Bypassing the Structural Bottleneck in the Ultrafast Melting of Electronic Order

• Published in: Physical review letters Vol. 125; no. 26; p. 266402
• Main Authors: Yang, L X, Rohde, G, Hanff, K, Stange, A, Xiong, R, Shi, J, Bauer, M, Rossnagel, K
• Format: Journal Article
• Language: English
• Published: United States 31.12.2020
• ISSN: 1079-7114
• DOI: 10.1103/PhysRevLett.125.266402

Impulsive optical excitation generally results in a complex nonequilibrium electron and lattice dynamics that involves multiple processes on distinct timescales, and a common conception is that for times shorter than about 100 fs the gap in the electronic spectrum is not seriously affected by lattice vibrations. Here, however, by directly monitoring the photoinduced collapse of the spectral gap in a canonical charge-density-wave material, the blue bronze Rb_{0.3}MoO_{3}, we find that ultrafast (∼60  fs) vibrational disordering due to efficient hot-electron energy dissipation quenches the gap significantly faster than the typical structural bottleneck time corresponding to one half-cycle oscillation (∼315  fs) of the coherent charge-density-wave amplitude mode. This result not only demonstrates the importance of incoherent lattice motion in the photoinduced quenching of electronic order, but also resolves the perennial debate about the nature of the spectral gap in a coupled electron-lattice system.