Resonant surface second harmonic generation from Au films on NaCl(100)

In this paper, we investigated the second harmonic (SH) and the third harmonic (TH) generations in nanorods and nanotubes. Nonlinear free and bound electrons responses of metal combined with the third-order nonlinearity of dielectric core were utilized to study the nonlinear response of nanotubes made of noble metals such as gold. The impacts of the dielectric constant of core medium, thickness of metal shell, and size of nanotube on the SH and TH conversion efficiency are reported. The physical interpretations behind the results are discussed. Finally, we have shown that enhancement of the SH and TH generations are more noticeable and adjustable by varying the core-shell parameters compared to those of nanorods.

We theoretically study how the intensity of second harmonic generation (SHG) for a sheet of two-dimensional (2D) material is controlled by an underlying layered structure. By utilizing the transfer matrix method with the inclusion of a nonlinear sheet current to describe the response of the 2D material, an explicit expression for the intensity of upward propagating second harmonic (SH) light is obtained, and the effects of the layered structure can be identified by a structure factor β, defined as the ratio of SH intensity from such a structure to that from a freely suspended 2D material. Our results show that the influence of a layered structure on the SHG intensity arises from interference effects of both the fundamental light and the SH light; the value of the structure factor is 0 ≤ β ≤ 64. Furthermore, when the incident light is pulsed, the interference effects are partially canceled due to the existence of many wave vectors and frequencies, and the cancellation becomes severe for thick films, small beam spots, and short pulses. For a specific structure of 2D material/dielectric film/substrate, the thickness of the dielectric film can effectively tune the value of β in an interval [βmin, βmax], and detailed discussions are performed for the thicknesses when these two extreme values can be obtained. When there is optical loss or the substrate is not perfectly reflective, the extreme value of βmax or βmin cannot reach 64 or 0. A large βmax requires two conditions to be fulfilled: (1) the substrate should be highly reflective, and (2) the refractive indices of the dielectric film at the fundamental and the SH frequencies should differ. Our results indicate how practical substrate structures can be used to achieve high SH signals, and the simple expression we give for the SH enhancement will be useful in characterizing the nonlinear susceptibility of 2D materials.

This paper demonstrates that the spatial distribution of electronic states of an arsenic ion implanted Si(111) substrate can be observed by using a wavelength tunable second harmonic (SH) microscope in a wide photon energy range from 2ℏω=1.96to5.19eV. The contrast in the SH intensity images between the As-doped area and the nondoped area depends greatly on the SH photon energy. For 2ℏω>3eV, optical second harmonic generation (SHG) from the nondoped area was stronger than from the doped area, and the contrast was reversed for 2ℏω⩽2.33eV. The contrast in the SH intensity images was considerably different from that in the linear optical reflection images, indicating that spectroscopic SH microscopy can provide different informations on electronic levels from that associated with the linear optical response. It is suggested that the larger SH intensity from the nondoped area for 2ℏω>3eV results from the resonant SHG enhancement effect associated with the bulk Si E1 (3.4eV) and E2 (4.3eV) gaps. In the case of the doped area, a small resonant enhancement of the SH intensity was observed around 2ℏω=2.33eV. This resonance may result from an energy level created by the ion implantation.

Although tightly focused input beams for efficient second harmonic (SH) generation (SHG) are usually avoided because of material damage, this is exactly the condition needed for the generation of spatial solitons (QSS) based on quadratic (χ(2)) nonlinearities.[1,2] These QSS’es are mutually self-trapped fundamental (FW) and harmonic (SH) optical beams in which the mutual beam narrowing due to photon exchange incipient in up and down conversion balances diffraction. The generation of quadratic solitons significantly affects the SHG process, for example by placing an upper limit on the amount of fundamental that can be converted to SH, by increasing the bandwidth of the process etc.[3] Of particular interest are periodically poled ferroelectric media which are an important limit of non-critical phase-matching. In fact, periodically poled LiNbO3 (PPLN) has been shown to have the lowest soliton threshold of 1.5 GW/cm2 reported to date [4]. That pioneering work established the existence of quadratic solitons in periodically poled media but neither this work, or any other work on QSSes has addressed the impact of QSS on the SHG tuning curves.

We theoretically study the gain-assisted double plasmonic resonances to enhance second harmonic generation (SHG) in a centrosymmetric multilayered silver-dielectric-gold-dielectric (SDGD) nanostructure. Introducing gain media into the dielectric layers can not only compensate the dissipation and lead to giant amplification of surface plasmons (SPs), but also excite local quadrupolar plasmon which can boost SHG by mode matching. Specifically, as the quadrupolar mode dominates SHG in our nanostructure, under the mode matching condition, the intensity of second harmonic near-field can be enhanced by 4.43 × 102 and 1.21 × 105 times when the super-resonance is matched only at the second harmonic (SH) frequency or fundamental frequency, respectively. Moreover, the intensity of SHG near-field is enhanced by as high as 6.55 × 107 times when the nanostructure is tuned to double super-resonances at both fundamental and SH frequencies. The findings in this work have potential applications in the design of nanosensors and nanolasers.

The visibility of inverted domain structures using the second harmonic generation (SHG) microscope is discussed based upon the three-wave coupling equations. Without reference second harmonic (SH) waves (non-interference case), the SHG intensity at a domain boundary decreases steeply along the perpendicular direction to the domain wall, which is observed as a dark line. Thus the non-interference SHG microscope reveals the location of domain boundaries but not the domain polarity which the SHG interference microscope can do. In the case of periodically poled domain structures, the clear observation criterion is expressed with the wave-number offset between the fundamental and SH waves.

Second Harmonic Generation (SHG) has become a powerful tool for studying the surfaces of liquids and other centric systems [1], but due to the symmetry rule no Second Harmonic (SH) can be produced from their bulk. It is then of great interest that a number of recent experimental studies have shown strong SHG from randomly oriented suspension of finely fragmented purple membranes of Halobacterium halobium contain Bacteriorhodopsin (BR) [2 ], which belongs to the family of retinal proteins. The understanding of the nature of the SH signal itself still constitutes an obscure matter. Most of the mechanisms proposed for the description of this effect, have focused on the hyper-Rayleigh incoherent scattering, but some of them suggest also coherent nonlinear contributions into the SH signal.

Depending on the chosen fabrication process, nonlinear waveguides realized in periodically oriented material such as periodically poled lithium niobate (PPLN) can present different fabrication errors. In this paper, we present a detailed numerical study of the impact on the nonlinear performances of one or several stitching errors occurring during the realization of the periodic domains by e-beam writing. This study shows that contrary to what was expected, a single finite stitching error does not simply decrease the nonlinear efficiency but splits the second harmonic (SH) signal into a double peak spectrum, where the position of the peaks and their width at half-maximum depend not only on the poling period, the total length of the grating, and the waveguide parameters, but also on the amplitude and the position of the defect. The numerical results are confirmed by second harmonic generation (SHG) experiments performed in PPLN waveguides obtained by Soft Proton Exchange and where the nonlinear grating was composed of one to four e-beam-written 1.5-mm-long PPLN sections between which important stitching errors can occur. In this case the spectrum can be quite complicated. It is worth noting that similar errors (domains merging or missing domains) can occur also in the e-field poling process but they are randomly distributed along the propagation path. Therefore, this study is a first attempt to take them into account to explain experimental results and indicate the steps that have to be taken to improve the quality of the components.

The changes of the morphology during heating and the degree of crystallinity of dry and hydrated starch granules are investigated using second harmonic generation (SHG) based Stokes polarimetry. A spatial distribution of various polarization parameters, such as the degree of polarization (DOP), the degree of linear polarization (DOLP), and the degree of circular polarization (DOCP) are extracted and compared with the two dimensional second harmonic (SH) Stokes images of starch granules. The SH signal from hydrated and dry starch on heating differed significantly in DOLP and DOCP values, indicating that hydrated starch has a greater degree of ultrastructural amylopectin disorder. The detail of denaturation and the phase transition of hydrated starch demonstrate the significant influence of thermal processing.

Based on vector diffraction theory, an analytical integral representation to calculate the field gradient of focused electromagnetic fields is derived by using the differential recursion formula between the Bessel functions with different order. Within the phenomenological model for second harmonic generation (SHG) of centrosymmetric material, the second harmonic (SH) response of a single centrosymmetric spherical particle excited by a focused beam under different values of the NA is investigated theoretically. The results show that, with increasing NA, the SH radiation pattern of the surface response hardly changes. For the larger value of the NA, because the elements of the field gradient are almost the same order of magnitude and the relative magnitudes of Ey and Ez increase, the bulk response related to the parameters δ′ and ζ become remarkable.

Forthcoming low-energy consumption oxide electronics rely on the deterministic control of ferroelectric and multiferroic domain states at the nanoscale. In this review, we address the recent progress in the field of investigation of ferroic order in thin films and heterostructures, with a focus on non-invasive optical second harmonic generation (SHG). For more than 50 years, SHG has served as an established technique for probing ferroic order in bulk materials. Here, we will survey the specific new aspects introduced to SHG investigation of ferroelectrics and multiferroics by working with thin film structures. We show how SHG can probe complex ferroic domain patterns non-invasively and even if the lateral domain size is below the optical resolution limit or buried beneath an otherwise impenetrable cap layer. We emphasize the potential of SHG to distinguish contributions from individual (multi-) ferroic films or interfaces buried in a device or multilayer architecture. Special attention is given to monitoring switching events in buried ferroic domain- and domain-wall distributions by SHG, thus opening new avenues towards the determination of the domain dynamics. Another aspect studied by SHG is the role of strain. We will finally show that by integrating SHG into the ongoing thin film deposition process, we can monitor the emergence of ferroic order and properties in situ, while they emerge during growth. Our review closes with an outlook, emphasizing the present underrepresentation of ferroic switching dynamics in the study of ferroic oxide heterostructures.

A number of liquid crystalline cyclic pentamethylsiloxane compounds were synthesized containing high concentrations of covalently attached disperse red 1(4-[N-ethyl, N- hydroxyethylamino]-4'-nitroazobenzene) pendant groups. Corona poling (1.0 (mu) A/-5 kV) was used to align these pendant groups in thin films (1 - 2 micrometers ) produced by spin coating onto ITO covered glass substrates. The measured second harmonic (SH) intensities of these films were comparable to 1 mm thick, y-cut quartz. The initial rise in the SH signal at 25 degree(s)C occurred in less than 10 seconds. This was followed by an additional 20 - 50% increase in the signal over the next 1 - 15 minutes to a final equilibrium value. The SH signal of compounds in the smectic or nematic phase increased to a value of 0.7 - 1.0 X the quartz standard upon heating. An upper temperature limit for each material was observed prior to the dielectric breakdown of the film. The SH intensity typically decayed back to its prepoling value within one hour for films that were poled at 25 degree(s)C. Long term SH stability was observed in films that were poled at elevated temperatures. The intensity of the SH signal was found to be a function of the composition, liquid crystalline phase, and temperature.

Second harmonic generation in selenium-metal structures

The enhanced second-harmonic (SH) generation from Si (111) stripes induced by external cylindrical strain is investigated. The dependence of the intensity of the strain-induced SH on the sample azimuth shows that the Si under cylindrical strain has 3m symmetry, which is similar to that of the Si (111) surface. Further studies indicate that the intensity of the enhanced SH is a quadratic function of the cylindrical strain within the magnitude that the Si stripe can bear. For the p-polarized and s-polarized SH, the intensities are, respectively, enhanced by 47.9% and 13% at epsilon(0)=2.93x10(-4). The enhancement of SH is due to the contributions from the strain-induced second-order nonlinear susceptibility chi(strain)(2) to the bulk dipole.

Using a novel combination of fundamental and harmonic polarizations, we have used optical second-harmonic (SH) generation to probe the nonlinear currents induced parallel to the surface plane of a Si(001) crystal upon adsorption of Na, K, and Cs. For all three alkalis, we observe abrupt thresholds in SH intensity and relative SH phase shift at the same coverage of very nearly one-sixth of a monolayer. We speculate that these thresholds correspond to insulator-metal transitions, and that a recently observed low-coverage (2 × 3) structure is a Mott-Hubbard-like insulator.