Exfoliation procedure-dependent optical properties of solution deposited MoS2 films.

The development of high-precision large-area optical coatings and devices comprising low-dimensional materials hinges on scalable solution-based manufacturability with control over exfoliation procedure-dependent effects. As such, it is critical to understand the influence of technique-induced transition metal dichalcogenide (TMDC) optical properties that impact the design, performance, and integration of advanced optical coatings and devices. Here, we examine the optical properties of semiconducting MoS2 films from the exfoliation formulations of four prominent approaches: solvent-mediated exfoliation, chemical exfoliation with phase reconversion, redox exfoliation, and native redox exfoliation. The resulting MoS2 films exhibit distinct refractive indices (n), extinction coefficients (k), dielectric functions (ε1 and ε2), and absorption coefficients (α). For example, a large index contrast of Δn ≈ 2.3 is observed. These exfoliation procedures and related chemistries produce different exfoliated flake dimensions, chemical impurities, carrier doping, and lattice strain that influence the resulting optical properties. First-principles calculations further confirm the impact of lattice defects and doping characteristics on MoS2 optical properties. Overall, incomplete phase reconfiguration (from 1T to mixed crystalline 2H and amorphous phases), lattice vacancies, intraflake strain, and Mo oxidation largely contribute to the observed differences in the reported MoS2 optical properties. These findings highlight the need for controlled technique-induced effects as well as the opportunity for continued development of, and improvement to, liquid phase exfoliation methodologies. Such chemical and processing-induced effects present compelling routes to engineer exfoliated TMDC optical properties toward the development of next-generation high-performance mirrors, narrow bandpass filters, and wavelength-tailored absorbers.

Laser-Fabricated 2D Molybdenum Disulfide Electronic Sensor Arrays for Rapid, Low-Cost, Ultrasensitive Detection of Influenza A and SARS-Cov-2.

Multiplex electronic antigen sensors for detection of SARS-Cov-2 spike glycoproteins and hemagglutinin from influenza A are fabricated using scalable processes for straightforward transition to economical mass-production. The sensors utilize the sensitivity and surface chemistry of a 2D MoS2 transducer for attachment of antibody fragments in a conformation favorable for antigen binding with no need for additional linker molecules. To make the devices, ultra-thin layers (3 nm) of amorphous MoS2 are sputtered over pre-patterned metal electrical contacts on a glass chip at room temperature. The amorphous MoS2 is then laser annealed to create an array of semiconducting 2H-MoS2 transducer regions between metal contacts. The semiconducting crystalline MoS2 region is functionalized with monoclonal antibody fragments complementary to either SARS-CoV-2 S1 spike protein or influenza A hemagglutinin. Quartz crystal microbalance experiments indicate strong binding and maintenance of antigen avidity for antibody fragments bound to MoS2. Electrical resistance measurements of sensors exposed to antigen concentrations ranging from 2-20 000 pg mL-1 reveal selective responses. Sensor architecture is adjusted to produce an array of sensors on a single chip suited for detection of analyte concentrations spanning six orders of magnitude from pg mL-1 to µg mL-1.

Optical microscopy and confocal data of aerosol jet printed lines over a 16-hour print duration.

Optical microscopy images and confocal data for Aerosol Jet Printed (AJP) lines over a 16 hour print duration is provide in this dataset ("Mapping Drift in Morphology and Electrical Performance in Aerosol Jet Printing" [1]). Lines were uninterruptedly printed by AJP on a glass substrate using silver nanoparticle ink over a 16-hour time frame. The ink used for this experiment was a 0.6:0.3:0.2 mL mixture of Clariant Prelect TPS 50 G2 silver nanoparticle ink, ethylene glycol, and deionized water, respectively. Deposition was achieved with an Optomec AJ 300-UP Aerosol JetTM Deposition System using a Sprint Series Ultrasonic Atomizer MAX, aerodynamic filtering, and a nozzle having an orifice diameter of 150 µm. The typical focus ratio of 1.75 within standard range was used. The optical microscopic images of 350 µm AJP printed lines at 80 different time points were then selectively collected. Keyence VK-X200 with 150x magnification was used, which provided 50 µm to 267 pixel resolution image with more than 1000 cross-sections at each time point. Filtering of the pixels with outlying heights was performed with a multi-file analyzer. The dataset was primarily collected to understand system-level, temporal drifts in print morphology, which would further allow to predict electrical performance in time domain. Additional purposes for the dataset include: 1) benchmark dataset for morphology and print performance between AJP systems and print settings, 2) test data for new image filtering, segmentation, and classification algorithms and 3) baseline training data for real-time, in situ classification of operational time windows for AJP feedback control.

Single-Shot Multi-Stage Damage and Ablation of Silicon by Femtosecond Mid-infrared Laser Pulses.

Although ultrafast laser materials processing has advanced at a breakneck pace over the last two decades, most applications have been developed with laser pulses at near-IR or visible wavelengths. Recent progress in mid-infrared (MIR) femtosecond laser source development may create novel capabilities for material processing. This is because, at high intensities required for such processing, wavelength tuning to longer wavelengths opens the pathway to a special regime of laser-solid interactions. Under these conditions, due to the λ2 scaling, the ponderomotive energy of laser-driven electrons may significantly exceed photon energy, band gap and electron affinity and can dominantly drive absorption, resulting in a paradigm shift in the traditional concepts of ultrafast laser-solid interactions. Irreversible high-intensity ultrafast MIR laser-solid interactions are of primary interest in this connection, but they have not been systematically studied so far. To address this fundamental gap, we performed a detailed experimental investigation of high-intensity ultrafast modifications of silicon by single femtosecond MIR pulses (λ = 2.7-4.2 µm). Ultrafast melting, interaction with silicon-oxide surface layer, and ablation of the oxide and crystal surfaces were ex-situ characterized by scanning electron, atomic-force, and transmission electron microscopy combined with focused ion-beam milling, electron diffractometry, and µ-Raman spectroscopy. Laser induced damage and ablation thresholds were measured as functions of laser wavelength. The traditional theoretical models did not reproduce the wavelength scaling of the damage thresholds. To address the disagreement, we discuss possible novel pathways of energy deposition driven by the ponderomotive energy and field effects characteristic of the MIR wavelength regime.

Ultrafast mid-infrared high harmonic and supercontinuum generation with n2 characterization in zinc selenide.

Polycrystalline ZnSe is an exciting source of broadband supercontinuum and high-harmonic generation via random quasi phase matching, exhibiting broad transparency in the mid-infrared (0.5-20 µm). In this work, the effects of wavelength, pulse power, intensity, propagation length, and crystallinity on supercontinuum and high harmonic generation are investigated experimentally using ultrafast mid-infrared pulses. Observed harmonic conversion efficiency scales linearly in propagation length, reaching as high as 36%. For the first time to our knowledge, n2 is measured for mid-infrared wavelengths in ZnSe: n2(λ=3.9 µm)=(1.2±0.3)×10-14 cm2/W. Measured n2 is applied to simulations modeling high-harmonic generation in polycrystalline ZnSe as an effective medium.

Femtosecond laser damage of germanium from near- to mid-infrared wavelengths.

Femtosecond laser-induced damage and ablation (fs-LIDA) is a rich field in extreme non-perturbative nonlinear optics with wide ranging applications, including laser micro- and nano-machining, waveguide writing, and eye surgery. Our understanding of fs-LIDA, however, is limited mostly to visible and near-infrared wavelengths. In this work, we systematically study single-shot, fs-laser ablation (fs-LIA) of single-crystal germanium from near- to mid-infrared wavelengths, and compare the fs-LIA wavelength scaling with two widely used models. We show that these models are inadequate, particularly at mid-infrared wavelengths. Instead, a hybrid model is proposed involving Keldysh ionization rates, a constant free-carrier density threshold, and multi-band effects, which yields good agreement with experimental observations. Aspects of this model may be applied to understanding other strong-field non-perturbative phenomena in solids.

Relativistic electron acceleration by mJ-class kHz lasers normally incident on liquid targets.

We report observation of kHz-pulsed-laser-accelerated electron energies up to 3 MeV in the -klaser (backward) direction from a 3 mJ laser interacting at normal incidence with a solid density, flowing-liquid target. The electrons/MeV/s.r. >1 MeV recorded here using a mJ-class laser exceeds or equals that of prior super-ponderomotive electron studies employing lasers at lower repetition-rates and oblique incidence. Focal intensity of the 40-fs-duration laser is 1.5 · 1018 W cm-2, corresponding to only ∼80 keV electron ponderomotive energy. Varying laser intensity confirms electron energies in the laser-reflection direction well above what might be expected from ponderomotive scaling in normal-incidence laser-target geometry. This direct, normal-incidence energy spectrum measurement is made possible by modifying the final focusing off-axis-paraboloid (OAP) mirror with a central hole that allows electrons to pass, and restoring laser intensity through adaptive optics. A Lanex-based, optics-free high-acquisition rate (>100 Hz) magnetic electron-spectrometer was developed for this study to enable shot-to-shot statistical analysis and real-time feedback, which was leveraged in finding optimal pre-plasma conditions. 3D Particle-in-cell simulations of the interaction show qualitative super-ponderomotive spectral agreement with experiment. The demonstration of a high-repetition-rate, high-flux source containing >MeV electrons from a few-mJ, 40 fs laser and a simple liquid target encourages development of future ≥kHz-repetition, fs-duration electron-beam applications.

Few-cycle pulse laser induced damage threshold determination of ultra-broadband optics.

A systematic study of few-cycle pulse laser induced damage threshold (LIDT) determination was performed for commercially-available ultra-broadband optics, (i.e. chirped mirrors, silver mirrors, beamsplitters, etc.) in vacuum and in air, for single and multi-pulse regime (S-on-1). Multi-pulse damage morphology at fluences below the single-pulse LIDT was studied in order to investigate the mechanisms leading to the onset of damage. Stark morphological contrast was observed between multi-pulse damage sites formed in air versus those in vacuum. One effect of vacuum testing compared to air included suppression of laser-induced periodic surface structures (LIPSS) formation, possibly influenced by a reduced presence of damage debris. Another effect of vacuum was occasional lowering of LIDT, which appears to be due to the stress-strain performance of the coating design during laser irradiation and under the external stress of vacuum ambience. A fused silica substrate is also examined, and a non-LIPSS nanostructuring is observed on the surface. Possible mechanisms are discussed.

Laser induced periodic surface structure formation in germanium by strong field mid IR laser solid interaction at oblique incidence.

Laser induced periodic surface structures (LIPSS or ripples) were generated on single crystal germanium after irradiation with multiple 3 µm femtosecond laser pulses at a 45° angle of incidence. High and low spatial frequency LIPSS (HSFL and LSFL, respectively) were observed for both s- and p-polarized light. The measured LSFL period for p-polarized light was consistent with the currently established LIPSS origination model of coupling between surface plasmon polaritons (SPP) and the incident laser pulses. A vector model of SPP coupling is introduced to explain the formation of s-polarized LSFL away from the center of the damage spot. Additionally, a new method is proposed to determine the SPP propagation length from the decay in ripple depth. This is used along with the measured LSFL period to estimate the average electron density and Drude collision time of the laser-excited surface. Finally, full-wave electromagnetic simulations are used to corroborate these results while simultaneously offering insight into the nature of LSFL formation.