56 research outputs found
Ar:N - a non-universal glass
The bias energies of various two-level systems (TLSs) and their strengths of
interactions with the strain are calculated for Ar:N glass. Unlike the case
in KBr:CN, a distinct class of TLSs having weak interaction with the strain and
untypically small bias energies is not found. The addition of CO molecules
introduces CO flips which form such a class of weakly interacting TLSs, albeit
at much lower coupling than are typically observed in solids. We conclude that
because of the absence of a distinct class of weakly interacting TLSs, Ar:N
is a non-universal glass, the first such system in three dimensions and in
ambient pressure. Our results further suggest that Ar:N:CO may show
universal properties, but at temperatures lower than K, much
smaller than typical temperature K associated with universality,
because of the untypical softness of this system. Our results thus shed light
on two long standing questions regarding low temperature properties of glasses:
the necessary and sufficient conditions for quantitative universality of phonon
attenuation, and what dictates the energy scale of K below which
universality it typically observed.Comment: 6 pages, 2 figures, results for excitations densities of states are
added, presentation improve
Identification of strong and weak interacting two level systems in KBr:CN
Tunneling two level systems (TLSs) are believed to be the source of phenomena
such as the universal low temperature properties in disordered and amorphous
solids, and noise. The existence of these phenomena in a large variety of
dissimilar physical systems testifies for the universal nature of the TLSs,
which however, is not yet known. Following a recent suggestion that attributes
the low temperature TLSs to inversion pairs [M. Schechter and P.C.E. Stamp,
arXiv:0910.1283.] we calculate explicitly the TLS-phonon coupling of inversion
symmetric and asymmetric TLSs in a given disordered crystal. Our work (a)
estimates parameters that support the theory in M. Schechter and P.C.E. Stamp,
arXiv:0910.1283, in its general form, and (b) positively identifies, for the
first time, the relevant TLSs in a given system.Comment: minor modifications, published versio
Decoherence from dipolar interspin interactions in molecular spin qubits
The realization of spin-based logical gates crucially depends on magnetically coupled spin qubits. Thus, understanding decoherence when spin qubits are in close proximity will become a roadblock to overcome. Herein, we propose a method free of fitting parameters to evaluate the qubit phase memory time Tm in samples with high electron spin concentrations. The method is based on a model aimed to estimate magnetic nuclear decoherence [P. C. E. Stamp and I. S. Tupitsyn, Phys. Rev. B 69, 014401 (2004)]. It is applied to a ground-spin J=8 magnetic molecule 1 displaying atomic clock transitions, namely [HoIII(W5O18)2]9−, which remarkably increase Tm at unusually high electron-spin concentrations. Our approach unveils the causes that limit the coherence reached at the clock transitions in challenging systems such as 1, where recent models fail
Molecular spins for quantum computation
Spins in solids or in molecules possess discrete energy levels, and the associated quantum states can be tuned and coherently manipulated by means of external electromagnetic fields. Spins therefore provide one of the simplest platforms to encode a quantum bit (qubit), the elementary unit of future quantum computers. Performing any useful computation demands much more than realizing a robust qubit¿one also needs a large number of qubits and a reliable manner with which to integrate them into a complex circuitry that can store and process information and implement quantum algorithms. This 'scalability' is arguably one of the challenges for which a chemistry-based bottom-up approach is best-suited. Molecules, being much more versatile than atoms, and yet microscopic, are the quantum objects with the highest capacity to form non-trivial ordered states at the nanoscale and to be replicated in large numbers using chemical tools
Theoretical evaluation of lanthanide binding tags as biomolecular handles for the organization of single ion magnets and spin qubits
Lanthanoid complexes are amongst the most promising compounds both in single ion magnetism and as molecular spin qubits, but their organization remains an open problem. We propose to combine Lanthanide Binding Tags (LBTs) with recombinant proteins as a path for an extremely specific and spatially-resolved organisation of lanthanoid ions as spin qubits. We develop a new computational subroutine for the freely available code SIMPRE that allows an inexpensive estimate of quantum decoherence times and qubit–qubit interaction strengths. We use this subroutine to evaluate our proposal theoretically for 63 different systems. We evaluate their behavior as single ion magnets and estimate both decoherence caused by the nuclear spin bath and the interqubit interaction strength by dipolar coupling. We conclude that Dy3+ LBT complexes are expected to behave as SIMs, but Yb3+ derivatives should be better spin qubits.Lanthanoid complexes are amongst the most promising compounds both in single ion magnetism and as molecular spin qubits, but their organization remains an open problem. We propose to combine Lanthanide Binding Tags (LBTs) with recombinant proteins as a path for an extremely specific and spatially-resolved organisation of lanthanoid ions as spin qubits. We develop a new computational subroutine for the freely available code SIMPRE that allows an inexpensive estimate of quantum decoherence times and qubit–qubit interaction strengths. We use this subroutine to evaluate our proposal theoretically for 63 different systems. We evaluate their behavior as single ion magnets and estimate both decoherence caused by the nuclear spin bath and the interqubit interaction strength by dipolar coupling. We conclude that Dy3+ LBT complexes are expected to behave as SIMs, but Yb3+ derivatives should be better spin qubits
Insights on the coupling between vibronically active molecular vibrations and lattice phonons in molecular nanomagnets
Spin-lattice relaxation is a key open problem to understand the spin dynamics of single-molecule magnets and molecular spin qubits. While modelling the coupling between spin states and local vibrations allows to determine the more relevant molecular vibrations for spin relaxation, this is not sufficient to explain how energy is dissipated towards the thermal bath. Herein, we employ a simple and efficient model to examine the coupling of local vibrational modes with long-wavelength longitudinal and transverse phonons in the clock-like spin qubit [Ho(W5O18)2]9−. We find that in crystals of this polyoxometalate the vibrational mode previously found to be vibronically active at low temperature does not couple significantly to lattice phonons. This means that further intramolecular energy transfer via anharmonic vibrations is necessary for spin relaxation in this system. Finally, we discuss implications for the spin-phonon coupling of [Ho(W5O18)2]9− deposited on a MgO (001) substrate, offering a simple methodology that can be extrapolated to estimate the effects on spin relaxation of different surfaces, including 2D materials
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