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Information technology demands high-speed optoelectronic devices, but goingbeyond the one terahertz (THz) barrier is challenging due to the difficultiesassociated with generating, detecting, and processing high-frequency signals.Here, we show that femtosecond-laser-driven phonons can be utilized tocoherently manipulate the excitonic properties of semiconductors at THzfrequencies. The precise control of the pump and subsequent time-delayedbroadband probe pulses enables the simultaneous generation and detectionprocesses of both periodic lattice vibrations and their couplings withelectronic states. Combining ultralow frequency Raman spectroscopy withfirst-principles calculations, we identify the unique phonon mode-selective andprobe-energy dependent features of electron-phonon interactions in layeredPdSe2. Two distinctive types of coherent phonon excitations could couplepreferentially to different types of electronic excitations: the intralayer(4.3 THz) mode to carriers and the interlayer (0.35 THz) mode to excitons. Thiswork provides new insights to understand the excited-state phonon interactionsof 2D materials, and to achieve future applications of optoelectronic devicesoperating at THz frequencies.

Phonon-assisted electronic states modulation of few-layer PdSe2 at terahertz frequencies