Quantum simulations of molecular systems on quantum computers often employ minimal basis sets of Gaussian orbitals. In comparison with more realistic basis sets, quantum simulations employing minimal basis sets require fewer qubits and quantum gates, but yield results of lower accuracy. A natural strategy to achieve more accurate results is to increase the basis set size, which in turn requires increasing the number of qubits and quantum gates. Here we explore the use of intrinsic atomic orbitals (IAOs) in quantum simulations of molecules, to improve the accuracy of energies and properties at the same computational cost required by a minimal basis. We investigate ground-state energies and one- and two-body density operators in the framework of the variational quantum eigensolver, employing and comparing different Ansätze. We also demonstrate the use of this approach in the calculation of ground- and excited-states energies of small molecules by a combination of quantum algorithms, using IBM Quantum computers.
Quantum protocols will be more efficient with high-dimensional entangled states. Photons carrying orbital angular momenta can be used to create a high-dimensional entangled state. In this paper we experimentally demonstrate the entanglement of the orbital angular momentum between the Stokes and anti-Stokes photons generated in a hot atomic ensemble using spontaneous four-wave-mixing. This experiment also suggests the existence of the entanglement concerned with spatial degrees of freedom between the hot atomic ensemble and the Stokes photon.
We report on the storage of orbital angular momentum of light in a cold ensemble of cesium atoms. We employ Bragg diffraction to retrieve the stored optical information impressed into the atomic coherence by the incident light fields. The stored information can be manipulated by an applied magnetic field and we were able to observe collapses and revivals due to the rotation of the stored atomic Zeeman coherence for times longer than 15 $μs$.
We study the effects of time uncertainty in the interaction of atoms with a standing light wave. We discuss its physical origin and the possibility to observe intrinsic decoherence effects by measuring the atomic momentum distribution.
Three-dimensional entanglement of orbital angular momentum states of an atomic qutrit and a single photon qutrit has been observed. Their full state was reconstructed using quantum state tomography. The fidelity to the maximally entangled state of Schmidt rank 3 exceeds the threshold 2/3. This result confirms that the density matrix cannot be decomposed into ensemble of pure states of Schmidt rank 1 or 2. That is, the Schmidt number of the density matrix must be equal to or greater than 3.
Photons carrying a well-defined orbital angular momentum have been proven to modify spectroscopic selection rules in atomic matter. Excitation profiles of electric quadrupole transitions have been measured with single trapped $^{40}$Ca$^+$ ions for varying polarizations. We further develop the photo-absorption formalism to study the case of arbitrary alignment of the beam's optical axis with respect to the ion's quantization axis and mixed multipolarity. Thus, predictions for M1-dominated $^{40}Ar^{13+}$, E3-driven $^{171}Yb^+$ and $^{172}Yb^+$, and B-like $^{20}Ne^{5+}$ are presented. The lat…
Duan-Lukin-Cirac-Zoller (DLCZ) quantum repeater protocol, which was proposed to realize long distance quantum communication, requires usage of quantum memories. Atomic ensembles interacting with optical beams based on off-resonant Raman scattering serve as convenient on-demand quantum memories. Here, a complete free space, three-dimensional theory of the associated read and write process for this quantum memory is worked out with the aim of understanding intrinsic retrieval efficiency. We develop a formalism to calculate the transverse mode structure for the signal and the idler photons and us…
Recently, atomic ensemble and single photons were successfully entangled by using collective enhancement [D. N. Matsukevich, \textit{et al.}, Phys. Rev. Lett. \textbf{95}, 040405(2005).], where atomic internal states and photonic polarization states were correlated in nonlocal manner. Here we experimentally clarified that in an ensemble of atoms and a photon system, there also exists an entanglement concerned with spatial degrees of freedom. Generation of higher-dimensional entanglement between remote atomic ensemble and an application to condensed matter physics are also discussed.
Interaction of spin and intrinsic orbital angular momentum of light is observed, as evidenced by length-dependent rotations of both spatial patterns and optical polarization in a cylindrically-symmetric isotropic optical fiber. Such rotations occur in straight few-mode fiber when superpositions of two modes with parallel and anti-parallel orientation of spin and intrinsic orbital angular momentum (IOAM=$2\hslash$) are excited, resulting from a degeneracy splitting of the propagation constants of the modes.
We propose a scheme to distinguish the orbital angular momentum state of the Laguerre-Gaussian (LG) beam based on the electromagnetically induced transparency modulated by a microwave field in atomic ensembles. We show that the transverse phase variation of a probe beam with the LG mode can be mapped into the spatial intensity distribution due to the change of atomic coherence caused by the microwave. The proposal may provide a useful tool for studying higher-dimensional quantum information based on atomic ensembles.
I study cross dimensionality of $p$-orbital atomic fermions loaded in an optical square lattice with repulsive interactions. The cross-dimensionality emerges when the transverse tunneling of $p$-orbital fermions is negligible. With renormalization group analysis, the system is found to support two dimensional charge, orbital, and spin density wave states with incommensurate wavevectors. The transition temperatures of these states are controlled by perturbations near a one dimensional Luttinger liquid fixed point. Considering transverse tunneling, the cross-dimensionality breaks down and the de…
We demonstrated that by using a pump field with non-zero orbital angular momentum (OAM) in the polarization self-rotation squeezing process it is possible to generate a squeezed vacuum optical field with the matching OAM. We found a similar level of maximum quantum noise reduction for a first-order Laguerre-Gaussian pump beam and a regular Gaussian pump beam, even though the optimal operational conditions differed in these two cases. Also, we investigated the effect of self-defocusing on the level of the vacuum squeezing by simultaneously monitoring the minimum quantum noise level and the outp…
We obtain an expression for the matrix element for a twisted (Laguerre-Gaussian profile) photon scattering from a hydrogen atom. We consider photons incoming with an orbital angular momentum (OAM) of $\ell \hbar$, carried by a factor of $e^{i \ell ϕ}$ not present in a plane-wave or pure Gaussian profile beam. The nature of the transfer of $+2\ell$ units of OAM from the photon to the azimuthal atomic quantum number of the atom is investigated. We obtain simple formulae for these OAM flip transitions for elastic forward scattering of twisted photons when the photon wavelength $λ$ is large compar…
We suggest a technique based on the transfer of topological charge from applied laser radiation to directional and coherent optical fields generated in ladder-type excited atomic media to identify the major processes responsible for their appearance. As an illustration, in Rb vapours we analyse transverse intensity and phase profiles of the forward-directed collimated blue and near-IR light using self-interference and astigmatic transformation techniques when either or both of two resonant laser beams carry orbital angular momentum. Our observations unambiguously demonstrate that emission at 1…
Chemical bonding concepts emerge naturally from maximally entangled atomic orbitals
Ludwig-Maximilians-Universität München（慕尼黑大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）
It is known for a long time that the long range asymptotic behavior of the Hartree-Fock orbitals is different from that of the orbitals in the local potential. However, there is no consensus about observable physical effects associated with this asymptotics. Here we argue that weaker decrease of the Hartree-Fock orbitals at large distances is responsible for the positron annihilation on the inner shell electrons, which is observed experimentally.
We report on the observation and coherent excitation of atoms on the narrow inner-shell orbital transition, connecting the erbium ground state $[\mathrm{Xe}] 4f^{12} (^3\text{H}_6)6s^{2}$ to the excited state $[\mathrm{Xe}] 4f^{11}(^4\text{I}_{15/2})^05d (^5\text{D}_{3/2}) 6s^{2} (15/2,3/2)^0_7$. This transition corresponds to a wavelength of 1299 nm and is optically closed. We perform high-resolution spectroscopy to extract the $g_J$-factor of the $1299$-nm state and to determine the frequency shift for four bosonic isotopes. We further demonstrate coherent control of the atomic state and ext…
Polariton formalism is applied for studying the propagation of a probe field of light in a cloud of cold atoms influenced by two control laser beams of larger intensity. The laser beams couple resonantly three hyperfine atomic ground states to a common excited state thus forming a tripod configuration of the atomic energy levels involved. The first control beam can have an optical vortex with the intensity of the beam going to zero at the vortex core. The second control beam without a vortex ensures the loseless (adiabatic) propagation of the probe beam at a vortex core of the first control la…
We investigate the influence of two resonant laser beams on the mechanical properties of degenerate atomic gases. The control and probe beams of light are considered to have Orbital Angular Momenta (OAM) and act on the three-level atoms in the Electromagnetically Induced Transparency (EIT) configuration. The theory is based on the explicit analysis of the quantum dynamics of cold atoms coupled with two laser beams. Using the adiabatic approximation, we obtain an effective equation of motion for the atoms driven to the dark state. The equation contains a vector potential type interaction as wel…
