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Register a new userStrong Coupling Nature of the Excitonic Insulator State in Ta$_2$NiSe$_5$
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We analyze the measured optical conductivity spectra using the density-functional-theory-based electronic structure calculation and density-matrix renormalization group calculation of an effective model. We show that, in contrast to a conventional description, the Bose-Einstein condensation of preformed excitons occurs in Ta$_2$NiSe$_5$, despite the fact that a noninteracting band structure is a band-overlap semimetal rather than a small band-gap semiconductor. The system above the transition temperature is therefore not a semimetal, but rather a state of preformed excitons with a finite band gap. A novel insulator state caused by the strong electron-hole attraction is thus established in a real material.
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Excitonic insulator (EI) is an intriguing insulating phase of matter, where electrons and holes are bonded into pairs, so called excitons, and form a phase-coherent state via Bose-Einstein Condensation (BEC). Its theoretical concept has been proposed several decades ago, but the followed research is very limited, due to the rare occurrence of EI in natural materials and the lack of manipulating method of excitonic condensation. In this paper, we report the realization of a doping-controlled EI-to-semi-metal transition in Ta$_2$NiSe$_5$ using $in$-$situ$ potassium deposition. Combining with angle-resolved photoemission spectroscopy (ARPES), we delineate the evolution of electronic structure through the EI transition with unprecedented precision. The results not only show that Ta$ _2 $NiSe$ _5 $ (TNS) is an EI originated from a semi-metal non-interacting band structure, but also resolve two sequential transitions, which could be attributed to the phase-decoherence and pair-breaking respectively. Our results unveil the Bardeen-Cooper-Schrieffer (BCS)-BEC crossover behavior of TNS and demonstrate that its band structure and excitonic binding energy can be tuned precisely via alkali-metal deposition. This paves a way for investigations of BCS-BEC crossover phenomena, which could provide insights into the many-body physics in condensed matters and other many-body systems.
In the presence of electron-phonon coupling, an excitonic insulator harbors two degenerate ground states described by an Ising-type order parameter. Starting from a microscopic Hamiltonian, we derive the equations of motion for the Ising order parameter in the phonon coupled excitonic insulator Ta$_2$NiSe$_5$ and show that it can be controllably reversed on ultrashort timescales using appropriate laser pulse sequences. Using a combination of theory and time-resolved optical reflectivity measurements, we report evidence of such order parameter reversal in Ta$_2$NiSe$_5$ based on the anomalous behavior of its coherently excited order-parameter-coupled phonons. Our work expands the field of ultrafast order parameter control beyond spin and charge ordered materials.
The excitonic insulator is an electronically-driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta$_2$NiSe$_5$ being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the materials electronic and crystal structure after light excitation reveals surprising spectroscopic fingerprints that are only compatible with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the electronic gap opening. Not only do our results uncover the long-sought mechanism driving the phase transition of Ta$_2$NiSe$_5$, but they also conclusively rule out any substantial excitonic character in this instability.
Tuning many-body electronic phases by an external handle is of both fundamental and practical importance in condensed matter science. The tunability mirrors the underlying interactions, and gigantic electric, optical and magnetic responses to minute external stimuli can be anticipated in the critical region of phase change. The excitonic insulator is one of the exotic phases of interacting electrons, produced by the Coulomb attraction between a small and equal number of electrons and holes, leading to the spontaneous formation of exciton pairs in narrow-gap semiconductors/semimetals. The layered chalcogenide Ta$_2$NiSe$_5$ has been recently discussed as such an excitonic insulator with an excitation gap of ~250 meV below $T_c$ = 328 K. Here, we demonstrate a drastic collapse of the excitation gap in Ta$_2$NiSe$_5$ and the realization of a zero-gap state by moving the tip of a cryogenic scanning tunneling microscope towards the sample surface by a few angstroms. The collapse strongly suggests the many-body nature of the gap in the insulating state of Ta$_2$NiSe$_5$, consistent with the formation of an excitonic state. We argue that the collapse of the gap is driven predominantly by the electrostatic charge accumulation at the surface induced by the proximity of the tip and the resultant carrier doping of the excitonic insulator. Our results establish a novel phase-change function based on excitonic insulators.
The three-chain Hubbard model for Ta$_2$NiSe$_5$ known as a candidate material for the excitonic insulator is investigated over the wide range of energy gap $D$ between the two-fold degenerate conduction bands and the nondegenerate valence band including both semiconducting ($D>0$) and semimetallic ($D<0$) cases. In the semimetallic case, the difference of the band degeneracy inevitably causes the imbalance of each Fermi wavenumber, resulting in a remarkable excitonic state characterized by the condensation of excitons with finite center-of-mass momentum $q$, the so-called Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) excitonic state. With decreasing $D$ corresponding to increasing pressure, the obtained excitonic phase diagram shows a crossover from BEC ($Dsimg 0$) to BCS ($Dsiml 0$) regime, and then shows a distinct phase transition at a certain critical value $D_c(<0)$ from the uniform ($q=0$) to the FFLO ($q e 0$) excitonic state, as expected to be observed in Ta$_2$NiSe$_5$ under high pressure.
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