하이니켈 NCM / NCMA 삼원계 양극재

Compact ground-state preparation circuits are essential for early fault-tolerant quantum chemistry. We introduce Variational Imaginary-time Majorana Evolution (VIME), a classical pre-training algorithm that extends operator-projected variational quantum imaginary-time evolution (OVQITE) to molecular electronic structure using a single compiled Majorana-propagation (MP) surrogate graph. We pair VIME with a compressed tiled Unitary Product State (c-tUPS) ansatz that we develop to reduce both classical simulation and quantum state-preparation costs. In the strongly correlated ruthenium complex TLD-1411, active-space calculations requiring up to 52 qubits achieve chemical precision against DMRG reference energies, with energy errors approximately $400\times$ smaller than those from ADAPT-VQE-based variational Majorana-propagation (ADAPT-VMPE). Across the strongly multireference acene series up to heptacene (60 qubits), VIME matches or improves on the MP-reported energy accuracy of the ADAPT-VMPE comparison points with up to $26\times$ fewer CNOTs and $167\times$ lower two-qubit depth. These results establish imaginary-time classical pre-training of compressed variational ansätze as a promising route to resource-efficient molecular ground-state preparation.

Nuclear quantum effects are critical for describing proton transfer and hydrogen bonding, but their incorporation into quantum chemistry calculations is often computationally prohibitive on classical hardware. A promising alternative are quantum computers due to their linear scaling in the space requirements with system size. We introduce a novel hybrid quantum-classical algorithm for ab-initio molecular dynamics that incorporates nuclear quantum effects via the nuclear-electronic orbital method. The proposed algorithm evaluates ground state energies and forces on the quantum computer using a variational quantum eigensolver, while the molecular geometries are updated classically. We validate our approach through simulations of $\text{H}_2$, $\text{H}_2\text{O}$ and the Zundel ion $\text{H}_5\text{O}_2^+$, comparing the simulated vibrational spectra with experimental data. Upon inclusion of nuclear quantum effects, the proton shuttling movement in the Zundel ion becomes effectively barrierless, and errors in the simulated frequencies improve significantly. Employing compact hardware-efficient ansatz circuits we achieve results comparable to the more accurate UCCSD ansatzes, which hints towards the feasibility of executing our algorithm on near-term quantum devices.

The photostability of DNA nucleobases relies on ultrafast nonradiative relaxation following ultraviolet excitation. In thymine, the competition between internal conversion (IC) and intersystem crossing (ISC) determines the balance between ultrafast energy dissipation and potentially long-lived photochemistry. However, the precise molecular mechanisms linking early singlet-state electronic and structural evolution to the formation of long-lived triplet dark states remain unresolved. Here, we investigate the gas-phase photodynamics of thymine using time-resolved multi-center X-ray photoelectron spectroscopy (tr-mc-XPS) supported by state-of-the-art ab initio quantum calculations. By simultaneously probing multiple carbon 1s core levels, we track site-specific electronic and nuclear dynamics. We discover that the long-lived dark state is not initially a pure triplet; rather, it exists as a mixture of singlet and triplet states for the first 240 ps before transitioning fully to the $^3ππ^*$ state. On the femtosecond timescale, we resolve atom-specific vibrational coherence at $\sim$730 cm$^{-1}$ (a ring-breathing mode with a period of 46 fs) that survives the initial $^1ππ^*$ to $^1nπ^*$ IC. Furthermore, we identify a critical dual role for the methyl group (C9H$_3$). During singlet relaxation, the methyl group acts as an inertia spectator, and its mass hinders direct internal conversion to the ground state. Upon $^3ππ^*$ state formation, however, state-dependent hyperconjugation couples the methyl group to the pyrimidine ring, turning it into a highly sensitive electronic reporter of ISC. These findings establish tr-mc-XPS as a powerful approach for disentangling the complex, multi-timescale photodynamics governing nucleobase stability.