Phase-shifting Electron Holography Research Articles

Reconstruction of Angstrom resolution exit-waves by the application of drift-corrected phase-shifting off-axis electron holography

Phase-shifting electron holography is an excellent method to reveal electron wave phase information with very high phase sensitivity over a large range of spatial frequencies. It circumvents the limiting trade-off between fringe spacing and visibility of standard off-axis holography. Previous implementations have been limited by the independent drift of biprism and sample. We demonstrate here an advanced drift correction scheme for the hologram series that exploits the presence of an interface of the TEM specimen to the vacuum area in the hologram. It allows to obtain reliable phase information up to 2π/452 at the 1 Å information limit of the Titan 80–300 kV environmental transmission electron microscope used, by applying a moderate voltage of 250 V to a single biprism for a fringe spacing of 1 Å. The obtained phase and amplitude information is validated at a thin Pt sample by use of multislice image simulation with the frozen lattice approximation and shows excellent agreement. The presented method is applicable in any TEM equipped with at least one electron biprism and thus enables achieving high resolution off-axis holography in various instruments including those for in-situ applications. A software implementation for the acquisition, calibration and reconstruction is provided.

Low-dose measurement of electric potential distribution in organic light-emitting diode by phase-shifting electron holography with 3D tensor decomposition.

To improve the performance of organic light-emitting diodes (OLEDs), it is essential to understand and control the electric potential in the organic semiconductor layers. Electron holography (EH) is a powerful technique for visualizing the potential distribution with a transmission electron microscope. However, it has a serious issue that high-energy electrons may damage the organic layers, meaning that a low-dose EH is required. Here, we used a machine learning technique, three-dimensional (3D) tensor decomposition, to denoise electron interference patterns (holograms) of bilayer OLEDs composed of N,N'-di-[(1-naphthyl)-N,N'-diphenyl]-(1,1'-biphenyl)-4,4'-diamine (α-NPD) and tris-(8-hydroxyquinoline)aluminum (Alq3), acquired under a low-dose rate of 130 e- nm-2 s-1. The effect of denoising on the phase images reconstructed from the holograms was evaluated in terms of both the phase measurement error and the peak signal-to-noise ratio. We achieved a precision equivalent to that of a conventional measurement that had an exposure time 60 times longer. The electric field within the Alq3 layer decreased as the cumulative dose increased, which indicates that the Alq3 layer was degraded by the electron irradiation. On the basis of the degradation of the electric field, we concluded that the tolerance dose without damaging the OLED sample is about 1.7 × 105 e- nm-2, which is about 0.6 times that of the conventional EH. The combination of EH and 3D tensor decomposition denoising is capable of making a time series measurement of an OLED sample without any effect from the electron irradiation.

Visualization of depletion layer in AlGaN homojunction p–n junction

We analyzed the p–n junction of an aluminum gallium nitride (AlGaN) homojunction tunnel junction (TJ) deep-ultraviolet light-emitting diode by phase-shifting electron holography. We clearly obtained a phase image reflecting the band alinement of the p–n homojunction and derived a depletion layer width of approximately 10 nm. In addition, the observed depletion layer width for the AlGaN TJ was in good agreement with the simulated one reflecting the diffusion profile of Mg and Si, thus enabling a discussion on the electrical conduction mechanism for an AlGaN p–n junction.

Direct visualization of electric potential distribution in organic light emitting diode by phase-shifting electron holography

We utilized phase-shifting electron holography on organic light emitting diodes consisting of N,N′-di-[(1-naphthyl)-N,N′-diphenyl]-(1,1′-biphenyl)-4,4′-diamine (α-NPD) and tris-(8-hydroxyquinoline)aluminum (Alq3) layers to visualize their built-in potential distribution. The bilayer showed three different electric fields, namely, the fields in the α-NPD layer, near the α-NPD/Alq3 interface, and in the Alq3 layer measured as −1.8 ± 0.4 MV m−1, −10.0 ± 2 MV m−1, 3.1 ± 0.6 MV m−1, respectively. We show that they are related to hole accumulation in the α-NPD layer, the charge carrier accumulation junction around the α-NPD/Alq3 interface, and the giant surface potential spontaneously polarized in the Alq3 layer.

Phase-shifting electron holography for accurate measurement of potential distributions in organic and inorganic semiconductors.

Phase-shifting electron holography (PS-EH) is an interference transmission electron microscopy technique that accurately visualizes potential distributions in functional materials, such as semiconductors. In this paper, we briefly introduce the features of the PS-EH that overcome some of the issues facing the conventional EH based on Fourier transformation. Then, we present a high-precision PS-EH technique with multiple electron biprisms and a sample preparation technique using a cryo-focused-ion-beam, which are important techniques for the accurate phase measurement of semiconductors. We present several applications of PS-EH to demonstrate the potential in organic and inorganic semiconductors and then discuss the differences by comparing them with previous reports on the conventional EH. We show that in situ biasing PS-EH was able to observe not only electric potential distribution but also electric field and charge density at a GaAs p-n junction and clarify how local band structures, depletion layer widths and space charges changed depending on the biasing conditions. Moreover, the PS-EH clearly visualized the local potential distributions of two-dimensional electron gas layers formed at AlGaN/GaN interfaces with different Al compositions. We also report the results of our PS-EH application for organic electroluminescence multilayers and point out the significant potential changes in the layers. The proposed PS-EH enables more precise phase measurement compared to the conventional EH, and our findings introduced in this paper will contribute to the future research and development of high-performance semiconductor materials and devices.

Accurate Measurement of Electric Potential Distributions at the Interfaces in Solids Using Phase-shifting Electron Holography

Accurate Measurement of Electric Potential Distributions at the Interfaces in Solids Using Phase-shifting Electron Holography

Visualization of different carrier concentrations in n-type-GaN semiconductors by phase-shifting electron holography with multiple electron biprisms.

Phase-shifting electron holography (PS-EH) using a transmission electron microscope (TEM) was applied to visualize layers with different concentrations of carriers activated by Si (at dopant levels of 1019, 1018, 1017 and 1016 atomscm-3) in n-type GaN semiconductors. To precisely measure the reconstructed phase profiles in the GaN sample, three electron biprisms were used to obtain a series of high-contrast holograms without Fresnel fringes generated by a biprism filament, and a cryo-focused-ion-beam (cryo-FIB) was used to prepare a uniform TEM sample with less distortion in the wide field of view. All layers in a 350-nm-thick TEM sample were distinguished with 1.8-nm spatial resolution and 0.02-rad phase-resolution, and variations of step width in the phase profile (corresponding to depletion width) at the interfaces between the layers were also measured. Thicknesses of the active and inactive layers at each dopant level were estimated from the observed phase profile and the simulation of theoretical band structure. Ratio of active-layer thickness to total thickness of the TEM sample significantly decreased as dopant concentration decreased; thus, a thicker TEM sample is necessary to visualize lower carrier concentrations; for example, to distinguish layers with dopant concentrations of 1016 and 1015 atomscm-3. It was estimated that sample thickness must be more than 700nm to make it be possible to detect sub-layers by the combination of PS-EH and cryo-FIB.

Precise Measurement of Carrier Concentrations in n-Type GaN by Phase-Shifting Electron Holography

Precise Measurement of Carrier Concentrations in n-Type GaN by Phase-Shifting Electron Holography

Direct Observation of a Li-Ionic Space-Charge Layer Formed at an Electrode/Solid-Electrolyte Interface.

When two different materials come into contact, mobile carriers redistribute at the interface according to their potential difference. Such a charge redistribution is also expected at the interface between electrodes and solid electrolytes. The redistributed ions significantly affect the ion conduction through the interface. Thus, it is essential to determine the actual distribution of the ionic carriers and their potential to improve ion conduction. We succeeded in visualizing the ionic and potential profiles in the charge redistribution layer, or space-charge layer (SCL), formed at the interface between a Cu electrode and Li-conductive solid electrolyte using phase-shifting electron holography and spatially resolved electron energy-loss spectroscopy. These electron microscopy techniques clearly showed the Li-ionic SCL, which dropped by 1.3 V within a distance of 10 nm from the interface. These techniques could contribute to the development of next-generation electrochemical devices.

Precise Potential Observation of a Biased GaAs p-n Junction by <i>in situ</i> Phase-shifting Electron Holography

Precise Potential Observation of a Biased GaAs p-n Junction by <i>in situ</i> Phase-shifting Electron Holography

Electric Potential Distributions of Two-Dimensional Electron Gas Layers at GaN/AlGaN Nano-Interfaces Observed by High Precision Phase-Shifting Electron Holography

Electric Potential Distributions of Two-Dimensional Electron Gas Layers at GaN/AlGaN Nano-Interfaces Observed by High Precision Phase-Shifting Electron Holography

Accurate Analysis of Group III–V Compound Semiconductors by High Precision Phase-Shifting Electron Holography and Possibility to High Speed Observation

Accurate Analysis of Group III–V Compound Semiconductors by High Precision Phase-Shifting Electron Holography and Possibility to High Speed Observation

Accurate measurement of electric potentials in biased GaAs compound semiconductors by phase-shifting electron holography.

The innate electric potentials in biased p- and n-type GaAs compound semiconductors and the built-in potential were successfully measured with high accuracy and precision by applying in situ phase-shifting electron holography to a wedge-shaped GaAs specimen. A cryo-focused-ion-beam system was used to prepare the 35°-wedge-shaped specimen with smooth surfaces for a precise measurement. The specimen was biased in a transmission electron microscope, and holograms with high-contrast interference fringes were recorded for the phase-shifting method. A clear phase image around the p-n junction was reconstructed even in a thick region (thickness of ~700 nm) at a spatial resolution of 1 nm and precision of 0.01 rad. The innate electric potentials of the unbiased p- and n-type layers were measured to be 12.96 ± 0.17 V and 14.43 ± 0.19 V, respectively. The built-in potential was determined to be 1.48 ± 0.02 V. In addition, the in situ biasing measurement revealed that the measured electric-potential difference between the p and n regions changed by an amount equal to the voltage applied to the specimen, which indicates that all of the external voltage was applied to the p-n junction and that no voltage loss occurred at the other regions.

High Precision Phase-Shifting Electron Holography with Multiple Biprisms for GaN Semiconductor Devices

High Precision Phase-Shifting Electron Holography with Multiple Biprisms for GaN Semiconductor Devices

Precise measurement of electric potential, field, and charge density profiles across a biased GaAs p-n tunnel junction by in situ phase-shifting electron holography

We combined an in situ biasing technique with phase-shifting electron holography, which can simultaneously achieve a high precision and high spatial resolution, to measure the electric potential, field, and charge density profiles across a GaAs p-n tunnel junction. A thin-film specimen was prepared by thinning one part of a bulk specimen using a cryo focused ion beam (FIB) system. We obtained precise electric potential profiles and successfully converted them into smooth electric field and charge density profiles without any fitting simulations. From the relationship between the applied voltage and measured height of the potential step across the p-n junction, the built-in potential of the p-n junction was determined to be 1.55 ± 0.02 V. The electric field profiles showed that the unbiased p-n junction had a depletion layer with a width of 24 ± 1 nm; the width increased to 26 ± 1 nm under a reverse bias of −0.3 V and decreased to 22 ± 1 nm under a forward bias of 0.5 V. Moreover, the charge density profiles indicated the presence of passivated dopants and/or trapped carriers even in the internal active layer of the specimen, with little damage introduced by FIB milling.

Reconstruction Method for Phase-Shifting Electron Holography Fitted with Fresnel Diffraction Affected Fringes

Phase shifting electron holography is a transmission electron microscope technique that a number of holograms with different initial phases are acquired by changing the angle of the incident electron beam, and the intensity variation at a certain point on the holograms is fitted by sinusoidal curve to retrieve the object wave passing through a specimen. In reality, however, Fresnel fringes caused by the electrostatic biprism modulates the electron wave, limits the fitting accuracy and results in phase errors in phase reconstruction. In this study, we suggest a modified phase reconstruction method for phase shifting electron holography. The intensity variations at a certain point on each hologram are fitted not by sinusoidal curve, but by Fresnel diffraction affected curve to retrieve the object wave. This would provide better fitting accuracy, and has a potential to improve the precision of phase shifting electron holography. Simulations demonstrated the improvements of this method comparing with conventional phase shifting holography method.

B23-P-10Visualization of two-dimensional potential map in organic electroluminescent materials with phase-shifting electron holography

Electron holography is one of TEM methods which can quantitatively measure electromagnetic fields of the samples [1-2]. In this study, we succeeded in observing local 2D electric potential distribution to be formed in an organic electroluminescent device inside quantitatively with phase-shifting electron holography. Organic electroluminescent multilayer samples fabricated on a Si substrate with vacuum evaporation were examined on HF-3300EH TEM and obtained 2D, as shown in Fig. 1. In the reconstructed image (Fig. 1(c)), we can clearly observe the contrast in the multilayer reflected their electric fields. Because the inner potential of materials is constant in each layer, we can consider phase shifts to be an electric potential change in samples.

B23-O-12Visualization of potential map in a thin-film solar cell by high sensitivity phase-shifting electron holography

B23-O-12Visualization of potential map in a thin-film solar cell by high sensitivity phase-shifting electron holography

Direct observation of dopant distribution in GaAs compound semiconductors using phase-shifting electron holography and Lorentz microscopy

Phase-shifting electron holography and Lorentz microscopy were used to map dopant distributions in GaAs compound semiconductors with step-like dopant concentration. Transmission electron microscope specimens were prepared using a triple beam focused ion beam (FIB) system, which combines a Ga ion beam, a scanning electron microscope, and an Ar ion beam to remove the FIB damaged layers. The p-n junctions were clearly observed in both under-focused and over-focused Lorentz microscopy images. A phase image was obtained by using a phase-shifting reconstruction method to simultaneously achieve high sensitivity and high spatial resolution. Differences in dopant concentrations between 1 × 10(19) cm(-3) and 1 × 10(18) cm(-3) regions were clearly observed by using phase-shifting electron holography. We also interpreted phase profiles quantitatively by considering inactive layers induced by ion implantation during the FIB process. The thickness of an inactive layer at different dopant concentration area can be measured from the phase image.

Development of advanced electron holographic techniques and application to industrial materials and devices

The development of a transmission electron microscope equipped with a field emission gun paved the way for electron holography to be put to practical use in various fields. In this paper, we review three advanced electron holography techniques: on-line real-time electron holography, three-dimensional (3D) tomographic holography and phase-shifting electron holography, which are becoming important techniques for materials science and device engineering. We also describe some applications of electron holography to the analysis of industrial materials and devices: GaAs compound semiconductors, solid oxide fuel cells and all-solid-state lithium ion batteries.