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Creators/Authors contains: "Batista, Victor S."

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  6. Accurate quantum dynamics simulations of nonadiabatic processes are important for studies of electron transfer, energy transfer, and photochemical reactions in complex systems. In this comparative study, we benchmark various approximate nonadiabatic dynamics methods with mapping variables against numerically exact calculations based on the tensor-train (TT) representation of high-dimensional arrays, including TT-KSL for zero-temperature dynamics and TT-thermofield dynamics for finite-temperature dynamics. The approximate nonadiabatic dynamics methods investigated include mixed quantum–classical Ehrenfest mean-field and fewest-switches surface hopping, linearized semiclassical mapping dynamics, symmetrized quasiclassical dynamics, the spin-mapping method, and extended classical mapping models. Different model systems were evaluated, including the spin-boson model for nonadiabatic dynamics in the condensed phase, the linear vibronic coupling model for electronic transition through conical intersections, the photoisomerization model of retinal, and Tully’s one-dimensional scattering models. Our calculations show that the optimal choice of approximate dynamical method is system-specific, and the accuracy is sensitively dependent on the zero-point-energy parameter and the initial sampling strategy for the mapping variables.

     
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    Free, publicly-accessible full text available July 14, 2025
  7. Experimental methods capable of selectively probing water at the DNA minor groove, major groove, and phosphate backbone are crucial for understanding how hydration influences DNA structure and function. Chiral-selective sum frequency generation spectroscopy (chiral SFG) is unique among vibrational spectroscopies because it can selectively probe water molecules that form chiral hydration structures around biomolecules. However, interpreting chiral SFG spectra is challenging since both water and the biomolecule can produce chiral SFG signals. Here, we combine experiment and computation to establish a theoretical framework for the rigorous interpretation of chiral SFG spectra of DNA. We demonstrate that chiral SFG detects the N–H stretch of DNA base pairs and the O–H stretch of water, exclusively probing water molecules in the DNA first hydration shell. Our analysis reveals that DNA transfers chirality to water molecules only within the first hydration shell, so they can be probed by chiral SFG spectroscopy. Beyond the first hydration shell, the electric field-induced water structure is symmetric and, therefore, precludes chiral SFG response. Furthermore, we find that chiral SFG can differentiate chiral subpopulations of first hydration shell water molecules at the minor groove, major groove, and phosphate backbone. Our findings challenge the scientific perspective dominant for more than 40 years that the minor groove “spine of hydration” is the only chiral water structure surrounding the DNA double helix. By identifying the molecular origins of the DNA chiral SFG spectrum, we lay a robust experimental and theoretical foundation for applying chiral SFG to explore the chemical and biological physics of DNA hydration.

     
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  10. Parametric gates and processes engineered from the perspective of the static effective Hamiltonian of a driven system are central to quantum technology. However, the perturbative expansions used to derive static effective models may not be able to efficiently capture all the relevant physics of the original system. In this work, we investigate the conditions for the validity of the usual low-order static effective Hamiltonian used to describe a Kerr oscillator under a squeezing drive. This system is of fundamental and technological interest. In particular, it has been used to stabilize Schrödinger cat states, which have applications for quantum computing. We compare the states and energies of the effective static Hamiltonian with the exact Floquet states and quasi-energies of the driven system and determine the parameter regime where the two descriptions agree. Our work brings to light the physics that is left out by ordinary static effective treatments and that can be explored by state-of-the-art experiments.

     
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    Free, publicly-accessible full text available March 25, 2025