Abstract
Ultrashort light pulses can selectively excite charges, spins, and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge-density wave (CDW) material 1T-TaSe2 After exciting the material with a femtosecond pulse, fast spatial smearing of the laser-excited electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This finding is in contrast to all previous observations in multiple materials to date, where the electron temperature decreases monotonically via electron-phonon scattering. By tuning the laser fluence, the magnitude of the electron temperature modulation changes from ∼200 K in the case of weak excitation, to ∼1,000 K for strong laser excitation. We also observe a phase change of π in the electron temperature modulation at a critical fluence of 0.7 mJ/cm2, which suggests a switching of the dominant coupling mechanism between the coherent phonon and electrons. Our approach opens up routes for coherently manipulating the interactions and properties of two-dimensional and other quantum materials using light.
Highlights
Ultrashort light pulses can selectively excite charges, spins, and phonons in materials, providing a powerful approach for manipulating their properties
As a prototypical charge-density wave (CDW) material, 1T-TaSe2 is a layered dichalcogenide consisting of hexagonal Ta and Se layers
We discuss how the electron temperature could be modulated coherently by the CDW amplitude mode, and what might give rise to the change in phase of π observed between the Te modulation and band shift at the critical laser fluence
Summary
Ultrashort light pulses can selectively excite charges, spins, and phonons in materials, providing a powerful approach for manipulating their properties. We use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge-density wave (CDW) material 1T-TaSe2. After exciting the material with a femtosecond pulse, fast spatial smearing of the laser-excited electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. Midinfrared or terahertz (THz) pulses can resonantly excite selected phonons in a material, to induce interesting new phenomena such as enhanced superconductivity [6,7,8,9], hidden states [10], and phonon upconversion [11] Such sophisticated excitations require precise knowledge of the phonon spectrum and fine-tuning of the THz excitation field.
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