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Multidimensional x-ray spectroscopy of valence and core excitations in cysteine
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View: Figures


Image of FIG. 1.
FIG. 1.

(Left) Pulse sequence for the four-wave mixing setup. (Right) The contributing loop diagrams for the and signals.

Image of FIG. 2.
FIG. 2.

Loop diagrams for the two-pulse SXRS signal.

Image of FIG. 3.
FIG. 3.

Loop diagrams for the three-pulse 2D-SXRS signal. Ω2 and Ω4 are the Fourier conjugates of the two delay times, and Ω5 is the monochrometer frequency. Peaks along Ω2 and Ω4 occur at valence frequencies, and those along Ω5 at core-excitation frequencies.

Image of FIG. 4.
FIG. 4.

Simulated x-ray absorption (XANES) spectra for cysteine at the nitrogen, oxygen, and sulfur K-edges, and the sulfur L2-edge. Stick spectra are shown in black, and simulated spectra with constant Lorentzian linewidths are shown in red. The following linewidths were used: and We plot also the power spectra for the ultrafast laser pulses used in the simulations here with FWHM in time and frequency of 128 as and 14.2 eV, respectively. The central frequencies for the N1s, O1s, S1s, and S2p pulses are 406.4 eV, 532.2 eV, 2473.5 eV, and 164.6 eV, respectively.

Image of FIG. 5.
FIG. 5.

3D contour plots of , the modulus of the photon echo NNNN signal with all four pulses tuned to the nitrogen K-edge, and all pulses polarized parallel (XXXX). (Left) The full 3D XPE signal. The portion of the signal enclosed in the red dashed box (multiplied by 5 here to increase visibility) is responsible for the x-ray Raman resonances. (Right) Enlarged spectrum of the region Ω2 > 0, highlighted by the red box in the full spectrum. The walls of the 3D box enclosing the contour plot show 2D projections of the 3D data, defined by Eq. (1) .

Image of FIG. 6.
FIG. 6.

2D projections of the 3D signal of Fig. 5 , using an NNNN pulse sequence and XXXX polarization. (Top row) , (middle row) , and (bottom row) . The left, middle, and right columns show , , and , respectively. Each signal is plotted using a nonlinear scale shown in the color bars.

Image of FIG. 7.
FIG. 7.

Same as Fig. 6 , using an OOOO pulse sequence and XXXX polarization.

Image of FIG. 8.
FIG. 8.

2D projections of the 3D signal using an NNOO pulse sequence with XXXX polarization.

Image of FIG. 9.
FIG. 9.

(Top) Constant-Ω2 slices of the 3D signal using an OOSS pulse sequence, XXXX polarization. Specifically, we plot , , and . (Bottom) The I2P-SXRS signal using an OS pulse sequence with XX polarization.

Image of FIG. 10.
FIG. 10.

signals simulated for an OOSS pulse sequence for three different polarization configurations. Each column represents a different polarization schemes, with the polarization vectors of pulses 1–4 indicated at the top of each column. The top row shows , the middle row , and the bottom row

Image of FIG. 11.
FIG. 11.

Frequency-dispersed SXRS spectra (Eq. (B4) ) for cysteine, for various pump pulse detunings with the probe tuned to the N1s-edge transition frequency. The vertical axis is the dispersed frequency Ω3, and the horizontal axis is the Fourier conjugate of the interpulse delay Ω2. The 2D signal is plotted using an arcsinh nonlinear scale, and the projections are shown, in a linear scale, in the top and right marginals. The trace along the top corresponds to the integrated SXRS signal.

Image of FIG. 12.
FIG. 12.

Same as Fig. 11 , but with the probe tuned to the oxygen K-edge.

Image of FIG. 13.
FIG. 13.

Same as Fig. 11 , but with the probe tuned to the sulfur K-edge.

Image of FIG. 14.
FIG. 14.

Same as Fig. 11 , but with the probe tuned to the sulfur L-edge.

Image of FIG. 15.
FIG. 15.

(Left column) Four-wave mixing signals using the OONN pulse sequence (XXXX polarized). On top is and on the bottom is . (Right column) The modulus D2P-SXRS signal with an ON pulse sequence, XX polarized.

Image of FIG. 16.
FIG. 16.

I3P-SXRS signals from cysteine with the first pulse resonant with the S1s transition and the third at the O1s transition, with XXX polarization.

Image of FIG. 17.
FIG. 17.

D3P-SXRS signals from cysteine using an SOO pulse configuration, with XXX polarization. Ω2 and Ω4 are valence excitations, and Ω5 represents core excitation.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Multidimensional x-ray spectroscopy of valence and core excitations in cysteine