Mode Kelvin Research Articles

Visualizing and Controlling of Photogenerated Electron-Hole Pair Separation in Monolayer WS2 Nanobubbles under Piezoelectric Field.

The piezoelectric properties of two-dimensional semiconductor nanobubbles present remarkable potential for application in flexible optoelectronic devices, and the piezoelectric field has emerged as an efficacious pathway for both the separation and migration of photogenerated electron-hole pairs, along with inhibition of recombination. However, the comprehension and control of photogenerated carrier dynamics within nanobubbles still remain inadequate. Hence, this study is dedicated to underscore the importance of in situ detection and detailed characterization of photogenerated electron-hole pairs in nanobubbles to enrich understanding and strategic manipulation in two-dimensional semiconductor materials. Utilizing frequency modulation kelvin probe force microscopy (FM-KPFM) and strain gradient distribution techniques, the existence of a piezoelectric field in monolayer WS2 nanobubbles was confirmed. Combining w/o and with illumination FM-KPFM, second-order capacitance gradient technique and in situ nanoscale tip-enhanced photoluminescence characterization techniques, the interrelationships among the piezoelectric effect, interlayer carrier transfer, and the funneling effect for photocarrier dynamics process across various nanobubble sizes were revealed. Notably, for a WS2/graphene bubble height of 15.45 nm, a 0 mV surface potential difference was recorded in the bubble region w/o and with illumination, indicating a mutual offset of piezoelectric effect, interlayer carrier transfer, and the funneling effect. This phenomenon is prevalent in transition metal dichalcogenides materials exhibiting inversion symmetry breaking. The implication of our study is profound for advancing the understanding of the dynamics of photogenerated electron-hole pair in nonuniform strain piezoelectric systems, and offers a reliable framework for the separation and modulation of photogenerated electron-hole pair in flexible optoelectronic devices and photocatalytic applications.

Study of high–low KPFM on a pn-patterned Si surface

Comparative measurements between frequency modulation Kelvin probe force microscopy (FM-KPFM) using low frequency bias voltage and heterodyne FM-KPFM using high frequency bias voltage were performed on the surface potential measurement. A silicon substrate patterned with p- and n-type impurities was used as a quantitative sample. The multi-pass scanning method in the measurements of FM-KPFM and heterodyne FM-KPFM was used to eliminate the effect of the tip–sample distance dependence. The measured surface potentials become lower in the order of the p-type region, n-type region and n+-type region by both FM-KPFM and heterodyne FM-KPFM, which are in good agreement with the order of the work functions of the pn-patterned Si sample. We observed the difference in the surface potentials due to the surface band bending measured by FM-KPFM and heterodyne FM-KPFM. The difference is due to the fact that the charge transfer between the surface and bulk levels may or may not respond to AC bias voltage.

Integrated Tapping Mode Kelvin Probe Force Microscopy with Photoinduced Force Microscopy for Correlative Chemical and Surface Potential Mapping (Small 37/2021)

Integrated Tapping Mode Kelvin Probe Force Microscopy with Photoinduced Force Microscopy for Correlative Chemical and Surface Potential Mapping (Small 37/2021)

Integrated Tapping Mode Kelvin Probe Force Microscopy with Photoinduced Force Microscopy for Correlative Chemical and Surface Potential Mapping.

Kelvin probe force microscopy (KPFM) is a popular technique for mapping the surface potential at the nanoscale through measurement of the Coulombic force between an atomic force microscopy (AFM) tip and sample. The lateral resolution of conventional KPFM variants is limited to between ≈35 and 100nm in ambient conditions due to the long-range nature of the Coulombic force. In this article, a novel way of generating the Coulombic force in tapping mode KPFM without the need for an external AC driving voltage is presented. A field-effect transistor (FET) is used to directly switch the electrical connectivity of the tip and sample on and off periodically. The resulting Coulomb force induced by Fermi level alignment of the tip and sample results in a detectable change of the cantilever oscillation at the FET-switching frequency. The resulting FET-switched KPFM delivers a spatial resolution of ≈25nm and inherits the high operational speed of the AFM tapping mode. Moreover, the FET-switched KPFM is integrated with photoinduced force microscopy (PiFM), enabling simultaneous acquisitions of high spatial resolution chemical distributions and surface potential maps. The integrated FET-switched KPFM with PiFM is expected to facilitate characterizations of nanoscale electrical properties of photoactive materials, semiconductors, and ferroelectric materials.

High-speed digitization of the amplitude and frequency in open-loop sideband frequency-modulation Kelvin probe force microscopy

A more inclusive and detailed measurement of various physical interactions is enabled by the advance of high-speed data digitization. For surface potential characterization, this was demonstrated recently in terms of open-loop amplitude modulation Kelvin probe force microscopy (OL AM-KPFM). Its counterpart, namely open-loop frequency modulation Kelvin probe force microscopy (OL FM-KPFM), is examined here across different materials and under various bias voltages in the form of OL sideband FM-KPFM. In this implementation the changes in the amplitude and resonance frequency of the cantilever were continuously tracked as a conductive AFM probe was modulated by a 2 kHz AC bias voltage around the first eigenmode frequency of the cantilever. The contact potential difference (CPD) between the AFM probe and sample was determined from the time series analysis of the high-speed 4 MHz digitized amplitude and frequency signals of the OL sideband FM-KPFM mode. This interpretation is demonstrated to be superior to the analysis of the parabolic bias dependent response, which is more commonly used to extract the CPD in OL KPFM modes. The measured OL sideband FM-KPFM amplitude and frequency responses are directly related to the electrostatic force and force-gradient between the AFM probe and sample, respectively. As a result, clear distinction was observed for the determined CPD in each of these cases across materials of different surface potentials, with far superior spatial resolution when the force-gradient detection was used. In addition, the CPD values obtained from OL sideband FM-KPFM amplitude and frequency measurements perfectly matched those determined from their closed-loop AM-KPFM and FM-KPFM counterparts, respectively.

Surface potential measurement by heterodyne frequency modulation Kelvin probe force microscopy in MHz range

The chemical and physical processes on surfaces are significantly influenced by the surface potential of materials. When using the frequency modulation Kelvin probe force microscopy (FM-KPFM), which has been widely used for measuring the surface potential distribution with high spatial resolution, it is very difficult to distinguish the surface potential due to the surface state from that due to the bulk state, because the charge transfer between the surface and bulk states occurs at a low-frequency ac bias voltage in the kHz range. Here, we propose a heterodyne FM-KPFM method using a high-frequency ac bias voltage in the MHz range to distinguish the surface and bulk states. This method is based on the heterodyne effect between the mechanical cantilever oscillation and the oscillating electrostatic force. For the first time, we succeeded in achieving the atomic-resolution imaging of the surface potential on an O-rich TiO2(110) surface using the electrostatic interaction in the MHz range. Furthermore, we could measure the upward and downward band bending on the surface at the atomic scale.

Symmetry changes during relaxation process and pulse discharge performance of the BaTiO3-Bi(Mg1/2Ti1/2)O3 ceramic

Lead free relaxor ferroelectrics have attracted continuing interest due to their outstanding and eco-friendly properties. In this paper, dielectric relaxation behavior of the 0.6BaTiO3-0.4Bi(Mg1/2Ti1/2)O3 ceramic (BT-40BMT), which is a typical lead free relaxor ferroelectric, is theoretically and experimentally investigated. At first, the observed dielectric relaxation was quantitatively characterized by a statistical model, indicating that the minority co-related polar nano regions (PNRs) dominate the total polarization. Kinetics of the PNRs were subsequently studied by micro-Raman measurements performed at various temperatures. Here, the relaxation of written domains formed by the piezoresponse force microscopy (PFM) tip-bias induced electric field was also studied, which describes the polarization retention performance of BT-40BMT. The absence of ferroelectric signal contribution in local switching was also confirmed by the contact mode Kelvin PFM technique, indicating the lack of local ferroelectricity. Moreover, the temperature insensitive energy storage property from 293 K to 443 K was obtained. High voltage pulsed discharge behavior was also investigated by using the pulsed current. A power density of 7.9 × 108 W/kg is obtained under a pulsed voltage of 50 kV. Combined with the fast discharge time, the 0.6BaTiO3-0.4Bi(Mg1/2Ti1/2)O3 ceramic is considered as a candidate material for high voltage pulse power applications.

Surface Chemistry Controls Anomalous Ferroelectric Behavior in Lithium Niobate.

Polarization switching in ferroelectric materials underpins a multitude of applications ranging from nonvolatile memories to data storage to ferroelectric lithography. While traditionally considered to be a functionality of the material only, basic theoretical considerations suggest that switching is expected to be intrinsically linked to changes in the electrochemical state of the surface. Hence, the properties and dynamics of the screening charges can affect or control the switching dynamics. Despite being recognized for over 50 years, analysis of these phenomena remained largely speculative. Here, we explore polarization switching on the prototypical LiNbO3 surface using the combination of contact mode Kelvin probe force microscopy and chemical imaging by time-of-flight mass-spectrometry and demonstratepronounced chemical differences between the domains. These studies provide a consistent explanation to the anomalous polarization and surface charge behavior observed in LiNbO3 and point to new opportunities in chemical control of polarization dynamics in thin films and crystals via control of surface chemistry, complementing traditional routes via bulk doping, and substrate-induced strain and tilt systems.

Nanoscale Mapping of the Surface Potential: Multifrequency Modulation Open-Loop Kelvin Probe Force Microscopy

In this letter, a new open-loop amplitude modulation Kelvin probe force microscopy is presented for nanoscale mapping of the surface potential. In this method, measurement of the contact potential difference (CPD) is performed with a normal probe under two electrostatic excitations. One excitation oscillates the probe in its second resonance mode with an amplitude of less than 5 nm and the other nonresonant excitation modulates this oscillation at a frequency much lower than the probe's first resonant frequency. With this approach, the probe-sample CPD can be measured directly from the periodic variations of the modulated amplitude and the phase without feedback control. Nanoscale mapping of the surface potential of the graphene-on-silicon sample shows that the proposed method has comparable performance to the conventional amplitude modulation Kelvin probe force microscopy. Further experimental results demonstrate that the proposed method can accurately map the surface potentials of various conductor, semiconductor and insulator materials.

Exploring Anomalous Polarization Dynamics in Organometallic Halide Perovskites.

Organometallic halide perovskites (OMHPs) have attracted broad attention as prospective materials for optoelectronic applications. Among the many anomalous properties of these materials, of special interest are the ferroelectric properties including both classical and relaxor-like components, as a potential origin of slow dynamics, field enhancement, and anomalous mobilities. Here, ferroelectric properties of the three representative OMHPs are explored, including FAPbx Sn1-x I3 (x = 0, x = 0.85) and FA0.85 MA0.15 PbI3 using band excitation piezoresponse force microscopy and contact mode Kelvin probe force microscopy, providing insight into long- and short-range dipole and charge dynamics in these materials and probing ferroelectric density of states. Furthermore, second-harmonic generation in thin films of OMHPs is observed, providing a direct information on the noncentrosymmetric polarization in such materials. Overall, the data provide strong evidence for the presence of ferroelectric domains in these systems; however, the domain dynamics is suppressed by fast ion dynamics. These materials hence present the limit of ferroelectric materials with spontaneous polarization dynamically screened by ionic and electronic carriers.

Decoding Apparent Ferroelectricity in Perovskite Nanofibers.

Ferroelectric perovskites are an important group of materials underpinning a wide variety of devices ranging from sensors and transducers to nonvolatile memories and photovoltaic cells. Despite the progress in material synthesis, ferroelectric characterization of nanoscale perovskites is still a challenge. Piezoresponse force microscopy (PFM) is one of the most popular tools for probing and manipulating nanostructures to study the ferroelectric properties. However, the interpretation of hysteresis data and alternate signal origins are critical. Here, we use a family of scanning probe microscopy (SPM) techniques to systematically investigate the ferroelectric behavior of electrospun potassium niobate (KNbO3) nanofibers. Band Excitation (BE) SPM scans reveal that PFM signals are dominated by changes in resonant frequency due to rough nanofiber surfaces, rather than the actual local piezoelectric strength. We investigate the bias-induced charge injection properties and electrostatic interactions on the PFM response of the nanofiber using contact mode Kelvin probe force microscopy (cKPFM). Furthermore, the impact of relative humidity on the KNbO3 nanofiber's piezoresponse, switching behavior, and tip-induced charges are explored. The resultant data from BE scans were utilized to estimate the piezoelectric constants of the KNO nanofiber. These observations will provide clarity in studying newly developed ferroelectric nanostructures and unambiguously interpreting the PFM data.

Effect of dopant density on contact potential difference across n-type GaAs homojunctions using Kelvin Probe Force Microscopy

In this study, cross-sectional surface potential imaging of n+/semi-insulating GaAs junctions is investigated by using amplitude mode kelvin probe force microscopy. The measurements have shown two different potential profiles, related to the difference in surface potential between the semi-insulating (SI) substrate and the epilayers. It is shown that the contact potential difference (CPD) between the tip and the sample is higher on the semi-insulating substrate side than on the n-type epilayer side. This change in CPD across the interface has been explained by means of energy band diagrams indicating the relative Fermi level positions. In addition, it has also been found that the CPD values across the interface are much smaller than the calculated values (on average about 25% of the theoretical values) and increase with the electron density. Therefore, the results presented in study are only in qualitative agreement with the theory.

Impacts of Indonesian Throughflow on seasonal circulation in the equatorial Indian Ocean

Impacts of the Indonesian Throughflow (ITF) on seasonal circulation in the equatorial eastern Indian Ocean are investigated using the ocean-only model LICOM by opening and closing ITF passages. LICOM had daily forcing from NCEP reanalysis data during 2000-2011. It can reproduce vertical profiles of mean density and buoyancy frequency of World Ocean Atlas 2013 data. The model also simulates well annual oscillation in the central Indian Ocean and semiannual oscillation in the eastern Indian Ocean of sea level anomalies (SLA) using satellite altimeter data, as well as the semiannual oscillation of surface zonal equatorial currents of Ocean Surface Current Analyses Real Time current data in the equatorial Indian Ocean. The wave decomposition method is used to analyze the propagation and reflection of equatorial long waves based on LICOM output. Wave analysis suggests that ITF blockage mainly influences waves generated from the Indian Ocean but not the Pacific Ocean, and eastern boundary reflections play an important role in semiannual oscillations of SLA and zonal current differences in the equatorial Indian Ocean associated with ITF. Reconstructed ITF-caused SLA using wave decomposition coefficient differences between closed and open ITF-passage experiments suggest both Kelvin and Rossby waves from the first baroclinic mode have comparable contributions to the semiannual oscillations of SLA difference. However, reconstructed ITF-caused surface zonal currents at the equator suggest that the first meridional-mode Rossby wave has much greater contribution than the first baroclinic mode Kelvin wave. Both reconstructed sea level and zonal currents demonstrate that the first baroclinic mode has a greater contribution than other baroclinic modes.

Fine structures of organic photovoltaic thin films probed by frequency-shift electrostatic force microscopy

The localized charge and electrostatic properties of organic photovoltaic thin films are predominating factors for controlling energy conversion efficiency. The surface potential and electrostatic structures of organic photovoltaic thin films were investigated by frequency shift mode Kelvin force microscopy (KFM) and electrostatic force microscopy (EFM). The KFM images of a poly[2-methoxy-5-(3′,7′-dimethyloctyloxy)-1,4-phenylene vinylene]/phenyl-C61-butyric-acid-methyl ester (PCBM) blend thin film reveals that the PCBM domains precipitate as the topmost layer on the thin films. We find fine structures that were not observed in the topography and KFM images. The bias dependence of the EFM images suggests that the EFM contrast reflects the field-induced polarization, indicating the presence of charge trapping sites.

Exploring local electrostatic effects with scanning probe microscopy: implications for piezoresponse force microscopy and triboelectricity.

The implementation of contact mode Kelvin probe force microscopy (cKPFM) utilizes the electrostatic interactions between tip and sample when the tip and sample are in contact with each other. Surprisingly, the electrostatic forces in contact are large enough to be measured even with tips as stiff as 4.5 N/m. As for traditional noncontact KPFM, the signal depends strongly on electrical properties of the sample, such as the dielectric constant, and the tip properties, such as the stiffness. Since the tip is in contact with the sample, bias-induced changes in the junction potential between tip and sample can be measured with higher lateral and temporal resolution compared to traditional noncontact KPFM. Significant and reproducible variations of tip-surface capacitance are observed and attributed to surface electrochemical phenomena. Observations of significant surface charge states at zero bias and strong hysteretic electromechanical responses at a nonferroelectric surface have significant implications for fields such as triboelectricity and piezoresponse force microscopy.

Noise performance of frequency modulation Kelvin force microscopy

Noise performance of a phase-locked loop (PLL) based frequency modulation Kelvin force microscope (FM-KFM) is assessed. Noise propagation is modeled step by step throughout the setup using both exact closed loop noise gains and an approximation known as “noise gain” from operational amplifier (OpAmp) design that offers the advantage of decoupling the noise performance study from considerations of stability and ideal loop response. The bandwidth can be chosen depending on how much noise is acceptable and it is shown that stability is not an issue up to a limit that will be discussed. With thermal and detector noise as the only sources, both approaches yield PLL frequency noise expressions equal to the theoretical value for self-oscillating circuits and in agreement with measurement, demonstrating that the PLL components neither modify nor contribute noise. Kelvin output noise is then investigated by modeling the surrounding bias feedback loop. A design rule is proposed that allows choosing the AC modulation frequency for optimized sharing of the PLL bandwidth between Kelvin and topography loops. A crossover criterion determines as a function of bandwidth, temperature and probe parameters whether thermal or detector noise is the dominating noise source. Probe merit factors for both cases are then established, suggesting how to tackle noise performance by probe design. Typical merit factors of common probe types are compared. This comprehensive study is an encouraging step toward a more integral performance assessment and a remedy against focusing on single aspects and optimizing around randomly chosen key values.

Potential sensitivities in frequency modulation and heterodyne amplitude modulation Kelvin probe force microscopes

In this paper, the potential sensitivity in Kelvin probe force microscopy (KPFM) was investigated in frequency modulation (FM) and heterodyne amplitude modulation (AM) modes. We showed theoretically that the minimum detectable contact potential difference (CPD) in FM-KPFM is higher than in heterodyne AM-KPFM. We experimentally confirmed that the signal-to-noise ratio in FM-KPFM is lower than that in heterodyne AM-KPFM, which is due to the higher minimum detectable CPD dependence in FM-KPFM. We also compared the corrugations in the local contact potential difference on the surface of Ge (001), which shows atomic resolution in heterodyne AM-KPFM. In contrast, atomic resolution cannot be obtained in FM-KPFM under the same experimental conditions. The higher potential resolution in heterodyne AM-KPFM was attributed to the lower crosstalk and higher potential sensitivity between topographic and potential measurements.

Observed intraseasonal thermocline variability in the Bay of Bengal

The time series of temperature data obtained from moored buoys deployed at 8°N, 12°N, and 15°N along 90°E in the Bay of Bengal (BoB) shows a persistent intraseasonal variability on 30-120 day time scale in three distinct periods 30-70 day, near 90 day, and near 120 day in the thermocline region. The standard deviation of moored buoy temperature data shows that half of the variability in the thermocline region is contributed from the 30-120 day variability. The relative contribution of local Ekman pumping velocity and remote wind forcing from equatorial Indian Ocean (EIO) to the intraseasonal thermocline variability in the BoB is examined using satellite-derived sea surface height anomaly (SSHA), wind and depths of 23° isotherm (D23, proxy for thermocline depth) derived from moored buoys temperature data. The analysis shows that large amplitude intraseasonal oscillations of thermocline - particularly the near 90 day and 120 day variability - could not be explained by local Ekman pumping velocity alone. The SSHA, D23, and wind fields reveal that the first and second baroclinic mode Kelvin and Rossby waves, which are generated remotely by winds from the EIO and eastern BoB, can significantly influence the thermocline variability in the BoB. The near 90 day and 120 day thermocline variability is driven primarily by the variability of equatorial zonal wind stress. While the 30-70 day thermocline variability is affected most by interior Ekman pumping over the Bay, it also appears to be influenced by zonal wind stress in the EIO and alongshore wind stress in the eastern BoB.

A design of a two-dimensional, supersonic KH experiment on OMEGA-EP

An experiment meant to investigate the evolution of single mode Kelvin–Helmholtz (KH) instability in the supersonic regime is presented and theoretically analyzed. This experiment is intended to provide a direct measurement of the two-dimensional vortex evolution so that the high-Mach-number effects can be measured. The proposed design takes advantage of the ability of OMEGA-EP to drive experiments for up to 30 ns to produce steady conditions for KH that endure long enough to observe substantial growth. KH growth for the proposed design has been analyzed using two-dimensional numerical simulations. The results were compared to synthetic temporal KH numerical simulations using non-dimensional scaling in the low and high Mach number regime. The comparisons show that the growth in the high Mach number regime is expected to be suppressed by up to a factor of two. The effects of two-dimensional rarefactions from the lateral boundaries of the experimental system were also investigated. It was found that they introduce no major uncertainties or hazards to the experiment. We produced simulated radiographs, which show that the proposed experimental system will enable observation of the KH structures. An experiment of this kind has not yet been performed, and therefore would serve to validate numerical results and analytical models presented here and in the literature.

The dynamics of wind‐driven intraseasonal variability in the equatorial Indian Ocean

Variability in the equatorial Indian Ocean on intraseasonal time scales (defined as periods of 30–110 days) is investigated using satellite and in situ observations and a simple analytical linear long‐wave equatorial β‐plane model. Despite the extreme simplicity of the model, which includes just the two gravest baroclinic mode Kelvin waves and first meridional mode Rossby waves, simulated surface zonal velocity and sea surface height compare very well with observations. Both observations and model are characterized by a red shift in the velocity spectrum relative to the wind forcing spectrum, which is attributable to a combination of factors, including (1) the near resonant excitation of Kelvin waves by eastward propagating winds, (2) constructive interference between wind‐forced waves and Rossby waves reflected from the eastern boundary, and (3) the favored excitation of low‐frequency waves whose zonal wavelengths are long compared to the zonal fetch of the wind. We decomposed variability in two broad period bands, namely, 30–70 days and 70–110 days, for detailed analysis. At periods of 30–70 days, zonal velocity tends to be stationary in the directly forced region along the equator owing to the competing contributions of Kelvin and Rossby waves. In contrast, at 70–110 day periods, zonal velocity propagates westward despite eastward propagation of zonal wind stress because of the combined influence of eastern boundary generated and wind‐forced Rossby waves. Kelvin waves reflected from the western boundary are negligibly small, indicating that basin mode resonances are not prominent as has been previously suggested.