Nanoparticles emitting two-photon luminescence are broadly used as photostable emitters for nonlinear microscopy. Second-harmonic generation (SHG) as another two-photon mechanism offers complementary optical properties but the reported sizes of nanoparticles are still large, of a few tens of nanometers. Herein, coherent SHG from single core/shell CdTe/CdS nanocrystals with a diameter of 10 to 15 nm is reported. The nanocrystal excitation spectrum reveals resonances in the nonlinear efficiency with an overall maximum at about 970 nm. Polarization analysis of the second-harmonic emission confirms the expected zinc blende symmetry, and allows extraction of the three-dimensional nanocrystal orientation. The small size of these nonlinearly active quantum dots, together with the intrinsic coherence and orientation sensitivity of the SHG process, are well adapted for ultrafast probing of optical near-fields with high resolution as well as for orientation tracking for bioimaging applications.

Single KTiOPO4 nanocrystals, isolated from a flux‐grown powder, efficiently generate a perfectly stable and blinking‐free second‐harmonic field under non‐resonant femtosecond optical excitation (see image). For each individual nanocrystal, size and three‐dimensional orientation are determined using combined atomic force microscopy and optical techniques.

We show that a dimer made of two gold nanospheres exhibits a remarkable efficiency for second-harmonic generation under femtosecond optical excitation. The detectable nonlinear emission for the given particle size and excitation wavelength arises when the two nanoparticles are as close as possible to contact, as in situ controlled and measured using the tip of an atomic force microscope. The excitation wavelength dependence of the second-harmonic signal supports a coupled plasmon resonance origin with radiation from the dimer gap. This nanometer-size light source might be used for high-resolution near-field optical microscopy.

We report an efficient colloidal synthesis of KTiOPO4 (KTP) nanocrystals with excellent crystallinity and the direct observation of optical second-harmonic generation (SHG) from discrete KTP nanocrystals in neurons cultured from mammalian brain cortex. Direct internalization and monitoring of these nanoparticles was successfully achieved without limitations from cytotoxicity, bleaching and blinking emission.

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We demonstrate the direct imaging of the second harmonic generation radiation from a single nonlinear nanocrystal using defocused nonlinear microscopy. This technique allows the retrieval of complete information on the 3D orientation of a nanocrystal as well as possible deviations from its purely crystalline nature, in a simple experimental implementation. The obtained images are modeled by calculation of the radiation diagram from a nonlinear dipole that accounts for the excitation beam, the crystal symmetry and the particle size. Experimental demonstrations are performed on Potassium Titanyl Phosphase (KTP) nanocrystals. The shape and structure of the radiation images show a strong dependence on both crystal orientation and field polarization state, as expected by the specific nonlinear coherent coupling between the induced dipole and the excitation field polarization state.

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We have detected, by using stimulated emission, an atomic parity violation (APV) in the form of a chiral optical gain of a cesium vapor on the 7S-6P(3/2) transition, consecutive to linearly polarized 6S-7S excitation. We demonstrate the validity of this detection method of APV, by presenting a 9% accurate measurement of expected sign and magnitude. We stress several advantages of this new approach which fully exploits the cylindrical symmetry of the setup. Future measurements at the percent level will provide an important cross-check of an existing more precise result obtained by a different method.