Determining ground states of correlated electron systems is fundamental to understanding novel phenomena in condensed matter physics. A difficulty, however, arises in a geometrically frustrated system in which the incompatibility between the global topology of an underlying lattice and local spin interactions gives rise to macroscopically degenerate ground states, potentially prompting the emergence of quantum spin states, such as resonating valence bond (RVB) and valence bond solid (VBS). Although theoretically proposed to exist in a kagome lattice -- one of the most highly frustrated lattices in two dimensions (2D) being comprised of corner-sharing triangles -- such quantum-fluctuation-induced states have not been observed experimentally. Here we report the first realization of the "pinwheel" VBS ground state in the S=1/2 deformed kagome lattice antiferromagnet Rb2Cu3SnF12. In this system, a lattice distortion breaks the translational symmetry of the ideal kagome lattice and stabilizes the VBS state.
We study the Heisenberg model on the pinwheel distorted kagome lattice as observed in the material Rb_2Cu_3SnF_12. Experimentally relevant thermodynamic properties at finite temperatures are computed utilizing numerical linked-cluster expansions. We also develop a Lanczos-based, zero-temperature, numerical linked cluster expansion to study the approach of the pinwheel distorted lattice to the uniform kagome-lattice Heisenberg model. We find strong evidence for a phase transition before the uniform limit is reached, implying that the ground state of the kagome-lattice Heisenberg model is likely…
Topological Triplons in the Pinwheel Valence Bond Solid on the Kagome Lattice
Technical University of Munich（慕尼黑工业大学）；TUM School of Natural Sciences（TUM自然科学学院）；Physics Department（物理系）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Institute of Physics, Ecole Polytechnique Federale de Lausanne (EPFL)（洛桑联邦理工学院物理研究所）
We consider Z2 spin liquids on the kagome lattice on the verge of a valence bond solid (VBS) transition, where vortex excitations carrying Z2 magnetic flux - so-called visons - condense. We show that these vison excitations can couple directly to the external electromagnetic field, even though they carry neither spin nor charge. This is possible via a magneto-elastic coupling mechanism recently identified by Potter et al and Hao. For the case of transitions to a 36-site unit cell VBS state the corresponding finite ac-conductivity has a specific power law frequency dependence, which is related …
Using $^{63,65}$Cu nuclear magnetic resonance (NMR) in magnetic fields up to 30 T we study the microscopic properties of the 12-site valence-bond-solid ground state in the "pinwheel" kagome compound Rb$_2$Cu$_3$SnF$_{12}$. We find that the ground state is characterized by a strong transverse staggered spin polarization whose temperature and field dependence points to a mixing of the singlet and triplet states. This is further corroborated by the field dependence of the gap $Δ(H)$, which has a level anticrossing with a large minimum gap value of $\approx Δ(0)/2$, with no evidence of a phase tra…
We present an effective $\mathbb{Z}_2$ gauge theory that captures various competing phases in spin-1/2 kagome lattice antiferromagnets: the topological $\mathbb{Z}_2$ spin liquid (SL) phase, and the 12-site and 36-site valence bond solid (VBS) phases. Our effective theory is a generalization of the recent $\mathbb{Z}_2$ gauge theory proposed for SL phases by Wan and Tchernyshyov. In particular, we investigate possible VBS phases that arise from vison condensations in the SL. In addition to the 12-site and 36-site VBS phases, there exists 6-site VBS that is closely related to the symmetry-break…
We present numerical evidence for the emergence of an extended valence bond solid (VBS) phase at $T=0$ in the kagome $S=1/2$ Heisenberg antiferromagnet with ferromagnetic further-neighbor interactions. The VBS is located at the boundary between two magnetically ordered regions and extends close to the nearest-neighbor Heisenberg point. It exhibits a diamond-like singlet covering pattern with a $12$-site unit-cell. Our results suggest the possibility of a direct, possibly continuous, quantum phase transition from the neighboring $\mathbf{q}=0$ coplanar magnetically ordered phase into the VBS ph…
The spin-1/2 quantum antiferromagnet on the Kagome lattice provides a quintessential example in the strongly correlated electron physics where both effects of geometric frustration and quantum fluctuation are pushed to their limit. Among possible non-magnetic ground states, the valence bond solid (VBS) with a 36-site unit cell is one of the most promising candidates. A natural theoretical framework for the analysis of such VBS order is to consider quantum states on a bond connecting the nearest-neighboring sites as fundamental quantum modes of the system and treat them as effectively independe…
We consider the $(2+1)$-d $SU(2)$ quantum link model on the honeycomb lattice and show that it is equivalent to a quantum dimer model on the Kagomé lattice. The model has crystalline confined phases with spontaneously broken translation invariance associated with pinwheel order, which is investigated with either a Metropolis or an efficient cluster algorithm. External half-integer non-Abelian charges (which transform non-trivially under the $\mathbb{Z}(2)$ center of the $SU(2)$ gauge group) are confined to each other by fractionalized strings with a delocalized $\mathbb{Z}(2)$ flux. The strand…
We show that the optical responses below the Mott gap can be used to probe the spin-triplet excitations in valence bond solid (VBS) phases in Mott insulators. The optical conductivity in this regime arises due to the electronic polarization mechanism via virtual electron hopping processes. We apply this mechanism to the Hubbard model with spin-orbit couplings and/or the corresponding spin model with significant Dzyaloshinskii-Moriya (DM) interactions, and compute the optical conductivity of VBS states on both ideal and deformed Kagome lattices. In case of the deformed Kagome lattice, we study …
The spin-$\frac{1}{2}$ kagome antiferromagnet is considered an ideal host for a quantum spin liquid ground state. We find that when the bonds of the kagome lattice are modulated with a periodic pattern, new quantum ground states emerge. Newly synthesized crystalline barlowite (Cu$_4$(OH)$_6$FBr) and Zn-substituted barlowite demonstrate the delicate interplay between singlet states and spin order on the spin-$\frac{1}{2}$ kagome lattice. Comprehensive structural measurements demonstrate that our new variant of barlowite maintains hexagonal symmetry at low temperatures with an arrangement of dis…
The frustrated magnet clinoatacamite, $γ$-Cu$_2$(OH)$_3$Cl, is attracting a lot of interest after suggestions that at low temperature it forms an exotic quantum state termed a Valence Bond Solid (VBS) made from dimerised Cu$^{2+}$ ($S=1/2$) spins.\cite{Lee_clinoatacamite} Key to the arguments surrounding this proposal were suggestions that the kagomé planes in the magnetic pyrochlore lattice of clinoatacamite are only weakly coupled, causing the system to behave as a quasi-2-dimensional magnet. This was reasoned from the near 95$^\circ$ angles made at the bridging oxygens that mediate exchange…
One of the most promising candidate ground states for the quantum antiferromagnetic Heisenberg model on the Kagome lattice is the valence bond solid (VBS) with a 36-site unit cell. We present a theory of triplet excitation spectra about this ground state using bond operator formalism. In particular we obtain dispersions of all 18 triplet modes in the reduced Brillouin zone. In the bond operator mean-field theory, it is found that a large number of triplet modes are non-dispersive. In particular, the lowest triplet excitation is non-dispersive and degenerate with a dispersive mode at the zone c…
High intensity pulsed neutron scattering reveals a new set of magnetic excitations in the pinwheel valence bond solid state of the distorted kagome lattice antiferromagnet Rb$_2$Cu$_3$SnF$_{12}$. The polarization of the dominant dispersive modes (2 meV $<\hbarω< $7 meV) is determined and found consistent with a dimer series expansion with strong Dzyaloshinskii-Moriya interactions ($D/J=0.18$). A weakly dispersive mode near 5 meV and shifted "ghosts" of the main modes are attributed to the enlarged unit cell below a $T=215$ K structural transition. Continuum scattering between 8 meV and 10 meV …
We introduce a method to design a local spin Hamiltonian to realize a Gutzwiller-projected parton wave functions (GPWF) as its ground state. For example, the Dirac spin liquid (DSL) state is quite close to the true ground state of the spin-1/2 Heisenberg model on kagome lattice. We examine what kind of perturbations we should add in order to drive the DSL to more stable chiral spin liquid (CSL), valence bond solid (VBS) or Gutzwiller-projected spin Hall (GSH) states. We compute the two-body reduced-density-matrices (2-RDM) of GPWFs for those target states, and compare them to the 2-RDM of the …
Motivated by a recent experiment on Rb2Cu3SnF12, where spin-1/2 Cu2+ moments reside on the layers of Kagome-like lattices, we investigate quantum ground states of the antiferromagnetic Heisenberg model on a series of deformed Kagome lattices. The deformation is characterized by a weaker exchange coupling (alpha*J) on certain lattice links appropriate for Rb2Cu3SnF12 with alpha=1 corresponding to the ideal Kagome lattice. In particular, we study possible valence bond solid phases using the perturbation theory around isolated dimer limits, dimer series expansion, and self-consistent bond operato…
Recent scanning tunnelling microscopy (STM) experiments on underdoped cuprates have displayed modulations in the local electronic density of states which are centered on a Cu-O-Cu bond (Kohsaka et. al., cond-mat/0703309). As a paradigm of the pinning of such bond-centered ordering in strongly correlated systems, we present the theory of valence bond solid (VBS) correlations near a single impurity in a square lattice antiferromagnet. The antiferromagnet is assumed to be in the vicinity of a quantum transition from a magnetically ordered Neel state to a spin-gap state with long-range VBS order. …
A three-dimensional system of interacting spins typically develops static long-range order when it is cooled. If the spins are quantum (S = 1/2), however, novel quantum paramagnetic states may appear. The most highly sought state among them is the resonating valence bond (RVB) state in which every pair of neighboring quantum spins form entangled spin singlets (valence bonds) and the singlets are quantum mechanically resonating amongst all the possible highly degenerate pairing states. Here we provide experimental evidence for such quantum paramagnetic states existing in frustrated antiferromag…
We have systematically investigated the variation of the exchange parameters and the ground state in the $S = 1/2$ kagome-lattice antiferromagnet (Rb$_{1-x}$Cs$_{x}$)$_2$Cu$_3$SnF$_{12}$, via magnetic measurements using single crystals. One of the parent compounds, Rb$_2$Cu$_3$SnF$_{12}$, which has a distorted kagome lattice accompanied by four sorts of nearest-neighbor exchange interaction, has a disordered ground state described by a pinwheel valence-bond-solid state. The other parent compound, Cs$_2$Cu$_3$SnF$_{12}$, which has a uniform kagome lattice at room temperature, has an ordered gro…
In recent work, we argued that a particular algebraic spin liquid (ASL) may be the ground state of the S = 1/2 kagome lattice Heisenberg antiferromagnet. This state, which lacks a spin gap, is appealing in light of recent experiments on herbertsmithite (ZnCu3(OH)6Cl2). Here, we study the properties of this ASL in more detail, using both the low-energy effective field theory and Gutzwiller-projected wavefunctions. We identify the competing orders of the ASL -- among them we find a set of magnetic orders lying at the M-points of the Brillouin zone, the q = 0 magnetic ordered state, the "Hastings…
We present an extensive quantum Monte Carlo study of a nearest-neighbor, singlet-projection model on the kagome lattice that exhibits SO($N$) symmetry and is sign-problem-free. We find that in contrast to the previously studied SU($N$) variations of this model, the non-bipartite lattices appear to harbor spin-liquid phases for intermediate values of $N$, a result also seen on the triangular lattice with this same model. Unlike the triangular lattice, however, the kagome lattice appears to admit no valence bond solid (VBS) phase for large $N$, instead remaining a spin-liquid. We also observe th…
Pinch point singularities, associated with flat band magnetic excitations, are tell-tale signatures of Coulomb spin liquids. While their properties in the presence of quantum fluctuations have been widely studied, the fate of the complementary non-analytic features -- shaped as half-moons and stars -- arising from adjacent shallow dispersive bands has remained unexplored. Here, we address this question for the spin $S=1/2$ Heisenberg antiferromagnet on the kagome lattice with second and third neighbor couplings, which allows one to tune the classical ground state from flat bands to being gover…
Nearest-neighbor interacting S = 1/2 spins on the ideal Kagomé lattice are predicted to form a variety of novel quantum entangled states, including quantum spin-liquid (SL) and valence bond solid (VBS) phases. In real materials, the presence of additional perturbative spin interactions may further expand the variety of entangled states, which recent theoretical analyses show are identifiable through the spontaneous loss of particular discrete point group symmetries. Here we comprehensively resolve the ground state point group symmetries of the prototypical Kagomé SL candidate ZnCu$_3$(OH)$_6$C…
We show the structures of magnetic excitations in spin-1/2 kagome-lattice antiferromagnets Cs$_2$Cu$_3$SnF$_{12}$ and Rb$_2$Cu$_3$SnF$_{12}$ investigated by inelastic neutron scattering in wide energy and momentum ranges. For Cs$_2$Cu$_3$SnF$_{12}$, four single-magnon excitation modes were observed. Low-energy three modes are assigned to be transverse modes and the high-energy fourth mode is suggested to be an amplitude mode. It was found that the broad excitation continuum without a marked structure spreads in a wide energy range from $0.15J$ to approximately $2.5J$ in contrast to the clearly…
By using the dual vortex method (DVM), we develop systematically a simple and effective scheme to use the vortex degree of freedoms on dual lattices to characterize the symmetry breaking patterns of the boson insulating states in the direct lattices. Then we apply our scheme to study quantum phases and phase transitions in an extended boson Hubbard model slightly away from $ 1/3 $ ($ 2/3 $) filling on frustrated lattices such as triangular and kagome lattice. In a triangular lattice at $ 1/3 $, we find a X-CDW, a stripe CDW phase which was found perviously by a density operator formalism (DOF)…
