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A charge density wave (CDW) is a phase of matter characterized by a periodic modulation of the valence electron density accompanied by a distortion of the lattice structure. The microscopic details of CDW formation are closely tied to the dynamic charge susceptibility, χ(q, ω), which describes the behavior of electronic collective modes. Despite decades of extensive study, the behavior of χ(q, ω) in the vicinity of a CDWtransition has never been measured with high energy resolution (∼meV). Here, we investigate the canonical CDW transition in ErTe3 using momentum-resolved electron energy loss spectroscopy (M-EELS), a technique uniquely sensitive to valence band charge excitations. Unlike phonons in these materials, which undergo conventional softening due to the Kohn anomaly at the CDW wavevector, the electronic excitations display purely relaxational dynamics that are well described by a diffusive model. The diffusivity peaks around 250 K, just below the critical temperature. Additionally, we report, for the first time, a divergence in the real part of χ(q, ω) in the static limit (ω → 0), a phenomenon predicted to characterize CDWs since the 1970s. These results highlight the importance of energy- and momentum-resolved measurements of electronic susceptibility and demonstrate the power of M-EELS as a versatile probe of charge dynamics in materials.
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Creation of a novel inverted charge density wave state
Charge density wave (CDW) order is an emergent quantum phase that is characterized by periodic lattice distortion and charge density modulation, often present near superconducting transitions. Here, we uncover a novel inverted CDW state by using a femtosecond laser to coherently reverse the star-of-David lattice distortion in 1T-TaSe2. We track the signature of this novel CDW state using time- and angle-resolved photoemission spectroscopy and the time-dependent density functional theory to validate that it is associated with a unique lattice and charge arrangement never before realized. The dynamic electronic structure further reveals its novel properties that are characterized by an increased density of states near the Fermi level, high metallicity, and altered electron–phonon couplings. Our results demonstrate how ultrafast lasers can be used to create unique states in materials by manipulating charge-lattice orders and couplings.
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- Award ID(s):
- 1734006
- PAR ID:
- 10589108
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- Structural Dynamics
- Volume:
- 9
- Issue:
- 1
- ISSN:
- 2329-7778
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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