arXiv subjects

Guanming Lao

Publications and source records attributed to Guanming Lao.

10 recordsLinked to original sources

arXiv2026

Yttrium ion as a platform for quantum information processing

Engineering large-scale quantum computers which simultaneously provide high-fidelity quantum operations, low memory errors, low crosstalk, and reasonable resource usage remains an outstanding challenge across quantum computing platforms. In trapped ions, progress has largely focused on alkaline-earth and ytterbium ions, whose simple electronic structures facilitate control over their internal state. Here we investigate singly-ionized yttrium ($^{89}\mathrm{Y}^+$), a two-valence-electron ion whose ground-state manifold hosts a nuclear-spin qubit and which also features a variety of low-lying metastable manifolds, for applications in quantum information processing. Because experimental data are limited, we perform high-resolution laser-induced fluorescence spectroscopy to measure the hyperfine structure of several low-lying levels, and carry out comprehensive electronic structure calculations to determine lifetimes, transition matrix elements, and hyperfine coefficients for manifolds addressable with visible, near-visible, or infrared wavelengths. Using these results, we analyze schemes for qubit storage, initialization, readout, leakage mitigation, and single- and two-qubit gates. These results position $^{89}\mathrm{Y}^+$ as a uniquely capable next-generation trapped-ion qubit, combining field-insensitive nuclear-spin or clock-qubit storage with spectrally isolated transitions for operations.

quant-ph↗

arXiv2026

A Surface-Scaffolded Molecular Qubit

Fluorescent spin qubits are central building blocks of quantum technologies. Placing these qubits at surfaces maximizes coupling to nearby spins and fields, enabling nanoscale sensing and facilitating integration with photonic and superconducting devices. However, reducing the dimensions or size of established qubit systems without sacrificing the qubit performance or degrading the coherence lifetime remains challenging. Here, we introduce a surface molecular qubit formed by pentacene molecules scaffolded on a two-dimensional (2D) material, hexagonal boron nitride (hBN). The qubit exhibits stable fluorescence and optically detected magnetic resonance (ODMR) from cryogenic to ambient conditions. With fully deuterated pentacene, the Hahn-echo coherence reaches 22 $μ$s and further extends to 214 $μ$s under dynamical decoupling, outperforming state-of-the-art shallow NV centers in diamond, despite being positioned directly on the surface. We map the local spin environment, resolving couplings to nearby nuclear and electron spins that can serve as auxiliary quantum resources. This platform combines true surface integration, long qubit coherence, and scalable fabrication, opening routes to quantum sensing, quantum simulation, and hybrid quantum devices. It also paves the way for a broader family of 2D material-supported molecular qubits.

quant-ph↗

arXiv2025

Unraveling vibronic interactions in molecules functionalized with optical cycling centers

We report detailed characterization of the vibronic interactions between the first two electronically excited states, A and B, in SrOPh (Ph = phenyl, -C6H5) and its deuterated counterpart, SrOPh-d5 (-C6D5). The vibronic interactions, which arise due to non-adiabatic coupling between the two electronic states, mix the B,v0 state with the energetically close vibronic level A,v21v33, resulting in extra transition probability into the latter state. This state mixing is more prominent in the deuterated molecule because of the smaller energy gap between the interacting states. We model the mixing of the A and B states using the Koppel-Domcke-Cederbaum (KDC) Hamiltonian parametrized in the diabatic framework of Ichino, Gauss, and Stanton on the basis of equation-of-motion coupled-cluster calculations. The simulation attributes the observed mixing to a second-order effect mediated by linear quasi-diabatic couplings between the A-C and B-C states. Based on the measured spectra, we deduce an effective coupling strength of 0.5 cm-1. Non-adiabatic couplings between different electronic states is an important factor that should be considered in the design of laser-cooling protocols for complex molecules.

physics.chem-ph↗

arXiv2025

Vibronic coupling limits the use of high-lying electronic states in complex molecules for laser cooling

Laser cooling of large, complex molecules is a long-standing goal, instrumental for enabling new quantum technology and precision measurements. A primary consideration for the feasibility of laser cooling, which determines the efficiency and technical requirements of the process, is the number of excited-state decay pathways leading to vibrational excitations. Therefore, the assessment of the laser-cooling potential of a molecule begins with estimate of the vibrational branching ratios of the first few electronic excited states theoretically to find the optimum cooling scheme. Such calculations, typically done within the BO and harmonic approximations, have suggested that one leading candidate for large, polyatomic molecule laser cooling, alkaline earth phenoxides, can most efficiently be laser-cooled via the third electronically excited C state. Here, we report the first detailed spectroscopic characterization of the C state in CaOPh and SrOPh. We find that nonadiabatic couplings between the A, B, and C states lead to substantial mixing, giving rise to vibronic states that enable additional decay pathways. Based on the intensity ratio of these extra decay channels, we estimate a non-adiabatic coupling strength of 0.1 cm-1. While this coupling strength is small, the large density of vibrational states available at photonic energy scales in a polyatomic molecule leads to significant mixing. Thus, this result is expected to be general for large molecules and implies that only the lowest electronic excited state should be considered when judging the suitability of a molecule for laser cooling.

physics.atom-ph↗

arXiv2024

Bottom-up approach to scalable growth of molecules capable of optical cycling

Gas-phase molecules capable of repeatable, narrow-band spontaneous photon scattering are prized for direct laser cooling and quantum state detection. Recently, large molecules incorporating phenyl rings have been shown to exhibit similar vibrational closure to the small molecules demonstrated so far, and it is not yet known if the high vibrational-mode density of even larger species will eventually compromise optical cycling. Here, we systematically increase the size of hydrocarbon ligands attached to single alkaline-earth-phenoxides from (-H) to -C$_{14}$H$_{19}$ while measuring the vibrational branching fractions of the optical transition. We find that varying the ligand size from 1 to more than 30 atoms does not systematically reduce the cycle closure, which remains around 90%. Theoretical extensions to larger diamondoids and bulk diamond surface suggest that alkaline earth phenoxides may maintain the desirable scattering behavior as the system size grows further, with no indication of an upper limit.

physics.chem-ph↗

arXiv2023

Extending the large molecule limit: The role of Fermi resonance in developing a quantum functional group

Polyatomic molecules equipped with optical cycling centers (OCCs), enabling continuous photon scattering during optical excitation, are exciting candidates for advancing quantum information science. However, as these molecules grow in size and complexity the interplay of complex vibronic couplings on optical cycling becomes a critical, but relatively unexplored consideration. Here, we present an extensive exploration of Fermi resonances in large OCC-containing molecules, surpassing the constraints of harmonic approximation. High-resolution dispersed laser-induced fluorescence and excitation spectroscopy reveal Fermi resonances in calcium and strontium phenoxides and their derivatives. This resonance manifests as vibrational coupling leading to intensity borrowing by combination bands near optically active harmonic bands. The resulting additional vibration-changing decays require more repumping lasers for effective optical cycling. To mitigate these effects, we explore altering vibrational energy level spacing through substitutions on the phenyl ring or changes in the OCC itself. While the complete elimination of vibrational coupling in complex molecules remains challenging, our findings underscore the potential for significant mitigation, opening new avenues for optimizing optical cycling in large polyatomic molecules.

physics.chem-ph↗

arXiv2023

Laser spectroscopy of aromatic molecules with optical cycling centers: strontium (I) phenoxides

We report the production and spectroscopic characterization of strontium (I) phenoxide ($\mathrm{SrOC}_6\mathrm{H}_5$, or SrOPh) and variants featuring electron-withdrawing groups designed to suppress vibrational excitation during spontaneous emission from the electronically excited state. Optical cycling closure of these species, which is the decoupling of vibrational state changes from spontaneous optical decay, is found by dispersed laser-induced fluorescence spectroscopy to be high, in accordance with theoretical predictions. A high-resolution, rotationally-resolved laser excitation spectrum is recorded for SrOPh, allowing the estimation of spectroscopic constants and identification of candidate optical cycling transitions for future work. The results confirm the promise of strontium phenoxides for laser cooling and quantum state detection at the single-molecule level.

physics.atom-ph↗

arXiv2022

Functionalizing Aromatic Compounds with Optical Cycling Centers

Molecular design principles provide guidelines for augmenting a molecule with a smaller group of atoms to realize a desired property or function. We demonstrate that these concepts can be used to create an optical cycling center that can be attached to a number of aromatic ligands, allowing the scattering of many photons from the resulting molecules without changing the molecular vibrational states. We provide further design principles that indicate the ability to expand this work. This represents a significant step towards a quantum functional group, which may serve as a generic qubit moiety that can be attached to a wide range of molecular structures and surfaces.

physics.atom-ph↗

arXiv2021

High-resolution laser-induced fluorescence spectroscopy of $^{28}$Si$^{16}$O$^+$ and $^{29}$Si$^{16}$O$^+$ in a cryogenic buffer-gas cell

The electronic, laser-induced fluorescence spectrum of the $B^2Σ^+\leftarrow X^2Σ^+$ transition in $^{28}$Si$^{16}$O$^+$ and $^{29}$Si$^{16}$O$^+$ has been recorded in a cryogenic buffer gas cell at $\approx$ 100 K. Molecular constants are extracted for both $^{28}$Si$^{16}$O$^+$ and $^{29}$Si$^{16}$O$^+$, including the Fermi contact hyperfine constant for both the $B$ and $X$ states of $^{29}$Si$^{16}$O$^+$, and used in a discussion of the suitability of SiO$^+$ in future quantum information experiments.

physics.chem-ph↗

arXiv2021

Interaction between vortex beams and diatomic molecules with rotation

The interaction between vortex beam (VB) and molecule has drawn much attention in recent years, but the lack of theoretical method somehow limits its further analysis, especially when the molecular rotational degree of freedom is involved and coupled with the molecular electronic states. To incorporate the molecular rotation into the theoretical study, in this paper, we describe the diatomic molecular states in Hund's coupling basis and express interaction Hamiltonian in form of spherical harmonics expansion, and then investigate the rotational transition of molecular states driven by VB. The theory clearly illustrates that each photon of VB may carry a total angular momentum of 0, $\hbar$, or 2$\hbar$, and therefore could drive O, P, Q, R and S branches of diatomic molecular rotational transitions with some specific selection rules. These results indicate that VB could provide new methods for preparing and measuring the diatomic molecular states.

physics.optics↗