Optical spin-orbit coupling is an important phenomenon and has fruitful applications. Here, we investigate the spin-orbit total angular momentum entanglement in the optical parametric downconversion process. Four pairs of entangled vector vortex modes are experimentally generated directly using a dispersion- and astigmatism-compensated single optical parametric oscillator, and for the first time, to the best of our knowledge, the spin-orbit quantum states are characterized on the quantum higher-order Poincaré sphere, and the relationship of spin-orbit total angular momentum Stokes entanglement is demonstrated. These states have potential applications in high-dimensional quantum communication and multiparameter measurement.
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http://dx.doi.org/10.1364/OL.487569 | DOI Listing |
J Phys Chem A
January 2025
School of Physical Science and Technology, Southwest University, Chongqing 400715, China.
Searching for single-molecule magnets (SMM) with large effective blocking barriers, long relaxation times, and high magnetic blocking temperatures is vitally important not only for the fundamental research of magnetism at the molecular level but also for the realization of new-generation magnetic memory unit. Actinides (An) atoms possess extremely strong spin-orbit coupling (SOC) due to their 5 orbitals, and their ground multiplets are largely split into several sublevels because of the strong interplay between the SOC of An atoms and the crystal field (CF) formed by ligand atoms. Compared to TM-based SMMs, more dispersed energy level widths of An-based SMMs will give a larger total zero field splitting (ZFS) and thus provide a necessary condition to derive a higher .
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States.
We revisit the naked transition metal cation (Ti) and methanol reaction and go beyond the standard Landau-Zener (LZ) picture when modeling the intersystem crossing (ISC) rate between the lowest doublet and quartet states. We use both (i) unconstrained Born-Oppenheimer molecular dynamics (BOMD) calculations with an approximate two-state method to estimate population transfer between spin diabats and (ii) constrained dynamics to explore energetically accessible portions of the - 1 crossing seam, where is the total number of internal degrees of freedom. Whereas previous LZ calculations (that necessarily relied on the Condon approximation to be valid) fell short and predicted much slower crossing probabilities than shown in experiment, we show that ISC can occur rapidly because the spin-orbit coupling (SOC) between the doublet and quartet surfaces can vary by 2 orders of magnitude (depending on where in the seam the crossing occurs during dynamics) and the crossing region is revisited multiple times during a dynamics run of a few hundred femtoseconds.
View Article and Find Full Text PDFPhys Chem Chem Phys
December 2024
Physics and Chemistry of Materials (T-1), Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
In the present work, we studied 27 FeH and 6 FeH electronic states using multireference configuration interaction (MRCI), Davidson-corrected MRCI (MRCI+Q), and coupled cluster singles doubles and perturbative triples [CCSD(T)] wavefunction theory (WFT) calculations conjoined with large quadruple- and quintuple- quality correlation consistent basis sets. We report their potential energy curves (PEC), energy related properties, spectroscopic parameters, and spin-orbit couplings. Dipole moment curves (DMC) and transition dipole moment curves (TDMC) of several low-lying electronic states of FeH and FeH are also introduced.
View Article and Find Full Text PDFAdv Mater
December 2024
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, Guangdong, 518055, China.
Vectorial metasurface holography, allowing for independent control over the amplitude, phase, and polarization distribution of holographic images enabled by metasurfaces, plays a crucial role in the realm of optical display, optical, and quantum communications. However, previous research on vectorial metasurface holography has typically been restricted to single degree of freedom input and single channel output, thereby demonstrating a very limited modulation capacity. This work presents a novel method to achieve multi-channel vectorial metasurface holography by harnessing spin-orbit-locking vortex beams.
View Article and Find Full Text PDFJ Phys Chem A
November 2024
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, China.
The S(D) + D → SD + D reaction is a prototype insertion chemical reaction that involves spin-orbit interactions in the exit channel. In this work, we report spin-orbit state-resolved differential cross sections (DCSs) of this reaction obtained by crossed beam experiments at collision energies of 266.2 and 206.
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