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Wide-area dynamic studies are of paramount importance to ensure the stability and reliability of power grids. This paper puts forth a comprehensive framework for inferring the dynamic responses in the small-signal regime using ubiquitous fast-rate ambient data collected during normal grid operations. We have shown that the impulse response between any pair of locations can be recovered in a model-free fashion by cross-correlating angle and power flow data streams collected only at these two locations, going beyond previous work based on frequency data only. The result has been established via model-based analysis of linearized second-order swing dynamics under certain conditions. Numerical validations demonstrate its applicability to realistic power system models including nonlinear, higher-order dynamics. In particular, the case study using synthetic PMU data on a synthetic Texas Interconnection (TI) system strongly corroborates the benefit of using angle PMU data over frequency one for real-world power system dynamic modeling.more » « less