We conducted 13C-NMR measurements for a TTF-CA single crystal, in which the central double-bonded carbon sites in TTF molecules were enriched by 13C isotopes. A magnetic field of 8 T was applied in a direction approximately 35° tilted from the a axis to the c axis. We used the so-called solid-echo pulse sequence of (π/2)x-τ-(π/2)y to acquire the 13C-NMR signals, where (π/2)i means a π/2 pulse of a radio frequency wave applied along the i axis in the rotational frame and τ is the time interval between the two π/2 pulses. The nuclear spin-lattice relaxation rate T1−1 was measured by the standard saturation recovery method. The relaxation curve of nuclear magnetization was well fitted by a single exponential function for every pressure studied (section S4). We used a clamp-type pressure cell made of nonmagnetic BeCu to apply hydrostatic pressure to the sample. The pressure medium used was Daphne 7373 oil. The pressure values quoted in the main text are the room temperature values.

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