(A) Experimental EPR spectrum (integrated from the first derivative) of ANCOOT in toluene at 100K (black line) and its hyperpolarized EPR spectrum recorded for 2.5 μs after a 355 nm laser pulse (blue line) and integrated using a boxcar averager over 0.3 μs (see SI for experimental details). The gain factor of −100 for the Boltzmann signal represents the ESP enhancement obtained from time resolved experiments (TREPR), see appendix 4. (B) Plot of the RQM selectivity factor, RD1 (black squares), and the corresponding values of Pe (red squares) as a function of the exchange parameter, ∣JCR∣ (JCR<0), for the case of pure RQM, i.e., process (ii) (scheme 1). N.B. solid black and dashed red interpolating lines are provided as guides to the eye.