Measurements of photon correlations of second harmonic generated light
CW second harmonic He-Ne laser light second order intensity correlation function measurements
Davidson, F.↗
SEARCH · Engineering Papers
Results for “Harmonic generation”
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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↗
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↗
Tunable Second Harmonic Generation in Twisted Bilayer Graphene
Twisted stacking of van der Waals (vdW) materials introduces a new way in bandstructure engineering and has given rise to numerous extraordinary physical phenomena. Despite the absence of second harmonic generation (SHG) in non-gated monolayer graphene, artificially twisted bilayer graphene (tBLG) possesses more possible point-group symmetries including those with broken inversion-symmetry. Here, we report twist-angle-dependent SHG from tBLG, which is the first demonstration of an elemental material with intrinsically tunable nonlinearity. We show that depending on the twist angle, the susceptibility of the dominant chiral tensor component of tBLGs can vary from 0 to 28×10 4 pm 2 /V, which is at the same order of magnitude as on-resonance susceptibility of monolayer MoS 2 . These results shed light on the underlying symmetry of tBLG systems and electronic band-structure near van Hove singularities (vHs). More importantly, they introduce a new degree of freedom, the twisting, in creating efficient second-order nonlinear material form centrosymmetric constituents
36 MATERIALS SCIENCE↗
High harmonic generation in graphene quantum dots
Abstract We study theoretically the generation of high harmonics in disk graphene quantum dots placed in linearly polarized short pulse. The quantum dots (QD) are described within an effective model of the Dirac type and the length gauge was used to describe the interaction of quantum dots with an optical pulse. The generated radiation spectra of graphene quantum dots can be controlled by varying the quantum dot size, i.e. its radius. With increasing the quantum dot radius, the intensities of low harmonics mainly decrease, while the cutoff frequency increases. The sensitivity of the cutoff frequency to the QD size increases with the intensity of the pulse.
Physics↗
Terahertz Second-Harmonic Generation from Lightwave Acceleration of Symmetry-Breaking Nonlinear Supercurrents
We report terahertz (THz) light-induced second harmonic generation, in superconductors with inversion symmetry that forbid even-order nonlinearities. The THz second harmonic emission vanishes above the superconductor critical temperature and arises from precession of twisted Anderson pseudospins at a multicycle, THz driving frequency that is not allowed by equilibrium symmetry. We explain the microscopic physics by a dynamical symmetry breaking principle at sub-THz-cycle by using quantum kinetic modeling of the interplay between strong THz-lightwave nonlinearity and pulse propagation. In this work, the resulting nonzero integrated pulse area inside the superconductor leads to light-induced nonlinear supercurrents due to subcycle Cooper pair acceleration, in contrast to dc-biased superconductors, which can be controlled by the band structure and THz driving field below the superconducting gap.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
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.↗
Heteroanionic Control of Exemplary Second-Harmonic Generation and Phase Matchability in 1D LiAsS 2– x Se x
The isostructural heteroanionic compounds β-LiAsS 2–x Se x (x = 0, 0.25, 1, 1.75, 2) show a positive correlation between selenium content and second-harmonic response and greatly outperform the industry standard AgGaSe 2 . These materials crystallize in the noncentrosymmetric space group Cc as one-dimensional $\frac{1}{∞}$ [AsQ 2 ] - (Q = S, Se, S/Se) chains consisting of corner-sharing AsQ3 trigonal pyramids with charge-balancing Li + atoms interspersed between the chains. LiAsS 2–x Se x melts congruently for 0 ≤ x ≤ 1.75, but when the Se content exceeds x = 1.75, crystallization is complicated by a phase transition. This behavior is attributed to the β- to α-phase transition present in LiAsSe 2 , which is observed in the Se-rich compositions. The band gap decreases with increasing Se content, starting at 1.63 eV (LiAsS 2 ) and reaching 1.06 eV (β-LiAsSe 2 ). Second-harmonic generation measurements as a function of wavelength on powder samples of β-LiAsS 2–x Se x show that these materials exhibit significantly higher nonlinearity than AgGaSe 2 (d 36 = 33 pm/V), reaching a maximum of 61.2 pm/V for LiAsS 2 . In comparison, single-crystal measurements for LiAsSSe yielded a d eff = 410 pm/V. LiAsSSe, LiAsS 0.25 Se 1.75 , and β-LiAsSe 2 show phase-matching behavior for incident wavelengths exceeding 3 μm. The laser-induced damage thresholds from two-photon absorption processes are on the same order of magnitude as AgGaSe 2 , with S-rich materials slightly outperforming AgGaSe 2 and Se-rich materials slightly underperforming AgGaSe 2 .
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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↗
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.↗
Third harmonic generation in phase-matched alkali metal vapors
We report improvements in conversion efficiency for third harmonic generation in sodium and rubidium vapor. 30-psec pulses of radiation at 1.064 micron have been converted to 0.3547 micron with an energy conversion efficiency of 10%. Factors limiting conversion efficiency are discussed.
Bloom, D. M.↗
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.↗
Direct reconstruction of isolated XUV or soft x-ray attosecond pulses from high-harmonic generation streaking spectra
Characterization of an isolated attosecond pulse (IAP) in the extreme ultraviolet (XUV) or soft x-ray (SXR) region is essential for its applications. Here we propose to retrieve an IAP in the time domain directly through the modulation of high-harmonic generation (HHG) spectra in the presence of a time-delayed intense few-cycle infrared or mid-infrared laser. The retrieval algorithm is derived based on the strong-field approximation and an extended quantitative rescattering model. We show that both isolated XUV pulses with a narrow spectral bandwidth and isolated SXR pulses with a broad bandwidth can be well characterized through the HHG streaking spectra. Such an all-optical method for characterizing the IAP differs from the commonly used approach based on the streaked photoelectron spectra that would require electron spectrometers. We check the robustness of the retrieval method by changing the dressing laser or by adjusting the steps of time delay. We also show that the XUV pulse can be accurately retrieved by treating the HHG streaking spectra calculated from solving the time-dependent Schrödinger equation for single atoms as the ‘experimental’ data.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Probing topological phase transitions using high-harmonic generation
We report the prediction and realization of topological insulators have sparked great interest in experimental approaches to the classification of materials. The phase transition between non-trivial and trivial topological states is important, not only for basic materials science but also for next-generation technology, such as dissipation-free electronics. It is therefore crucial to develop advanced probes that are suitable for a wide range of samples and environments. Here we demonstrate that circularly polarized laser-field-driven high-harmonic generation is distinctly sensitive to the non-trivial and trivial topological phases in the prototypical three-dimensional topological insulator bismuth selenide. The phase transition is chemically initiated by reducing the spin–orbit interaction strength through the substitution of bismuth with indium atoms. We find strikingly different high-harmonic responses of trivial and non-trivial topological surface states that manifest themselves as a conversion efficiency and elliptical dichroism that depend both on the driving laser ellipticity and the crystal orientation. The origins of the anomalous high-harmonic response are corroborated by calculations using the semiconductor optical Bloch equations with pairs of surface and bulk bands. As a purely optical approach, this method offers sensitivity to the electronic structure of the material, including its nonlinear response, and is compatible with a wide range of samples and sample environments.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
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↗
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↗
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↗