Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Surface chemical trapping of optical cycling centers

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/d0cp04525j· OSTI ID:1852891
 [1];  [2];  [2];  [2];  [2];  [2];  [2];  [2]
  1. Univ. of California, Los Angeles, CA (United States); OSTI
  2. Univ. of California, Los Angeles, CA (United States)
+ Show Author Affiliations
Quantum information processors based on trapped atoms utilize laser-induced optical cycling transitions for state preparation and measurement. These transitions consist of an electronic excitation from the ground to an excited state and a decay back to the initial ground state, associated with a photon emission. While this technique has been used primarily with atoms, it has also recently been shown to work for some divalent metal hydroxides (e.g. SrOH) and alkoxides (e.g. SrOCH3). Additionally, this extension to molecules is possible because these molecules feature nearly isolated, atomic-like ground and first-excited electronic states centered on the radical metal atom. We theoretically investigate the extension of this idea to a larger scale by growing the alkyl group, R, beyond the initial methyl group, CH3, while preserving the isolated and highly vertical character of the electronic excitation on the radical metal atom, M. Theory suggests that in the limit as the size of the ligand carbon chain increases, it can be considered a functionalized diamond (or cubic boron nitride) surface. Several requirements must be observed for the cycling centers to function when bound to the surface. First, the surface must have a significant band gap that fully encapsulates both the ground and excited states of the cycling center. Second, while the surface lattice imposes strict limits on the achievable spacing between the SrO– groups, at high coverage, SrO– centers can interact, and show geometric changes and/or electronic state mixing. We show that the coverage of the diamond surface with SrO– cycling centers needs to be significantly sub-monolayer for the functionality of the cycling center to be preserved. Having the lattice-imposed spatial control of SrO– placements will allow nanometer-scale proximity between qubits and will eliminate the need for atom traps for localized cycling emitters. Our results also imply that a functionalization could be done on a scanning microscope tip for local quantum sensing or on photonic structures for optically-mediated quantum information processing.
Research Organization:
Univ. of California, Los Angeles, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0019152; SC0019245
OSTI ID:
1852891
Alternate ID(s):
OSTI ID: 1755972
OSTI ID: 1907374
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 1 Vol. 23; ISSN 1463-9076; ISSN PPCPFQ
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (44)

Proposal for Laser Cooling of Complex Polyatomic Molecules journal November 2016
Internally contracted multiconfiguration-reference configuration interaction calculations for excited states journal October 1992
An efficient method for the evaluation of coupling coefficients in configuration interaction calculations journal April 1988
Treatment of electronic excitations within the adiabatic approximation of time dependent density functional theory journal July 1996
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Hydrogen-terminated diamond surfaces and interfaces journal January 1996
A fast and robust algorithm for Bader decomposition of charge density journal June 2006
Laser spectroscopy of the and transitions of SrOD journal November 2006
New Basis Set Exchange: An Open, Up-to-Date Resource for the Molecular Sciences Community journal October 2019
Large-Scale Benchmark of Exchange–Correlation Functionals for the Determination of Electronic Band Gaps of Solids journal July 2019
Benchmarking the Performance of Time-Dependent Density Functional Theory Methods on Biochromophores journal November 2019
SmB 6 – Cluster Anion: Covalency Involving f Orbitals journal February 2017
Gas-phase inorganic chemistry: laser spectroscopy of calcium and strontium monothiolates and monohydrosulfides journal April 1991
Laser spectroscopy of strontium and calcium monoalkylamides journal May 1987
Laser spectroscopy of alkaline earth monoalkoxide free radicals journal April 1986
Electrostatic catalysis of a Diels–Alder reaction journal March 2016
Quantum simulations with trapped ions journal April 2012
Exchange-correlation functionals for band gaps of solids: benchmark, reparametrization and machine learning journal July 2020
Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy journal January 2005
Accurate Coulomb-fitting basis sets for H to Rn journal January 2006
Adiabatic time-dependent density functional methods for excited state properties journal October 2002
Influence of the exchange screening parameter on the performance of screened hybrid functionals journal December 2006
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
Analytical Hessian of electronic excited states in time-dependent density functional theory with Tamm-Dancoff approximation journal July 2011
Analytical approach for the excited-state Hessian in time-dependent density functional theory: Formalism, implementation, and performance journal November 2011
A second order multiconfiguration SCF procedure with optimum convergence journal June 1985
An efficient internally contracted multiconfiguration–reference configuration interaction method journal November 1988
Rationale for mixing exact exchange with density functional approximations journal December 1996
Toward reliable density functional methods without adjustable parameters: The PBE0 model journal April 1999
Trapped-ion quantum computing: Progress and challenges journal June 2019
A quantum engineer's guide to superconducting qubits journal June 2019
Ab initiomolecular dynamics for liquid metals journal January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal May 1994
Projector augmented-wave method journal December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
High-Fidelity Readout of Trapped-Ion Qubits journal May 2008
Radiative Force from Optical Cycling on a Diatomic Molecule journal November 2009
2D Magneto-Optical Trapping of Diatomic Molecules journal April 2013
Sisyphus Laser Cooling of a Polyatomic Molecule journal April 2017
Generalized Gradient Approximation Made Simple journal October 1996
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] journal February 1997
Fast Quantum Gates for Neutral Atoms journal September 2000
Introduction of Oxygen-Containing Functional Groups onto Diamond Electrode Surfaces by Oxygen Plasma and Anodic Polarization journal January 1999

Similar Records

Metal halide vapor laser
Patent · Mon Jan 19 23:00:00 EST 1976 · OSTI ID:7357084

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
molecular qubits
optical cycling
surface patterning
theory