arXiv subjects

Andrei Derevianko

Publications and source records attributed to Andrei Derevianko.

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

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

Ab initio calculations of $^{229}$Th band-to-band internal conversion rate in $^{229}$ThO$_2$

We present an ab initio calculation of the band-to-band internal-conversion rate of the $\hbarω_{\rm nuc} \approx 8.35$ eV isomeric transition in $^{229}$ThO$_2$. Because the nuclear transition energy exceeds the electronic band gap of ThO$_2$, the isomer can decay nonradiatively by resonantly promoting a valence electron into the conduction band. We formulate this process as a Brillouin-zone sum over vertical interband transitions weighted by local Th-centered hyperfine matrix elements, which are evaluated directly from all-electron full-potential linearized augmented-plane-wave Bloch spinors. A finite nuclear magnetization model is included to regularize the short-range hyperfine interaction and to account for the Bohr-Weisskopf effect. After applying scissor shifts to span the experimentally reported ThO$_2$ band gaps, we find calculated internal-conversion lifetimes in the range of $1-16~μ{\rm s}$. The lifetime increases strongly as the band gap approaches $ω_{\rm nuc}$ because the resonant interband phase space at the nuclear transition energy is reduced. For the larger reported ThO$_2$ gaps, the calculated lifetime is comparable to the measured conversion-electron Mössbauer lifetime [Nature 648, 300 (2025)]. Our analysis implies that choosing solid-state hosts with band-gap values slightly lower than $ω_{\rm nuc}$ can optimize solid-state nuclear clock performance with internal-conversion electron readout.

nucl-th↗

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

Tuning long-range interactions in Sr Rydberg atoms: the effect of series perturbations

We investigate the effect of series perturbation on the second-order dipole-dipole interactions between strontium atoms in the $5sns({^1}S_0)$ and $5snp({^1}P_1)$ Rydberg states as a means of engineering long-range interactions between atoms. The series perturbation in these atoms enables modifying the strength and the sign of the interaction by varying the principal quantum number $n$ of the Rydberg electron. We utilize experimentally available data to estimate the importance of perturber states, and find that van der Waals interaction between two strontium atoms in the $5snp({^1}P_1)$ states shows strong peaks outside the anticipated hydrogenic $n^{11}$ scaling. We identify this to be the result of the perturbation of $5snd({^1}D_2)$ intermediate states by the $4d^2({^1}D_2)$ and $4dn's({^1}D_2)$ states in the $n<20$ range. This demonstrates that divalent atoms offer a unique advantage for generating substantially stronger or weaker inter-atomic interactions than those that can be achieved using alkali metal atoms. This is due to the highly perturbed spectra of divalent atoms and other multivalent atoms that can persist up to high $n$. Such irregularities can be especially useful in engineering asymmetric Ry blockade requiring the simultaneous presence of both ``weak'' and ``strong'' interactions.

physics.atom-ph↗

arXiv2026

Suppression of differential light shifts in ground and metastable trapped-ion qubits

In the presence of a magnetic field, hyperfine clock qubits can acquire a vector differential light shift that can be tuned via polarization to suppress the total differential light shift of high-power, off-resonant laser light. We experimentally measure this "magic" polarization condition, suppressing differential light shifts in both the ${}^2\mathrm{S}_{1/2}$ ground and ${}^2\mathrm{F}_{7/2}^o$ metastable clock qubits of $^{171}\mathrm{Yb}^+$. We present calculations of the minimum bias magnetic fields required to suppress differential light shifts in the ground state clock qubits of commonly trapped ion species, finding that they are below the strengths of fields already typically present in experiments. We further present methods for metastable clock-qubit control in $^{171}\mathrm{Yb}^+$, demonstrating a state preparation and measurement infidelity of $2.9^{+3.0}_{-1.5}\times10^{-4}$ ($-35 \pm 4 \, \mathrm{dB}$).

physics.atom-ph↗

arXiv2026

GPS constellation search for exotic physics messengers coincident with the binary neutron star merger GW170817

The Global Positioning System (GPS) includes a continuously operating, planet-scale network of atomic clocks that, beyond navigation and time dissemination, enables precision tests of fundamental physics. Here we use GPS carrier phase archival data to perform a retrospective search for exotic low-mass fields (ELFs) that might be emitted by the binary neutron-star merger GW170817, complementing gravitational wave and electromagnetic modalitiesnin multi-messenger astronomy. Such ultra-relativistic fields would imprint a dispersive, anti-chirp signature in clock-frequency time series, delayed with respect to the LIGO-Virgo gravitational wave detection. We construct network-median pseudo-frequency data from eighteen Rb satellite clocks referenced to a terrestrial hydrogen maser and conduct a template-bank search spanning ELF pulse duration, arrival delay, and characteristic frequency. No statistically significant signal is observed after accounting for noise statistics and template-bank trials. We derive 95\% confidence-level lower bounds on the interaction energy scale $Λ_α$ of quadratic couplings driving variations in electromagnetic fine-structure constant. These limits improve upon existing astrophysical and gravity-test constraints across the ELF-energy range $\approx10^{-18}$--$10^{-14}\,\mathrm{eV}$. This demonstrates that mature global satellite-clock networks provide an observational capability for retrospective, multi-messenger searches for new physics using decades of archival timing data.

astro-ph.IM↗

arXiv2026

Electric field gradient in accurate quantum chemical calculations

The electric field gradients (EFGs) at the (non-spherical) nucleus contribute to atomic and molecular hyperfine structure and govern Nuclear Quadrupole Resonance (NQR) and Mössbauer spectra. EFGs provide a highly sensitive probe of local bonding, symmetry, and crystal defect geometry and electronic structure. The EFGs can be obtained from electronic structure calculations and can also be extracted from spectroscopic measurements, thus linking electronic structure theory and spectroscopic observables. In this work, we present a methodological study of EFGs for a range of molecules and crystalline materials, using both periodic boundary conditions and embedded cluster models, and compare the results with reported experimental data. We analyze the sensitivity of EFG values to details of the calculations, such as the selection of the model Hamiltonians, basis sets, and the geometries of molecules and crystals. We also address persistent differences in EFG sign conventions and tensor definitions employed in the literature and in widely used quantum chemistry codes. While the EFG sign does not affect zero B-field NQR spectra, they can become critical in Mossbauer spectroscopy or when the quadrupolar interactions are combined with other interactions of the nucleus with the environment. Together, our systematic study results provide practical guidelines for computing, interpreting, and exploiting EFGs as quantitative descriptors of electronic structure and chemical environment.

physics.chem-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

$^{229}$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↗

arXiv2025

Tutorial on running median subtraction filter with application to searches for exotic field transients in multi-messenger astronomy

Running Median Subtraction Filter (RMSF) is a robust statistical tool for removing slowly varying baselines in data streams containing transients (short-duration signals) of interest. In this work, we explore the RMSF performance and properties using simulated time series and analytical methods. We study the RMSF fidelity in preserving the signal of interest in the data using (i) a Gaussian pulse and (ii) a transient oscillatory signal. Such signals may be generated by hypothetical exotic low-mass fields (ELFs) associated with intense astrophysical events like binary black hole or neutron star mergers. We consider and assess RMSF as a candidate method to extract transient ELF signals. RMSF operates by sliding a window across the data and subtracting the median value within each window from the data points. With a suitable choice of running window size, RMSF effectively filters out baseline variations without compromising the integrity of transients. The RMSF window width is a critical parameter: it must be wide enough to encompass a short transient but narrow enough to remove the slowly varying baseline. We show that the RMSF removes the mean of a normally distributed white noise while preserving its variance and higher order moments in the limit of large windows. In addition, RMSF does not color the white noise stream, i.e., it does not induce any significant correlation in the filtered data. Ideally, a filter would preserve both the signal of interest and the statistical characteristics of the stochastic component of the data, while removing the background clutter and outliers. We find the RMSF to satisfy these practical criteria for data pre-processing. While we rigorously prove several RMSF properties, the paper is organized as a tutorial with multiple illustrations of RMSF applications.

astro-ph.IM↗

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

$^{229}\mathrm{ThF}_4$ 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↗

arXiv2024

Laser excitation of the $^{229}$Th nuclear isomeric transition in a solid-state host

LiSrAlF$_6$ crystals doped with $^{229}$Th are used in a laser-based search for the nuclear isomeric transition. Two spectroscopic features near the nuclear transition energy are observed. The first is a broad excitation feature that produces red-shifted fluorescence that decays with a timescale of a few seconds. The second is a narrow, laser-linewidth-limited spectral feature at $148.38219(4)_{\textrm{stat}}(20)_{\textrm{sys}}$ nm ($2020407.3(5)_{\textrm{stat}}(30)_{\textrm{sys}}$ GHz) that decays with a lifetime of $568(13)_{\textrm{stat}}(20)_{\textrm{sys}}$ s. This feature is assigned to the excitation of the $^{229}$Th nuclear isomeric state, whose energy is found to be $8.355733(2)_{\textrm{stat}}(10)_{\textrm{sys}}$ eV in $^{229}$Th:\thor:LiSrAlF$_6$.

physics.atom-ph↗

arXiv2024

Feasibility of extracting the proton weak charge from quantum-control measurements of atomic parity violation on the $2s-3s$ or $2s-4s$ transition in hydrogen

We explore the feasibility of extracting electroweak observables from a measurement of atomic parity violation in hydrogen. Our proposed quantum-control scheme focuses on the $2s-3s$ or $2s-4s$ transitions in hydrogen. This work is motivated by the recently observed anomaly in the W-boson mass, which may substantially modify the Standard Model value of the proton weak charge. We also study the accuracy of the previously employed approximations in computing parity-violating effects in hydrogen.

physics.atom-ph↗

arXiv2023

Multi-messenger astronomy in the new physics modality with GPS constellation

We explore a novel, exotic physics, modality in multi-messenger astronomy. We are interested in exotic fields emitted by the mergers and their direct detection with a network of atomic clocks. We specifically focus on the rubidium clocks onboard satellites of the Global Positioning System. Bursts of exotic fields may be produced during the coalescence of black hole singularities, releasing quantum gravity messengers. To be detectable such fields must be ultralight and ultra-relativistic and we refer to them as exotic low-mass fields (ELFs). Since such fields possess non-zero mass, the ELF bursts lag behind the gravitational waves emitted by the very same merger. Then the gravitational wave observatories provide a detection trigger for the atomic clock networks searching for the feeble ELF signals. ELFs would imprint an anti-chirp transient across the sensor network. ELFs can be detectable by atomic clocks if they cause variations in fundamental constants. We report our progress in the development of techniques to search for ELF bursts with clocks onboard GPS satellites. We focus on the binary neutron star merger GW170817 of August 17, 2017. We find an intriguing excess in the clock noise post LIGO gravitational wave trigger. Potentially the excess noise could be explained away by the increased solar electron flux post LIGO trigger.

astro-ph.IM↗

arXiv2023

Eliminating qubit type cross-talk in the $\textit{omg}$ protocol

The $\textit{omg}$ protocol is a promising paradigm that uses multiple, application-specific qubit subspaces within the Hilbert space of each single atom during quantum information processing. A key assumption for $\textit{omg}$ operation is that a subspace can be accessed independently without deleterious effects on information stored in other subspaces. We find that intensity noise during laser-based quantum gates in one subspace can cause decoherence in other subspaces, potentially complicating $\textit{omg}$ operation. We show, however, that a magnetic-field-induced vector light shift can be used to eliminate this source of decoherence. As this technique requires simply choosing a certain, magnetic field dependent, polarization for the gate lasers it is straightforward to implement and potentially helpful for $\textit{omg}$ based quantum technology.

quant-ph↗