Abstract Rich electron-matter interactions fundamentally enable electron probe studies of materials such as scanning transmission electron microscopy (STEM). Inelastic interactions often result in structural modifications of the material, ultimately limiting the quality of electron probe measurements. However, atomistic mechanisms of inelastic-scattering-driven transformations are difficult to characterize. Here, we report direct visualization of radiolysis-driven restructuring of rutile TiO2under electron beam irradiation. Using annular dark field imaging and electron energy-loss spectroscopy signals, STEM probes revealed the progressive filling of atomically sharp nanometer-wide cracks with striking atomic resolution detail. STEM probes of varying beam energy and precisely controlled electron dose were found to constructively restructure rutile TiO2according to a quantified radiolytic mechanism. Based on direct experimental observation, a “two-step rolling” model of mobile octahedral building blocks enabling radiolysis-driven atomic migration is introduced. Such controlled electron beam-induced radiolytic restructuring can be used to engineer novel nanostructures atom-by-atom. 
                        more » 
                        « less   
                    
                            
                            Quantitative Electron Beam‐Single Atom Interactions Enabled by Sub‐20‐pm Precision Targeting
                        
                    
    
            Abstract The ability to probe and control matter at the picometer scale is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy offers powerful capabilities for materials analysis and modification, but sample damage, drift, and scan distortions hinder single atom analysis and deterministic manipulation. Materials analysis and modification via electron–solid interactions can be transformed by precise delivery of electrons to a specified atomic location, maintaining the beam position despite drift, and minimizing collateral dose. Here a fast, low‐dose, sub‐20‐pm precision electron beam positioning technique is developed, “atomic lock‐on,” (ALO), which offers the ability to position the beam on a specific atomic columnwithoutpreviously irradiating that column. This technique is used to lock onto a single selected atomic location to repeatedly measure its weak electron energy loss signal despite sample drift. Moreover, electron beam‐matter interactions in single atomic events are measured with time resolution. This enables observation of single‐atom dynamics, such as atomic bistability, revealing partially bonded atomic configurations and recapture phenomena. This opens prospects for using electron microscopy for high‐precision measurements and deterministic control of matter for quantum technologies. 
        more » 
        « less   
        
    
                            - Award ID(s):
- 2421694
- PAR ID:
- 10609662
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Science
- Volume:
- 12
- Issue:
- 34
- ISSN:
- 2198-3844
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            Abstract Both high resolution and high precision are required to quantitatively determine the atomic structure of complex nanostructured materials. However, for conventional imaging methods in scanning transmission electron microscopy (STEM), atomic resolution with picometer precision cannot usually be achieved for weakly-scattering samples or radiation-sensitive materials, such as 2D materials. Here, we demonstrate low-dose, sub-angstrom resolution imaging with picometer precision using mixed-state electron ptychography. We show that correctly accounting for the partial coherence of the electron beam is a prerequisite for high-quality structural reconstructions due to the intrinsic partial coherence of the electron beam. The mixed-state reconstruction gains importance especially when simultaneously pursuing high resolution, high precision and large field-of-view imaging. Compared with conventional atomic-resolution STEM imaging techniques, the mixed-state ptychographic approach simultaneously provides a four-times-faster acquisition, with double the information limit at the same dose, or up to a fifty-fold reduction in dose at the same resolution.more » « less
- 
            A majority of ultracold atom experiments utilize resonant absorption imaging techniques to obtain the atomic density. To make well-controlled quantitative measurements, the optical intensity of the probe beam must be precisely calibrated in units of the atomic saturation intensityIsat. In quantum gas experiments, the atomic sample is enclosed in an ultra-high vacuum system that introduces loss and limits optical access; this precludes a direct determination of the intensity. Here, we use quantum coherence to create a robust technique for measuring the probe beam intensity in units ofIsatvia Ramsey interferometry. Our technique characterizes the ac Stark shift of the atomic levels due to an off-resonant probe beam. Furthermore, this technique gives access to the spatial variation of the probe intensity at the location of the atomic cloud. By directly measuring the probe intensity just before the imaging sensor our method in addition yields a direct calibration of imaging system losses as well as the quantum efficiency of the sensor.more » « less
- 
            Abstract Spatially resolved in situ transmission electron microscopy (TEM), equipped with direct electron detection systems, is a suitable technique to record information about the atom-scale dynamics with millisecond temporal resolution from materials. However, characterizing dynamics or fluxional behavior requires processing short time exposure images which usually have severely degraded signal-to-noise ratios. The poor signal-to-noise associated with high temporal resolution makes it challenging to determine the position and intensity of atomic columns in materials undergoing structural dynamics. To address this challenge, we propose a noise-robust, processing approach based on blob detection, which has been previously established for identifying objects in images in the community of computer vision. In particular, a blob detection algorithm has been tailored to deal with noisy TEM image series from nanoparticle systems. In the presence of high noise content, our blob detection approach is demonstrated to outperform the results of other algorithms, enabling the determination of atomic column position and its intensity with a higher degree of precision.more » « less
- 
            We present a quantum optics-based detection method for determining the position and current of an electron beam. As electrons pass through a dilute vapor of rubidium atoms, their magnetic field perturbs the atomic spin's quantum state and causes polarization rotation of a laser resonant with an optical transition of the atoms. By measuring the polarization rotation angle across the laser beam, we recreate a 2D projection of the magnetic field and use it to determine the e-beam position, size, and total current. We tested this method for an e-beam with currents ranging from 30 to 110 μA. Our approach is insensitive to electron kinetic energy, and we confirmed that experimentally between 10 and 20 keV. This technique offers a unique platform for noninvasive characterization of charged particle beams used in accelerators for particle and nuclear physics research.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
