Multiple Quantum Coherences from Hyperfine Transitions in a Vanadium(IV) Complex
Abstract
We report a vanadium complex in a nuclear-spin free ligand field that displays two key properties for an ideal candidate qubit system: long coherence times that persist at high temperature, T2 = 1.2 μs at 80 K, and the observation of quantum coherences from multiple transitions. The electron paramagnetic resonance (EPR) spectrum of the complex [V(C8S8)3]2- displays multiple transitions arising from a manifold of states produced by the hyperfine coupling of the S = 1/2 electron spin and I = 7/2 nuclear spin. Transient nutation experiments reveal Rabi oscillations for multiple tran-sitions. These observations suggest that each pair of hyperfine levels hosted within [V(C8S8)3]2- are candidate qubits. The realization of multiple quantum coherences within a transition metal complex illustrates an emerging method of developing scalability and addressability in electron spin qubits. This study presents a rare molecular demonstration of multiple Rabi oscillations originating from separate transitions. These results extend observations of multiple quantum coherences from prior reports in solid-state compounds to the new realm of highly modifiable coordination compounds.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Div.
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1596783
- Alternate Identifier(s):
- OSTI ID: 1657172
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 136; Journal Issue: 45; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Qubit; rabi oscillations; quantum; ligands; oscillation; electron paramagnetic resonance spectroscopy; quantum mechanics; nuclear spin
Citation Formats
Zadrozny, Joseph M., Niklas, Jens, Poluektov, Oleg G., and Freedman, Danna E. Multiple Quantum Coherences from Hyperfine Transitions in a Vanadium(IV) Complex. United States: N. p., 2014.
Web. doi:10.1021/ja507846k.
Zadrozny, Joseph M., Niklas, Jens, Poluektov, Oleg G., & Freedman, Danna E. Multiple Quantum Coherences from Hyperfine Transitions in a Vanadium(IV) Complex. United States. https://doi.org/10.1021/ja507846k
Zadrozny, Joseph M., Niklas, Jens, Poluektov, Oleg G., and Freedman, Danna E. Thu .
"Multiple Quantum Coherences from Hyperfine Transitions in a Vanadium(IV) Complex". United States. https://doi.org/10.1021/ja507846k. https://www.osti.gov/servlets/purl/1596783.
@article{osti_1596783,
title = {Multiple Quantum Coherences from Hyperfine Transitions in a Vanadium(IV) Complex},
author = {Zadrozny, Joseph M. and Niklas, Jens and Poluektov, Oleg G. and Freedman, Danna E.},
abstractNote = {We report a vanadium complex in a nuclear-spin free ligand field that displays two key properties for an ideal candidate qubit system: long coherence times that persist at high temperature, T2 = 1.2 μs at 80 K, and the observation of quantum coherences from multiple transitions. The electron paramagnetic resonance (EPR) spectrum of the complex [V(C8S8)3]2- displays multiple transitions arising from a manifold of states produced by the hyperfine coupling of the S = 1/2 electron spin and I = 7/2 nuclear spin. Transient nutation experiments reveal Rabi oscillations for multiple tran-sitions. These observations suggest that each pair of hyperfine levels hosted within [V(C8S8)3]2- are candidate qubits. The realization of multiple quantum coherences within a transition metal complex illustrates an emerging method of developing scalability and addressability in electron spin qubits. This study presents a rare molecular demonstration of multiple Rabi oscillations originating from separate transitions. These results extend observations of multiple quantum coherences from prior reports in solid-state compounds to the new realm of highly modifiable coordination compounds.},
doi = {10.1021/ja507846k},
journal = {Journal of the American Chemical Society},
number = 45,
volume = 136,
place = {United States},
year = {Thu Oct 23 00:00:00 EDT 2014},
month = {Thu Oct 23 00:00:00 EDT 2014}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 63 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:
Simulating physics with computers
journal, June 1982
- Feynman, Richard P.
- International Journal of Theoretical Physics, Vol. 21, Issue 6-7
Simulated Quantum Computation of Molecular Energies
journal, September 2005
- Aspuru-Guzik, A.
- Science, Vol. 309, Issue 5741
Simulating Chemistry Using Quantum Computers
journal, May 2011
- Kassal, Ivan; Whitfield, James D.; Perdomo-Ortiz, Alejandro
- Annual Review of Physical Chemistry, Vol. 62, Issue 1
Finding low-energy conformations of lattice protein models by quantum annealing
journal, August 2012
- Perdomo-Ortiz, Alejandro; Dickson, Neil; Drew-Brook, Marshall
- Scientific Reports, Vol. 2, Issue 1
Molecular routes for spin cluster qubits
journal, January 2006
- Affronte, Marco; Troiani, Filippo; Ghirri, Alberto
- Dalton Transactions, Issue 23
Molecular spins for quantum information technologies
journal, January 2011
- Troiani, Filippo; Affronte, Marco
- Chemical Society Reviews, Vol. 40, Issue 6
Design of magnetic coordination complexes for quantum computing
journal, January 2012
- Aromí, Guillem; Aguilà, David; Gamez, Patrick
- Chem. Soc. Rev., Vol. 41, Issue 2
Rare-earth solid-state qubits
journal, January 2007
- Bertaina, S.; Gambarelli, S.; Tkachuk, A.
- Nature Nanotechnology, Vol. 2, Issue 1
Coherent Manipulation of Electron Spins up to Ambient Temperatures in Doped
journal, September 2007
- Nellutla, S.; Choi, K. -Y.; Pati, M.
- Physical Review Letters, Vol. 99, Issue 13
Spin-Orbit Qubits of Rare-Earth-Metal Ions in Axially Symmetric Crystal Fields
journal, November 2009
- Bertaina, S.; Shim, J. H.; Gambarelli, S.
- Physical Review Letters, Vol. 103, Issue 22
Multiphoton Coherent Manipulation in Large-Spin Qubits
journal, February 2009
- Bertaina, S.; Chen, L.; Groll, N.
- Physical Review Letters, Vol. 102, Issue 5
A quantum memory intrinsic to single nitrogen–vacancy centres in diamond
journal, June 2011
- Fuchs, G. D.; Burkard, G.; Klimov, P. V.
- Nature Physics, Vol. 7, Issue 10
Quantum control of hybrid nuclear–electronic qubits
journal, December 2012
- Morley, Gavin W.; Lueders, Petra; Hamed Mohammady, M.
- Nature Materials, Vol. 12, Issue 2
Direct Observation of Quantum Coherence in Single-Molecule Magnets
journal, October 2008
- Schlegel, C.; van Slageren, J.; Manoli, M.
- Physical Review Letters, Vol. 101, Issue 14
Quantum oscillations in a molecular magnet
journal, May 2008
- Bertaina, S.; Gambarelli, S.; Mitra, T.
- Nature, Vol. 453, Issue 7192
Electron spin–lattice and spin–spin relaxation study of a trinuclear iron( iii ) complex and its relevance in quantum computing
journal, January 2008
- Mitrikas, George; Sanakis, Yiannis; Raptopoulou, Catherine P.
- Phys. Chem. Chem. Phys., Vol. 10, Issue 5
Coherent Manipulation and Decoherence of Single-Molecule Magnets
journal, February 2009
- Takahashi, Susumu; van Tol, Johan; Beedle, Christopher C.
- Physical Review Letters, Vol. 102, Issue 8
Molecular Prototypes for Spin-Based CNOT and SWAP Quantum Gates
journal, September 2011
- Luis, F.; Repollés, A.; Martínez-Pérez, M. J.
- Physical Review Letters, Vol. 107, Issue 11
Spin decoherence in an iron-based magnetic cluster
journal, November 2011
- Wang, Zhenxing; Datta, Saiti; Papatriantafyllopoulou, Constantina
- Polyhedron, Vol. 30, Issue 18
Observing Quantum Oscillation of Ground States in Single Molecular Magnet
journal, June 2012
- Yang, Jiahui; Wang, Ya; Wang, Zixiang
- Physical Review Letters, Vol. 108, Issue 23
Chemical Engineering of Molecular Qubits
journal, March 2012
- Wedge, C. J.; Timco, G. A.; Spielberg, E. T.
- Physical Review Letters, Vol. 108, Issue 10
Heterodimetallic [LnLn′] Lanthanide Complexes: Toward a Chemical Design of Two-Qubit Molecular Spin Quantum Gates
journal, August 2014
- Aguilà, David; Barrios, Leoní A.; Velasco, Verónica
- Journal of the American Chemical Society, Vol. 136, Issue 40
Spin-based quantum computers made by chemistry: hows and whys
journal, January 2009
- Stamp, Philip C. E.; Gaita-Ariño, Alejandro
- J. Mater. Chem., Vol. 19, Issue 12
Decoherence in crystals of quantum molecular magnets
journal, July 2011
- Takahashi, S.; Tupitsyn, I. S.; van Tol, J.
- Nature, Vol. 476, Issue 7358
Gd-Based Single-Ion Magnets with Tunable Magnetic Anisotropy: Molecular Design of Spin Qubits
journal, June 2012
- Martínez-Pérez, M. J.; Cardona-Serra, S.; Schlegel, C.
- Physical Review Letters, Vol. 108, Issue 24
Coherent manipulation of spin qubits based on polyoxometalates: the case of the single ion magnet [GdW30P5O110]14−
journal, January 2013
- Baldoví, José J.; Cardona-Serra, Salvador; Clemente-Juan, Juan M.
- Chemical Communications, Vol. 49, Issue 79
Potential for spin-based information processing in a thin-film molecular semiconductor
journal, October 2013
- Warner, Marc; Din, Salahud; Tupitsyn, Igor S.
- Nature, Vol. 503, Issue 7477
Influence of Electronic Spin and Spin–Orbit Coupling on Decoherence in Mononuclear Transition Metal Complexes
journal, May 2014
- Graham, Michael J.; Zadrozny, Joseph M.; Shiddiq, Muhandis
- Journal of the American Chemical Society, Vol. 136, Issue 21
Coherence window in the dynamics of quantum nanomagnets
journal, January 2004
- Stamp, P. C. E.; Tupitsyn, I. S.
- Physical Review B, Vol. 69, Issue 1
Pairwise Decoherence in Coupled Spin Qubit Networks
journal, November 2006
- Morello, Andrea; Stamp, P. C. E.; Tupitsyn, Igor S.
- Physical Review Letters, Vol. 97, Issue 20
A New Honeycomb Assemblage of a Trisdithiolene Vanadium(IV) Complex, (PPh 4 ) 2 [V(dbddto) 3 ](C 6 H 4 Cl 2 )(hexane) 0.5
journal, January 2006
- Okubo, Takashi; Maeda, Ryoko; Kondo, Mitsuru
- Chemistry Letters, Vol. 35, Issue 1
EasySpin, a comprehensive software package for spectral simulation and analysis in EPR
journal, January 2006
- Stoll, Stefan; Schweiger, Arthur
- Journal of Magnetic Resonance, Vol. 178, Issue 1, p. 42-55
Formation and structure of the tris(catecholato)vanadate(IV) complex in aqueous solution
journal, April 1990
- Branca, Mario; Micera, Giovanni; Dessi, Alessandro
- Inorganic Chemistry, Vol. 29, Issue 8
Molecular and Electronic Structure of Octahedral o -Aminophenolato and o -Iminobenzosemiquinonato Complexes of V(V), Cr(III), Fe(III), and Co(III). Experimental Determination of Oxidation Levels of Ligands and Metal Ions
journal, August 2001
- Chun, Hyungphil; Verani, Claudio Nazari; Chaudhuri, Phalguni
- Inorganic Chemistry, Vol. 40, Issue 17
One- and Two-Electron Reduced 1,2-Diketone Ligands in [Cr III (L • ) 3 ] ( S = 0) and Na 2 (Et 2 O) 2 [V IV (L Red ) 3 ] ( S = 1 / 2 )
journal, December 2008
- Spikes, Geoffrey H.; Sproules, Stephen; Bill, Eckhard
- Inorganic Chemistry, Vol. 47, Issue 23
Single-crystal electron paramagnetic resonance study of a trigonal vanadium tris(dithiolate) complex
journal, October 1973
- Kwik, Whei Lu; Stiefel, Edward I.
- Inorganic Chemistry, Vol. 12, Issue 10
In(III), Tl(III) and V(IV) tris-chelates of the heterocyclic dithiolene and diselenolene ligands 1,3-dithiole-2-thione-4,5-dithiolate (dmit), 1,2-dithiole-3-thione-4,5-dithiolate (dmt) and 1,3-diselenole-2-selone-4,5-diselenolate (dsis). Crystal and molecular structure of (Bu4N)2 [V(dmt)3]
journal, April 1987
- Olk, Ruth-Maria; Dietzsch, W.; Kirmse, R.
- Inorganica Chimica Acta, Vol. 128, Issue 2
Spectroscopic and electrical properties of VO(dmit)2 and V(dmit)3 anion complexes and x-ray crystal structure of [NMP]2[V(dmit)3] (dmit = 2-thioxo-1,3-dithiole-4,5-dithiolate, NMP = N-methylphenazinium)
journal, December 1988
- Matsubayashi, Genetsu; Akiba, Kazuki; Tanaka, Toshio
- Inorganic Chemistry, Vol. 27, Issue 26
Six-Membered Electron Transfer Series [V(dithiolene) 3 ] z ( z = 1+, 0, 1−, 2−, 3−, 4−). An X-ray Absorption Spectroscopic and Density Functional Theoretical Study
journal, June 2010
- Sproules, Stephen; Weyhermüller, Thomas; DeBeer, Serena
- Inorganic Chemistry, Vol. 49, Issue 11
Works referencing / citing this record:
Coherent coupling between Vanadyl Phthalocyanine spin ensemble and microwave photons: towards integration of molecular spin qubits into quantum circuits
journal, October 2017
- Bonizzoni, C.; Ghirri, A.; Atzori, M.
- Scientific Reports, Vol. 7, Issue 1
A flexible iron( ii ) complex in which zero-field splitting is resistant to structural variation
journal, January 2016
- Zadrozny, Joseph M.; Greer, Samuel M.; Hill, Stephen
- Chemical Science, Vol. 7, Issue 1
Giant spin–phonon bottleneck effects in evaporable vanadyl-based molecules with long spin coherence
journal, January 2016
- Tesi, L.; Lunghi, A.; Atzori, M.
- Dalton Transactions, Vol. 45, Issue 42
A concentrated array of copper porphyrin candidate qubits
journal, January 2019
- Yu, Chung-Jui; Krzyaniak, Matthew D.; Fataftah, Majed S.
- Chemical Science, Vol. 10, Issue 6
Synthetic Hilbert Space Engineering of Molecular Qu d its: Isotopologue Chemistry
journal, February 2019
- Wernsdorfer, Wolfgang; Ruben, Mario
- Advanced Materials, Vol. 31, Issue 26
Molecular spin qudits for quantum algorithms
journal, January 2018
- Moreno-Pineda, Eufemio; Godfrin, Clément; Balestro, Franck
- Chemical Society Reviews, Vol. 47, Issue 2
Counterion influence on dynamic spin properties in a V( iv ) complex
journal, January 2019
- Lin, Chun-Yi; Ngendahimana, Thacien; Eaton, Gareth R.
- Chemical Science, Vol. 10, Issue 2
Quantum coherence in a processable vanadyl complex: new tools for the search of molecular spin qubits
journal, January 2016
- Tesi, Lorenzo; Lucaccini, Eva; Cimatti, Irene
- Chemical Science, Vol. 7, Issue 3
Ligand Radicals as Modular Organic Electron Spin Qubits
journal, November 2018
- McGuire, Jake; Miras, Haralampos N.; Donahue, James P.
- Chemistry - A European Journal, Vol. 24, Issue 66
Novel Topologies in Vanadium-bis-β-Diketone Chemistry: A [V4] and a [V6] Metallacyclophane
journal, December 2015
- Borilovic, Ivana; Roubeau, Olivier; Fernández Vidal, Irene
- Magnetochemistry, Vol. 1, Issue 1
Chromium( iii )-based potential molecular quantum bits with long coherence times
journal, January 2019
- Lenz, Samuel; Bamberger, Heiko; Hallmen, Philipp P.
- Physical Chemistry Chemical Physics, Vol. 21, Issue 13
Nuclear Spin Isomers: Engineering a Et 4 N[DyPc 2 ] Spin Qudit
journal, July 2017
- Moreno-Pineda, Eufemio; Damjanović, Marko; Fuhr, Olaf
- Angewandte Chemie International Edition, Vol. 56, Issue 33
Vanadyl dithiolate single molecule transistors: the next spintronic frontier?
journal, January 2018
- Cardona-Serra, S.; Gaita-Ariño, A.
- Dalton Transactions, Vol. 47, Issue 16
Molecules Designed to Contain Two Weakly Coupled Spins with a Photoswitchable Spacer
journal, August 2017
- Uber, Jorge Salinas; Estrader, Marta; Garcia, Jordi
- Chemistry - A European Journal, Vol. 23, Issue 55
Field-induced slow magnetic relaxation in low-spin S = 1/2 mononuclear osmium( v ) complexes
journal, January 2020
- Su, Qian-Qian; Fan, Kun; Huang, Xin-Da
- Dalton Transactions, Vol. 49, Issue 13
The Rise of Single-Ion Magnets as Spin Qubits
journal, November 2016
- Ding, You-Song; Deng, Yi-Fei; Zheng, Yan-Zhen
- Magnetochemistry, Vol. 2, Issue 4
Progress towards creating optically addressable molecular qubits
journal, January 2018
- Fataftah, Majed S.; Freedman, Danna E.
- Chemical Communications, Vol. 54, Issue 98
Nuclear Spin Isomers: Engineering a Et 4 N[DyPc 2 ] Spin Qudit
journal, July 2017
- Moreno‐Pineda, Eufemio; Damjanović, Marko; Fuhr, Olaf
- Angewandte Chemie, Vol. 129, Issue 33
Synthetic Hilbert Space Engineering of Molecular Qudits: Isotopologue Chemistry
text, January 2019
- Wernsdorfer, W.; Ruben, M.
- Karlsruhe
Molecular Spin Qudits for Quantum Algorithms
text, January 2017
- Moreno-Pineda, Eufemio; Godfrin, Clément; Balestro, Franck
- arXiv
Millisecond Coherence Time in a Tunable Molecular Electronic Spin Qubit
journal, December 2015
- Zadrozny, Joseph M.; Niklas, Jens; Poluektov, Oleg G.
- ACS Central Science, Vol. 1, Issue 9
Toward the Quantum Computer: Magnetic Molecules Back in the Race
journal, December 2015
- Sessoli, Roberta
- ACS Central Science, Vol. 1, Issue 9
Storage and retrieval of microwave pulses with molecular spin ensembles
journal, August 2020
- Bonizzoni, Claudio; Ghirri, Alberto; Santanni, Fabio
- npj Quantum Information, Vol. 6, Issue 1
Coherent coupling between Vanadyl Phthalocyanine spin ensemble and microwave photons: towards integration of molecular spin qubits into quantum circuits
journal, October 2017
- Bonizzoni, C.; Ghirri, A.; Atzori, M.
- Scientific Reports, Vol. 7, Issue 1
Quantum coherence in a processable vanadyl complex: new tools for the search of molecular spin qubits
journal, January 2016
- Tesi, Lorenzo; Lucaccini, Eva; Cimatti, Irene
- Chemical Science, Vol. 7, Issue 3
Mapping Magnetic Properties and Relaxation in Vanadium(IV) Complexes with Lanthanides by Electron Paramagnetic Resonance
journal, December 2019
- Kurganskii, Ivan V.; Bazhina, Evgeniya S.; Korlyukov, Alexander A.
- Molecules, Vol. 24, Issue 24