Protected ultrathin cuprous oxide film for photocatalysis: Excitation and relaxation dynamics

Name: Protected ultrathin cuprous oxide film for photocatalysis: Excitation and relaxation dynamics
Creator: Zenodo
Published: 2023-03-28T13:32:40+08:00

Zenodo2023-03-28 更新2026-05-26 收录

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The main data analysis was done with Wavemetrics Igor Pro 7.08 using user-defined macros. Data files given in *.itx format are human-readable text files that can be opened in Igor Pro. User-defined macros are available from the authors upon reasonable request. Static spectra are measured with the proprietary "Croissant" software for the channeltron analyzer and saved in human-readable *.plsp format, or SpecsLab Prodigy 4.60.1 for the 2D analyzer and saved in the proprietary SPECS *.sle format or exported into *.itx format. Time-resolved spectra are measured with a proprietary LabView program and exported in the binary HDF5 *.h5 file format. ******************************************** Fig. 1 LEED and He Ia ARPES ******************************************** LEED images taken with SBIG STF-8300 CCD Camera, the SBIG format is a 16-bit grayscale bitmap with metadata. Fig. 1a: LEED image at 120 eV LEED220210_120eV_Cu111_hBN_Cu2O.SBIG Fig. 1b: LEED image at 48 eV LEED220210_048eV_Cu111_hBN_Cu2O.SBIG other energies (not shown in the figure): see Fig. S2/S3 Fig. 1c: He Ia spectrum second derivative as function of parallel momentum and binding energy Spectra measured with VG ESCALAB 220 channeltron hemispherical analyzer by tilting the sample at two fixed azimuthal angles and using a Gammadata VUV 5050 monochromated helium lamp. The azimuthal angles correspond to the M and K directions, respectively, as determined by x-ray photoelectron diffraction of the Cu(111) surface. Measurement parameters are given in the files. Positive parallel momentum: M direction, VG2Z220628N015.plsp Negative parallel momentum: K direction, VG2Z220628N016.plsp Combined ARPES spectrum as a function of parallel momentum and binding energy: VG2Z220628N015_N016.itx Second derivative along energy direction: VG2Z220628N015_N016d.itx; smoothed: VG2Z220628N015_N016d_smth.itx ************************************************ Fig. 2 He IIa ARPES ************************************************ All ARPES spectra measured with SPECS Phoibos 150 WAL hemispherical analyzer (2D detector) using SpecsLab Prodigy software and non-monochromated helium lamp. Fig. 2a: Detail of He IIa spectrum measured on h-BN/Cu(111) Full angle-resolved spectrum (intensity as function of angular coordinate and kinetic energy), summed over all energy channels and scans, exported from SpecsLab Prodigy as Igor Text. All measurement parameters are given in the file. Spectrum HeIIa h-BN Cu111 20201023.itx Spectrum scale converted into parallel momentum and binding energy: Spectrum HeIIa h-BN Cu111 20201023 k2.itx Fig. 2b: Detail of He IIa spectrum measured on h-BN/Cu2O/Cu(111) Full angle-resolved spectrum (intensity as function of angular coordinate and kinetic energy), summed over all energy channels and scans, exported from SpecsLab Prodigy as Igor Text. All measurement parameters are given in the file. Spectrum HeIIa h-BN Cu2O Cu111 20220211.itx Spectrum scale converted into parallel momentum and binding energy: Spectrum HeIIa h-BN Cu2O Cu111 20220211 k2.itx Fig. 2c: Spectra integrated over given parallel momentum range Intensity as a function of binding energy Spectrum HeIIa h-BN Cu111 20201023 k2 042_092.txt Spectrum HeIIa h-BN Cu2O Cu111 20220211 k2 041_091.txt ************************* Fig. 3 2PPE spectra of Cu(111), h-BN/Cu(111) and h-BN/Cu2O/Cu(111) ************************* Spectra measured with SPECS Phoibos 150 WAL hemispherical analyzer (2D detector) using SpecsLab Prodigy software and exported as Igor Text. All measurement parameters are given in the files. 3eV wavelength was 412nm, p-polarized. A -10V bias voltage was applied to the sample. Cu(111) 2PPE: P=1mW, Cu111 2022-04-14_20h47m45s.itx Cu(111) 3PPE: P=3mW, Cu111 2022-04-14_21h09m29s.itx h-BN/Cu(111) 2PPE: P=1.0mW, 0.5mm entrance slit, Cu111 hBN Spectrum3eV_2B_ppol.itx h-BN/Cu(111) 3PPE: P=0.4mW, 3.0mm entrance slit, Cu111 hBN Spectrum3eV_4B_ppol.itx h-BN/Cu2O/Cu(111) 2PPE: P~0.1mW, Cu111 hBN Cu2O 2022-02-11_17h07m34s.itx h-BN/Cu2O/Cu(111) 3PPE: P~0.1mW, Cu111 hBN Cu2O 2022-02-11_16h58m49s.itx ************************************************* Fig. 4 Delay Scan ************************************************* Delay scans are recorded with proprietary LabView software and saved in binary HDF5 format as a 3D stack of detector images (intensity as function of angular coordinate and kinetic energy) as a function of pump-probe delay. Bias -5V, 3eV=413nm 0.3mW p-pol, 6eV=208nm 1nA p-pol, Ekin=11.9eV, Epass=20eV, 1mm slit, exposure 10x500ms, 20 scans, 10fs steps Raw data, 256 angular pixels x 348 energy pixels x 201 delays x 20 scans: WAL_20220215_UZH_JB_dscan_040_0to9.h5 WAL_20220215_UZH_JB_dscan_040_10to19.h5 Sum of all scans (transposed): WAL_20220215_UZH_JB_dscan_040_sum.h5 Cropped to active detector window and applied distortion correction and correct scaling: dscan_20220215_040_data3Dcorrected.h5 Integrated over +-10° angular window: dscan040.itx Background averaged over delay positions 0-19 subtracted and energy and delay scales corrected: Fig. 4a: dscan040bgi0.itx Delay scan with 50ps range and 0.2ps steps, not shown in figure but analyzed the same way: dscan041bgi.itx Fig. 4b: Intensity as a function of intermediate state energy 50 fs, delay positions 40-50: dscan040t0mbg.txt 1 ps, delay positions 140-150: dscan040t2mbg.txt 10 ps, delay positions 55-65 in dscan041bgi: dscan041t3mbg.txt Fig. 4c: detector image obtained by averaging images at delay positions 40-50 and subtracting the background image, then correcting the angular distortion by normalizing the intensity at the Fermi energy dscan040image_diff0.itx ************************************************* Fig. 5 Fit Curves ************************************************* The Igor Pro batch fitting procedure was used with a custom fitting function to fit the delay scan dscan040bgi binned in 0.1 eV intervals with index 0 at -0.3 eV. The displayed curves have index 13 (1.0 eV), 6 (0.3 eV) and 4 (0.1 eV). Binned delay scan: dscan040bgi_pix.itx Fit parameters: dscan040bgi_fitparams.txt Fit result: dscan040bgi_pixRateFits.itx Fast component: dscan040bgi_FastComponent.itx Slow component: dscan040bgi_SlowComponent.itx ******************************************* Fig. 6 Fit Results Comparison ******************************************* Relaxation times are extracted from the batch fit results of different delay scans. 3 nJ pump: dscan040bgi_fitparams.txt dscan_220215_040 20 nJ pump: dscan010_BG4_fitparams.txt dscan220703_010 (data: dscan010_BG4.itx, binned: dscan010_BG4_pix.itx, fits: dscan010_BG4_pixFit.itx) h-BN/Cu(111): dscan033_fitparams.txt (binned data: dscan044_hBN_side_pix1.itx, fits: dscan033_hBN_side_pixFits.itx) Lisowski et al.: LifetimesLisowski.txt (data from M. Lisowski, P. A. Loukakos, U. Bovensiepen, and M. Wolf, Femtosecond Dynamics and Transport of Optically Excited Electrons in Epitaxial Cu Films on Si(111)-7 x 7, Appl. Phys. A 79, 739 (2004)) Extrapolation: fit_LifetimesLisowski.txt, using power law tau=0.054797*E^(-1.1419) **************************************************** Fig. S1 XPS **************************************************** Preparation 1 before oxidation: Preparation 1 after oxidation: Preparation 2 after oxidation: B 1s: VG2Z220209N005.pesp B 1s: VG2Z220210N023.pesp B 1s: VG2Z220628N002.pesp N 1s: VG2Z220209N006.pesp N 1s: VG2Z220210N024.pesp N 1s: VG2Z220628N003.pesp C 1s: VG2Z220209N007.pesp C 1s: VG2Z220210N025.pesp C 1s: VG2Z220628N004.pesp O 1s: VG2Z220209N008.pesp O 1s: VG2Z220210N026.pesp O 1s: VG2Z220628N005.pesp Cu 2p:VG2Z220209N009.pesp Cu 2p:VG2Z220210N027.pesp Cu 2p:VG2Z220628N006.pesp **************************************************** Fig. S2 LEED **************************************************** 48 eV: LEED220209_048eV_Cu111_hBN.SBIG 70 eV: LEED220209_070eV_Cu111_hBN.SBIG 100 eV: LEED220209_100eV_Cu111_hBN.SBIG not shown in figure: 40 eV: LEED220209_040eV_Cu111_hBN.SBIG 120 eV: LEED220209_120eV_Cu111_hBN.SBIG **************************************************** Fig. S3 LEED **************************************************** 40 eV: LEED220210_040eV_Cu111_hBN_Cu2O.SBIG 48 eV: LEED220210_048eV_Cu111_hBN_Cu2O.SBIG 70 eV: LEED220210_070eV_Cu111_hBN_Cu2O.SBIG 100 eV: LEED220210_100eV_Cu111_hBN_Cu2O.SBIG 120 eV: LEED220210_120eV_Cu111_hBN_Cu2O.SBIG 150 eV: LEED220210_150eV_Cu111_hBN_Cu2O.SBIG **************************************************** Fig. S4 LEED **************************************************** 40 eV: LEED220628_040eV_Cu111_hBN_Cu2O.SBIG 48 eV: LEED220628_048eV_Cu111_hBN_Cu2O.SBIG 70 eV: LEED220628_070eV_Cu111_hBN_Cu2O.SBIG 100 eV: LEED220628_100eV_Cu111_hBN_Cu2O.SBIG 110 eV: LEED220628_110eV_Cu111_hBN_Cu2O.SBIG 140 eV: LEED220628_140eV_Cu111_hBN_Cu2O.SBIG 180 eV: LEED220628_180eV_Cu111_hBN_Cu2O.SBIG not shown in figure: 120 eV: LEED220628_120eV_Cu111_hBN_Cu2O.SBIG 150 eV: LEED220628_150eV_Cu111_hBN_Cu2O.SBIG ********************************************* Fig. S5 Work function maps ********************************************* Ekin=10.4eV, Epass=20eV, 6eV=208.5nm 0.2nA p-pol, 1mm slit, -5V bias, exposure 1x500ms, 0.1mm steps, 81x81 pixels Preparation 1: Data cube after lens correction and correct scaling: dscan_220221_003_data3Dcorrected.h5 Integrated over all angles and brought into raster format: dscan_220221_003_raster.h5 Work function map: dscan_220221_003_rasterWF.itx Inset: Photograph of the sample after preparation 1, "Photograph hBN Cu2O Cu.png" Preparation 2: Data cube after lens correction and correct scaling: dscan_220704_011_data3Dcorrected.h5 Integrated over all angles: dscan_220704_011_raster.h5 Work function map: dscan_220704_011_rasterWF.itx ************************************************ Fig. S6 Delay Scans ************************************************ See description of Fig. 4 for processing details. Pump power was measured with a thermal powermeter and probe power was measured with a Thorlabs SM05PD7A GaP-photodiode with 14.4 mA/W sensitivity at 208nm. The thermal powermeter has an accuracy of +-0.1mW. 1.0mW pump power at 100kHz repetition rate equals 10nJ pulse energy. 1.0nA photodiode current equals approximately 70nW probe power or 0.7 pJ probe energy. Common settings: Bias voltage -5V, exposure time 20x500ms, 20 scans, 20fs steps, entrance slit size 1mm, Pass energy 20eV, Kinetic energy 11.9 eV, pump wavelength 413nm, pump and probe beam are p-polarized. Differing settings are written for each dataset. Fig. S6a: dscan_220215_040/dscan040bgi0.itx, processed raw data: dscan_220215_040_data3Dcorrected.h5 0.3mW pump, 208nm 1.0nA probe, 10fs steps, exposure 10x500ms Fig. S6b: dscan_220217_045/dscan045bgi.itx, processed raw data: dscan_220217_045_data3Dcorrected.h5 0.3mW pump, 208nm 1.0nA probe, 10fs steps, Ekin=13.3eV, Epass=30eV, 7mm slit, 50 scans Fig. S6c: dscan_220216_041/dscan041bgi.itx, processed raw data: dscan_220216_041_data3Dcorrected.h5 0.3mW pump, 208nm 1.0nA probe, 200fs steps, exposure 10x500ms, 10 scans ************************************************ Fig. S7 Delay Scans ************************************************ Common settings: same as in Fig. S6 Fig. S7a: dscan_220701_020/dscan020bgi0.itx, processed raw data: dscan_220701_020_data3Dcorrected.h5 0.5mW pump, 209nm 0.9nA probe, 3mm slit Fig. S7b: dscan_220712_029/dscan029_BG.itx, processed raw data: dscan_220712_029_data3Dcorrected.h5 1.5mW pump, 209nm 1.0nA probe Fig. S7c: dscan_220703_010/dscan010_BG4.itx, processed raw data: dscan_220703_010_data3Dcorrected.h5 2.0mW pump, 209nm 0.9nA probe Fig. S7d: dscan_220417_033/dscan033_hBN_side0.itx, processed raw data: dscan_220417_033_data3Dcorrected.h5 1.0mW pump, 208nm 0.1nA probe, Ekin=11.8eV, 40 scans *********************************************** Fig. S8 Beam profiles *********************************************** 8-bit CCD images were acquired with a Basler puA1280-54um CCD camera and Basler pylonViewer 5.0 acquisition software. Sensor resolution: 1280x960, pixel size: 3.75x3.75 micrometers 3 eV image: 10 microseconds exposure time, Spot3eV 10us 20mm.bmp 6 eV image: 100 milliseconds exposure time, Spot6eV 100ms 20mm.bmp

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Zenodo

创建时间：

2023-03-28

Protected ultrathin cuprous oxide film for photocatalysis: Excitation and relaxation dynamics

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