TY - JOUR
T1 - Using Hyperoptimized Tensor Networks and First-Principles Electronic Structure to Simulate the Experimental Properties of the Giant {Mn84} Torus
AU - Chen, Dian Teng
AU - Helms, Phillip
AU - Hale, Ashlyn R.
AU - Lee, Minseong
AU - Li, Chenghan
AU - Gray, Johnnie
AU - Christou, George
AU - Zapf, Vivien S.
AU - Chan, Garnet Kin Lic
AU - Cheng, Hai Ping
PY - 2022/3/17
Y1 - 2022/3/17
N2 - The single-molecule magnet {Mn84} is a challenge to theory because of its high nuclearity. We directly compute two experimentally accessible observables, the field-dependent magnetization up to 75 T and the temperature-dependent heat capacity, using parameter-free theory. In particular, we use first-principles calculations to derive short- and long-range exchange interactions and compute the exact partition function of the resulting classical Potts and Ising spin models for all 84 Mn S = 2 spins to obtain observables. The latter computation is made possible by using hyperoptimized tensor network contractions, a technique developed to simulate quantum supremacy circuits. We also synthesize the magnet and measure its heat capacity and magnetization, observing qualitative agreement between theory and experiment and identifying an unusual bump in the heat capacity and a plateau in the magnetization. Our work also identifies some limitations of current theoretical modeling in large magnets, such as sensitivity to small, long-range exchange couplings.
AB - The single-molecule magnet {Mn84} is a challenge to theory because of its high nuclearity. We directly compute two experimentally accessible observables, the field-dependent magnetization up to 75 T and the temperature-dependent heat capacity, using parameter-free theory. In particular, we use first-principles calculations to derive short- and long-range exchange interactions and compute the exact partition function of the resulting classical Potts and Ising spin models for all 84 Mn S = 2 spins to obtain observables. The latter computation is made possible by using hyperoptimized tensor network contractions, a technique developed to simulate quantum supremacy circuits. We also synthesize the magnet and measure its heat capacity and magnetization, observing qualitative agreement between theory and experiment and identifying an unusual bump in the heat capacity and a plateau in the magnetization. Our work also identifies some limitations of current theoretical modeling in large magnets, such as sensitivity to small, long-range exchange couplings.
UR - http://www.scopus.com/inward/record.url?scp=85126677512&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.2c00354
DO - 10.1021/acs.jpclett.2c00354
M3 - Article
VL - 13
SP - 2365
EP - 2370
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 10
ER -