Monolayers of transition metal dichalcogenides (TMdC) are promising candidates for realization of a new generation of optoelectronic devices. The optical properties of these two-dimensional materials, however, vary from flake to flake, or even across individual flakes, and change over time, all of which makes control of the optoelectronic properties challenging. There are many different perturbations that can alter the optical properties, including charge doping, defects, strain, oxidation, and water intercalation.Identifying which perturbations are present is usually not straightforward and requires 1 arXiv:1909.08214v1 [cond-mat.mtrl-sci] 18 Sep 2019 multiple measurements using multiple experimental modalities, which presents barriers when attempting to optimise preparation of these materials. Here, we apply highresolution photoluminescence and differential reflectance hyperspectral imaging in situ to CVD-grown WS 2 monolayers. By combining these two optical measurements and using a statistical correlation analysis we are able to disentangle three contributions modulating optoelectronic properties of these materials: electron doping, strain and defects. In separating these contributions, we also observe that the B-exciton energy is less sensitive to variations in doping density than A-excitons.

Despite 2D materials holding great promise for a broad range of applications, the proliferation of devices and their fulfillment of real-life demands are still far from being realized. Experimentally obtainable samples commonly experience a wide range of perturbations (ripples and wrinkles, point and line defects, grain boundaries, strain field, doping, water intercalation, oxidation, edge reconstructions) significantly deviating the properties from idealistic models. These perturbations, in general, can be entangled or occur in groups with each group forming a complex perturbation making the interpretations of observable physical properties and the disentanglement of simultaneously acting effects a highly non-trivial task even for an experienced researcher. Here we generalise statistical correlation analysis of excitonic spectra of monolayer WS2, acquired by hyperspectral absorption and photoluminescence imaging, to a multidimensional case, and examine multidimensional correlations via unsupervised machine learning algorithms. Using principal component analysis we are able to identify four dominant components that are correlated with tensile strain, disorder induced by adsorption or intercalation of environmental molecules, multi-layer regions and charge doping, respectively. This approach has the potential to determine the local environment of WS2 monolayers or other 2D materials from simple optical measurements, and paves the way toward advanced, machine-aided, characterization of monolayer matter.

Michelson interferometers have been routinely used in various applications ranging from testing optical components to interferometric time-resolved spectroscopy measurements. Traditionally, plate beamsplitters are employed to redistribute radiation between the two arms of an interferometer. However, such an interferometer is susceptible to relative phase fluctuations between the two arms resulting from vibrations of the beamsplitter. This drawback is circumvented in diffraction-grating-based interferometers, which are especially beneficial in applications where highly stable delays between the replica beams are required. In the vast majority of grating-based interferometers, reflective diffraction gratings are used as beamsplitters. Their diffraction efficiency, however, is strongly wavelength dependent. Therefore transmission-grating interferometers can be advantageous for spectroscopy methods, since they can provide high diffraction efficiency over a wide spectral range. Here, we present and characterize a transmission grating-based Michelson interferometer, which is practically dispersion-free, has intrinsically high symmetry and stability and moderate throughput efficiency, and is promising for a wide range of applications.

Investigating the optical properties of various chemical compounds using UV–vis spectrophotometers is an essential part of education in chemistry. However, commercial spectrophotometers are usually treated as “magic black boxes”, where the dominant majority of optical elements are hidden “under the hood”. This often limits understanding of the mechanisms behind the generation of spectral curves, which in turn may impede the ability to understand the limitations of the applied method and, in some cases, interpret the acquired data. In addition, the study of optical emission phenomena using fluorescence spectrophotometers is seldom implemented in educational laboratories due to the practical challenges and costs of the devices, which severely limit pedagogic access to this topic. For students to be more confident with these two basic spectroscopy techniques, we have developed a laboratory kit that provides a multifaceted learning experience. Starting with a basic exploration of an instrument assembly, it teaches, for example, such technical concepts as spectral resolution and detection sensitivity. More fundamentally, it enables deeper learning of the Beer–Lambert law and the notion of Stokes shift. The spectrophotometer is built from cost-efficient materials and is easily scalable, making it affordable for many educational laboratories. Due to a modular design, it is adaptable to various levels of education and has been successfully applied during high school-, undergraduate-, and graduate-level classes.

The generation and characterization of ultrashort laser pulses in the deep ultraviolet spectral region is challenging, especially at high pulse repetition rates and low pulse energies. Here, we combine achromatic second harmonic generation and adaptive pulse compression for the efficient generation of sub-10 fs deep ultraviolet laser pulses at a laser repetition rate of 200 kHz. Furthermore, we simplify the pulse compression scheme and reach pulse durations of ≈10 fs without the use of adaptive optics. We demonstrate straight-forward tuning from 250 to 320 nm, broad pulse spectra of up to 63 nm width, excellent stability and a high robustness against misalignment. These features make the approach appealing for numerous spectroscopy and imaging applications.

Coherent Raman scattering (CRS) spectroscopy techniques have been widely developed and optimized for different applications in biomedicine and fundamental science. The most utilized CRS technique has been coherent anti-Stokes Raman scattering (CARS), and more recently, stimulated Raman scattering (SRS). Coherent Stokes Raman scattering (CSRS) has been largely ignored mainly because it is often strongly affected by fluorescence, particularly for resonance enhanced measurements.However, in the cases of resonant excitation the information contained in the CSRS signal can be different and complementary to that of CARS. Here we combine the approaches of pulse shaping, interferometric heterodyne detection, 8-step phase cycling and Fourier-transform of time-domain measurements, developed in CARS and 2D electronic spectroscopy communities, to measure resonant CSRS and CARS spectra using a Titanium:sapphire oscillator. The signal is essentially background-free (both fluorescent and non-resonant background signals are suppressed) with high spectral resolution and high sensitivity, and can access low-energy modes down to ~30 cm -1 . We demonstrate the ability to easily select between CSRS and CARS schemes and show an example in which acquisition of both CSRS and CARS spectra allows vibrational modes on the excited electronic state to be distinguished from those on the ground electronic state.

Any ultrafast optical spectroscopy experiment is usually accompanied by the necessary routine of ultrashort-pulse characterization. The majority of pulse characterization approaches solve either a one-dimensional (e.g., via interferometry) or a two-dimensional (e.g., via frequency-resolved measurements) problem. Solution of the two-dimensional pulse-retrieval problem is generally more consistent due to the problem’s over-determined nature. In contrast, the one-dimensional pulse-retrieval problem, unless constraints are added, is impossible to solve unambiguously as ultimately imposed by the fundamental theorem of algebra. In cases where additional constraints are involved, the one-dimensional problem may be possible to solve, however, existing iterative algorithms lack generality, and often stagnate for complicated pulse shapes. Here we use a deep neural network to unambiguously solve a constrained one-dimensional pulse-retrieval problem and show the potential of fast, reliable and complete pulse characterization using interferometric correlation time traces determined by the pulses with partial spectral overlap.

We present an erratum regarding the calculated phase matching bandwidths for achromatic second harmonic generation presented in our paper [Opt. Express 29, 25593 (2021)10.1364/OE.425053].