Millisecond Coherence Time in a Tunable Molecular Electronic Spin Qubit

Zadrozny, Joseph M.; Niklas, Jens; Poluektov, Oleg G.; Freedman, Danna E.

doi:10.1021/acscentsci.5b00338

Title: Millisecond Coherence Time in a Tunable Molecular Electronic Spin Qubit

Full Record
Other Related Research

Abstract

Here, quantum information processing (QIP) could revolutionize areas ranging from chemical modeling to cryptography. One key figure of merit for the smallest unit for QIP, the qubit, is the coherence time (T₂), which establishes the lifetime for the qubit. Transition metal complexes offer tremendous potential as tunable qubits, yet their development is hampered by the absence of synthetic design principles to achieve a long T₂. We harnessed molecular design to create a series of qubits, (Ph₄P)₂[V(C₈S₈)₃] (1), (Ph₄P)₂[V(β-C₃S₅)₃] (2), (Ph₄P)₂[V(α-C₃S₅)₃] (3), and (Ph₄P)₂[V(C₃S₄O)₃] (4), with T₂s of 1–4 μs at 80 K in protiated and deuterated environments. Crucially, through chemical tuning of nuclear spin content in the vanadium(IV) environment we realized a T₂ of ~1 ms for the species (d₂₀-Ph₄P)₂[V(C₈S₈)₃] in CS₂, a value that surpasses the coordination complex record by an order of magnitude. This value even eclipses some prominent solid-state qubits. Electrochemical and continuous wave electron paramagnetic resonance (EPR) data reveal variation in the electronic influence of the ligands on the metal ion across 1–4. However, pulsed measurements indicate that the most important influence on decoherence is nuclear spins in the protiated and deuterated solvents utilized herein. Our results illuminate a path forward in synthetic design principles, whichmore »« less

Authors:

Zadrozny, Joseph M. ^[1]; Niklas, Jens ^[2]; Poluektov, Oleg G. ^[2]; Freedman, Danna E. ^[1]

Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439, United States

Publication Date:: Wed Dec 02 00:00:00 EST 2015

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

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

OSTI Identifier:: 1227593

Alternate Identifier(s):: OSTI ID: 1351545

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Published Article

Journal Name:: ACS Central Science

Additional Journal Information:: Journal Name: ACS Central Science Journal Volume: 1 Journal Issue: 9; Journal ID: ISSN 2374-7943

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Zadrozny, Joseph M., Niklas, Jens, Poluektov, Oleg G., and Freedman, Danna E. Millisecond Coherence Time in a Tunable Molecular Electronic Spin Qubit.  United States: N. p., 2015. 
Web.  doi:10.1021/acscentsci.5b00338.

Copy to clipboard


                    Zadrozny, Joseph M., Niklas, Jens, Poluektov, Oleg G., & Freedman, Danna E. Millisecond Coherence Time in a Tunable Molecular Electronic Spin Qubit.  United States.  https://doi.org/10.1021/acscentsci.5b00338

Copy to clipboard


                    Zadrozny, Joseph M., Niklas, Jens, Poluektov, Oleg G., and Freedman, Danna E. Wed .  
"Millisecond Coherence Time in a Tunable Molecular Electronic Spin Qubit".  United States.  https://doi.org/10.1021/acscentsci.5b00338.

Copy to clipboard


                    
@article{osti_1227593,

  title        = {Millisecond Coherence Time in a Tunable Molecular Electronic Spin Qubit},

  author       = {Zadrozny, Joseph M. and Niklas, Jens and Poluektov, Oleg G. and Freedman, Danna E.},

  abstractNote = {Here, quantum information processing (QIP) could revolutionize areas ranging from chemical modeling to cryptography. One key figure of merit for the smallest unit for QIP, the qubit, is the coherence time (T2), which establishes the lifetime for the qubit. Transition metal complexes offer tremendous potential as tunable qubits, yet their development is hampered by the absence of synthetic design principles to achieve a long T2. We harnessed molecular design to create a series of qubits, (Ph4P)2[V(C8S8)3] (1), (Ph4P)2[V(β-C3S5)3] (2), (Ph4P)2[V(α-C3S5)3] (3), and (Ph4P)2[V(C3S4O)3] (4), with T2s of 1–4 μs at 80 K in protiated and deuterated environments. Crucially, through chemical tuning of nuclear spin content in the vanadium(IV) environment we realized a T2 of ~1 ms for the species (d20-Ph4P)2[V(C8S8)3] in CS2, a value that surpasses the coordination complex record by an order of magnitude. This value even eclipses some prominent solid-state qubits. Electrochemical and continuous wave electron paramagnetic resonance (EPR) data reveal variation in the electronic influence of the ligands on the metal ion across 1–4. However, pulsed measurements indicate that the most important influence on decoherence is nuclear spins in the protiated and deuterated solvents utilized herein. Our results illuminate a path forward in synthetic design principles, which should unite CS2 solubility with nuclear spin free ligand fields to develop a new generation of molecular qubits.},

  doi          = {10.1021/acscentsci.5b00338},

  journal      = {ACS Central Science},

  number       = 9,

  volume       = 1,

  place        = {United States},

  year         = {Wed Dec 02 00:00:00 EST 2015},

  month        = {Wed Dec 02 00:00:00 EST 2015}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Publisher's Version of Record
https://doi.org/10.1021/acscentsci.5b00338

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 236 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Similar Records in DOE PAGES and OSTI.GOV collections:

Long coherence times in nuclear spin-free vanadyl qubits

Journal Article Yu, Chung -Jui ; Graham, Michael J. ; Zadrozny, Joseph M. ; ... - Journal of the American Chemical Society

Quantum information processing (QIP) offers the potential to create new frontiers in fields ranging from quantum biology to cryptography. Two key figures of merit for electronic spin qubits, the smallest units of QIP, are the coherence time (T₂), the lifetime of the qubit, and the spin–lattice relaxation time (T₁), the thermally defined upper limit of T₂. To achieve QIP, processable qubits with long coherence times are required. Recent studies on (Ph₄P-d₂₀)₂[V(C₈S₈)₃], a vanadium-based qubit, demonstrate that millisecond T₂ times are achievable in transition metal complexes with nuclear spinfree environments. Applying these principles to vanadyl complexes offers a route to combinemore »« less
Cited by 92
https://doi.org/10.1021/jacs.6b08467

Full Text Available
Synthesis of new chiral ferrocenyl amine sulfide complexes and their applications as asymmetric catalysts. The structure of (R,S)-C/sub 5/H/sub 5/FeC/sub 5/H/sub 3/(CHMeNMe/sub 2/)(SCH/sub 3/)(PdCl/sub 2/)

Journal Article Okoroafor, M O ; Ward, D L ; Brubaker, Jr, C H - Organometallics; (United States)

New chiral ferrocenyl sulfide ligands of the type (R,S)-C/sub 5/H/sub 5/FeC/sub 5/H/sub 3/(CHMeNMe/sub 2/)(SR), where R = Me, Et, i-Pr, n-Bu, i-Bu, t-Bu, i-Pent, Ph, CH/sub 2/Ph, p-tolyl, or 4-chlorophenyl, have been prepared by lithiation of optically active N,N-dimethyl-1-ferrocenylethylamine followed by reaction with appropriate disulfide. These compounds are air-stable and readily chelate palladium and platinum chloride to form chiral heterobimetallic complexes (R,S)-C/sub 5/H/sub 5/FeC/sub 5/H/sub 3/(CHMeNMe/sub 2/)(SR)(MCl/sub 2/) (R = Me, i-Pr, n-Pr, i-Bu, Ph, p-tolyl, 4-chlorophenyl; M = Pd,Pt). Both the ligands and the complexes were characterized by /sup 1/H and /sup 13/C NMR spectroscopy, mass spectrometry, and infraredmore »« less
https://doi.org/10.1021/om00097a009
Si and SiGe based double top gated accumulation mode single electron transistors for quantum bits.

Conference Wendt, Joel Robert ; Ten Eyck, Gregory A ; Childs, Kenton David ; ...

There is significant interest in forming quantum bits (qubits) out of single electron devices for quantum information processing (QIP). Information can be encoded using properties like charge or spin. Spin is appealing because it is less strongly coupled to the solid-state environment so it is believed that the quantum state can better be preserved over longer times (i.e., that is longer decoherence times may be achieved). Long spin decoherence times would allow more complex qubit operations to be completed with higher accuracy. Recently spin qubits were demonstrated by several groups using electrostatically gated modulation doped GaAs double quantum dots (DQD)more »« less
Spin-chemical effects on intramolecular photoinduced charge transfer reactions in bisphenanthroline copper( i )-viologen dyad assemblies

Journal Article Lazorski, Megan S. ; Schapiro, Igor ; Gaddie, Ross S. ; ... - Chemical Science

Two covalently linked donor–acceptor copper phenanthroline complexes (C–A dyads) of interest for solar energy conversion/storage schemes, [Cu(I)(^Rphen(OMV)₂⁴⁺)₂]⁹⁺ = ^RC⁺A₄⁸⁺ with ^RC⁺ = [Cu(I)^Rphen₂]⁺ involving 2,9-methyl (R = Me) or 2,9-phenyl (R = Ph)-phenanthroline ligands that are 5,6-disubstituted by 4-(n-butoxy) linked methylviologen electron acceptor groups (A²⁺ = OMV²⁺), have been synthesized and investigated via quantum chemical calculations and nanosecond laser flash spectroscopy in 1,2-difluorobenzene/methanol (dfb/MeOH) mixtures. Upon photoexcitation, charge transfer (CT) states ^RC²⁺A⁺A₃⁶⁺ are formed in less than one ns and decay by charge recombination on a time scale of 6–45 ns. The CT lifetime of ^RC²⁺A⁺A₃⁶⁺ has a strong dependencemore »« less
https://doi.org/10.1039/D0SC00830C
Molecular structures of tris(1- tert -butyl-2-mercaptoimidazolyl)hydroborate complexes of titanium, zirconium and hafnium

Journal Article Rong, Yi ; Sambade, David ; Parkin, Gerard - Acta Crystallographica. Section C, Structural Chemistry (Online)

Cyclopentadienyl and tris(pyrazolyl)hydroborate have found much use as supporting ligands in the chemistry of titanium, zirconium and hafnium, especially with respect to applications involving olefin polymerization catalysis. In contrast, closely related tris(1-alkyl-2-mercaptoimidazolyl)hydroborate, [Tm^R], ligands have so far found little application to the chemistry of these elements, despite the fact that such ligands are currently used extensively in coordination chemistry. In view of the fact that a substituent in the 2-position exerts a direct influence on the steric environment of the metal center, we report here the application of the sterically demanding tris(1-tert-butyl-2-mercaptoimidazolyl)hydroborate [Tm^{{\rm Bu}^{\rm t}}] ligand to these metals. Dichlorido(η⁵-cyclopentadienyl)[tris(1-tert-butyl-2-sulfanylidene-2,3-dihydro-1H-imidazol-3-yl)borato-κ³S,S',H]zirconium(IV)more »« less
https://doi.org/10.1107/s2053229616008925

Similar Records