complexes: The fundamental role of noise-assisted transport
text, January 2009
- Caruso, Filippo; Chin, Alex W.; Datta, Animesh
- arXiv
Gate count estimates for performing quantum chemistry on small quantum computers
text, January 2013
- Wecker, Dave; Bauer, Bela; Clark, Bryan K.
- arXiv
Scalable Quantum Simulation of Molecular Energies
text, January 2015
- O'Malley, P. J. J.; Babbush, R.; Kivlichan, I. D.
- arXiv
Hybrid Quantum-Classical Hierarchy for Mitigation of Decoherence and Determination of Excited States
text, January 2016
- McClean, Jarrod R.; Schwartz, Mollie E.; Carter, Jonathan
- arXiv
Witnessing eigenstates for quantum simulation of Hamiltonian spectra
text, January 2016
- Santagati, R.; Wang, J.; Gentile, A. A.
- arXiv
Strategies for quantum computing molecular energies using the unitary coupled cluster ansatz
preprint, January 2017
- Romero, Jonathan; Babbush, Ryan; McClean, Jarrod R.
- arXiv
Studying Light-Harvesting Models with Superconducting Circuits
text, January 2017
- Potočnik, Anton; Bargerbos, Arno; Schröder, Florian A. Y. N.
- arXiv
Exact two-qubit universal quantum circuit
text, January 2002
- Zhang, Jun; Vala, Jiri; Sastry, Shankar
- arXiv
Optimal Quantum Circuits for General Two-Qubit Gates
text, January 2003
- Vatan, Farrokh; Williams, Colin
- arXiv
A quantum algorithm providing exponential speed increase for finding eigenvalues and eigenvectors
text, January 1998
- Abrams, Daniel S.; Lloyd, Seth
- arXiv
Works referencing / citing this record:
Decoding quantum errors with subspace expansions
journal, January 2020
- McClean, Jarrod R.; Jiang, Zhang; Rubin, Nicholas C.
- Nature Communications, Vol. 11, Issue 1
Quantum computational chemistry
text, January 2018
- McArdle, Sam; Endo, Suguru; Aspuru-Guzik, Alan
- arXiv
Decoding quantum errors with subspace expansions
text, January 2019
- McClean, Jarrod R.; Jiang, Zhang; Rubin, Nicholas C.
- arXiv