Nondegenerate Two-photon Absorption Research Articles

Dispersion of two-photon absorption and nonlinear refraction in β -Ga2O3 from 350 to 515 nm

We report the wavelength dependencies of the two-photon absorption coefficients β as well as the nonlinear refractive index n2 of undoped β-Ga2O3 single crystal in the spectral range 350–515 nm (0.51 < Ephoto/Eg < 0.75). Femtosecond Z-scan measurements show that n2 decreases monotonically toward the shortwave side, while the maximum value of n2 is 5.0 × 10−19 m2/W near half of the bandgap, Eg. Interestingly, a second upward trend in β was observed when the incident photon energy is larger than 0.6Eg, indicating the impact of additional inter-band transitions with higher energy. A higher-energy band-to-band transition around 6.0 eV was determined by both femtosecond nondegenerate two-photon absorption spectroscopy and ab initio calculations. Our results could provide guidance for designing nonlinear β-Ga2O3 photonic devices in the UV-visible spectral range.

Research advances in nondegenerate two-photonabsorption and its applications

Nondegenerate two-photon absorption is a nonlinear optical effect in which two photons with different energy are absorbed by a medium simultaneously, resulting in a single electron transition from ground state to excited state through an intermediate virtual state. Compared with the degenerate two-photon absorption coefficient, the absorption coefficient of nondegenerate two-photon absorption is increased by tens or even hundreds of times due to the intermediate resonance effect, so it has great potentials in many nonlinear optical applications. Firstly, the basic principle of two-photon absorption is introduced and the enhancement mechanism of non-degenerate two-photon absorption is explained in this paper. Secondly, the basic method of measuring two-photon absorption is introduced in detail. Thirdly, the reports on nondegenerate two-photon absorption of three-dimensional semiconductor materials and two-dimensional materials are reviewed. Finally, the application progress of infrared detection and imaging, two-photon fluorescence microscope, all-optical switch and optical modulation is summarized, and the future research in this field is summarized and prospected.

Degenerate and non-degenerate two-photon absorption of coumarin dyes.

Two-photon absorption (2PA) spectroscopy is a robust bioimaging tool that depends on the determined cross-sections (σ2PA). The absorption of both photons occurs simultaneously with equivalent (degenerate) or different (non-degenerate) photon energies, D-2PA and ND-2PA, respectively. The former has been investigated experimentally and computationally for many systems, while the latter remains relatively unexplored computationally and limited experimentally. In this study, response theory using time-dependent density functional theory (TD-DFT) and the 2-state model (2SM) have been utilized to investigate σD-2PA and σND-2PA for the excitation to the lowest energy singlet state (S1) of coumarin, coumarin 6, coumarin 120, coumarin 307, and coumarin 343. Solvents involved were methanol (MeOH), chloroform (ClForm), and dimethylsulfoxide (DMSO), where the latter leads to the largest σ2PA. Values of σ2PA are largest for coumarin 6 and lowest for coumarin, which illustrates the effect of substituents. The 2SM clarifies how the largest cross-sections correspond to molecules with the largest transition dipole moments, μ01. In general, σD-2SM computations agree with σD-2PA. Moreover, σND-2SM are in qualitative agreement with σND-2PA with comparable enhancement relative to σD-2PA. Overall, σND-2PA are larger than σD-2PA where the increase is in the range of 22% to 49%, depending on the coumarin as well as the relative energies of the two photons. This work aids in future investigations into various fluorophores to understand their photophysical properties for ND-2PA.

Spectral imaging at high definition and high speed in the mid-infrared.

Spectral imaging in the mid-infrared (MIR) range provides simultaneous morphological and chemical information of a wide variety of samples. However, current MIR technologies struggle to produce high-definition images over a broad spectral range at acquisition rates that are compatible with real-time processes. We present a novel spectral imaging technique based on nondegenerate two-photon absorption of temporally chirped optical MIR pulses. This approach avoids complex image processing or reconstruction and enables high-speed acquisition of spectral data cubes (xyω) at high-pixel density in under a second.

Strong effects of fast collisions between pulsed optical beams in a linear medium with weak cubic loss

We investigate fast collisions between pulsed optical beams in a linear medium with weak cubic loss that arises due to nondegenerate two-photon absorption. We introduce a perturbation method with two small parameters and use it to obtain general formulas for the collision-induced changes in the pulsed-beam’s shape and amplitude. Moreover, we use the method to design and characterize collision setups that lead to strong localized and nonlocalized intensity reduction effects. The values of the collision-induced changes in the pulsed-beam’s shape in both setups are larger by one to two orders of magnitude compared with the values obtained in previous studies of fast two-pulse collisions. Furthermore, we show that for nonlocalized setups, the graph of the collision-induced amplitude shift vs the difference between the first-order dispersion coefficients for the two pulsed-beams has two local minima. This finding represents the first observation of a deviation of the graph from the common funnel shape that was obtained in all previous studies of fast two-pulse collisions in the presence of weak nonlinear loss. The predictions of our perturbation theory are in good agreement with results of numerical simulations with the perturbed linear propagation model, despite the strong collision-induced effects. Our results can be useful for multisequence optical communication links and for reshaping of pulsed optical beams.

Single-Photon Infrared Imaging With a Silicon Camera Based on Long-Wavelength-Pumping Two-Photon Absorption

We experimentally demonstrated an ultra-sensitive imaging system for telecom photons based on the non-degenerate two-photon absorption in a silicon-based electron multiplying charge-coupled device (EMCCD). The proposed long-wavelength-pumping scheme with mid-infrared pulsed excitation could not only effectively increase the two-photon absorption coefficient, but also significantly suppress the background noise caused by the harmonic absorption of the strong pumping field. In comparison to the photoelectric response via the degenerate two-photon absorption, the implemented configuration could offer over 30-folded enhancement of the photon-counting rate in the infrared imaging. The resulting detection sensitivity up to 1 photon/pixel/pulse was unprecedentedly approached, thus facilitating the single-photon operation. The elimination of the stringent phase matching as typically required in the optical parametric conversion has led to a high spatial resolution of 13 μm. Moreover, the on-chip nonlinearity of the optical imager would enable a broadband spectral window and an enlarged field of view. In combination with the 5-ps temporal resolution due to the coincident optical gating, the presented imaging system would find various promising applications, such as low-light fluorescence lifetime microscopy and photon counting time-of-flight 3D imaging.

Publisher Correction: Sensitive mid-infrared detection in wide-bandgap semiconductors using extreme non-degenerate two-photon absorption

Publisher Correction: Sensitive mid-infrared detection in wide-bandgap semiconductors using extreme non-degenerate two-photon absorption

Near-infrared non-degenerate two-photon absorption coefficients of bulk GaAs and Si.

We investigate the non-degenerate two-photon absorption coefficient β(ω1, ω2) as a function of the non-degeneracy parameter ω1/ω2 for bulk GaAs and Si at a constant transition energy ℏ ω 1+ℏ ω 2=1.57eV. In both materials, the two-photon absorption strength increases with increasing ω1/ω2 regardless of the direct and indirect character of the bandgap. The GaAs measurement data agrees well with corresponding theoretical predictions for direct semiconductors. The Si data reveals similar trends albeit with smaller overall absorption strength. In addition, different crystallographic orientations and polarization configurations are analyzed.

High-speed 2D and 3D mid-IR imaging with an InGaAs camera.

Recent work on mid-infrared (MIR) detection through the process of non-degenerate two-photon absorption (NTA) in semiconducting materials has shown that wide-field MIR imaging can be achieved with standard Si cameras. While this approach enables MIR imaging at high pixel densities, the low nonlinear absorption coefficient of Si prevents fast NTA-based imaging at lower illumination doses. Here, we overcome this limitation by using InGaAs as the photosensor. Taking advantage of the much higher nonlinear absorption coefficient of this direct bandgap semiconductor, we demonstrate high-speed MIR imaging up to 500 fps with under 1 ms exposure per frame, enabling 2D or 3D mapping without pre- or post-processing of the image.

Nondegenerate two-photon absorption in ZnSe: Experiment and theory

We experimentally and theoretically investigate the non-degenerate two-photon absorption coefficient $\beta(\omega_1,\omega_2)$ in the prototypical semiconductor ZnSe. In particular, we provide a comprehensive data set on the dependence of $\beta(\omega_1,\omega_2)$ on the non-degeneracy parameter $\omega_1/\omega_2$ with the total frequency sum $\omega_1+\omega_2$ kept constant. We find a substantial increase of the two-photon absorption strength with increasing $\omega_1/\omega_2$. In addition, different crystallographic orientations and polarization configurations are investigated. The nonlinear optical response is analyzed theoretically by evaluating the multiband semiconductor Bloch equations including inter- and intraband excitations in the length gauge. The band structure and the matrix elements are taken an eight-band k.p model. The simulation results are in very good agreement with the experiment.

Tunable nonlinear optical responses of few-layer graphene through lithium intercalation

Abstract Intercalation has been demonstrated to be a powerful tool for tuning the physical and chemical properties of two-dimensional (2D) materials, providing the highest possible doping level and an ideal system to study various electronic states. In this work, we demonstrate that the nonlinear absorption effect of few-layer graphene (about 6–8 layers) is changed from saturable absorption (SA) to reverse saturable absorption (RSA) after lithium intercalation. This is attributed to the increase of Fermi energy owing to the charge transfer from Li to graphene layers in intercalated compounds (LiC6). And the change of nonlinear absorption effect is revisable after deintercalation. In addition, the modulation depth of RSA in lithiated graphene is found to rise with the decrease of incident laser wavelength, different from that of pristine graphene. Besides, the dispersion relationships of degenerate and nondegenerate two-photon absorption are analyzed from the results of nonlinear absorption and transient dynamics of lithiated graphene, indicating the 1.91–2.21 eV upshift of the Fermi surface. Our findings of the intercalation-tunable nonlinear optical absorption effect pave the way for the construction of nonlinear optical devices based on 2D intercalation compounds.

Rapid chemically selective 3D imaging in the mid-infrared.

The emerging technique of mid-infrared optical coherence tomography (MIR-OCT) takes advantage of the reduced scattering of MIR light in various materials and devices, enabling tomographic imaging at deeper penetration depths. Because of challenges in MIR detection technology, the image acquisition time is, however, significantly longer than for tomographic imaging methods in the visible/near-infrared. Here we demonstrate an alternative approach to MIR tomography with high-speed imaging capabilities. Through femtosecond nondegenerate two-photon absorption of MIR light in a conventional Si-based CCD camera, we achieve wide-field, high-definition tomographic imaging with chemical selectivity of structured materials and biological samples in mere seconds.

Highly Sensitive Detection of Infrared Photons by Nondegenerate Two-Photon Absorption Under Midinfrared Pumping

We demonstrate highly sensitive photon counting in the infrared region based on two-photon absorption (2PA) in a silicon avalanche photodiode, where the required photon energy for inducing effective conductivity is provided by an intense midinfrared (MIR) field at 3 $\ensuremath{\mu}\mathrm{m}$. The used MIR pumping scheme can not only benefit from the enhanced 2PA coefficient in the nondegenerate regime, but also eliminate the detrimental background noises due to the pump harmonic excitation of the pump. Consequently, the enhancement factor for the signal counting rate unprecedentedly reached about ${10}^{5}$ with input infrared pulses at the femtojoule level. Additionally, the noise equivalent power is substantially improved by 2 orders of magnitude in comparison to conventional schemes with near-infrared pumping. Therefore, the presented configuration might provide an alternative to realize sensitive infrared detection and imaging with desirable features of room-temperature operation, no phase-matching requirement, and broadband responding window, which can find a variety of applications, including remote ranging, sensitive sensing, biochemical imaging, and trace spectroscopy.

Adaptive noise canceling for transient absorption microscopy.

.Significance: Ultrafast fiber lasers are an attractive alternative to bulk lasers for nonlinear optical microscopy for their compactness and low cost. The high relative intensity noise (RIN) of these lasers poses a challenge for pump-probe measurements such as transient absorption and stimulated Raman scattering, along with modalities that provide label-free contrast from the vibrational and electronic structure of molecules.Aim: Digital adaptive filtering was applied to determine the applicability for canceling laser RIN in a transient absorption microscope with an ultrafast fiber laser source.Approach: Digitized signals from the transmitted probe and reference photodetectors were fed to an adaptive filter in MATLAB, running in a noise canceling configuration. This result was then fed to a software lock-in algorithm to demodulate the pump-probe signal. Images were built up one line scan at a time with a 3.5-kHz resonant scanner, with averaging. The imaging target was , which exhibits nondegenerate two-photon absorption at the pump/probe wavelengths used (530-nm pump and 490-nm probe).Results: Without adaptive noise cancellation, the lock-in output primarily passes the laser RIN within its detection bandwidth, resulting in images that closely follow the linear transmissivity and lack sensitivity to pump-probe time delay. With adaptive noise cancellation in front of the lock-in, the RIN rejection is enough to restore the z-sectioning and sensitivity to pump-probe delay, as expected for transient absorption. Results were limited primarily by noise from the photodetector and analog-to-digital converter.Conclusions: Digital adaptive noise cancellation, even when limited by electronics noise, can recover pump-probe signals by removal of laser RIN, under conditions where averaging alone fails.

Determination of the contributions of degenerate and non-degenerate two-photon absorption response in silicon avalanche photodiode for infrared photon detection

The study of non-linear interactions in semiconductor photo-electronic devices to achieve effective and fast photon identification is an ongoing and important task. We investigated the specific contribution of degenerate and non-degenerate two-photon absorption (D-TPA and ND-TPA) response in silicon avalanche photodiode (Si-APD) for infrared photon detection at room temperature. We experimentally demonstrated that when the two laser pulses overlapped, the average D-TPA quantum detection efficiencies at 1800 nm, and that at 1550 nm were measured as 3.3 × 10−16 counts•pulse/photon2, 4.3 × 10−15 counts•pulse/photon2, respectively. And the ND-TPA quantum detection efficiency of 1800 nm and 1550 nm was measured to be 7.9 × 10−16 counts•pulse/photon2. This study provides a solution for the practical infrared photon detection devices based on TPA effect in Si-APDs.

Infrared chemical imaging through non-degenerate two-photon absorption in silicon-based cameras

Chemical imaging based on mid-infrared (MIR) spectroscopic contrast is an important technique with a myriad of applications, including biomedical imaging and environmental monitoring. Current MIR cameras, however, lack performance and are much less affordable than mature Si-based devices, which operate in the visible and near-infrared regions. Here, we demonstrate fast MIR chemical imaging through non-degenerate two-photon absorption (NTA) in a standard Si-based charge-coupled device (CCD). We show that wide-field MIR images can be obtained at 100 ms exposure times using picosecond pulse energies of only a few femtojoules per pixel through NTA directly on the CCD chip. Because this on-chip approach does not rely on phase matching, it is alignment-free and does not necessitate complex postprocessing of the images. We emphasize the utility of this technique through chemically selective MIR imaging of polymers and biological samples, including MIR videos of moving targets, physical processes and live nematodes.

Error-free data transmission through fast broadband all-optical modulation in graphene–silicon optoelectronics

Ultrafast third order nonlinearity in silicon photonics is promising for all-optical signal processing beyond 100 Gbit/s. However, the coexistence of slower dynamical responses, such as mesoscopic Drude free-carrier plasma or thermal nonlinearities, degrades high-speed signal integrity. Here, we introduce atomic-layer graphene onto the silicon nanophotonic platform to leverage its unique nondegenerate two-photon absorption and ultrafast carrier dynamics, demonstrating broadband and fast bitrate transmission through cross-absorption modulation. Multichannel error-free optical transmission across telecommunication C- and L-bands is demonstrated with 10−12 bit-error rates at a data transmission rate of 1 Gbps. The bandwidth of the hybrid silicon–graphene structure is demonstrated at least up to 25 GHz. The broadband cross-absorption modulation over 640 nm in graphene–silicon optoelectronics provides a promising scalable material platform for high-speed all-optical signal processing.

Highly Conjugated, Fused-Ring, Quadrupolar Organic Chromophores with Large Two-Photon Absorption Cross-Sections in the Near-Infrared.

The two-photon absorption (2PA) properties are investigated for two series of organic, π-conjugated, fused-ring, quadrupolar A-π-D-π-A chromophores of the type originally developed as nonfullerene acceptors for organic photovoltaics. These molecules are found to exhibit large nondegenerate two-photon absorption (ND2PA) cross-sections (ca. 6-27 × 103 GM) in the near-infrared (NIR). In the first series, involving molecules of varying core size, ND2PA spectra and cross-sections characterized by femtosecond ND2PA spectroscopy in chloroform solutions reveal that increases in core size, and thus conjugation length, leads to substantially red-shifted and enhanced 2PA. In a second series, variation of the strength of the terminal acceptor (A) with constant core size (seven rings, indacene-based) led to less dramatic variation in the 2PA properties. Among the two core types studied, compounds in which the donor has a thieno[3,2-b]thiophene center demonstrate larger 2PA cross-sections than their indacene-centered counterparts, due to the greater electron-richness of their cores amplifying intramolecular charge transfer. Excited-state absorption (ESA) contributions to nonlinear absorption measured by open-aperture Z-scans are deduced for some of the compounds by analyzing the spectral overlap between 2PA bands and NIR ESA transitions obtained by ND2PA and transient absorption measurements, respectively. ESA cross-sections extracted from transient absorption and irradiance-dependent open-aperture Z-scans are in reasonable agreement, and their moderate magnitudes (ca. 10-21 m2) suggest that, although ESA contributions are non-negligible, the effective response is predominantly instantaneous 2PA.

Nondegenerate two-photon absorption in GaAs/AlGaAs multiple quantum well waveguides

We present femtosecond pump-probe measurements of the nondegenerate (1960$\,$nm excitation and 1176--1326$\,$nm probe) two-photon absorption spectra of 8 $\,$nm GaAs/12$\,$nm Al$_{0.32}$Ga$_{0.68}$As quantum well waveguides. Experiments were performed with light pulses co-polarized normal and tangential to the quantum well plane. The results are compared to perturbative calculations of transition rates between states determined by the $\mathbf{k}\cdot\mathbf{p}$ method with an 8 or 14 band basis. We find excellent agreement between theory and experiment for normal polarization, then use the model to support predictions of orders-of-magnitude enhancement of nondegenerate two-photon absorption as one constituent photon energy nears an intersubband resonance.

Sensitive Infrared Photon Counting Detection by Nondegenerate Two-Photon Absorption in Si APD

We report on the sensitive detection of photons at broadband infrared wavelengths based on the nondegenerate two-photon absorption in the Si avalanche photodiodes. The detected 1700~1850 nm infrared photon energy is lower than Si band gap and the energy difference is complemented by a high intensity pump laser field at 1550 nm. It is thus possible to capitalize on the low noise property of large band gap materials for detecting low energy photons. And the linear intensity response of the detector to the incident infrared photons was observed when the power of pump laser was about $12.42\mu $ W, indicating the dominance of nondegenerate two-photon absorption in the infrared photon detection. An enhancement factor of 20 was observed for the incident signal photon numbers of $\sim 0.14\times 10^{\mathbf {6}}$ photons per pulse. We offer an alternative to sensitive detection of infrared light. This may also provide new ideas for broadband infrared photon detection in different applications such as optical comb laser ranging, infrared bio-image and so forth.