arXiv subjects

Eric R. Hudson

Publications and source records attributed to Eric R. Hudson.

At least 19 recordsLinked to original sources

arXiv2026

Investigation into thorium sulfate as a spinless crystal for a high-performance solid-state $^{229}Th$ nuclear clock

The $^{229}Th$ isotope has a laser-accessible nuclear transition allowing the construction of a solid-state nuclear clock. Solid-state $^{229}Th$ nuclear clock development has focused on $^{229}Th$-doped $CaF_2$ and other metal fluorides as the solid material. However, the accuracy of any fluoride-based clock will be reduced by nuclear magnetic dipole coupling to $^{19}F$ and by inhomogeneities in the thorium defect environments. Here we explore thorium sulfate, $Th(SO_4)_2$, as a solution to both problems. Strong bonding and charge delocalization in the $SO_4^{2-}$ anion may give $Th(SO_4)_2$ the wide band gap needed for a good clock. In this work we synthesize $Th(SO_4)_2$ and probe it as a nuclear clock material spectroscopically, finding that it is opaque to the 148 nm radiation that excites the $^{229}Th$ nucleus. Theoretical analysis of the optical spectra shows that charge transfer excitons are responsible for the absorption. We give guidelines for future material development and assess the prospects for $Th(SO_4)_2$ as a clock material.

cond-mat.mtrl-sci↗

arXiv2026

A broadband, individually addressing two- and three-dimensional photonic integrated circuit for trapped-ion qubit control

Trapped ions provide a high-fidelity platform for quantum information processing, yet delivery of multiple, distinct wavelengths across large networks of interaction zones remains a bottleneck. Conventional free-space light delivery lacks scalability, while on-chip grating couplers suffer from narrow operational bandwidth that increases circuit footprint and optical interfacing complexity. Here we show a broadband photonic integrated circuit capable of addressing individual ions. The circuit combines a planar waveguide lens with a micromirror fabricated using two-photon polymerization at wafer scale. This implementation can address three individual ions from $λ$ = 405 - 880 nm with -27 dB average intensity crosstalk at $5\,μ\mathrm{m}$ pitch. We trap $^{40}\mathrm{Ca}^{+}$ and $^{138}\mathrm{Ba}^{+}$ ions above such devices, characterize optical crosstalk with barium ions, and demonstrate individual repumping of calcium ions. This monolithic photonic architecture brings broadband addressing in an on-chip modality to trapped-ion technology. More generally, integrating additive manufacturing into quantum devices is poised to unlock expanded design space for implementing novel quantum architectures.

quant-ph↗

arXiv2026

Defect assignment of the clock site in $^{229}\text{Th:CaF}_2$

The performance of solid-state $^{229}\text{Th}$ nuclear clocks depends sensitively on the microscopic environment of the thorium nucleus in the host crystal. Here we reassess the dominant quadrupole-split thorium site in $^{229}\text{Th:CaF}_2$, which has been assigned to a thorium dimer in recent spectroscopic work. Thermodynamic estimates, density functional theory calculations, and electric-field-gradient comparisons instead favor an isolated $\text{Th}^{4+}$ substitution on a $\text{Ca}^{2+}$ site charge-compensated by two nearby fluorine interstitials in a relaxed $90^\circ$ motif. The same calculation identifies a higher-energy mixed-shell interstitial motif as a plausible minor site. The clock-active quadrupole-split site is therefore controlled by local fluoride compensation rather than unavoidable thorium aggregation. This defect assignment also has implications for achievable linewidths and provides a microscopic basis for reducing broadening in solid-state nuclear clocks.

physics.atom-ph↗

arXiv2026

Colloquium: Nuclear clocks

The Th-229 nuclear isomeric state has the lowest energy of all known nuclear excited states, placing it within the reach of current table-top laser technology. This extraordinary property has made this nuclear isomer an attractive candidate for a nuclear optical clock of incredibly high precision and accuracy, both as isolated trapped Th-229 ions and embedded into solid-state platforms. Activity around Th-229 has surged in recent years, driven by breakthroughs in its direct laser excitation. The underlying nuclear physics that gives rise to this unique isomer will be elucidated, as well as the nearly half-century of efforts that led to its direct excitation. The design and systematics of a Th-229 nuclear clock will be discussed, both in ion traps and in the solid-state. These systematics, such as frequency shifts and quenching channels, can be leveraged both to probe the local chemical environment, and as a control knob during clock operation. Finally, the nuclear clock's high sensitivity to the variations of fundamental constants will be discussed.

physics.atom-ph↗

arXiv2026

Nonlinear-enhanced wideband sensing via subharmonic excitation of a quantum harmonic oscillator

A key advantage of quantum metrology is the ability to surpass the standard quantum limit~(SQL) for measurement precision through the use of non-classical states. However, there is typically little to no improvement in precision with the use of non-classical states for measurements whose duration exceeds the decoherence time of the underlying quantum states. Measurements aimed at the ultimate possible precision are thus performed almost exclusively with classical states and, therefore, are constrained by the SQL. Here, we demonstrate that by using the phenomenon of subharmonic excitation, in combination with a recently demonstrated technique of Raman excitation of a harmonic oscillator, the frequency of an electric field can be measured at a resolution below the SQL of the corresponding linear generator. With this method we measure a radio-frequency electrical signal with a fractional frequency uncertainty of 0.56~Hz/80~MHz=7e-9 , which to our knowledge is the most precise frequency measurement of a radio-frequency electrical signal using a quantum harmonic oscillator. Because the input states can be classical, the coherence time is not degraded by the enhanced decoherence typically associated with nonclassical states, thereby improving the ultimate achievable precision. While we demonstrate this technique using motional Raman subharmonic excitation of a single \ca\ ion through engineered Floquet states, this technique is expected to be extendable to other platforms, such as NV centers, solid-state qubits, and neutral atoms, where it can provide metrological gain for sensing across the radio frequency, microwave, and optical domains.

physics.atom-ph↗

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↗

arXiv2025

Barium Autoionization for Efficient Ion Trap Loading

We report a theoretical and experimental investigation of autoionizing resonances from the $5d6p\,{}^3\mathrm{D}_1^o$ manifold in neutral barium for efficient loading of ion traps. Our calculations predict large resonant cross sections for many narrow autoionizing resonances, but we find experimentally that for most of these, Doppler broadening during trap loading depresses the effective cross sections that can be achieved in practice. We identify and demonstrate a strong, broad transition at $531\,\mathrm{nm}$, and show that it furnishes an order-of-magnitude increase in trap loading efficiency compared to other demonstrated resonances.

physics.atom-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↗

arXiv2025

Host-dependent frequency offsets in $^{229}$Th nuclear clockwork

Recent advances in laser excitation of the low-energy nuclear isomer transition in $^{229}$Th have opened avenues for developing nuclear clocks, a novel quantum technology with exceptional performance and sensitivity to exotic physics. Here we explore the host-dependence of the nuclear clock frequency, focusing on the isomer shift induced by the difference in the nuclear charge distribution between the ground and excited nuclear states. We combine relativistic many-body methods of atomic structure with periodic density functional theory to evaluate the isomer shifts in solid-state hosts. We elucidate the critical importance of the ``relaxation'' effect in evaluating the isomer shifts. Our analysis predicts nuclear clock frequencies for various solid-state and trapped ion platforms: $ ω_\text{clk}(\text{solid state}) = 2,020,407,384(40) \, \text{MHz}$, $ω_\text{clk}(^{229}\text{Th}^{4+}) = 2,020,407,648(70) \, \text{MHz}$, and $ ω_\text{clk}(^{229}\text{Th}^{3+}) = 2,020,407,114(70) \, \text{MHz}$. We also determine the nuclear transition energy for the bare $^{229}$Th nucleus to be $ω_\text{nuc} = 8.272(22) \,\text{eV}$. Our calculated valence-band isomer shifts for different host materials constrain the nuclear transition frequencies to an 80 MHz-wide frequency window, aiding experimental searches for the $^{229}$Th nuclear transition in novel materials.

physics.atom-ph↗

arXiv2025

A cryogenic Paul trap for probing the nuclear isomeric excited state $^{229\text{m}}$Th$^{3+}$

While laser excitation of the nuclear isomeric transition in $^{229}$Th has been recently achieved for thorium atoms embedded in large-bandgap crystals, laser excitation and characterization of the nuclear transition in trapped $^{229}$Th$^{3+}$ ions has not yet been accomplished. To address these experiments, a cryogenic Paul trap setup has been designed, built, and commissioned at LMU Munich. Here, we present the specifications of the new experimental platform and demonstrate its successful operation, showing the extraction, subsequent ion-guiding, mass-purification, and trapping of $^{229}$Th$^{3+}$ and $^{229\text{m}}$Th$^{3+}$ ions from a newly designed buffer-gas stopping cell as well as of $^{88}$Sr$^{+}$ ions from laser ablation of a solid target. Further, we show sympathetic laser cooling of $^{229\text{(m)}}$Th$^{3+}$ by Doppler-cooled $^{88}$Sr$^{+}$ ions and the formation of mixed-species Coulomb crystals.

physics.atom-ph↗

arXiv2025

Super-resolution of two Closely-spaced Electromagnetic Fields via Walsh-Modulated Dynamical Decoupling Spectroscopy

Due to quantum fluctuations, non-orthogonal quantum states cannot be distinguished with complete certainty, making their underlying physical parameters difficult to resolve. Traditionally, it has been believed that the linewidth of a system behaves like these quantum fluctuations to set the ultimate limit on frequency resolution as two oscillating electromagnetic fields are applied. Consequently, the measurement time required to resolve a frequency difference $Δω$ was assumed to diverge as $Δω\rightarrow 0$. Here, we show that linewidth does not play a defining role in resolving two closely spaced frequencies. Instead, the ultimate limit is set by parameter-independent quantum fluctuations, such as shot noise in our case. We propose and experimentally demonstrate the first general broadband protocol for super-resolution spectroscopy. Specifically, our protocol uses a Walsh-modulated dynamical decoupling (WMDD) sequence to encode $Δω$ between two unknown tones into a quantum state. This leverages phase information to suppress parameter-independent shot noise, thereby enhancing the signal-to-noise ratio and enabling super-resolution spectroscopy. With this approach, we resolve two randomly chosen oscillating electric fields of order 100 MHz separated by 5 Hz, with a measured frequency difference of 5.0(1.6) Hz using a measurement time per run of just 1 ms, representing an improvement of 200 beyond the traditional resolution limit. As such, our technique accelerates data acquisition by more than $10^5$ magnitude compared to conventional methods. Crucially, as our protocol is rooted in the motional Raman (quantum vector signal analyzer) framework, it is effective across an arbitrary frequency range and thus promises to enhance broadband sensing of electromagnetic fields and improve spectral efficiency of next-generation communication systems.

physics.atom-ph↗

arXiv2025

$^{229}$Th Nuclear Spectroscopy in an Opaque Material: Laser-Based Conversion Electron Mössbauer Spectroscopy of $^{229}$ThO$_2$

Here, we report the first demonstration of laser-induced conversion electron Mössbauer spectroscopy of the $^{229}$Th nuclear isomeric state, which provides the ability to probe the nuclear transition in a material that is opaque to light resonant with the nuclear transition. Specifically, we excite the nuclear transition in a thin ThO$_2$ sample whose band gap ($\sim$ 6 eV) is considerably smaller than the nuclear isomeric state energy (8.4 eV). As a result, the excited nucleus can quickly decay by internal conversion, resulting in the ejection of electrons from the surface. By collecting these conversion electrons, nuclear spectroscopy can be recorded. Unlike fluorescence spectroscopy, this technique is compatible with materials whose work function is less than the nuclear transition energy, opening a wider class of systems to study. Further, because ThO$_2$ can be made from spinless isotopes and the internal conversion decay process reduces the isomeric state lifetime to only $\sim$10 $μ$s, allowing $\sim$10$^8$ relative reduction in clock interrogation time, a conversion-electron-based nuclear clock could lead to a $\sim$10$^4$ reduction in clock instability.

physics.atom-ph↗

arXiv2025

Theory of internal conversion of the thorium-229 nuclear isomer in solid-state hosts

Laser excitation of thorium-229 nuclei in doped wide bandgap crystals has been demonstrated recently, opening the possibility of developing ultrastable solid-state clocks and sensitive searches for new physics. We develop a quantitative theory of the internal conversion of isomeric thorium-229 in solid-state hosts. The internal conversion of the isomer proceeds by resonantly exciting a valence band electron to a defect state, accompanied by multi-phonon emission. We demonstrate that, if the process is energetically allowed, it generally quenches the isomer on timescales much faster than the isomer's radiative lifetime, despite thorium being in the +4 charge state in the valence band.

physics.atom-ph↗

arXiv2024

Photo-Induced Quenching of the 229Th Isomer in a Solid-State Host

The population dynamics of the 229Th isomeric state is studied in a solid-state host under laser illumination. A photoquenching process is observed, where off-resonant vacuum-ultraviolet (VUV) radiation leads to relaxation of the isomeric state. The cross-section for this photoquenching process is measured and a model for the decay process, where photoexcitation of electronic states within the material bandgap opens an internal conversion decay channel, is presented and appears to reproduce the measured cross-section.

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↗

arXiv2024

Quantum Vector Signal Analyzer: Wideband Electric Field Sensing via Motional Raman Transitions

Ultrasensitive detection of the frequency, phase, and amplitude of radio frequency (RF) electric fields is central to a variety of important applications, including radio communication, cosmology, dark matter searches, and high-fidelity qubit control. Quantum harmonic oscillator (QHO) systems, especially trapped ions, have been used with several quantum sensing techniques to achieve electric field sensing with state-of-the-art sensitivity and nanometer spatial resolution. However, these systems are limited to a narrow frequency range centered around either the motional frequency of the trapped ion oscillator or the frequency of an optical transition in the ion; often these techniques are not sensitive to the RF phase. Here, we propose and demonstrate a procedure that unlocks the extreme sensitivity of a QHO to allow high precision wideband detection of the frequency, phase, and amplitude of an unknown electric field. Specifically, we use motional Raman transitions in a single trapped ion, cooled near its motional ground state to realize state of the art sensitivities to frequency, phase, and amplitude, and show the technique works over a frequency range that is >800x larger than previous techniques. Further, this technique is shown to be compatible with both quantum amplification via squeezing and measurement in the Fock basis, allowing performance 3.4(20) dB below the standard quantum limit and the potential for several orders of magnitude improvement in sensitivity with moderate upgrades. In addition to providing an attractive platform for quantum sensing of small fields, this technique allows in situ calibration of qubit control lines in QHO systems, as well as transduction of external, non-resonant drives into oscillator excitation. Additionally, this approach can be extended to other QHO systems, such as a superconducting qubit-resonator system.

physics.atom-ph↗

arXiv2024

$^{229}\mathrm{ThF}_4$ thin films for solid-state nuclear clocks

After nearly fifty years of searching, the vacuum ultraviolet $^{229}$Th nuclear isomeric transition has recently been directly laser excited [1,2] and measured with high spectroscopic precision [3]. Nuclear clocks based on this transition are expected to be more robust [4,5] than and may outperform [6,7] current optical atomic clocks. They also promise sensitive tests for new physics beyond the standard model [5,8,9]. In light of these important advances and applications, a dramatic increase in the need for $^{229}$Th spectroscopy targets in a variety of platforms is anticipated. However, the growth and handling of high-concentration $^{229}$Th-doped crystals [5] used in previous measurements [1-3,10] are challenging due to the scarcity and radioactivity of the $^{229}$Th material. Here, we demonstrate a potentially scalable solution to these problems by demonstrating laser excitation of the nuclear transition in $^{229}$ThF$_4$ thin films grown with a physical vapor deposition process, consuming only micrograms of $^{229}$Th material. The $^{229}$ThF$_4$ thin films are intrinsically compatible with photonics platforms and nanofabrication tools for integration with laser sources and detectors, paving the way for an integrated and field-deployable solid-state nuclear clock with radioactivity up to three orders of magnitude smaller than typical \thor-doped crystals [1-3,10]. The high nuclear emitter density in $^{229}$ThF$_4$ also potentially enables quantum optics studies in a new regime. Finally, we describe the operation and present the estimation of the performance of a nuclear clock based on a defect-free ThF$_4$ crystal.

physics.atom-ph↗