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Condens. Matter 2019, 4, 5 4 of 12 work [15]. The incident soft X-ray was generated by the synchrotron light source, concentrated by the bendaCbonldenms. Miratrtoerr2,0a19n, 4d, xsFhOeRdPEoERnRaEVsIaEWmple. The soft X-ray fluorescence photons were4eomf 1i2tted from the sample, and were differentiated by an ultra-high efficiency spectrometer equipped with optics the schematic illustration of the mRIXS system in the endstation, which has been detailed in and a charge-coupled device (CCD) detector. mRIXS data were collected with a 0.2 eV step size in previous work [15]. The incident soft X-ray was generated by the synchrotron light source, excitation energy across the full O-K absorption edges. At each excitation energy, the collected RIXS concentrated by the bendable mirror, and shed on a sample. The soft X-ray fluorescence photons signals wwereereneomrimtteadlifzroemd tohethsaemipnlce,idaenndtwbeereamdifflfeurexntaiantedddbaytancoultlreac-htioghn etfifmicie.ncTyhsepencotrromeatleirzed RIXS equipped with optics and a charge-coupled device (CCD) detector. mRIXS data were collected with cuts at the individual excitation energy were summarized together into a color-scale mRIXS image a 0.2 eV step size in excitation energy across the full O-K absorption edges. At each excitation energy, with the intensity represented by the color. Details on data processing can be found in a previous the collected RIXS signals were normalized to the incident beam flux and data collection time. The publication [14]. normalized RIXS cuts at the individual excitation energy were summarized together into a color-scale mRIXS image with the intensity represented by the color. Details on data processing can 2.2. Presentations of O-K mRIXS be found in a previous publication [14]. mRIXS results are 2D images with two energy axes, one corresponding to the indecent X-ray 2.2. Presentations of O-K mRIXS excitation energies, while the other is the emitted photon energies measured through an RIXS mRIXS results are 2D images with two energy axes, one corresponding to the indecent X-ray spectrometer. Therefore, mRIXS could be presented in three typical ways in the literature (Figure 2), excitation energies, while the other is the emitted photon energies measured through an RIXS andeachswpeocturoldmehteirg.hTlhiegrheftorteh,emoRrIXigSincouolfdcberptareisnenstiegdninaltshrfereotmypidcaiflfweraeynsitnetlhecltirteornatiucred(eFcigauyrsed2)u,ringthe and each would highlight the origin of certain signals from different electronic decays during the spectroscopic process [8]. spectroscopic process [8]. Figure 2. O-K mRIXS of a fully charged (1st Ch 4.6 V) LR-NMC electrode presented in three different Figure 2. O-K mRIXS of a fully charged (1st Ch 4.6 V) LR-NMC electrode presented in three different ways to emphasize different features. (a) mRIXS image (top) plotted together with extracted XAS ways to emphasize different features. (a) mRIXS image (top) plotted together with extracted XAS channelsc(hbaontnteolms()b.oTttohme)e.Txhcietaextcioitnatieonerngerygyisisththeehorizonntatlaalxaisx,iws,hwichischpriesfeprreedfebryrmedosbtymmateorisatlmaterial scientistssbceiecnatuistssembecRaIuXseSrmeRsuIXltSscreasnulbtsecaonmbpearceodmdpairedctldyirwecittlhyXwAithSfXeAatSurfeast.uSreusc.hSducihrecdtirceocmtparison comparison shows that Feature-1 corresponds to the two main peaks in the O-K XAS pre-edge range, shows that Feature-1 corresponds to the two main peaks in the O-K XAS pre-edge range, which is of which is of TM(3d) character from the TM(3d)-O(2p) hybridization. Feature-2 corresponds to the XAS TM(3d) character from the TM(3d)-O(2p) hybridization. Feature-2 corresponds to the XAS hump at high hump at high energy, and is of TM(4s/4p) character from TM(4s/4p)-O(2p) hybridization. The striking energy, and is of TM(4s/4p) character from TM(4s/4p)-O(2p) hybridization. The striking Feature-5 is the Feature-5 is the oxidized oxygen feature that could be extracted through sPFY-II by integrating the oxidized osixgynaglesnarfoeuantdutrheetchatraccoteurlisdticbe52e3x.7treaVcetemdissthiornoeungehrgysPraFnYg-eI.IsbPyFYi-nI(tTeMgr-aOt)inisgthtehientseigrnataiolsnaorfound the the mRIXS intensity in the emission energy range around 525 eV, emphasizing TM-O hybridization characteristic 523.7 eV emission energy range. sPFY-I(TM-O) is the integration of the mRIXS intensity features. It is clear that conventional XAS TFY signals are dominated by TM-O hybridization in the emission energy range around 525 eV, emphasizing TM-O hybridization features. It is clear features, especially in the pre-edge regime. (b) A typical way of plotting mRIXS with emission that conventional XAS TFY signals are dominated by TM-O hybridization features, especially in the energy along the horizontal axis. The broad Feature 1 and 2 are consistent with typical O-K RIXS pre-edge regime. (b) A typical way of plotting mRIXS with emission energy along the horizontal axis. The broad Feature 1 and 2 are consistent with typical O-K RIXS results of oxides remaining constant around 525 eV emission energy. (c) mRIXS results with energy loss values plotted along the horizontal axis. This is preferred in physics because it shows the value of energy loss for specific RIXS excitations, e.g., Feature-4 displays an energy loss of less than 1 eV, which is likely from the excitation of vibronic modes (see text).PDF Image | Oxygen Redox Reactions in Batteries Resonant Inelastic X-ray Scattering
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