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High Field Specific Heat of 2D Quantum Spin System SrCu2(BO3)2

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 Added by Guillermo Jorge
 Publication date 2003
  fields Physics
and research's language is English




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We report measurements of the specific heat of the quantum spin liquid system SrCu2(BO3)2 in continuous magnetic fields H of up to 33 T. The specific heat vs temperature at zero field shows an anomaly at 8 K, marking the opening of a gap in the spin singlet excitations. At fields H~12 T, we clearly see a second anomaly that shifts to lower temperatures as H is increased. We attribute its origin to single triplet excitations of the singlet dimer ground state. This conclusion is supported by calculations of the specific heat, which reproduce the experimental data, made using the finite temperature Lanczos method to solve a Shastry-Sutherland Hamiltonian including nearest and next-nearest neighbor Dzyaloshinsky-Moriya interactions. The parameters used to fit the data are the exchange constants J = 74 K and J/J = 0.62, and the Dzyaloshinsky-Moriya coupling constants |D|=6.1K, and $|D|=2.2K.



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We report heat capacity measurements of SrCu$_2$(BO$_3$)$_2$ under high pressure along with simulations of relevant quantum spin models and map out the $(P,T)$ phase diagram of the material. We find a first-order quantum phase transition between the low-pressure quantum dimer paramagnet and a phase with signatures of a plaquette-singlet state below T = $2$ K. At higher pressures, we observe a transition into a previously unknown antiferromagnetic state below $4$ K. Our findings can be explained within the two-dimensional Shastry-Sutherland quantum spin model supplemented by weak inter-layer couplings. The possibility to tune SrCu$_2$(BO$_3$)$_2$ between the plaquette-singlet and antiferromagnetic states opens opportunities for experimental tests of quantum field theories and lattice models involving fractionalized excitations, emergent symmetries, and gauge fluctuations.
We report on the real space profile of spin polarons in the quasi two-dimensional frustrated dimer spin system SrCu2(BO3)2 doped with 0.16% of Zn. The 11B nuclear magnetic resonance spectrum exhibits 15 additional boron sites near non-magnetic Zn impurities. With the help of exact diagonalizations of finite clusters, we have deduced from the boron spectrum the distribution of local magnetizations at the Cu sites with fine spatial resolution, providing direct evidence for an extended spin polaron. The results are confronted with those of other experiments performed on doped and undoped samples of SrCu2(BO3)2.
We have performed $mu$SR studies on single crystals of SrCu$_2$(BO$_3$)$_2$, a quasi-two-dimensional spin system with a spin singlet ground state. We observe two different muon sites which we associate with muons located adjacent to the two inequivalent O sites. One site, presumed to be located in the Cu-O-Cu superexchange path, exhibits a large increase in the frequency shift with decreasing temperature which is unaffected by the singlet formation, indicating that the muon has locally broken the singlet bond. We have also performed $mu$SR on single crystals of SrMg$_{0.05}$Cu$_{1.95}$(BO$_3$)$_2$, Sr$_{0.96}$La$_{0.04}$Cu$_2$(BO$_3$)$_2$, and Sr$_{0.95}$Na$_{0.05}$Cu$_2$(BO$_3$)$_2$. We have found that the frequency shifts of these doped samples are equivalent and contain three branches at low temperatures. Two of these branches map on to the branches observed in the pure sample reasonably well and so we attribute the third branch to effect of the dopants. Specifically, this third branch represents the case when the muon sits at a site in the superexchange path lacking a corresponding singlet, due to it already being broken as a result of doping. This then leads to the conclusion that singlets are broken in this system when it is doped both in and out of the CuBO$_3$ planes.
The magnetization process of the orthogonal-dimer antiferromagnet SrCu2(BO3)2 is investigated in high magnetic fields of up to 118 T. A 1/2 plateau is clearly observed in the field range 84 to 108 T in addition to 1/8, 1/4 and 1/3 plateaux at lower fields. Using a combination of state-of-the-art numerical simulations, the main features of the high-field magnetization, a 1/2 plateau of width 24 T, a 1/3 plateau of width 34 T, and no 2/5 plateau, are shown to agree quantitatively with the Shastry-Sutherland model if the ratio of inter- to intra-dimer exchange interactions J/J=0.63. It is further predicted that the intermediate phase between the 1/3 and 1/2 plateau is not uniform but consists of a 1/3 supersolid followed by a 2/5 supersolid and possibly a domain-wall phase, with a reentrance into the 1/3 supersolid above the 1/2 plateau.
Motivated by the intriguing properties of the Shastry-Sutherland compound SrCu2(BO3)2 under pressure, with a still debated intermediate plaquette phase appearing at around 20 kbar and a possible deconfined critical point at higher pressure upon entering the antiferromagnetic phase, we have investigated its high-field properties in this pressure range using tunnel diode oscillator (TDO) measurements. The two main new phases revealed by these measurements are fully consistent with those identified by infinite Projected Entangled Pair states (iPEPS) calculations of the Shastry-Sutherland model, a 1/5 plateau and a 10 x 2 supersolid. Remarkably, these phases are descendants of the full-plaquette phase, the prominent candidate for the intermediate phase of SrCu2(BO3)2. The emerging picture for SrCu2(BO3)2 is shown to be that of a system dominated by a tendency to an orthorhombic distortion at intermediate pressure, an important constraint on any realistic description of the transition into the antiferromagnetic phase.
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