Anisotropy of the molecular magnet<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi>V</mml:mi><mml:mn>15</mml:mn></mml:msub></mml:math>spin Hamiltonian detected by high-field electron spin resonance

Martens, Mathew; Tol, Johan van; Dalal, Naresh S.; Bertaina, Sylvain; Barbara, B.; Tsukerblat, Boris; Müller, Achim; Garai, Somenath; Miyashita, Seiji; Chiorescu, Irinel

doi:10.1103/physrevb.89.195439

Cited by 5 publications

(11 citation statements)

References 30 publications

(34 reference statements)

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“…However, for completness of the study, a summary of the properties of the static term H st is presented in this section following our previous study, Ref. [16]. The Zeeman term is given by:…”

Section: Resultsmentioning

confidence: 99%

“…Sample temperature can be varied from room temperature down to 2.5 K. A single crystal of regular shape (as in [16]) of volume < ∼ 0.1 mm 3 was positioned on a rotating stage allowing for continuous change of the angle θ between B 0 and the c axis of the molecule following the procedure described in [16]. The homogeneity of the magnet compared to the size of the crystal allows us to ignore B 0 as a source of broadening.…”

Section: Experimental Datamentioning

confidence: 99%

“…where H 0 describes the Zeeman splitting in an external field B 0 , H J is the symmetric exchange term, and H DM is the anti-symmetric Dzyaloshinsky-Moriya (DM) term (see [16] for a detailed formulation). H st eigenvalues are shown in Fig.…”

Section: Fluctuations In Spin Hamiltonianmentioning

confidence: 99%

“…The method presented below is general and can be applied to any other molecular system. We calculate the minimum and maximum excitation frequencies f min,max leading to resonance fields B max,min using the first moment method [16]. Their difference is:…”

Section: Field-frequency Conversionmentioning

confidence: 99%

“…Exchange couplings between the spins in the triangle and hexagons exceed 100 K [13,14] and at low temperatures this spin system can be modeled as a triangle of spins 1/2. The spin Hamiltonian is, as discussed in Supplemental Material [15] (SM) Section I:where H 0 describes the Zeeman splitting in an external field B 0 , H J is the symmetric exchange term, and H DM is the anti-symmetric Dzyaloshinsky-Moriya (DM) term (see [16] for a detailed formulation). H st eigenvalues are shown in Fig.…”

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Spin-orbit coupling fluctuations as a mechanism of spin decoherence

et al. 2017

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We discuss a general framework to address spin decoherence resulting from fluctuations in a spin Hamiltonian. We performed a systematic study on spin decoherence in the compound K6[V15As6O42(D2O)] · 8D2O, using high-field Electron Spin Resonance (ESR). By analyzing the anisotropy of resonance linewidths as a function of orientation, temperature and field, we find that the spin-orbit term is a major decoherence source. The demonstrated mechanism can alter the lifetime of any spin qubit and we discuss how to mitigate it by sample design and field orientation. INTRODUCTIONIn solid-state systems, interactions between electronic spins and their environment are the limiting factor of spin phase lifetime, or decoherence time. Important advances have been recently realized in demonstrating long-lived spin coherence via spin dilution [1][2][3][4][5][6] and isolating a spin in non-magnetic cages [7], for instance. The presence of a lattice can be felt by spins through orbital symmetries and spin-orbit coupling. An isolated free electron has a spin angular momentum associated with a g-factor g e = 2.00232 but in general, spin-orbit coupling changes the g-factor by the admixture of excited orbital states [8] into the ground state. In this Letter, we demonstrate that fluctuations in the spin-orbit interaction can be a significant source of spin decoherence. We present a general theoretical framework to obtain noise spectrum. The method is applied to fluctuations of the long-range dipolar interactions and we observe how the spin-orbit term is modulating the induced decoherence. The model describes spin dilution and thermal excitations effects as well. Experimentally, we analyze shape and orientation anisotropy of ESR linewidths of the molecular compound. This system has shown spin coherence at low temperatures [5,9] and interesting out of equilibrium spin dynamics due to phonon bottlenecking [10,11]. However, the details of the spin decoherence are still not fully understood. In the case of diluted or molecular spins, little evidence has been brought up to now on the role of spin-orbit coupling on spin coherence time. This study elucidates this decoherence mechanism and how to mitigate its effect. FLUCTUATIONS IN SPIN HAMILTONIANThe V 15 cluster anions form a lattice with trigonal symmetry containing two clusters per unit cell [12]. Individual molecules have fifteen V IV s = 1/2 ions arranged into three layers, two non-planar hexagons sandwiching a triangle (see Fig. 1a). Exchange couplings between the spins in the triangle and hexagons exceed 100 K [13,14] and at low temperatures this spin system can be modeled as a triangle of spins 1/2. The spin Hamiltonian is, as discussed in Supplemental Material [15] (SM) Section I:where H 0 describes the Zeeman splitting in an external field B 0 , H J is the symmetric exchange term, and H DM is the anti-symmetric Dzyaloshinsky-Moriya (DM) term (see [16] for a detailed formulation). H st eigenvalues are shown in Fig. 1(b) and are used to calculate resonant field positions B res of the E...

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Section: Resultsmentioning

confidence: 99%

Section: Experimental Datamentioning

confidence: 99%

Section: Fluctuations In Spin Hamiltonianmentioning

confidence: 99%

Section: Field-frequency Conversionmentioning

confidence: 99%

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confidence: 99%

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Spin-orbit coupling fluctuations as a mechanism of spin decoherence

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Magneto-Structural Analysis of Iron(III) Keggin Polyoxometalates

et al. 2017

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A computational study and magnetic susceptibility measurements of three homonuclear Fe(III) Keggin structures are herein presented: the [FeO 4 @Fe 12 F 24 (μ− OCH 3 ) 12 ] 5− anion (1), the [Bi 6 {FeO 4 @Fe 12 O 12 (OH) 12 }(μ-O 2 CCCl 3 ) 12 ] + cation (2) and its polymorph [Bi 6 {FeO 4 @ Fe 12 O 12 (OH) 10 (H 2 O) 2 }(μ-O 2 CCF 3 ) 10 ] 3+ (3). These results are contrasted with the exchange interactions present in the previously characterized [Fe 6 (OH) 3 Ge 2 W 18 O 68 (OH) 6 ] 11− and [H 12 As 4 Fe 8 W 30 O 120 (H 2 O) 2 ] 4− anions. The computational analysis shows that the most significant antiferromagnetic spin coupling takes place at the junction between each of the {Fe 3 O 6 (OH) 3 }/{Fe 3 F 6 (OCH 3 ) 3 } framework motifs, a possibility that had been previously discarded in the literature on the basis of the Fe−Fe distances. For all the examined iron(III) Keggin structures, it is found that the magnitude of the magnetic couplings within each structural subunit follows the same trend.

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Three-Dimensional Architectures of [Mn^IICr^III(oxalate)₃]⁻ Complexes with Cage-Type Networks Surrounding Supramolecular Cations

Endô

Kubo

Yoshitake

et al. 2015

Crystal Growth & Design

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Metal−organic network structure based on oxalate bridges {[Mn II Cr III (oxalate) 3 ] − } ∞ and supramolecular cations (H 2 PPD 2+ )(benzo[18]crown-6) 2 [MnCr(oxalate) 3 ]-(CH 3 OH)(CH 3 CN) 2 (1) and (o-FAni + ) 2 (DCH[18]crown-6) 2 [Mn(CH 3 OH)Cr(oxalate) 3 ][MnCr(oxalate) 3 ](CH 3 OH)(2), where H 2 PPD 2+ , o-FAni + , and DCH[18]crown-6 denote p-phenylenediammonium 2+ , o-fluoroanilinium + , and cis-syn-cisdicyclohexano[18]crown-6, respectively, were synthesized. The crystal structure of 1 was the combination of [Mn(Λ)-Cr(Λ)(oxalate) 3 ] − and [Mn(Λ)Cr(Δ)(oxalate) 3 ] − , whereas that of crystal 2 was the combination of [Mn(Λ)(CH 3 OH)-Cr(Δ)(oxalate) 3 ] and [Mn(Λ)Cr(Δ)(oxalate) 3 ]. Large flexible supramolecular cations provide the three-dimensional structure of {[Mn II Cr III (oxalate) 3 ] − } ∞ , which is different from the twodimensional honeycomb structure often observed for {[Mn II Cr III (oxalate) 3 ] − } ∞ complexes. Temperature-dependent magnetic susceptibilities of the complexes 1 and 2 exhibited ferromagnetic behaviors following the Curie−Weiss law (C = 11.5 cm 3 K mol −1 , θ = 13.0 K for 1; C = 4.14 cm 3 K mol −1 , θ = 12.3 K for 2).

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Anisotropy of the molecular magnetV15spin Hamiltonian detected by high-field electron spin resonance

Cited by 5 publications

References 30 publications

Spin-orbit coupling fluctuations as a mechanism of spin decoherence

Spin-orbit coupling fluctuations as a mechanism of spin decoherence

Magneto-Structural Analysis of Iron(III) Keggin Polyoxometalates

Three-Dimensional Architectures of [Mn^IICr^III(oxalate)₃]⁻ Complexes with Cage-Type Networks Surrounding Supramolecular Cations

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Anisotropy of the molecular magnetV15spin Hamiltonian detected by high-field electron spin resonance

Cited by 5 publications

References 30 publications

Spin-orbit coupling fluctuations as a mechanism of spin decoherence

Spin-orbit coupling fluctuations as a mechanism of spin decoherence

Magneto-Structural Analysis of Iron(III) Keggin Polyoxometalates

Three-Dimensional Architectures of [MnIICrIII(oxalate)3]− Complexes with Cage-Type Networks Surrounding Supramolecular Cations

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Product

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About

Three-Dimensional Architectures of [Mn^IICr^III(oxalate)₃]⁻ Complexes with Cage-Type Networks Surrounding Supramolecular Cations