DFT dataset of phlogopite K(Mg,Fe)3Si3AlO10(OH)2 monolayers

The present dataset is related to the monolayer structures of phlogopite (Phl), whose chemical formula is K(Mg,Fe)3Si3AlO10(OH)2, with Mg/Fe ratio >= 2, which were investigated within the Density Functional Theory (DFT) framework. The objective was to characterise the effects of divalent iron (Fe2+) in place of magnesium cations (Mg2+) in the octahedral sheet of the single layer of the mineral on the 2D crystal structure, electronic and vibrational properties.

All the DFT simulations were carried out using the CRYSTAL code (https://www.crystal.unito.it/). This dataset reports both the input and output files produced during the simulations.

Three models were considered: (1) a stoichiometric KMg3Si3AlO10(OH)2 phlogopite monolayer, labelled as Phl-Fe0-ML; (2) a phlogopite model with a single Fe2+/Mg2+ substitution, with chemical formula KMg2.5Fe0.5Si3AlO10(OH)2 (model Phl-Fe1-ML); (3) a phlogopite model with two single Fe2+/Mg2+ substitutions in the octahedral sheet, with chemical formula KMg2FeSi3AlO10(OH)2 (model Phl-Fe2-ML).

The data are subdivided between each model and are organized as follows. The folder of each phlogopite monolayer (Phl-Fe0-ML, Phl-Fe1-ML and Phl-Fe2-ML) contains these sub-folders:

- Band structure --> contains the electronic band structure of the mineral single layer;

- Density of states --> contains the atom-projected (suffix "_atoms" in the file name) and shell-projected (suffix "_XX" in the file name, with "XX" being the name of the atom whose shells were considered) density of states (PDOS) calculated for the monolayer;

- Hirshfeld charges --> contains the calculation of the atomic charges (valence state) for the atoms in the structure, which was performed using a iterative Hirshfeld population analysis;

- Structure --> contains the relaxed monolayer structure and the associated wavefunction (file with extension ".f9") obtained with CRYSTAL;

- Spin-polarized --> (only for Phl-Fe1-ML and Phl-Fe2-ML models) contains the spin-polarized self-consistent field (SCF) calculation of the wavefunction of the mineral monolayrt , which was employed for the calculation of the electronic properties;

- Topond --> contains the analysis of the topological analysis of the electron density, which was used to characterise the type of bonds between the atoms in the monolayer structures;

- Vibrational properties --> contains the calculated vibrational frequencies (file with extension ".out") that can be visually inspected using the Moldraw software (http://www.moldraw.unito.it) and the calculated infrared (IR) and Raman spectra of the mineral single layer.

本数据集涉及金云母（Phlogopite, Phl）的单层结构，其化学式为K(Mg,Fe)₃Si₃AlO₁₀(OH)₂，且Mg/Fe比值≥2，相关研究基于密度泛函理论（Density Functional Theory, DFT）框架开展。研究目标是表征矿物单层八面体片层中二价铁离子（Fe²+）取代镁阳离子（Mg²+）对二维晶体结构、电子及振动性质的影响。

所有DFT模拟均使用CRYSTAL程序（https://www.crystal.unito.it/）完成。本数据集包含模拟过程中产生的全部输入与输出文件。

本次研究共考虑三类模型：(1) 化学计量比为KMg₃Si₃AlO₁₀(OH)₂的金云母单层，标记为Phl-Fe0-ML；(2) 存在一处Fe²+/Mg²+取代的金云母模型，化学式为KMg₂.5Fe0.5Si₃AlO₁₀(OH)₂（模型编号Phl-Fe1-ML）；(3) 八面体片层中存在两处独立Fe²+/Mg²+取代的金云母模型，化学式为KMg₂FeSi₃AlO₁₀(OH)₂（模型编号Phl-Fe2-ML）。

数据按模型分类，组织形式如下。每个金云母单层（Phl-Fe0-ML、Phl-Fe1-ML及Phl-Fe2-ML）的文件夹均包含以下子文件夹：
- 能带结构（Band structure）：存储该矿物单层的电子能带结构数据；
- 态密度（Density of states）：存储针对该单层计算得到的原子投影态密度（文件名后缀为"_atoms"）与壳层投影态密度（文件名后缀为"_XX"，其中"XX"为对应原子的壳层标识），两类数据均为投影态密度（PDOS）；
- Hirshfeld电荷：存储通过迭代Hirshfeld布居分析计算得到的结构中各原子的原子电荷（价态）；
- 结构文件（Structure）：存储经CRYSTAL程序优化得到的弛豫后单层结构及其关联的波函数文件（扩展名为".f9"）；
- 自旋极化计算（Spin-polarized，仅适用于Phl-Fe1-ML与Phl-Fe2-ML模型）：存储针对该矿物单层波函数的自旋极化自洽场（SCF）计算结果，该结果用于后续电子性质的计算；
- Topond：存储电子密度拓扑分析结果，用于表征该单层结构中原子间的键合类型；
- 振动性质（Vibrational properties）：存储计算得到的振动频率数据（扩展名为".out"，可通过Moldraw软件（http://www.moldraw.unito.it）可视化查看），以及该矿物单层的红外（IR）与拉曼光谱计算结果。