Phonon properties

[materialsvirtuallab]

Phonon properties

[shyuep]

EDIFF_PER_ATOM was premised on the idea that because we only care about energies per atom for phase diagrams, so as long as we get a normalized energy that is within a certain error, that is good enough. The problem was that no one thought about the force convergence requirement. VASP sets EDIFFG=10xEDIFF by default. You can imagine that your 444 atom structure has an energy error that is 444x that of a single atom structure and all the forces are nowhere close to 0.

The results are not deterministic. And I don't think there is a one-size fits all algo. As a strategy, I would just choose one algo, set a timer for the calculation and if the time exceeds say 5mins or so, you terminate the calculation and forget about having predictions for that structure. It is not important to have predictions for EVERY structure, as long as most structures are done.

[shyuep]

Just to conclude - for MLP properties for MP, I went with the BFGS. Note that the input structures are already DFT-relaxed. Presumably, it really shouldn't require a conjugate gradient type relaxation. Initial informal tests suggest that BFGS is more reliable and faster.

@JiQi535 The phonon results of matcalc are affected by the fact that (a) you have MLP vs DFT error, and (b) force convergence error. The former is already an MAE of 0.17 eV/A or so.

[janosh]

Since PropCalc.calc will return a dict, might make sense to define a TypedDict for each PropCalc subclass's return type to get better editor completions and type checking.

[shyuep]

Depends on how stringent we want to be. The problem is that we will need to specify a typeddict for every single return. Also, I am not clear of the benefits over say... returning a DataClass. That would yield the type checking benefits + other benefits.

[janosh]

DataClass is good too.

[shyuep]

@lbluque and @BowenD-UCB @janosh I think a first draft of the phonon properties is ready. Pls take a look and give comments. Note that these will be used for the MLP properties for MP effort, which will include both m3gnet and chgnet predicted properties for all materials.

[BowenD-UCB]

@shyuep
Hi, Shyueping, thanks for the effort developing the codebase.
Everything looks nice so far, I have one concern:
The default relaxation convergence threshold is set to fmax=0.01
Do you know how many steps does it usually take for structures, especially large structures and supecells to converge to fmax=0.01 ?

From my, experience with CHGNet + FIRE, this can be very hard, sometimes 10K steps won't give fmax = 0.1 for large structures.
In this case, I'm worrying it will never converge under such thershhold.

[janosh]

@BowenD-UCB Funny anecdote on that topic: I tried CHGNet-relaxing the largest structure in MP yesterday.

from mp_api.client import MPRester
from chgnet.model import StructOptimizer

structure = MPRester().summary.search(num_sites=444)[0].structure

trajectory = StructOptimizer().relax(structure)["trajectory"]

Didn't get anywhere close to 0.01 eV/A (and also broke the P2_1/c symmetry):

FIRE 500th step fmax: 24.1346

CHGNet initialized with 400,438 parameters
CHGNet will run on cpu
      Step     Time          Energy         fmax
*Force-consistent energies used in optimization.
FIRE:    0 16:46:42    15138.197479*  319650.2225
FIRE:    1 16:46:43     -874.923697*   21483.3231
FIRE:    2 16:46:43     -833.215493*    9006.1643
FIRE:    3 16:46:44      624.891586*   51479.3593
FIRE:    4 16:46:45    -1343.892282*     559.4396
FIRE:    5 16:46:45    -1379.200321*     390.3657
FIRE:    6 16:46:46    -1386.432106*     496.6045
FIRE:    7 16:46:47    -1732.092175*  359458.5265
FIRE:    8 16:46:47     2357.845974*   26155.4632
FIRE:    9 16:46:48    16479.414734* 8946970.2089
FIRE:   10 16:46:49     3825.782272*  399353.2884
FIRE:   11 16:46:49      225.877150*  154064.6199
FIRE:   12 16:46:50    -1378.453176*    7283.6928
FIRE:   13 16:46:50    -1434.287158*    2739.2725
FIRE:   14 16:46:51     -438.079794*  125434.1262
FIRE:   15 16:46:52    -1432.569085*     198.4648
FIRE:   16 16:46:52    -1435.132433*     344.5283
FIRE:   17 16:46:53    -1436.001526*     337.1128
FIRE:   18 16:46:53    -1437.775068*     325.8546
FIRE:   19 16:46:54    -1440.105529*     278.6157
FIRE:   20 16:46:54    -1442.665277*     231.3465
FIRE:   21 16:46:55    -1445.176226*     225.6978
FIRE:   22 16:46:55    -1448.129448*     220.6011
FIRE:   23 16:46:56    -1451.660654*     236.9788
FIRE:   24 16:46:56    -1456.303156*     201.0574
FIRE:   25 16:46:57    -1461.145835*     189.5195
FIRE:   26 16:46:57    -1466.661346*     180.7054
FIRE:   27 16:46:58    -1473.633356*     208.6732
FIRE:   28 16:46:59    -1482.561407*     182.0297
FIRE:   29 16:46:59    -1491.647504*     239.7862
FIRE:   30 16:47:00    -1502.065716*     209.4893
FIRE:   31 16:47:00    -1515.223317*     190.2158
FIRE:   32 16:47:01    -1530.529833*     225.3925
FIRE:   33 16:47:01    -1545.377878*     269.4074
FIRE:   34 16:47:02    -1562.177307*     952.5687
FIRE:   35 16:47:03    -1577.176517*     111.7413
FIRE:   36 16:47:03    -1599.099149*     175.8905
FIRE:   37 16:47:04    -1618.521841*     211.9425
FIRE:   38 16:47:05    -1640.593203*     177.5069
FIRE:   39 16:47:05    -1661.105066*     507.7115
FIRE:   40 16:47:06    -1664.202890*     340.9267
FIRE:   41 16:47:06    -1664.018486*     211.6701
FIRE:   42 16:47:07    -1664.694071*     201.2644
FIRE:   43 16:47:08    -1665.973257*     194.6137
FIRE:   44 16:47:08    -1668.168961*     232.3385
FIRE:   45 16:47:09    -1670.925922*     153.3879
FIRE:   46 16:47:09    -1672.016470*     233.2453
FIRE:   47 16:47:10    -1673.014498*     164.2860
FIRE:   48 16:47:11    -1674.752684*     146.1330
FIRE:   49 16:47:11    -1676.918747*     193.9374
FIRE:   50 16:47:12    -1680.053621*     165.4781
FIRE:   51 16:47:12    -1683.649189*     201.0871
FIRE:   52 16:47:13    -1686.143412*     415.1638
FIRE:   53 16:47:14    -1689.775394*     911.9369
FIRE:   54 16:47:14    -1691.151758*     135.3926
FIRE:   55 16:47:15    -1691.273177*     229.2452
FIRE:   56 16:47:16    -1691.350877*     216.6474
FIRE:   57 16:47:16    -1691.495267*     190.1320
FIRE:   58 16:47:17    -1691.685917*     151.4553
FIRE:   59 16:47:17    -1691.899750*     103.9541
FIRE:   60 16:47:18    -1692.113159*      86.4731
FIRE:   61 16:47:19    -1692.307408*      87.7406
FIRE:   62 16:47:19    -1692.500493*     127.5687
FIRE:   63 16:47:20    -1692.773500*     149.4497
FIRE:   64 16:47:21    -1693.176395*     146.3048
FIRE:   65 16:47:21    -1693.741253*     161.4323
FIRE:   66 16:47:22    -1694.550536*     416.4899
FIRE:   67 16:47:23    -1695.988721*     283.0004
FIRE:   68 16:47:23    -1698.005630*     265.9407
FIRE:   69 16:47:24    -1697.880507*     670.2471
FIRE:   70 16:47:25    -1698.359831*     575.4662
FIRE:   71 16:47:25    -1699.179382*     360.1235
FIRE:   72 16:47:26    -1699.475255*     115.5474
FIRE:   73 16:47:27    -1699.711106*     125.1741
FIRE:   74 16:47:27    -1699.930867*     224.9025
FIRE:   75 16:47:28    -1700.010155*     488.3739
FIRE:   76 16:47:29    -1700.090183*     409.7753
FIRE:   77 16:47:29    -1700.205357*     251.5991
FIRE:   78 16:47:30    -1700.288984*     104.4901
FIRE:   79 16:47:30    -1700.322012*     114.2426
FIRE:   80 16:47:31    -1700.342760*     135.1059
FIRE:   81 16:47:32    -1700.373035*     135.0575
FIRE:   82 16:47:32    -1700.415167*     134.0854
FIRE:   83 16:47:33    -1700.474871*     137.0845
FIRE:   84 16:47:34    -1700.557228*     145.9653
FIRE:   85 16:47:34    -1700.669755*     157.6181
FIRE:   86 16:47:35    -1700.819756*     136.7887
FIRE:   87 16:47:36    -1700.971979*      61.3948
FIRE:   88 16:47:36    -1701.051373*     379.3562
FIRE:   89 16:47:37    -1701.275368*     247.2444
FIRE:   90 16:47:38    -1701.507726*     117.4423
FIRE:   91 16:47:38    -1701.721770*     175.2324
FIRE:   92 16:47:39    -1702.052364*     141.4816
FIRE:   93 16:47:39    -1702.386240*     241.6488
FIRE:   94 16:47:40    -1702.843334*     113.1796
FIRE:   95 16:47:41    -1703.301275*     190.0270
FIRE:   96 16:47:41    -1703.956324*     119.7880
FIRE:   97 16:47:42    -1704.589036*     286.2856
FIRE:   98 16:47:43    -1705.552237*      38.1229
FIRE:   99 16:47:43    -1706.519142*     186.5149
FIRE:  100 16:47:44    -1707.867771*      69.4893
FIRE:  101 16:47:44    -1709.364284*     171.0310
FIRE:  102 16:47:45    -1711.051234*     136.2270
FIRE:  103 16:47:46    -1713.379472*     148.9718
FIRE:  104 16:47:46    -1715.888197*     346.9569
FIRE:  105 16:47:47    -1719.134434*      58.6558
FIRE:  106 16:47:48    -1722.154982*     586.1258
FIRE:  107 16:47:48    -1720.155856*     505.0674
FIRE:  108 16:47:49    -1723.693520*     963.6056
FIRE:  109 16:47:50    -1727.099602*      65.7817
FIRE:  110 16:47:50    -1723.954565*     213.5025
FIRE:  111 16:47:51    -1724.373127*     543.5174
FIRE:  112 16:47:52    -1724.782479*     146.5072
FIRE:  113 16:47:52    -1724.932268*      81.6786
FIRE:  114 16:47:53    -1725.081634*      72.8217
FIRE:  115 16:47:54    -1725.286257*     132.7082
FIRE:  116 16:47:54    -1725.619709*     156.5599
FIRE:  117 16:47:55    -1725.940247*      72.7412
FIRE:  118 16:47:56    -1726.185943*      57.9503
FIRE:  119 16:47:56    -1726.524370*      66.9272
FIRE:  120 16:47:57    -1727.163646*     403.1359
FIRE:  121 16:47:58    -1729.283873*     435.9983
FIRE:  122 16:47:58    -1730.080770*      31.1854
FIRE:  123 16:47:59    -1730.174772*     302.9309
FIRE:  124 16:47:59    -1730.276608*     184.8966
FIRE:  125 16:48:00    -1730.380560*      81.4150
FIRE:  126 16:48:01    -1730.483242*      78.7149
FIRE:  127 16:48:01    -1730.622974*     100.0944
FIRE:  128 16:48:02    -1730.803568*     102.3073
FIRE:  129 16:48:03    -1730.997923*      64.8872
FIRE:  130 16:48:03    -1731.167295*      30.8212
FIRE:  131 16:48:04    -1731.350747*      30.7882
FIRE:  132 16:48:05    -1731.556641*      30.7411
FIRE:  133 16:48:05    -1731.798102*      56.3851
FIRE:  134 16:48:06    -1732.056501*     126.6069
FIRE:  135 16:48:07    -1732.427004*     144.0747
FIRE:  136 16:48:07    -1732.975877*      82.8569
FIRE:  137 16:48:08    -1733.578420*      42.1296
FIRE:  138 16:48:09    -1734.279940*      44.4759
FIRE:  139 16:48:09    -1735.096739*      92.0295
FIRE:  140 16:48:10    -1736.190250*      62.8475
FIRE:  141 16:48:11    -1737.297735*     196.7959
FIRE:  142 16:48:11    -1738.819759*      28.6378
FIRE:  143 16:48:12    -1740.367825*     166.5469
FIRE:  144 16:48:13    -1742.361128*     215.8919
FIRE:  145 16:48:13    -1744.593352*     165.3391
FIRE:  146 16:48:14    -1747.540223*      37.4007
FIRE:  147 16:48:15    -1750.042809*     273.8597
FIRE:  148 16:48:15    -1753.980297*      92.4606
FIRE:  149 16:48:16    -1756.761818*     450.2110
FIRE:  150 16:48:17    -1758.694571*     486.7705
FIRE:  151 16:48:17    -1763.185696*     348.9674
FIRE:  152 16:48:18    -1760.650824*     836.7579
FIRE:  153 16:48:19    -1762.678001*     772.1707
FIRE:  154 16:48:19    -1764.101789*     154.5855
FIRE:  155 16:48:20    -1764.110682*     202.2236
FIRE:  156 16:48:21    -1764.173879*     170.7151
FIRE:  157 16:48:21    -1764.277619*     152.9172
FIRE:  158 16:48:22    -1764.391734*     129.9363
FIRE:  159 16:48:23    -1764.497169*      98.4435
FIRE:  160 16:48:23    -1764.587465*      60.7606
FIRE:  161 16:48:24    -1764.663895*      70.9254
FIRE:  162 16:48:25    -1764.730585*      73.4512
FIRE:  163 16:48:25    -1764.800663*      63.4256
FIRE:  164 16:48:26    -1764.880903*      82.8677
FIRE:  165 16:48:27    -1764.981045*     105.5027
FIRE:  166 16:48:27    -1765.127340*     106.3243
FIRE:  167 16:48:28    -1765.346784*      81.6102
FIRE:  168 16:48:29    -1765.624131*      39.2951
FIRE:  169 16:48:29    -1765.909736*      41.1226
FIRE:  170 16:48:30    -1766.216300*      62.2461
FIRE:  171 16:48:31    -1766.618348*      79.0488
FIRE:  172 16:48:31    -1767.138957*      79.9291
FIRE:  173 16:48:32    -1767.779609*      22.0443
FIRE:  174 16:48:33    -1768.481446*      59.1917
FIRE:  175 16:48:34    -1769.391083*      58.6609
FIRE:  176 16:48:34    -1770.492004*      81.3855
FIRE:  177 16:48:35    -1771.736681*      76.7022
FIRE:  178 16:48:36    -1773.364775*     116.3352
FIRE:  179 16:48:36    -1774.885846*     393.6739
FIRE:  180 16:48:37    -1773.668163*    1343.5660
FIRE:  181 16:48:38    -1777.018353*     133.7857
FIRE:  182 16:48:38    -1777.075304*      99.0792
FIRE:  183 16:48:39    -1777.166977*      77.5923
FIRE:  184 16:48:40    -1777.276011*      66.2249
FIRE:  185 16:48:40    -1777.409180*      82.1904
FIRE:  186 16:48:41    -1777.564156*      41.9134
FIRE:  187 16:48:42    -1777.629576*     148.1220
FIRE:  188 16:48:43    -1777.641220*     136.8288
FIRE:  189 16:48:43    -1777.662603*     115.2765
FIRE:  190 16:48:44    -1777.689280*      86.4772
FIRE:  191 16:48:45    -1777.717438*      53.2043
FIRE:  192 16:48:45    -1777.744961*      29.3613
FIRE:  193 16:48:46    -1777.772060*      36.9813
FIRE:  194 16:48:47    -1777.801065*      48.8541
FIRE:  195 16:48:47    -1777.838751*      56.6020
FIRE:  196 16:48:48    -1777.888927*      58.7164
FIRE:  197 16:48:49    -1777.954983*      54.4380
FIRE:  198 16:48:49    -1778.038610*      41.4979
FIRE:  199 16:48:50    -1778.137270*      27.9075
FIRE:  200 16:48:51    -1778.248421*      50.3788
FIRE:  201 16:48:51    -1778.376085*      55.6707
FIRE:  202 16:48:52    -1778.523651*      27.3273
FIRE:  203 16:48:53    -1778.692177*      76.1983
FIRE:  204 16:48:53    -1778.914902*      38.6633
FIRE:  205 16:48:54    -1779.189285*      79.8483
FIRE:  206 16:48:55    -1779.536711*      67.1153
FIRE:  207 16:48:55    -1779.954002*      20.8480
FIRE:  208 16:48:56    -1780.437561*      39.8254
FIRE:  209 16:48:57    -1781.021473*      41.0957
FIRE:  210 16:48:58    -1781.750410*      31.2540
FIRE:  211 16:48:58    -1782.638981*      34.0015
FIRE:  212 16:48:59    -1783.670671*     157.8230
FIRE:  213 16:49:00    -1784.315769*     407.9015
FIRE:  214 16:49:00    -1785.167501*     583.7265
FIRE:  215 16:49:01    -1786.260590*     116.8049
FIRE:  216 16:49:02    -1786.109425*     302.1226
FIRE:  217 16:49:02    -1786.197922*     230.4971
FIRE:  218 16:49:03    -1786.310978*     114.7673
FIRE:  219 16:49:04    -1786.407732*      76.8650
FIRE:  220 16:49:04    -1786.510414*      51.9809
FIRE:  221 16:49:05    -1786.543230*     160.6760
FIRE:  222 16:49:06    -1786.551699*     150.7354
FIRE:  223 16:49:06    -1786.566942*     132.7678
FIRE:  224 16:49:07    -1786.587055*     106.3042
FIRE:  225 16:49:08    -1786.608862*      75.1683
FIRE:  226 16:49:08    -1786.631304*      44.9117
FIRE:  227 16:49:09    -1786.652899*      40.5455
FIRE:  228 16:49:10    -1786.674494*      46.0483
FIRE:  229 16:49:10    -1786.700747*      53.6835
FIRE:  230 16:49:11    -1786.733351*      60.1246
FIRE:  231 16:49:12    -1786.775059*      73.0090
FIRE:  232 16:49:12    -1786.827988*      75.2224
FIRE:  233 16:49:13    -1786.892984*      54.3400
FIRE:  234 16:49:14    -1786.965603*      20.0917
FIRE:  235 16:49:14    -1787.038433*      79.5033
FIRE:  236 16:49:15    -1787.130318*      89.7924
FIRE:  237 16:49:16    -1787.252054*      32.0723
FIRE:  238 16:49:16    -1787.389881*      87.1031
FIRE:  239 16:49:17    -1787.576614*      40.9775
FIRE:  240 16:49:18    -1787.791718*      91.6200
FIRE:  241 16:49:19    -1788.060596*      20.8101
FIRE:  242 16:49:19    -1788.368431*      68.4054
FIRE:  243 16:49:20    -1788.755236*      22.4236
FIRE:  244 16:49:21    -1789.216988*      76.6950
FIRE:  245 16:49:21    -1789.764696*     139.7653
FIRE:  246 16:49:22    -1790.388622*     257.7319
FIRE:  247 16:49:23    -1790.950516*     340.9254
FIRE:  248 16:49:23    -1791.896038*     313.6993
FIRE:  249 16:49:24    -1792.899570*     105.0490
FIRE:  250 16:49:25    -1794.150599*     139.8150
FIRE:  251 16:49:25    -1795.092733*     691.5354
FIRE:  252 16:49:26    -1795.811508*     207.9420
FIRE:  253 16:49:27    -1795.870577*     157.7357
FIRE:  254 16:49:27    -1795.954628*      99.8245
FIRE:  255 16:49:28    -1796.045454*      48.3920
FIRE:  256 16:49:29    -1796.071707*     175.9919
FIRE:  257 16:49:29    -1796.083775*     156.2440
FIRE:  258 16:49:30    -1796.103041*     118.9990
FIRE:  259 16:49:31    -1796.125059*      68.2394
FIRE:  260 16:49:32    -1796.144537*      32.6378
FIRE:  261 16:49:32    -1796.161051*      37.5620
FIRE:  262 16:49:33    -1796.177353*      62.1500
FIRE:  263 16:49:34    -1796.196831*      80.2401
FIRE:  264 16:49:35    -1796.224354*      88.1680
FIRE:  265 16:49:35    -1796.262463*      82.6002
FIRE:  266 16:49:36    -1796.311581*      55.4194
FIRE:  267 16:49:37    -1796.366627*      19.1557
FIRE:  268 16:49:38    -1796.422731*      73.8739
FIRE:  269 16:49:38    -1796.494715*      93.4169
FIRE:  270 16:49:39    -1796.593586*      28.9563
FIRE:  271 16:49:40    -1796.701984*      66.1197
FIRE:  272 16:49:40    -1796.838753*      75.6664
FIRE:  273 16:49:41    -1797.013206*      19.8675
FIRE:  274 16:49:42    -1797.212008*      86.9879
FIRE:  275 16:49:42    -1797.464584*      28.8387
FIRE:  276 16:49:43    -1797.763950*      50.3421
FIRE:  277 16:49:44    -1798.130007*      82.2494
FIRE:  278 16:49:45    -1798.579691*      58.1896
FIRE:  279 16:49:45    -1799.121260*      75.4069
FIRE:  280 16:49:46    -1799.740528*     153.7882
FIRE:  281 16:49:47    -1800.318512*     427.4783
FIRE:  282 16:49:47    -1800.546318*     452.0652
FIRE:  283 16:49:48    -1801.095509*     313.9549
FIRE:  284 16:49:49    -1801.432983*      62.0948
FIRE:  285 16:49:49    -1801.445051*      56.2538
FIRE:  286 16:49:50    -1801.467070*      50.1621
FIRE:  287 16:49:51    -1801.498404*      45.8009
FIRE:  288 16:49:51    -1801.537148*      43.4152
FIRE:  289 16:49:52    -1801.582031*      38.3568
FIRE:  290 16:49:53    -1801.630726*      37.0489
FIRE:  291 16:49:54    -1801.681961*      38.7623
FIRE:  292 16:49:54    -1801.741030*      21.3083
FIRE:  293 16:49:55    -1801.808355*      33.2232
FIRE:  294 16:49:56    -1801.891771*      48.1107
FIRE:  295 16:49:56    -1802.003134*      37.4647
FIRE:  296 16:49:57    -1802.143925*      36.1138
FIRE:  297 16:49:58    -1802.317743*      24.9072
FIRE:  298 16:49:58    -1802.524590*      39.4083
FIRE:  299 16:49:59    -1802.778225*      28.6337
FIRE:  300 16:50:00    -1803.087330*      33.0789
FIRE:  301 16:50:00    -1803.467571*      39.7419
FIRE:  302 16:50:01    -1803.939909*      29.5077
FIRE:  303 16:50:02    -1804.498838*      86.5741
FIRE:  304 16:50:02    -1805.096512*     220.2998
FIRE:  305 16:50:03    -1805.558899*     524.1461
FIRE:  306 16:50:04    -1805.987411*      40.0788
FIRE:  307 16:50:05    -1805.862288*     273.0672
FIRE:  308 16:50:05    -1805.913946*     236.6964
FIRE:  309 16:50:06    -1805.991222*     162.1347
FIRE:  310 16:50:07    -1806.060665*      77.0298
FIRE:  311 16:50:07    -1806.093904*      66.9355
FIRE:  312 16:50:08    -1806.096233*      62.0461
FIRE:  313 16:50:09    -1806.100679*      54.3183
FIRE:  314 16:50:09    -1806.106819*      45.6873
FIRE:  315 16:50:10    -1806.114653*      36.9726
FIRE:  316 16:50:11    -1806.123756*      29.2509
FIRE:  317 16:50:11    -1806.133707*      28.4365
FIRE:  318 16:50:12    -1806.144928*      27.5099
FIRE:  319 16:50:13    -1806.158901*      25.7488
FIRE:  320 16:50:14    -1806.175415*      28.6475
FIRE:  321 16:50:14    -1806.196375*      32.9051
FIRE:  322 16:50:15    -1806.222416*      30.5879
FIRE:  323 16:50:16    -1806.254385*      20.2432
FIRE:  324 16:50:16    -1806.292706*      18.1700
FIRE:  325 16:50:17    -1806.338648*      20.1854
FIRE:  326 16:50:18    -1806.395599*      27.4766
FIRE:  327 16:50:18    -1806.466736*      19.4705
FIRE:  328 16:50:19    -1806.553963*      18.1434
FIRE:  329 16:50:20    -1806.660244*      23.8976
FIRE:  330 16:50:20    -1806.790873*      18.1171
FIRE:  331 16:50:21    -1806.949024*      21.2709
FIRE:  332 16:50:22    -1807.142109*      19.9633
FIRE:  333 16:50:23    -1807.377113*      18.3499
FIRE:  334 16:50:23    -1807.663988*      18.0289
FIRE:  335 16:50:24    -1808.012684*      33.8160
FIRE:  336 16:50:25    -1808.434422*      41.4747
FIRE:  337 16:50:26    -1808.939999*      71.6841
FIRE:  338 16:50:26    -1809.526028*     135.1077
FIRE:  339 16:50:27    -1810.146355*     353.8209
FIRE:  340 16:50:28    -1810.426455*     385.5728
FIRE:  341 16:50:28    -1810.849251*     282.9666
FIRE:  342 16:50:29    -1811.088066*      66.1306
FIRE:  343 16:50:30    -1811.099075*      61.0204
FIRE:  344 16:50:30    -1811.120247*      53.4741
FIRE:  345 16:50:31    -1811.149040*      46.3300
FIRE:  346 16:50:32    -1811.184397*      43.7966
FIRE:  347 16:50:33    -1811.223988*      37.1870
FIRE:  348 16:50:33    -1811.266331*      39.0798
FIRE:  349 16:50:34    -1811.310368*      40.2055
FIRE:  350 16:50:35    -1811.360544*      25.8503
FIRE:  351 16:50:35    -1811.418131*      37.1540
FIRE:  352 16:50:36    -1811.489902*      48.0449
FIRE:  353 16:50:37    -1811.587292*      36.1936
FIRE:  354 16:50:37    -1811.710087*      26.9605
FIRE:  355 16:50:38    -1811.858923*      27.4327
FIRE:  356 16:50:39    -1812.037611*      23.6367
FIRE:  357 16:50:40    -1812.255255*      29.1286
FIRE:  358 16:50:40    -1812.521381*      30.3146
FIRE:  359 16:50:41    -1812.852928*      38.6074
FIRE:  360 16:50:42    -1813.260269*      45.6679
FIRE:  361 16:50:42    -1813.732183*      94.4371
FIRE:  362 16:50:43    -1814.259567*     277.1966
FIRE:  363 16:50:44    -1814.549618*     368.2322
FIRE:  364 16:50:44    -1814.883070*     253.2373
FIRE:  365 16:50:45    -1815.001631*     188.4719
FIRE:  366 16:50:46    -1815.025555*     137.4569
FIRE:  367 16:50:46    -1815.055830*      61.4363
FIRE:  368 16:50:47    -1815.079754*      40.7912
FIRE:  369 16:50:48    -1815.099232*      60.3210
FIRE:  370 16:50:49    -1815.120403*      93.9962
FIRE:  371 16:50:49    -1815.150255*     107.2692
FIRE:  372 16:50:50    -1815.191540*      93.4784
FIRE:  373 16:50:51    -1815.243622*      46.8569
FIRE:  374 16:50:51    -1815.295704*      41.1943
FIRE:  375 16:50:52    -1815.349480*     111.1539
FIRE:  376 16:50:53    -1815.436495*      78.6302
FIRE:  377 16:50:54    -1815.540447*      32.7819
FIRE:  378 16:50:54    -1815.653715*      83.9994
FIRE:  379 16:50:55    -1815.809750*      26.2401
FIRE:  380 16:50:56    -1815.984627*      90.5975
FIRE:  381 16:50:56    -1816.213068*      27.9204
FIRE:  382 16:50:57    -1816.477501*      85.1170
FIRE:  383 16:50:58    -1816.820480*      38.2075
FIRE:  384 16:50:58    -1817.227398*      28.0172
FIRE:  385 16:50:59    -1817.711380*     102.3247
FIRE:  386 16:51:00    -1818.220768*     338.9057
FIRE:  387 16:51:01    -1818.305666*     385.8868
FIRE:  388 16:51:01    -1818.743917*     301.9980
FIRE:  389 16:51:02    -1819.002211*      71.3766
FIRE:  390 16:51:03    -1819.013643*      66.6071
FIRE:  391 16:51:03    -1819.035238*      58.3333
FIRE:  392 16:51:04    -1819.064878*      49.9828
FIRE:  393 16:51:05    -1819.099812*      45.7181
FIRE:  394 16:51:06    -1819.137497*      36.4673
FIRE:  395 16:51:06    -1819.176029*      45.9337
FIRE:  396 16:51:07    -1819.214985*      51.4149
FIRE:  397 16:51:08    -1819.260080*      34.2819
FIRE:  398 16:51:08    -1819.313644*      42.2979
FIRE:  399 16:51:09    -1819.381182*      50.1136
FIRE:  400 16:51:10    -1819.472643*      36.4228
FIRE:  401 16:51:10    -1819.586123*      27.1764
FIRE:  402 16:51:11    -1819.720985*      29.5589
FIRE:  403 16:51:12    -1819.885489*      29.1666
FIRE:  404 16:51:13    -1820.085136*      33.4227
FIRE:  405 16:51:13    -1820.331150*      39.4629
FIRE:  406 16:51:14    -1820.640255*      31.5822
FIRE:  407 16:51:15    -1821.011181*      60.0084
FIRE:  408 16:51:15    -1821.440117*     120.5329
FIRE:  409 16:51:16    -1821.902081*     330.8937
FIRE:  410 16:51:17    -1822.038425*     379.1618
FIRE:  411 16:51:18    -1822.403423*     297.4668
FIRE:  412 16:51:18    -1822.609634*     105.5998
FIRE:  413 16:51:19    -1822.622761*      86.1874
FIRE:  414 16:51:20    -1822.645203*      65.7905
FIRE:  415 16:51:20    -1822.672937*      50.3008
FIRE:  416 16:51:21    -1822.701307*      45.3632
FIRE:  417 16:51:22    -1822.729677*      61.5541
FIRE:  418 16:51:22    -1822.760376*      83.1978
FIRE:  419 16:51:23    -1822.795732*      78.0566
FIRE:  420 16:51:24    -1822.839769*      37.3021
FIRE:  421 16:51:24    -1822.887405*      41.5064
FIRE:  422 16:51:25    -1822.944569*      75.6175
FIRE:  423 16:51:26    -1823.027138*      45.9471
FIRE:  424 16:51:27    -1823.125374*      37.2891
FIRE:  425 16:51:27    -1823.241182*      55.7824
FIRE:  426 16:51:28    -1823.387054*      26.4523
FIRE:  427 16:51:29    -1823.558968*      59.2620
FIRE:  428 16:51:29    -1823.775553*      29.7028
FIRE:  429 16:51:30    -1824.040409*      39.3119
FIRE:  430 16:51:31    -1824.357136*      96.7603
FIRE:  431 16:51:31    -1824.718111*     149.6757
FIRE:  432 16:51:32    -1825.110209*     310.3924
FIRE:  433 16:51:33    -1825.310068*     368.8151
FIRE:  434 16:51:34    -1825.599695*     258.7631
FIRE:  435 16:51:34    -1825.695179*     190.1873
FIRE:  436 16:51:35    -1825.717197*     144.3051
FIRE:  437 16:51:36    -1825.747684*      80.5236
FIRE:  438 16:51:36    -1825.774149*      40.7820
FIRE:  439 16:51:37    -1825.791298*      68.7236
FIRE:  440 16:51:38    -1825.804424*     122.7806
FIRE:  441 16:51:38    -1825.826866*     141.4377
FIRE:  442 16:51:39    -1825.863705*     116.5147
FIRE:  443 16:51:40    -1825.910282*      40.7451
FIRE:  444 16:51:40    -1825.947756*      69.8885
FIRE:  445 16:51:41    -1825.987135*     136.2399
FIRE:  446 16:51:42    -1826.061871*      86.2378
FIRE:  447 16:51:43    -1826.144440*      50.5361
FIRE:  448 16:51:43    -1826.231031*     108.1125
FIRE:  449 16:51:44    -1826.359966*      17.0316
FIRE:  450 16:51:45    -1826.493347*     105.9526
FIRE:  451 16:51:45    -1826.679445*      20.1435
FIRE:  452 16:51:46    -1826.881422*     119.4513
FIRE:  453 16:51:47    -1827.151571*      97.6267
FIRE:  454 16:51:47    -1827.474014*      41.5524
FIRE:  455 16:51:48    -1827.861031*      32.9981
FIRE:  456 16:51:49    -1828.330404*      98.3928
FIRE:  457 16:51:50    -1828.699425*     514.8524
FIRE:  458 16:51:50    -1827.525673*     822.4120
FIRE:  459 16:51:51    -1829.068022*     307.8562
FIRE:  460 16:51:52    -1829.307261*     295.3814
FIRE:  461 16:51:52    -1829.366753*     220.8519
FIRE:  462 16:51:53    -1829.438313*      96.1280
FIRE:  463 16:51:54    -1829.483408*      82.0705
FIRE:  464 16:51:54    -1829.529562*      86.3701
FIRE:  465 16:51:55    -1829.572117*     113.3996
FIRE:  466 16:51:56    -1829.613190*     178.6559
FIRE:  467 16:51:57    -1829.672894*     206.0828
FIRE:  468 16:51:57    -1829.771130*     167.3574
FIRE:  469 16:51:58    -1829.856028*      51.6142
FIRE:  470 16:51:59    -1829.837397*     329.1641
FIRE:  471 16:51:59    -1829.876564*     235.6474
FIRE:  472 16:52:00    -1829.919966*      92.9158
FIRE:  473 16:52:01    -1829.940502*      41.8986
FIRE:  474 16:52:02    -1829.943466*     119.7705
FIRE:  475 16:52:02    -1829.945160*     115.6655
FIRE:  476 16:52:03    -1829.948759*     106.5815
FIRE:  477 16:52:04    -1829.953205*      94.4340
FIRE:  478 16:52:04    -1829.958921*      78.5064
FIRE:  479 16:52:05    -1829.964638*      58.8477
FIRE:  480 16:52:06    -1829.970566*      37.8955
FIRE:  481 16:52:06    -1829.976282*      23.7194
FIRE:  482 16:52:07    -1829.982210*      20.1158
FIRE:  483 16:52:08    -1829.988773*      31.8837
FIRE:  484 16:52:09    -1829.996395*      48.2722
FIRE:  485 16:52:09    -1830.006134*      58.4998
FIRE:  486 16:52:10    -1830.019472*      57.0730
FIRE:  487 16:52:11    -1830.036409*      42.8795
FIRE:  488 16:52:12    -1830.056946*      22.1711
FIRE:  489 16:52:12    -1830.080235*      16.2580
FIRE:  490 16:52:13    -1830.107758*      33.9708
FIRE:  491 16:52:14    -1830.141420*      42.9470
FIRE:  492 16:52:14    -1830.185246*      30.9745
FIRE:  493 16:52:15    -1830.238174*      16.1934
FIRE:  494 16:52:16    -1830.300631*      35.2793
FIRE:  495 16:52:17    -1830.377483*      37.1695
FIRE:  496 16:52:17    -1830.472332*      16.2617
FIRE:  497 16:52:18    -1830.584965*      35.6324
FIRE:  498 16:52:19    -1830.724697*      16.2335
FIRE:  499 16:52:19    -1830.891953*      42.7074
FIRE:  500 16:52:20    -1831.096893*      24.1346

We could consider instead setting fmax_per_atom.

[shyuep]

There is no such thing called fmax per atom. fmax by its very nature is a per atom definition.
The default fmax for relaxation is 0.1. It is only for phonon and EOS that it is decreased to 0.01. But we can switch to just 0.1 for all properties since the UPs don't have a force accuracy better than 0.1-0.2 eV/A anyway. That will lead to greater stochasticity in the predicted results and errors. But that is limit I guess for now until better UPs are developed.

[janosh]

If we can have a lower fmax for small structures without failing convergence I would keep that. Nothing prevents us from defining fmax = fmax_per_atom * len(structure) where fmax_per_atom is some constant we tune to give optimal results for different-sized structures. Maybe len(structure)**0.5 would give better scaling.

[shyuep]

I think if there is tuning of fmax, it should be done on the fly. Something similar to how neural network optimizers use adaptive learning rates. But I don't think fmax has a relationship with nsites. Extensive energy - yes. That was why we used EDIFF_PER_ATOM for vasp calculations in the past (to disastrous consequences it turns out). But EDIFFG cannot be defined per atom. It is the max force on ANY single atom.

ASE unfortunately does not have an adaptive fmax strategy. To be honest, I am not even convinced FIRE is always the best algo. I have tried FIRE on some hypothetical structures and they refuse to converge even to fmax=0.1 but BFGS did the trick.

Based on the ASE own benchmarks https://wiki.fysik.dtu.dk/gpaw/devel/ase_optimize/ase_optimize.html, it doesn't even seem like FIRE is the optimal one.

[janosh]

Was EDIFF_PER_ATOM the problem or was it just set too loose? 5.0e-05 seems too high. That's 1e-3 for a 20 atom structure, i.e. two orders of magnitude higher than our current EDIFF: 1.e-05.

On the topic of ASE optimizers, were your results with BFGS deterministic? I noticed that CHGNet relaxations can very significantly if you repeat them with the same initial structure. I thought that was due to FIRE but yesterday saw the same behavior with BFGS.

[BowenD-UCB]

The big structure @janosh has tested looks like one of the outliers that we failed to converge, which gets incredibly high energy in the first step. I haven't seen a lot of stochastic relaxation most time.

[JiQi535]

I would like to add that when related to Phonons, it is usually recommended to have small EDIFFG and EDIFF. I am wondering how sensitive the Phonon results of matcal would be for different convergence, say 0.05 vs 0.1 vs 0.2 eV/A. If the difference is not significant, then it should be fine.