<div dir="ltr"><span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Dear CP2K developers, <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">while optimizing the cell of 2d layered covalent-organic frameworks (think: graphite with holes) we are encountering instabilities that can seemingly be quenched by increasing the number of layers used in the cell (increasing the K_POINTS works as well).<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Since the materials tend to have a PBE gap above 2eV and should be van-der-Waals bonded only, we find that surprising.<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">In the following we report one of these problematic cases, COF-1, using PBE-D3(BJ) functional.<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Figure 1 shows the starting unit cell, which contains 2 layers of the material (before and after the cell_opt with kpoints). <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"><img src="https://lh5.googleusercontent.com/o3cUphm9FNeYKOJ-RlXj0_BJUhq_UIZb194_Cx-U0jcgFqyMZAT82udeDIcd65EaZoTnj0gCW1zfEGqh4JficKp8wAEtcjmTq7J062Tkq5ZRr6-jX9VzbxWJ6OaJ8OtpJLHgrvlB" width="602" height="409" style="border-width: initial; border-style: none; transform: rotate(0rad);"><span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Figure 2 shows the convergence of the total energy, once using just the Gamma point and once using 1x1x2 k-points (2 k-points along the z direction). Note that for the second one we use DIAGONALIZATION and EXTRAPOLATION=USE_GUESS, as required for using kpoints, but the same CELL_OPT settings. <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"><img src="https://lh3.googleusercontent.com/WJ1Wpwtf-lZ8qTPJVBNJpT0i91Db16kJKPlmJ5KiWRATI-UuYOUzIiuQ-WO0CVv3hmKe5VKYh7CYKwAK1somx_B9pj6s33U9IDYt_vUQf61E0xkBqDj4Zqf3JtsfITn896IPDsQZ" width="602" height="345" style="border-width: initial; border-style: none; transform: rotate(0rad);"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">The cell find its optimal dimension by tilting in the xy plane and, in the case of Gamma calculation, the optimization oscillates without converging.<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">- ot-gamma inp: <a href="https://www.dropbox.com/s/g5usnojtblhomi3/ot_inp.txt?dl=0"><span style="font-size: 11pt; font-family: Arial; background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; text-decoration-line: underline; text-decoration-skip-ink: none; vertical-align: baseline; white-space: pre-wrap;">https://www.dropbox.com/s/g5usnojtblhomi3/ot_inp.txt?dl=0</a><span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">- kpoints inp: <a href="https://www.dropbox.com/s/d69170jnqfuq4g6/kp_inp.txt?dl=0"><span style="font-size: 11pt; font-family: Arial; background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; text-decoration-line: underline; text-decoration-skip-ink: none; vertical-align: baseline; white-space: pre-wrap;">https://www.dropbox.com/s/d69170jnqfuq4g6/kp_inp.txt?dl=0</a><span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">- coord+inputs+outputs zipped: <a href="https://www.dropbox.com/s/k3kl6sw9u8ine2y/cof1_ot_vs_kpoints.zip?dl=1"><span style="font-size: 11pt; font-family: Arial; background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; text-decoration-line: underline; text-decoration-skip-ink: none; vertical-align: baseline; white-space: pre-wrap;">https://www.dropbox.com/s/k3kl6sw9u8ine2y/cof1_ot_vs_kpoints.zip?dl=1</a><span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">We used K-POINTS because the perpendicular width in z direction is 6.920 Angs at the start and gets 6.766 Angsat the end, however we are confused on why the K-POINTS in z directions are so important for the stability of the calculation. Is there any other parameter that I can tune to stabilize the no-K-POINTS+OT calculation?<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">I tested already many options without kpoints, without success (always experiencing jumps in the energy during the CELL_OPT):<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">1) lower EPS_SCF<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">2) higher CUTOFF<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">3) DIAGONALIZATION<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">4) EXTRAPOLATION=USE_GUESS<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">and with (a partial) success:<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">5) Duplicating the cell in z direction gives almost exactly the same result as with K-POINTS (and is more efficients in terms of speed, albeit not an elegant solution)<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">6) CG or (much) lower TRUST_RADIUS=0.1, do not jump but they are *very* inefficient, and therefore not a solution.<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">7) Using the PW code Quantum Espresso (much slower than CP2K for this system) with Gamma approximation. In that case PBE-D3 does always lead to a smooth cell_opt convergence using bfgs. As expected, the z dimension of the cell is small, but "not so small" to cause problems.<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Therefore, the most efficient solution for now it would be to duplicate my 2D materials in the z direction (mod #5) to have a robust convergence with the price of a ~2x slower calculation and having a bigger reference cell. This does not *always* solve the cell_opt convergence problems, but it works for most of the problematic cases. Consider that, as in my previous post on OT convergence problems (<a href="https://groups.google.com/forum/#!msg/cp2k/X8RhYjSVVWc/TXdeLTMUCQAJ"><span style="font-size: 11pt; font-family: Arial; background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; text-decoration-line: underline; text-decoration-skip-ink: none; vertical-align: baseline; white-space: pre-wrap;">https://groups.google.com/forum/#!msg/cp2k/X8RhYjSVVWc/TXdeLTMUCQAJ</a><span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">) our aim is to use general setting for high-throughput calculation. <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Do you have any other suggestion to try solving my problem?<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">I expect that these 2D-layers have a corrugated potential surface: I'm not looking for the absolute minima, but at least a reasonable one without geometry convergence problem. I'm wondering if there are some threshold value that I can tune not to have interference with the CELL_OPT, without increasing much the computational cost (not more than ~2x).<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Any suggestion is welcome, thanks!<span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;"> <span style="font-size: 11pt; font-family: Arial; color: rgb(0, 0, 0); background-color: transparent; font-variant-numeric: normal; font-variant-east-asian: normal; vertical-align: baseline; white-space: pre-wrap;">Daniele Ongari </div>