Drexel

   Goran Karapetrov

Ultrafast dynamics in normal and CDW phase of NbSe2

(a) Transient reflectivity data taken at 3 K with the pump fluence of 0.5 mJ/cm2. Arrows indicate the coherent oscillations within the first picosecond. (b) Kinetic trace at λ=500 nm showing the coherent oscillations.

In this recent work we have performed broadband ultrafast optical pump-probe experiments in which we have varied laser fluence and temperature to explore the electron-phonon dynamics in NbSe2 single crystals. Displacive excitation of coherent phonons showed CDW-associated coherent oscillations of the soft phonon mode across the whole spectral range. Temperature evolution of this coherent phonon mode in the low-excitation linear regime shows softening of the mode down to the CDW transition temperature TCDW with subsequent hardening below TCDW. From first principle calculations of electron-phonon coupling we associate the few picosecond electron-phonon relaxation time τ2 with a specific group of phonons with frequencies around 20 meV. On the other hand, the anomalously long relaxation time of τ3~100 ps is associated with anharmonicity-driven phonon-phonon scattering. All relaxation processes result from anomalies near the second order CDW phase transition that are reflected in the temperature dependencies of the characteristic relaxation times and amplitudes of optical densities. At highest fluences we observe electronic melting of the CDW and disappearance of the mode hardening below TCDW. For more details see the manuscript