Abstract
Crystallisation pathways are explored by direct analysis of the potential energy landscape for a system of Lennard-Jones particles with periodic boundary conditions. A database of minima and transition states linking liquid and crystalline states is constructed using discrete path sampling and the entire potential energy landscape from liquid to crystal is visualised. We demonstrate that there is a strong negative correlation between the number of atoms in the largest crystalline cluster and the potential energy. In common with previous results we find a strong bias towards the growth of FCC rather than HCP clusters, despite a very small potential energy difference. We characterise three types of perfect crystals with very similar energies: pure FCC, pure HCP, and combinations of FCC and HCP layers. There are also many slightly defective crystalline structures. The effect of the simulation box is analysed for a supercell containing 864 atoms. There are low barriers between some of the different crystalline structures via pathways involving sliding layers, and many different defective structures with FCC layers stacked at an angle to the periodic box. Finally, we compare a binary Lennard-Jones system and visualise the potential energy landscape from supercooled liquid to crystal.
Highlights
ContentsCrystallisation is the formation of an ordered solid from a disordered liquid
We will describe the energy landscape obtained from discrete path sampling for the 864-atom Lennard-Jones supercell defined above
Having found an initial path between the liquid and crystalline states we explored the landscape in the crystal/nucleation region around it
Summary
Crystallisation is the formation of an ordered solid from a disordered liquid. The average w1.a itIinntgrotidmuectbieotnween such events is much longer than the timescale of the proces2s itsel1f.,1s.o Pitocteonntsitaitluetneesrgayralarendesvceanpte.sI. E.n.er.g.y o4f the 1sy.3s.t eCmr.yRstaarleliseavteinotns oafrethdei Lceunlntatrod-sJtoundeyseflxupiedr.im. N. u.cle7i form spontaneously in a supersaturated solution, but redissolve rather than grow, 2un. The probability that a critical nucleus form8s spon2t.1a.n eOourdsleyr, paanrdamtheeterssp.e.ed. The probability that a critical nucleus form8s spon2t.1a.n eOourdsleyr, paanrdamtheeterssp.e.ed. .at. .w.hi.ch. .it. s.u.bs.e.qu. e.n.tl.y .g.ro.w.s,. d. e.te. r.m.in.e. t.h.e .cr.y.sta8l nucl2e.a2t. ioLnowra-teen.eCrgryyssttarlulicstautrieosn. .ca.n. b. e. s.tu. d. ie. d. e. x.p.er.im. e.n.ta. ll.y. w. i.th. .co.ll.oi.d.al. s.u.sp.e1n1-
Sign-in/Register to view highlights & summary Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callMore From: Journal of Statistical Mechanics: Theory and Experiment
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
