附件G：AuCuI（）化合物无序化过程的合金基因浓度跟踪研究

G.1　混合焓实验路径的合金基因浓度跟踪法

对于给定成分的合金，由等有序度Gibbs能平衡路径法获得最小Gibbs能（）-T路径（见图G.1（a）），在平衡等有序度（-T）网络图中绘制（-T ）亚平衡路径（见图G.1（b）），随后相继获得混合Gibbs能（-T ）（见图G.1（c）），有序度（σ-T ）（见图G.1（d））、合金基因浓度（（-T）（见图G.2）和其他性质s,x（qs,x-T）亚平衡全息网络路径图（见图G.3～G.18）[6]：（-T）→（-T）→（σ-T）→（（）-T）→（q-T）s,xs,xs,x

图G.1　AuCuI（）化合物无序化的EHNP和SHNP路径图Fig.G.1　EHNP- and SHNP-charts on disordering AuCuI（）：（a）Minimal mixed Gibbs energy-Tpath obtained by iso-order degree Gibbs energy equilibrium path method；（b）Experimental mixed enthalpy-T path method based on network chart of iso-order degree mixed enthalpies equilibrium paths, attaching equilibrium-T path；（c）（OABC）and（Oabc）paths of equilibrium and subequilibrium order→disorder transitions, wheredenoting superheated driving Gibbs energy；（d）σe（OABCD）and σs（OabcD）paths of equilibrium and subequilibrium order→disorder transitions, where Δσhdenoting hysteresis order degree

（To be continued）

图G.2 AuCuI（）化合物无序化的合金基因浓度跟踪图Fig.G.2 AG-concentration SHNP charts on disordering AuCuI（）：（a）, （b）Three-dimension-T-i and-T-i SHNP charts；（c）, （d）Two-dimension iso-order degree-i and-i SHNP charts；（e）, （f）Two-dimension iso-Gibbs energy level-σ and-σ SHNP charts

图 G.3 AuCuI（）化合物无序化时载有平衡和亚平衡路径的ΔGm-平衡全息网络路径图Fig.G.3 EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension mixed Gibbs energy ΔGm-T-σ EHNP chart with-T and-T paths；（b）-T and-T　paths

图 G.4 AuCuI（）化合物无序化时载有平衡和亚平衡路径的-平衡全息网络路径图Fig.G.4　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension mixed characteristic Gibbs energy ΔG∗m-T-σ EHNP chart with-T and-T paths；（b）-T　and-T paths

图G.5 AuCuI（）化合物无序化时载有平衡和亚平衡路径的ΔHm-平衡全息网络路径图Fig.G.5　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension mixed enthalpy ΔHm-T-σ EHNP chart with-T and-T paths；（b）-T and-T　paths

图G.6　AuCuI（）化合物无序化时载有平衡和亚平衡路径的ΔEm-平衡全息网络路径图Fig.G.6　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension mixed potential energy ΔEm-T-σ EHNP chart with-T and-T paths；（b）-T and-T　paths

图G.7 AuCuI（）化合物无序化时载有平衡和亚平衡路径的ΔVm-平衡全息网络路径图Fig.G.7　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension mixed volume ΔVm-T-σ EHNP chart with-T and-T paths；（b）-T and-T　paths

图G.8　AuCuI（）化合物无序化时载有平衡和亚平衡路径的Sc-平衡全息网络路径图Fig.G.8　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension configurational entropy Sc-T-σ EHNP chart with-T and-T paths；（b）-T and-T paths

图 G.9 AuCuI（）化合物无序化时载有平衡和亚平衡路径的ΔUm.v-平衡全息网络路径图Fig.G.9 EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension generalized vibration energy-T-σ EHNP chart with-T and-T paths；（b）-T　and-T paths

图G.10 AuCuI（）化合物无序化时载有平衡和亚平衡路径的ΔSv-平衡全息网络路径图Fig.G.10　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension generalized vibration entropy ΔSv-T-σ EHNP chart with-T and-T paths；（b）-T and-T paths

图 G.11 AuCuI（）化合物无序化时载有平衡和亚平衡路径的TSc-平衡全息网络路径图Fig.G.11　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension configurational entropy energy TSc-T-σ EHNP chart with-T and-T paths；（b）-T and-T paths

图G.12　AuCuI（）化合物无序化时载有平衡和亚平衡路径的TΔSv-平衡全息网络路径图Fig.G.12　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension generalized vibration entropy energy TΔSv-T-σ EHNP chart with-T and-T paths；（b）-T　and-T paths

图 G.13　AuCuI（）化合物无序化时载有平衡和亚平衡路径的ΔXv-平衡全息网络路径图Fig.G.13　EHNP charts with EHNP and SHNP curves of the first order thermodynamic properties on disordering AuCuI（）：（a）Three-dimension generalized vibration free energy ΔXv-T-σ EHNP chart with-T and-T paths；（b）-T　and-T paths

图G.14　AuCuI（）化合物无序化时载有平衡和亚平衡路径的c-x-T平衡全息网络路径图pFig.G.14　The second order thermodynamic properties （heat capacity）on disordering AuCuI（）：（a）-T and-T　paths on cp-x-T EHNP diagram；（b）-T and-T paths

图G.15　AuCuI（）化合物无序化时载有平衡和亚平衡路径的c-T-σ平衡全息网络路径图pFig.G.15　The second order thermodynamic properties （heat capacity）on disordering AuCuI（）：（a）-T and-T　paths on c-T-σ EHNP diagram；（b）-σ and-σ pathsp

图 G.16　AuCuI（）化合物无序化时载有平衡和亚平衡路径的热膨胀α-x-T平衡全息网络路径图Fig.G.16　The second order thermodynamic properties （thermal expansion coefficient）on disordering AuCuI（）：（a）αe-T　and αs-T paths on α-x-T EHNP chart；（b）αe-T and αs-T paths

图 G.17 AuCuI（）化合物无序化时载有平衡和亚平衡路径的热膨胀α-T-σ平衡全息网络路径图Fig.G.17　The second order thermodynamic properties （thermal expansion coefficient）on disordering AuCuI（）：（a）αe-T　and αs-T paths on α-T-σ EHNP diagram；（b）αe-σ and αs-σ paths

（To be continued）

图G.18　AuCuI（）化合物无序化时载有平衡和亚平衡路径的活度a-平衡全息网络路径图Fig.G.18　Activities on disordering AuCuI（）：（a）, （b）-T,-T and-T,-T paths on aAu-x-T and aCu-x-T EHNP diagrams；（c）, （d）-T,-T and-T,-T paths；（e）, （f）-T,-T and-T ,-T paths on a-T-σ and a-T-σ EHNP charts；（g,h）-σ,-σ and-σ,-σAuCupaths

G.2　AuCuI（）无序化路径分析[6]

我们采用实验生成焓路径的合金浓度跟踪法，确定了AuCuI（）化合物的统计非均匀亚平衡和递次性有序一无序转变路径：AuCuI（）→AuCu（H）→PTP-AuCu →SPAP-AuCu（L）→AuCu（D）。该路径的动力学特征与加热速度的关系受RA-SA机制、过热驱动Gibbs能、跳变有序度，以及高温时原子一空位移动机制等控制：

1）当0≤T＜Tonset（593 K）时，它是有序度不变的AuCuI（）亚稳期。

2）当Tonset＜T≤620 K，1.000＞σs≥0.990时，它是高有序度合金AuCu（H）的生长期（见图9（a）和（b））。它具有晶胞尺度的不均匀性：含有较多的3（RA-SA）晶胞的早期一（RA-SA）晶胞区，含有较少的3（RA-SA）晶胞的中期一（RA-SA）晶胞区，没有3（RA-SA）晶胞的晚期一AuCuI（）晶胞区（见图G.19（c））。

3）当620 K＜T≤650 K，0.990＞σs≥0.925时，它是统计周期反向（SPAP）AuCuII区的生长期（见图9（c）和（d））。它具有区域尺度的不均匀性：含有较多的3（RA-SA）晶胞的原早期一（RA-SA）晶胞区成长为早期一（SPAP）-AuCuII区，含有较少的3（RA-SA）晶胞的原中期一（RA-SA）晶胞区成长为含有较多的3（RA-SA）晶胞的中期一（RA-SA）晶胞区，原晚期一AuCuI（）晶胞区成长为含有较少的3（RA-SA）晶胞的晚期一（RA-SA）晶胞区（见图G.19（d））。此时，亚平衡合金具有区域尺度的不均匀性：AuCu（H）区和SPAP-AuCuII区共存，它可称之为“伪二相（PTP）”AuCu合金。

4）当650 K＜T＜683 K，0.925＞σs＞0.807时，它是SPAP-AuCuII合金的成熟期（见图9（e）和（f））。在此阶段，SPAP-AuCuII合金含有早期一，中期一和晚期一（SPAP）-AuCuII区。

5）当0.807≥σs≥0.786时，它是SPAP-AuCuII合金的跳变期（见图9（g）和（h））。在此阶段，跳变合金基因浓度呈现最大“涌现”现象。跳变温度Tj由跳变有序度和过热驱动Gibbs能决定，后者与加热速度有关。

6）当0.4545≥σs＞0时，它是低有序度AuCu（L）合金的存在期（见图9（g）和（h））。当σs=0时，即T≥Tc（683 K），合金AuCu（D）处于无序状态。

图 G.19　AuCuI（）化合物无序化时3（RA-SA）机制和晶胞尺度与区域尺度不均匀性简图Fig.G.19　The 3（RA-SA）mechanism and schemes of cell-scale and region-scale heterogeneities on disordering AuCuI（）：（a）AG arranging structure after A-manner alternating in 3（RA-SA）mechanism of threepairs in a single cell；（b）AG arranging structure after B-manner alternating in 3（RA-SA）mechanism of threepairs in a single cell；（c）AuCu（H）alloy containing three regions with cell-scale heterogeneity；（d）PTP-[AuCuI（H）+PAP-AuCuII] alloy containing three regions with region-scale heterogeneity；（e）AG arranging structure of a early SPAP-AuCuII cell

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