Development of an optimized second harmonic generator cell Final scientific report, 12 Jun. 1969 - 12 Mar. 1970
Optimized second harmonic generator cell
Bass, M.↗
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Phonon second harmonic generation in NaBr studied by inelastic neutron scattering and computer simulation
The phenomenon of second harmonic generation (SHG) was found for phonons in anharmonic NaBr by inelastic neutron scattering. The temperature dependence of this phonon SHG was measured from 300 K to 650 K. At 300 K the second harmonic (SH) is seen as a high-energy branch around 33 meV, nearly independent of $\overrightarrow{Q}$. The temperature effective potential (TDEP) method and classical molecular dynamics (MD) simulation with machine learning interatomic potential were able to reproduce the SH, and showed that SHG occurs with the flat transverse optical (TO) phonon branch. A classical model of a nonlinear medium explains the intensity and lifetime of the SH, compared to those of the TO modes. Also successful was a quantum model based on the Heisenberg-Langevin equation for interacting phonons coupled to a thermal bath, which also predicts a spectral distribution of the SH. In conclusion, the measured temperature dependence of the intensity of the second harmonic showed that it follows the Planck distribution of a one-phonon quasiparticle, and not two TO phonons.
36 MATERIALS SCIENCE↗
Limitations on squeezing and formation of the superposition of two macroscopically distinguishable states at fundamental frequency in the process of second harmonic generation
The results of numerical simulations of quantum state evolution in the process of second harmonic generation (SHG) are discussed. It is shown that at a particular moment of time in the fundamental mode initially coherent state turns into a superposition of two macroscopically distinguished states. The question of whether this superposition exhibits quantum interference is analyzed.
Nikitin, S. P.↗
Observation of seeded second harmonic generation in bulk germanosilicate fiber preforms
Simultaneous irradiation of a bulk fiber preform with molar concentrations of 3 pct Ge and 0.5 pct P doped silica core region resulted in self-organized second harmonic generation with an effective chi(2) of about 1.2 x 10 to the -16th m/V. The experiments revealed that the bulk preform requires the same critical IR intensity (10 GW/sq cm) as the drawn fibers to prepare. Attempts to self-prepare the preform field, indicating that self-preparation in fibers is most likely initiated by second harmonic generation associated with the core-cladding interface.
Lawandy, N. M.↗
Simultaneous mode-locking and second-harmonic generation by the same nonlinear crystal.
Simultaneous mode locking of Nd YAG laser and intracavity second harmonic generation in high temperature Li niobate or BaNa niobate
Gurski, T. R.↗
Two-pass-internal second-harmonic generation using a prism coupler.
A dispersive quartz prism is used to couple the total second harmonic generated in both directions by an internal cavity frequency doubler. The study shows that the dispersion of air and mirror reflection phase shifts can be compensated for by a slight nonphase match condition in the doubler.
Gonzalez, D. G.↗
Absolute and relative nonlinear optical coefficients of KDP, KD(asterisk)P, BaB2O4, LiIO3, MgO:LiNbO3, and KTP measured by phase-matched second-harmonic generation
Both absolute and relative nonlinear optical coefficients of six nonlinear materials measured by second-harmonic generation are discussed. A single-mode, injection-seeded, Q-switched Nd:YAG laser with spatially filtered output was used to generate the 1.064-micron fundamental radiation. The following results were obtained: d36(KDP) = 0.38 pm/V, d36(KD/asterisk/P) = 0.37 pm/V, (parallel)d22(BaB2O4)(parallel) = 2.2 pm/V, d31(LiIO3) = -4.1 pm/V, d31(5 percentMgO:MgO LiNbO3) = -4.7 pm/V, and d(eff)(KTP) = 3.2 pm/V. The accuracy of these measurements is estimated to be better than 10 percent.
Eckardt, Robert C.↗
Phase matching in second-harmonic generation using artificial periodic structures.
The use of artificial periodic structures, consisting of spatial modulations of the linear and nonlinear susceptibilities of a nonlinear optical medium, to achieve phase matching in second-harmonic generation is analyzed. Dispersion relations and approximate formulas for the second-harmonic fields generated under various conditions are obtained and used to evaluate the experimental situation.
Tang, C. L.↗
Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package
Abstract Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a priori. A recent open-source code, ♯SHAARP. si , can provide such closed form solutions for crystals with arbitrary symmetries, orientations, and anisotropic properties at a single interface. However, optical components are often in the form of slabs, thin films on substrates, and multilayer heterostructures with multiple reflections of both the fundamental and up to ten different SHG waves at each interface, adding significant complexity. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry in Multilayers (♯SHAARP. ml ). The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes using standard and commonly used nonlinear optical materials as well as twisted 2-dimensional heterostructures.
36 MATERIALS SCIENCE↗
Insulating moiré homobilayers lack a threefold symmetric second-harmonic generation
Atoms within moiré bilayers relax in plane to minimize elastic energy; such relaxation brings their space group symmetries down to P1. Here, the ab initio second harmonic generation (SHG) of twisted and atomistically optimized hBN bilayers was determined at four twist angles (θ = 38.21°, 60.00°, 73.17°, and 98.21°) and for three displacements τ measured away from the ground state AA' configuration. All moiré bilayers have a P1 space symmetry after structural optimization. This situation is quite different to monolayers with hexagonal lattices, which retain a threefold symmetry. We point out that the actual symmetries of the SHG reported for hBN bilayers on two experimental works do not coincide with the sixfold symmetric theoretical profiles they provide [either sin 2 (3Φ) or cos 2 (3Φ)], and show that the intrinsic low structural symmetry of (atomically optimized) hBN bilayer moirés can in fact be read out from experimental SHG intensity profiles—which are tunable by θ and by the frequency of light ω: The SHG is most definitely not sixfold symmetric because moirés do not retain a threefold symmetry. Furthermore, an extrinsic twofold symmetry of the SHG emission is realized by tilting the pump by an angle α away from the 2D material's normal, regardless of θ and ω. Furthermore, the design of in-plane and ultrathin sources of SHG with low symmetry could be useful for the eventual creation of entanglement sources from 2D materials.
2-dimensional systems↗
Diacetylene and Polydiacetylene Derivatives of 2-Methyl-4-Nitroaniline for Second-Harmonic Generation
A novel diacetylene derivative of 2-Methyl-4-NitroAniline (MNA), a well-known material for Second-Harmonic Generation (SHG), is synthesized. This monomer DiAcetylene MethylNitroAniline, (DAMNA) is characterized by means of the Kurtz technique at 1064 nm and is found to have an SHG powder efficiency 62.5 % that of MNA itself. Thin crystalline films of DAMNA are grown onto quartz, Teflon, and Kapton substrates by means of vapor deposition in vacuum. These films are then polymerized in the solid state by exposure to long-wavelength UV radiation to give crystalline polydiacetylene thin films (PDAMNA). The films are next characterized for SHG, using an unpolymerized DAMNA film as a reference. Interestingly, films grown onto Teflon exhibit greater orientation and significantly greater SHG than those grown onto quartz and Kapton. This result is promising in that it demonstrates the potential of PDAMNA as both a crystalline and polymeric material for SHG applications, in which highly oriented thin films are desired. Computational modeling (usingAM1) is also carried out on DAMNA and is compared to the experimental results.
Paley, M. S.↗
Hidden anomalies in topological t – PtBi 2 – x probed by second harmonic generation
The noncentrosymmetric Weyl semimetal PtBi 2–x (t-PtBi 2–x ) exhibits various interesting technologically important physical properties. We report the experimental investigation of PtBi 1.6 via second harmonic generation (SHG), single-crystal x-ray diffraction, magnetic susceptibility, and electrical resistivity measurements. While bulk structural, magnetic, and electrical properties show no phase transitions below room temperature, the temperature dependence of the SHG intensity reveals two anomalies: one at T* ~ 60 K and another at T x ~ 200 K. Quantitative analysis indicates that the SHG signal results from both the buckled Bi1 surface termination with the 3m symmetry and flat Bi2 surface termination with the m symmetry. However, the anomalies are mainly driven by Bi1 on the surface: (1) T* marks the onset of surface states which is also manifested in the c-axis resistivity drop and (2) T x corresponds to the lowest thermal contraction of the structure and enhanced magnetic susceptibility. Furthermore, this study demonstrates that SHG is a powerful technique for probing surface properties even for noncentrosymmetric materials.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Large Non‐Resonant Infrared Optical Second Harmonic Generation in Bulk Crystals of Van der Waals Semiconductor, SnP 2 Se 6
2D van der Waals (vdW) materials have emerged as a highly promising candidates for nonlinear optical (NLO) applications. This study presents the synthesis, comprehensive linear optical, and optical second harmonic generation (SHG) characterization of a novel 2D vdW semiconductor SnP2Se6 in its bulk single crystal form. It exhibits an indirect bandgap of ≈1.47 eV and an exceptional non-resonant SHG coefficient of d 33 ∼ −222 ± 30 pm V −1 at a fundamental wavelength of 2 µm, which is ≈7 times larger than that of the commercial AgGaSe 2 with a comparable bandgap. Density functional theory (DFT) calculations of the linear and nonlinear optical properties exhibit reasonable agreement with the experimental measurements, revealing the chemical origin of the enhanced properties. Moreover, SnP 2 Se 6 can exhibit both type-I and type-II phase matching over a wide spectral range, fulfilling one of the key criteria for an ideal NLO crystal. These exceptional properties position SnP 2 Se 6 as a highly promising candidate for NLO applications.
36 MATERIALS SCIENCE↗
Optomechanical Tuning of Second Harmonic Generation Anisotropy in Janus MoSSe/MoS 2 Heterostructures
Symmetry breaking in van der Waals materials enables the realization of quantum states and advanced device functionalities. Janus transition-metal dichalcogenides (TMDs) exhibit distinctive nonlinear optical properties due to their broken out-of-plane mirror symmetry. However, the dynamic control of second harmonic generation (SHG) anisotropy and resonance behavior via optical excitation remains elusive. Here, in this work, we investigate the SHG response of Janus MoSSe/MoS 2 heterostructures with 2H and 3R stackings. We can tune the SHG response by varying the incident photon wavelength from 800 to 1000 nm, which shows a resonance-dependent enhancement in intensity and a deviation from 6-fold symmetry, indicating wavelength-dependent anisotropy. The ratio between maximum and minimum intensity in the armchair directions, associated with the SHG anisotropy, reaches a value of 1.73 at the excitation wavelength of 1000 nm. Group theory analysis and first-principles calculations reveal that the observed anisotropy arises from optically induced strain. Our findings highlight the role of symmetry breaking and optical resonance contributing to the optomechanical tuning of SHG anisotropy, offering opportunities for developing Janus TMD-based photonic devices for frequency conversion, light generation, and optical switching.
Janus transition metal dichalcogenides↗
Efficient second harmonic generation of a diode-laser-pumped CW Nd:YAG laser using monolithic MgO:LiNbO3 external resonant cavities
56-percent efficient external-cavity-resonant second-harmonic generation of a diode-laser pumped, CW single-axial-mode Nd:YAG laser is reported. A theory of external doubling with a resonant fundamental is presented and compared to experimental results for three monolithic cavities of nonlinear MgO:LiNbO3. The best conversion efficiency was obtained with a 12.5-mm-long monolithic ring cavity doubler, which produced 29.7 mW of CW, single-axial model 532-nm radiation from an input of 52.5 mW.
Kozlovsky, William J.↗
Anomalous Second Harmonic Generation from Atomically Thin MnBi 2 Te 4
MnBi 2 Te 4 is a van der Waals topological insulator with intrinsic intralayer ferromagnetic exchange and A-type antiferromagnetic (AFM) interlayer coupling. Theoretically, it belongs to a class of structurally centrosymmetric crystals whose layered antiferromagnetic order breaks inversion symmetry for even layer numbers, making optical second harmonic generation (SHG) an ideal probe of the coupling between the crystal and magnetic structures. Here, we perform magnetic field and temperature dependent SHG measurements on MnBi 2 Te 4 flakes ranging from bulk to monolayer thickness. We find that the dominant SHG signal from MnBi 2 Te 4 is unexpectedly unrelated to both magnetic state and layer number. As a result, we suggest that surface SHG is the likely source of the observed strong SHG, whose symmetry matches that of the MnBi 2 Te 4 -vacuum interface. Our results highlight the importance of considering the surface contribution to inversion symmetry breaking in van der Waals centrosymmetric magnets.
2D magnets↗
Plasmonic Nonlinear Energy Transfer Enhanced Second Harmonic Generation Nanoscopy
Nonlinear optical response is a fingerprint of various physicochemical properties of materials related to symmetry, including crystallography, interfacial configuration, and carrier dynamics. However, the intrinsically weak nonlinear optical susceptibility and the diffraction limit of far-field optics restrict probing deep-subwavelength-scale nonlinear optics with measurable signal-to-noise ratio. Here, we propose an alternative approach toward efficient second harmonic generation (SHG) nanoscopy for SHG-active sample (zinc oxide nanowire; ZnO NW) using an SHG-active plasmonic nanotip. Our full-wave simulation suggests that the experimentally observed high near-field SHG contrast is possible when the nonlinear response of ZnO NW is enhanced and/or that of the tip is suppressed. Here, this result suggests possible evidence of quantum mechanical nonlinear energy transfer between the tip and the sample, modifying the nonlinear optical susceptibility. Further, this process probes the nanoscale corrosion of ZnO NW, demonstrating potential use in studying various physicochemical phenomena in nanoscale resolution.
36 MATERIALS SCIENCE↗
Magnetic Properties and Large Second-Harmonic Generation Response of a Chiral Ternary Chalcogenide: Eu 2 SiSe 4
Eu(II)-containing chalcogenides are an emerging class of materials that are of great interest due to their high optical activity and intriguing magnetism. Here, we synthesized Eu 2 SiSe 4 as red-colored single crystals and characterized its structure with single-crystal X-ray diffraction, confirming the reported chiral monoclinic P2 1 symmetry at room temperature. The crystal structure of Eu 2 SiSe 4 comprises distorted SiSe 4 tetrahedral units and charge-balancing Eu(II) cations. Here, we develop a two-step solid-state synthesis method for Eu 2 SiSe 4 and compare it to the known boron chalcogenide method. We find the second-harmonic generation (SHG) activity of polycrystalline Eu 2 SiSe 4 to be ∼7 × AgGaS 2 , placing it among the highest-known SHG-active chalcogenides. No symmetry lowering is observed down to 100 K in single-crystal X-ray diffraction, although an anomalous expansion in the b-axis lattice parameter occurs and may be correlated to lattice modes of the SiSe 4 tetrahedra. We investigate the physical properties of Eu 2 SiSe 4 using magnetometry and heat capacity measurements and find a transition to an antiferromagnetic ground state at T N ≈ 5.5 K. The low-temperature transition releases less entropy than expected, which may be due to the complex crystal electric field effects of Eu(II).
36 MATERIALS SCIENCE↗