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Two-color terahertz (THz) generation is a field-matter process combining an optical pulse and its second harmonic. Its application in condensed matter is challenged by the lack of phase matching among multiple interacting fields. Here, we demonstrate phase-matching-free two-color THz conversion in condensed matter by introducing a highly resonant absorptive system. The generation is driven by a third-order nonlinear interaction localized at the surface of a narrow-band-gap semiconductor, and depends directly on the relative phase between the two colors. We show how to isolate the third-order effect among other competitive THz-emitting surface mechanisms, exposing the general features of the two-color process. [ABSTRACT FROM AUTHOR]

Two-color terahertz (THz) generation is a field-matter process combining an optical pulse and its second harmonic. Its application in condensed matter is challenged by the lack of phase matching among multiple interacting fields. Here, we demonstrate phase-matching-free two-color THz conversion in condensed matter by introducing a highly resonant absorptive system. The generation is driven by a third-order nonlinear interaction localized at the surface of a narrow-band-gap semiconductor, and depends directly on the relative phase between the two colors. We show how to isolate the third-order effect among other competitive THz-emitting surface mechanisms, exposing the general features of the two-color process.

Terahertz (THz) imaging is a rapidly emerging field, thanks to many potential applications in diagnostics, manufacturing, medicine and material characterisation. However, the relatively coarse resolution stemming from the large wavelength limits the deployment of THz imaging in micro- and nano-technologies, keeping its potential benefits out-of-reach in many practical scenarios and devices. In this context, single-pixel techniques are a promising alternative to imaging arrays, in particular when targeting subwavelength resolutions. In this work, we discuss the key advantages and practical challenges in the implementation of time-resolved nonlinear ghost imaging (TIMING), an imaging technique combining nonlinear THz generation with time-resolved time-domain spectroscopy detection. We numerically demonstrate the high-resolution reconstruction of semi-transparent samples, and we show how the Walsh-Hadamard reconstruction scheme can be optimised to significantly reduce the reconstruction time. We also discuss how, in sharp contrast with traditional intensity-based ghost imaging, the field detection at the heart of TIMING enables high-fidelity image reconstruction via low numerical-aperture detection. Even more striking-and to the best of our knowledge, an issue never tackled before-the general concept of "resolution" of the imaging system as the "smallest feature discernible" appears to be not well suited to describing the fidelity limits of nonlinear ghost-imaging systems. Our results suggest that the drop in reconstruction accuracy stemming from non-ideal detection conditions is complex and not driven by the attenuation of high-frequency spatial components (i.e., blurring) as in standard imaging. On the technological side, we further show how achieving efficient optical-to-terahertz conversion in extremely short propagation lengths is crucial regarding imaging performance, and we propose low-bandgap semiconductors as a practical framework to obtain THz emission from quasi-2D structures, i.e., structure in which the interaction occurs on a deeply subwavelength scale. Our results establish a comprehensive theoretical and experimental framework for the development of a new generation of terahertz hyperspectral imaging devices., Competing Interests: The authors declare no conflict of interest.

Nanohybrid materials based on nanoparticles of the intrinsically microporous polymer PIM-1 and graphene oxide (GO) are prepared from aqueous dispersions with a reprecipitation method, resulting in the surface of the GO sheets being decorated with nanoparticles of PIM-1. The significant blueshift in fluorescence signals for the GO/PIM-1 nanohybrids indicates modification of the optoelectronic properties of the PIM-1 in the presence of the GO due to their strong interactions. The stiffening in the Raman G peak of GO (by nearly 6 cm -1 ) further indicates p-doping of the GO in the presence of PIM. Kelvin probe force microscopy (KPFM) and electrochemical reduction measurements of the nanohybrids provide direct evidence for charge transfer between the PIM-1 nanoparticles and the GO nanosheets. These observations will be of importance for future applications of GO-PIM-1 nanohybrids as substrates and promoters in catalysis and sensing.

We introduce a method for diagnosing the electric surface potential of a semiconductor based on THz surface generation. In our scheme, that we name Optical Pump Rectification Emission, a THz field is generated directly on the surface via surface optical rectification of an ultrashort pulse after which the DC surface potential is screened with a second optical pump pulse. As the THz generation directly relates to the surface potential arising from the surface states, we can then observe the temporal dynamics of the static surface field induced by the screening effect of the photo-carriers. Such an approach is potentially insensitive to bulk carrier dynamics and does not require special illumination geometries.