Pulsed Laser Excitation Research Articles

Correlated-photon-pair generation via SFWM in tapered optical fibers with femtosecond laser pump

Spontaneous four-wave mixing (SFWM) in optical micro-/nanofibers is studied theoretically and experimentally. Joint spectral intensity of the biphoton field generated via SFWM under excitation of femtosecond laser pulses is measured and calculated considering self-phase modulation of the pump pulses and SFWM throughout the tapered fibers. In comparison with the previous study (Shukhin et al 2020 Phys. Rev. A 101 053822), replacing picosecond pump by a femtosecond one with the same average power makes it possible to increase the photon pair generation rate tenfold.

Continuously wavelength tunable, continuous wave laser ideal for UV Raman spectroscopy

AbstractWe utilize a novel, high‐power, tunable, continuous wave (CW) deep UV laser to measure resonance Raman spectra of phenolate solutions with high signal‐to‐noise ratios (SNR). In UV resonance Raman (UVRR), increased coupling of the excitation light with a chromophore can transfer molecules into excited states that cause increased heating and photochemistry. Deep UV lasers have traditionally utilized high peak powers to enable efficient single‐pass nonlinear conversion from visible into near infrared light. Nonlinear phenomena such as the formation of transient radical species, Raman saturation, thermal heating, and dielectric breakdown can introduce extraneous light sources that can complicate the interpretation of the Raman spectrum. Dielectric breakdown can increase the baseline, increase noise, and sometimes saturate the detector, preventing Raman detection. Spontaneous Raman scattering intensities should scale linearly with the excitation light intensity. However, this linear behavior does not always occur with pulsed laser excitation. This occurs because stimulated Raman scattering can cause a superlinear intensity response, or transient absorption can cause sublinear intensity responses. CW laser excitation excites samples with electric fields that are much lower than typical pulsed laser excitation. This eliminates the nonlinear responses. The geometry of our new CW laser enables high gain in the harmonic generation cavities that achieve high harmonic generation efficiencies. Average power in the deep UV is >30 mW for wavelengths as short as 206 nm. In the work here, we demonstrate that CW excitation is ideal for resonance Raman measurements in general to reduce spectral complexity.

Photoacoustic speckle pattern interferometry for detecting cracks of different sizes.

A system and method for non-destructive detection of cracks of different width and depths based on digital speckle interferometry coupled with pulsed laser excitation is introduced and tested. Based on photoacoustic effect, acoustic waves are induced onto the rear of the samples by pumping a pulsed laser beam on it. The generated mechanical wave propagates from the rear surface of the sample to the front while front surface is monitored by speckle interferometry. In order to acquire information about surface deformation, the front surface is illuminated by continuous wave laser and interference are imaged onto the camera as speckle images. After processing the produced fringe patterns, it indicates the presence and location of the cracks in qualitative way. In this study, the system and method mentioned above are validated by detecting medium density fiberboard with simulated cracks. The fringe patterns from areas with or without defects are compared and discussed. Besides, the system and method to distinguish and predict cracks sizes is proposed and validated.

Single Atom Stabilization of Phosphinate Ester-Containing Rhodamines Yields Cell Permeable Probes for Turn-On Photoacoustic Imaging.

Photoacoustic imaging (PAI) is an emerging imaging technique that uses pulsed laser excitation with near-infrared (NIR) light to elicit local temperature increases through non-radiative relaxation events, ultimately leading to the production of ultrasound waves. The classical xanthene dye scaffold has found numerous applications in fluorescence imaging, however, xanthenes are rarely utilized for PAI since they do not typically display NIR absorbance. Herein, we report the ability of Nebraska Red (NR) xanthene dyes to produce photoacoustic (PA) signal and provide a rational design approach to reduce the hydrolysis rate of ester containing dyes, affording cell permeable probes. To demonstrate the utility of this approach, we construct the first cell permeable rhodamine-based, turn-on PAI imaging probe for hypochlorous acid (HOCl) with maximal absorbance within the range of commercial PA instrumentation. This probe, termed SNR700 -HOCl, is capable of detecting exogenous HOCl in mice. This work provides a new set of rhodamine-based PAI agents as well as a rational design approach to stabilize esterified versions of NR dyes with desirable properties for PAI. In the long term, the reagents described herein could be utilized to enable non-invasive imaging of HOCl in disease-relevant model systems.

Ultrafast terahertz spin and orbital transport in magnetic/nonmagnetic multilayer heterostructures and a perspective

Ultrafast optically excited ferromagnetic (FM)/nonmagnetic (NM) multilayer heterostructures have been demonstrated recently as efficient, high-power, and broadband sources of terahertz (THz) electromagnetic radiation. Since these spintronic THz emitters exploit the conversion from ultrafast spin to charge current, either in bulk or at the interface, the THz pulses inhere all the characteristics of the involved mechanisms and dynamics associated with spin-charge interconversion processes. Deconvolving the same requires meticulous and careful experimentation and analysis. In this article, we review the current state-of-the-art in this field and provide a perspective on the emerging phenomena, which are prospering as new research avenues and demonstrate application potential for futuristic THz technologies. In the process of developing efficient spintronic THz emitters by optimizing various conditions including those with material parameters and excitation light, it turns out that THz emission spectroscopy itself can be a unique experimental tool for probing microscopic dynamical magnetic and spintronic effects, induced by femtosecond laser pulse excitation, in a noncontact and noninvasive manner. Several breakthroughs can be listed from the literature in this regard from the last decade. Just recently, ultrafast orbitronics is another dimension that is taking shape and will impact the field immensely. A fair account to this topic is also presented in the article.

GaN film optical nonlinearity: wavelength dependent refractive index for All-Optical switching application

Gallium Nitride (GaN) is fast becoming a potential replacement for silicon in complex electronic and photonics circuitries and systems. At higher optical intensity, optical effects such as non-linear effects would become non-trivial. To this end, we investigated nonlinear optical properties of metal–organic chemical vapor deposited GaN. Specifically, continuous-wave laser Z-scan techniques were employed to obtain nonlinear refractive index, n2, of a 1-µm thin layer on a c-plane sapphire substrate. FESEM, PL, XRD and EDS analysis confirmed the good quality growth of GaN thin film. We detected a reversal of polarity of the n2 value at 637 nm and 405 nm of CW laser excitation and femtosecond laser pulse at 808 nm. This is substantiated by theoretical calculation of GaN’s n2 showing sign switchover at wavelength shorter than 420 nm. This presents a new all-optical switching scheme based on the switchover of wavelength dependent n2. These findings point to opportunities for GaN-based integrated photonics for nonlinear and quantum photonics applications.

Micrometer-Scale Carrier Transport in the Solid Film of Giant CdSe/CdS Nanocrystals Imaged by Transient Absorption Microscopy.

For the practical applications in solar cells and photodetectors, semiconductor colloidal nanocrystals (NCs) are assembled into a high-concentration film with carrier transport characteristics, the full understanding and effective control of which are critical for the achievement of high light-to-electricity conversion efficiencies. Here we have applied transient absorption microscopy to the solid film of giant CdSe/CdS NCs and discovered that at high pump fluences the carrier transport could reach a long distance of ∼2 μm within ∼30 ps after laser pulse excitation. This intriguing behavior is attributed to the metal-insulator transition and the associated bandlike transport, which are promoted by the enhanced electronic coupling among neighboring NCs with extended wave functions overlap of the excited-state charge carriers. Besides providing fundamental transport information in the regime of high laser pump fluences, the above findings shed light on the rational design of high-power light detecting schemes based on colloidal NCs.

A New Gas Analysis Method Based on Single-Beam Excitation Stimulated Raman Scattering in Hollow Core Photonic Crystal Fiber Enhanced Raman Spectroscopy.

We previously developed a hollow-core photonic crystal fiber (HCPCF) based Raman scattering enhancement technique for gas/human breath analysis. It enhances photon-gas molecule interactions significantly but is still based on CW laser excitation spontaneous Raman scattering, which is a low-probability phenomenon. In this work, we explored nanosecond/sub-nanosecond pulsed laser excitation in HCPCF based fiber enhanced Raman spectroscopy (FERS) and successfully induced stimulated Raman scattering (SRS) enhancement. Raman measurements of simple and complex gases were performed using the new system to assess its feasibility for gas analysis. We studied the gas Raman scattering characteristics, the relationship between Raman intensities and pump energies, and the energy threshold for the transition from spontaneous Raman scattering to SRS. H2, CO2, and propene (C3H6) were used as test gases. Our results demonstrated that a single-beam pulsed pump combined with FERS provides an effective Raman enhancement technique for gas analysis. Furthermore, an energy threshold for SRS initiation was experimentally observed. The SRS-capable FERS system, utilizing a single-beam pulsed pump, shows great potential for analyzing complex gases such as propene, which is a volatile organic compound (VOC) gas, serving as a biomarker in human breath for lung cancer and other human diseases. This work contributes to the advancement of gas analysis and opens alternative avenues for exploring novel Raman enhancement techniques.

Excitation-Wavelength-Dependent Charge Injection and Hole Localization in Diblock Oligomers Anchored to TiO2.

A series of diblock oligomers containing oligothiophene (Tn, n = 4, 5) and 4,7-di(thiophen-2-yl)benzo[c][1,2,5]thiadizole (TBT) segments, functionalized with carboxylic acid anchoring groups, were prepared and anchored to mesoporous TiO2 films to study wavelength-dependent interfacial electron transfer mechanisms. Thin films of the surface-anchored diblock oligomers contained two absorption bands centered at 400 and 500 nm, corresponding to the Tn and TBT blocks, respectively. Pulsed-laser excitation of the oligomer-sensitized films yielded local excited-states that promoted electron injection into TiO2. The injection pathway was dependent on the excitation wavelength, as electron injection occurred from the oligomer block that was locally excited. Recombination between the injected electron and the oxidized oligomer was sensitive to the bridging unit that separates the oligomer conjugated segments (-C≡C- vs trans-Pt(PBu3)2-). When the bridge facilitated strong coupling between the two blocks (-C≡C- bridge), the excitation wavelength had no effect on the recombination pathway, as the hole was delocalized over the entire oligomer. However, in the weak coupling case (Pt(PBu3)2- bridge), selective excitation resulted in wavelength-dependent hole localization that persisted to the μs time scale, providing control over the recombination pathway by varying the excitation wavelength. Dye-sensitized solar cells (DSSCs) were fabricated by using the diblock oligomers as sensitizers. The photocurrent action spectra were measured, and the absorbed photon-to-current efficiency (APCE) provided further insight into the electron-transfer mechanisms that are operative under continuous illumination.

Photoluminescence of high energy xenon ion irradiated magnesium aluminate spinel single crystals

Laser confocal microscopy technique (60 ps laser pulse excitation at 445 nm) and a time-correlated single photon counting (TCSPC) technique have been used to study the photoluminescence (PL) in 152 MeV Xe ion irradiated MgAl2O4 single crystals. It was shown that radiation defects produced by swift xenon ions give rise to broad luminescence band positioned in the 470–800 nm wavelength range. The measurements of the PL decay curves have evidenced that lifetime of defect-related PL signal gradually increases from 6 to 10 ns in 500–620 nm spectral range and decreases with ion fluence increasing. The decrease of the luminescence intensity observed after fluences ∼1013 cm−2 is attributed to overlapping of individual ion track core regions.

Ultrafast photoacoustic cavitation pumped by picosecond laser for high-efficient and long-term shockwave theranostics

Photoacoustic (PA) theranostics is a new emerging field that uniquely combines diagnosis and treatment in one modality. However, its current status is compromised by the indispensable dependence on nonreversible phase-change nanoprobes that provides one-time-only action. Here, we demonstrate a picosecond-laser-pumped ultrafast PA cavitation technique for highly efficient shockwave theranostics, guaranteeing sustained PA cavitation by using non-phase-change nanoprobes. Theoretical simulations validate that, when compressing the excitation laser pulse width to hundred-picosecond, the thermal confinement effects of a conventional nanoprobe will induce transient heating of the extremely thin surrounding liquid layer of the nanoprobes beyond its cavitation point in a localized area at nanoscale, resulting in intense cavitation and PA shockwaves by the environment rather than the nanoprobes. Both cellular and mouse model experiments have demonstrated the highly effective anti-tumor effects. This method provides a sustainable, reproducible, and highly effective strategy for PA theranostics, prefiguring great potential for the clinical applications.

LIBS at high duty-cycles: effect of repetition rate and temporal width on the excitation laser pulses

Laser-induced breakdown spectroscopy (LIBS) is becoming a more mature technology every year with new variants such as laser ablation molecular isotopic spectrometry, reheating by various discharge techniques, and multiple pulse excitation schemes, in which sometimes lasers of different pulse lengths are used. However, lasers with inherent parameters like pulse length and repetition rate are still almost exclusively employed. Recent years have witnessed the advent of novel high-repetition-rate laser concepts for machining processes, like welding, milling, and engraving. Here, a comprehensive study of single-pulse LIBS spectra of a single aluminum target is presented to showcase the applicability of flexible high duty-cycle master oscillator power amplifier (MOPA) lasers. Although traditional flashlamp-pumped Fabry–Pérot lasers only permit a variation in the pulse energy and are operated at very low duty-cycles, MOPA lasers add repetition rate and pulse length as variable parameters. A thorough analysis of the temporal plasma behavior revealed the emission dynamic to closely match the excitation laser pulse pattern. An aluminum sample’s spectral response was shown to be significantly impacted by variations in both rate and length. Although the spectral emission strength of the elemental lines of Al, Sr, and Ca all peaked at slightly different parameter settings, the strongest impact was found on the relative abundance of molecular AlO bands. Unlike in previous laser ablation molecular isotopic spectrometry (LAMIS) publications, the latter could be readily detected with a good intensity and well-resolved spectral features without any temporal gating of the detector. This finding, together with the fact that MOPA lasers are both inexpensive and dependable, makes for a promising combination for future studies including the detection of diatomic band structures.

Laser-plasma sound sources in atmospheric air: A systematic experimental study

Laser-plasma sound sources are increasingly utilized in technological and scientific applications as attractive alternatives to conventional electromechanical or piezoelectric transducers. This work presents a systematic experimental study of laser-plasma sound sources generated in atmospheric air by strong, short and ultrashort laser pulses. Emphasis is given on the dependence of their acoustic emission on the characteristics of the optical radiation. In the experiments, nanosecond and femtosecond laser pulses with different energies and optical wavelengths are focused in atmospheric air using lenses of different focusing power. The produced acoustic pulses are captured via a system with high dynamic range and broad frequency response in the far field of the plasma source. The acoustic signals are analysed both in the time and frequency domains to extract their primary characteristics, particularly the total acoustic energy, peak pressure, spectral magnitude and spectral peak frequency. The results are systematically examined and compared with respect to the characteristics of the exciting laser pulses. The experimental observations are supported by theoretical calculations of the generated plasma density via rate equations that account for the main ionization and electron loss mechanisms. The presented analysis provides a frame for controlling the acoustic characteristics of laser-plasma sound sources, which is particularly important for applications in the fields of acoustic measurements, sound reproduction and biomedicine.

Optical blood-brain-tumor barrier modulation expands therapeutic options for glioblastoma treatment

The treatment of glioblastoma has limited clinical progress over the past decade, partly due to the lack of effective drug delivery strategies across the blood-brain-tumor barrier. Moreover, discrepancies between preclinical and clinical outcomes demand a reliable translational platform that can precisely recapitulate the characteristics of human glioblastoma. Here we analyze the intratumoral blood-brain-tumor barrier heterogeneity in human glioblastoma and characterize two genetically engineered models in female mice that recapitulate two important glioma phenotypes, including the diffusely infiltrative tumor margin and angiogenic core. We show that pulsed laser excitation of vascular-targeted gold nanoparticles non-invasively and reversibly modulates the blood-brain-tumor barrier permeability (optoBBTB) and enhances the delivery of paclitaxel in these two models. The treatment reduces the tumor volume by 6 and 2.4-fold and prolongs the survival by 50% and 33%, respectively. Since paclitaxel does not penetrate the blood-brain-tumor barrier and is abandoned for glioblastoma treatment following its failure in early-phase clinical trials, our results raise the possibility of reevaluating a number of potent anticancer drugs by combining them with strategies to increase blood-brain-tumor barrier permeability. Our study reveals that optoBBTB significantly improves therapeutic delivery and has the potential to facilitate future drug evaluation for cancers in the central nervous system.

Single- and two-photon absorption induced all-optical control of gallium selenide integrated silicon nitride photonic devices in the 700–800 nm wavelength range

In this work, we report single- and two-photon absorption (TPA) induced transmission and resonance modulation in a multilayer gallium selenide (GaSe) integrated silicon nitride (Si3N4) waveguide and ring resonator operating in the 700–800 nm wavelength range. Intensity dependent saturable absorption at low optical powers followed by TPA at higher power levels in GaSe integrated Si3N4 waveguides is observed at 785 nm pulsed laser excitation. A TPA coefficient of 0.117 cm/GW for the GaSe–Si3N4 composite waveguide and a three-photon absorption coefficient of 7.876 × 10−6 cm3/GW2 for the bare Si3N4 waveguide are extracted from intensity dependent transmission measurements. The single-photon absorption process induced by a blue laser incident on the multilayer GaSe transferred on top of the Si3N4 ring resonator is used for all-optical resonance tuning through the free-carrier refraction effect. A strong blue shift of the resonance by ∼12.3 pm/mW combined with resonance broadening is observed due to the free-carrier induced refractive index and absorption modulation. The TPA in the GaSe integrated Si3N4 ring resonator is also shown to result in a blue shift of the resonances excited using a 785 nm pulsed laser. This work demonstrates the all-optical control of 2D material integrated Si3N4 guided-wave structures operating in the shorter near-infrared wavelength range with potential applications in integrated quantum photonics, miniaturized sensing devices, and biomedical imaging.

Multiscale out-of-equilibrium dynamics driven by pulsed laser excitation in spin-crossover materials: A combined thermoelastic and mechanoelastic study

Multiscale out-of-equilibrium dynamics driven by pulsed laser excitation in spin-crossover materials: A combined thermoelastic and mechanoelastic study

Approximation Schemes to Include Nuclear Motion in Laser-Driven Ab Initio Electron Dynamics: Application to High Harmonic Generation.

The quantum mechanical description of many-electron dynamics in molecules driven by short laser pulses is at the heart of theoretical attochemistry. In addition to the formidable time-dependent electronic structure problem, the field faces the challenge that nuclear motion, ideally also treated quantum mechanically, may not be negligible, but scales enormously in effort. As a consequence, most first-principles calculations on ultrafast electron dynamics in molecules are done within the fixed-nuclear approximation. For laser-pulse excitation in H2+, where an "exact" treatment of the coupled nuclear-electron dynamics is possible, it has been shown that nuclear motion can have a nonnegligible impact on high harmonic generation (HHG) spectra (Witzorky et al., J. Chem. Theor. Comput. 2021, 17, 7353-7365). It is not so clear, however, how to include (quantum) nuclear motion also for more complicated molecules, with more electrons and/or nuclei, in particular when the electronic structure is described by correlated, multistate wavefunction methods such as the time-dependent configuration interaction (TD-CI). In this work, we suggest a scheme in which the Born-Oppenheimer potential energy surfaces of a molecule are approximated by model potentials (harmonic and asymptotic, as an expansion in 1/R), obtained from only a few ab initio calculations, with the prospect to treat complex molecular systems. The method is tested successfully for HHG by few-cycle laser pulses for the "exact" H2+ reference. It is then applied for diatomic molecules with more electrons and for a two-dimensional model of the water molecule using TD-CIS (S = single) for the electronic structure part.

Singlet oxygen lifetime changes in dying glioblastoma cells.

Time-resolved phosphorescence detection was employed to determine the lifetime of singlet oxygen in live cells. Using hypericin as a photosensitizer, singlet oxygen was generated in U87MG glioblastoma cells. The phosphorescence of singlet oxygen was detected in aqueous cell suspensions following pulsed laser excitation. Our goal was to eliminate or reduce the problems associated with lifetime measurements in water-based cell suspensions. The apparatus enabled simultaneous singlet oxygen phosphorescence and transient absorption measurements, reducing uncertainty in lifetime estimation. The changes in singlet oxygen lifetime were observed during early and late apoptosis induced by photodynamic action. Our findings show that the effective lifetime of singlet oxygen in the intracellular space of the studied glioblastoma cells is 0.4 μs and increases to 1.5 μs as apoptosis progresses. Another group of hypericin, presumably located in the membrane blebs and the plasma membrane of apoptotic cells, generates singlet oxygen with a lifetime of 1.9 μs.

Terahertz photocurrent spectrum analysis of AlGaAs/GaAs/GaAsBi multi-junction solar cells

Characterizing subcells in two-terminal multi-junction (M-J) solar cells is challenging due to the lack of direct electrical access. This work presents a novel contactless spectral characterization technique for analysing individual subcells. The technique involves probing terahertz (THz) radiation generated by femtosecond laser pulse excitation and varying the exciting wavelength to selectively absorb light in the desired subcell. The registered THz pulse integral is then proportional to the induced photocurrent in that subcell. The THz photocurrent spectroscopy technique is demonstrated on GaAs and AlGaAs single-junction solar cells, as well as on the triple-junction AlGaAs/GaAs/GaAsBi solar cell. The results show that the recently developed GaAsBi-based subcell, with a nominal energy bandgap of 1.0 eV, exhibits improved electron–hole separation efficiency and can enhance energy harvesting by M-J solar cells.

Emission Spectra of Molecular Gases CHF3, CCl2F2, SF6 in the Range 3–20 nm under Pulsed Laser Excitation Using Various Gas Jets as Targets

Emission Spectra of Molecular Gases CHF3, CCl2F2, SF6 in the Range 3–20 nm under Pulsed Laser Excitation Using Various Gas Jets as Targets