The intrinsic competition among multiple charge transfer (CT) pathways in copper-phenylacetylide (PhC2Cu) has hindered the desirable development of its photoactive properties, whereas substantial spectral and temporal overlap among these pathways has obscured direct mechanistic understanding. Herein, hydrostatic pressure was employed as a clean and reversible external stimulus to continuously compress the one-dimensional Cu(I)–Cu(I) ladder in pristine PhC2Cu without modifying its chemical composition. In situ high-pressure photoluminescence and transient absorption (TA) spectroscopy reveal a pressure-induced evolution of CT from copper to the acetylide carbon. High-pressure crystallographic analysis and X-ray absorption near-edge structure measurements (XANES) demonstrate that anisotropic contraction of the Cu(I) ladder reconstructs the copper coordination environment and consequently modulates the relative contributions of metal-to-ligand CT pathways. These structure-dependent electronic dynamics provide direct insight into the CT mechanism of PhC2Cu and establish hydrostatic pressure as a general and non-destructive strategy for investigating CT processes in one-dimensional (1D) coordination compounds.
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Research Article
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Open Access
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Since the successful synthesis of bulk sp3 amorphous carbon in 2021, this material has attracted considerable attention owing to its ultrahigh hardness, mechanical isotropy, potential for shaping and machining, and distinctive electronic structure. These features make it a promising candidate for applications in ultra-precision machining and optoelectronic detection. Recent studies have mainly focused on the formation mechanism, thermodynamic stability, structural and property regulation, and synthesis process optimization of sp3 amorphous carbon materials derived from fullerenes under high-pressure and high-temperature conditions. These studies have not only deepened the understanding of the formation mechanism of sp3 amorphous carbon, but also promoted the further development of its functional applications. This review systematically summarizes the relevant research progress and discusses future key directions, including the large-size and high-quality synthesis, precision shaping, and functional application expansion of sp3 amorphous carbon.
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