Two-photon Lasing Research Articles

Cooperative two-photon lasing in two quantum dots embedded inside a photonic microcavity

Cooperative two-photon lasing in two quantum dots embedded inside a photonic microcavity

Nondegenerate two-photon lasing in a single quantum dot

Nondegenerate two-photon lasing in a single quantum dot

Laser Microsurgery in Drosophila Larvae Using the MicroPoint Ablation System.

Laser microsurgery is a robust method to ablate specific cells in the nervous system and probe the functional consequences of their loss in the animal. By introducing focal lesions to small locations in the animal, laser microsurgery also enables disruptions of specific connections within neuronal circuits and the study of how the nervous system responds to precise forms of damage (for instance, damage to specific axons or dendrites, which have been found to evoke different kinds of responses in neurons). The MicroPoint laser is a pulsed dye laser that can be mounted onto any standard microscope, hence is an affordable alternative to two-photon lasers for providing high powered focal ablations. This protocol describes how to use a MicroPoint laser ablation system to induce focal injuries in Drosophila larvae. This protocol guides a user who has access to a MicroPoint laser that has already been installed onto an appropriate microscope for high-resolution imaging and configured for laser ablation using Coumarin 440 dye. The protocol covers how to use the laser to carry out surgeries or ablation, how to change the laser dye and calibrate the power settings, and how to make sure the laser is properly focused. While the protocol provides an example of axotomy (axon severing) in the peripheral nervous system of Drosophila larvae, use of the MicroPoint system can be adapted to other focal surgeries in other organisms.

Modeling and analysis of buffer gas effect on 52S1/2→52D5/2 and 52S1/2→72S1/2 broadened two-photon pumped Rb vapor lasers

The study introduces helium (He) as a buffer gas to theoretically investigate the characteristics of two-photon pumped Rb vapor laser (Rb-TPAL) in order to enhance the pumping absorption efficiency of Rb-TPAL and consequently achieve high-power laser output. The analysis is based on a three-dimensional computational model, incorporating the spectral distribution of pump and absorption, as well as the influence of He on the absorption spectrum. The theoretical calculation of the dependence of the 52S1/2 → 52D5/2 transition broadened as a function of the pressure of He has good agreement with experimental results. We also simulated the influence of the pump linewidth and pressure of He on the output characteristics when 52S1/2 → 52D5/2 and 52S1/2 → 72S1/2 transitions in Rb-TPAL. A comparative analysis revealed that opting for the 52S1/2 → 72S1/2 transition can achieve higher optical–optical efficiency. The results also substantiate that the addition of a small amount of He has a positive impact on the laser output, consistent with experimental findings. Our study is crucial for designing the high-power multi-wavelength output Rb-TPAL system.

Dynamic Multiplex Tissue Imaging in Inflammation Research.

Inflammation is a highly dynamic process with immune cells that continuously interact with each other and parenchymal components as they migrate through tissue. The dynamic cellular responses and interaction patterns are a function of the complex tissue environment that cannot be fully reconstructed ex vivo, making it necessary to assess cell dynamics and changing spatial patterning in vivo. These dynamics often play out deep within tissues, requiring the optical focus to be placed far below the surface of an opaque organ. With the emergence of commercially available two-photon excitation lasers that can be combined with existing imaging systems, new avenues for imaging deep tissues over long periods of time have become available. We discuss a selected subset of studies illustrating how two-photon microscopy (2PM) has helped to relate the dynamics of immune cells to their in situ function and to understand the molecular patterns that govern their behavior in vivo. We also review some key practical aspects of 2PM methods and point out issues that can confound the results, so that readers can better evaluate the reliability of conclusions drawn using this technology.

Two-Photon Lasing from Two-Dimensional Homologous Ruddlesden-Popper Perovskite with Giant Nonlinear Absorption and Natural Microcavities.

Two-dimensional Ruddlesden-Popper perovskites (RPPs) with multiple quantum well-like structures, strong excitonic quantum confinement, and high stability are promising optical gain media. However, the lasing from such material with a small number of inorganic well layers is difficult to achieve. Herein, we demonstrate the low-threshold upconversion lasing from the homologous RPP (PEA)2(MA)n-1PbnI3n+1 (n = 2 and 3) microflakes with wavelength varies from 598 to 637 nm under 800 nm laser excitation at low temperature (≤153 K). Using the micro Z-scan technique, we discovered that the RPP flakes have a giant two-photon absorption coefficient β as high as 3.6 × 103 cm GW-1, resulting in the effective upconversion transition under two-photon excitation. Furthermore, the self-formation of Fabry-Pérot microcavities provides the support for lasing emission from the n ≥ 2 RPP flakes. Calculation results and microscopic transient absorption measurements reveal that low-threshold lasing is due to the high differential gain coefficient and the suppressed nonradiative Auger recombination rate inside the quantum confinement structures. These properties enable RPPs as potential gain media for developing upconversion microcavity lasers.

New Two-Photon Absorbing Squaraine Derivative with Efficient Near-Infrared Fluorescence, Superluminescence, and High Photostability

The nature of linear photophysical and nonlinear optical properties of a new squaraine derivative 2,4-bis[4-(azetidyl)-2-hydroxyphenyl]squaraine (1) with efficient near-infrared (NIR) emission was comprehensively analyzed based on spectroscopic, photochemical, and two-photon absorption (2PA) measurements, along with quantum chemical analysis. The steady-state absorption, fluorescence, and excitation anisotropy spectra of 1 and its fluorescence emission lifetimes revealed the multiple aspects of the electronic structure of 1, including the relative orientations of the main transition dipoles, effective rotational volumes in solvents of different polarities, and a maximum molar extinction of 1.35 × 10-5 M-1·cm-1, which is unusually small for similar symmetric squaraines. The degenerate 2PA spectrum of 1 was obtained over a broad spectral range under femtosecond excitation, using standard open-aperture Z-scan and two-photon induced fluorescence methods, revealing maximum 2PA cross sections of ∼400 GM. Squaraine 1 exhibited efficient superluminescence emission in the polar solvent (dichloromethane) at room temperature under femtosecond pumping conditions. Quantum chemical analysis of the electronic structure of 1 was performed using the DFT/TD-DFT level of theory and found to be in good agreement with experimental data. The new squaraine derivative 1 displayed high fluorescence quantum yield, efficient NIR superluminescence, large 2PA cross sections, and high photostability with a photodecomposition quantum yield ∼4 × 10-6, suggesting its potential for applications in two-photon fluorescent bioimaging and lasing.

Two-photon excited lasing for detection of amyloids in brain tissue.

Two-photon excitation of emissive markers with near-infrared (NIR) light is of a particular interest for imaging in biology and medicine because NIR light is relatively weakly absorbed and scattered by tissues. At the same time the mechanism of two-photon absorption allows excitation of molecules located deep inside a scattering medium. In this work we demonstrate that the two-photon excitation combined with the effect of light amplification in the stimulated emission process provides a sensitive method for detecting amyloids of different forms. We investigate the two-photon excited amplified spontaneous emission (ASE) of a fluorescent dye, coumarin 307, in the brain tissue infiltrated with various amyloid phantoms i.e. oligomers, protofibrils and mature fibrils. All these forms of amyloids can be detected by observation of ASE and determination of thresholds for light amplification. On this basis we suggest that a relatively simple extension of currently used emission-based optical spectroscopy techniques can provide key information on pathogenic amyloid structures in tissue.

Mutual cooperative effects between the mode components of two-photon and Raman induced cavity lasing processes

The paper proposes to unify the two-photon laser and induced cooperative scattering Raman lasing in which the flying ensemble of two-level excited radiators are coupled with the bimodal cavity field in nonlinear two-photon and scattering interactions. It discusses the situation in which the induced two-quantum lasing takes place together with the cooperative scattering conversion of photons between the pump, Stokes, and anti-Stokes cavity modes. The proposed master equation describes cooperative energy exchanges between Raman and two-photon lasing processes by portions of energies multiple to the energy of the entangled photon pair.The generators of such emission and absorption processes belonging to the symmetries of Raman conversion and two-photon cooperative generation are unified. The first symmetry belongs to su(2) algebra connected to the scattering conversion in the Stokes, pump, and anti-Stokes modes of cavity (Opt. Commun.,285(5) (2012) 686–692). The second one belongs to multi-mode su(1,1) symmetry which quantifies the cooperative process belonging to two-photon emission in cavity/fiber mode components of field (see Opt. Commun. 247(4–6) (2005) 381–392). The bimodal collective photon operators are introduced describing the emission or absorption acts of the fixed portion of energy from the cavity equal to the transition energy between the states of each excited atom. A key impact of the study focuses on the statistical properties of the bimodal field and their detection possibilities are proposed for the description of the time evolution of quantum correlations between the field components of Raman conversion and two-photon emission.

Advances in Two-Photon Imaging in Plants.

Live and deep imaging play a significant role in the physiological and biological study of organisms. Two-photon excitation microscopy (2PEM), also known as multiphoton excitation microscopy, is a fluorescent imaging technique that allows deep imaging of living tissues. Two-photon lasers use near-infrared (NIR) pulse lasers that are less invasive and permit deep tissue penetration. In this review, recent advances in two-photon imaging and their applications in plant studies are discussed. Compared to confocal microscopy, NIR 2PEM exhibits reduced plant-specific autofluorescence, thereby achieving greater depth and high-resolution imaging in plant tissues. Fluorescent proteins with long emission wavelengths, such as orange–red fluorescent proteins, are particularly suitable for two-photon live imaging in plants. Furthermore, deep- and high-resolution imaging was achieved using plant-specific clearing methods. In addition to imaging, optical cell manipulations can be performed using femtosecond pulsed lasers at the single cell or organelle level. Optical surgery and manipulation can reveal cellular communication during development. Advances in in vivo imaging using 2PEM will greatly benefit biological studies in plant sciences.

Second harmonic generation in colloidal CdSe/CdS nanoplatelets

In this Letter, we report the second harmonic generation (SHG) in a colloidal solution of CdSe/CdS nanoplatelets (NPLs) in the case of two-photon excitation in the region of exciton transition from the light holes sub-band to the conduction sub-band (549 nm, 1lh-1e) by femtosecond laser pulses (1064 nm, 100 kHz). Discovery of the SHG in colloidal solutions of NPLs opens up new perspectives for their use as biomarkers or for optical imaging, since in contrast to two-photon photoluminescence the SHG can increase both spectral and temporal resolution by several orders of magnitude. The SHG is also extremely important to consider when designing two-photon pumping lasers.

Exciting Wavelength and Concentration Related Two-Photon Fluorescence of Single and Mixed Laser Dyes.

Two-photon nonlinear process induced fluorescence of Rhodamine 6G (R6G), Rhodamine B (RB), and their mixed aqueous solutions in mass proportion of 1:1, is experimentally observed by different exciting wavelengths. It shows that, for each sample, the exciting wavelength can influence the fluorescence intensity considerably but only slightly influence the peak wavelength of the spectrum. The optimal exciting wavelengths of R6G and the mixed dyes are around 700nm. While for RB, the optimal exciting wavelengths can be 700nm and 620nm. For each dye sample, the spectral red-shift will occur as increase of the solution concentration. The mixing of the two dyes will cause the spectral red-shift with regard to the single dye under our experimental conditions. Moreover, in comparison, at lower concentrations, the mixed dye has relatively intense fluorescence. This work is of significance for determining the optimal exciting wavelength and developing the tunable two-photon dye lasers.

Water-resistant perovskite nanodots enable robust two-photon lasing in aqueous environment

Owing to their large absorption cross-sections and high photoluminescence quantum yields, lead halide perovskite quantum dots (PQDs) are regarded as a promising candidate for various optoelectronics applications. However, easy degradation of PQDs in water and in a humid environment is a critical hindrance for applications. Here we develop a Pb-S bonding approach to synthesize water-resistant perovskite@silica nanodots keeping their emission in water for over six weeks. A two-photon whispering-gallery mode laser device made of these ultra-stable nanodots retain 80% of its initial emission quantum yield when immersed in water for 13 h, and a two-photon random laser based on the perovskite@silica nanodots powder could still operate after the nanodots were dispersed in water for up to 15 days. Our synthetic approach opens up an entirely new avenue for utilizing PQDs in aqueous environment, which will significantly broaden their applications not only in optoelectronics but also in bioimaging and biosensing.

Adiabatic population transfer in the D1 transition of K39

Four-photon stimulated Raman adiabatic passage–like (STIRAP-like) processes in the frame of the D1 optical transition line of atomic 39K are investigated theoretically by means of a rigorous model that takes into account all the atomic states involved in the interaction with the pump and Stokes light fields and is valid for any field intensities. The same sequential up-down-up-down transition involving two pump (up) and two Stokes (down) photons, going from the initial ground state |F=2,M=+2? to the final ground state |F=1,M=0?, which was proven in the past to be very convenient for two-photon amplification and lasing, is considered here. The fact that two atomic states, one with F=1 and another with F=2, participate at each intermediate step of the multiphoton process makes the existence of an ideal unique adiabatic transfer state impossible, and at exact four-photon resonance the population-transfer efficiency to the final atomic state is low (below 60% in general, 80% in the best conditions). Nevertheless, it is shown that by choosing appropriate static detunings for the pump and Stokes fields with respect to the atomic transitions the system follows, sequentially, two adiabatic states, connected by an efficient diabatic passage, so that population-transfer efficiency asymptotically approaching 100% for increasing field amplitudes can be reached. These results are quite robust and suggest the possibility of using STIRAP (or STIRAP-like) pumping to, among other applications, increase the (presently very low) efficiency of two-photon amplification and lasing, a so far unfulfilled goal in quantum and nonlinear optics.

Intraparticle FRET for Enhanced Efficiency of Two-Photon Activated Photodynamic Therapy.

Photodynamic therapy (PDT) still faces two main problems on cancer therapy. One is how to improve PDT efficiency against hypoxic environment of tumors. The other one is how to overcome the limit of short wavelength light to increase PDT treatment depth. In this work, an intraparticle fluorescence resonance energy transfer (FRET) platform is designed to address these problems together. The nanoparticles are doped with multicomponents, such as catalase, two-photon dyes, and traditional photosensitizers, with a simple "one-pot" and green method. On the one hand, catalase can catalyze intracellular H2 O2 into O2 and promote PDT efficiency. One the other hand, photosensitizers can be excited indirectly by two-photon lasers through an intraparticle FRET mechanism, which results in deeper tissue penetration for PDT. These properties are verified through the material induced cytotoxicity in light or in dark and in vivo blocking blood-vessel experiment.

Resolution improvement of 3D stereo-lithography through the direct laser trajectory programming: Application to microfluidic deterministic lateral displacement device

The vast majority of current microfluidic devices are produced using soft lithography, a technique with strong limitations regarding the fabrication of three-dimensional architectures. Additive manufacturing holds great promises to overcome these limitations, but conventional machines still lack the resolution required by most microfluidic applications. 3D printing machines based on two-photon lasers, in contrast, have the needed resolution but are too limited in speed and size of the global device. Here we demonstrate how the resolution of conventional stereolithographic machines can be improved by a direct programming of the laser path and can contribute to bridge the gap between the two above technologies, allowing the direct printing of features between 10 and 100 μm, corresponding to a large fraction of microfluidic applications. This strategy allows to achieve resolutions limited only by the physical size of the laser beam, decreasing by a factor at least 2× the size of the smallest features printable, and increasing their reproducibility by a factor 5. The approach was applied to produce an open microfluidic device with the reversible seal, integrating periodical patterns using the simple motifs, and validated by the fabrication of a deterministic lateral displacement particles sorting device. The sorting of polystyrene beads (diameter: 20 μm and 45 μm) was achieved with a specificity >95%, comparable with that achieved with arrays prepared by microlithography.

Two-Photon Laser Scanning Stereomicroscopy for Fast Volumetric Imaging.

Bessel beams have been successfully used in two-photon laser scanning fluorescence microscopy to extend the depth of field (EDF), which makes it possible to observe fast events volumetrically. However, the depth information is lost due to integration of fluorescence signals along the propagation direction. We describe the design and implementation of two-photon lasers scanning stereomicroscopy, which allows viewing dynamic processes in three-dimensional (3D) space stereoscopically in real-time with shutter glasses at the speed of 1.4 volumes per second. The depth information can be appreciated by human visual system or be recovered with correspondence algorithms for some cases.

Multilayer Microcapsules for FRET Analysis and Two-Photon-Activated Photodynamic Therapy.

Microcapsules obtained by layer-by-layer assembly provide a good platform for biological analysis owing to their component diversity, multiple binding sites, and controllable wall thickness. Herein, different assembly species were obtained from two-photon dyes and traditional photosensitizers, and further assembled into microcapsules. Fluorescence resonance energy transfer (FRET) was shown to occur between the two-photon dyes and photosensitizers. Confocal laser scanning microscopy (CLSM) with one- and two-photon lasers, fluorescence lifetime imaging microscopy (FLIM), and time-resolved fluorescence spectroscopy were used to analyze the FRET effects in the microcapsules. The FRET efficiency could easily be controlled through changing the assembly sequence. Furthermore, the capsules are phototoxic upon one- or two-photon excitation. These materials are thus expected to be applicable in two-photon-activated photodynamic therapy for deep-tissue treatment.

Observation of Nondegenerate Two-Photon Gain in GaAs.

Two-photon lasers require materials with large two-photon gain (2PG) coefficients and low linear and nonlinear losses. Our previous demonstration of large enhancement of two-photon absorption in semiconductors for very different photon energies translates directly into enhancement of 2PG. We experimentally demonstrate nondegenerate 2PG in optically excited bulk GaAs via femtosecond pump-probe measurements. 2PG is isolated from other pump induced effects through the difference between measurements performed with parallel and perpendicular polarizations of pump and probe. An enhancement in the 2PG coefficient of nearly 2 orders of magnitude is reported. The results point a possible way toward two-photon semiconductor lasers.

Synthesis, structures, and photophysical properties of two novel trinuclear Hg(II)complexes

ABSTRACTTwo novel trinuclear Hg(II) complexes, namely, [Hg3Cl6(L1)2] (1) and [Hg3Cl6(L2)2] (2), (L1 = trans-4-[(p-N,N-dimethylamino)styryl]-N-acetic-acidpyridinium, L2 = trans-4-[(p-N-2-hydroxyethyl-N-methylamino)styryl]-N-acetic-acid pyridinium) have been synthesized and characterized by IR spectroscopy, elemental analysis, and X-ray single-crystal diffraction. In both 1 and 2, the tri- and tetra-coordinated Hg(II) atoms are linked by the carboxyl groups, resulting in the formation of trinuclear structures. Their linear absorption, one-photon fluorescence, two-photon fluorescence, and two-photon pumped up-conversion lasing are investigated. Upon pumped by 1064 nm laser beam, complexes 1 and 2 exhibit excellent two-photon lasing at ∼627 nm.