Accurate geometrical calibration between the scan coordinates and the camera coordinates is critical in four-dimensional scanning transmission electron microscopy (4D-STEM) for both quantitative imaging and ptychographic reconstructions. For atomic-resolved, in-focus 4D-STEM datasets, we propose a hybrid method incorporating two sub-routines, namely a J-matrix method and a Fourier method, which can calibrate the uniform affine transformation between the scan-camera coordinates using raw data, without a priori knowledge of the crystal structure of the specimen. The hybrid method is found robust against scan distortions and residual probe aberrations. It is also effective even when defects are present in the specimen, or the specimen becomes relatively thick. We will demonstrate that a successful geometrical calibration with the hybrid method will lead to a more reliable recovery of both the specimen and the electron probe in a ptychographic reconstruction. We will also show that, although the elimination of local scan position errors still requires an iterative approach, the rate of convergence can be improved, and the residual errors can be further reduced if the hybrid method can be firstly applied for initial calibration. The code is made available as a simple-to-use tool to correct affine transformations of the scan-camera coordinates in 4D-STEM experiments.

The ‘Mystery Interval’ (MI, 17.5−14.5 ka) was the first stage of the last deglaciation, a key interval for understanding mechanisms of glacial–interglacial cycles. To elucidate possible causes of the MI, here we present three high-resolution, precisely dated oxygen-isotope records of stalagmites from Qingtian and Hulu Caves in China, reflecting changes in the East Asian summer monsoon (EASM) then. Based on well-established chronologies using precise 230Th dates and annual-band counting results, the two-cave δ18O profiles of ~7-yr resolution match well at decadal timescales. Both of the two-cave records document an abrupt weakening (2‰ of δ18O rise within 20 yr) in the EASM at ~16.1 ka, coinciding with the transition of the two-phased MI reconstructed from New Mexico's Lake Estancia. Our results indicate that the maximum southward displacement of the Intertropical Convergence Zone and associated southward shift of polar jet stream may generate this two-phase feature of the MI during that time. We also discover a linear relationship among decreasing EASM intensity, rising atmospheric CO2 and weakening Atlantic Meridional Overturning Circulation between the MI and Younger Dryas episodes, suggesting a strong coupling of atmospheric/oceanic circulations in response to the millennial-scale forcing, which in turn regulates global climate changes and carbon cycles.

A high-resolution, annual layer-counted and 230Th-dated multi-proxy record is constructed from a stalagmite in Hulu Cave, China. These proxies, including δ18O, annual layer thickness (ALT), gray level (GL) and Sr/Ca, cover a time span of ~ 3000 yr from 21 to 24 ka. The physical proxies (ALT and GL) and the geochemical index (Sr/Ca), all primarily reflecting karst hydrological processes, vary in concert and their coherence is supported by wavelet analyses. Variations in the δ18O data agree with fluctuations in the ALT and Sr/Ca records on multi-decadal to centennial scales, suggesting that the Hulu δ18O signal is strongly associated with varying local rainfall amounts on short timescales. A monsoon failure event at ~ 22.2 ka correlates with a decrease in tropical rainfall, a reduction in global CH 4 and an ice-rafted event in the North Atlantic. This correlation highlights roles of the Asian monsoon and tropical hydrological cycle in modulating global CH 4, because the high-latitude emission was inhibited during the Last Glacial Maximum (LGM). Spectral analysis of the δ18O record displays peaks at periodicities of 139, 59, 53, 43, 30, 23 and 19"15 yr. The absence of typical centennial solar cycles may be related to muted changes in ocean circulation during the LGM.