A rapidly-growing interest in WTe2 has been triggered by the giant magnetoresistance effect discovered in this unique system. While many efforts have been made towards uncovering the electron- and spin-relevant mechanisms, the role of lattice vibration remains poorly understood. Here, we study the coherent vibrational dynamics in WTe2 crystals by using ultrafast pump-probe spectroscopy. The oscillation signal in time domain in WTe2 has been ascribed as due to the coherent dynamics of the lowest energy A1 optical phonons with polarization- and wavelength-dependent measurements. With increasing temperature, the phonon energy decreases due to anharmonic decay of the optical phonons into acoustic phonons. Moreover, a significant drop (15%) of the phonon energy with increasing pump power is observed which is possibly caused by the lattice anharmonicity induced by electronic excitation and phonon-phonon interaction.
We introduce a novel configuration for two-dimensional electronic spectroscopy (2DES) that combines the partially collinear pump-probe geometry with active phase locking. We demonstrate the method on a solution sample of CdSe/ZnS nanocrystals by employing two non-collinear optical parametric amplifiers as the pump and probe sources. The two collinear pump pulse replicas are created using a Mach-Zehnder interferometer phase stabilized by active feedback electronics. Taking the advantage of separated paths of the two pump pulses in the interferometer, we improve the signal-to-noise ratio with double modulation of the individual pump beams. In addition, a quartz wedge pair manipulates the phase difference between the two pump pulses, enabling the recovery of the rephasing and non-rephasing signals. Our setup integrates many advantages of available 2DES techniques with robust phase stabilization, ultrafast time resolution, two-color operation, long delay scan, individual polarization manipulation and the ease of implementation.
Two-dimensional electronic spectroscopy (2DES) is a powerful method to probe the coherent electron dynamics in complicated systems. Stabilizing the phase difference of the incident ultrashort pulses is the most challenging part for experimental demonstration of 2DES. Here, we present a tutorial review on the 2DES protocols based on active phase managements which are originally developed for quantum optics experiments. We introduce the 2DES techniques in box and pump-probe geometries with phase stabilization realized by interferometry, and outline the fully collinear 2DES approach with the frequency tagging by acoustic optical modulators and frequency combs. The combination of active phase managements, ultrashort pulses and other spectroscopic methods may open new opportunities to tackle essential challenges related to excited states.
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