Contact interface properties are important in determining the performances of devices based on atomically thin two-dimensional (2D) materials, especially those with short channels. Understanding the contact interface is therefore quite important to design better devices. Herein, we use scanning transmission electron microscopy, electron energy loss spectroscopy, and first-principles calculations to reveal the electronic structures within the metallic (1T')-semiconducting (2H) MoTe2 coplanar phase boundary across a wide spectral range and correlate its properties and atomic structure. We find that the 2H-MoTe2 excitonic peaks cross the phase boundary into the 1T' phase within a range of approximately 150 nm. The 1T'-MoTe2 crystal field can penetrate the boundary and extend into the 2H phase by approximately two unit cells. The plasmonic oscillations exhibit strong angle dependence, i.e., a red-shift of π+σ (approximately 0.3 eV-1.2 eV) occurs within 4 nm at 1T'/2H-MoTe2 boundaries with large tilt angles, but there is no shift at zero-tilted boundaries. These atomic-scale measurements reveal the structure-property relationships of 1T'/2H-MoTe2 boundary, providing useful information for phase boundary engineering and device development based on 2D materials. 3Two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted extensive attention due to their potential applications in nanoelectronics [1,2]. In these atomically thin TMDs devices, contact interface properties can significantly influence the performance, especially in short-channel devices [3,4]. An imperfect interface between the electrode and a 2D semiconducting TMD can cause Fermi level pinning and thus result in high resistance across the contact [5,6], which limits potential applications as device sizes scale down. Recent strategies such as indium/gold contacts [7], tunneling contacts [8], and metallic 2D material contacts [9] have been used to reduce contact resistance in long-channel devices [3,[7][8][9][10]. However, these techniques are less effective in short-channel devices or large-scale applications.Recently, heterophase (e.g. metallic 1T'-MoTe2 [11,12] and semiconducting 2H-MoTe2 [13,14]) coplanar [15][16][17]) structures have been demonstrated to effectively reduce contact resistances in stable integrated circuits [18] by avoiding introduction of defects and impurities from step-by-step device fabrication processes [19][20][21][22]. These keep the promise of phase engineering as an effective way to reduce short-channel device contact resistances in order to achieve the low contact resistance requirements of the International Technology Roadmap for Semiconductors [4].The properties of these coplanar boundaries (e.g., 1T'/2H-MoTe2) should be dictated to their atomic structures, such as the interfacial sharpness, relative orientation between metallic and semiconducting phases, and nature of the interfacial bonds, which, unfortunately, remain largely unknown due to a lack of techniques that correlate the electronic structures of atomi...