DOI: 10.5061/dryad.4b8gthtkq
title: Bridging length scales in organic mixed ionic-electronic conductors through internal strain and mesoscale dynamics

description: Understanding structural and dynamic properties of inherently disordered
 systems at the mesoscale is crucial. This is particularly important in
 organic mixed ionic-electronic conductors (OMIECs), which undergo
 significant and complex structural changes when operated in electrolyte.
 In this study, we investigate the mesoscale strain, reversibility, and
 dynamics of a model OMIEC material under external electrochemical
 potential using operando X-ray photon correlation spectroscopy. Our
 results reveal mesoscale strain and structural hysteresis that depend on
 the sample's cycling history, establishing a comprehensive kinetic
 sequence bridging the macroscopic and microscopic behaviors of OMIECs.
 Furthermore, we uncover equilibrium and non-equilibrium dynamics of charge
 carriers and material doping states, highlighting the unexpected coupling
 between charge carrier dynamics and mesoscale order. These findings
 advance our understanding of the structure-dynamics-function relationships
 in OMIECs, opening pathways for designing and engineering materials with
 improved performance and functionality in non-equilibrium states during
 device operation.
description: # Bridging length scales in organic mixed ionic-electronic conductors
 through internal strain and mesoscale dynamics
 In this dataset, we have
 incorporated the initial scattering patterns collected at beamline 8-ID-I
 (Advanced Photon Source, Argonne National Laboratory). The X-ray energy
 used for the measurements was 10.92 keV. The data was obtained through
 operando grazing incidence X-ray photon correlation spectroscopy (GIXPCS)
 using an optimized cone cell. ## Contact Information Name: R. Wu
 Affiliations: Department of Biomedical Engineering, Northwestern
 University, Evanston, IL, USA ORCID ID:
 Email:
 ## Description of the data and file
 structure The dataset is available in either the original H5 file format
 or a supplementary type encapsulated within zip files. These zip files
 encompass both the H5 files and data subjected to primary treatment. The
 experimental conditions are detailed within the filename. To illustrate
 with an example labeled
 "D224_Acid_PEDOT_Sample5_RbBr_step1_5_025C_att04_001.zip”, this
 dataset involves acid-treated PEDOT:PSS cycled in a 100mM RbBr solution at
 room temperature, using an attenuator identified as att4. The datasets
 starting with the letter "E" also represent measurements
 conducted on acid-treated PEDOT:PSS. However, in this case, the cycling
 was performed in a 100mM NaCl solution. The files and folders inside each
 zip file can be expressed by the following tree: SuppMats_Data \|--
 DXXX_SampleX_XXX_attX # Name of the example dataset \| |--
 AVGN_DXXX_SampleX_XXX_attX # Scattering pattern extracted from h5 file and
 averaged over each N (noted in "AVGN") frames. \| |-- Cut_r2c2 #
 Local cut of the diffuse scattering part on the second row and the second
 column. The area was defined as: DiffScat_xstart=1298; DiffScat_xend=1552;
 DiffScat_ystart=262; DiffScat_yend=515; \| |-- Sum # A further sum of the
 cutted frames \| |-- Iteration # This folder saves the result after each
 iteration \| |-- FinalAlign # This folder saves the result after the final
 iteration, sometimes this folder will be empty \| |-- XXIteration.mat #
 These MAT format files save the final alignment result as pixel shift \|
 |-- Cut_r2c3 # Local cut of the diffuse scattering part on the second row
 and the second column. The area was defined as: DiffScat_xstart=1298;
 DiffScat_xend=1552; DiffScat_ystart=522; DiffScat_yend=775, the subfolders
 inside are the same as r2c2; \| |-- DXXX_SampleX_XXX_attX.batchinfo #
 Measurement information of the dataset \| |-- DXXX_SampleX_XXX_attX.hdf #
 head file for h5 file, no use for data treatment \| |--
 DXXX_SampleX_XXX_attX.h5 # H5 file that can be treated with python or
 matlab code in the code pack \|-- DXXX_SampleX_XXX_attX # Name of another
 example dataset \|-- EXXX_SampleX_XXX_attX # Name of another example
 dataset, the letter "E" represent measurements conducted on
 acid-treated PEDOT:PSS in 100 mM NaCl For the .mat files
 (XXIteration.mat), each file includes two arrays: "Shiftx" and
 "Shifty". Both of them are 1D array of pixel shift to the first
 frame. For the .h5 files, the scattering pattern is in
 ['entry']['data']['data']. The file only
 have 'entry' category, under this is 'data' and
 'instrument' (for instrumental information). Under the
 'data', there is only another 'data' for data storage.
 ## Sharing/Access information The original data will also be posted on NU
 MRSEC DATA RETRIEVAL (NECTAR) later. ## Code/Software The Matlab and
 Python codes are provided in the associated Zenodo repository. For
 processing the original H5 files, it is recommended to utilize the
 attached code "XPCS alignment - multifolders.ipynb," which is
 included in the archive
 "Jupyter_notebook_for_alignment_and_fitting.zip." The Jupyter
 notebook is the preferred tool for alignment and fitting procedures. For
 users preferring Matlab, the alignment code is available in the
 "Matlab_Code_Pack_20220504.zip" archive. The alignment process
 is executed by running the command lines within the "Intotal.m"
 file. Please note that this version is the older one, predating the
 code's rewriting in Python. Following alignment, the final G-map is
 calculated and visualized using the command lines provided in the
 "Matlab_correlation.zip". Moreover, the comprehensive data
 treatment, including self-dynamics model fitting and additional data
 verification tools such as variance and Poisson distribution checks, are
 compacted within the
 "Jupyter_notebook_for_alignment_and_fitting.zip" package. Here
 is the information of the code included: SuppMats_Software \|-- Jupyter
 notebook for alignment and fitting \| |-- Export APS Lambda 2M as TIFs
 v1.ipynb # Export the H5 file to tiff files \| |-- XPCS alignment -
 multifolders.ipynb # Further cut the tiff files and align the diffuse
 scattering region \| |-- XPCS alignment - skimage_224.ipynb # Align the
 diffuse scattering region using skimage package \| |-- variance-SI.ipynb #
 Variance check of the pattern \| |-- Poisson Distribution Cycle
 Multipic.ipynb # Poisson distribution check of the pattern \| |-- Fitting
 g2 - Multi (D224) - Averaged - Redope - Lim - Corrected - diag.ipynb #
 Self-dynamics model fitting using diagonal cut \| |-- Fitting g2 - Multi
 (D224) - Averaged - Redope - Lim - Corrected.ipynb # Self-dynamics model
 fitting using average cut \| |-- Figure 5 spinodal
 model_cubic_R_decay_plot.ipynb # Langevin model B diagram for Figure 5 \|
 |-- XPCS Stack XXXXX.ipynb # Data visualization \|-- Matlab_correlation \|
 |-- g2Correlation_XXX.m # G map calculation \| |-- Plot_G2_Map - XXX.m # G
 map visualization \|-- Intotal.m # This is the Matlab command line to
 align the diffuse scattering region \|-- Code Pack 20220504 # This code
 pack will be called in "Intotal.m" for Matlab alignment