Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) 2 ] 2

doi:10.1021/acs.inorgchem.6b03097

Title: Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) ₂ ] ₂

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Abstract

Diamond anvil cell techniques, synchrotron-based infrared and Raman spectroscopies, and lattice dynamics calculations are combined with prior magnetic property work to reveal the pressure–temperature phase diagram of Co[N(CN)2]2. The second-order structural boundaries converge on key areas of activity involving the spin state exposing how the pressure-induced local lattice distortions trigger the ferromagnetic → antiferromagnetic transition in this quantum material.

Authors:

; O’Neal, K. R. ^[1]; Brinzari, T. V. ^[1]; Chen, P. ^[1]; Schlueter, J. A. ^[2]; Manson, J. L. ^[3]; Litvinchuk, A. P. ^[4]; Liu, Z. ^[5]

Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States
Division of Materials Research, National Science Foundation, Arlington, Virginia 22230, United States
Department of Chemistry and Biochemistry, Eastern Washington University, Cheney, Washington 99004, United States
Texas Center for Superconductivity and Department of Physics, University of Houston, Houston, Texas 77204, United States
Geophysical Laboratory, Carnegie Institution of Washington, Washington, D.C. 20015, United States

Publication Date:: Fri Apr 07 00:00:00 EDT 2017

Research Org.:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI Identifier:: 1409589

Report Number(s):: BNL-114641-2017-JA¿¿¿
Journal ID: ISSN 0020-1669

DOE Contract Number:: SC0012704

Resource Type:: Journal Article

Resource Relation:: Journal Name: Inorganic Chemistry; Journal Volume: 56; Journal Issue: 9

Country of Publication:: United States

Language:: English

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

Citation Formats


                    Musfeldt, J. L., O’Neal, K. R., Brinzari, T. V., Chen, P., Schlueter, J. A., Manson, J. L., Litvinchuk, A. P., and Liu, Z.. Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) 2 ] 2.  United States: N. p., 2017. 
        Web.  doi:10.1021/acs.inorgchem.6b03097.

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                    Musfeldt, J. L., O’Neal, K. R., Brinzari, T. V., Chen, P., Schlueter, J. A., Manson, J. L., Litvinchuk, A. P., & Liu, Z.. Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) 2 ] 2.  United States.  doi:10.1021/acs.inorgchem.6b03097.

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                    Musfeldt, J. L., O’Neal, K. R., Brinzari, T. V., Chen, P., Schlueter, J. A., Manson, J. L., Litvinchuk, A. P., and Liu, Z.. Fri .  
        "Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) 2 ] 2".  United States.  
        doi:10.1021/acs.inorgchem.6b03097.

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@article{osti_1409589,

  title        = {Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) 2 ] 2},

  author       = {Musfeldt, J. L. and O’Neal, K. R. and Brinzari, T. V. and Chen, P. and Schlueter, J. A. and Manson, J. L. and Litvinchuk, A. P. and Liu, Z.},

  abstractNote = {Diamond anvil cell techniques, synchrotron-based infrared and Raman spectroscopies, and lattice dynamics calculations are combined with prior magnetic property work to reveal the pressure–temperature phase diagram of Co[N(CN)2]2. The second-order structural boundaries converge on key areas of activity involving the spin state exposing how the pressure-induced local lattice distortions trigger the ferromagnetic → antiferromagnetic transition in this quantum material.},

  doi          = {10.1021/acs.inorgchem.6b03097},

  journal      = {Inorganic Chemistry},

  number       = 9,

  volume       = 56,

  place        = {United States},

  year         = {Fri Apr 07 00:00:00 EDT 2017},

  month        = {Fri Apr 07 00:00:00 EDT 2017}

}

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Journal Article:

DOI: 10.1021/acs.inorgchem.6b03097

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Pressure-temperature phase diagram, inverse isotope effect, and superconductivity in excess of 13 K in. kappa. -(BEDT-TTF) sub 2 Cu(N(CN) sub 2 )Cl, where BEDT-TTF is bis(ethylenedithio)tetrathiafulvalene

Schirber, J.E. ; Overmyer, D.L. ; Carlson, K.D. ; ... - Physical Review, B: Condensed Matter; (United States)

The pressure-temperature phase diagram of the highest-{ital T}{sub {ital c}} organic superconductor, {kappa}-(BEDT-TTF){sub 2}Cu(N(CN){sub 2})Cl is determined, where BEDT-TTF is bis(ethylenedithio)tetrathiafulvalene. Semiconducting, insulating, metallic, and superconducting regimes are seen at pressures below 1 kbar. Superconductivity at 12.5 K and 0.3 kbar {ital increases} by 0.5--1.5 K upon deuteration of BEDT-TTF, in striking contrast to the normal isotope effect determined previously for {kappa}-(BEDT-TTF){sub 2}Cu(N(CN){sub 2})Br.
DOI: 10.1103/PhysRevB.44.4666
Evidence for structural and electronic instabilities at intermediate temperatures in K-(BEDT-TTF){sub 2}X for X=Cu[N(CN){sub 2}]Cl, Cu[N(CN){sub 2}]Br and Cu(NCS){sub 2} : implications for the phase diagram of these quasi-2D organic superconductors.

Muller, J. ; Lang, M. ; Steglich, F. ; ... - Phys. Rev. B

We present high-resolution measurements of the coefficient of thermal expansion {alpha}(T)={partial_derivative} ln l(T)/{partial_derivative}T of the quasi-two-dimensional (quasi-2D) salts {kappa}-(BEDT-TTF){sub 2}X with X=Cu[N(CN){sub 2}]Cl, Cu[N(CN){sub 2}]Br and Cu(NCS){sub 2} in the temperature range T<{approx}150 K. Three distinct kinds of anomalies corresponding to different temperature ranges have been identified. These are (A) phase-transition anomalies into the superconducting (X=Cu(NCS){sub 2}, Cu[N(CN){sub 2}]Br) and antiferromagnetic (X=Cu[N(CN){sub 2}]Cl) ground state, (B) phase-transition-like anomalies at intermediate temperatures (30-50) K for the superconducting salts, and (C) kinetic, glasslike transitions at higher temperatures, i.e., (70-80) K for all compounds. By a thermodynamic analysis of the discontinuities at themore »« less
DOI: 10.1103/PhysRevB.65.144521
Lattice effects and entropy release at the low-temperature phase transition in the spin-liquid candidate kappa-(BEDT-TTF){sub 2}Cu{sub 2}(CN){sub 3}.

Manna, R. S. ; de Souza, M. ; Bruhl, A. ; ... - Phys. Rev. Lett.

The spin-liquid candidate {kappa}-(BEDT-TTF){sub 2}Cu{sub 2}(CN){sub 3} has been studied by measuring the uniaxial expansion coefficients {alpha}{sub i}, the specific heat, and magnetic susceptibility. Special emphasis was placed on the mysterious anomaly around 6K - a potential spin-liquid instability. Distinct and strongly anisotropic lattice effects have been observed at 6K, clearly identifying this feature as a second-order phase transition. Owing to the large anomalies in {alpha}{sub i}, the application of Grueneisen scaling has enabled us to determine the corresponding specific heat contribution and the entropy release. Comparison of the latter with available spin models suggests that spin degrees of freedommore »« less
DOI: 10.1103/PhysRevLett.104.016403
Direct lanthanide-transition metal interactions: Synthesis of (NH{sub 3}){sub 2}YbFe(CO){sub 4} and crystal structures of ([(CH{sub 3}CN){sub 3}YbFe(CO){sub 4}]{sub 2}{center_dot}CH{sub 3}CN){infinity} and [(CH{sub 3}CN){sub 3}YbFe(CO){sub 4}]{sub infinity}

Deng, H. ; Chun, Sung-Ho ; Florian, P. ; ... - Inorganic Chemistry

The heterometallic complex (NH{sub 3}){sub 2}YbFe(CO){sub 4} was prepared from the reduction of Fe{sub 3}(CO){sub 12} by Yb in liquid ammonia. Ammonia was displaced from (NH{sub 3}){sub 2}YbFe(CO){sub 4} by acetonitrile in acetonitrile solution, and the crystalline compounds ([(CH{sub 3}CN){sub 3}YbFe(CO){sub 4}]{sub 2}{center_dot}CH{sub 3}CN){sub infinity} showed that it is a ladder polymer with direct Yb-Fe bonds. In the present study, an X-ray crystal structure analysis also showed that [(CH{sub 3}CN){sub 3}YbFe(CO){sub 4}]{sub infinity} showed that it is a ladder polymer with direct Yb-Fe bonds. In the present study, an X-ray crystal structure analysis also showed that [(CH{sub 3}CN){sub 3}YbFe(CO){sub 4}]{submore »« less
DOI: 10.1021/ic9515113
Synthesis and characterization by sup 1 H, sup 13 C, and sup 19 F NMR spectroscopy of (CH sub 3 CN) sub n (CO) sub 4 minus n (NO)W(. mu. -F)BF sub 3 and ((CH sub 3 CN) sub n+1 (CO) sub 4 minus n (NO)W)(BF sub 4 )(n = 0 minus 2), tungsten mononitrosyl carbonyl cations with labile acetonitrile and ((. mu. -F)BF sub 3 ) sup minus ligands

Hersh, W.H. - Inorganic Chemistry; (USA)

Addition of (NO)(BF{sub 4}) to CH{sub 3}CNW(CO){sub 5} in CH{sub 2}Cl{sub 2} gives a mixture of five mononitrosyl compounds, mer-(cis-CH{sub 3}CN)(trans-NO)(CO){sub 3}W({mu}-F)BF{sub 3} (1), (mer,cis-(CH{sub 3}CN){sub 2}W(CO){sub 3}(NO))(BF{sub 4}) (2a), cis,cis,trans-(CH{sub 3}CN){sub 2}(CO){sub 2}(NO)W({mu}-F)BF{sub 3} (3), (fac-(CH{sub 3}CN){sub 3} W(CO){sub 2}(NO))(BF){sub 4} (4a), and trans-(NO)(CO){sub 4}W({mu}-F)BF{sub 3} (5); in a typical experiment the yield is 90%, and the ratio 1:2a:3:4a:5 is 47:14:11:1:27. Support for the identities of 1-5 is obtained by reaction of the mixture with Me{sub 3}P, giving (mer-(cis-CH{sub 3}CN)(trans-Me{sub 3}P)W(CO){sub 3}(NO))(BF{sub 4}) (7a), (cis,cis,trans-(CH{sub 3}CN){sub 2}(CO){sub 2}(NO)W(PMe{sub 3}))(BF{sub 4}) (8a), (trans-Me{sub 3}P(CO){sub 4}WNO)(BF{sub 4}) (9), and the previouslymore »« less
DOI: 10.1021/ic00329a029

Title: Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) 2 ] 2

Abstract

Citation Formats

Title: Pressure–Temperature Phase Diagram Reveals Spin–Lattice Interactions in Co[N(CN) ₂ ] ₂