Schematics of self-consistent calculation of core-excited states. The ECA (left) replaces a core with the next highest element in the periodic table, the FCH (middle) fixes the occupation of the core-orbital, neglecting the excited electron, whereas the XCH (right) fixes the occupation of both orbitals.
The XDQC technique.
(Left) The two diagrams contributing to the double quantum coherence signal. (Right) Molecular structure and REW-TDDFT level scheme. |O j N i ⟩ refers to the double core-excited states with the O1s electron excited to the jth virtual orbital of the self-consistent core state, while the N1s to ith orbital excitation is obtained through response theory, as described in the text.
Calculated (grey) nitrogen (left) and oxygen (right) K-edge XANES for formamide. Experimental EELS spectra 137 are given as black lines, and power spectra of the pulses used in the calculation of the 2D-QCS signals as dashed lines. The simulated energies were shifted (+13.065 eV for nitrogen and +14.5 eV for oxygen K-edge) to fit the EELS signals. 137
The ONNO signal with XXXX polarization configuration. The total signal (left column) is the sum of the contributions from diagram A (middle column) and diagram B (right column) of Fig. 3 . Each circle in the stick spectra (top row) has a complex contribution to the signal from a combination of states, with the radius of the circle proportional to the square root of the amplitude, and colored according to the phase of the contributing peak. The following three rows show the absolute value, real and imaginary parts of the complex signal after convoluting with a Lorentzian of width 0.1 eV. All signals were scaled so that abs( ) has a maximum value of one.
Same as Fig. 5 , but for the pulse sequence NONO.
Comparison of the absolute parts of the ONNO (left) and NONO (right) signals. XANES spectra are shown in the marginals.
Comparison of the two protocols to calculate the double-core excited states | f ⟩ for the all-parallel ONNO signal as discussed in Sec. VI B . Contributions from diagram A (left column) and B (right column) with protocols i (top row) or protocol ii (bottom row). All graphs were multiplied by the same scaling factor used in Fig. 5 .
for the ONNO pulse configuration.
for the NONO pulse configuration.
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