Excitonium is a condensate and it exhibits macroscopic quantum phenomena, like a superconductor, or superfluid, or insulating electronic crystal. It’s made up of excitons, particles that are formed in a very strange quantum mechanical pairing, namely that of an escaped electron and the hole it left behind.
Above – Artist’s depiction of the collective excitons of an excitonic solid. These excitations can be thought of as propagating domain walls (yellow) in an otherwise ordered solid exciton background (blue). Image courtesy of Peter Abbamonte, U. of I. Department of Physics and Frederick Seitz Materials Research Laboratory
It defies reason, but it turns out that when an electron, seated at the edge of a crowded-with-electrons valence band in a semiconductor, gets excited and jumps over the energy gap to the otherwise empty conduction band, it leaves behind a “hole” in the valence band. That hole behaves as though it were a particle with positive charge, and it attracts the escaped electron. When the escaped electron with its negative charge, pairs up with the hole, the two remarkably form a composite particle, a boson—an exciton.
Until now, scientists have not had the experimental tools to positively distinguish whether what looked like excitonium wasn’t in fact a Peierls phase. Though it’s completely unrelated to exciton formation, Peierls phases and exciton condensation share the same symmetry and similar observables—a superlattice and the opening of a single-particle energy gap.
Abbamonte and his team were able to overcome that challenge by using a novel technique they developed called momentum-resolved electron energy-loss spectroscopy (M-EELS). M-EELS is more sensitive to valence band excitations than inelastic x-ray or neutron scattering techniques. Kogar retrofit an EEL spectrometer, which on its own could measure only the trajectory of an electron, giving how much energy and momentum it lost, with a goniometer, which allows the team to measure very precisely an electron’s momentum in real space.
They have made the first-ever observation in any material of the precursor to exciton condensation, a soft plasmon phase that emerged as the material approached its critical temperature of 190 Kelvin. This soft plasmon phase is “smoking gun” proof of exciton condensation in a three-dimensional solid and the first-ever definitive evidence for the discovery of excitonium.
Probing an excitonic condensate
Excitons—bound states of electrons and holes in solids—are expected to form a Bose condensate at sufficiently low temperatures. Excitonic condensation has been studied in systems such as quantum Hall bilayers where physical separation between electrons and holes enables a longer lifetime for their bound states. Kogar et al. observed excitons condensing in the three-dimensional semimetal 1T-TiSe2. In such systems, distinguishing exciton condensation from other types of order is tricky. To do so, the authors used momentum-resolved electron energy-loss spectroscopy, a technique developed to probe electronic collective excitations. The energy needed to excite an electronic mode became negligible at a finite momentum, signifying the formation of a condensate.
Abstract
Bose condensation has shaped our understanding of macroscopic quantum phenomena, having been realized in superconductors, atomic gases, and liquid helium. Excitons are bosons that have been predicted to condense into either a superfluid or an insulating electronic crystal. Using the recently developed technique of momentum‐resolved electron energy‐loss spectroscopy (M-EELS), we studied electronic collective modes in the transition metal dichalcogenide semimetal 1T‐TiSe2. Near the phase-transition temperature (190 kelvin), the energy of the electronic mode fell to zero at nonzero momentum, indicating dynamical slowing of plasma fluctuations and crystallization of the valence electrons into an exciton condensate. Our study provides compelling evidence for exciton condensation in a three-dimensional solid and establishes M-EELS as a versatile technique sensitive to valence band excitations in quantum materials.
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