Metadata File for: Jayabalan, R.; Hanumantharaju, G.K.; Hettiger, T.; Sarkar, A.; Zu, F.; Ullrich, A.; Abfalterer, A.; Urban, A.S.; Koch, N.; Andrienko, D.; Scheele, M.; Brütting, W. Optimizing Carrier Balance in CsPbBr3 Nanocrystal LEDs: The Role of Alkyl Ligands and Polar Electron Transport Layers. Accepted in Advanced Optical Materials. Acknowledgements: This work was funded by Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) within Priority Programme "Perovskite Semiconductors: From Fundamental Properties to Devices" (SPP 2196) under project nos. 424708673 & 426008387, by DFG project no. 443153421 and under Germany's Excellence Strategy EXC 2089/1-390776260 (Excellence Cluster 'e-conversion') as well as by the Bavarian State Ministry of Science, Research and Arts through the grant 'Solar Technologies go Hybrid (SolTech)' along with the KAUST CRG program "INSIGHT into Interfacial Charge Carrier Recombination Processes in Metal Halide Perovskite Solar Cells". A. Sarkar and D. Andrienko would also like to thank the Max Planck Computing & Data Facility (MPCDF/Raven) for providing supercomputing resources. This research was funded in whole or in part by the Austrian Science Fund (FWF) 10.55776/J4863. For the purpose of open access, the authors have applied a CC BY public copyright license to any Author Accepted Manuscript (AAM) version arising from this submission. The following data files are deposited in this Open Data LMU entry and correspond to the published data as follows: Figure2-TEM Native NCs.dm4: The TEM image of OA/OAm covered nanocrystals presented in Figure 2a). DDABr NCs.dm4: The TEM image of DDABr covered nanocrystals presented in Figure 2b). The image files can be opened using, e.g., ImageJ[1], which is freeware, or Gatan DigitalMicrograph Software. Figure3-NMR 11-05092024-TH.txt: Contains the 1H NMR data of DDABr-treated nanocrystals. RJ_OAOAm_NCs_03072024.txt: Contains the 1H NMR data of OA/OAm covered nanocrystals. TH_24062024_DDABr.txt: Contains the 1H NMR data of DDABr. kleinesNMR.py: Contains a Python script used to plot the three datasets for Figure 3. Figure4-Spectroelectrochemistry (SEC) 39.txt: Contains the cyclic voltammetry data presented in Figure 4a). Spot2_SeriesSpec_1sT300x_0d0OD_39.asc: Contains the photoluminescence spectra measured as a function of the Potential vs. Ag PRE (V). DDABr1x_paper.py: Contains a Python script used to process the two datasets and plot the datasets as a 2D plot in Figure 4b). Figure 4c) and d) originate from that data. OxpotentialsvsFc.docx: Summarizes the oxidation potentials determined for the four samples (DDABr 1x washed, DDABr 2x washed, native 1x washed, native 2x washed). DDABr 1x washed: Oxidation potential was averaged from measurements #39 and #43. DDABr 2x washed: Oxidation potential was averaged from measurements #46 and #32 (2x). Native 1x washed: Two measurements were taken (#64 and #69); the oxidation potential value from measurement #69 was used. Native 2x washed: Oxidation potential was averaged from measurements #75 and #78 (2x). Folder '43' contains the cyclic voltammetry dataset '43.txt' and photoluminescence spectrum dataset 'Spot2_SeriesSpec_1sT600x_0d0OD_43.asc' for measurement #43. Spot2_SeriesSpec_1sT600x_0d0OD_43_NEU1_DDABr_1x.py: Contains a Python script used to extract the oxidation potential value for measurement #43. Folder '46' contains the cyclic voltammetry dataset '46.txt' and photoluminescence spectrum dataset 'Spot3_SeriesSpec_1sIT_300x_0d0OD_46.asc' for measurement #46. Spot3_SeriesSpec_1sIT_300x_0d0OD_46NEU_DDABr_2x.py: Contains a Python script used to extract the oxidation potential value for measurement #46. Folder '32' contains the cyclic voltammetry dataset '32.txt' and photoluminescence spectrum dataset 'Spot3_SeriesSpec_1sIT_600x_0d0OD_32.asc' for measurement #32. For the dataset related to measurement #69, please refer to Figure S5. Folder '64' contains the cyclic voltammetry dataset '64.txt' and photoluminescence spectrum dataset 'Spot2_SeriesSpec_300x1sIT_0OD_64.asc' for measurement #64. Spot2_SeriesSpec_300x1sIT_0OD_64NEU_OAOAm_1x.py: Contains a Python script used to extract the oxidation potential value for measurement #64. For the dataset related to measurement #75, please refer to Figure S6. Folder '78' contains the cyclic voltammetry dataset '78.txt' and photoluminescence spectrum dataset 'Spot3_SeriesSpec_1sIT600x_0d0OD_78.asc' for measurement #78. Spot3_SeriesSpec_1sIT600x_0d0OD_78NEU_OAOAm_2x.py: Contains a Python script used to extract the oxidation potential value for measurement #78. Figure5-UPS DDABr_SECO_low flux.xy: Contains the secondary electron cut-off spectrum of the DDABr-covered nanocrystals, used to create Figure 5a) bottom. Native_SECO_low flux.xy: Contains the secondary electron cut-off spectrum of the OA/OAm covered nanocrystals, used to create Figure 5a) bottom. PEDOT_PTAA_SECO_med flux.xy: Contains the secondary electron cut-off spectrum of the PTAA sample, used to create Figure 5a) bottom. DDABr_VB_Ef_low flux.xy: Contains the valence band spectrum of the DDABr-covered nanocrystals, used to create Figure 5a) top. Native_VB_Ef_low flux.xy: Contains the valence band spectrum of the OA/OAm covered nanocrystals, used to create Figure 5a) top. PEDOT_PTAA_VB_short_med flux.xy: Contains the valence band spectrum of the PTAA sample, used to create Figure 5a) top. Figure6-Single carrier devices E_only_DDABr.uil: Contains the current, voltage, and photocurrent data of an electron-only device prepared with DDABr-capped nanocrystals presented in Figure 6a). E_only_Native.uil: Contains the current, voltage, and photocurrent data of an electron-only device prepared with native nanocrystals presented in Figure 6a). H_only_DDABr.uil: Contains the current, voltage, and photocurrent data of a hole-only device prepared with DDABr-capped nanocrystals presented in Figure 6a). H_only_Native.uil: Contains the current, voltage, and photocurrent data of a hole-only device prepared with native nanocrystals presented in Figure 6a). To obtain the current density, the current is divided by the pixel area (4.8 mm2). Figure7-DFT CsPbBr3_barePNC_optimized.xyz: Contains the coordinate file for the bare nanocrystal. CsPbBr3_oleate18_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 hexanoates (mimicking OA). CsPbBr3_oleate18_oleyl6_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 OA and one hexylammonium (mimicking OAm). CsPbBr3_oleyl18_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 OAm. CsPbBr3_DDABr18_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 dihexylammonium (mimicking DDABr). The coordinate files are in .xyz format and are in Angstrom units, which describes the position of the atoms (Cs/Pb/Br/C/H/N/O) in Cartesian space. geo_opt_sample.inp: sample input file for geometry optimization. pdos_sample.inp: sample input file for PDOS calculation. description.docx: Contains information on how the data for Figure 7 was processed using 'get-smearing-pdos.py' and 'pdos.py' codes. Figure8-DFT CsPbBr3_barePNC_optimized.xyz: Contains the coordinate file for the bare nanocrystal. CsPbBr3_oleate6_optimized.xyz: Contains the coordinate file for the nanocrystal with 6 hexanoates (mimicking OA). CsPbBr3_oleate18_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 hexanoates (mimicking OA). CsPbBr3_oleate36_optimized.xyz: Contains the coordinate file for the nanocrystal with 36 hexanoates (mimicking OA). CsPbBr3_oleate18_oleyl6_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 OA and one hexylammonium (mimicking OAm). CsPbBr3_oleyl6_optimized.xyz: Contains the coordinate file for the nanocrystal with 6 OAm. CsPbBr3_oleyl18_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 OAm. CsPbBr3_DDABr6_optimized.xyz: Contains the coordinate file for the nanocrystal with 6 dihexylammonium (mimicking DDABr). CsPbBr3_DDABr18_optimized.xyz: Contains the coordinate file for the nanocrystal with 18 dihexylammonium (mimicking DDABr). The coordinate files are in .xyz format and are in Angstrom units, which describes the position of the atoms (Cs/Pb/Br/C/H/N/O) in Cartesian space. HOMO_LUMO_sample.inp: sample input file for HOMO and LUMO calculation. description.docx: Contains information on how the data for Figure 8 was processed. Figure9-LEDs PeLED_Native_B3PyMPM.xls: Contains the LED characteristics of the native NC PeLED employing B3PyMPM as ETL, used to create Figures 9a) and b). PeLED_Native_TPBi.xls: Contains the LED characteristics of the native NC PeLED employing TPBi as ETL, used to create Figures 9a) and b). Figure10-LEDs PeLED_DDABr.xls: Contains the LED characteristics of the PeLED incorporating DDABr-ligand exchanged nanocrystals. This data was used to create Figures 10a) and b). PeLED_Native_TPBi.xls: Contains the LED characteristics of the PeLED incorporating native, unwashed nanocrystals. This data was used to create Figures 10a) and b), and is the same as presented in Figure S12. EL_spectra_DDABr_PeLED.txt: Contains the EL spectrum of the PeLED incorporating DDABr-ligand exchanged nanocrystals. This data was used to create Figure 10c). EL_spectra_Native_PeLED.txt: Contains the EL spectrum of the PeLED incorporating native, unwashed nanocrystals. This data was used to create Figure 10c). FigureS1-qNMR 10-05092024-TH.txt: Contains the 1H NMR data of bound DDABr to nanocrystals in toluene-d8 for nanocrystals with excess DDABr. 11-05092024-TH.txt: Contains the 1H NMR data of bound DDABr to nanocrystals in toluene-d8 for nanocrystals covered with DDABr after one washing step. 12-05092024-TH.txt: Contains the 1H NMR data of bound DDABr to nanocrystals in toluene-d8 for nanocrystals covered with DDABr after two washing steps. 3-06092024-TH.txt: Contains the quantitative NMR data with ethylene carbonate as standard in DMSO-d6 for nanocrystals with excess DDABr. 04-06092024-TH.txt: Contains the quantitative NMR data with ethylene carbonate as standard in DMSO-d6 for nanocrystals covered with DDABr after one washing step. 5-06092024-TH.txt: Contains the quantitative NMR data with ethylene carbonate as standard in DMSO-d6 for nanocrystals covered with DDABr after two washing steps. qNMR_Vergleich.py: Contains a Python script used to plot the six datasets to create Figure S1. FigureS2-PLdecay Data_FigureS2.xlsx: Contains the PL decay data presented in Figure S2, processed from the raw data as described in the Supporting Information of the publication. The first sheet includes the data for the left panel of Figure S2 (solution measurements). The second sheet contains the data for the right panel (thin film measurements). For the thin films, three PL decay measurements were taken at different spots (1–3) on each film. The example shown in the right panel of Figure S2 corresponds to Spot 1 for the native nanocrystal thin film and Spot 3 for the DDABr-treated nanocrystal thin film. RawData_FigureS2.xlsx: Contains the raw, unprocessed PL decay data (as measured) prior to the processing steps described in the Supporting Information of the publication. This processing yielded the data presented in Figure S2. The first sheet includes the raw data corresponding to the left panel of Figure S2 (solution measurements). The second sheet contains the raw data corresponding to the right panel (thin film measurements). For the thin films, three PL decay measurements were taken at different spots (1–3) on each film. The example shown in the right panel of Figure S2 corresponds to Spot 1 for the native nanocrystal thin film and Spot 3 for the DDABr-treated nanocrystal thin film. FigureS3-Spectroelectrochemistry (SEC) Spot2_SeriesSpec_1sT300x_0d0OD_late.asc: Contains the photoluminescence spectra measured as a function of time, used to prepare Figure S3a). Spot3_SeriesSpec_1sIT_600x_0d0OD.asc: Contains the photoluminescence spectra measured as a function of time, used to prepare Figure S3c). Spot3_SeriesSpec_300x1sIT_0OD.asc: Contains the photoluminescence spectra measured as a function of time, used to prepare Figure S3e). Spot3_SeriesSpec_1sIT300x_0d0OD_2.asc: Contains the photoluminescence spectra measured as a function of time, used to prepare Figure S3g). PL_ElectrolytesNEU.py: Contains a Python script used to process the four datasets and plot the datasets as contour plots in Figure S3a),c),e), and g). Figure S3b) is derived from the data shown in Figure S3a). Figure S3d) is derived from the data shown in Figure S3c). Figure S3f) is derived from the data shown in Figure S3e). Figure S3h) is derived from the data shown in Figure S3g). FigureS4-Spectroelectrochemistry (SEC) 1.txt: Contains the cyclic voltammetry data of PC/TBAHFP. 24.txt: Contains the cyclic voltammetry data of Fc/Fc+. PC_CV_Fc.py: Contains a Python script used to process the two datasets and plot the datasets in Figure S4. FigureS5-Spectroelectrochemistry (SEC) 69.txt: Contains the cyclic voltammetry data presented in Figure S5a). Spot3_SeriesSpec_300x1sIT_0OD_69.asc: Contains the photoluminescence spectra measured as a function of the Potential vs. Ag PRE (V). BspOAOAm1x_mitCV.py: Contains a Python script used to process the two datasets and plot the datasets as a 2D plot in Figure S5b). Figure S5c) and d) originate from that data. FigureS6-Spectroelectrochemistry (SEC) 75.txt: Contains the cyclic voltammetry data presented in Figure S6a). Spot3_SeriesSpec_1sIT300x_0d0OD_75.asc: Contains the photoluminescence spectra measured as a function of the Potential vs. Ag PRE (V). BspOAOAm2x_mitCV.py: Contains a Python script used to process the two datasets and plot the datasets as a 2D plot in Figure S6b). Figure S6c) and d) originate from that data. FigureS7-Spectroelectrochemistry (SEC) 32.txt: Contains the cyclic voltammetry data presented in Figure S7a). Spot3_SeriesSpec_1sIT_600x_0d0OD_32.asc: Contains the photoluminescence spectra measured as a function of the Potential vs. Ag PRE (V). BspDDABr2x_mitCV.py: Contains a Python script used to process the two datasets and plot the datasets as a 2D plot in Figure S7b). Figure S7c) and d) originate from that data. FigureS8-XPS File 'survey-120W.csv' in the folder 'CsPbBr3 NCs_DDABr' contains the XPS survey spectrum of DDABr NCs presented in Figure S8. File' survey-120w.csv' in the folder 'CsPbBr3 NCs_native' contains the XPS survey spectrum of native NCs presented in Figure S8. FigureS9-XPS File 'core levels.csv' in the subfolder 'CsPbBr3 NCs_DDABr' contains the XPS core level spectrum of DDABr NCs presented in Figure S9. File 'Br and Cs core levels.csv' in the subfolder 'CsPbBr3 NCs_native' contains the XPS core level spectrum for Br and Cs of native NCs presented in Figure S9. File 'Pb 4f-120W.csv' in the subfolder 'CsPbBr3 NCs_native' contains the XPS core level spectrum for Pb of native NCs presented in Figure S9. FigureS10-DFT CsPbBr3_oleate6_Cs_optimized.xyz: Contains the coordinate file for the nanocrystal with 6 hexanoates, in which the carboxylate oxygens are bonded to the Cs+ ions. CsPbBr3_oleate6_Pb_optimized.xyz: Contains the coordinate file for the nanocrystal with 6 hexanoates, in which the carboxylate oxygens are directly bonded to the Pb2+ sites. The coordinate files are in .xyz format and are in Angstrom units, which describes the position of the atoms (Cs/Pb/Br/C/H/N/O) in Cartesian space. HOMO_LUMO_sample.inp: sample input file for HOMO and LUMO calculation. description.docx: Contains information on how the data for Figure 8 was processed. FigureS11-Kelvin probe Files 'TPBi_Xnm.CPD' in the subfolder 'KP_DDABr' contain the contact potential difference (CPD) data measured by Kelvin probe as a function of the thickness of TPBi evaporated on DDABr nanocrystals. The 'X' in the filename indicates the TPBi layer thickness, ranging from 0 to 100 nm in 20 nm steps, deposited on the nanocrystals. The values shown in Figure S11 represent averages of the measured values. Files 'TPBi_Xnm.CPD' in the subfolder 'KP_Native' contain the CPD data measured by Kelvin probe as a function of the thickness of TPBi evaporated on native nanocrystals. The 'X' in the filename indicates the TPBi layer thickness, ranging from 0 to 100 nm in 20 nm steps, deposited on the nanocrystals. The values shown in Figure S11 represent averages of the measured values. FigureS12-LEDs PeLED_Native_TPBi.xls: Contains the LED characteristics of the PeLED incorporating native, unwashed NCs. This data was used to create Figure S12. PeLED_Native_washed.xls: Contains the LED characteristics of the PeLED incorporating native, washed NCs. This data was used to create Figure S12. FigureS13-LEDs ptaa_tpbi_EL.txt: Contains the EL spectrum of the PTAA/TPBi bilayer device. FigureS14-LEDs DDABr_PeLED_Lifetime.csv: Contains the operational lifetime data of a DDABr nanocrystal LED. Native_PeLED_Lifetime.csv: Contains the operational lifetime data of a native nanocrystal LED. 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