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

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

Dual-heterodyne Kelvin probe force microscopy

International audienceWe present a new open-loop implementation of Kelvin probe force microscopy (KPFM) that provides access to the Fourier spectrum of the time-periodic surface electrostatic potential generated under optical (or electrical) pumping with an atomic force microscope. The modulus and phase coefficients are probed by exploiting a double heterodyne frequency mixing effect between the mechanical oscillation of the cantilever, modulated components of the time-periodic electrostatic potential at harmonic frequencies of the pump, and an ac bias modulation signal. Each harmonic can be selectively transferred to the second cantilever eigenmode. We show how phase coherent sideband generation and signal demodulation at the second eigenmode can be achieved by using two numerical lock-in amplifiers configured in cascade. Dual-heterodyne KPFM (DHe-KPFM) can be used to map any harmonic (amplitude/phase) of the time-periodic surface potential at a standard scanning speed. The Fourier spectrum (series of harmonics) can also be recorded in spectroscopic mode (DHe-KPFM spectroscopy), and 2D dynamic images can be acquired in data cube mode. The capabilities of DHe-KPFM in terms of time-resolved measurements, surface photovoltage (SPV) imaging, and detection of weak SPV signals are demonstrated through a series of experiments on difference surfaces: a reference substrate, a bulk organic photovoltaic heterojunction thin film, and an optoelectronic interface obtained by depositing caesium lead bromide perovskite nanosheets on a graphite surface. The conclusion provides perspectives for future improvements and applications

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

Numerical analysis of single-point spectroscopy curves used in photo-carrier dynamics measurements by Kelvin probe force microscopy under frequency-modulated excitation

In recent years, the investigation of the complex interplay between the nanostructure and photo-transport mechanisms has become of crucial importance for the development of many emerging photovoltaic technologies. In this context, Kelvin probe force microscopy under frequency-modulated excitation has emerged as a useful technique for probing photo-carrier dynamics and gaining access to carrier lifetime at the nanoscale in a wide range of photovoltaic materials. However, some aspects about the data interpretation of techniques based on this approach are still the subject of debate, for example, the plausible presence of capacitance artifacts. Special attention shall also be given to the mathematical model used in the data-fitting process as it constitutes a determining aspect in the calculation of time constants. Here, we propose and demonstrate an automatic numerical simulation routine that enables to predict the behavior of spectroscopy curves of the average surface photovoltage as a function of a frequency-modulated excitation source in photovoltaic materials, enabling to compare simulations and experimental results. We describe the general aspects of this simulation routine and we compare it against experimental results previously obtained using single-point Kelvin probe force microscopy under frequency-modulated excitation over a silicon nanocrystal solar cell, as well as against results obtained by intensity-modulated scanning Kelvin probe microscopy over a polymer/fullerene bulk heterojunction device. Moreover, we show how this simulation routine can complement experimental results as additional information about the photo-carrier dynamics of the sample can be gained via the numerical analysis

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

Multimodal noncontact atomic force microscopy and Kelvin probe force microscopy investigations of organolead tribromide perovskite single crystals

In this work, methylammonium lead tribromide (MAPbBr3) single crystals are studied by noncontact atomic force microscopy (nc-AFM) and Kelvin probe force microscopy (KPFM). We demonstrate that the surface photovoltage and crystal photostriction can be simultaneously investigated by implementing a specific protocol based on the acquisition of the tip height and surface potential during illumination sequences. The obtained data confirm the existence of lattice expansion under illumination in MAPbBr3 and that negative photocarriers accumulate near the crystal surface due to band bending effects. Time-dependent changes of the surface potential occurring under illumination on the scale of a few seconds reveal the existence of slow ion-migration mechanisms. Lastly, photopotential decay at the sub-millisecond time scale related to the photocarrier lifetime is quantified by performing KPFM measurements under frequency-modulated illumination. Our multimodal approach provides a unique way to investigate the interplay between the charges and ionic species, the photocarrier-lattice coupling and the photocarrier dynamics in hybrid perovskites

Hidden surface photovoltages revealed by pump probe KPFM

32 pages, 9 figures, supporting information (5 SI figures), submitted for publicationIn this work, we use pump-probe Kelvin Probe Force Microscopy (pp-KPFM) to investigate light-induced surface potential dynamics in alumina-passivated crystalline silicon, and in an organic bulk heterojunction thin film based on the PTB7-PC71BM tandem. In both cases, we demonstrate that it is possible to identify and separate the contributions of two different kinds of photo-induced charge distributions that give rise to potential shifts with opposite polarities, each characterized by different dynamics. The data acquired on the passivated crystalline silicon are shown to be fully consistent with the band-bending at the silicon-oxide interface, and with electron trapping processes in acceptors states and in the passivation layer. The full sequence of events that follow the electron-hole generation can be observed on the pp-KPFM curves. Two dimensional dynamical maps of the organic blend photo-response are obtained by recording the pump-probe KPFM curves in data cube mode, and by implementing a specific batch processing protocol. Sample areas displaying an extra positive SPV component characterized by decay time-constants of a few tens of microseconds are thus revealed, and are tentatively attributed to specific interfaces formed between a polymer-enriched skin layer and recessed acceptor aggregates. Decay time constant images of the negative SPV component confirm that the acceptor clusters act as electron-trapping centres. Whatever the photovoltaic technology, our results exemplify how some of the SPV components may remain completely hidden to conventional SPV imaging by KPFM, with possible consequences in terms of photo-response misinterpretation. This work furthermore highlight the need of implementing time-resolved techniques that can provide a quantitative measurement of the time-resolved potential

Hidden surface photovoltages revealed by pump probe KPFM

32 pages, 9 figures, supporting information (5 SI figures), submitted for publicationIn this work, we use pump-probe Kelvin Probe Force Microscopy (pp-KPFM) to investigate light-induced surface potential dynamics in alumina-passivated crystalline silicon, and in an organic bulk heterojunction thin film based on the PTB7-PC71BM tandem. In both cases, we demonstrate that it is possible to identify and separate the contributions of two different kinds of photo-induced charge distributions that give rise to potential shifts with opposite polarities, each characterized by different dynamics. The data acquired on the passivated crystalline silicon are shown to be fully consistent with the band-bending at the silicon-oxide interface, and with electron trapping processes in acceptors states and in the passivation layer. The full sequence of events that follow the electron-hole generation can be observed on the pp-KPFM curves. Two dimensional dynamical maps of the organic blend photo-response are obtained by recording the pump-probe KPFM curves in data cube mode, and by implementing a specific batch processing protocol. Sample areas displaying an extra positive SPV component characterized by decay time-constants of a few tens of microseconds are thus revealed, and are tentatively attributed to specific interfaces formed between a polymer-enriched skin layer and recessed acceptor aggregates. Decay time constant images of the negative SPV component confirm that the acceptor clusters act as electron-trapping centres. Whatever the photovoltaic technology, our results exemplify how some of the SPV components may remain completely hidden to conventional SPV imaging by KPFM, with possible consequences in terms of photo-response misinterpretation. This work furthermore highlight the need of implementing time-resolved techniques that can provide a quantitative measurement of the time-resolved potential