arXiv subjects

S. Schiller

Publications and source records attributed to S. Schiller.

At least 19 recordsLinked to original sources

arXiv2025

Determination of a set of fundamental constants from molecular hydrogen ion spectroscopy: a modeling study

The rovibrational transition frequencies of molecular hydrogen ions (MHI) can be accurately computed using ab initio nonrelativistic quantum electrodynamics. A subset of the fundamental constants are required input. We analyze how, once upcoming ultra-high-accuracy spectroscopy data has been obtained, that subset of constants can be determined with greater accuracy. Our analysis shows that under realistic assumptions the uncertainties of the mass ratios of proton, deuteron and triton relative to the electron, and of the triton charge radius can be reduced more than onehundred-fold compared to today (CODATA 2022). Furthermore, the Rydberg constant, as well as the proton and deuteron charge radii can be determined with uncertainties similar to those of today, but solely using data from electronic systems. The implications are discussed.

physics.atom-ph↗

arXiv2022

Solution of the two-center Dirac equation with 20 digits precision using the finite-element technique

We present a precise fully relativistic numerical solution of the two-center Coulomb problem. The special case of unit nuclear charges is relevant for the accurate description of the ${\rm H}_2^+$ molecular ion and its isotopologues, systems that are an active experimental topic. The computation utilizes the 2-spinor minmax approach and the finite-element method. The computed total energies have estimated fractional uncertainties of a few times $10^{-20}$ for unit charges and a bond length of 2 atomic units. The fractional uncertainty of the purely relativistic contribution is $1\times10^{-17}$. The result is relevant for future precision experiments, whereas at present the uncertainties arising from the quantum electrodynamic treatment of the rovibrational transition frequencies. are dominant.

quant-ph↗

arXiv2021

Search for oscillations of fundamental constants using molecular spectroscopy

A possible implication of an ultralight dark matter (UDM) field interacting wibeginth the Standard Model (SM) degrees of freedom is oscillations of fundamental constants. Here, we establish direct experimental bounds on the coupling of an oscillating UDM field to the up, down, and strange quarks and to the gluons, for oscillation frequencies between 10 Hz and 10^8 Hz. We employ spectroscopic experiments that take advantage of the dependence of molecular transition frequencies on the nuclear masses. Our results apply to previously unexplored frequency bands, and improve on existing bounds at frequencies > 5 MHz. We identify a sector of UDM - SM coupling space where the bounds from Equivalence Principle tests may be challenged by next-generation experiments of the present kind.

hep-ph↗

arXiv2021

Proton-electron mass ratio by high-resolution optical spectroscopy of ion ensembles in the resolved-carrier regime

Optical spectroscopy in the gas phase is a key tool to elucidate the structure of atoms and molecules and of their interaction with external fields. The line resolution is usually limited by a combination of first-order Doppler broadening due to particle thermal motion and of a short transit time through the excitation beam. For trapped particles, suitable laser cooling techniques can lead to strong confinement (Lamb-Dicke regime, LDR) and thus to optical spectroscopy free of these effects. For non-laser coolable spectroscopy ions, this has so far only been achieved when trapping one or two atomic ions, together with a single laser-coolable atomic ion [1,2]. Here we show that one-photon optical spectroscopy free of Doppler and transit broadening can also be obtained with more easily prepared ensembles of ions, if performed with mid-infrared radiation. We demonstrate the method on molecular ions. We trap approximately 100 molecular hydrogen ions (HD$^{+}$) within a Coulomb cluster of a few thousand laser-cooled atomic ions and perform laser spectroscopy of the fundamental vibrational transition. Transition frequencies were determined with lowest uncertainty of 3.3$\times$10$^{-12}$ fractionally. As an application, we determine the proton-electron mass ratio by matching a precise ab initio calculation with the measured vibrational frequency.

quant-ph↗

arXiv2020

Hyperfine structure and electric quadrupole transitions in the deuterium molecular ion

Molecular hydrogen ions are of metrological relevance due to the possibility of precise theoretical evaluation of their spectrum and of external-field-induced shifts. In homonuclear molecular ions the electric dipole $E1$ transitions are strongly suppressed, and of primary laser spectroscopy interest is the electric quadrupole ($E2$) transition spectrum. In continuation of previous work on the H$_2^+$ ion, we report here the results of the calculations of the hyperfine structure of the laser-induced electric quadrupole transitions between a large set of ro-vibrational states of D$_2^+$; the inaccuracies of previous evaluations have been corrected. The effects of the laser polarization are studied in detail. We show that the electric quadrupole moment of the deuteron can in principle be determined with low fractional uncertainty $(\simeq1\times10^{-4})$ by comparing the results presented here with future data from precision spectroscopy of D$_2^+$.

physics.atom-ph↗

arXiv2020

Time keeping and searching for new physics using metastable states of Cu, Ag and Au

We study the prospects of using the electric quadrupole transitions from the ground states of Cu, Ag and Au to the metastable state $^2{\rm D}_{5/2}$ as clock transitions in optical lattice clocks. We calculate lifetimes, transition rates, systematic shifts, and demonstrate that the fractional uncertainty of the clocks can be similar to what is achieved in the best current optical clocks. The use of these proposed clocks for the search of new physics, such as time variation of the fine structure constant, search for low-mass scalar dark matter, violation of Local Position Invariance and violation of Lorenz Invariance is discussed.

physics.atom-ph↗

arXiv2019

SAGE: A Proposal for a Space Atomic Gravity Explorer

The proposed mission "Space Atomic Gravity Explorer" (SAGE) has the scientific objective to investigate gravitational waves, dark matter, and other fundamental aspects of gravity as well as the connection between gravitational physics and quantum physics using new quantum sensors, namely, optical atomic clocks and atom interferometers based on ultracold strontium atoms.

astro-ph.IM↗

arXiv2018

Canceling spin-dependent contributions and systematic shifts in precision spectroscopy of the molecular hydrogen ions

We consider the application of a basic principle of quantum theory, the tracelessness of a certain class of hamiltonians, to the precision spectroscopy of the molecular hydrogen ions. We show that it is possible to obtain the spin-averaged transition frequencies between states from a simple weighted sum of experimentally accessible spin-dependent transition frequencies. We discuss the cases ${\rm H}_{2}^{+}$ and ${\rm HD}^{+}$, which are distinct in the multipole character of their rovibrational transitions. Inclusion of additional frequencies permits canceling also the electric quadrupole shift, the Zeeman shift and partially the Stark shift. In this context, we find that measuring electric quadrupole transitions in ${\rm HD}^{+}$ is advantageous. The required experimental effort appears reasonable.

physics.atom-ph↗

arXiv2018

Additional clock transitions in neutral ytterbium bring new possibilities for testing physics beyond the Standard Model

We study the prospects of using transitions from the ytterbium ground state to metastable states $^3{\rm P}^{\rm o}_2$ at $E=19\,710.388~$cm$^{-1}$ and $4f^{13}5d6s^2\,(J=2)$ at $E=23\,188.518~$cm$^{-1}$ as clock transitions in an optical lattice clock. Having more than one clock transition in Yb could benefit the search for new physics beyond the Standard Model via studying the non-linearity of King's plot or the time-variation of the ratio of the frequencies of two clock transitions. We calculate the lifetime of the states, relevant transition amplitudes, systematic shifts, and the sensitivities of the clock transitions to a variation of the fine structure constant and to the gravitational potential. We find that both transitions can probably support ultra-high accuracy, similar to what is already achieved for the $^1$S$_0$ - $^3$P$^{\rm o}_0$ clock transition.

physics.atom-ph↗

arXiv2016

Resonator with ultra-high length stability as a probe for Equivalence-Principle-violating physics

In order to investigate the long-term dimensional stability of matter, we have operated an optical resonator fabricated from crystalline silicon at 1.5$\,$K continuously for over one year and repeatedly compared its resonance frequency $f_{res}$ with the frequency of a GPS-monitored hydrogen maser. After allowing for an initial settling time, over a 163-day interval we found a mean fractional drift magnitude $|f_{res}^{-1}df_{res}/dt|<1.4\times10^{-20}$/s. The resonator frequency is determined by the physical length and the speed of light, and we measure it with respect to the atomic unit of time. Thus, the bound rules out, to first order, a hypothetical differential effect of the universe's expansion on rulers and atomic clocks. We also constrain a hypothetical violation of the principle of Local Position Invariance for resonator-based clocks and derive bounds for the strength of space-time fluctuations.

gr-qc↗

arXiv2016

Development of a strontium optical lattice clock for the SOC mission on the ISS

The ESA mission "Space Optical Clock" project aims at operating an optical lattice clock on the ISS in approximately 2023. The scientific goals of the mission are to perform tests of fundamental physics, to enable space-assisted relativistic geodesy and to intercompare optical clocks on the ground using microwave and optical links. The performance goal of the space clock is less than $1 \times 10^{-17}$ uncertainty and $1 \times 10^{-15} τ^{-1/2}$ instability. Within an EU-FP7-funded project, a strontium optical lattice clock demonstrator has been developed. Goal performances are instability below $1 \times 10^{-15} τ^{-1/2}$ and fractional inaccuracy $5 \times 10^{-17}$. For the design of the clock, techniques and approaches suitable for later space application are used, such as modular design, diode lasers, low power consumption subunits, and compact dimensions. The Sr clock apparatus is fully operational, and the clock transition in $^{88}$Sr was observed with linewidth as small as 9 Hz.

physics.atom-ph↗

arXiv2015

Development of a strontium optical lattice clock for the SOC mission on the ISS

Ultra-precise optical clocks in space will allow new studies in fundamental physics and astronomy. Within an European Space Agency (ESA) program, the Space Optical Clocks (SOC) project aims to install and to operate an optical lattice clock on the International Space Station (ISS) towards the end of this decade. It would be a natural follow-on to the ACES mission, improving its performance by at least one order of magnitude. The payload is planned to include an optical lattice clock, as well as a frequency comb, a microwave link, and an optical link for comparisons of the ISS clock with ground clocks located in several countries and continents. Within the EU-FP7-SPACE-2010-1 project no. 263500, during the years 2011-2015 a compact, modular and robust strontium lattice optical clock demonstrator has been developed. Goal performance is a fractional frequency instability below 1x10^{-15}, tau^{-1/2} and a fractional inaccuracy below 5x10^{-17}. Here we describe the current status of the apparatus' development, including the laser subsystems. Robust preparation of cold {88}^Sr atoms in a second stage magneto-optical trap (MOT) is achieved.

physics.atom-ph↗

arXiv2012

The Space Optical Clocks Project: Development of high-performance transportable and breadboard optical clocks and advanced subsystems

The use of ultra-precise optical clocks in space ("master clocks") will allow for a range of new applications in the fields of fundamental physics (tests of Einstein's theory of General Relativity, time and frequency metrology by means of the comparison of distant terrestrial clocks), geophysics (mapping of the gravitational potential of Earth), and astronomy (providing local oscillators for radio ranging and interferometry in space). Within the ELIPS-3 program of ESA, the "Space Optical Clocks" (SOC) project aims to install and to operate an optical lattice clock on the ISS towards the end of this decade, as a natural follow-on to the ACES mission, improving its performance by at least one order of magnitude. The payload is planned to include an optical lattice clock, as well as a frequency comb, a microwave link, and an optical link for comparisons of the ISS clock with ground clocks located in several countries and continents. Undertaking a necessary step towards optical clocks in space, the EU-FP7-SPACE-2010-1 project no. 263500 (SOC2) (2011-2015) aims at two "engineering confidence", accurate transportable lattice optical clock demonstrators having relative frequency instability below 1\times10^-15 at 1 s integration time and relative inaccuracy below 5\times10^-17. This goal performance is about 2 and 1 orders better in instability and inaccuracy, respectively, than today's best transportable clocks. The devices will be based on trapped neutral ytterbium and strontium atoms. One device will be a breadboard. The two systems will be validated in laboratory environments and their performance will be established by comparison with laboratory optical clocks and primary frequency standards. In this paper we present the project and the results achieved during the first year.

quant-ph↗

arXiv2012

Addressing and manipulation of individual hyperfine states in cold trapped molecular ions and application to HD^{+} frequency metrology

Advanced techniques for manipulation of internal states, standard in atomic physics, are demonstrated for a charged molecular species for the first time. We address individual hyperfine states of ro-vibrational levels of a diatomic ion by optical excitation of individual hyperfine transitions, and achieve controlled transfer of population into a selected hyperfine state. We use molecular hydrogen ions (HD^{+}) as a model system and employ a novel frequency-comb-based, continuous-wave 5 \mum laser spectrometer. The achieved spectral resolution is the highest obtained so far in the optical domain on a molecular ion species. As a consequence, we are also able to perform the most precise test yet of the ab-initio theory of a molecule.

physics.atom-ph↗

arXiv2012

Observation of a rotational transition in trapped and sympathetically cooled molecular ions

We demonstrate rotational excitation of molecular ions that are sympathetically cooled by laser-cooled atomic ions to a temperature as low as ca. 10 mK. The molecular hydrogen ions HD+ and the fundamental rotational transition $(v=0,\, N=0)\rightarrow(v'=0,\, N'=1)$ at 1.3 THz, the most fundamental dipole-allowed rotational transition of any molecule, are used as a test case. This transition is here observed for the first time directly. Rotational laser cooling was employed in order to increase the signal, and resonance-enhanced multiphoton dissociation was used as detection method. The black-body-radiation-induced rotational excitation is also observed. The extension of the method to other molecular species is briefly discussed.

quant-ph↗

arXiv2011

Resonant multi-photon IR dissociation spectroscopy of a trapped and sympathetically cooled biomolecular ion species

In this work we demonstrate vibrational spectroscopy of polyatomic ions that are trapped and sympathetically cooled by laser-cooled atomic ions. We use the protonated dipeptide tryptophane-alanine (HTyrAla+) as a model system, cooled by Barium ions to less than 800mK secular temperature. The spectroscopy is performed on the fundamental vibrational transition of a local vibrational mode at 2.74 μm using a continuous-wave optical parametric oscillator (OPO). Resonant multi-photon IR dissociation spectroscopy (without the use of a UV laser) generates charged molecular fragments, which are sympathetically cooled and trapped, and subsequently released from the trap and counted. We measured the cross section for R-IRMPD under conditions of low intensity, and found it to be approximately two orders smaller than the vibrational excitation cross section. The observed rotational bandwidth of the vibrational transition is larger than the one expected from the combined effects of 300 K black-body temperature, conformer-dependent line shifts, and intermolecular vibrational relaxation broadening (J. Stearns et al., J. Chem. Phys., 127, 154322-7 (2007)). This indicates that as the internal energy of the molecule grows, an increase of the rotational temperature of the molecular ions well above room temperature (up to on the order of 1000K), and/or an appreciable shift of the vibrational transition frequency (approx. 6-8 cm$^{-1}$) occurs.

physics.chem-ph↗

arXiv2009

Measurement of small photodestruction rates of cold, charged biomolecules in an ion trap

In this work, we demonstrate measurements of photodestruction rates of translationally cold, charged biomolecules. The long-term stable storage of the molecular ions in an ion trap at ultra-high vacuum conditions allows measurement of small rates and verification that rates are linear in photodestruction laser intensity. Measurements were performed on singly protonated molecules of the organic compound glycyrrhetinic acid (C30H46O4), dissociated by a continuous-wave UV laser (266 nm) using different intensities. The molecules were sympathetically cooled by simultaneously trapped laser-cooled barium ions to translational temperatures of below 150 mK. Destruction rates of less than 0.05 s^-1 and a cross section of (1.1 +/- 0.1) * 10^-17 cm^2 have been determined. An extension to tunable UV laser sources would permit high-resolution dissociation spectroscopic studies on a wide variety of cold complex molecules.

physics.atom-ph↗

arXiv2008

Translational cooling and storage of protonated proteins in an ion trap at subkelvin temperatures

Gas-phase multiply charged proteins have been sympathetically cooled to translational temperatures below 1 K by Coulomb interaction with laser-cooled barium ions in a linear ion trap. In one case, an ensemble of 53 cytochrome c molecules (mass ~ 12390 amu, charge +17 e) was cooled by ~ 160 laser-cooled barium ions to less than 0.75 K. Storage times of more than 20 minutes have been observed and could easily be extended to more than an hour. The technique is applicable to a wide variety of complex molecules.

physics.atom-ph↗