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Register a new userSpin-Triplet Excitonic Insulator: The Case of Graphone
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While various excitonic insulators have been studied in the literature, due to the perceived too-small spin splitting, spin-triplet excitonic insulator is rare. In two-dimensional systems such as a graphone, however, it is possible, as revealed by first-principles calculations coupled with Bethe-Salpeter equation. The critical temperature, given by an effective Hamiltonian, is 11.5 K. While detecting excitonic insulators is still a daunting challenge, the condensation of triplet excitons will result in spin superfluidity, which can be directly measured by a transport experiment. Nonlocal dielectric screening also leads to an unexpected phenomenon, namely, an indirect-to-direct transition crossover between single-particle band and exciton dispersion in graphone, which offers yet another test by experiment.
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Direct-gap materials hold promises for excitonic insulator. In contrast to indirect-gap materials, here the difficulty to distinguish from a Peierls charge density wave is circumvented. However, direct-gap materials still suffer from the divergence of polarizability when the band gap approaches zero, leading to diminishing exciton binding energy. We propose that one can decouple the exciton binding energy from the band gap in materials where band-edge states have the same parity. First-principles calculations of two-dimensional GaAs and experimentally mechanically exfoliated single-layer TiS 3 lend solid supports to the new principle.
First-principles calculations reveal an unusual electronic state (dubbed as half excitonic insulator) in monolayer 1T-MX2 (M = Co, Ni and X = Cl, Br). Its one spin channel has a many-body ground state due to excitonic instability, while the other is characterized by a conventional band insulator gap. This disparity arises from a competition between the band gap and exciton binding energy, which exhibits a spin-dependence due to different orbital occupations. Such a state can be identified by optical absorption measurements and angle-resolved photoemission spectroscopy. Our theory not only provides new insights for the study of exciton condensation in magnetic materials but also suggests that strongly-correlated materials could be fertile candidates for excitonic insulators.
The compounds A2Cu3O(SO4)3 (A=Na,K) are characterized by copper hexamers which are weakly coupled along the b-axis to realize one-dimensional antiferromagnetic chains below TN=3 K, whereas the interchain interactions along the a- and c-axes are negligible. We investigated the energy-level splittings of the copper hexamers by inelastic neutron scattering below and above TN. The eight lowest-lying hexamer states could be unambiguously assigned and parametrized in terms of a Heisenberg exchange Hamiltonian, providing direct experimental evidence for an S=1 triplet ground-state associated with the copper hexamers. Therefore, the compounds A2Cu3O(SO4)3 serve as novel cluster-based spin-1 antiferromagnets to support Haldanes conjecture that a gap appears in the excitation spectrum below TN, which was verified by inelastic neutron scattering.
Half a century ago, Mott noted that tuning the carrier density of a semimetal towards zero produces an insulating state in which electrons and holes form bound pairs. It was later argued that such pairing persists even if a semiconducting gap opens in the underlying band structure, giving rise to what has become known as the strong coupling limit of an `excitonic insulator. While these `weak and `strong coupling extremes were subsequently proposed to be manifestations of the same excitonic state of electronic matter, the predicted continuity of such a phase across a band gap opening has not been realized experimentally in any material. Here we show the quantum limit of graphite, by way of temperature and angle-resolved magnetoresistance measurements, to host such an excitonic insulator phase that evolves continuously between the weak and strong coupling limits. We find that the maximum transition temperature T_EI of the excitonic phase is coincident with a band gap opening in the underlying electronic structure at B_0= 46 +/- 1 T, which is evidenced above T_EI by a thermally broadened inflection point in the magnetoresistance. The overall asymmetry of the observed phase boundary around B_0 closely matches theoretical predictions of a magnetic field-tuned excitonic insulator phase in which the opening of a band gap marks a crossover from predominantly momentum-space pairing to real-space pairing.
Excitonic insulators (EI) arise from the formation of bound electron-hole pairs (excitons) in semiconductors and provide a solid-state platform for quantum many-boson physics. Strong exciton-exciton repulsion is expected to stabilize condensed superfluid and crystalline phases by suppressing both density and phase fluctuations. Although spectroscopic signatures of EIs have been reported, conclusive evidence for strongly correlated EI states has remained elusive. Here, we demonstrate a strongly correlated spatially indirect two-dimensional (2D) EI ground state formed in transition metal dichalcogenide (TMD) semiconductor double layers. An equilibrium interlayer exciton fluid is formed when the bias voltage applied between the two electrically isolated TMD layers, is tuned to a range that populates bound electron-hole pairs, but not free electrons or holes. Capacitance measurements show that the fluid is exciton-compressible but charge-incompressible - direct thermodynamic evidence of the EI. The fluid is also strongly correlated with a dimensionless exciton coupling constant exceeding 10. We further construct an exciton phase diagram that reveals both the Mott transition and interaction-stabilized quasi-condensation. Our experiment paves the path for realizing the exotic quantum phases of excitons, as well as multi-terminal exciton circuitry for applications.
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