White-light Continuum Generation Research Articles

Full-Spectrum CARS Microscopy of Cells and Tissues with Ultrashort White-Light Continuum Pulses.

Coherent anti-Stokes Raman scattering (CARS) microscopy is an emerging nonlinear vibrational imaging technique that delivers label-free chemical maps of cells and tissues. In narrowband CARS, two spatiotemporally superimposed picosecond pulses, pump and Stokes, illuminate the sample to interrogate a single vibrational mode. Broadband CARS (BCARS) combines narrowband pump pulses with broadband Stokes pulses to record broad vibrational spectra. Despite recent technological advancements, BCARS microscopes still struggle to image biological samples over the entire Raman-active region (400-3100 cm-1). Here, we demonstrate a robust BCARS platform that answers this need. Our system is based on a femtosecond ytterbium laser at a 1035 nm wavelength and a 2 MHz repetition rate, which delivers high-energy pulses used to produce broadband Stokes pulses by white-light continuum generation in a bulk YAG crystal. Combining such pulses, pre-compressed to sub-20 fs duration, with narrowband pump pulses, we generate a CARS signal with a high (<9 cm-1) spectral resolution in the whole Raman-active window, exploiting both the two-color and three-color excitation mechanisms. Aided by an innovative post-processing pipeline, our microscope allows us to perform high-speed (≈1 ms pixel dwell time) imaging over a large field of view, identifying the main chemical compounds in cancer cells and discriminating tumorous from healthy regions in liver slices of mouse models, paving the way for applications in histopathological settings.

Efficient generation of UV-enhanced intense supercontinuum in solids: Toward sub-cycle transient

Ultrabroadband generation of white-light continuum spanning from ultraviolet to near-infrared (375–920 nm) is demonstrated by using induced-phase modulation between two-color femtosecond pulses in multiple thin plates. The fundamental wave and its second-harmonic wave from one Ti:sapphire chirped-pulse amplifier are injected into nine 100 μm-thick fused silica plates. When the two pulses are temporally and spatially optimized in the plates, an intense supercontinuum is efficiently achieved by utilizing self-phase modulation and self-steepening together with induced-phase modulation. As a result, using 1 kHz, 1 mJ, and 35 fs pulses at 800 nm as the pump, we demonstrate the generation of 0.6 mJ white-light pulses with an ultra-broad bandwidth supporting 1.6 fs transform-limited pulses corresponding to 0.6-optical-cycle at a central wavelength of 750 nm. Analysis of the calculated spectrum fits the experimental results well, and the pulse is quasi-linearly chirped and compressible. The resulting intense robust supercontinuum could be a promising light source for an ever greater degree of tailored optical waveform coherent control in new parameter spaces.

Deep reinforcement learning control of white-light continuum generation

White-light continuum (WLC) generation in bulk media finds numerous applications in ultrafast optics and spectroscopy. Due to the complexity of the underlying spatiotemporal dynamics, WLC optimization typically follows empirical procedures. Deep reinforcement learning (RL) is a branch of machine learning dealing with the control of automated systems using deep neural networks. In this Letter, we demonstrate the capability of a deep RL agent to generate a long-term-stable WLC from a bulk medium without any previous knowledge of the system dynamics or functioning. This work demonstrates that RL can be exploited effectively to control complex nonlinear optical experiments.

Nonlinear Optical Investigation of Microbial Chromoproteins.

Membrane-bound or cytosolic light-sensitive proteins, playing a crucial role in energy- and signal-transduction processes of various photosynthetic microorganisms, have been optimized for sensing or harvesting light by myriads of years of evolution. Upon absorption of a photon, they undergo a usually cyclic reaction series of conformations, and the accompanying spectro-kinetic events assign robust nonlinear optical (NLO) properties for these chromoproteins. During recent years, they have attracted a considerable interest among researchers of the applied optics community as well, where finding the appropriate NLO material for a particular application is a pivotal task. Potential applications have emerged in various branches of photonics, including optical information storage and processing, higher-harmonic and white-light continuum generation, or biosensorics. In our earlier work, we also raised the possibility of using chromoproteins, such as bacteriorhodopsin (bR), as building blocks for the active elements of integrated optical (IO) circuits, where several organic and inorganic photonic materials have been considered as active components, but so far none of them has been deemed ideal for the purpose. In the current study, we investigate the linear and NLO properties of biofilms made of photoactive yellow protein (PYP) and bR. The kinetics of the photoreactions are monitored by time-resolved absorption experiments, while the refractive index of the films and its light-induced changes are measured using the Optical Waveguide Lightmode Spectroscopy (OWLS) and Z-scan techniques, respectively. The nonlinear refractive index and the refractive index change of both protein films were determined in the green spectral range in a wide range of intensities and at various laser repetition rates. The nonlinear refractive index and refractive index change of PYP were compared to those of bR, with respect to photonics applications. Our results imply that the NLO properties of these proteins make them promising candidates for utilization in applied photonics, and they should be considered as valid alternatives for active components of IO circuits.

Near-infrared laser driven white light continuum generation: materials, photophysical behaviours and applications.

The pursuit of efficient light sources has stimulated continued effort in the search of materials and methods for generating white light emission. In addition to the white light produced by light-emitting diodes (LEDs) and fluorescent lamps that involves spectral conversion of high energy to low energy emission, recent studies showed that it was also possible to produce white visible light by irradiating different active materials with near-infrared (NIR) constant-wave (CW) lasers. In this review, we begin by introducing and categorizing different materials that exhibit NIR laser driven white light emission, including normal inorganic phosphors, organometallic compounds, graphene, etc. We then discuss the photophysical behavior of this process in terms of optical spectra, temperature evolution and photoelectric response. Different mechanisms of while light generation are analyzed afterwards, and the possibility of a more general physical picture of this process is discussed. This review is concluded with a summary of the current understanding and discussion on potential applications and future perspectives.

White light continuum in negative hollow-core fiber filled with inert gases

As of the writing of this work, generation of white light continuum (WLC) in hollow-core photonic crystal fibers (HCPCF) filled with gases is being thoroughly researched. These structures allow the possibility of adjusting light generation properties by changing the fill gas pressure. Kagomé hollow-core PCF and silica capillaries have been used to study the nonlinear effects in gases as they facilitate exploring these weak properties. In this paper, we numerically analyze the generation of WLC in a new type of hollow-core PCF, called negative curvature hollow-core fiber (NCHCF), itself filled with different inert gases. We show that this type of fiber is a better alternative to the Kagomé and capillary fibers because it exhibits low losses and the WLC spectrum generated presents a relatively flat wavelength span from around 400[Formula: see text]nm to 2400[Formula: see text]nm under certain circumstances.

High average power 88 W OPCPA system for high-repetition-rate experiments at the LCLS x-ray free-electron laser.

We present a 100kHz, sub-20fs optical parametric chirped-pulse amplifier (OPCPA) system delivering 88.6W average power at a center wavelength of 800nm. The seed pulses are derived from the pump laser via white-light continuum generation and are amplified in three non-collinear OPCPA stages. The final two high-power stages are pumped with a 661W Yb:YAG InnoSlab amplifier. A simple and robust design is used for the OPCPA system to avoid thermal effects and enhance long-term stability, resulting in excellent beam quality and high conversion efficiency. To the best of our knowledge, this is the highest average power OPCPA system reported to date.

Cross-correlation frequency-resolved optical gating of white-light continuum (500–900 nm) generated in bulk media by 1053 nm laser pulses

We have efficiently characterized the white-light continuum (WLC) generation covering 500–900 nm in a bulk sapphire plate using 280 fs pulse duration, 1053 nm center-wavelength seed laser pulses. We have acquired the well-optimized smoother region of the WLC spectrum successfully by using an FGS-900 color glass filter (Edmund Optics, Inc.). We have suppressed the spectral components below 500 nm and over 900 nm including an intense 1053 nm residual seed laser peak of the WLC spectrum. The experimental artifacts have been avoided by suppressing the intense 1053 nm seed laser. We employed the sum frequency generation cross-correlation frequency-resolved optical gating (SFG-XFROG) technique for characterization. The XFROG measurement was carried out by introducing the crystal dithering method up to 10° in 2° intervals to obtain the phase matching effectively over the filtered and smoother region of the WLC spectrum. This well-optimized WLC region covering 500–900 nm has significant importance for use as a seed pulse in an optical parametric chirped pulse amplification (OPCPA) system.

Nonlinear bubble nucleation and growth following filament and white-light continuum generation induced by a single-shot femtosecond laser pulse into dielectrics based on consideration of the time scale

Bubble nucleation and growth following plasma channeling (filament) and white-light continuum in liquid irradiated by a single-shot fs-pulse were experimentally investigated with close observation of the time scale. Making full use of a new confocal system and time-resolved visualization techniques, we obtained evidence suggestive of a major/minor role of the non-linear/thermal effects during the fs-pulse-induced bubble's fountainhead (10−13 s) and growth (10−7 s), which was never observed with the use of the ns-pulse (i.e., optic cavitation). In this context, the fs-pulse-induced bubble is not an ordinary optic cavitation but rather is nonlinear-optic cavitation. We present the intrinsic differences in the dominant-time domain of the fs-pulse and ns-pulse excitation, and intriguingly, a mere hundred femtoseconds' excitation predetermines the size of the bubble appearing several microseconds after irradiation. That is, the nucleation happens temporally beyond a six-order-of-magnitude difference.

Long-term stabilization of high power optical parametric chirped-pulse amplifiers

The long-term stability of optical parametric chirped-pulse amplifiers is hindered by thermal path length drifts affecting the temporal pump-to-signal overlap. A kilowatt-pumped burst amplifier is presented delivering broadband 1.4 mJ pulses with a spectral bandwidth supporting sub-7 fs pulse duration. Active temporal overlap control can be achieved by feedback of optical timing signals from cross-correlation or spectral measurements. Using a balanced optical cross-correlator, we achieve a pump-to-signal synchronization with a residual jitter of only (46 ± 2) fs rms. Additionally, we propose passive pump-to-signal stabilization with an intrinsic jitter of (7.0 ± 0.5) fs rms using white-light continuum generation.

Rogue-wave-like statistics in ultrafast white-light continuum generation in sapphire

We experimentally study the statistics of the white-light continuum generated by focusing of 130 fs, 800 nm pulses in a sapphire plate and show that the statistical distributions of the spectral intensity of the blue-shifted continuum components obey the extreme-value statistics. This rogue-wave-like behavior is detected only within a narrow input-pulse energy interval. By the use of numerical simulations, we show that the observed rogue-wave-like behavior is associated with pulse splitting and build-up of intense trailing pulse. The extreme events are thereafter suppressed by the intensity clamping.

Interference pattern generation and simulation in the single beam of a white light continuum

We demonstrate the interference phenomenon in the White Light Continuum (WLC) generated by a single femtosecond laser beam. Different kinds of spatial interference patterns of the WLC generation under various conditions were investigated. The spatial patterns were attributed to interference between the filaments in the WLC generated by the fundamental laser beam yielding the diffraction effect from spatial confinement. Simulations of different patterns were performed. By comparing the results of simulation with those of experiments, the distances of several micrometers between the neighboring filaments can be derived, which agree with the literature values from direct measurements.

Nonlinear optical effects during femtosecond photodisruption

Several nonlinear effects (i.e., continuum generation, self-focusing, and material damage) were studied during femtosecond photodisruption. Numerical aperture dependence of white-light continuum generation and material damage were determined and a relation between the two effects was shown. We showed the possibility of reducing nonlinear side effects and at the same time ensuring precise cut by using lenses of a suitable numerical aperture for refractive surgery, cell surgery, and tissue dissection. Other side effects associated with optical breakdown in model substance were also discussed.

Development of a Tunable Ultrashort Dye Laser System by Using Molecular Photonic Processes and a Nanosecond Pumping Laser

The paper presents the physical processes and operational characteristics of an original subpicosecond dye laser system which is designed and successfully developed at our laboratory basing on the combination use of three photonic processes of dye molecules: 1) Fast spectrotemporal evolutions in the broadband dye laser emissions; 2) Generation of a chain of ultrashort pulses (spikes) from low-Q micro-cavity dye lasers; and 3) Non-linear resonant interaction between ultrashort laser pulses and highly-saturated dye media. Such a laser system provides a stable generation of single 500 fs pulses with a peak power of 300 MW at 606 nm. Particularly, the whole sub-picosecond laser system is pumped by a single nanosecond laser (Q-switched Nd:YAG laser). The spectral and time processes involved in these pulse-shortening methods are analyzed with a rate-equation model extended to wavelengths. A white light continuum generation was obtained by focusing the 500 fs pulses into 2 cm water cell. As a result, it enables us to produce widely tunable ultrashort laser pulses with a spectral selection and amplification of the supercontinuum spectrum.

Sum and difference frequency generation of white light continuum with the ps pulses of Nd+3:YAG laser in a thick BBO crystal

The white light continuum (WLC) generated in water/D2O mixture by pumping with the fundamental of ps Nd+3:YAG laser has been used as a variable frequency source for the sum frequency generation as well as for its amplification. 35ps long pulses with 8mJ energy at 1064nm were mixed collinearly with the WLC generated by the same laser beam in a 20mm thick BBO crystal. The obtained tunable output has been identified as the sum frequency between the fundamental and a portion of the WLC with the required phase matching. Theoretical simulations are also given along with a few initial experiments to use this combination for the difference frequency generation (optical parametric amplification) under non-collinear geometry.

Optimal control of filamentation in air

The authors demonstrate optimal control of the propagation of ultrashort, ultraintense (multiterawatt) laser pulses in air over distances up to 36m in a closed-loop scheme. They optimized three spectral ranges within the white-light continuum as well as the ionization efficiency. Optimization results in signal enhancements by typical factors of 2 and 1.4 for the target parameters. The optimization results in shorter pulses by reducing their chirp in the case of white-light continuum generation, while they correct the pulse from its defects and set the filamentation onset near the detector as far as air ionization is concerned.

Spatial modes in a PCF fiber generated continuum

We measure the propagation properties of a highly nonlinear photonic crystal fiber (PCF). The spatial, temporal and frequency dependent properties of the propagating modes are measured under conditions of high power, seven picosecond excitation, white light continuum generation. The experimentally determined multi-mode nature of the white light continuum is found to be in good agreement with numerical simulations.

Enhancing red-shifted white-light continuum generation in optical fibers for applications in nonlinear Raman microscopy

We report an efficient red-shifted continuum generation of picosecond pulses in conventional optical fibers. By using a novel highrepetition rate, high-energy oscillator operating at the fundamental wavelength of 1064 nm, we achieved more than 60% of the output energy in the spectral range from 1150 to 1300 nm, perfectly suitable for broadband coherent anti-Stokes Raman spectroscopy.

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Toward Highly Active Two-Photon Absorbing Liquids. Synthesis and Characterization of 1,3,5-Triazine-Based Octupolar Molecules

Three novel two-photon absorbing (TPA) chromophores with 1,3,5-triazine as the π-electron deficient core, dialkylfluorene as aromatic bridges, and diphenylamino groups as the electron-donating end-groups were prepared. Designated as AF-450 (2,4,6-tris[7-(diphenylamino)-9,9-didecylfluoren-2-yl]-1,3,5-triazine), AF-455 (2,4,6-tris[9,9-bis(3,7-dimethyloctyl)-7-(diphenylamino)-fluoren-2yl]-1,3,5-triazine), and AF-457 (2,4,6-tris[(7-(diphenylamino)-9,9-diprop-2-enylfluoren-2-yl]-1,3,5-triazine), their overall molecular structure and local symmetry (D3h) are similar to those of previously reported three-armed AF-350 (N,N,N-tris[4-{7-(2-benzothiazolyl)-9,9-diethylfluoren-2-yl}phenyl]amine) and AF-380 (N,N,N,-tris[7-(2-benzothiazolyl)-9,9-diethylfluoren-2-yl]amine). Among the family of AFX chromophores previously reported by us, AF-450 possesses one of the largest effective TPA cross-sections (σ2‘ = 39 500 × 10-50 cm4-sec/photon-molecule, or 39 500 GM) as determined by nonlinear transmission method in the nanosecond regime at 800 nm. In contrast, AF-455, a mixture of stereoisomers with the same chemical formula as AF-450, is a glassy material that becomes fluid (molasses-like) upon heating at 70−80 °C and has noticeably smaller effective σ2‘ value (33 300 GM). AF-457 (σ2‘ = 27 800 GM) with six allyl side groups was prepared as a precursor toward the synthesis of a TPA liquid. The intrinsic TPA cross-sections of these chromophores were also determined as a function of excitation wavelengths via a femtosecond white-light continuum generation and direct degenerate-TPA measurement technique. At the TPA peaks ∼779 nm, their σ2‘ values are 216, 214, and 199 GM (±15%) for AF-450, AF-455, and AF-457, in that order. They are in the same trend as the nanosecond values, albeit two orders of magnitude lower.