Effective mass path integral simulations of quasiparticles in condensed phases
Abstract
The quantum manybody problem in condensed phases is often simplified using a quasiparticle description, such as effective mass theory for electron motion in a periodic solid. These approaches are often the basis for understanding many fundamental condensed phase processes, including the molecular mechanisms underlying solar energy harvesting and photocatalysis. Despite the importance of these effective particles, there is still a need for computational methods that can explore their behavior on chemically relevant length and time scales. This is especially true when the interactions between the particles and their environment are important. We introduce an approach for studying quasiparticles in condensed phases by combining effective mass theory with the path integral treatment of quantum particles. This framework incorporates the generally anisotropic electronic band structure of materials into path integral simulation schemes to enable modeling of quasiparticles in quantum confinement, for example. We demonstrate the utility of effective mass path integral simulations by modeling an exciton in solid potassium chloride and electron trapping by a sulfur vacancy in monolayer molybdenum disulfide.
 Publication:

Journal of Chemical Physics
 Pub Date:
 September 2020
 DOI:
 10.1063/5.0020555
 arXiv:
 arXiv:2007.00599
 Bibcode:
 2020JChPh.153l1104R
 Keywords:

 Condensed Matter  Statistical Mechanics;
 Physics  Chemical Physics
 EPrint:
 7 pages, 2 figures