高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (5): 950.doi: 10.7503/cjcu20190038
收稿日期:
2019-01-14
出版日期:
2019-04-17
发布日期:
2019-04-17
作者简介:
联系人简介: 王长生, 男, 博士, 教授, 博士生导师, 主要从事理论与计算化学研究. E-mail:
基金资助:
LI Xiaolei, WANG Changsheng*()
Received:
2019-01-14
Online:
2019-04-17
Published:
2019-04-17
Contact:
WANG Changsheng
E-mail:chwangcs@lnnu.edu.cn
Supported by:
摘要:
将水分子视为由2个O—H键偶极构成, 再将水分子间的三体作用视为长程诱导作用和短程校正之和, 使用Thole模型计算长程诱导作用, 通过同时考虑不同水分子间的置换和同一个水分子中2个键偶极间的置换计算短程校正, 从而提出了一个可快速计算水团簇三体作用强度的新方法. 根据已报道的12347个水三聚体的结构和CCSD(T)三体作用能, 确定了该方法所需参数. 将该方法和所确定的参数应用于67个水团簇体系, 计算这些体系的三体作用能, 并与CCSD(T), MP2, M06-2X方法的计算结果进行比较. 结果表明, 相对于CCSD(T)方法的总三体作用能, 本文方法的均方根偏差(RMSD)仅为3.32 kJ/mol, 平均相对偏差(MRD)仅为2.43%; 对较大水团簇体系, 该方法计算精度稍优于MP2方法, 明显优于M06-2X方法, 并且更快捷高效.
中图分类号:
TrendMD:
李晓蕾, 王长生. 可快速计算水团簇三体作用强度的新方法. 高等学校化学学报, 2019, 40(5): 950.
LI Xiaolei,WANG Changsheng. Rapid Calculation of the Three-body Interaction Energies in Water Clusters†. Chem. J. Chinese Universities, 2019, 40(5): 950.
No. | Cluster | Ref. | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
---|---|---|---|---|---|---|---|---|---|---|---|
E3B | Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | ||||
1 | 3w-1a | -5.82c | -5.77 | 0.05 | 0.86 | -5.65 | 0.17 | 2.92 | -5.77 | 0.05 | 0.86 |
2 | 3w-1b | 4.52c | 4.35 | -0.17 | 3.76 | 5.36 | 0.84 | 18.58 | 4.85 | 0.33 | 7.30 |
3 | 3w-1c | -10.13c | -10.29 | -0.16 | 1.58 | -11.34 | -1.21 | 11.94 | -10.00 | 0.13 | 1.28 |
4 | 4w-1 | -25.82d | -25.94 | -0.12 | 0.46 | -26.53 | -0.71 | 2.75 | -25.27 | 0.55 | 2.13 |
5 | 4w-2 | -24.73d | -24.85 | -0.12 | 0.49 | -25.23 | -0.50 | 2.02 | -24.60 | 0.13 | 0.53 |
6 | 4w-3 | -15.40d | -16.11 | -0.71 | 4.61 | -19.04 | -3.64 | 23.64 | -14.64 | 0.76 | 4.94 |
7 | 5w-1 | -37.95d | -37.87 | 0.08 | 0.21 | -36.90 | 1.05 | 2.77 | -38.41 | -0.46 | 1.21 |
8 | 5w-2 | -31.46d | -32.22 | -0.76 | 2.42 | -32.38 | -0.92 | 2.92 | -30.84 | 0.62 | 1.97 |
9 | 5w-3 | -26.57d | -27.82 | -1.25 | 4.70 | -29.71 | -3.14 | 11.82 | -27.07 | -0.50 | 1.88 |
10 | 5w-4 | -24.85d | -25.94 | -1.09 | 4.39 | -27.95 | -3.10 | 12.47 | -24.27 | 0.58 | 2.33 |
11 | 5w-5 | -24.18d | -25.31 | -1.13 | 4.67 | -26.07 | -1.89 | 7.82 | -23.30 | 0.88 | 3.64 |
12 | 5w-6 | -26.07d | -26.53 | -0.46 | 1.76 | -26.32 | -0.25 | 0.96 | -24.48 | 1.59 | 6.10 |
13 | 5w-7 | -25.94d | -26.36 | -0.42 | 1.62 | -26.48 | -0.54 | 2.08 | -25.06 | 0.88 | 3.39 |
14 | 6w-prism | -36.40d | -38.07 | -1.67 | 4.59 | -37.99 | -1.59 | 4.37 | -37.91 | -1.51 | 4.15 |
15 | 6w-cage | -37.53d | -38.99 | -1.46 | 3.89 | -40.29 | -2.76 | 7.35 | -38.07 | -0.54 | 1.44 |
16 | 6w-book1 | -43.43d | -43.76 | -0.33 | 0.76 | -42.97 | 0.46 | 1.06 | -43.22 | 0.21 | 0.48 |
17 | 6w-book2 | -42.30d | -42.84 | -0.54 | 1.28 | -41.21 | 1.09 | 2.58 | -41.80 | 0.50 | 1.18 |
18 | 6w-bag | -43.30d | -44.10 | -0.80 | 1.85 | -41.59 | 1.71 | 3.95 | -41.59 | 1.71 | 3.95 |
19 | 6w-chair | -49.29d | -49.08 | 0.21 | 0.43 | -48.53 | 0.76 | 1.54 | -51.13 | -1.84 | 3.73 |
20 | 6w-boat1 | -47.45d | -47.36 | 0.09 | 0.19 | -46.28 | 1.17 | 2.47 | -49.08 | -1.63 | 3.44 |
21 | 6w-boat2 | -47.45d | -47.40 | 0.05 | 0.11 | -46.32 | 1.13 | 2.38 | -49.41 | -1.96 | 4.13 |
RMSD | 0.74 | 1.68 | 1.02 | ||||||||
MAD | 1.67 | 3.64 | 1.96 | ||||||||
MRD(%) | 2.12 | 6.11 | 2.86 |
Table 1 Calculated total three-body interaction energies(E3B) of 21 small water clustersa
No. | Cluster | Ref. | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
---|---|---|---|---|---|---|---|---|---|---|---|
E3B | Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | ||||
1 | 3w-1a | -5.82c | -5.77 | 0.05 | 0.86 | -5.65 | 0.17 | 2.92 | -5.77 | 0.05 | 0.86 |
2 | 3w-1b | 4.52c | 4.35 | -0.17 | 3.76 | 5.36 | 0.84 | 18.58 | 4.85 | 0.33 | 7.30 |
3 | 3w-1c | -10.13c | -10.29 | -0.16 | 1.58 | -11.34 | -1.21 | 11.94 | -10.00 | 0.13 | 1.28 |
4 | 4w-1 | -25.82d | -25.94 | -0.12 | 0.46 | -26.53 | -0.71 | 2.75 | -25.27 | 0.55 | 2.13 |
5 | 4w-2 | -24.73d | -24.85 | -0.12 | 0.49 | -25.23 | -0.50 | 2.02 | -24.60 | 0.13 | 0.53 |
6 | 4w-3 | -15.40d | -16.11 | -0.71 | 4.61 | -19.04 | -3.64 | 23.64 | -14.64 | 0.76 | 4.94 |
7 | 5w-1 | -37.95d | -37.87 | 0.08 | 0.21 | -36.90 | 1.05 | 2.77 | -38.41 | -0.46 | 1.21 |
8 | 5w-2 | -31.46d | -32.22 | -0.76 | 2.42 | -32.38 | -0.92 | 2.92 | -30.84 | 0.62 | 1.97 |
9 | 5w-3 | -26.57d | -27.82 | -1.25 | 4.70 | -29.71 | -3.14 | 11.82 | -27.07 | -0.50 | 1.88 |
10 | 5w-4 | -24.85d | -25.94 | -1.09 | 4.39 | -27.95 | -3.10 | 12.47 | -24.27 | 0.58 | 2.33 |
11 | 5w-5 | -24.18d | -25.31 | -1.13 | 4.67 | -26.07 | -1.89 | 7.82 | -23.30 | 0.88 | 3.64 |
12 | 5w-6 | -26.07d | -26.53 | -0.46 | 1.76 | -26.32 | -0.25 | 0.96 | -24.48 | 1.59 | 6.10 |
13 | 5w-7 | -25.94d | -26.36 | -0.42 | 1.62 | -26.48 | -0.54 | 2.08 | -25.06 | 0.88 | 3.39 |
14 | 6w-prism | -36.40d | -38.07 | -1.67 | 4.59 | -37.99 | -1.59 | 4.37 | -37.91 | -1.51 | 4.15 |
15 | 6w-cage | -37.53d | -38.99 | -1.46 | 3.89 | -40.29 | -2.76 | 7.35 | -38.07 | -0.54 | 1.44 |
16 | 6w-book1 | -43.43d | -43.76 | -0.33 | 0.76 | -42.97 | 0.46 | 1.06 | -43.22 | 0.21 | 0.48 |
17 | 6w-book2 | -42.30d | -42.84 | -0.54 | 1.28 | -41.21 | 1.09 | 2.58 | -41.80 | 0.50 | 1.18 |
18 | 6w-bag | -43.30d | -44.10 | -0.80 | 1.85 | -41.59 | 1.71 | 3.95 | -41.59 | 1.71 | 3.95 |
19 | 6w-chair | -49.29d | -49.08 | 0.21 | 0.43 | -48.53 | 0.76 | 1.54 | -51.13 | -1.84 | 3.73 |
20 | 6w-boat1 | -47.45d | -47.36 | 0.09 | 0.19 | -46.28 | 1.17 | 2.47 | -49.08 | -1.63 | 3.44 |
21 | 6w-boat2 | -47.45d | -47.40 | 0.05 | 0.11 | -46.32 | 1.13 | 2.38 | -49.41 | -1.96 | 4.13 |
RMSD | 0.74 | 1.68 | 1.02 | ||||||||
MAD | 1.67 | 3.64 | 1.96 | ||||||||
MRD(%) | 2.12 | 6.11 | 2.86 |
No. | Cluster | CCSD(T) | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | |||||
1 | 10w-1 | -70.58 | -73.64 | -3.06 | 4.34 | -61.63 | 8.95 | 12.68 | -70.63 | -0.05 | 0.07 |
2 | 10w-2 | -71.13 | -74.52 | -3.39 | 4.77 | -65.81 | 5.32 | 7.48 | -68.74 | 2.39 | 3.36 |
3 | 10w-3 | -66.94 | -70.84 | -3.90 | 5.83 | -61.09 | 5.85 | 8.74 | -66.40 | 0.54 | 0.81 |
4 | 10w-4 | -69.41 | -72.97 | -3.56 | 5.13 | -62.76 | 6.65 | 9.58 | -69.79 | -0.38 | 0.55 |
5 | 10w-5 | -70.84 | -73.30 | -2.46 | 3.47 | -61.04 | 9.80 | 13.83 | -75.02 | -4.18 | 5.90 |
6 | 10w-6 | -68.37 | -73.01 | -4.64 | 6.79 | -64.43 | 3.94 | 5.76 | -71.09 | -2.72 | 3.98 |
No. | Cluster | CCSD(T) | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | |||||
7 | 10w-7 | -70.42 | -72.59 | -2.17 | 3.08 | -61.67 | 8.75 | 12.43 | -75.27 | -4.85 | 6.89 |
8 | 10w-8 | -70.08 | -72.89 | -2.81 | 4.01 | -61.09 | 8.99 | 12.83 | -73.47 | -3.39 | 4.84 |
9 | 10w-9 | -69.45 | -71.84 | -2.39 | 3.44 | -59.20 | 10.25 | 14.76 | -72.01 | -2.56 | 3.69 |
10 | 10w-10 | -66.57 | -70.17 | -3.60 | 5.41 | -61.21 | 5.36 | 8.05 | -66.44 | 0.13 | 0.20 |
11 | 11w-1 | -79.54 | -82.09 | -2.55 | 3.21 | -70.00 | 9.54 | 11.99 | -82.01 | -2.47 | 3.11 |
12 | 11w-2 | -82.63 | -84.89 | -2.26 | 2.74 | -73.43 | 9.20 | 11.13 | -82.30 | 0.33 | 0.40 |
13 | 11w-3 | -78.87 | -81.80 | -2.93 | 3.71 | -69.54 | 9.33 | 11.83 | -79.54 | -0.67 | 0.85 |
14 | 11w-4 | -82.26 | -84.22 | -1.96 | 2.38 | -69.41 | 12.85 | 15.62 | -81.92 | 0.34 | 0.41 |
15 | 11w-5 | -81.76 | -83.60 | -1.84 | 2.25 | -71.84 | 9.92 | 12.13 | -82.09 | -0.33 | 0.40 |
16 | 12w-1 | -88.70 | -92.47 | -3.77 | 4.25 | -77.78 | 10.92 | 12.31 | -87.91 | 0.79 | 0.89 |
17 | 13w-1 | -99.87 | -103.51 | -3.64 | 3.64 | -85.77 | 14.10 | 14.12 | -99.54 | 0.33 | 0.33 |
18 | 14w-1 | -111.55 | -115.48 | -3.93 | 3.52 | -95.10 | 16.45 | 14.75 | -108.95 | 2.60 | 2.33 |
19 | 15w-1 | -123.39 | -127.90 | -4.51 | 3.66 | -101.96 | 21.43 | 17.37 | -121.92 | 1.47 | 1.19 |
20 | 17w-1 | -142.05 | -148.36 | -6.31 | 4.44 | -117.32 | 24.73 | 17.41 | -138.87 | 3.18 | 2.24 |
21 | 17w-2 | -146.15 | -150.92 | -4.77 | 3.26 | -120.75 | 25.40 | 17.38 | -142.67 | 3.48 | 2.38 |
22 | 21w-1 | -182.17 | -190.54 | -8.37 | 4.59 | -141.46 | 40.71 | 22.35 | -181.71 | 0.46 | 0.25 |
23 | 21w-2 | -184.81 | -191.42 | -6.61 | 3.58 | -136.86 | 47.95 | 25.95 | -179.16 | 5.65 | 3.06 |
RMSD | 4.04 | 17.91 | 2.50 | ||||||||
MAD | 8.37 | 47.95 | 5.65 | ||||||||
MRD(%) | 3.98 | 13.50 | 2.09 |
Table 2 Calculated total three-body interaction energies of 23 medium-sized water clustersa
No. | Cluster | CCSD(T) | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | |||||
1 | 10w-1 | -70.58 | -73.64 | -3.06 | 4.34 | -61.63 | 8.95 | 12.68 | -70.63 | -0.05 | 0.07 |
2 | 10w-2 | -71.13 | -74.52 | -3.39 | 4.77 | -65.81 | 5.32 | 7.48 | -68.74 | 2.39 | 3.36 |
3 | 10w-3 | -66.94 | -70.84 | -3.90 | 5.83 | -61.09 | 5.85 | 8.74 | -66.40 | 0.54 | 0.81 |
4 | 10w-4 | -69.41 | -72.97 | -3.56 | 5.13 | -62.76 | 6.65 | 9.58 | -69.79 | -0.38 | 0.55 |
5 | 10w-5 | -70.84 | -73.30 | -2.46 | 3.47 | -61.04 | 9.80 | 13.83 | -75.02 | -4.18 | 5.90 |
6 | 10w-6 | -68.37 | -73.01 | -4.64 | 6.79 | -64.43 | 3.94 | 5.76 | -71.09 | -2.72 | 3.98 |
No. | Cluster | CCSD(T) | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | |||||
7 | 10w-7 | -70.42 | -72.59 | -2.17 | 3.08 | -61.67 | 8.75 | 12.43 | -75.27 | -4.85 | 6.89 |
8 | 10w-8 | -70.08 | -72.89 | -2.81 | 4.01 | -61.09 | 8.99 | 12.83 | -73.47 | -3.39 | 4.84 |
9 | 10w-9 | -69.45 | -71.84 | -2.39 | 3.44 | -59.20 | 10.25 | 14.76 | -72.01 | -2.56 | 3.69 |
10 | 10w-10 | -66.57 | -70.17 | -3.60 | 5.41 | -61.21 | 5.36 | 8.05 | -66.44 | 0.13 | 0.20 |
11 | 11w-1 | -79.54 | -82.09 | -2.55 | 3.21 | -70.00 | 9.54 | 11.99 | -82.01 | -2.47 | 3.11 |
12 | 11w-2 | -82.63 | -84.89 | -2.26 | 2.74 | -73.43 | 9.20 | 11.13 | -82.30 | 0.33 | 0.40 |
13 | 11w-3 | -78.87 | -81.80 | -2.93 | 3.71 | -69.54 | 9.33 | 11.83 | -79.54 | -0.67 | 0.85 |
14 | 11w-4 | -82.26 | -84.22 | -1.96 | 2.38 | -69.41 | 12.85 | 15.62 | -81.92 | 0.34 | 0.41 |
15 | 11w-5 | -81.76 | -83.60 | -1.84 | 2.25 | -71.84 | 9.92 | 12.13 | -82.09 | -0.33 | 0.40 |
16 | 12w-1 | -88.70 | -92.47 | -3.77 | 4.25 | -77.78 | 10.92 | 12.31 | -87.91 | 0.79 | 0.89 |
17 | 13w-1 | -99.87 | -103.51 | -3.64 | 3.64 | -85.77 | 14.10 | 14.12 | -99.54 | 0.33 | 0.33 |
18 | 14w-1 | -111.55 | -115.48 | -3.93 | 3.52 | -95.10 | 16.45 | 14.75 | -108.95 | 2.60 | 2.33 |
19 | 15w-1 | -123.39 | -127.90 | -4.51 | 3.66 | -101.96 | 21.43 | 17.37 | -121.92 | 1.47 | 1.19 |
20 | 17w-1 | -142.05 | -148.36 | -6.31 | 4.44 | -117.32 | 24.73 | 17.41 | -138.87 | 3.18 | 2.24 |
21 | 17w-2 | -146.15 | -150.92 | -4.77 | 3.26 | -120.75 | 25.40 | 17.38 | -142.67 | 3.48 | 2.38 |
22 | 21w-1 | -182.17 | -190.54 | -8.37 | 4.59 | -141.46 | 40.71 | 22.35 | -181.71 | 0.46 | 0.25 |
23 | 21w-2 | -184.81 | -191.42 | -6.61 | 3.58 | -136.86 | 47.95 | 25.95 | -179.16 | 5.65 | 3.06 |
RMSD | 4.04 | 17.91 | 2.50 | ||||||||
MAD | 8.37 | 47.95 | 5.65 | ||||||||
MRD(%) | 3.98 | 13.50 | 2.09 |
No. | Cluster | CCSD(T) | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | |||||
1 | 16w-1 | -135.65 | -141.75 | -6.10 | 4.50 | -120.16 | 15.49 | 11.42 | -135.44 | 0.21 | 0.15 |
2 | 16w-2 | -141.00 | -147.70 | -6.70 | 4.75 | -125.69 | 15.31 | 10.86 | -139.58 | 1.42 | 1.01 |
3 | 16w-3 | -150.21 | -154.60 | -4.39 | 2.92 | -129.45 | 20.76 | 13.82 | -149.91 | 0.30 | 0.20 |
4 | 16w-4 | -150.21 | -154.60 | -4.39 | 2.92 | -130.46 | 19.75 | 13.15 | -150.79 | -0.58 | 0.39 |
5 | 16w-5 | -152.17 | -156.82 | -4.65 | 3.06 | -132.17 | 20.00 | 13.14 | -149.83 | 2.34 | 1.54 |
6 | 17w-3 | -132.59 | -137.90 | -5.31 | 4.00 | -111.67 | 20.92 | 15.78 | -128.24 | 4.35 | 3.28 |
7 | 17w-4 | -140.88 | -147.07 | -6.19 | 4.39 | -116.02 | 24.86 | 17.65 | -139.49 | 1.39 | 0.99 |
8 | 18w-1 | -147.07 | -152.80 | -5.73 | 3.90 | -123.30 | 23.77 | 16.16 | -141.21 | 5.86 | 3.98 |
9 | 19w-1 | -164.89 | -172.00 | -7.11 | 4.31 | -128.57 | 36.32 | 22.03 | -155.98 | 8.91 | 5.40 |
10 | 20w-1 | -173.05 | -180.54 | -7.49 | 4.33 | -140.50 | 32.55 | 18.81 | -179.24 | -6.19 | 3.58 |
11 | 20w-2 | -170.75 | -178.45 | -7.70 | 4.51 | -144.01 | 26.74 | 15.66 | -170.75 | 0 | 0 |
12 | 20w-3 | -166.23 | -173.22 | -6.99 | 4.21 | -140.25 | 25.98 | 15.63 | -173.34 | -7.11 | 4.28 |
13 | 20w-4 | -167.99 | -175.98 | -7.99 | 4.76 | -133.93 | 34.06 | 20.28 | -173.76 | -5.77 | 3.43 |
14 | 20w-5 | -170.87 | -178.49 | -7.62 | 4.46 | -143.30 | 27.57 | 16.14 | -175.60 | -4.73 | 2.77 |
15 | 20w-6 | -166.23 | -175.81 | -9.58 | 5.76 | -144.10 | 22.13 | 13.31 | -172.09 | -5.86 | 3.53 |
16 | 20w-7 | -166.65 | -175.39 | -8.74 | 5.24 | -136.02 | 30.63 | 18.38 | -167.86 | -1.21 | 0.73 |
17 | 20w-8 | -166.86 | -174.22 | -7.36 | 4.41 | -138.41 | 28.45 | 17.05 | -171.25 | -4.39 | 2.63 |
18 | 20w-9 | -168.49 | -176.19 | -7.70 | 4.57 | -133.97 | 34.52 | 20.49 | -167.44 | 1.05 | 0.62 |
19 | 20w-10 | -167.82 | -175.77 | -7.95 | 4.74 | -137.44 | 30.38 | 18.10 | -172.42 | -4.60 | 2.74 |
20 | 22w-1 | -164.81 | -173.43 | -8.62 | 5.23 | -124.73 | 40.08 | 24.32 | -154.64 | 10.17 | 6.17 |
21 | 30w-1 | -209.87 | -221.42 | -11.55 | 5.50 | -166.73 | 43.14 | 20.56 | -217.36 | -7.49 | 3.57 |
22 | 30w-2 | -196.77 | -211.88 | -15.11 | 7.68 | -157.19 | 39.58 | 20.11 | -203.64 | -6.87 | 3.49 |
23 | 30w-3 | -193.34 | -215.60 | -22.26 | 11.51 | -164.47 | 28.87 | 14.93 | -193.30 | 0.04 | 0.02 |
RMSD | 8.98 | 28.91 | 4.98 | ||||||||
MAD | 22.26 | 43.14 | 10.17 | ||||||||
MRD(%) | 4.85 | 16.86 | 2.37 |
Table 3 Calculated total three-body interaction energies of 23 water nanoparticlesa
No. | Cluster | CCSD(T) | MP2/aug-cc-pVDZ | M06-2X/jul-cc-pVTZ | This work | ||||||
---|---|---|---|---|---|---|---|---|---|---|---|
Δ | δ(%) | Δ | δ(%) | E3B | Δ | δ(%) | |||||
1 | 16w-1 | -135.65 | -141.75 | -6.10 | 4.50 | -120.16 | 15.49 | 11.42 | -135.44 | 0.21 | 0.15 |
2 | 16w-2 | -141.00 | -147.70 | -6.70 | 4.75 | -125.69 | 15.31 | 10.86 | -139.58 | 1.42 | 1.01 |
3 | 16w-3 | -150.21 | -154.60 | -4.39 | 2.92 | -129.45 | 20.76 | 13.82 | -149.91 | 0.30 | 0.20 |
4 | 16w-4 | -150.21 | -154.60 | -4.39 | 2.92 | -130.46 | 19.75 | 13.15 | -150.79 | -0.58 | 0.39 |
5 | 16w-5 | -152.17 | -156.82 | -4.65 | 3.06 | -132.17 | 20.00 | 13.14 | -149.83 | 2.34 | 1.54 |
6 | 17w-3 | -132.59 | -137.90 | -5.31 | 4.00 | -111.67 | 20.92 | 15.78 | -128.24 | 4.35 | 3.28 |
7 | 17w-4 | -140.88 | -147.07 | -6.19 | 4.39 | -116.02 | 24.86 | 17.65 | -139.49 | 1.39 | 0.99 |
8 | 18w-1 | -147.07 | -152.80 | -5.73 | 3.90 | -123.30 | 23.77 | 16.16 | -141.21 | 5.86 | 3.98 |
9 | 19w-1 | -164.89 | -172.00 | -7.11 | 4.31 | -128.57 | 36.32 | 22.03 | -155.98 | 8.91 | 5.40 |
10 | 20w-1 | -173.05 | -180.54 | -7.49 | 4.33 | -140.50 | 32.55 | 18.81 | -179.24 | -6.19 | 3.58 |
11 | 20w-2 | -170.75 | -178.45 | -7.70 | 4.51 | -144.01 | 26.74 | 15.66 | -170.75 | 0 | 0 |
12 | 20w-3 | -166.23 | -173.22 | -6.99 | 4.21 | -140.25 | 25.98 | 15.63 | -173.34 | -7.11 | 4.28 |
13 | 20w-4 | -167.99 | -175.98 | -7.99 | 4.76 | -133.93 | 34.06 | 20.28 | -173.76 | -5.77 | 3.43 |
14 | 20w-5 | -170.87 | -178.49 | -7.62 | 4.46 | -143.30 | 27.57 | 16.14 | -175.60 | -4.73 | 2.77 |
15 | 20w-6 | -166.23 | -175.81 | -9.58 | 5.76 | -144.10 | 22.13 | 13.31 | -172.09 | -5.86 | 3.53 |
16 | 20w-7 | -166.65 | -175.39 | -8.74 | 5.24 | -136.02 | 30.63 | 18.38 | -167.86 | -1.21 | 0.73 |
17 | 20w-8 | -166.86 | -174.22 | -7.36 | 4.41 | -138.41 | 28.45 | 17.05 | -171.25 | -4.39 | 2.63 |
18 | 20w-9 | -168.49 | -176.19 | -7.70 | 4.57 | -133.97 | 34.52 | 20.49 | -167.44 | 1.05 | 0.62 |
19 | 20w-10 | -167.82 | -175.77 | -7.95 | 4.74 | -137.44 | 30.38 | 18.10 | -172.42 | -4.60 | 2.74 |
20 | 22w-1 | -164.81 | -173.43 | -8.62 | 5.23 | -124.73 | 40.08 | 24.32 | -154.64 | 10.17 | 6.17 |
21 | 30w-1 | -209.87 | -221.42 | -11.55 | 5.50 | -166.73 | 43.14 | 20.56 | -217.36 | -7.49 | 3.57 |
22 | 30w-2 | -196.77 | -211.88 | -15.11 | 7.68 | -157.19 | 39.58 | 20.11 | -203.64 | -6.87 | 3.49 |
23 | 30w-3 | -193.34 | -215.60 | -22.26 | 11.51 | -164.47 | 28.87 | 14.93 | -193.30 | 0.04 | 0.02 |
RMSD | 8.98 | 28.91 | 4.98 | ||||||||
MAD | 22.26 | 43.14 | 10.17 | ||||||||
MRD(%) | 4.85 | 16.86 | 2.37 |
No. | Cluster | CCSD(T) | WHBB | This work | ||||
---|---|---|---|---|---|---|---|---|
E3B/(kJ·mol-1) | Δ/(kJ·mol-1) | δ(%) | E3B/(kJ·mol-1) | Δ/(kJ·mol-1) | δ(%) | |||
1 | 11w-1 | -79.54 | -81.17 | -1.63 | 2.05 | -82.01 | -2.47 | 3.11 |
2 | 11w-2 | -82.63 | -82.84 | -0.21 | 0.25 | -82.30 | 0.33 | 0.40 |
3 | 11w-3 | -78.87 | -81.59 | -2.72 | 3.45 | -79.54 | -0.67 | 0.85 |
4 | 11w-4 | -82.26 | -83.68 | -1.42 | 1.73 | -81.92 | 0.34 | 0.41 |
5 | 11w-5 | -81.76 | -83.26 | -1.50 | 1.83 | -82.09 | -0.33 | 0.40 |
6 | 12w-1 | -88.70 | -93.30 | -4.60 | 5.19 | -87.91 | 0.79 | 0.89 |
7 | 13w-1 | -99.87 | -103.76 | -3.89 | 3.90 | -99.54 | 0.33 | 0.33 |
8 | 14w-1 | -111.55 | -115.06 | -3.51 | 3.15 | -108.95 | 2.60 | 2.33 |
9 | 15w-1 | -123.39 | -123.01 | 0.38 | 0.31 | -121.92 | 1.47 | 1.19 |
10 | 17w-1 | -142.05 | -148.95 | -6.90 | 4.86 | -138.87 | 3.18 | 2.24 |
11 | 17w-2 | -146.15 | -144.77 | 1.38 | 0.94 | -142.67 | 3.48 | 2.38 |
12 | 17w-3 | -132.59 | -140.16 | -7.57 | 5.71 | -128.24 | 4.35 | 3.28 |
13 | 17w-4 | -140.88 | -141.84 | -0.96 | 0.68 | -139.49 | 1.39 | 0.99 |
14 | 18w-1 | -147.07 | -153.97 | -6.90 | 4.69 | -141.21 | 5.86 | 3.98 |
15 | 19w-1 | -164.89 | -169.03 | -4.14 | 2.51 | -155.98 | 8.91 | 5.40 |
16 | 21w-1 | -182.17 | -193.30 | -11.13 | 6.11 | -181.71 | 0.46 | 0.25 |
17 | 21w-2 | -184.81 | -190.37 | -5.56 | 3.01 | -179.16 | 5.65 | 3.06 |
18 | 22w-1 | -164.81 | -190.37 | -25.56 | 15.51 | -154.64 | 10.17 | 6.17 |
RMSD/(kJ·mol-1) | 7.61 | 4.14 | ||||||
MAD/(kJ·mol-1) | 25.56 | 10.17 | ||||||
MRD(%) | 3.66 | 2.09 |
Table 4 Calculated total three-body interaction energies of 18 water clusters
No. | Cluster | CCSD(T) | WHBB | This work | ||||
---|---|---|---|---|---|---|---|---|
E3B/(kJ·mol-1) | Δ/(kJ·mol-1) | δ(%) | E3B/(kJ·mol-1) | Δ/(kJ·mol-1) | δ(%) | |||
1 | 11w-1 | -79.54 | -81.17 | -1.63 | 2.05 | -82.01 | -2.47 | 3.11 |
2 | 11w-2 | -82.63 | -82.84 | -0.21 | 0.25 | -82.30 | 0.33 | 0.40 |
3 | 11w-3 | -78.87 | -81.59 | -2.72 | 3.45 | -79.54 | -0.67 | 0.85 |
4 | 11w-4 | -82.26 | -83.68 | -1.42 | 1.73 | -81.92 | 0.34 | 0.41 |
5 | 11w-5 | -81.76 | -83.26 | -1.50 | 1.83 | -82.09 | -0.33 | 0.40 |
6 | 12w-1 | -88.70 | -93.30 | -4.60 | 5.19 | -87.91 | 0.79 | 0.89 |
7 | 13w-1 | -99.87 | -103.76 | -3.89 | 3.90 | -99.54 | 0.33 | 0.33 |
8 | 14w-1 | -111.55 | -115.06 | -3.51 | 3.15 | -108.95 | 2.60 | 2.33 |
9 | 15w-1 | -123.39 | -123.01 | 0.38 | 0.31 | -121.92 | 1.47 | 1.19 |
10 | 17w-1 | -142.05 | -148.95 | -6.90 | 4.86 | -138.87 | 3.18 | 2.24 |
11 | 17w-2 | -146.15 | -144.77 | 1.38 | 0.94 | -142.67 | 3.48 | 2.38 |
12 | 17w-3 | -132.59 | -140.16 | -7.57 | 5.71 | -128.24 | 4.35 | 3.28 |
13 | 17w-4 | -140.88 | -141.84 | -0.96 | 0.68 | -139.49 | 1.39 | 0.99 |
14 | 18w-1 | -147.07 | -153.97 | -6.90 | 4.69 | -141.21 | 5.86 | 3.98 |
15 | 19w-1 | -164.89 | -169.03 | -4.14 | 2.51 | -155.98 | 8.91 | 5.40 |
16 | 21w-1 | -182.17 | -193.30 | -11.13 | 6.11 | -181.71 | 0.46 | 0.25 |
17 | 21w-2 | -184.81 | -190.37 | -5.56 | 3.01 | -179.16 | 5.65 | 3.06 |
18 | 22w-1 | -164.81 | -190.37 | -25.56 | 15.51 | -154.64 | 10.17 | 6.17 |
RMSD/(kJ·mol-1) | 7.61 | 4.14 | ||||||
MAD/(kJ·mol-1) | 25.56 | 10.17 | ||||||
MRD(%) | 3.66 | 2.09 |
Method | RMSD/(kJ·mol-1) | MAD/(kJ·mol-1) | MRD(%) |
---|---|---|---|
MP2 | 5.78 | 22.26 | 3.70 |
M06-2X | 19.95 | 47.95 | 12.34 |
This work | 3.32 | 10.17 | 2.43 |
Table 5 Deviations of different methods with respect to the CCSD(T) three-body interaction energies of 67 water clusters
Method | RMSD/(kJ·mol-1) | MAD/(kJ·mol-1) | MRD(%) |
---|---|---|---|
MP2 | 5.78 | 22.26 | 3.70 |
M06-2X | 19.95 | 47.95 | 12.34 |
This work | 3.32 | 10.17 | 2.43 |
Fig.1 Correlation plots for the total three-body interaction energies of the 67 water clusters (A) MP2/aug-cc-pVDZ; (B) M06-2X/jul-cc-pVTZ; (C) this work.
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