TY - JOUR
T1 - Which Options Exist for NISQ-Friendly Linear Response Formulations?
AU - Ziems, Karl Michael
AU - Kjellgren, Erik Rosendahl
AU - Reinholdt, Peter
AU - Jensen, Phillip W.K.
AU - Sauer, Stephan P.A.
AU - Kongsted, Jacob
AU - Coriani, Sonia
PY - 2024
Y1 - 2024
N2 - Linear response (LR) theory is a powerful tool in classic quantum chemistry crucial to understanding photoinduced processes in chemistry and biology. However, performing simulations for large systems and in the case of strong electron correlation remains challenging. Quantum computers are poised to facilitate the simulation of such systems, and recently, a quantum linear response formulation (qLR) was introduced [Kumar et al., J. Chem. Theory Comput. 2023, 19, 9136-9150]. To apply qLR to near-term quantum computers beyond a minimal basis set, we here introduce a resource-efficient qLR theory, using a truncated active-space version of the multiconfigurational self-consistent field LR ansatz. Therein, we investigate eight different near-term qLR formalisms that utilize novel operator transformations that allow the qLR equations to be performed on near-term hardware. Simulating excited state potential energy curves and absorption spectra for various test cases, we identify two promising candidates, dubbed "proj LRSD" and "all-proj LRSD".
AB - Linear response (LR) theory is a powerful tool in classic quantum chemistry crucial to understanding photoinduced processes in chemistry and biology. However, performing simulations for large systems and in the case of strong electron correlation remains challenging. Quantum computers are poised to facilitate the simulation of such systems, and recently, a quantum linear response formulation (qLR) was introduced [Kumar et al., J. Chem. Theory Comput. 2023, 19, 9136-9150]. To apply qLR to near-term quantum computers beyond a minimal basis set, we here introduce a resource-efficient qLR theory, using a truncated active-space version of the multiconfigurational self-consistent field LR ansatz. Therein, we investigate eight different near-term qLR formalisms that utilize novel operator transformations that allow the qLR equations to be performed on near-term hardware. Simulating excited state potential energy curves and absorption spectra for various test cases, we identify two promising candidates, dubbed "proj LRSD" and "all-proj LRSD".
U2 - 10.1021/acs.jctc.3c01402
DO - 10.1021/acs.jctc.3c01402
M3 - Journal article
C2 - 38662999
SN - 1549-9618
VL - 20
SP - 3551
EP - 3565
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
ER -