Sum-frequency Generation Process Research Articles

Effective nonlinearity of trigonal BaGa2GeS6

Implementing second-harmonic and sum-frequency generation processes with a specially oriented sample, we determine the magnitude and sign of the nonlinear optical coefficients d11, d22, and d31 of the recently developed trigonal BaGa2GeS6. We conclude that it is a viable alternative to the widely used chalcopyrite AgGaS2 for 1 µm pumped frequency downconversion to the mid-IR spectral range.

Wideband and low-spurious optical waveform generator for optically addressable quantum systems manipulation and control

Optical manipulation of quantum systems requires stable laser sources able to produce complex waveforms over a large frequency range. In the visible region, such waveforms can be generated using an acousto-optic modulator driven by an arbitrary waveform generator, but these suffer from a limited tuning range typically of a few tens of MHz. Visible-range electro-optic modulators are an alternative option offering a larger modulation bandwidth, however they have limited output power which drastically restricts the scalability of quantum applications. There is currently no architecture able to perform phase-stabilized waveforms over several GHz in the visible or near infrared region while providing sufficient optical power for quantum applications. Here we propose and develop a modulation and frequency conversion set-up able to deliver optical waveforms over a large frequency range, with a high spurious extinction ratio, scalable to the entire visible/near infrared region with high optical power. The optical waveforms are first generated at telecom wavelength and then converted to the emitter wavelength through a sum frequency generation process. By adapting the pump laser frequency, the optical waveforms can be tuned to interact with a broad range of optical quantum emitters or qubits such as alkali atoms, trapped ions, rare earth ions, or fluorescent defects in solid-state matrices. Using this architecture, we were able to detect and study a single erbium ion in a nanoparticle. We also generated high bandwidth signals at 606 nm, which would enable frequency multiplexing of on-demand read-out Pr3+:Y2SiO5 quantum memories.

Analytical solution to second-harmonic generation of ultrashort laser pulse

We present an analytical method to evaluate the second-harmonic generation (SHG) process of ultrashort laser pulses in a nonlinear medium within the small-signal regime. Building upon the broadband nonlinear coupled wave theory, we derive an analytical solution that allows one to investigate the fundamental physics and detailed dynamics of the nonlinear interaction between ultrashort laser pulses. We find that SHG for ultrashort laser pulses in a nonlinear crystal arises from a series of self-SHG and self sum-frequency generation processes involving different frequency components. We have applied the analytical method to investigate specific pulse profiles with Gaussian and sech functions and found good agreement between analytical theory and numerical simulations, validating the accuracy of the analytical approach. The analytical method enables one to explore the evolution of the second-harmonic wave under various pulse profiles, pulse widths, and crystal thicknesses, and offers a more efficient and insightful approach to study the nonlinear optical dynamics of ultrashort laser pulses.

One to many one-way control in quadripartite asymmetric Einstein-Podolsky-Rosen steering

Einstein–Podolsky–Rosen (EPR) steering is different from quantum entanglement because of its unique asymmetry. Multipartite asymmetric EPR steering can break through one-to-one monogamy steering and achieve one to many one-way steering. That is to say, the state of one part can steer the other rest parts simultaneously, while the other parts cannot steer this part. Here, a scheme is proposed to generate one to many one-way steering by optical parametric amplification cascaded with a sum-frequency generation process. One to many non-monogamy EPR steering, such as one to two and one to three one-way steering are demonstrated based on the criterion for asymmetric EPR steering. It is also find that different kinds of asymmetric EPR steering can be obtained by choosing different nonlinear parameters. This non-monogamous one to many quantum control has potential application in constructing quantum networks and realizing one-way quantum computing.

Sum-frequency generation and amplification processes in semiconductor superlattices

Semiconductor superlattices are very well-known structures due to their specific electron transport properties, making them extremely attractive to be employed in electronic or optoelectronic devices. The interest in such structures has been recently additionally stirred up due to the first successful experimental demonstration of parametric gain in GaAs/AlGaAs superlattices, resulting in the generation of harmonics, half-harmonics and fractional harmonics. This invention paves the way for a successful realization of superlattice-based generators and amplifiers up to the terahertz frequency range. Despite the emerging experimental results and decade-long theoretical research, unresolved aspects, related to the physical processes inside the superlattices, persist. Lately, the biasing effect was extensively analysed for the case of degenerate processes in the superlattice; however, the non-degenerate case was left out of frame until now. Within this research, we further expand the boundaries of previous investigation by exploring the differences of non-degenerate processes. The study uncovers the asymmetry appearance of the probe field vs. relative phase dependences as well as the possibility of parametric fractional frequency generation. Finally, the concept of energy reflow between two participating probes is predicted and discussed.

Sum-frequency generation at interfaces: A Fresnel story. I. Designing high contrast in two interface systems.

When a homogeneous film of finite thickness is optically probed, interference due to multiple reflections modulates in amplitude the electric field of light. For optical processes located only at the interfaces between two media, as is common for Sum-Frequency Generation (SFG), interference also modulates the contrast between signals generated at the entrance and exit planes of the film. We introduce a universal formalism for Fresnel factors, which bear all the information about interference, valid at any point in a three-layer system and for the three beams involved in the SFG process. Their analysis provides general rules for obtaining a high contrast. In particular, we define four configurations leading to the cancellation of the SFG response from the entrance side of the film when its thickness or the angles of incidence are tuned. Cancellation conditions depend on the polarization of light and follow simple analytical rules, leading to a straightforward experimental implementation. Such a selective cancellation makes it possible to independently measure single components of the nonlinear susceptibility, for example, in a ppp experiment and to separate surface from bulk response by combining a few measurements.

Sum-frequency generation at interfaces: A Fresnel story. II. Analytical expressions for multilayer systems.

The well-known formalism for Sum-Frequency Generation (SFG) reflected or transmitted by a three-layer system involves three equations defining the emitted SFG intensity, the effective nonlinear susceptibility, and a set of Fresnel factors specific to the three-layer system. We generalize the equations to an N-layer system, where all media have non-vanishing thicknesses, by leaving the first two equations unchanged and modifying only the Fresnel factors. These universal Fresnel factors bear all the complexity of light propagation and interference in the system, in amplitude and phase. They are analytically known anywhere in the N-layer system, either at any interface or in any of the bulks, and share common expressions for the three beams, incoming or emitted, of the SFG process in reflection. Enclosing an ultrathin layer (e.g., a molecular monolayer) in the system does not modify the Fresnel factors except for boundary conditions at this layer, as in the three-layer case. Specific rules are elaborated to simplify systems containing macroscopic layers. Equations for the four- and five-layer systems are explicitly provided. Simulations in the four-layer system allow for the recovery of the results of the transfer matrix formalism at a lower complexity cost for SFG users. Finally, when several interfaces in the system produce SFG signals, we show that it is possible to probe only the most buried one by canceling all the SFG responses except at this last interface, generalizing the results of the three-layer system.

Electric double layer contribution to sum frequency generation signal from Au electrode.

Understanding the electric double layer (EDL) of the metal electrode-electrolyte interface is essential to electrochemistry and relevant disciplines. In this study, potential-dependent electrode Sum Frequency Generation (SFG) intensities of polycrystalline gold electrodes in HClO4 and H2SO4 electrolytes were thoroughly analyzed. The potential of zero charges (PZC) of the electrodes was -0.06 and 0.38V in HClO4 and H2SO4, respectively, determined from differential capacity curves. Without specific adsorption, the total SFG intensity was dominated by the contribution from the Au surface and increased similar to that of the visible (VIS) wavelength scanning, which pushed the SFG process closer to the double resonant condition in HClO4. However, the EDL contributed about 30% SFG signal with specific adsorption in H2SO4. Below PZC, the total SFG intensity was dominated by the Au surface contribution and increased with potential at a similar slope in these two electrolytes. Around PZC, as the EDL structure became less ordered and the electric field changed direction, there would be no EDL SFG contribution. Above PZC, the total SFG intensity increased much more rapidly with potential in H2SO4 than in HClO4, which suggested that the EDL SFG contribution kept increasing with more specific adsorbed surface ions from H2SO4.

Proposal of optically tunable and reconfigurable multi-channel bandstop filter using sum-frequency generation in a PPLN waveguide

A multi-wavelength bandstop filter is proposed and numerically demonstrated using the sum-frequency generation (SFG) process in a waveguide of periodically poled lithium niobate (PPLN). This proposed device achieves channels number reconfigurable, central filtering wavelength of each filtering channel independently tunable and extinction ratios (ERs) equalized via all-optical methods.

Photo-induced cascaded harmonic and comb generation in silicon nitride microresonators.

Silicon nitride (Si3N4) is an ever-maturing integrated platform for nonlinear optics but mostly considered for third-order [χ(3)] nonlinear interactions. Recently, second-order [χ(2)] nonlinearity was introduced into Si3N4 via the photogalvanic effect, resulting in the inscription of quasi-phase-matched χ(2) gratings. However, the full potential of the photogalvanic effect in microresonators remains largely unexplored for cascaded effects. Here, we report combined χ(2) and χ(3) nonlinear effects in a normal dispersion Si3N4 microresonator. We demonstrate that the photo-induced χ(2) grating also provides phase-matching for the sum-frequency generation process, enabling the initiation and successive switching of primary combs. In addition, the doubly resonant pump and second-harmonic fields allow for effective third-harmonic generation, where a secondary optically written χ(2) grating is identified. Last, we reach a broadband microcomb state evolved from the sum-frequency-coupled primary comb. These results expand the scope of cascaded effects in microresonators.

Long-wave infrared to short-wave infrared upconversion through sum-frequency generation in a silicon symmetric metasurface integrated with two-dimensional material

Optical resonances supported by subwavelength nanostructures have significant local-field enhancement effects and are important in the field of nanophotonics such as photoemission and nonlinear optics. In this paper, silicon metasurface with toroidal dipole resonance in the short-wave infrared band is investigated. The formation and properties of the high-quality toroidal dipole resonance are analyzed in detail by the near- and far-field analysis, and the electromagnetic multipole decomposition methods in the metasurface with different structural parameters. In addition, a layer of two-dimensional nonlinear material GaSe is combined with the silicon metasurface, to enhance the long-wave infrared to short-wave infrared upconversion by the nonlinear sum-frequency generation (SFG) process through toroidal dipole resonance. The upconversion efficiency in the GaSe/ silicon metasurface bilayer system is nearly a thousand times more than that in the GaSe/planar silicon bilayer system, indicating the effectiveness of the toroidal dipole resonance generated by the metasurface. This method provides a feasible and viable strategy for upconverting mid-wave infrared or long-wave infrared to near- or short-wave infrared by the nonlinear process induced by the metasurface, which is potentially very attractive for the sensing and imaging of long-wavelength photons that beyond the capability of mature silicon/germinium detectors.

Energy-transfer controlled dual-wavelength visible laser generation based on parallel nonlinear frequency up-conversions

A compact frequency up-conversion scheme is demonstrated for dual-wavelength visible laser generation. The parallel sum-frequency generation (SFG) and second-harmonic generation (SHG) processes are simultaneously phase-matched and integrated in a well-designed periodically poled MgO:LiNbO3 crystal. Concurrent nonlinear up-conversions of the coupled SFG and SHG are thus realized. In the proof-of-principle experiment, two near-IR lasers at wavelengths of 800 nm and 1180 nm were used as independent fundamental beams. As a result, the generation of blue light at ∼477 nm by SFG (800 nm + 1180 nm → 477 nm) and the orange light at ∼590 nm by SHG of 1180 nm (1180 nm + 1180 nm → 590 nm) was simultaneously achieved. Finally, it is proved the relative strength of these two coupled nonlinear interactions and consequently the relative power of the blue and orange light could be freely controlled by changing the pump intensities of the fundamental beams, and a maximum photon conversion efficiency (∼25%) comparable to that of the separated SHG process was observed for this simultaneous dual-up-conversion device. This result provides a promising strategy for developing high-efficiency multi-wavelength visible laser systems. Combined with an engineered QPM crystal with different poling periods in sequence, more prospective nonlinear applications may be realized based a series of cascaded single- and dual-QPM nonlinear processes.

Detuning modulated composite segments for robust optical frequency conversion

The creation of efficient broadband frequency conversion devices while maintaining robustness to manufacturing and setup errors is crucial for accurate multiphoton spectroscopy, broadband imaging and the design of robust optical sources. Traditionally, nonlinear optical conversion processes are either efficient but narrowband or broadband but with low photon conversion yield. Several methods have been introduced in recent years to obtain both with great success, among them we can find adiabatic frequency conversion and Shaka–Pines composite segmented design. Here, we expand the composite design and introduce the detuning modulated composite segmented (DMCS) scheme in nonlinear optics, which offers a broadband, efficient and robust method for frequency conversion. We also present the constant-length DMCS scheme, which offers multiple efficient and robust wavelength regimes for broadband upconversion. We apply these schemes to a system of quasi-phase-matching crystal for the sum frequency generation process, and demonstrate the high robustness and bandwidth of the composite schemes. We show that these schemes are robust to temperature and crystal length variations and can have a superior conversion bandwidth under length and power constraints compared to other conversion schemes, such as periodically poled and adiabatic chirped crystals. We believe that the new family of DMCS schemes will have many uses in applications of frequency conversion, due to their robustness, low energy demand and compact size.

Broadband yellow-orange light generation based on a step-chirped PPMgLN ridge waveguide.

Yellow-orange lights, valuable in photodynamic therapies, spectroscopy, and optogenetics, are limited by the narrow bandwidth and bulky setup via the conventional Raman or optical parametric oscillation processes. Moreover, flatness in the broad-band spectrum is also important for the aforementioned applications with extended functions. In this paper, by carefully designing grating-periods of a step-chirped PPMgLN ridge waveguide for sum frequency generation (SFG), we report a compact broad-band yellow-orange light with bandwidth of 5.6 nm and an un-reported flatness (<1.5 dB). Correspondingly, the optical conversion efficiency is 232.08%/W, which is the best SFG efficiency for PPMgLN at the yellow-orange region, to the best of our knowledge. The results could also be adopted for other broad-band SFG process toward the vis-infrared region in an integrated structure.

Sum-Frequency Generation in High-Q GaP Metasurfaces Driven by Leaky-Wave Guided Modes.

Resonant metasurfaces provide a unique platform for enhancing multiwave nonlinear interactions. However, the difficulties over mode matching and material transparency place significant challenges in the enhancement of these multiwave processes. Here we demonstrate efficient nonlinear sum-frequency generation (SFG) in multiresonant GaP metasurfaces based on guided-wave bound-state in the continuum resonances. The excitation of the metasurface by two near-infrared input beams generates strong SFG in the visible spectrum with a conversion efficiency of 2.5 × 10-4 W-1, 2 orders of magnitude higher than the one reported in Mie-type resonant metasurfaces. In addition, we demonstrate the nontrivial polarization dependence on the SFG process. In contrast to harmonic generation, the SFG process is enhanced when using nonparallel polarized input-beams. Importantly, by varying the input pump beam polarization it is possible to direct the SFG emission to different diffraction orders, thereby opening up new opportunities for nonlinear light sources and infrared to visible light conversion.

Nonlinear optics in gallium phosphide cavities: simultaneous second and third harmonic generation

We demonstrate the simultaneous generation of second and third harmonic signals from a telecom wavelength pump in a gallium phosphide (GaP) microdisk. Using analysis of the power scaling of both the second and third harmonic outputs and calculations of nonlinear cavity mode coupling factors, we study contributions to the third harmonic signal from direct and cascaded sum frequency generation processes. We find that despite the relatively high material absorption in GaP at the third harmonic wavelength, both of these processes can be significant, with relative magnitudes that depend closely on the detuning between the second harmonic wavelengths of the cavity modes.

Eye-Safe Aerosol and Cloud Lidar Based on Free-Space Intracavity Upconversion Detection

We report an eye-safe aerosol and cloud lidar with an Erbium-doped fiber laser (EDFL) and a free-space intracavity upconversion detector as the transmitter and receiver, respectively. The EDFL was home-made, which could produce linearly-polarized pulses at a repetition rate of 15 kHz with pulse energies of ~70 μJ and pulse durations of ~7 ns centered at 1550 nm. The echo photons were upconverted to ~631 nm via the sum frequency generation process in a bow-tie cavity, where a Nd:YVO4 and a PPLN crystal served as the pump and nonlinear frequency conversion devices, respectively. The upconverted visible photons were recorded by a photomultiplier tube and their timestamps were registered by a customized time-to-digital converter for distance-resolved measurement. Reflected signals peaked at ~6.8 km from a hard target were measured with a distance resolution of 0.6 m for an integral duration of 10 s. Atmospheric backscattered signals, with a range of ~6 km, were also detectable for longer integral durations. The evolution of aerosols and clouds were recorded by this lidar in a preliminary experiment with a continuous measuring time of over 18 h. Clear boundary and fine structures of clouds were identified with a spatial resolution of 9.6 m during the measurement, showing its great potential for practical aerosol and cloud monitoring.

Simultaneous Characterization of Two Ultrashort Optical Pulses at Different Frequencies Using a WS2 Monolayer.

The precise characterization of ultrashort laser pulses has been of interest to the scientific community for many years. Frequency-resolved optical gating (FROG) has been extensively used to retrieve the temporal and spectral field distributions of ultrashort laser pulses. In this work, we exploit the high, broad-band nonlinear optical response of a WS2 monolayer to simultaneously characterize two ultrashort laser pulses with different frequencies. The relaxed phase-matching conditions in a WS2 monolayer enable the simultaneous acquisition of the spectra resulting from both four-wave mixing (FWM) and sum-frequency generation (SFG) nonlinear processes while varying the time delay between the two ultrashort pulses. Next, we introduce an adjusted double-blind FROG algorithm, based on iterative fast Fourier transforms between two FROG traces, to extract the intensity distribution and phase of two ultrashort pulses from the combination of their FWM and SFG FROG traces. Using this algorithm, we find an agreement between the computed and observed FROG traces for both the FWM and SFG processes. Exploiting the broad-band nonlinear response of a WS2 monolayer, we additionally characterize one of the pulses using a second-harmonic generation (SHG) FROG trace to validate the pulse shapes extracted from the combination of the FWM and SFG FROG traces. The retrieved pulse shape from the SHG FROG agrees well with the pulse shape retrieved from our nondegenerate cross-correlation FROG measurement. In addition to the nonlinear parametric processes, we also observe a nonlinearly generated photoluminescence (PL) signal emitted from the WS2 monolayer. Because of its nonlinear origin, the PL signal can also be used to obtain complementary autocorrelation and cross-correlation traces.

Development and Demonstration of Australian First Working Sodium Guide Star Laser

The Australian first working sodium guide star laser system has been designed and developed for various astronomical and space-related applications. A completely diode-pumped pulsed system was developed initially followed by a largely fiber-based continuous wave (CW) system operating at 589 nm achieved through a unique wavelength conversion scheme by combining 1342 and 1050 nm through a sum frequency generation process. For the CW system, single-mode laser beams at both 1342 and 1050 nm are achieved from fiber-based seed oscillators and fiber amplifiers. The output power of ~25 W at 1342 nm is achieved from a single frequency fiber Raman amplifier. Output power up to 70 W at 1050 nm is achieved from a Yb-doped fiber pre-amplifier followed by a Yb-doped fiber power amplifier. For the sum frequency generation process, optimum focusing parameters are evaluated and determined. The CW system has generated more than 20 W output power at 589 nm, a circularly polarised beam with a good beam quality, spectral linewidth ≤ 2 MHz, and the laser output locked on the sodium D2 line at 589.159 nm. The system has been successfully demonstrated at EOS Space Research Centre, Mt Stromlo, Canberra, and become the Australian first working sodium guide star laser system.

Second-harmonic and sum-frequency generation based on birefringence phase matching of BaMgF4 crystal.

BaMgF4 is a ferroelectric nonlinear crystal with a very wide transparency window ranging from 125 nm to 13µm of the wavelength. Therefore, it is a candidate material to generate ultraviolet or deep ultraviolet laser, which is very important in lithography, semiconductor manufacturing, and advanced instrument development. Here, the second-order birefringence phase-matching processes of the BaMgF4 crystal were studied, including second-harmonic generation (SHG) and sum-frequency generation (SFG). In the experiments, we measured the phase-matching angle, nonlinear frequency conversion efficiency, and angle bandwidth of SHG and SFG processes of BaMgF4 crystal, which are in well agreement with the theoretical calculations. This study may promote the research of nonlinear optical process of BaMgF4 crystal and also the further development of all-solid-state vacuum ultraviolet lasers.