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Register a new userUltrafast melting and recovery of collective order in the excitonic insulator Ta$_{2}$NiSe$_{5}$
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The layered chalcogenide Ta$_{2}$NiSe$_{5}$ has been proposed to host an excitonic condensate in its ground state, a phase that could offer a unique platform to study and manipulate many-body states at room temperature. However, identifying the dominant microscopic contribution to the observed spontaneous symmetry breaking remains challenging, perpetuating the debate over the ground state properties. Here, using broadband ultrafast spectroscopy we investigate the out-of-equilibrium dynamics of Ta$_{2}$NiSe$_{5}$ and demonstrate that the transient reflectivity in the near-infrared range is connected to the systems low-energy physics. We track the status of the ordered phase using this optical signature, establishing that high-fluence photoexcitations can suppress this order. From the sub-50 fs quenching timescale and the behaviour of the photoinduced coherent phonon modes, we conclude that electronic correlations provide a decisive contribution to the excitonic order formation. Our results pave the way towards the ultrafast control of an exciton condensate at room temperature.
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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.
Excitonic insulators host a condensate of electron-hole pairs at equilibrium, giving rise to collective many-body effects. Although several materials have emerged as excitonic insulator candidates, evidence of long-range coherence is lacking and the origin of the ordered phase in these systems remains controversial. Here, using ultrafast pump-probe microscopy, we investigate the possible excitonic insulator Ta$_2$NiSe$_5$. Below 328 K, we observe the anomalous micrometer-scale propagation of coherent modes at velocities of the order of $sim10^5$ m/s, which we attribute to the hybridization between phonon modes and the phase mode of the condensate. We develop a theoretical framework to support this explanation and propose that electronic interactions provide a significant contribution to the ordered phase in Ta$_2$NiSe$_5$. These results allow us to understand how the condensates collective modes transport energy and interact with other degrees of freedom. Our study provides a unique paradigm for the investigation and manipulation of these properties in strongly correlated materials.
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.
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.
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.
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