Optical spin-state polarization in a binuclear europium complex towards molecule-based coherent light-spin interfaces

AbstractThe success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ion (REI)-based molecular systems, whose quantum properties could be tuned taking advantage of molecular engineering strategies, are one of the systems actively pursued for the implementation of QIP schemes. Herein, we demonstrate the efficient polarization of ground-state nuclear spins—a fundamental requirement for all-optical spin initialization and addressing—in a binuclear Eu(III) complex, featuring inhomogeneously broadened 5D0 → 7F0 optical transition. At 1.4 K, long-lived spectral holes have been burnt in the transition: homogeneous linewidth (Γh) = 22 ± 1 MHz, which translates as optical coherence lifetime (T2opt) = 14.5 ± 0.7 ns, and ground-state spin population lifetime (T1spin) = 1.6 ± 0.4 s have been obtained. The results presented in this study could be a progressive step towards the realization of molecule-based coherent light-spin QIP interfaces.

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Molecule-based coherent light-spin interfaces for quantum information processing – optical spin state polarization in a binuclear Europium complex

10.21203/rs.3.rs-131741/v1 ◽

2021 ◽

Author(s):

Kuppusamy Senthil Kumar ◽

Diana Serrano ◽

Aline Nonat ◽

Benoît Heinrich ◽

Lydia Karmazin ◽

...

Keyword(s):

Information Processing ◽

Quantum Information ◽

Ground State ◽

Quantum Information Processing ◽

Optical Transition ◽

Molecular Engineering ◽

Coherent Light ◽

Rare Earth Ion ◽

Homogeneous Linewidth ◽

State Spin

Abstract The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ion (REI)- based molecular systems, whose quantum properties could be tuned taking advantage of molecular engineering strategies, are one of the systems actively pursued for the implementation of QIP schemes. Herein, we demonstrate the efficient polarization of 2 ground-state nuclear spins—a fundamental requirement for all-optical spin initialization and addressing—in a binuclear Eu(III) complex, featuring inhomogeneously broadened 5D0→7 F0 optical transition. At 1.4 K, long-lived spectral holes have been burnt in the transition: homogeneous linewidth (Γh) = 22 +/- 1 MHz, which translates as optical coherence lifetime (T2opt) = 14.5 +/- 0.7 ns, and ground-state spin population lifetime (T1spin) = 1.6 +/- 0.4 s have been obtained. The results presented in this study are a progressive step towards the realization of molecule-based coherent light-spin QIP interfaces.

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Optically addressable molecular spins for quantum information processing

Science ◽

10.1126/science.abb9352 ◽

2020 ◽

Vol 370 (6522) ◽

pp. 1309-1312 ◽

Cited By ~ 1

Author(s):

S. L. Bayliss ◽

D. W. Laorenza ◽

P. J. Mintun ◽

B. D. Kovos ◽

D. E. Freedman ◽

...

Keyword(s):

Quantum Information ◽

Ground State ◽

Information Science ◽

Quantum Information Processing ◽

Building Blocks ◽

Quantum Systems ◽

Quantum Information Science ◽

Molecular Systems ◽

Wide Range ◽

State Spin

Spin-bearing molecules are promising building blocks for quantum technologies as they can be chemically tuned, assembled into scalable arrays, and readily incorporated into diverse device architectures. In molecular systems, optically addressing ground-state spins would enable a wide range of applications in quantum information science, as has been demonstrated for solid-state defects. However, this important functionality has remained elusive for molecules. Here, we demonstrate such optical addressability in a series of synthesized organometallic, chromium(IV) molecules. These compounds display a ground-state spin that can be initialized and read out using light and coherently manipulated with microwaves. In addition, through atomistic modification of the molecular structure, we vary the spin and optical properties of these compounds, indicating promise for designer quantum systems synthesized from the bottom-up.

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Однородные и неоднородные ширины линий в оптических спектрах кристалла Y-=SUB=-2-=/SUB=-SiO-=SUB=-5-=/SUB=- : -=SUP=-171-=/SUP=-Yb-=SUP=-3+-=/SUP=-

Оптика и спектроскопия ◽

10.21883/os.2022.01.51885.29-21 ◽

2022 ◽

Vol 130 (1) ◽

pp. 23

Author(s):

Eloise Lafitte-Houssat ◽

Alban Ferrier ◽

Mikael Afzelius ◽

Perrine Berger ◽

Loic Morvan ◽

...

Keyword(s):

Rare Earth ◽

Ground State ◽

Spin Systems ◽

Rare Earth Ions ◽

Zero Magnetic Field ◽

Unusual Property ◽

Nuclear Spins ◽

Spin Coherence ◽

Slowing Down ◽

State Spin

Rare earth ions are actively investigated as optically addressable spin systems for quantum technologies thanks to their long optical and spin coherence lifetimes. 171Yb3+, which has 1/2 electron and nuclear spins, recently raised interest for its simple hyperfine structure that moreover can result in long coherence lifetimes at zero magnetic field, an unusual property for paramagnetic rare earth ions. Here, we report on the optical inhomogeneous and homogeneous linewidths in 171Yb3+:Y2SiO5 (site 2) for different doping concentrations. While inhomogeneous linewidth is not correlated to 171Yb3+ concentration, the homogeneous one strongly decreases between 10 and 2 ppm doping level, reaching 255 Hz at 3 K. This is attributed to a slowing down of 171Yb3+ ground state spin flip-flops.

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Shape coexistence inBr71and the question of the ground-state spin ofKr71

Physical Review C ◽

10.1103/physrevc.72.024321 ◽

2005 ◽

Vol 72 (2) ◽

Cited By ~ 9

Author(s):

S. M. Fischer ◽

T. Anderson ◽

P. Kerns ◽

G. Mesoloras ◽

D. Svelnys ◽

...

Keyword(s):

Ground State ◽

Shape Coexistence ◽

Ground State Spin ◽

State Spin

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A Class of Non-Kekulé Molecules with Low Excitation Energies

Zeitschrift für Naturforschung B ◽

10.1515/znb-2007-1112 ◽

2007 ◽

Vol 62 (11) ◽

pp. 1433-1436

Author(s):

Fritz Dietz ◽

Nedko Drebov ◽

Nikolai Tyutyulkov

Keyword(s):

Molecular Orbital ◽

Ground State ◽

Excitation Energies ◽

Triplet Ground State ◽

Molecular Systems ◽

Structural Principle

A class of non-Kekulé molecular systems with a new structural principle and low excitation energies or with a triplet ground state was investigated theoretically. The systems consist of a non-Kekulé monoradical, possessing a non-bonding molecular orbital linked in a specific way to another monoradical.

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A Mn17Octahedron with a Giant Ground-State Spin: Occurrence in Discrete Form and as Multidimensional Coordination Polymers

Inorganic Chemistry ◽

10.1021/ic801795x ◽

2009 ◽

Vol 48 (12) ◽

pp. 5049-5051 ◽

Cited By ~ 102

Author(s):

Eleni E. Moushi ◽

Theocharis C. Stamatatos ◽

Wolfgang Wernsdorfer ◽

Vassilios Nastopoulos ◽

George Christou ◽

...

Keyword(s):

Coordination Polymers ◽

Ground State ◽

Discrete Form ◽

Ground State Spin ◽

State Spin

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Application of multireference linearized coupled-cluster theory to atomic and molecular systems

Journal of Theoretical and Computational Chemistry ◽

10.1142/s0219633618500165 ◽

2018 ◽

Vol 17 (02) ◽

pp. 1850016 ◽

Cited By ~ 2

Author(s):

Jiang Yi ◽

Feiwu Chen

Keyword(s):

Ground State ◽

Basis Sets ◽

Coupled Cluster ◽

Vibration Frequencies ◽

Electron Affinities ◽

Proton Affinities ◽

Coupled Cluster Theory ◽

Molecular Systems ◽

Ground State Energies ◽

Second Order Perturbation Theory

Applications of the multireference linearized coupled-cluster single-doubles (MRLCCSD) to atomic and molecular systems have been carried out. MRLCCSD is exploited to calculate the ground-state energies of HF, H2O, NH3, CH4, N2, BF, and C2with basis sets, cc-pVDZ, cc-pVTZ and cc-pVQZ. The equilibrium bond lengths and vibration frequencies of HF, HCl, Li2, LiH, LiF, LiBr, BH, and AlF are computed with MRLCCSD and compared with the experimental data. The electron affinities of F and CH as well as the proton affinities of H2O and NH3are also calculated with MRLCCSD. These results are compared with the results produced with second-order perturbation theory, linearized coupled-cluster doubles (LCCD), coupled-cluster doubles (CCD), coupled-cluster singles and doubles (CCSD), CCSD with perturbative triples correction (CCSD(T)). It is shown that all results obtained with MRLCCSD are reliable and accurate.

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On the Ground State Spin of Ti47and Mn55

Progress of Theoretical Physics ◽

10.1143/ptp.18.661 ◽

1957 ◽

Vol 18 (6) ◽

pp. 661-662 ◽

Cited By ~ 1

Author(s):

Sadaaki Yanagawa

Keyword(s):

Ground State ◽

Ground State Spin ◽

State Spin

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Увеличение эффективности тандема полупроводниковый лазер-оптический усилитель на основе самоорганизующихся 8s квантовых точек

Физика и техника полупроводников ◽

10.21883/ftp.2021.12.51710.9713 ◽

2021 ◽

Vol 55 (12) ◽

pp. 1223

Author(s):

А.Е. Жуков ◽

Н.В. Крыжановская ◽

Э.И. Моисеев ◽

А.С. Драгунова ◽

А.М. Надточий ◽

...

Keyword(s):

Quantum Dots ◽

Excited State ◽

Laser Diode ◽

Ground State ◽

Semiconductor Optical Amplifier ◽

Optical Transition ◽

Optical Amplifier ◽

Rate Equations ◽

Resonator Length ◽

Optimal Value

The rate equations are used to analyze the characteristics of a tandem consisting of a laser diode and a semiconductor optical amplifier made of a single heterostructure with quantum dots. The optimal value of the current distribution coefficient the amplifier and the laser, as well as the optimal resonator length that provides the highest output power of the tandem were determined. It is shown that the use of the tandem allows, at the same total consumed current, to significantly (more than 4 times for 1 A) increase the power emitted through the ground-state optical transition in comparison with that achievable with a laser diode solely being limited by the onset of lasing through an excited-state optical transition.

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