Arbitrary manipulation of broadband terahertz waves with flexible polarization shaping at the source has great potential in expanding numerous applications, such as imaging, information encryption, and all-optical coherent control of terahertz nonlinear phenomena. Topological insulators featuring unique spin-momentum–locked surface state have already exhibited very promising prospects in terahertz emission, detection, and modulation, which may lay a foundation for future on-chip topological insulator-based terahertz systems. However, polarization-shaped terahertz emitters based on topological insulators with an arbitrarily manipulated temporal evolution of the amplitude and the electric-field vector direction have not yet been explored. We systematically investigated the terahertz radiation from topological insulator Bi2Te3 nanofilms driven by femtosecond laser pulses and successfully realized the generation of efficient chiral terahertz waves with controllable chirality, ellipticity, and principal axis. The convenient engineering of the chiral terahertz waves was interpreted by a photogalvanic effect (PGE)-induced photocurrent, while the linearly polarized terahertz waves originated from linear PGE-induced shift currents. Our work not only provides further understanding of femtosecond coherent control of ultrafast spin currents but also describes an effective way to generate spin-polarized terahertz waves at the source.
Femtosecond control of electron spin not only promises the capability of satisfying the ever-increasing demand of storage information and ultrafast manipulation of magnetization in mediums, but also delivering controllable, highlyefficient, cost-effective and compact terahertz sources. Femtosecond spin dynamics have been extensively investigated these years with the methods of ultrafast magnetic-optical Kerr effect, inverse Faraday effect, inverse spin Hall effect and so on. Recently emerged coherent terahertz emission spectroscopy can also be employed to study this ultrafast spin dynamics with its unique advantages. For example, terahertz emission spectroscopy is a coherent, time-resolved, contactless Ampere-meter, which can be used to deduce the spin-charge conversion. However, femtosecond laser interaction with magnetic mediums is a rather complex process, there are still lots of physical mechanisms waiting to be unveiled. Here, we systematically investigate the femtosecond spin dynamics in ferromagnetic materials via polarization-resolved terahertz emission spectroscopy. We obtain detectable electromagnetic field radiation with its polarization parallel to the external magnetic field direction, which was not observed in the same materials in previous work. Inverse spin-orbit torque tilting is responsible for the observed phenomenon. Based on this mechanism, the efficiency and polarization of the generated terahertz waves can be coherently controlled and manipulated not only by the external magnetic fields, but also by the sample structures and the pumping femtosecond laser pulses. Our work not only helps further deepen understanding of the physical mechanism of all-optical magnetization reversal, boosting future spin recording technology, but also offers a very promising way for developing novel and efficient terahertz functional sources and devices.
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