Monitoring the low doping regime in graphene using Raman 2D peak-splits: Comparison of gated Raman and transport measurements

Avoiding charge density fluctuations and impurities in graphene is vital for high-quality graphene-based devices. Traditional characterization methods require device fabrication and electrical transport measurements, which are labor-intensive and time-consuming. Existing optical methods using Raman spectroscopy only work for doping levels higher than ~10^12 cm^-2. Here, we propose an optical method using Raman 2D peak-splitting (split between the Raman 2D1 and 2D2 peaks at low doping levels). Electrostatically gated Raman measurements combined with transport measurements were used to correlate the 2D peak-split with the charge density on graphene with high precision (2x10^10 cm^-2 per 2D peak-split wavenumber). We found that the Raman 2D peak-split has a strong correlation with the charge density at low doping levels, and that a lower charge density results in a larger 2D peak-split. Our work provides a simple and non-invasive optical method to quantify the doping level of graphene from 10^10 cm^-2 to 10^12 cm^-2, two orders of magnitude higher precision than previously reported optical methods. This method provides a platform for estimating the doping level and quality of graphene before fabricating graphene deviceshttps://arxiv.org/abs/1908.10961First author draf

A simple KPFM-based approach for electrostatic-free topographic measurements: the case of MoS2_2 on SiO2_2

A simple implementation of Kelvin probe force microscopy is reported that enables recording topographic images in the absence of any component of the electrostatic force. Our approach is based on a close loop z-spectroscopy operated in data cube mode. Curves of the tip-sample distance as a function of time are recorded onto a 2D grid. A dedicated circuit holds the KPFM compensation bias and subsequently cut off the modulation voltage during well-defined time-windows within the spectroscopic acquisition. Topographic images are recalculated from the matrix of spectroscopic curves. This approach is applied to the case of transition metal dichalcogenides (TMD) monolayers grown by chemical vapour deposition on silicon oxide substrates. In addition, we check to what extent a proper stacking height estimation can also be performed by recording series of images for decreasing values of the bias modulation amplitude. The outputs of both approaches are shown to be fully consistent. The results exemplify how in the operating conditions of non-contact AFM under ultra-high vacuum, the stacking height values can dramatically be overestimated due to variations in the tip-surface capacitive gradient, even though the KPFM controller nullifies the potential difference. We show that the number of atomic layers of a TMD can be safely assessed, only if the KPFM measurement is performed with a modulated bias amplitude reduced at its strict minimum or, even better, without any modulated bias. Last, the spectroscopic data reveal that defects at the TMD/oxide interface can have a counterintuitive impact on the electrostatic landscape, resulting in an apparent decrease of the measured stacking height by conventional nc-AFM/KPFM compared to non-defective sample areas. Hence, electrostatic free z-imaging proves to be a promising tool to assess the existence of defects in atomically thin TMD layers grown on oxide

Characterizing optical and electrical properties of monolayer MoS2 by backside absorbing layer microscopy

Nanomaterials are playing an increasing role in novel technologies, and it is important to develop optical methods to characterize them in situ.  To that end, backside absorbing layer microscopy (BALM) has emerged as a powerful tool, being capable to resolve sub-nanometer height profiles, with video-rate acquisition speeds and a suitable geometry to couple live experiments.  In the internship, several techniques involving BALM were developed, and applied to study optical and electrical properties of the transition metal dichalcogenide (TMD) monolayer MoS2, a type of 2-dimensional (2D) crystalline semiconductor.  A simulations toolkit was created in MATLAB to model BALM, a workflow to reliably extract linear intensities from the CMOS detector was realized, and 2D MoS2 was synthesized by chemical vapor deposition followed by transfer to appropriate substrates.  BALM data of the 2D MoS2 was acquired and combined with simulations, giving a preliminary result for its complex refractive index at 5 optical wavelengths.  In addition, the first steps towards coupling BALM with a gate biased 2D MoS2 field-effect transistor were explored.  To complement BALM measurements, the grown samples were also characterized by conventional optical microscopy, scanning electron microscopy, atomic force microscopy, photoluminescence spectroscopy, and Raman spectroscopy.  This work provides new additions to an existing platform of BALM techniques, enabling novel BALM experiments with nanomaterial systems.  In particular, it introduces a new alternative for local extraction of optical parameters and for probing of electrical charging effects, both of which are vital in the research and development of nano-optoelectronics

Field-effect transistor based biosensing of glucose using carbon nanotubes and monolayer MoS2

As part of the EU SmartVista project to develop a multi-modal wearable sensor for health diagnostics, field-effect transistor (FET) based biosensors were explored, with glucose as the analyte, and carbon nanotubes (CNTs) or monolayer MoS2 as the semiconducting sensing layer.  Numerous arrays of CNT-FETs and MoS2-FETs were fabricated by photolithographic methods and packaged as integrated circuits.  Functionalization of the sensing layer using linkers and enzymes was performed, and the samples were characterized by atomic force microscopy, scanning electron microscopy, optical microscopy, and electrical measurements. ON/OFF ratios of 102 p-type and < 102 n-type were acheived, respectively, and the work helped survey the viability of realizing such sensors in a wearable device.EU Horizon 2020 - SmartVista (825114

Field-effect transistor based biosensing of glucose using carbon nanotubes and monolayer MoS2

As part of the EU SmartVista project to develop a multi-modal wearable sensor for health diagnostics, field-effect transistor (FET) based biosensors were explored, with glucose as the analyte, and carbon nanotubes (CNTs) or monolayer MoS2 as the semiconducting sensing layer.  Numerous arrays of CNT-FETs and MoS2-FETs were fabricated by photolithographic methods and packaged as integrated circuits.  Functionalization of the sensing layer using linkers and enzymes was performed, and the samples were characterized by atomic force microscopy, scanning electron microscopy, optical microscopy, and electrical measurements. ON/OFF ratios of 102 p-type and < 102 n-type were acheived, respectively, and the work helped survey the viability of realizing such sensors in a wearable device.EU Horizon 2020 - SmartVista (825114

Characterizing optical and electrical properties of monolayer MoS2 by backside absorbing layer microscopy

Nanomaterials are playing an increasing role in novel technologies, and it is important to develop optical methods to characterize them in situ.  To that end, backside absorbing layer microscopy (BALM) has emerged as a powerful tool, being capable to resolve sub-nanometer height profiles, with video-rate acquisition speeds and a suitable geometry to couple live experiments.  In the internship, several techniques involving BALM were developed, and applied to study optical and electrical properties of the transition metal dichalcogenide (TMD) monolayer MoS2, a type of 2-dimensional (2D) crystalline semiconductor.  A simulations toolkit was created in MATLAB to model BALM, a workflow to reliably extract linear intensities from the CMOS detector was realized, and 2D MoS2 was synthesized by chemical vapor deposition followed by transfer to appropriate substrates.  BALM data of the 2D MoS2 was acquired and combined with simulations, giving a preliminary result for its complex refractive index at 5 optical wavelengths.  In addition, the first steps towards coupling BALM with a gate biased 2D MoS2 field-effect transistor were explored.  To complement BALM measurements, the grown samples were also characterized by conventional optical microscopy, scanning electron microscopy, atomic force microscopy, photoluminescence spectroscopy, and Raman spectroscopy.  This work provides new additions to an existing platform of BALM techniques, enabling novel BALM experiments with nanomaterial systems.  In particular, it introduces a new alternative for local extraction of optical parameters and for probing of electrical charging effects, both of which are vital in the research and development of nano-optoelectronics

A simple KPFM-based approach for electrostaticfree topographic measurements: the case of MoS2_2 on SiO2_2

A simple implementation of Kelvin probe force microscopy is reported that enables recording topographic images in the absence of any component of the electrostatic force. Our approach is based on a close loop z-spectroscopy operated in data cube mode. Curves of the tip-sample distance as a function of time are recorded onto a 2D grid. A dedicated circuit holds the KPFM compensation bias and subsequently cut off the modulation voltage during well-defined time-windows within the spectroscopic acquisition. Topographic images are recalculated from the matrix of spectroscopic curves. This approach is applied to the case of transition metal dichalcogenides (TMD) monolayers grown by chemical vapour deposition on silicon oxide substrates. In addition, we check to what extent a proper stacking height estimation can also be performed by recording series of images for decreasing values of the bias modulation amplitude. The outputs of both approaches are shown to be fully consistent. The results exemplify how in the operating conditions of non-contact AFM under ultra-high vacuum, the stacking height values can dramatically be overestimated due to variations in the tip-surface capacitive gradient, even though the KPFM controller nullifies the potential difference. We show that the number of atomic layers of a TMD can be safely assessed, only if the KPFM measurement is performed with a modulated bias amplitude reduced at its strict minimum or, even better, without any modulated bias. Last, the spectroscopic data reveal that defects at the TMD/oxide interface can have a counterintuitive impact on the electrostatic landscape, resulting in an apparent decrease of the measured stacking height by conventional nc-AFM/KPFM compared to non-defective sample areas. Hence, electrostatic free z-imaging proves to be a promising tool to assess the existence of defects in atomically thin TMD layers grown on oxide

A simple KPFM-based approach for electrostaticfree topographic measurements: the case of MoS2 on SiO2

A simple implementation of Kelvin probe force microscopy is reported that enables recording topographic images in the absence of any component of the electrostatic force. Our approach is based on a close loop z-spectroscopy operated in data cube mode. Curves of the tip-sample distance as a function of time are recorded onto a 2D grid. A dedicated circuit holds the KPFM compensation bias and subsequently cut off the modulation voltage during well-defined time-windows within the spectroscopic acquisition. Topographic images are recalculated from the matrix of spectroscopic curves. This approach is applied to the case of transition metal dichalcogenides (TMD) monolayers grown by chemical vapour deposition on silicon oxide substrates. In addition, we check to what extent a proper stacking height estimation can also be performed by recording series of images for decreasing values of the bias modulation amplitude. The outputs of both approaches are shown to be fully consistent. The results exemplify how in the operating conditions of non-contact AFM under ultra-high vacuum, the stacking height values can dramatically be overestimated due to variations in the tip-surface capacitive gradient, even though the KPFM controller nullifies the potential difference. We show that the number of atomic layers of a TMD can be safely assessed, only if the KPFM measurement is performed with a modulated bias amplitude reduced at its strict minimum or, even better, without any modulated bias. Last, the spectroscopic data reveal that defects at the TMD/oxide interface can have a counterintuitive impact on the electrostatic landscape, resulting in an apparent decrease of the measured stacking height by conventional nc-AFM/KPFM compared to non-defective sample areas. Hence, electrostatic free z-imaging proves to be a promising tool to assess the existence of defects in atomically thin TMD layers grown on oxide

A simple KPFM-based approach for electrostaticfree topographic measurements: the case of MoS2 on SiO2

A simple implementation of Kelvin probe force microscopy is reported that enables recording topographic images in the absence of any component of the electrostatic force. Our approach is based on a close loop z-spectroscopy operated in data cube mode. Curves of the tip-sample distance as a function of time are recorded onto a 2D grid. A dedicated circuit holds the KPFM compensation bias and subsequently cut off the modulation voltage during well-defined time-windows within the spectroscopic acquisition. Topographic images are recalculated from the matrix of spectroscopic curves. This approach is applied to the case of transition metal dichalcogenides (TMD) monolayers grown by chemical vapour deposition on silicon oxide substrates. In addition, we check to what extent a proper stacking height estimation can also be performed by recording series of images for decreasing values of the bias modulation amplitude. The outputs of both approaches are shown to be fully consistent. The results exemplify how in the operating conditions of non-contact AFM under ultra-high vacuum, the stacking height values can dramatically be overestimated due to variations in the tip-surface capacitive gradient, even though the KPFM controller nullifies the potential difference. We show that the number of atomic layers of a TMD can be safely assessed, only if the KPFM measurement is performed with a modulated bias amplitude reduced at its strict minimum or, even better, without any modulated bias. Last, the spectroscopic data reveal that defects at the TMD/oxide interface can have a counterintuitive impact on the electrostatic landscape, resulting in an apparent decrease of the measured stacking height by conventional nc-AFM/KPFM compared to non-defective sample areas. Hence, electrostatic free z-imaging proves to be a promising tool to assess the existence of defects in atomically thin TMD layers grown on oxide