▎ 摘　　要

A strictly two-dimensional (2D) material such as freestanding graphene (FSG) is rarely investigated at the atomic scale by scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). A basic difficulty in probing FSG by STM and STS is the mechanical instability when a highly compliant 2D atomic layer interacts with a proximal tip. Here we report a detailed method to conduct reliable STM and STS on FSG with atomic precision. We found that FSG is intrinsically rippled and exhibits a nonlinear strain-stress relation under applied normal forces; it shows a very soft region of bending strain and stiffer regions of in-plane tensile strain once the nanoscale ripples of FSG are eliminated. The elimination of the nanoripples can be controlled by tip-induced pulling or pushing force through the so-called closed-loop Z-V STS mode which can monitor the FSG deformation. A key factor for controllable STM and STS measurements is to select tunneling set points to place FSG in metastable configurations, as determined from stress-strain (i.e., Z-V) response. Atomic imaging and electronic states thus measured must be interpreted by considering the dynamical deformation of FSG as tunneling parameters, and therefore tip-FSG forces, are varied.