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We report results for XUV-IR two-photon ionization of Ar, Ne, NO, and O2, where an XUV attosecond pulse train is superimposed with a synchronized IR pulse, obtained at the ATTOLab laser facility using electron–ion coincidence 3D momentum spectroscopy. Temporally resolved photoelectron angular distributions providing angle-resolved time-delays for np ionization of Ar and Ne, achieved by reconstruction of attosecond beating by interference of two-photon transitions through a unified formalism (Joseph et al. in J Phys B At Mol Opt Phys 53:184007, 2020), are summarized. For inner valence XUV-IR dissociative photoionization of NO and O2 molecules, we report electron–ion kinetic energy correlation diagrams and disentangle the dissociative photoionization processes relying on parallel XUV experiments at Synchrotron SOLEIL. For ionization into the NO+( c 3 Π ) ionic state, extending the formalism developed for single-photon ionization, we focus on photoelectron angular distributions averaged on the delay between the XUV and the IR field in the field frame, molecular frame, and electron frame of reference. [ABSTRACT FROM AUTHOR]

Graphene (G)-plasmonic nanoparticles (NPs) systems have found immense nanoscale applications via utilizing the sensitive optical response of graphene to the photo-induced electrons transferred from attached NPs. These electrons are emitted from the plasmonic metal NPs under the influence of a Localized Surface Plasmon Resonance (LSPR). Here, we first present theoretical investigations of the photoemission electrons in the G-plasmonic NPs system influenced by the LSPR of NPs. A rigorous theoretical approach is used to determine the level of photo-exited electrons and the optimal parameters for achieving a highest photoemission yield. The photoemission of electrons is mainly driven by the surface photoelectric effect in which an electron near the particle surface absorbs photon energy and overcomes the potential barrier at the metal–graphene boundary. For a thorough investigation, we study the effects of the material and geometry of NPs and the intensity of the LSPR field on the rate of photoemission. It is shown that silver nanoparticles combined with graphene are more effective in enhancing light–matter interaction in graphene owing to the lower interfacial energy barrier and higher field enhancement. Finally, we verify that the photo-induced electron density predicted by our calculations is matched with that obtained by combining theoretical and Raman-based experimental results. [ABSTRACT FROM AUTHOR]

The antiferromagnetic Mott insulator α-Sr2CrO4 possesses multiple spin and orbital ordered phases, but their unique interplay is still relatively unexplored. Here, we used femtosecond optical spectroscopy to study ultrafast spin and orbital ordering dynamics in α-Sr2CrO4 through their non-equilibrium response to photoexcitation. By varying the pump photon energy, we selectively drove inter-site spin hopping between neighboring Cr t2g orbitals and charge transfer-type transitions between oxygen 2p and Cr eg orbitals. The resulting transient reflectivity dynamics revealed temperature-dependent anomalies across the Néel temperature for spin ordering as well as the transition temperatures linked to different types of orbital order. Our results reveal distinct relaxation timescales for spin and orbital orders in α-Sr2CrO4 and provide experimental evidence for the phase transition at TO, possibly related to antiferro-type orbital ordering. Strongly correlated electron systems, such as the chromates, can exhibit a range of unique electronic configurations, the phase diagram of which can become even richer when considering non-equilibrium properties. Here, the authors apply ultrafast optical spectroscopy to α-Sr2CrO4 in order to investigate its spin and orbital ordering dynamics and the changes that occur when varying the pump photon energy. [ABSTRACT FROM AUTHOR]

The antiferromagnetic Mott insulator α-Sr2CrO4 possesses multiple spin and orbital ordered phases, but their unique interplay is still relatively unexplored. Here, we used femtosecond optical spectroscopy to study ultrafast spin and orbital ordering dynamics in α-Sr2CrO4 through their non-equilibrium response to photoexcitation. By varying the pump photon energy, we selectively drove inter-site spin hopping between neighboring Cr t2g orbitals and charge transfer-type transitions between oxygen 2p and Cr eg orbitals. The resulting transient reflectivity dynamics revealed temperature-dependent anomalies across the Néel temperature for spin ordering as well as the transition temperatures linked to different types of orbital order. Our results reveal distinct relaxation timescales for spin and orbital orders in α-Sr2CrO4 and provide experimental evidence for the phase transition at TO, possibly related to antiferro-type orbital ordering. Strongly correlated electron systems, such as the chromates, can exhibit a range of unique electronic configurations, the phase diagram of which can become even richer when considering non-equilibrium properties. Here, the authors apply ultrafast optical spectroscopy to α-Sr2CrO4 in order to investigate its spin and orbital ordering dynamics and the changes that occur when varying the pump photon energy. [ABSTRACT FROM AUTHOR]

The heterogeneous nature of extracellular vesicles (EVs) creates the need for single EV characterization techniques. However, many common biochemical and functional EV analysis techniques lack single EV resolution. Two-photon fluorescence lifetime imaging microscopy (FLIM) is widely used to functionally characterize the reduced form of nicotinamide adenine dinucleotide and nicotinamide adenine dinucleotide phosphate (NAD(P)H) in cells and tissues. Here, we demonstrate that FLIM can also be used to image and characterize NAD(P)H in single isolated EVs. EVs were isolated using standard differential ultracentrifugation techniques from multiple cell lines and imaged using a custom two-photon FLIM system. The presented data show that the NAD(P)H fluorescence lifetimes in isolated cell-derived EVs follow a wide Gaussian distribution, indicating the presence of a range of different protein-bound and free NAD(P)H species. EV NAD(P)H fluorescence lifetime distribution has a larger standard deviation than that of cells and a significantly different fluorescence lifetime distribution than the nuclei, mitochondria, and cytosol of cells. Additionally, changes in the metabolic conditions of cells were reflected in changes in the mean fluorescence lifetime of NAD(P)H in the produced EVs. These data suggest that FLIM of NAD(P)H could be a valuable tool for EV research. [ABSTRACT FROM AUTHOR]

Hydrogen sulfide radicals in the ground state, SH(X), and hydrogen disulfide molecules, H2S, are both detected in the interstellar medium, but the returned SH(X)/H2S abundance ratios imply a depletion of the former relative to that predicted by current models (which assume that photon absorption by H2S at energies below the ionization limit results in H + SH photoproducts). Here we report that translational spectroscopy measurements of the H atoms and S(1D) atoms formed by photolysis of jet-cooled H2S molecules at many wavelengths in the range 122 ≤ λ ≤155 nm offer a rationale for this apparent depletion; the quantum yield for forming SH(X) products, Γ, decreases from unity (at the longest excitation wavelengths) to zero at short wavelengths. Convoluting the wavelength dependences of Γ, the H2S parent absorption and the interstellar radiation field implies that only ~26% of photoexcitation events result in SH(X) products. The findings suggest a need to revise the relevant astrochemical models. Sulfur is abundant in the Universe, but the observed abundance ratio of SH to H2S doesn't agree with astrochemical models. The authors measure product state-resolved translational energy spectra of photoproducts in a jet-cooled H2S beam as a function of wavelength, showing that SH yield is lower than assumed in the models. [ABSTRACT FROM AUTHOR]

The application of transparent plastic bags with a gas barrier layer as inexpensive photobioreactors for H2 production by the cyanobacterium Anabaena sp. PCC 7120 ∆Hup mutant cells was explored outdoors in Moscow region for the first time. Two experiments were performed in July and August, the average daily temperature being 21.7 and 20.6 °C, the average daily light intensity being 290 and 340 µmol photon m−2 s−1 in experiment #1 and #2, respectively. The maximal H2 production rate was 20.6 mL day−1 L−1 of culture, with accumulation of 33.2 mL L−1 during 5 days and a final H2 content of 1.1% (v/v). Molecular nitrogen added to the Ar gas at 3.3% significantly affected neither the rate nor the duration of H2 production. Low morning temperatures as well as high daytime light intensities (especially at low cell concentrations) seemed to reduce the H2 production rate. The activities obtained were lower as compared to the previously reported data. It could be attributable to suboptimal weather conditions and simple device arrangement. However, results prove that H2 production by cyanobacteria is still feasible outdoors in plastic bags, the cheapest photobioreactors. [ABSTRACT FROM AUTHOR]

Titanium oxide materials have multiple functions such as photocatalytic and photovoltaic effects. Ferroelectrics provide access to light energy conversion that delivers above-bandgap voltages arising from spatial inversion symmetry breaking, whereas their wide bandgap leads to poor absorption of visible light. Bandgap narrowing offers a potential solution, but this material modification suppresses spontaneous polarization and, hence, sacrifices photovoltages. Here, we report successive-redox mediated ferrophotovoltaics that exhibit a robust visible-light response. Our single-crystal experiments and ab initio calculations, along with photo-luminescence analysis, demonstrate that divalent Fe2+ and trivalent Fe3+ coexisted in a prototypical ferroelectric barium titanate BaTiO3 introduce donor and acceptor levels, respectively, and that two sequential Fe3+/Fe2+ redox reactions enhance the photogenerated power not only under visible light but also at photon energies greater than the bandgap. Our approach opens a promising route to the visible-light activation of photovoltaics and, potentially, of photocatalysts. Photovoltaic response from normal ferroelectric materials generates large voltages but low current due to poor absorption of visible light. Noguchi et al. dope ferrous and ferric ion couple into barium titanate crystals to enhance the photogeneration at photon energies both below and above bandgap. [ABSTRACT FROM AUTHOR]

We consider the escape of a photon from a single-mode optical cavity with a controlled variable intensity. The source of the photon is a relaxing two-level atom. The quantum bottleneck effect involves a counterintuitive decrease of the probability of photon escape from the cavity with the increase of its escape intensity. Numerical simulations of the process were carried out using the basic Lindblad quantum equation for the Jaynes-Cummings model with thermal relaxation. A quasi-classical description of the bottleneck mechanism is presented, similar to the Zeno effect. The counterintuitive behavior described plays an important role in the description of the exchange of single photons in nanosystems and in molecular complexes converting solar energy in bacteria. [ABSTRACT FROM AUTHOR]

Two-photon spectroscopy has been applied to measure the Rydberg transition energies in the n1S0 state of 40Ca atoms at n = 40–120. The ionization potential determined from these experimental data is 49305.91966(4) cm−1. Using the frequency-doubled radiation and fundamental radiation from a diode laser, the frequencies of two-photon transitions to Rydberg states with the principal quantum numbers of 75 and 76 have been measured simultaneously with the frequencies of resonances of saturated absorption in a rubidium vapor cell. The chosen transition frequencies for rubidium atoms are known with high accuracy. Such frequency references make it possible to improve the accuracy of determination of the Rydberg transition energies in 40Ca atoms. [ABSTRACT FROM AUTHOR]

We propose a scheme to realize all-optical temporal differentiation calculation to input pulse in an inverse Y-type four-level atomic system driven by a strong standing-wave. Two optical blockades are created at individual wavelengths of two probe fields in presence of one single strong standing-wave field. On one hand, ultra-narrow transmission windows are produced for probe pulse field 1 when probe field 2 is so strong as a controlling field in EIT configuration. The system can be designed as a phase-reverter of weak probe field 1 and can perform temporal differentiation calculation to it because aπ phase shift is created. On the other hand, the blockade at probe field 2 can be burst in two-photon resonance configuration when probe field 1 becomes strong and saturated absorption takes effect. So a two-photon switching is also expected in this standing-wave-dressed atomic system. The scheme has a potential for an all-optical transistor in quantum logical circuits. [ABSTRACT FROM AUTHOR]

Dispersions of molybdenum blues have been synthesized by reducing a molybdate with hydroquinone in an acidic medium. Spectrophotometry and photon-correlation spectroscopy have been employed to study the formation regularities of molybdenum blues particles (large molybdenum oxide clusters) under the conditions of varied reductant/molybdate ratio and dispersion medium pH. [ABSTRACT FROM AUTHOR]

In this topical review of two-photon stereolithography (TPS), we discuss novel materials and demonstrate applications of this technology. Two-photon-initiated chemical processes are used to fabricate arbitrary three-dimensional structures in TPS. In the first part of this article, the development of novel photoactive materials to fabricate pure inorganic or organic–inorganic hybrid microstructures is discussed. The second part discusses the fabrication of functional microstructures for highly specific applications to demonstrate the importance of TPS in different fields of science. [ABSTRACT FROM AUTHOR]

Abstract: The decay of polarized fluorescence of tryptophan in water-propylene glycol solution two-photon excited by femtosecond laser pulses was explored. Linearly and circularly polarized light in the wavelength band of 385-510 nm was used for excitation. Processing of the experimental fluorescence signals as functions of time and light polarization provided an opportunity to identify two characteristic lifetimes characterizing the fluorescence intensity decay and the rotational diffusion time τrot. The spectral dependences of the anisotropy parameter Ω and anisotropy parameters r for linearly and circularly polarized excitation have been determined. It is shown that the fluorescence temporal dependence is well described by the sum of two exponents with amplitudes a1 and a2 and characteristic times τf1 and τf2 at all wavelengths in the studied spectral range. The experimental dependences of parameters Ω, r, τf1, and a2/a1 are nontrivial, which indicates the complexity of the excitation relaxation processes. The obtained results can be used for interpretation of the experiments and prove of the theoretical models describing the intensity and polarization of fluorescence of tryptophan molecules in solutions and organic compounds under optical excitation. [ABSTRACT FROM AUTHOR]

It is essential for everyone working with experimental science to be certain that their instruments produce reliable results, and for fluorescence lifetime experiments, information about fluorescence lifetime standards is crucial. A large part of the literature on lifetime standards dates back to the 1970s and 1980s, and the use of newer and faster measuring devices may deem these results unreliable. We have tested the three commonly used fluorophores fluorescein, quinine sulfate and green fluorescent protein for their suitability to serve as lifetime standards, especially to be used with two-photon excitation measurements in the time-domain. We measured absorption and emission spectra for the fluorophores to determine optimal wavelengths to use for excitation and detector settings. Fluorescence lifetimes were measured for different concentrations, ranging from 10− 3 − 10− 5 M, as well as for various solvents. Fluorescein was soluble in both ethanol, methanol and sulfuric acid, while quinine sulfate was only soluble in sulfuric acid. Green fluorescent protein was prepared in a commercial Tris-HCl, EDTA solution, and all three fluorophores produced stable lifetime results with low uncertainties. No siginificant variation with concentration was measured for any of the fluorophores, and all showed single-exponential decays. All lifetime measurements were carried out using two-photon excitation and lifetime data was obtained in the time-domain using time-correlated single-photon counting. [ABSTRACT FROM AUTHOR]

Imaging the brain of living laboratory animals at a microscopic scale can be achieved by two-photon microscopy thanks to the high penetrability and low phototoxicity of the excitation wavelengths used. However, knowledge of the two-photon spectral properties of the myriad fluorescent probes is generally scarce and, for many, non-existent. In addition, the use of different measurement units in published reports further hinders the design of a comprehensive imaging experiment. In this review, we compile and homogenize the two-photon spectral properties of 280 fluorescent probes. We provide practical data, including the wavelengths for optimal two-photon excitation, the peak values of two-photon action cross section or molecular brightness, and the emission ranges. Beyond the spectroscopic description of these fluorophores, we discuss their binding to biological targets. This specificity allows in vivo imaging of cells, their processes, and even organelles and other subcellular structures in the brain. In addition to probes that monitor endogenous cell metabolism, studies of healthy and diseased brain benefit from the specific binding of certain probes to pathology-specific features, ranging from amyloid-β plaques to the autofluorescence of certain antibiotics. A special focus is placed on functional in vivo imaging using two-photon probes that sense specific ions or membrane potential, and that may be combined with optogenetic actuators. Being closely linked to their use, we examine the different routes of intravital delivery of these fluorescent probes according to the target. Finally, we discuss different approaches, strategies, and prerequisites for two-photon multicolor experiments in the brains of living laboratory animals. [ABSTRACT FROM AUTHOR]

Some results of experimental and numerical studies on the transmission of a nonchain high-frequency (HF) laser beam through germanium (Ge) single crystals of differing thickness and specific resistance are presented. Based on the experimental data for the HF(DF) lasing spectrum, the coefficient of two-photon absorption in germanium has been estimated as K2 = 55 ± 10 cm/GW at λ = 2.8 μm. The results are in good agreement with theory. The developed experimental data-processing software has enabled the numerical study of the transmission of a high-power beam with λ = 2.6-3 μm through Ge at any laser-pulse-impact moment. It has been shown that thin germanium coatings can efficiently smoothen the distribution of energy over the beam aperture for high-power laser radiation with λ = 2.6-4 μm. [ABSTRACT FROM AUTHOR]

Rhodamine group of molecules are widely used dyes for imaging of biological molecules. Application of these dyes however includes a limitation that these molecules absorb in the visible range of the spectrum, which does not fall in the ‘biologically transparent window’ (BTW). Two photon absorption (TPA) process could come up with an alternate solution to this as these dyes could be excited in the near infrared (NIR) window to extract similar information. To validate this we have investigated TPA cross section (TPACS, σ2) of two rhodamine dyes, namely Rhodamine 6G (R6G), Rhodamine B (RhB), site selectively bound with a model protein, bovine serum albumin (BSA), by exciting at 800 nm. Two photon spectroscopy and imaging confirms the binding of the dye to the protein. The decreases in TPACS with increasing temperature at a fixed BSA concentration excellently follows the temperature induced structural transition of BSA as the protein transforms from a molten globule to unfolded conformation beyond 60 °C, which has previously been established through circular dichroism (CD) measurements. The thus established resemblance in TPACS and CD measurement trends thus strongly affirms the suitability of TPA process in protein imaging and as an alternative marker to tracking its conformational transformations using NIR radiation. [ABSTRACT FROM AUTHOR]

Three-dimensional (3D) microstructures are fabricated with accumulated voxels layer-by-layer in two-photon polymerization (TPP). The overlap ratio and layer spacing between two neighboring layers both affects the surface accuracy and the processing efficiency. Presented in this paper is an adaptive direct slicing method that applies tilted voxels of TPP to satisfy contour change of 3D microstructure model with given overlap ratio. It extracted the contour line from a projected image of the original 3D microstructure model. The relative position of every two adjacent points on the contour line was used to reflect the interlayer spacing and calculate the tilted angle and overlap ratio of two neighboring voxels. The optimal interlayer spacing could be determined when the overlap ratio of tilted voxels of two neighboring layers exceeded a specified overlap ratio. Both axis-symmetry revolve and complex non-symmetrical microstructures were successfully sliced with higher efficiency and accuracy. The layer number reduces more than 30% compared with the adaptive direct slicing method based on vertical voxels by appropriate selection of overlap ratio and size of voxel. Quantitative analysis shows that the staircase errors decreased significantly with this adaptive direct slicing method. Unlike traditional slicing method, smaller overlap ratio and larger voxel benefits reducing layer number but has little effect on precision. [ABSTRACT FROM AUTHOR]

We experimentally observed a two-photon interference between a squeezed vacuum state from an optical parametric amplifier and a weak coherent state on a beam splitter with continuous variables. The photon statistics properties of the mixed field were investigated by calculating the correlations among four permutations of measured quadratures components, which were obtained by two homodyne detection systems. This also means that the two-photon interference occurred at analysis frequency differing from the previous two-photon interference reports. The nonclassical effect of photon anti-bunching occurred when an amplitude squeezed vacuum state acted as one of interference sources. On the other hand, the photon bunching effect appeared when a phase squeezed vacuum state was employed. Graphical abstract: [ABSTRACT FROM AUTHOR]

The dependences of the energy that is absorbed in a crystal exposed to the action of a femtosecond light pulse on the radiation intensity at a fixed pulse duration and on the pulse duration at a fixed pulse energy have been determined under the conditions of a two-photon-one-photon double resonance on interband transitions in the crystal. [ABSTRACT FROM AUTHOR]

A theory of the transient absorption of femtosecond light pulses at a two-photon-one-photon double resonance on adjacent interband transitions in the electronic system has been developed. Approximate expressions for the reactive component of the nonlinear polarization of the three-level system, P , which determines the absorbed power in the medium, have been obtained, and the dependences of P on the light intensity and detunings of resonances have been calculated. [ABSTRACT FROM AUTHOR]

Polarized fluorescence decay in NADH molecules in aqueous solution under two-photon excitation by femtosecond laser pulses has been studied. The excitation was carried out by linear and circularly polarized radiation at four wavelengths: 720, 730, 740, and 750 nm. Time-dependent polarized fluorescence signals were recorded as a function of the excitation light polarization and used for determination of a set of molecular parameters, two lifetimes characterizing the molecular excited states, and the rotation correlation time τ. The results obtained can be used to create and prove theoretical models describing the intensity and polarization of fluorescence in NADH involved in the regulation of the redox reactions in cells and tissues of living organisms. [ABSTRACT FROM AUTHOR]

We describe a two-photon microscopy-based method to evaluate the in vivo systemic transport of compounds. This method comprises imaging of the intact liver, kidney and intestine, the main organs responsible for uptake and elimination of xenobiotics and endogenous molecules. The image quality of the acquired movies was sufficient to distinguish subcellular structures like organelles and vesicles. Quantification of the movement of fluorescent dextran and fluorescent cholic acid derivatives in different organs and their sub-compartments over time revealed significant dynamic differences. Calculated half-lives were similar in the capillaries of all investigated organs but differed in the specific sub-compartments, such as parenchymal cells and bile canaliculi of the liver, glomeruli, proximal and distal tubules of the kidney and lymph vessels (lacteals) of the small intestine. Moreover, tools to image immune cells, which can influence transport processes in inflamed tissues, are described. This powerful approach provides new possibilities for the analysis of compound transport in multiple organs and can support physiologically based pharmacokinetic modeling, in order to obtain more precise predictions at the whole body scale. [ABSTRACT FROM AUTHOR]

A differential two-photon method of measuring the temperature of 40Ca atoms in a continuously operating magneto-optical trap is demonstrated. Coherent two-photon resonances at the 4s21S0–501S0 Rydberg transition have been investigated experimentally using resonance laser beams propagating at different angles. The temperature of the cloud of 40Ca atoms was measured depending on the frequency detuning of the cooling laser radiation. [ABSTRACT FROM AUTHOR]

We study power broadening of coherent two-photon resonances on Rydberg transitions in lithium-7 atoms in a magneto-optical trap (MOT). We apply the spectroscopic technique based on the reduction of resonance fluorescence in the MOT. One of the main contributions to the spectral broadening is associated with heating of the trapped atoms by laser cooling beams. We suggest a new nondestructive method to measure the atomic temperature in a working MOT using two-photon spectroscopy with variable directions of probe beams. [ABSTRACT FROM AUTHOR]

This paper gives a review of the experiments performed since the 1980s at the Laboratoire Kastler Brossel in Paris on two-photon spectroscopy of atomic hydrogen. Firstly devoted to the 2S- nS and 2S- nD transitions, they are currently running on the 1S-3S transition at 205 nm. During all that time, they were inspired by the plentiful ideas proposed by Ted Hänsch and were complementary with the measurements developed in parallel in his groups. [ABSTRACT FROM AUTHOR]

We investigate the role of tip-sample interaction in nonlinear optical scanning near-field microscopy. The experiment was performed by tightly focusing femtosecond laser pulses onto a sharp gold tip that was positioned in close proximity to the surface of a sample with gold nanostructures on a Si-substrate by shear force feedback. The nonlinear optical signal consists of two-photon photoluminescence and second harmonic signal from the gold tip and the gold nanostructures. These signals can be used to characterize different coupling parameters such as geometry, material and width of the tip-sample gap and enable to reveal the mechanism responsible for the image contrast. Under the excitation with 776-nm and 110-fs laser pulses nonlinear imaging is almost background free and yields super resolution showing features with dimensions significantly below the diffraction limit with a signal intensity following quadratic excitation power law. [ABSTRACT FROM AUTHOR]

A study of the optical spectra of ultracold highly excited Li7 atoms has revealed coherent and non-coherent components of two-photon excitation. The high sensitivity of the method makes it possible to record pure coherent resonances at a detuning of 803.5 MHz from the intermediate 2 P resonance. [ABSTRACT FROM AUTHOR]

In this letter, aggregation from two-photon absorption (2PA) molecules in living cells were firstly observed and the related aggregation induced emission (AIE) properties were investigated as a cell tracer for L ((Z)-3-(4-(Bis(4-ethoxyphenyl) amino)phenyl)-2-(4-amino-phenyl)- acrylonitrile cyano-substituted ) based on triphenylamine with D-π-A model. L was further used as a two-photon absorption (2PA, λ = 900, λ = 550 nm δ = 156 GM) live-cell marker for real-time, long-term cell growth and proliferation monitoring, with rapidly adhering whole intracellular membrane-rich system. Remarkably, different from existing organic AIE chromophores and other commercially available probes, L exhibited intense intracellular-AIE property with stable nuclear envelope (NE) staining under two-photon excited microscopy (TPEM) through detailed in cellulo studies. [ABSTRACT FROM AUTHOR]

Two-photon-induced lithography is a versatile method to generate arbitrary three-dimensional microstructures. Although the lithographic result sensitively depends on the experimental conditions, there is a lack of in situ methods to measure process conditions prior to structuring. Current methods rely on determining the size of cross-linked structures, such as single-volume pixels (voxels), as a result of a set of parameters. This procedure is time consuming and possesses several inherent drawbacks, since results are not easily interpretable. Therefore, we established an in situ method, called the voxel onset time (VOT) method, which is easy to integrate in an existing two-photon lithographic setup and is based on determining the time that a voxel necessitates to form by measuring the transmitted laser intensity. In this study, we demonstrate how the VOT method can be used to determine the influence of the axial focal position on voxel formation for different experimental conditions. We find that the voxel onset time is strongly linked to the maximum intensity that is influenced by specimen-induced spherical aberration, especially for a high-numerical-aperture objective. [ABSTRACT FROM AUTHOR]

In vivo imaging at high spatiotemporal resolution is key to the understanding of complex biological systems. We integrated an optical phase-locked ultrasound lens into a two-photon fluorescence microscope and achieved microsecond-scale axial scanning, thus enabling volumetric imaging at tens of hertz. We applied this system to multicolor volumetric imaging of processes sensitive to motion artifacts, including calcium dynamics in behaving mouse brain and transient morphology changes and trafficking of immune cells. [ABSTRACT FROM AUTHOR]

Background: We previously visualized in vivo responses to chemotherapy in a colorectal liver metastatic xenograft model using in vivo real-time and time-series intravital two-photon laser scanning microscopy (TPLSM). In this study, we established the method for evaluating the response of peritoneal xenografts to chemotherapy of metastatic gastric cancer using intravital TPLSM. Methods: Red fluorescent protein-expressing gastric cancer cells (NUGC4) were inoculated into the peritoneal cavity of green fluorescent protein nude mice. Results: Laparotomy revealed that 2 weeks after inoculation, macroscopic peritoneal metastatic nodules were formed. The first intravital TPLSM session revealed that they were composed of red tumor cell clusters and green surrounding stroma. Paclitaxel was administered intraperitoneally after the first TPLSM three times a week for 7 days in the treatment group. At the second laparotomy, there were significantly fewer and smaller nodules in the treated mice than in the controls. The second intravital TPLSM session showed tumor cell fragmentation, swelling, and nuclear condensation in the metastatic nodules-a response to chemotherapy. There were multinuclear tumor cells in the paclitaxel-treated living mice. Conclusions: Our method may become a powerful tool for evaluating the efficacy of novel anti-gastric cancer drugs in a preclinical murine model with minimum interindividual variation. [ABSTRACT FROM AUTHOR]

Sulforhodamine 101 (SR101) is widely used for astrocyte identification, though the labeling mechanism remains unknown and the efficacy of labeling in different brain regions is heterogeneous. By combining region-specific isolation of astrocytes followed by transcriptome analysis, two-photon excitation microscopy, and mouse genetics, we identified the thyroid hormone transporter OATP1C1 as the SR101-uptake transporter in hippocampus and cortex. [ABSTRACT FROM AUTHOR]

The precision of laser spectroscopy of antiprotonic helium (a helium atom with one of its electrons replaced by an antiproton) has improved by almost 4 orders of magnitude over its 20 years of history. Experimental transition frequencies can be compared to 3-body QED calculations to derive the antiproton-electron mass ratio. In the latest measurements of the Asacusa experiment at CERN, two-photon transitions of antiprotonic helium were excited using two counter-propagating laser beams. This method reduces the Doppler-broadening caused by the thermal motion of the atoms, and allowed us to measure the transition frequencies with a fractional precision of 2.5-5 parts in 10. From these frequencies, we derived an antiproton-electron mass ratio of 1836.1526736(23). Our precision approaches that of the experimental value of the proton-electron mass ratio, and agrees with the latter within errors. Assuming CPT symmetry (i.e. $m_{p}=m_{\overline {p}}$), we further derived the electron's atomic mass as m = 0.0005485799091(7) u from the more accurately known atomic mass of the proton. [ABSTRACT FROM AUTHOR]

We report the fabrication of distributed feedback lasers in Rhodamin 6G doped SU-8 by direct femtosecond laser writing. The devices are fabricated by point-by-point exposure and consist of a core layer with a low-order Bragg grating on the surface. A quarter-wavelength phase shift is introduced in the middle of the grating section to obtain single-mode emission. Lasing at different wavelengths is demonstrated by changing the grating pitch. Spectral emission, threshold and lifetime characterization is performed by pumping the laser with a pulsed, frequency double Nd:YAG laser. [ABSTRACT FROM AUTHOR]

We present simulations for a design of a high-energy single-stage mid-IR difference frequency generation adapted to a two-color Ti:sapphire amplifier system. The optimized mixing process is based on chirped pulse difference frequency generation (CP-DFG), allowing for a higher conversion efficiency and reduced two-photon absorption losses. The numerical start-to-end simulations include stretching, chirped pulse difference frequency generation and pulse compression. Realistic design parameters for commercially available nonlinear crystals (GaSe, AgGaS, LiInSe, LiGaSe) are considered. Compared with conventional unchirped DFG directly pumped by Ti:sapphire technology, we predict a threefold increase in the quantum efficiency. Our CP-DFG scheme provides up to 340 μJ pulse energy directly at 7.2 μm when pumped with 8 mJ and supports a bandwidth of up to 350 nm. The resulting 240 fs mid-IR pulses are inherently phase stable. [ABSTRACT FROM AUTHOR]

We show in proof-of-principle experiments an axial resolution improvement in two-photon-excited fluorescence and polymerization enabled by the short coherence length of two counter-propagating ultrashort laser pulses. The interference of these pulses generate a spatial interference fringe pattern, whose width scales inversely to the spectral bandwidth and is therefore considerably shorter than the effective focal length of a laser beam conventionally focused from only one side. [ABSTRACT FROM AUTHOR]

Two-photon excitation of a sensitizer with a focused laser beam was used to create a spatially-localized subcellular population of reactive oxygen species, ROS, in single HeLa cells. The sensitizer used was protoporphyrin IX, PpIX, endogenously derived from 5-aminolevulinic acid delivered to the cells. Although we infer that singlet oxygen, O2(a1Δg), is one ROS produced upon irradiation of PpIX under these conditions, it is possible that the superoxide ion, O2−Ṗ, may also play a role in this system. With a “high” dose of PpIX-sensitized ROS, the expected death of the cell was observed. However, under “low dose” conditions, clear signs of cell proliferation were observed. The present results facilitate studies of ROS-mediated signalling in imaging-based single cell experiments. [ABSTRACT FROM AUTHOR]

In this paper, we have briefly reviewed the work on two-photon spectroscopy of alkali elements and its applications. The technique of Doppler-free two-photon spectroscopy is briefly summarized. A review of various techniques adopted for measuring absolute frequencies of the atomic transitions and precision measurements of isotope shifts and hyperfine structures (HFS) is presented. Some of the recent works on precision measurements of HFS constants of 6 s S level of K and K, 9 s Slevel and 7 d D level of Cs are also discussed. [ABSTRACT FROM AUTHOR]

Phosphors with the composition YErYbOS have been prepared by solid-state reaction. We have analyzed the diffuse reflectance, luminescence excitation, and photoluminescence spectra of this material under Stokes and anti-Stokes optical excitation by two light sources. Visible luminescence was observed when two resonance infrared photons of different energies were absorbed successively. This effect can be understood in terms of the metastable states of the I excited-state level of the erbium ion, from which transitions to higher energy levels occur when infrared photons are absorbed. [ABSTRACT FROM AUTHOR]

Entanglement of two artificial two-level atoms with degenerate two-photon transitions is considered in the case in which the atoms interact with the thermal single-mode field in an ideal cavity. The possibility of controlling the atomic entanglement degree in such a system due to the induction of atomic coherence and direct dipole-dipole interaction of atoms is shown. [ABSTRACT FROM AUTHOR]

The temporal profile of the second and third harmonic emissions of a Ti:sapphire laser was measured using an autocorrelator consisting of a mass spectrometer as a two-photon-response detector. A number of organic compounds that are potentially applicable for two-photon excitation and subsequent one-photon ionization were investigated using density functional theory calculations. N, N′-dimethylaniline and acetonitrile were used for the measurement of the pulse width for the second and third harmonic emissions of the Ti:sapphire laser. This approach has the potential for use in measuring pulse widths as short as 1–3 fs in the ultraviolet region. [ABSTRACT FROM AUTHOR]

Two-photon excited fluorescence (TPEF) is a standard technique in modern microscopy, but is still affected by photodamage to the probe. It has been proposed that TPEF can be enhanced using entangled photons, but this has proven challenging. Recently, it was shown that some features of entangled photons can be mimicked with thermal light, which finds application in ghost imaging, subwavelength lithography and metrology. Here, we use true thermal light from a superluminescent diode to demonstrate TPEF that is enhanced compared to coherent light, using two common fluorophores and luminescent quantum dots, which suit applications in imaging and microscopy. We find that the TPEF rate is directly proportional to the measured degree of second-order coherence, as predicted by theory. Our results show that photon bunching in thermal light can be exploited in two-photon microscopy, with the photon statistic providing a new degree of freedom. [ABSTRACT FROM AUTHOR]

Development of sensitive and selective probes for cupric ions (Cu2+) at cell and tissue level is a challenging work for progress in understanding the biological effects of Cu2+. Here, we report a ratiometric two-photon probe for Cu2+ based on the organic-inorganic hybrids of graphene quantum dots (GQDs) and Nile Blue dye. Meanwhile, Cu-free derivative of copper-zinc superoxide dismutase (SOD) - E2Zn2SOD is designed as the unique receptor for Cu2+ and conjugated on the surface of GQDs. This probe shows a blue-to-yellow color change in repose to Cu2+, good selectivity, low cytotoxicity, long-term photostability, and insensitivity to pH over the biologically relevant pH range. The developed probe allows the direct visualization of Cu2+ levels in live cells as well as in deep-tissues at 90-180 mm depth through the use of two-photon microscopy. Furthermore, the effect of ascorbic acid is also evaluated on intracellular Cu2+ binding to E2Zn2SOD by this probe [ABSTRACT FROM AUTHOR]

The generalized two-photon Rabi model is proposed due to the recent interests on the ultrastrong-coupling regime of the circuit QED. The dipole interaction between the qubits in the two-qubit Rabi model with one qubit degenerate in energy is also taken into account, which can be applied to generate entanglement. Their exact solutions are obtained in the Bargmann space. Some isolated exact solutions for the generalized two-photon Rabi model are also obtained by a Bogoliubov transformation, and are compared with the full exact solutions. It is shown that both kinds of solutions coincide with each other. [ABSTRACT FROM AUTHOR]

Under two-photon 523.5 nm interband picosecond laser excitation, we measured the kinetics of induced absorption in PbWO 4, ZnWO 4, and PbMoO 4 crystals with 532 to 633 nm continuous probe radiation. We obtained real-time information about the dynamics of the generation, relaxation, and accumulations of electronic excitations over a wide time range (from picoseconds to hundreds of seconds) and the 77–300 K temperature range. For the studied crystals, exponential temperature-independent growth of the induced absorption (IA) with 60 ns rise time reflects the dynamics of the generation of electronic excitation. The kinetics of the IA exponential growth with temperature-dependent 3.5–11 μs time constants reflect the dynamics of energy migration between neighboring tungstate (molibdate) ions to traps for the studied crystals. The multiexponential relaxation absorption kinetics strongly depend on temperature, and the relaxation decay time of induced absorption increased from tens to hundreds of milliseconds to seconds under crystal cooling from 300 to 77 K. We found that the increase in the laser pump repetition rate (0–10 Hz) leads to the accumulation of electronic excitations. Control of the repetition rate and the number of excitations allowed us to change the relaxation time of the induced absorption by more than two orders of magnitude. Due to accumulation of excitations at 77 K, the absorption relaxation time can exceed 100 s for PbWO 4 and PbMoO 4 crystals. In the initially transparent crystals, two-photon interband absorption (2PA) leads to crystals opacity at the 523 and 633 nm wavelengths. (An inverse optical transmission of the crystals exceeds 50–55 at a 50–100 GW/cm 2 pump intensity.) Measured at ∼1 mW probe radiation of 532 and 633 nm wavelengths, the induced absorption values are comparable with those obtained under two-photon absorption at ∼5 kW pump power. An optical 2PA shutter for the visible spectral range is proposed with a variable shutting time from hundreds of microseconds to tens of seconds. [ABSTRACT FROM AUTHOR]

Myc levels are highly regulated and usually low in vivo. Dimerized with Max, it regulates most expressed genes and so directly and indirectly controls most cellular processes. Intranuclear diffusion of a functional c-Myc-eGFP, expressed from its native locus in murine fibroblasts and 3T3 cells or by transient transfection, was monitored using Two Photon Fluorescence Correlation Spectroscopy, revealing concentration and size (mobility) of complexes. With increased c-Myc-eGFP, a very immobile pool saturates as a 'mobile' pool increases. Both pools diffuse too slowly to be free Myc-Max dimers. Following serum stimulation, eGFP-c-Myc accumulated in the presence of the proteasome inhbitor MG132. Stimulating without MG132, Myc peaked at 2.5 hrs, and at steady was ~8 ± 1.3 nM. Inhbiting Myc-Max dimerization by Max-knockdown or drug treatment increased the 'mobile' c-Myc pool size. These results indicate that Myc populates macromolecular complexes of widely heterogenous size and mobility in vivo. [ABSTRACT FROM AUTHOR]

Functional magnetic resonance imaging (fMRI) based on blood oxygen level-dependent (BOLD) contrast is widely used for probing brain activity, but its relationship to underlying neural activity remains elusive. Here, we combined fMRI with fiber-optic recordings of fluorescent calcium indicator signals to investigate this relationship in rat somatosensory cortex. Electrical forepaw stimulation (1-10 Hz) evoked fast calcium signals of neuronal origin that showed frequency-dependent adaptation. Additionally, slower calcium signals occurred in astrocyte networks, as verified by astrocyte-specific staining and two-photon microscopy. Without apparent glia activation, we could predict BOLD responses well from simultaneously recorded fiber-optic signals, assuming an impulse response function and taking into account neuronal adaptation. In cases with glia activation, we uncovered additional prolonged BOLD signal components. Our findings highlight the complexity of fMRI BOLD signals, involving both neuronal and glial activity. Combined fMRI and fiber-optic recordings should help to clarify cellular mechanisms underlying BOLD signals. [ABSTRACT FROM AUTHOR]

We have investigated the eigenenergy spectrum of the two-photon Rabi model at the critical coupling, particularly the special feature "spectral collapse", by means of an elementary quantum mechanics approach. The eigenenergy spectrum is found to consist of both a set of discrete energy levels and a continuous energy spectrum. Each of these eigenenergies has a two-fold degeneracy corresponding to the spin degree of freedom. The discrete eigenenergy spectrum has a one-to-one mapping with that of a particle in a "Lorentzian function" potential well, and the continuous energy spectrum can be derived from the scattering problem associated with a potential barrier. The number of bound states available at the critical coupling is determined by the energy difference between the two atomic levels so that the extent of the "spectral collapse" can be monitored in a straightforward manner. [ABSTRACT FROM AUTHOR]