Spectral Phase Control of Interfering Chirped Pulses for High-Energy Narrowband Terahertz Generation

Abstract

Highly-efficient optical generation of narrowband terahertz (THz) radiation enables unexplored technologies and sciences from compact electron acceleration to charge manipulation in solids. State-of-the-art conversion efficiencies are currently achieved using difference-frequency generation (DFG) driven by temporal beating of chirped pulses but remain, however, far lower than desired or predicted. Here we show that high-order spectral phase fundamentally limits the efficiency of narrowband DFG using chirped-pulse beating and resolve this limitation by introducing a novel technique based on tuning the relative spectral phase of the pulses. For optical terahertz generation, we demonstrate a 13-fold enhancement in conversion efficiency for 1%-bandwidth, 0.361 THz pulses, yielding a record energy of 0.6 mJ and exceeding previous optically-generated energies by over an order of magnitude. Our results prove the feasibility of millijoule-scale applications like terahertz-based electron accelerators and light sources and solve the long-standing problem of temporal irregularities in the pulse trains generated by interfering chirped pulses.

arXiv comment25 pages, 5 figures, updated to the state before review at Nature Communications (updated the affiliations, title, some content, methods, etc.)

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• Cascaded Multi-cycle terahertz driven ultrafast electron acceleration and manipulation
• Highly efficient narrowband terahertz generation driven by a two-spectral-line laser in PPLN
• Multicycle terahertz pulse generation by optical rectification in LiNbO${}_3$, LiTaO${}_3$, and BBO crystals
• Hyper Spectral Resolution Stimulated Raman Spectroscopy with Amplified fs Pulse Bursts
• Generation of 0.7 mJ multicycle 15 THz radiation by phase-matched optical rectification in lithium niobate
• Raman Shifting induced by Cascaded Quadratic Nonlinearities for Terahertz Generation
• Coherent generation and control of tunable narrowband THz radiation from laser-induced air-plasma filament
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• Fiber-based mid-infrared frequency-swept laser at 50 MScans/s via frequency down-conversion of time-stretched pulses
• Self-calibration technique for characterization of integrated THz waveguides
• 35 megawatt multicycle THz pulses from a homemade periodically poled macrocrystal
• Accurate simulation of THz generation with Finite-Element Time Domain methods
• Combined tools for Particle-In-Cell simulations performed with transversely asymmetric chirped lasers