Nanoscale linear permittivity imaging based on scanning nonlinear dielectric microscopy.

A nanoscale linear permittivity imaging method based on scanning nonlinear dielectric microscopy (SNDM) was developed. The ∂C/∂z-mode SNDM (∂C/∂z-SNDM) technique described herein employs probe-height modulation to suppress disturbances originating from stray capacitance and to improve measurement stability. This method allows local permittivity distributions to be examined with extremely low noise levels (approximately 0.01 aF) by virtue of the highly sensitive probe. A cross-section of a multilayer oxide film was visualized using ∂C/∂z-SNDM as a demonstration, and numerical simulations of the response signals were conducted to gain additional insights. The experimental signal intensities were found to be in a good agreement with the theoretical values, with the exception of the background components, demonstrating that absolute sample permittivity values could be determined. The signal profiles near the boundaries between different dielectrics were calculated using various vibration amplitudes and the boundary transition widths were obtained. The beneficial aspects of higher-harmonic response imaging are discussed herein, taking into account assessments of spatial resolution and quantitation.

Charge gradient microscopy.

Here we present a simple and fast method to reliably image polarization charges using charge gradient microscopy (CGM). We collected the current from the grounded CGM probe while scanning a periodically poled lithium niobate single crystal and single-crystal LiTaO3 thin film on the Cr electrode. We observed current signals at the domains and domain walls originating from the displacement current and the relocation or removal of surface charges, which enabled us to visualize the ferroelectric domains at a scan frequency above 78 Hz over 10 µm. We envision that CGM can be used in high-speed ferroelectric domain imaging and piezoelectric energy-harvesting devices.

Interfacial Charge States in Graphene on SiC Studied by Noncontact Scanning Nonlinear Dielectric Potentiometry.

We investigate pristine and hydrogen-intercalated graphene synthesized on a 4H-SiC(0001) substrate by using noncontact scanning nonlinear dielectric potentiometry (NC-SNDP). Permanent dipole moments are detected at the pristine graphene-SiC interface. These originate from the covalent bonds of carbon atoms of the so-called buffer layer to the substrate. Hydrogen intercalation at the interface eliminates these covalent bonds and the original quasi-(6×6) corrugation, which indicates the conversion of the buffer layer into a second graphene layer by the termination of Si bonds at the interface. NC-SNDP images suggest that a certain portion of the Si dangling bonds remains even after hydrogen intercalation. These bonds are thought to act as charged impurities reducing the carrier mobility in hydrogen-intercalated graphene on SiC.

In-plane distribution of huge local permittivity of KTa1-xNbxO3 estimated from local phase transition temperatures and spatially averaged permittivity.

Potassium tantalate niobate (KTa1-xNbxO3, KTN) single crystals have a very large relative permittivity εr (>104) just above the paraelectric to ferroelectric phase transition temperature (TC). The quadratic electro-optic coefficient and the electro-strictive coefficient are also very large because of their proportionality to εr2. However, the local relative permittivity can easily vary spatially due to the incongruently melting nature of KTN. In this study, we quantitatively estimated the in-plane distribution of the huge local relative permittivity of KTN. First, we measured the spatial distribution of TC using scanning nonlinear dielectric microscopy, then deposited the electrodes and measured the temperature dependence of the spatially averaged permittivity using an LCR meter. Following that, we evaluated the spatial distribution of the huge local permittivity from the combination of the spatial distribution of TC and the spatially averaged permittivity. Finally, we measured the deflection angle of light to confirm the validity of the εr estimation procedure. The maximum error for the estimated permittivity was estimated to be around 3.3%.

Boxcar Averaging Scanning Nonlinear Dielectric Microscopy.

Scanning nonlinear dielectric microscopy (SNDM) is a near-field microwave-based scanning probe microscopy method with a wide variety of applications, especially in the fields of dielectrics and semiconductors. This microscopy method has often been combined with contact-mode atomic force microscopy (AFM) for simultaneous topography imaging and contact force regulation. The combination SNDM with intermittent contact AFM is also beneficial for imaging a sample prone to damage and using a sharp microscopy tip for improving spatial resolution. However, SNDM with intermittent contact AFM can suffer from a lower signal-to-noise (S/N) ratio than that with contact-mode AFM because of the shorter contact time for a given measurement time. In order to improve the S/N ratio, we apply boxcar averaging based signal acquisition suitable for SNDM with intermittent contact AFM. We develop a theory for the S/N ratio of SNDM and experimentally demonstrate the enhancement of the S/N ratio in SNDM combined with peak-force tapping (a trademark of Bruker) AFM. In addition, we apply the proposed method to the carrier concentration distribution imaging of atomically thin van der Waals semiconductors. The proposed method clearly visualizes an anomalous electron doping effect on few-layer Nb-doped MoS2. The proposed method is also applicable to other scanning near-field microwave microscopes combined with peak-force tapping AFM such as scanning microwave impedance microscopy. Our results indicate the possibility of simultaneous nanoscale topographic, electrical, and mechanical imaging even on delicate samples.

Material Design Strategy for Enhancement of Readback Signal Intensity in Ferroelectric Probe Data Storage.

Ferroelectric probe data storage (FPDS) based on scanning nonlinear dielectric microscopy is expected as a next-generation data storage method with its large potential for improvement of the recording density. However, this novel method has a problem of low reading speed. To overcome this problem, a novel ferroelectric recording medium with large nonlinear permittivity is required because this data storage method uses the nonlinear dielectric response induced by small-amplitude ac bias to detect the bit data recorded in the form of polarization direction. Therefore, this article discusses nonlinear permittivity enhancement from the viewpoint of data storage application in the framework of the phenomenological theory. We reveal that the Curie-point control is one of the key techniques in material design for FPDS because nonlinear permittivity increases precipitously as the Curie temperature is approached, as with the linear permittivity and piezoelectric constants. A similar conclusion is also obtained through actual measurements of nonlinear permittivity in LiTaO3 single crystals. On the other hand, we also reveal that there is a tradeoff relationship between nonlinear permittivity and polarization stability. To avoid this undesirable situation in data storage applications, pinning-site control will also be important. We also propose to employ a double-layer structure in the ferroelectric recording media for further improvement.

Carrier distribution imaging using ∂C/∂z-mode scanning nonlinear dielectric microscopy.

Scanning nonlinear dielectric microscopy (SNDM) can be used to visualize the carrier distribution in semiconductors with high sensitivity and spatial resolution. We recently proposed a complementary method named ∂C/∂z-SNDM that avoids the problem of contrast reversal. This paper describes a methodology for calculating the signal intensity in ∂C/∂z-SNDM using examples. For the simulation, the capacitance of a conductive-probe metal/oxide/semiconductor model was calculated and then the response signal for various probe-sample distances was analyzed. The simulation results confirm that the ∂C/∂z-SNDM signal intensity increases monotonically with dopant concentration, avoiding contrast reversal. Moreover, in addition to the fundamental (1ω) signal, higher-harmonic (2ω, 3ω) signals have sufficient intensities to be detected. The results suggest that the detection sensitivity for low dopant concentrations can be improved by conducting the measurement under an appropriate dc bias.

Nanoscale ferroelectric information storage based on scanning nonlinear dielectric microscopy.

An investigation of ultrahigh-density ferroelectric data storage based on scanning nonlinear dielectric microscopy (SNDM) is described. For the purpose of obtaining fundamental knowledge on high-density ferroelectric data storage, several experiments on nanodomain formation in a lithium tantalate (LiTaO3) single crystal were conducted. Through domain engineering, a domain dot array with an areal density of 1.5 Tbit/inch2 was formed on congruent LiTaO3 (CLT). Sub-nanosecond (500 psec) domain switching speed also has been achieved. Next, actual information storage is demonstrated at a density of 1 Tbit/inch2. Finally, it is described that application of a very small dc offset voltage is very effective in accelerating the domain switching speed and in stabilizing the reversed nano-domain dots. Applying this offset application technique, we formed a smallest artificial nano-domain single dot of 5.1 nm in diameter and artificial nano-domain dot-array with a memory density of 10.1 Tbit/inch2 and a bit spacing of 8.0 nm, representing the highest memory density for rewritable data storage reported to date.

Scanning nonlinear magnetic microscopy.

Scanning nonlinear magnetic microscopy (SNMM) is introduced as a new microscopic technique for measurement of the distribution of magnetization. The technique is based on the detection of inductance variation in a magnetic material under application of an external alternating magnetic field. The measured inductance thus reflects the nonlinear magnetic response of the material, giving the nonlinear magnetic permeability (mu(333)) and the direction and magnitude of magnetization. SNMM is demonstrated in application to measurement of the magnetization distribution of a floppy disk.

Novel HDD-type SNDM ferroelectric data storage system aimed at high-speed data transfer with single probe operation.

In this study, several read/write tests were conducted using a novel ferroelectric data storage test system equipped with a spindle motor, targeted at high-speed data transfer using a single probe head. A periodically inverted signal can be read out correctly with a bit rate of 100 kbps using this test system, and 10 Mbps data transfer is also possible during writing operations. The effect of a dc-offset voltage applied to the writing waveform with high-speed probe scanning is discussed. In addition, a novel noncontact probe height control technique was adopted to solve the problem of tip abrasion.

Scanning nonlinear dielectric potentiometry.

Measuring spontaneous polarization and permanent dipoles on surfaces and interfaces on the nanoscale is difficult because the induced electrostatic fields and potentials are often influenced by other phenomena such as the existence of monopole fixed charges, screening charges, and contact potential differences. A method based on tip-sample capacitance detection and bias feedback is proposed which is only sensitive to polarization- or dipole-induced potentials, unlike Kelvin probe force microscopy. The feasibility of this method was demonstrated by simultaneously measuring topography and polarization-induced potentials on a reconstructed Si(111)-(7 × 7) surface with atomic resolution.

Nano-domains and related phenomena in congruent lithium tantalate single crystals studied by scanning nonlinear dielectric microscopy.

Nanodomains and their related phenomena in congruent lithium tantalate (CLT) single crystals are studied using scanning nonlinear dielectric microscopy (SNDM). We carried out two specific investigations: super higher order nonlinear dielectric spectroscopy studies on thick multi-domain congruent CLT single crystals and electrical conduction in nanodomains in thin CLT single crystals. First, without using a special sharp tip, we achieve improved lateral resolution in SNDM through the measurement of super higher order nonlinearity up to the fourth order. We also found a marked enhancement of nonlinear dielectric constants when the applied tip-sample voltage exceeded a particular threshold value. This is due to domain nucleation activated by a huge electric field under the tip. Low frequencies (less than a few hundred hertz) do not enhance nonlinearity. An effectively lower electric field caused by ion conduction in the sample under the tip is a possible reason for the frequency-dependent characteristics of the enhanced nonlinearity for the applied voltage. Finally, electrical current flow behavior was investigated for nanodomains formed in a thin CLT single-crystal plate. When the nanodomains are relatively large, with diameters of about 100 nm, current flow is detected along the domain wall. However, when the nanodomains were about 40 nm or smaller in size, current flowed through the entire nanodomain. Schottky-like rectifying behavior was observed. A clear temperature dependence of the current is found, indicating that the conduction mechanism for nanodomains in CLT may involve thermally activated carrier hopping.

Actual information storage with a recording density of 4 Tbit∕in. in a ferroelectric recording medium.

A new method to achieve real information recording with a density above 1 Tbit∕in.(2) in ferroelectric data storage systems is proposed. In this system, data bits were written in the form of the polarization direction, and the data were read by scanning nonlinear dielectric microscopy technique. The domain-switching characteristics of the virgin and inversely prepolarized media were compared, and the conditions of the pulse voltage for writing were optimized. As a result, actual data containing 64×64 bits were recorded at an areal density of 4 Tbit∕in.(2). The bit error rate was evaluated to be 1.2×10(-2).

Intermittent contact scanning nonlinear dielectric microscopy.

Intermittent contact scanning nonlinear dielectric microscopy (IC-SNDM) was developed as a novel technique for surface topography measurements and observation of domain structures. Domain structures on ferroelectric single crystals were observed with nanoscale resolution using IC-SNDM. The reproducibility of measurements was improved in comparison to a conventional SNDM operated under contact mode, because the tip and/or sample damage are reduced when using intermittent contact mode. The minimum loading force of the probe to provide basic performance was experimentally determined for IC-SNDM.

Atomic dipole moment distribution of Si atoms on a Si111-(7 x 7) surface studied using noncontact scanning nonlinear dielectric microscopy.

A local atomic electric dipole moment distribution of Si atoms on Si(111)-(7 x 7) surface is clearly resolved by using a new technique called noncontact scanning nonlinear dielectric microscopy. The dc-bias voltage dependence of the atomic dipole moment on the Si(111)-(7 x 7) surface is measured. At the weak applied voltage of -0.5 V, a positive dipole moment is detected on the Si adatom sites, whereas a negative dipole moment is observed at the interstitial sites of inter Si adatoms. Moreover, the quantitative dependence of the surface dipole moment as a function of the applied dc voltage is also revealed at a fixed point above the sample surface. This is the first successful demonstration of direct atomic dipole moment observation achieved in the field of capacitance measurement.

Three-dimensional observation of nanoscale ferroelectric domains using scanning nonlinear dielectric microscopy with electric field correction by Kelvin probe force microscopy.

An advanced technique for the measurement of three-dimensional ferroelectric domain structure is described. Scanning nonlinear dielectric microscopy is used to measure the polarization components both perpendicular and parallel to the specimen surface. A nanoscale electric field correction is devised and performed using Kelvin probe force microscopy to allow more precise measurement of the nanoscale polarization component parallel to the specimen surface. Using this electric field correction, three-dimensional imaging of the ferroelectric polarization orientation is demonstrated.

Visualization of charges stored in the floating gate of flash memory by scanning nonlinear dielectric microscopy.

By applying scanning nonlinear dielectric microscopy (SNDM), we succeeded in clarifying that electrons existed in the poly-Si layer of the floating gate of a flash memory. The charge accumulated in the floating gate can be detected by SNDM as a change in the capacitance of the poly-Si (floating gate) by scanning the surface of the SiO(2)-SiN(4)-SiO(2) (ONO) film covering the floating gate. There was a clear black contrast region in the SNDM image of the floating gate area, where electrons were injected. However, no clear contrast appeared in the floating gate where electrons were not injected. We confirmed that SNDM is one of the most useful methods of observing the charge accumulated in flash memory.

Nanodomain manipulation for ultrahigh density ferroelectric data storage.

Nanosized inverted domain dots in ferroelectric materials have potential application in ultrahigh density rewritable data storage systems. Herein, a data storage system is presented based on scanning non-linear dielectric microscopy and a thin film of ferroelectric single-crystal lithium tantalite. Through domain engineering, we succeeded in forming our smallest artificial nanodomain single dot at 5.1 nm diameter and an artificial nanodomain dot array with a memory density of 10.1 Tbit inch(-2) and a bit spacing of 8.0 nm, representing the highest memory density for rewritable data storage reported to date. Subnanosecond (500 ps) domain switching speed has also been achieved. Next, actual information storage with a low bit error and high memory density was performed. A bit error ratio of less than 1 × 10(-4) was achieved at an areal density of 258 Gbit inch(-2). Moreover, actual information storage is demonstrated at a density of 1 Tbit inch(-2).