Search results for "Quantum"
showing 10 items of 9714 documents
On fermionic shadow wave functions for strongly correlated multi-reference systems based on a single Slater determinant
2015
We demonstrate that extending the Shadow Wave Function to fermionic systems facilitates to accurately calculate strongly-correlated multi-reference systems such as the stretched H2 molecule. This development considerably extends the scope of electronic structure calculations and enables to efficiently recover the static correlation energy using just a single Slater determinant.
Resonating valence bond quantum Monte Carlo: Application to the ozone molecule
2015
We study the potential energy surface of the ozone molecule by means of Quantum Monte Carlo simulations based on the resonating valence bond concept. The trial wave function consists of an antisymmetrized geminal power arranged in a single-determinant that is multiplied by a Jastrow correlation factor. Whereas the determinantal part incorporates static correlation effects, the augmented real-space correlation factor accounts for the dynamics electron correlation. The accuracy of this approach is demonstrated by computing the potential energy surface for the ozone molecule in three vibrational states: symmetric, asymmetric and scissoring. We find that the employed wave function provides a de…
Nuclear quantum effects in liquid water from path-integral simulations using anab initioforce-matching approach
2014
We have applied path integral simulations, in combination with new ab initio based water potentials, to investigate nuclear quantum effects in liquid water. Because direct ab initio path integral simulations are computationally expensive, a flexible water model is parameterized by force-matching to density functional theory-based molecular dynamics simulations. The resulting effective potentials provide an inexpensive replacement for direct ab inito molecular dynamics simulations and allow efficient simulation of nuclear quantum effects. Static and dynamic properties of liquid water at ambient conditions are presented and the role of nuclear quantum effects, exchange-correlation functionals…
A new monomeric interpretation of intrinsic optical bistability observed in Yb3+-doped bromide materials
2003
We present a mechanism able to show intrinsic bistable behaviour involving single Yb3+ ions embedded into bromide lattices, in which intrinsic optical bistability (IOB) has been observed. The mechanism is based on the experimentally found coupling between the Yb3+ ion and the totally symmetric local mode of vibration of the [YbBr6]3- coordination unit. The model reproduces the IOB observed in CsCdBr3:1% Yb3+ and allows to understand the experimentally found presence of the phenomenon in the other bromides, but its absence in Cs3Lu2Cl9:Yb3+.
Nitrogen-Vacancy Magnetometry of Individual Fe-Triazole Spin Crossover Nanorods
2023
[Fe(Htrz)2(trz)](BF4) (Fe-triazole) spin crossover molecules show thermal, electrical, and optical switching between high spin (HS) and low spin (LS) states, making them promising candidates for molecular spintronics. The LS and HS transitions originate from the electronic configurations of Fe(II), and are considered to be diamagnetic and paramagnetic respectively. The Fe(II) LS state has six paired electrons in the ground states with no interaction with the magnetic field and a diamagnetic behavior is usually observed. While the bulk magnetic properties of Fe-triazole compounds are widely studied by standard magnetometry techniques their properties at the individual level are missing. Here…
Algorithmic Cooling of Nuclear Spin Pairs using a Long-Lived Singlet State
2019
Algorithmic cooling methods manipulate an open quantum system in order to lower its temperature below that of the environment. We show that significant cooling is achieved on an ensemble of spin-pair systems by exploiting the long-lived nuclear singlet state, which is an antisymmetric quantum superposition of the "up" and "down" qubit states. The effect is demonstrated by nuclear magnetic resonance (NMR) experiments on a molecular system containing a coupled pair of near-equivalent 13C nuclei. The populations of the system are subjected to a repeating sequence of cyclic permutations separated by relaxation intervals. The long-lived nuclear singlet order is pumped well beyond the unitary lim…
Theory for polaritonic quantum tunneling
2022
I investigate the tunneling decay rate of a polaritonic system formed by a strong coupling between a vacuum cavity mode and $N$ metastable systems. Using a simple model potential, I find the instanton solutions controlling the low-temperature tunneling rate. The resulting rate modification due to the cavity is proportional to the mean of the second power of the light-matter coupling. No collective effect that would enhance the rates by a factor of $\sqrt{N}$ is present, which is in line with the results in the thermal activation regime.
The evolution and revival structure of angular momentum quantum wave packets (Tutorial)
1999
In this paper a coherent superposition of angular momentum states created by absorption of polarized light by molecules is analyzed. Attention is paid to the time evolution of wave packets representing spatial orientation of internuclear axis of diatomic molecule. Two examples are considered in detail. Molecules absorbing light in a permanent magnetic field experiencing Zeeman effect and molecules absorbing light in a permanent electric field experiencing quadratic Stark effect. In a magnetic field we have a wave packet that evolves in time exactly as classical dipole oscillator in a permanent magnetic field. In the second case we have the wave packet that goes through periodical changes of…
Cavity-induced bifurcation in classical rate theory
2022
We show how coupling an ensemble of bistable systems to a common cavity field affects the collective stochastic behavior of this ensemble. In particular, the cavity provides an effective interaction between the systems, and parametrically modifies the transition rates between the metastable states. We predict that the cavity induces a collective phase transition at a critical temperature which depends linearly on the number of systems. It shows up as a spontaneous symmetry breaking where the stationary states of the bistable system bifurcate. We observe that the transition rates slow down independently of the phase transition, but the rate modification vanishes for alternating signs of the …
Geometry of Degeneracy in Potential and Density Space
2022
In a previous work [J. Chem. Phys. 155, 244111 (2021)], we found counterexamples to the fundamental Hohenberg-Kohn theorem from density-functional theory in finite-lattice systems represented by graphs. Here, we demonstrate that this only occurs at very peculiar and rare densities, those where density sets arising from degenerate ground states, called degeneracy regions, touch each other or the boundary of the whole density domain. Degeneracy regions are shown to generally be in the shape of the convex hull of an algebraic variety, even in the continuum setting. The geometry arising between density regions and the potentials that create them is analyzed and explained with examples that, amo…