Bypassing the Structural Bottleneck in the Ultrafast Melting of Electronic Order.

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.

Erratum: Ultrafast Doublon Dynamics in Photoexcited 1T-TaS_{2} [Phys. Rev. Lett. 120, 166401 (2018)].

This corrects the article DOI: 10.1103/PhysRevLett.120.166401.

Ultrafast Doublon Dynamics in Photoexcited 1T-TaS_{2}.

Strongly correlated materials exhibit intriguing properties caused by intertwined microscopic interactions that are hard to disentangle in equilibrium. Employing nonequilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS_{2}, we identify a spectroscopic signature of doubly occupied sites (doublons) that reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on timescales of electronic hopping ℏ/J≈14 fs. Despite strong electron-phonon coupling, the dynamics can be explained by purely electronic effects captured by the single-band Hubbard model under the assumption of weak hole doping, in agreement with our static sample characterization. This sensitive interplay of static doping and vicinity to the metal-insulator transition suggests a way to modify doublon relaxation on the few-femtosecond timescale.

Ultrafast Formation of a Fermi-Dirac Distributed Electron Gas.

Time- and angle-resolved photoelectron spectroscopy with 13 fs temporal resolution is used to follow the different stages in the formation of a Fermi-Dirac distributed electron gas in graphite after absorption of an intense 7 fs laser pulse. Within the first 50 fs after excitation, a sequence of time frames is resolved that are characterized by different energy and momentum exchange processes among the involved photonic, electronic, and phononic degrees of freedom. The results reveal experimentally the complexity of the transition from a nascent nonthermal towards a thermal electron distribution due to the different timescales associated with the involved interaction processes.

Time-resolved ARPES with sub-15 fs temporal and near Fourier-limited spectral resolution.

An experimental setup for time- and angle-resolved photoelectron spectroscopy with sub-15 fs temporal resolution is presented. A hollow-fiber compressor is used for the generation of 6.5 fs white light pump pulses, and a high-harmonic-generation source delivers 11 fs probe pulses at a photon energy of 22.1 eV. A value of 13 fs full width at half-maximum of the pump-probe cross correlation signal is determined by analyzing a photoemission intensity transient probing a near-infrared interband transition in 1T-TiSe2. Notably, the energy resolution of the setup conforms to typical values reported in conventional time-resolved photoemission studies using high harmonics, and an ultimate resolution of 170 meV is feasible.

Time-domain classification of charge-density-wave insulators.

Distinguishing insulators by the dominant type of interaction is a central problem in condensed matter physics. Basic models include the Bloch-Wilson and the Peierls insulator due to electron-lattice interactions, the Mott and the excitonic insulator caused by electron-electron interactions, and the Anderson insulator arising from electron-impurity interactions. In real materials, however, all the interactions are simultaneously present so that classification is often not straightforward. Here, we show that time- and angle-resolved photoemission spectroscopy can directly measure the melting times of electronic order parameters and thus identify-via systematic temporal discrimination of elementary electronic and structural processes-the dominant interaction. Specifically, we resolve the debates about the nature of two peculiar charge-density-wave states in the family of transition-metal dichalcogenides, and show that Rb intercalated 1T-TaS(2) is a Peierls insulator and that the ultrafast response of 1T-TiSe(2) is highly suggestive of an excitonic insulator.