High-contrast coercive field engineering for periodic poling of RbKTiOPO4 with Ba2+/K+ ion-exchange.

We investigate a new method of coercive field engineering for periodic poling of RbKTiOPO4 (RKTP). By ion exchanging RKTP in a molten salt containing 7 mol% Ba(NO3)2 and 93 mol% KNO3 we achieve more than an order of magnitude difference in polarization switching time between the exchanged and non-exchanged regions. This method is used to fabricate periodic gratings of 2.92 µm in 1 mm thick bulk RKTP for second harmonic generation at 779 nm with a normalized conversion efficiency of 2%/Wcm. We show that the poled domain structures are stable at 300 °C, and that there is no bulk refractive index modification associated with the periodic ion exchange.

Efficient first-order quasi-phase-matched backward second-harmonic generation.

We demonstrate first-order quasi-phase-matched backward second-harmonic generation (BSHG) with an efficiency of 18.7%. This represents an increase by two orders of magnitude from earlier experiments employing higher-order quasi-phase-matching. The efficient BSHG is demonstrated in bulk periodically poled Rb:KTiOPO4 with a poling period of 317 nm. Using these structures, the frequency doubling in the backward direction is achieved for the fundamental wavelength of 2309 nm. Here we report on the experimental investigation of the BSHG properties such as spectral bandwidth, temperature tuning, and temperature bandwidth by employing broadband and narrowband fundamental wavelength sources. The BSHG properties are compared with those of co-propagating second harmonic generation to reveal the BSHG potential for novel applications that were proposed theoretically but have not been realized in practice so far.

Feature issue introduction: advanced solid-state lasers.

This joint issue of Optics Express and Optical Materials Express features 36 state-of-the art articles written by authors who participated in the international conference advanced solid state lasers held online from October 3-7, 2021. This review provides a summary of these articles covering a wide spectrum of topics around solid-state lasers from materials research to sources and from design innovation to applications.

µJ-level multi-cycle terahertz generation in a periodically poled Rb:KTP crystal.

We demonstrate multi-cycle terahertz (MC-THz) generation in a 15.5 mm long periodically poled rubidium (Rb)-doped potassium titanyl phosphate (Rb:PPKTP) crystal with a poling period of 300 µm. By cryogenically cooling the crystal to 77 K, up to 0.72 µJ terahertz energy is obtained at a frequency of 0.5 THz with a 3 GHz bandwidth. A maximum internal optical-to-terahertz conversion efficiency of 0.16% is achieved, which is comparable with results achieved using periodically poled lithium niobate crystal. Neither photorefractive effects nor damage was observed with up to 900mJ/cm2, showing the great potential of Rb:PPKTP for multi-millijoule-level MC-THz generation.

Ion-exchanged waveguides in periodically poled Rb-doped KTiOPO4 for efficient second harmonic generation.

An ion-exchange process has been developed for periodically poled Rb-doped KTiOPO4 (RKTP) which warrants high efficiency and low loss channel waveguides. The domain stability was investigated, and it was found that domain gratings with uncharged walls could stand the ion-exchange process without deterioration. 3.1 mW of blue second harmonic light was generated from 74 mW of radiation at 940.2 nm coupled into an 8 µm wide and 7 mm long waveguide, corresponding to a normalized conversion efficiency of 115%/Wcm2. Waveguides in PPRKTP open the possibility for stable operation at high optical powers, as well as generating entangled photons at low optical powers, and enable the investigation of novel nonlinear processes such as counter-propagating interactions in a waveguide format.

Development and experimental demonstration of negative first-order quasi-phase matching in a periodically poled Rb-doped KTiOPO4 crystal.

We worked on a new scheme of quasi-phase matching (QPM) based on the negative first order of the spatial modulation of the sign of the second-order nonlinearity. Applying this scheme in the case of angular-QPM (AQPM) in a biaxial crystal reveals new directions of propagation for efficient parametric frequency conversion as well as "giant" spectral acceptances. The experimental validation is performed in a periodically poled rubidium-doped KTiOPO4 biaxial crystal. This new approach naturally extends to other periodically poled uniaxial crystals such as periodically poled LiNbO3.

High resolution and sensitivity up-conversion mid-infrared photon-counting LIDAR.

A single-photon-counting mid-infrared LIDAR is presented. 2.4 µm mid-infrared photons were up-converted to 737 nm by intra-cavity mixing in a periodically poled rubidium-doped KTiOPO4 crystal inside a Nd:YVO4 laser. The up-converted photons were detected by a Si single-photon avalanche photodiode (SPAD). A temporal resolution of 42 ps and a dark count rate of 500 Hz were achieved, limited by the SPAD and ambient light leakage. It allowed for detection of two targets separated by only a few millimeters. This technique is easily extendable to longer wavelengths, limited primarily by the nonlinear crystal transparency.

Coherent phase transfer and pulse compression at 1.4 µm in a backward-wave OPO.

The frequency modulation transfer property of a backward-wave optical parametric oscillator (BWOPO) is investigated in the context of near-IR pulse compression. The maximum transferrable bandwidth from the pump to the forward wave in a BWOPO is determined by the group dispersion mismatch. In comparison, the third-order phase introduced in a single-grating compressor setup is more detrimental to achieve optimum compression of the BWOPO forward wave. Nevertheless, we demonstrate a 220 GHz bandwidth transfer from 800 nm to 1.4 µm, with a compression factor of 115, leading to near-IR pulses as short as 1.3 ps with µJ energy.

Narrowband, tunable, infrared radiation by parametric amplification of a chirped backward-wave OPO signal.

The strict momentum conservation constraints for backward-wave optical parametric oscillators (BWOPOs) gives an inherently narrowband backward-generated wave, even with broadband pumping. Unfortunately, the limited tuning range of this wave restricts potential applications. Here we demonstrate a method to circumvent this restriction and increase the tuning range by more than one order of magnitude. A linearly chirped pump modulation is transferred to the forward-generated BWOPO wave, which is then mixed with an identically chirped pump in a conventional optical parametric amplifier to obtain narrowband (38 GHz), broadly tunable, infrared radiation around 1.86 µm, with an output energy of 19 µJ.

Flexoelectric Fracture-Ratchet Effect in Ferroelectrics.

The propagation front of a crack generates large strain gradients and it is therefore a strong source of gradient-induced polarization (flexoelectricity). Herein, we demonstrate that, in piezoelectric materials, a consequence of flexoelectricity is that crack propagation is helped or hindered depending on whether it is parallel or antiparallel to the piezoelectric polar axis. The discovery of crack propagation asymmetry proves that fracture physics cannot be assumed to be symmetric in polar materials, and indicates that flexoelectricity should be incorporated in any realistic model.

Validation of the angular quasi-phase-matching theory for the biaxial optical class using PPRKTP.

We report the first experimental validation of angular quasi-phase-matching (AQPM) theory in a biaxial crystal by performing second-harmonic generation (SHG) in the periodically-poled Rb-doped KTiOPO4 (PPRKTP) crystal cut as a sphere. Both AQPM and birefringence phase-matching (BPM) angles were measured thanks to a Kappa circle.

Elasticity Modulation Due to Polarization Reversal and Ionic Motion in the Ferroelectric Superionic Conductor KTiOPO4.

The coupling between ionic degrees of freedom and ferroelectricity has received renewed attention in recent years, given that surface electrochemical processes have been shown to be intrinsically linked to ferroelectric phase stability in ultrathin ferroelectric films. However, the coupling between bulk ionic transport and local polarization switching has received less attention, as typically the bulk ionic mobilities are low for common ferroelectrics at room temperature. Here, we use the coupled band-excitation method in conjunction with site-correlated time-of-flight secondary ion mass spectrometry, to determine the coupling between ferroelectric switching and ionic motion in single crystal KTiOPO4. The local scanning probe measurements indicate a substantial softening, as determined by resonant frequency changes, during reversal of polarization along one direction. These changes are correlated with the mass spectrometry measurements, showing a polarization-dependent accumulation of K ions at the polar surfaces, thus corroborating their role in the screening process. These studies shed light on the interplay between ionic dynamics and bulk ferroelectric switching and have implications for studies on domain wall conductivity, chemical switching, and bulk and surface-screening phenomena.

Quasi-phase matched second harmonic generation in periodically poled Rb-doped KTiOPO4 ridge waveguide.

A 10.8 µm wide ridge waveguide was fabricated by diamond-blade dicing in an ion-exchanged periodically poled Rb-doped KTiOPO4 sample. The waveguide was used to generate blue second harmonic light at 468.8 nm in the TM00 mode through first order Type I quasi-phase matching, exploiting the large d33 coefficient of the crystal. It was evaluated using a cw Ti:Sapphire laser, and 6.7 µW of blue light was generated with 5.8 mW of fundamental radiation at 933.8 nm coupled through the waveguide. The results presented here pave the way for efficient nonlinear processes in a waveguide format.

Highly efficient mirrorless optical parametric oscillator pumped by nanosecond pulses.

A highly efficient mirrorless optical parametric oscillator (MOPO), pumped by narrowband nanosecond pulses at 1064 nm, is demonstrated. The MOPO is based on quasi-phase-matched parametric interaction of counter-propagating photons in 1-mm-thick periodically poled Rb-doped KTiOPO4 crystal with a period of 755 nm. It generates a co-propagating signal at 1740 nm and a counter-propagating idler at 2741 nm, achieving mJ-level output with a total signal-and-idler conversion efficiency of 47%. Both generated waves present narrow spectral bandwidths, thanks to the unique properties of the counter-propagating nonlinear interaction. The high conversion efficiency, inherently narrow spectral width, and simplicity of the optical setup make the MOPO an attractive alternative to conventional co-propagating optical parametric oscillators.

Cascaded counter-propagating nonlinear interactions in highly-efficient sub-µm periodically poled crystals.

Mirrorless optical parametric oscillators (MOPOs) are very attractive parametric devices that rely on the nonlinear interaction of counter-propagating photons to inherently establish distributed feedback, without the use of external mirrors or surface coatings. These devices offer unique spectral and coherence properties that will benefit a large variety of applications ranging from spectroscopy to quantum communications. The major obstacle in exploiting their full potential is ascribed to the difficulty in engineering a nonlinear material in which the generation of counter-propagating waves can be phase matched. Here we present a reliable and consistent technique for fabrication of highly-efficient sub-micrometer periodically poled Rb-doped KTiOPO4. We experimentally demonstrate the first cascaded counter-propagating interactions in which the generated forward signal serves as a pump for a secondary MOPO process, reaching pump depletion larger than 60%. The cascaded process exemplifies the high efficiency of our nonlinear photonic structures. Our domain-engineering technique paves the way to realize counter-propagating schemes and devices that have been deemed unfeasible until now.

Fully-resonant, tunable, monolithic frequency conversion as a coherent UVA source.

We demonstrate a monolithic frequency converter incorporating up to four tuning degrees of freedom, three temperature and one strain, allowing resonance of pump and generated wavelengths simultaneous with optimal phase-matching. With a Rb-doped periodically-poled potassium titanyl phosphate (KTP) implementation, we demonstrate efficient continuous-wave second harmonic generation from 795 to 397, with low-power efficiency of 72% and high-power slope efficiency of 4.5%. The measured performance shows good agreement with theoretical modeling of the device. We measure optical bistability effects, and show how they can be used to improve the stability of the output against pump frequency and amplitude variations.

Counter-propagating parametric interaction with phonon-polaritons in periodically poled KTiOPO4.

Strongly enhanced backward stimulated polariton scattering (BSPS) is demonstrated in periodically-poled KTiOPO4 (KTP) crystals with a high power-conversion efficiency up to 70%. We study the physical mechanism of such counter-propagating parametric interaction with phonon-polaritons in χ(2) modulated structures. BSPS is a three-wave mixing that is distinguished from backward stimulated Raman scattering (BSRS), while a strong absorption at large polariton wave-vectors can still make BSPS display certain characteristics of BSRS such as self-compression of the Stokes pulse. We also compare BSPS with counter-propagating parametric oscillation in the near- and mid-infrared range, providing an estimation of the fabrication error margin to expect the outcome of their competition in the same device.

Periodic poling of Rb-doped KTiOPO4 by coercive field engineering.

We demonstrate fine-pitch periodic poling of bulk Rb-doped KTiOPO4 using a coercive field grating induced by ion-exchange. These samples were used for quasi phase matched (QPM) second harmonic generation at 795 nm with a normalized conversion efficiency of 1.7% W-1cm-1. Additionally, the ion-exchange introduced a refractive index change over the sample thickness resulting in a phasematching wavelength shift of 0.21 nm, adding extra tunability to the QPM device.

Parametric down-conversion with nonideal and random quasi-phase-matching.

Quasi-phase-matching (QPM) has enriched the capacity of parametric down-conversion (PDC) in generating biphotons for many fundamental tests and advanced applications. However, it is not clear how the nonidealities and randomness in the QPM grating of a parametric down-converter may affect the quantum properties of the biphotons. This paper intends to provide insights into the interplay between PDC and nonideal or random QPM structures. Using a periodically poled nonlinear crystal with short periodicity, we conduct experimental and theoretical studies of PDC subject to nonideal duty cycle and random errors in domain lengths. We report the observation of biphotons emerging through noncritical birefringent-phasematching, which is impossible to occur in PDC with an ideal QPM grating, and a biphoton spectrum determined by the details of nonidealities and randomness. We also observed QPM biphotons with a diminished strength. These features are both confirmed by our theory. Our work provides new perspectives for biphoton engineering with QPM.

Studies of sub-millisecond domain dynamics in periodically poled Rb-doped KTiOPO(4), using online in situ second harmonic generation.

The temporal evolution of in situ second-harmonic generation was employed to study domain dynamics during periodic poling in Rb-doped KTP. With this method we investigated the influence of various poling parameters, including electric-field pulse shape, pulse magnitude, and number of pulses, on the quality of the QPM structure. It was found that the grating formation can be a sub-millisecond process and the benefits of using symmetric triangular electric-field pulse shape over square pulse shape in the single-pulse poling regime were demonstrated. Multiple-pulse poling with triangular pulses was shown to have a detrimental effect on the QPM structure quality, while multiple square pulses can provide additional flexibility to the structuring process.