Second-harmonic Signal Research Articles

Mechanism of Enhanced Optical Second-Harmonic Generation in the Conducting Pyrochlore-TypePb2Ir2O7−xOxide Compound

The structural, electronic, and optical properties of pyrochlore-type Pb(2)Ir(2)O(6)O(0.55)('), which is a metal without spatial inversion symmetry at room temperature, were investigated. Structural analysis revealed that the structural distortion relevant to the breakdown of the inversion symmetry is dominated by the Pb-O' network but is very small in the Ir-O network. At the same time, gigantic second-harmonic generation signals were observed, which can only occur if the local environment of the Ir 5d electrons features broken inversion symmetry. First-principles electronic structure calculations reveal that the underlying mechanism for this phenomenon is the induction of the noncentrosymmetricity in the Ir 5d bands by the strong hybridization with O' 2p orbitals. Our results stimulate theoretical study of inversion-broken iridates, where exotic quantum states such as a topological insulator and Dirac semimetal are anticipated.

Nonlinear photonic crystal: effects of negative refractive indices and dispersion in the resonant region

We investigate second-harmonic generation of photons in nonlinear photonic crystal composed of N periods of bilayers with dispersive complex magnetic permeability and dielectric permittivity. Analytical expressions for the reflected and transmitted fundamental fields (FFs) and the second-harmonic (SH) fields are obtained. We find interesting features in the SH fields versus pump frequency and relative thickness of the bilayers for the same real values of permittivity and permeability but with different signs. Negative permeability is a substitute for periodical poling. A stronger SH signal is found when one of the layers has negative refractive index. For certain parameters, the backward and forward SH signals can be generated over a broad frequency range. Around the resonant region with strong dispersions, the reflected and transmitted signals depend on the magnetic and dielectric resonances of each layer. The transmitted FF field shows a narrow transparency window that can be controlled by the thickness of the layers. Also, a negative index around the resonant region reduces the SH peak. These results provide insights for designing efficient nonlinear photonics devices with dielectric–magnetic materials.

Simulation and analysis of second-harmonic signal based on tunable diode laser absorption spectroscopy

Tunable diode laser absorption spectroscopy (TDLAS) is a new gas detection technique developed recently with high spectral resolution, high sensitivity and fast time response. The second-harmonic signal of wavelength modulation spectroscopy (WMS) is often used as the detection signal for gas concentration inversion. Using Simulink, a visual modeling and simulation platform, the authors simulated the WMS signal based on TDLAS, and got the second-harmonic signal by using lock-in amplifier algorithm. Digital orthogonal algorithm was studied in this paper. The relationship between second-harmonic signals and the modulation indexes was analyzed by comparing changes of second-harmonic under different modulation indexes, in order to find out the optimized parameters for second-harmonic detection.

Čerenkov-type second-harmonic spectroscopy in random nonlinear photonic structures

We report on experimental and theoretical studies of Čerenkov-type second-harmonic generation in random nonlinear photonic structures with different two-dimensional distributions of the ferroelectric domains. We utilize Čerenkov-type second-harmonic generation spectroscopy to estimate the average ferroelectric domain size by analyzing the spatial Fourier spectrum of the domain patterns. This is measured by scanning the Čerenkov second-harmonic signal for different angles of incidence and light polarizations of the fundamental wave. By comparing the experimental results with numerically simulated Fourier spectra, the corresponding domain patterns are retrieved, which are in a good correspondence with images obtained by Čerenkov-type second-harmonic generation microscopy.

Chirp-encoded excitation for dual-frequency ultrasound tissue harmonic imaging

Dual-frequency (DF) transmit waveforms comprise signals at two different frequencies. With a DF transmit waveform operating at both fundamental frequency (f(0)) and second-harmonic frequency (2f(0)), tissue harmonic imaging can be simultaneously performed using not only the conventional 2f(0) second-harmonic signal but also using the f(0 )frequency-difference harmonic signal. Nonetheless, when chirp excitation is incorporated into the DF transmit waveform for harmonic SNR improvement, a particular waveform design is required to maintain the bandwidth of the f(0) harmonic signal. In this study, two different DF chirp waveforms are proposed to produce equal harmonic bandwidth at both the f(0) and 2f(0) frequencies to achieve speckle reduction by harmonic spectral compounding and to increase harmonic SNR for enhanced penetration and sensitivity. The UU13 waveform comprises an up-sweeping f(0) chirp and an up-sweeping 2f(0) chirp with triple bandwidth, whereas the UD11 waveform includes an up-sweeping f(0) chirp and a down-sweeping 2f(0) chirp with equal bandwidth. Experimental results indicate that the UU13 tends to suffer from a high range side lobe level resulting from 3f(0) interference. Consequently, the 2f(0) harmonic envelopes of the UD11 and the UU13 waveforms have compression qualities of 87% and 77%, respectively, when the signal bandwidth is 30%. When the bandwidth increases to 50%, the compression quality of the 2f(0) harmonic envelope degrades to 78% and 54%, respectively, for the UD11 and the UU13 waveforms. The compression quality value of the f0 harmonic envelope remains similar between the two DF transmit waveforms for all signal bandwidths. B-mode harmonic images also show that the UD11 is less contaminated by range side lobe artifacts than is the UU13. Compared with a short pulse with equal bandwidth, the UD11 waveform not only preserves the same spatial resolution after compression but also improves the image SNR by about 10 dB. Moreover, the image contrast-to-noise ratio (CNR), defined as the ratio of the mean to the standard deviation of image intensity in the speckle region, can be increased from 1.0 to about 1.2 when DF spectral compounding is performed. Therefore, it is concluded that the UD11 waveform is a potential solution for chirp-encoded DF harmonic imaging.

Femtosecond-Pulsed Plasmonic Nanotweezers

We demonstrate for the first time plasmonic nanotweezers based on Au bowtie nanoantenna arrays (BNAs) that utilize a femtosecond-pulsed input source to enhance trapping of both Rayleigh and Mie particles. Using ultra-low input power densities, we demonstrate that the high-peak powers associated with a femtosecond source augment the trap stiffness to 2x that of nanotweezers employing a continuous-wave source, and 5x that of conventional tweezers using a femtosecond source. We show that for trapped fluorescent microparticles the two-photon response is enhanced by 2x in comparison to the response without nanoantennas. We also demonstrate tweezing of 80-nm diameter Ag nanoparticles, and observe an enhancement of the second-harmonic signal of ~3.5x for the combined nanoparticle-BNA system compared to the bare BNAs. Finally, under select illumination conditions, fusing of Ag nanoparticles to the BNAs is observed which holds potential for in situ fabrication of three-dimensional, bimetallic nanoantennas.

Development of a high spectral resolution lidar based on confocal Fabry–Perot spectral filters

The high spectral resolution lidar (HSRL) instrument described in this paper utilizes the fundamental and second-harmonic output from an injection seeded Nd:YAG laser as the laser transmitter. The light scattered in the atmosphere is collected using a commercial Schmidt-Cassegrain telescope with the optical receiver train first splitting the fundamental and second-harmonic return signal with the fundament light monitored using an avalanche photodiode. The second-harmonic return signal is mode matched into a tunable confocal Fabry-Perot (CFP) interferometer with a free spectral range of 7.5 GHz and a finesse of 50.7 (312) at 532 nm (1064 nm) placed in the optical receiver for spectrally filtering the molecular and aerosol return signals. The light transmitted through the CFP is used to monitor the aerosol return signal while the light reflected from the CFP is used to monitor the molecular return signal. Data collected with the HSRL are presented and inversion results are compared to a co-located solar radiometer, demonstrating the successful operation of the instrument. The CFP-based filtering technique successfully employed by this HSRL instrument is easily portable to other arbitrary wavelengths, thus allowing for the future development of multiwavelength HSRL instruments.

Temperature oscillating optical second-harmonic generation in TlGaSe2 and TlInS2 single crystals

Second-harmonic (SH) generation effects have been investigated in TlGaSe2 and TlInS2 layered crystals. Pronounced periodical changes of the SH signal with temperature are discovered. The observed effect is explained within the phase synchronism condition, which changes with temperature in the course of thermal expansion. A major role of the high value of dispersion for the refractive indexes of the investigated crystals in the observed phenomenon is proposed.

Computer Simulation of the Nonlinear Optical Properties of Langmuir–Blodgett Films of a Squaraine Derivative

The linear and nonlinear optical properties (L&NLO) of a monolayer of (4-(N-methyl-N-(carboxypropyl)amino)-phenyl-4′-(N,N-dibutylamino)phenylsquaraine (SBA) were computed by a combination of molecular dynamics simulations, molecular quantum-mechanical, and discrete local-field model calculations to compute the macroscopic optical susceptibilities. Langmuir films on water and graphite were simulated and several structural properties investigated. In addition, SBA in water and dimethylsulfoxide (DMSO) solutions were simulated, and the aggregation behavior of SBA in these solvents was analyzed. The molecular (hyper)polarizabilities of SBA were calculated with density functional theory and validated with MP2 correlated ab initio calculations. An unusual large component perpendicular to the molecular dipole moment is obtained for the molecular first hyperpolarizability, which is a main contributor to the large in-plane anisotropy of the computed macroscopic second-harmonic generation signal of the Langmuir–Blo...

Mapping of gold nanostructure-enhanced near fields via laser scanning second-harmonic generation and ablation

The optical near-field of metal films can be modified in a straightforward manner by incorporating nanostructures on the surface. The corresponding field enhancement, which may be due to the lightning rod effect as well as the excitation of plasmon modes, results in a local change of the optical surface response. A transparent thin film on top of the nanostructures can be partially ablated via illumination with near-infrared light. Local variations of the ablation rate due to field enhancement are readily mapped with subdiffractional resolution, as confirmed by a direct comparison to theoretical calculations. Variation of the thickness of the transparent film enables discrimination between localized enhancements at the sharp corners of the structures and collective enhancements at locations between the structures due to surface plasmon polariton modes. In addition, applying the same method to study the effect of nanostructure morphology on localized second-harmonic generation using arrays of rectangular as well as triangular structures, we observed a second-harmonic (SH) signal from both centrosymmetric and noncentrosymmetric nanostructure arrays, indicating that the SH excitation is not due to a collective phenomenon but originates locally from the individual structures.

Second-harmonic generation from electron beam deposited SiO films

It is demonstrated that as-grown e-beam deposited SiOx thin films on fused silica substrates show a second-order nonlinear response that is dependent on film thickness. Using a Maker fringes method the effective nonlinear coefficient for a SiO thin film is estimated to be comparable to that of crystalline quartz. Variation of process parameters has been used to investigate the origin of the nonlinear response. The second-harmonic signal is very sensitive to annealing of the film and can be totally removed by annealing at a few hundred degrees. It is also demonstrated that a retarding grid that traps charged particles between the crucible and the sample reduces the nonlinear signal from a SiO thin film significantly. It is suggested that oriented dipoles arise during deposition due to a negatively charged film from oxygen ions, thus, resulting in a non-centrosymmetric film. Finally, using e-beam lithography, well-defined nonlinear 2D structures can be synthesized, thus opening the door to a new and practical way to create nonlinear structures for planar waveguide technology.

Multiphoton microscopy imaging of developing tooth germs

Traditionally, tooth germ is observed by histological investigation with hematoxylin and eosin stain and information may loss during the process. The purpose of this study is to use multiphoton laser fluorescence microscopy to observe the developing tooth germs of mice for building up the database of the images of tooth germs and compare with those from conventional histological analysis. Tooth germs were isolated from embryonic and newborn mice with age of Embryonic Day 14.5 and Postnatal Days 1, 3, 5, and 7. Comparison of the images of tooth germ sections in multiphoton microscopy with the images of histology was performed for investigating the molar tooth germs. It was found that various signals arose from different structures of tooth germs. Pre-dentin and dentin have strong second-harmonic generation signals, while ameloblasts and enamel tissues were shown with strong autofluorescence signals. In this study, a novel multiphoton microscopy database of images from developing tooth germs in mice was set up. We confirmed that multiphoton laser microscopy is a powerful tool for investigating the development of tooth germ and is worthy for further application in the study of tooth regeneration.

Silencing and enhancement of second-harmonic generation in optical gap antennas

Amplifying local electromagnetic fields by engineering optical interactions between individual constituents of an optical antenna is considered fundamental for efficient nonlinear wavelength conversion in nanometer-scale devices. In contrast to this general statement we show that high field enhancement does not necessarily lead to an optimized nonlinear activity. In particular, we demonstrate that second-harmonic responses generated at strongly interacting optical gap antennas can be significantly suppressed. Numerical simulations are confirming silencing of second-harmonic in these coupled systems despite the existence of local field amplification. We then propose a simple approach to restore and amplify the second-harmonic signal by changing the manner in which electrically-connected optical antennas are interacting in the charge-transfer plasmon regime. Our observations provide critical design rules for realizing optimal structures that are essential for a broad variety of nonlinear surface-enhanced characterizations and for realizing the next generation of electrically-driven optical antennas.

In vivo imaging of unstained tissues using a compact and flexible multiphoton microendoscope

We use a compact and flexible multiphoton microendoscope (MPME) to acquire in vivo images of unstained liver, kidney, and colon from an anesthetized rat. The device delivers femtosecond pulsed 800 nm light from the core of a raster-scanned dual-clad fiber (DCF), which is focused by a miniaturized gradient-index lens assembly into tissue. Intrinsic fluorescence and second-harmonic generation signal from the tissue is epi-collected through the core and inner clad of the same DCF. The MPME has a rigid distal tip of 3 mm in outer diameter and 4 cm in length. The image field-of-view measures 115 μm by 115 μm and was acquired at 4.1 frames/s with 75 mW illumination power at the sample. Organs were imaged after anesthetizing Sprague-Dawley rats with isofluorane gas, accessing tissues via a ventral-midline abdominal incision, and isolating the organs with tongue depressors. In vivo multiphoton images acquired from liver, kidney, and colon using this device show features similar to that of conventional histology slides, without motion artifact, in ~75% of imaged frames. To the best of our knowledge, this is the first demonstration of multiphoton imaging of unstained tissue from a live subject using a compact and flexible MPME device.

Diffusion of Chlorin-p6 Across Phosphatidyl Choline Liposome Bilayer Probed by Second Harmonic Generation

We have investigated the diffusion of the photosensitizer Chlorin-p(6) (Cp(6)) across a egg lecithin lipid bilayer at different pH by the Second Harmonic Generation (SHG) method. Cp(6) has three ionizable carboxylic acid groups, and consequently, neutral and several ionic forms of Cp(6) are expected to be present in the pH range 3-8. The absorption spectra of Cp(6) get considerably modified in the presence of liposomes as the pH is decreased indicating that the drug liposome binding is pH dependent. The first pK(a) of interconversion (D-C) has been identified at pH ~7.0 by fluorescence measurement in an earlier work. In this work, the second pK(a) of interconversion (C-B) has been identified at pH ~4.8 by the hyper-Rayleigh scattering method. At acidic pH (3, 4, and 5), where species A, B, and C are dominant, the addition of liposomes to a Cp(6) solution generates an instantaneous rise (less than 1 s) in the second harmonic (SH) signal followed by decays whose time constants ranged from ten to hundreds of seconds. The instantaneous rise is attributed to the adsorption of Cp(6) to the outer lipid bilayer, and the decay is attributed to the diffusion of the neutral and charged (A and B) species of the drug. The observed fast and slow time constants for diffusion in the pH range 3-5 are attributed to the neutral (A) and ionic form (B) of Cp(6), respectively. At pH 6, the intensity of the generated SH signals on the addition of liposome reduced, and at physiological pH, it was too weak to be detected. These results are consistent with previous studies that show that the interaction between Cp(6) and egg-PC liposomes is pH dependent. At lower pH due to the presence of the hydrophobic species (A and B) of Cp(6), its interaction with liposomes is strong, and at higher pH, the abundance of the negatively charged hydrophilic species (C and D) decreases the interaction with the like charged liposomes. We have also studied the effect of increasing the bilayer rigidity by decreasing the temperature of the medium or by incorporating 50 mol % cholesterol in the lipid bilayer and observed that lowering of temperature has more profound effect on the diffusion rates. The characteristics of the SH signal changed significantly when liposomes incorporating 50 mol % cholesterol were used at a low (3 °C) temperature. Under these conditions, the SH signal consisted of an instantaneous (<1s) followed by a slower rise (10-90s), and then, it decayed on a much longer time scale. This slow rise of the SH signal at pH 3 and 4 may be attributed to the temperature dependent adsorption of the anionic species (B) of Cp(6) with the liposomes. Further investigations are required in order to understand clearly the pH dependent diffusion of this drug across lipid bilayers.

Multibeam second-harmonic generation by spatiotemporal shaping of femtosecond pulses

We present a technique for efficient generation of the second-harmonic signal at several points of a nonlinear crystal simultaneously. Multispot operation is performed by using a diffractive optical element that splits the near-infrared light of a mode-locked Ti:sapphire laser into an arbitrary array of beams that are transformed into an array of foci at the nonlinear crystal. We show that, for pulse temporal durations under 100 fs, spatiotemporal shaping of the pulse is mandatory to overcome chromatic dispersion effects that spread both in space and time the foci showing a reduced peak intensity that prevents nonlinear phenomena. We experimentally demonstrate arbitrary irradiance patterns for the second-harmonic signal consisting of more than 100 spots with a multipass amplifier delivering 28 fs, 0.8 mJ pulses at 1 kHz repetition rate.

Novel method for correcting light intensity fluctuation in the TDLAS system

A novel method for online correction of light intensity fluctuation in a practical tunable diode laser absorption spectroscopy (TDLAS) system with wavelength modulation is presented. The proposed method is developed according to the linear relation between peaks at multiple frequencies of sine modulation in the power spectral density of the demodulated second-harmonic (2f) signal and the incident light intensity. Those peaks are demonstrated experimentally and explained as residual power at the first-harmonic and third-harmonic frequencies after 2f demodulation of the residual amplitude modulation signal due to the limited integrating time constant of the lock-in-amplifier. This method can achieve real-time correction of light intensity fluctuations with only little calculation. It can work well in a very large range of light intensity and has great potential applications in the wavelength modulation spectroscopy system.

Structures and properties of layered barium borates Ba0.975[B6O9(OH)(O0.975Br0.025) · B2O(OH)3], Ba2[B5O8(OH)2](OH), Na2Ba2[B20O34(OH)4], and Ba5[B20O33(OH)4]H2O

A new hexaborate, Ba0.975[B6O9(OH)(O0.975Br0.025) · B2O(OH)3], was synthesized under hydrothermal conditions. This compound is structurally similar to tunnelite and the synthetic borates Pb[B6O10(OH) · B2O(OH)3], Pr[B6O10(OH) · B2O(OH)4], and Nd[B6O10 · B3O3(OH)4] · H2O studied earlier. In the new hexaborate and the refined pentaborate Ba2[B5O8(OH)2]OH, in which the polyanions adopt an orientation in layers unusual for pentaborates, thermal vibrations of the terminal groups were revealed. This fact reflects the real crystal structure. The nonlinear optical properties of the crystals of the polar pentaborate Na4Ba4[B20O34(OH)4] were determined. The crystal structure of the related pentaborate Ba5[B20O33(OH)4]H2O was considered. The factors most likely responsible for the difference in the second-harmonic generation signal for this pair were revealed.

Second-harmonic generation from coupled plasmon modes in a single dimer of gold nanospheres

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.

A new stilbazolium salt with perfectly aligned chromophores for second-order nonlinear optics: 4-N,N-Dimethylamino-4′-N′-methyl-stilbazolium 3-carboxy-4-hydroxybenzenesulfonate

A new organic nonlinear optical crystal 4-N,N-dimethylamino-4′-N′-methyl-stilbazolium 3-carboxy-4-hydroxybenzenesulfonate (DSCHS) has been developed with very promising properties for quadratic nonlinear optical applications. DSCHS single crystals with non-centrosymmetric structure have been obtained from aqueous methanol solution. X-ray crystallographic analysis revealed that the crystal structure of DSCHS is triclinic P1 with the chromophores aligned perfectly parallel, leading to the maximum possible order parameter <cos3θ> = 1 in the crystalline state, which is optimal for electro-optics, THz-wave generation and field detection applications. Kurtz powder test has shown that DSCHS exhibits a very large second-order optical nonlinearity, with a 30 percent higher second-harmonic signal than the well-known organic nonlinear optical crystal 4-N,N-dimethylamino-4′-N′-methyl-stilbazolium tosylate (DAST).