TY - JOUR
T1 - Subspace methods for the simulation of molecular response properties on a quantum computer
AU - Reinholdt, Peter
AU - Kjellgren, Erik Rosendahl
AU - Fuglsbjerg, Juliane Holst
AU - Ziems, Karl Michael
AU - Coriani, Sonia
AU - Sauer, Stephan P. A.
AU - Kongsted, Jacob
PY - 2024/5/1
Y1 - 2024/5/1
N2 - We explore Davidson methods for obtaining excitation energies and other linear response properties within quantum self-consistent linear response (q-sc-LR) theory. Davidson-type methods allow for obtaining only a few selected excitation energies without explicitly constructing the electronic Hessian since they only require the ability to perform Hessian-vector multiplications. We apply the Davidson method to calculate the excitation energies of hydrogen chains (up to H10) and analyze aspects of statistical noise for computing excitation energies on quantum simulators. Additionally, we apply Davidson methods for computing linear response properties such as static polarizabilities for H2, LiH, H2O, OH−, and NH3, and show that unitary coupled cluster outperforms classical projected coupled cluster for molecular systems with strong correlation. Finally, we formulate the Davidson method for damped (complex) linear response, with application to the nitrogen K-edge X-ray absorption of ammonia, and the C6 coefficients of H2, LiH, H2O, OH−, and NH3.
AB - We explore Davidson methods for obtaining excitation energies and other linear response properties within quantum self-consistent linear response (q-sc-LR) theory. Davidson-type methods allow for obtaining only a few selected excitation energies without explicitly constructing the electronic Hessian since they only require the ability to perform Hessian-vector multiplications. We apply the Davidson method to calculate the excitation energies of hydrogen chains (up to H10) and analyze aspects of statistical noise for computing excitation energies on quantum simulators. Additionally, we apply Davidson methods for computing linear response properties such as static polarizabilities for H2, LiH, H2O, OH−, and NH3, and show that unitary coupled cluster outperforms classical projected coupled cluster for molecular systems with strong correlation. Finally, we formulate the Davidson method for damped (complex) linear response, with application to the nitrogen K-edge X-ray absorption of ammonia, and the C6 coefficients of H2, LiH, H2O, OH−, and NH3.
KW - Faculty of Science
KW - Quantum Computing
KW - linear response theory
KW - excitation energies
KW - polarizability
U2 - 10.48550/arXiv.2402.12186
DO - 10.48550/arXiv.2402.12186
M3 - Journal article
C2 - 38691524
VL - 20
SP - 3729
EP - 3740
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
SN - 1549-9618
IS - 9
ER -