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Raman spectroscopy's capability to provide meaningful composition predictions is heavily reliant on a pre-processing step to remove insignificant spectral variation. This is crucial in biofluid analysis. Widespread adoption of diagnostics using Raman requires a robust model which can withstand routine spectra discrepancies due to unavoidable variations such as age, diet, and medical background. A wealth of pre-processing methods are available, and it is often up to trial-and-error or user experience to select the method which gives the best results. This process can be incredibly time consuming and inconsistent for multiple operators. In this study we detail a method to analyze the statistical variability within a set of training spectra and determine suitability to form a robust model. This allows us to selectively qualify or exclude a pre-processing method, predetermine robustness, and simultaneously identify the number of components which will form the best predictive model. We demonstrate the ability of this technique to improve predictive models of two artificial biological fluids. Raman spectroscopy is ideal for noninvasive, nondestructive analysis. Routine health monitoring which maximizes comfort is increasingly crucial, particularly in epidemic-level diabetes diagnoses. High variability in spectra of biological samples can hinder Raman's adoption for these methods. Our technique allows the decision of optimal pre-treatment method to be determined for the operator; model performance is no longer a function of user experience. We foresee this statistical technique being an instrumental element to widening the adoption of Raman as a monitoring tool in a field of biofluid analysis.

While silicon nanocrystals (ncSi) embedded in silicon dioxide thin films have been intensively studied in physics, the potential of batch synthesis of silicon nanocrystals from the solid-state disproportionation of SiO powder has not drawn much attention in chemistry. Herein we describe some remarkable effects observed in the diffraction, microscopy and spectroscopy of SiO powder upon thermal processing in the temperature range 850-1100 °C. Quantum confinement effects and structural changes of the material related to the size of the silicon nanocrystals nucleated and grown in this way were established by Photoluminescence (PL), Raman, FTIR and UV-Visible spectroscopy, PXRD and STEM, pinpointing that the most significant disproportionation transformations happened in the temperature range between 900 and 950 °C. With this know-how a high yield synthesis was developed that produced polydispersions of decyl-capped, hexane-soluble silicon nanocrystals predominantly with near infrared (NIR) PL. Using size-selective precipitation, these polydispersions were separated into monodisperse fractions, which allowed their PL absolute quantum yield (AQY) to be studied as a function of silicon nanocrystal size. This investigation yielded volcano-shaped plots for the AQY confirming the most efficient PL wavelength for ncSi to be located at around 820-830 nm, which corresponded to a size of 3.5-4.0 nm. This work provides opportunities for applications of size-selected near infrared emitting silicon nanocrystals in biomedical imaging and photothermal therapy.

While silicon nanocrystals (ncSi) embedded in silicon dioxide thin films have been intensively studied in physics, the potential of batch synthesis of silicon nanocrystals from the solid-state disproportionation of SiO powder has not drawn much attention in chemistry. Herein we describe some remarkable effects observed in the diffraction, microscopy and spectroscopy of SiO powder upon thermal processing in the temperature range 850-1100 °C. Quantum confinement effects and structural changes of the material related to the size of the silicon nanocrystals nucleated and grown in this way were established by Photoluminescence (PL), Raman, FTIR and UV-Visible spectroscopy, PXRD and STEM, pinpointing that the most significant disproportionation transformations happened in the temperature range between 900 and 950 °C. With this know-how a high yield synthesis was developed that produced polydispersions of decyl-capped, hexane-soluble silicon nanocrystals predominantly with near infrared (NIR) PL. Using size-selective precipitation, these polydispersions were separated into monodisperse fractions, which allowed their PL absolute quantum yield (AQY) to be studied as a function of silicon nanocrystal size. This investigation yielded volcano-shaped plots for the AQY confirming the most efficient PL wavelength for ncSi to be located at around 820-830 nm, which corresponded to a size of 3.5-4.0 nm. This work provides opportunities for applications of size-selected near infrared emitting silicon nanocrystals in biomedical imaging and photothermal therapy.

While silicon nanocrystals (ncSi) embedded in silicon dioxide thin films have been intensively studied in physics, the potential of batch synthesis of silicon nanocrystals from the solid-state disproportionation of SiO powder has not drawn much attention in chemistry. Herein we describe some remarkable effects observed in the diffraction, microscopy and spectroscopy of SiO powder upon thermal processing in the temperature range 850-1100 °C. Quantum confinement effects and structural changes of the material related to the size of the silicon nanocrystals nucleated and grown in this way were established by Photoluminescence (PL), Raman, FTIR and UV-Visible spectroscopy, PXRD and STEM, pinpointing that the most significant disproportionation transformations happened in the temperature range between 900 and 950 °C. With this know-how a high yield synthesis was developed that produced polydispersions of decyl-capped, hexane-soluble silicon nanocrystals predominantly with near infrared (NIR) PL. Using size-selective precipitation, these polydispersions were separated into monodisperse fractions, which allowed their PL absolute quantum yield (AQY) to be studied as a function of silicon nanocrystal size. This investigation yielded volcano-shaped plots for the AQY confirming the most efficient PL wavelength for ncSi to be located at around 820-830 nm, which corresponded to a size of 3.5-4.0 nm. This work provides opportunities for applications of size-selected near infrared emitting silicon nanocrystals in biomedical imaging and photothermal therapy.

While silicon nanocrystals (ncSi) embedded in silicon dioxide thin films have been intensively studied in physics, the potential of batch synthesis of silicon nanocrystals from the solid-state disproportionation of SiO powder has not drawn much attention in chemistry. Herein we describe some remarkable effects observed in the diffraction, microscopy and spectroscopy of SiO powder upon thermal processing in the temperature range 850-1100 °C. Quantum confinement effects and structural changes of the material related to the size of the silicon nanocrystals nucleated and grown in this way were established by Photoluminescence (PL), Raman, FTIR and UV-Visible spectroscopy, PXRD and STEM, pinpointing that the most significant disproportionation transformations happened in the temperature range between 900 and 950 °C. With this know-how a high yield synthesis was developed that produced polydispersions of decyl-capped, hexane-soluble silicon nanocrystals predominantly with near infrared (NIR) PL. Using size-selective precipitation, these polydispersions were separated into monodisperse fractions, which allowed their PL absolute quantum yield (AQY) to be studied as a function of silicon nanocrystal size. This investigation yielded volcano-shaped plots for the AQY confirming the most efficient PL wavelength for ncSi to be located at around 820-830 nm, which corresponded to a size of 3.5-4.0 nm. This work provides opportunities for applications of size-selected near infrared emitting silicon nanocrystals in biomedical imaging and photothermal therapy.

While silicon nanocrystals (ncSi) embedded in silicon dioxide thin films have been intensively studied in physics, the potential of batch synthesis of silicon nanocrystals from the solid-state disproportionation of SiO powder has not drawn much attention in chemistry. Herein we describe some remarkable effects observed in the diffraction, microscopy and spectroscopy of SiO powder upon thermal processing in the temperature range 850-1100 °C. Quantum confinement effects and structural changes of the material related to the size of the silicon nanocrystals nucleated and grown in this way were established by Photoluminescence (PL), Raman, FTIR and UV-Visible spectroscopy, PXRD and STEM, pinpointing that the most significant disproportionation transformations happened in the temperature range between 900 and 950 °C. With this know-how a high yield synthesis was developed that produced polydispersions of decyl-capped, hexane-soluble silicon nanocrystals predominantly with near infrared (NIR) PL. Using size-selective precipitation, these polydispersions were separated into monodisperse fractions, which allowed their PL absolute quantum yield (AQY) to be studied as a function of silicon nanocrystal size. This investigation yielded volcano-shaped plots for the AQY confirming the most efficient PL wavelength for ncSi to be located at around 820-830 nm, which corresponded to a size of 3.5-4.0 nm. This work provides opportunities for applications of size-selected near infrared emitting silicon nanocrystals in biomedical imaging and photothermal therapy.

Creating miniature chip scale implementations of optical quantum information protocols is a dream for many in the quantum optics community. This is largely because of the promise of stability and scalability. Here we present a monolithically integratable chip architecture upon which is built a photonic device primitive called a Bragg reflection waveguide (BRW). Implemented in gallium arsenide, we show that, via the process of spontaneous parametric down conversion, the BRW is capable of directly producing polarization entangled photons without additional path difference compensation, spectral filtering or post-selection. After splitting the twin-photons immediately after they emerge from the chip, we perform a variety of correlation tests on the photon pairs and show non-classical behaviour in their polarization. Combined with the BRW's versatile architecture our results signify the BRW design as a serious contender on which to build large scale implementations of optical quantum processing devices.