Laser Excitation of the Th-229 Nucleus.

The 8.4 eV nuclear isomer state in Th-229 is resonantly excited in Th-doped CaF_{2} crystals using a tabletop tunable laser system. A resonance fluorescence signal is observed in two crystals with different Th-229 dopant concentrations, while it is absent in a control experiment using Th-232. The nuclear resonance for the Th^{4+} ions in Th:CaF_{2} is measured at the wavelength 148.3821(5) nm, frequency 2020.409(7) THz, and the fluorescence lifetime in the crystal is 630(15) s, corresponding to an isomer half-life of 1740(50) s for a nucleus isolated in vacuum. These results pave the way toward Th-229 nuclear laser spectroscopy and realizing optical nuclear clocks.

Evaluation of a

We report on an evaluation of an optical clock that uses the ^{2}S_{1/2}→^{2}D_{5/2} transition of a single ^{88}Sr^{+} ion as the reference. In contrast to previous work, we estimate the effective temperature of the blackbody radiation that shifts the reference transition directly during operation from the corresponding frequency shift and the well-characterized sensitivity to thermal radiation. We measure the clock output frequency against an independent ^{171}Yb^{+} ion clock, based on the ^{2}S_{1/2}(F=0)→^{2}F_{7/2}(F=3) electric octupole (E3) transition, and determine the frequency ratio with a total fractional uncertainty of 2.3×10^{-17}. Relying on a previous measurement of the ^{171}Yb^{+} (E3) clock frequency, we find the absolute frequency of the ^{88}Sr^{+} clock transition to be 444 779 044 095 485.277(59) Hz. Our result reduces the uncertainty by a factor of 3 compared with the previously most accurate measurement and may help to resolve so far inconsistent determinations of this value. We also show that for three simultaneously interrogated ^{88}Sr^{+} ions, the increased number causes the expected improvement of the short-term frequency instability of the optical clock without degrading its systematic uncertainty.

Improved Limits on the Coupling of Ultralight Bosonic Dark Matter to Photons from Optical Atomic Clock Comparisons.

We present improved constraints on the coupling of ultralight bosonic dark matter to photons based on long-term measurements of two optical frequency ratios. In these optical clock comparisons, we relate the frequency of the ^{2}S_{1/2}(F=0)↔^{2}F_{7/2}(F=3) electric-octupole (E3) transition in ^{171}Yb^{+} to that of the ^{2}S_{1/2}(F=0)↔^{2}D_{3/2}(F=2) electric-quadrupole (E2) transition of the same ion, and to that of the ^{1}S_{0}↔^{3}P_{0} transition in ^{87}Sr. Measurements of the first frequency ratio ν_{E3}/ν_{E2} are performed via interleaved interrogation of both transitions in a single ion. The comparison of the single-ion clock based on the E3 transition with a strontium optical lattice clock yields the second frequency ratio ν_{E3}/ν_{Sr}. By constraining oscillations of the fine-structure constant α with these measurement results, we improve existing bounds on the scalar coupling d_{e} of ultralight dark matter to photons for dark matter masses in the range of about (10^{-24}-10^{-17}) eV/c^{2}. These results constitute an improvement by more than an order of magnitude over previous investigations for most of this range. We also use the repeated measurements of ν_{E3}/ν_{E2} to improve existing limits on a linear temporal drift of α and its coupling to gravity.

Erratum: Coherent Excitation of the Highly Forbidden Electric Octupole Transition in

This corrects the article DOI: 10.1103/PhysRevLett.125.163001.

Excitation of an Electric Octupole Transition by Twisted Light.

We study the coherent excitation of the ^{2}S_{1/2}→^{2}F_{7/2} electric octupole (E3) transition by twisted light modes with a single ^{171}Yb^{+} ion in the dark center of a vortex beam. The intensity distribution of the beam is mapped as a function of the ion's position by measuring the light shift on an auxiliary electric quadrupole transition. In the center of the vortex beam, we observe excitation of the E3 transition with a fivefold reduced light shift in comparison to excitation by plane wave radiation for the same Rabi frequency. We measure the excitation probabilities for Laguerre-Gaussian twisted light modes of first and second order for different polarization patterns at various orientations of the ion quantization axis with respect to the beam propagation vector. We compare the experimental results with theoretical predictions and find good qualitative agreement.

Lifetime of the

We report a measurement of the radiative lifetime of the ^{2}F_{7/2} level of ^{171}Yb^{+} that is coupled to the ^{2}S_{1/2} ground state via an electric octupole transition. The radiative lifetime is determined to be 4.98(25)×10^{7} s, corresponding to 1.58(8) yr. The result reduces the relative uncertainty in this exceptionally long excited state lifetime by 1 order of magnitude with respect to previous experimental estimates. Our method is based on the coherent excitation of the corresponding transition and avoids limitations through competing decay processes. The explicit dependence on the laser intensity is eliminated by simultaneously measuring the resonant Rabi frequency and the induced quadratic Stark shift. Combining the result with information on the dynamic differential polarizability permits a calculation of the transition matrix element to infer the radiative lifetime.

Improved Limits for Violations of Local Position Invariance from Atomic Clock Comparisons.

We compare two optical clocks based on the ^{2}S_{1/2}(F=0)→^{2}D_{3/2}(F=2) electric quadrupole (E2) and the ^{2}S_{1/2}(F=0)→^{2}F_{7/2}(F=3) electric octupole (E3) transition of ^{171}Yb^{+} and measure the frequency ratio ν_{E3}/ν_{E2}=0.932829404530965376(32), improving upon previous measurements by an order of magnitude. Using two caesium fountain clocks, we find ν_{E3}=642121496772645.10(8) Hz, the most accurate determination of an optical transition frequency to date. Repeated measurements of both quantities over several years are analyzed for potential violations of local position invariance. We improve by factors of about 20 and 2 the limits for fractional temporal variations of the fine structure constant α to 1.0(1.1)×10^{-18}/yr and of the proton-to-electron mass ratio µ to -8(36)×10^{-18}/yr. Using the annual variation of the Sun's gravitational potential at Earth Φ, we improve limits for a potential coupling of both constants to gravity, (c^{2}/α)(dα/dΦ)=14(11)×10^{-9} and (c^{2}/µ)(dµ/dΦ)=7(45)×10^{-8}.

Coherent Suppression of Tensor Frequency Shifts through Magnetic Field Rotation.

We introduce a scheme to coherently suppress second-rank tensor frequency shifts in atomic clocks, relying on the continuous rotation of an external magnetic field during the free atomic state evolution in a Ramsey sequence. The method retrieves the unperturbed frequency within a single interrogation cycle and is readily applicable to various atomic clock systems. For the frequency shift due to the electric quadrupole interaction, we experimentally demonstrate suppression by more than two orders of magnitude for the ^{2}S_{1/2}→^{2}D_{3/2} transition of a single trapped ^{171}Yb^{+} ion. The scheme provides particular advantages in the case of the ^{171}Yb^{+} ^{2}S_{1/2}→^{2}F_{7/2} electric octupole (E3) transition. For an improved estimate of the residual quadrupole shift for this transition, we measure the excited state electric quadrupole moments Θ(^{2}D_{3/2})=1.95(1)ea_{0}^{2} and Θ(^{2}F_{7/2})=-0.0297(5)ea_{0}^{2} with e the elementary charge and a_{0} the Bohr radius, improving the measurement uncertainties by one order of magnitude.

Coherent Excitation of the Highly Forbidden Electric Octupole Transition in

We report on the first coherent excitation of the highly forbidden ^{2}S_{1/2}→^{2}F_{7/2} electric octupole (E3) transition in a single trapped ^{172}Yb^{+} ion, an isotope without nuclear spin. Using the transition in ^{171}Yb^{+} as a reference, we determine the transition frequency to be 642 116 784 950 887.6(2.4) Hz. We map out the magnetic field environment using the forbidden ^{2}S_{1/2}→^{2}D_{5/2} electric quadrupole (E2) transition and determine its frequency to be 729 476 867 027 206.8(4.4) Hz. Our results are a factor of 1×10^{5} (3×10^{5}) more accurate for the E2 (E3) transition compared to previous measurements. The results open up the way to search for new physics via precise isotope shift measurements and improved tests of local Lorentz invariance using the metastable ^{2}F_{7/2} state of Yb^{+}.

Nuclear Charge Radii of

The isotope ^{229}Th is unique in that it possesses an isomeric state of only a few electron volts above the ground state, suitable for nuclear laser excitation. An optical clock based on this transition is expected to be a very sensitive probe for variations of fundamental constants, but the nuclear properties of both states have to be determined precisely to derive the actual sensitivity. We carry out isotope shift calculations in Th^{+} and Th^{2+} including the specific mass shift, using a combination of configuration interaction and all-order linearized coupled-cluster methods and estimate the uncertainty of this approach. We perform experimental measurements of the hyperfine structure of Th^{2+} and isotopic shift between ^{229}Th^{2+} and ^{232}Th^{2+} to extract the difference in root-mean-square radii as δ⟨r^{2}⟩^{232,229}=0.299(15) fm^{2}. Using the recently measured values of the isomer shift of lines of ^{229m}Th, we derive the value for the mean-square radius change between ^{229}Th and its low-lying isomer ^{229m}Th to be δ⟨r^{2}⟩^{229m,229}=0.0105(13) fm^{2}.

Single-Ion Atomic Clock with 3×10(-18) Systematic Uncertainty.

We experimentally investigate an optical frequency standard based on the (2)S1/2(F=0)→(2)F7/2(F=3) electric octupole (E3) transition of a single trapped (171)Yb+ ion. For the spectroscopy of this strongly forbidden transition, we utilize a Ramsey-type excitation scheme that provides immunity to probe-induced frequency shifts. The cancellation of these shifts is controlled by interleaved single-pulse Rabi spectroscopy, which reduces the related relative frequency uncertainty to 1.1×10(-18). To determine the frequency shift due to thermal radiation emitted by the ion's environment, we measure the static scalar differential polarizability of the E3 transition as 0.888(16)×10(-40) J m(2)/V(2) and a dynamic correction η(300 K)=-0.0015(7). This reduces the uncertainty due to thermal radiation to 1.8×10(-18). The residual motion of the ion yields the largest contribution (2.1×10(-18)) to the total systematic relative uncertainty of the clock of 3.2×10(-18).

Frequency Comparison of [Formula: see text] Ion Optical Clocks at PTB and NPL via GPS PPP.

We used precise point positioning, a well-established GPS carrier-phase frequency transfer method to perform a direct remote comparison of two optical frequency standards based on single laser-cooled [Formula: see text] ions operated at the National Physical Laboratory (NPL), U.K. and the Physikalisch-Technische Bundesanstalt (PTB), Germany. At both institutes, an active hydrogen maser serves as a flywheel oscillator which is connected to a GPS receiver as an external frequency reference and compared simultaneously to a realization of the unperturbed frequency of the (2)S1/2(F=0)-(2)D3/2(F=2) electric quadrupole transition in [Formula: see text] via an optical femtosecond frequency comb. To profit from long coherent GPS-link measurements, we extrapolate the fractional frequency difference over the various data gaps in the optical clock to maser comparisons which introduces maser noise to the frequency comparison but improves the uncertainty from the GPS-link instability. We determined the total statistical uncertainty consisting of the GPS-link uncertainty and the extrapolation uncertainties for several extrapolation schemes. Using the extrapolation scheme with the smallest combined uncertainty, we find a fractional frequency difference [Formula: see text] of -1.3×10(-15) with a combined uncertainty of 1.2×10(-15) for a total measurement time of 67 h. This result is consistent with an agreement of the frequencies realized by both optical clocks and with recent absolute frequency measurements against caesium fountain clocks within the corresponding uncertainties.

Improved limit on a temporal variation of mp/me from comparisons of Yb+ and Cs atomic clocks.

Accurate measurements of different transition frequencies between atomic levels of the electronic and hyperfine structure over time are used to investigate temporal variations of the fine structure constant α and the proton-to-electron mass ratio µ. We measure the frequency of the (2)S1/2→(2)F7/2 electric octupole (E3) transition in (171)Yb(+) against two caesium fountain clocks as f(E3)=642,121,496,772,645.36 Hz with an improved fractional uncertainty of 3.9×10(-16). This transition frequency shows a strong sensitivity to changes of α. Together with a number of previous and recent measurements of the (2)S1/2→(2)D3/2 electric quadrupole transition in (171)Yb(+) and with data from other elements, a least-squares analysis yields (1/α)(dα/dt)=-0.20(20)×10(-16)/yr and (1/µ)(dµ/dt)=-0.5(1.6)×10(-16)/yr, confirming a previous limit on dα/dt and providing the most stringent limit on dµ/dt from laboratory experiments.

Generalized Ramsey excitation scheme with suppressed light shift.

We experimentally investigate a recently proposed optical excitation scheme V. I. Yudin et al. [Phys. Rev. A 82, 011804(R) (2010)] that is a generalization of Ramsey's method of separated oscillatory fields and consists of a sequence of three excitation pulses. The pulse sequence is tailored to produce a resonance signal that is immune to the light shift and other shifts of the transition frequency that are correlated with the interaction with the probe field. We investigate the scheme using a single trapped ^{171}Yb^{+} ion and excite the highly forbidden (2)S(1/2) - (2)F(7/2) electric-octupole transition under conditions where the light shift is much larger than the excitation linewidth, which is in the hertz range. The experiments demonstrate a suppression of the light shift by four orders of magnitude and an immunity against its fluctuations.

High-accuracy optical clock based on the octupole transition in 171Yb+.

We experimentally investigate an optical frequency standard based on the 467 nm (642 THz) electric-octupole reference transition (2)S(1/2)(F=0)→(2)F(7/2)(F=3) in a single trapped (171)Yb(+) ion. The extraordinary features of this transition result from the long natural lifetime and from the 4f(13)6s(2) configuration of the upper state. The electric-quadrupole moment of the (2)F(7/2) state is measured as -0.041(5)ea(0)(2), where e is the elementary charge and a(0) the Bohr radius. We also obtain information on the differential scalar and tensorial components of the static polarizability and of the probe-light-induced ac Stark shift of the octupole transition. With a real-time extrapolation scheme that eliminates this shift, the unperturbed transition frequency is realized with a fractional uncertainty of 7.1×10(-17). The frequency is measured as 642 121 496 772 645.15(52) Hz.

Atomic clocks with suppressed blackbody radiation shift.

We develop a concept of atomic clocks where the blackbody radiation shift and its fluctuations can be suppressed by 1-3 orders of magnitude independent of the environmental temperature. The suppression is based on the fact that in a system with two accessible clock transitions (with frequencies ν1 and ν2) which are exposed to the same thermal environment, there exists a "synthetic" frequency ν(syn) ∝ (ν1 - ε12ν2) largely immune to the blackbody radiation shift. For example, in the case of 171Yb+ it is possible to create a synthetic-frequency-based clock in which the fractional blackbody radiation shift can be suppressed to the level of 10(-18) in a broad interval near room temperature (300±15 K). We also propose a realization of our method with the use of an optical frequency comb generator stabilized to both frequencies ν1 and ν2, where the frequency ν(syn) is generated as one of the components of the comb spectrum.

Excitation of the isomeric 229mTh nuclear state via an electronic bridge process in 229Th+.

We consider the excitation of the nuclear transition 229gTh-229mTh near 7.6 eV in singly ionized thorium via an electronic bridge process. The process relies on the excitation of the electron shell by two laser photons whose sum frequency is equal to the nuclear transition frequency. This scheme allows us to determine the nuclear transition frequency with high accuracy. Based on calculations of the electronic level structure of Th+ which combine the configuration-interaction method and many-body perturbation theory, we estimate that a nuclear excitation rate in the range of 10 s⁻¹ can be obtained using conventional laser sources.

Sub-Hertz optical frequency comparisons between two trapped 171Yb+ ions.

We compare the frequencies of the 6s2S(1/2)(F = 0)-->5d2D(3/2)(F = 2) reference transition in 171Yb+ for two single ions stored in independent traps. The quadrupole moment of the 5d2D(3/2) state is measured to be 9.32(48) x 10(-40) C m2 and from the quadratic Stark shift the relevant scalar and tensor polarizabilities are determined to be alphaS(S(1/2)) - alphaS(D(3/2)) = -6.9(1.4) x 10(-40) J m2/V2 and alphaT(D(3/2)) = -13.6(2.2) x 10(-40) J m2/V2, respectively. In the absence of external perturbations we find a mean frequency difference between the two trapped ions of 0.26(42) Hz, corresponding to a relative difference of 3.8(6.1) x 10(-16). This is comparable to the agreement found in the most accurate comparisons between cesium fountain clocks.

Limit on the present temporal variation of the fine structure constant.

The comparison of different atomic transition frequencies over time can be used to determine the present value of the temporal derivative of the fine structure constant alpha in a model-independent way without assumptions on constancy or variability of other parameters, allowing tests of the consequences of unification theories. We have measured an optical transition frequency at 688 THz in 171Yb+ with a cesium atomic clock at 2 times separated by 2.8 yr and find a value for the fractional variation of the frequency ratio f(Yb)/f(Cs) of (-1.2+/-4.4)x10(-15) yr(-1), consistent with zero. Combined with recently published values for the constancy of other transition frequencies this measurement sets an upper limit on the present variability of alpha at the level of 2.0x10(-15) yr(-1) (1sigma), corresponding so far to the most stringent limit from laboratory experiments.

Absolute frequency measurement of the In+ clock transition with a mode-locked laser.

The absolute frequency of the In(+) 5s(2) (1)S(0)5s5p (3)P(0) clock transition at 237 nm was measured with an accuracy of 1.8 parts in 10(13). Using a phase-coherent frequency chain, we compared the (1)S(0)(3)P(0) transition with a methane-stabilized HeNe laser at 3.39 microm, which was calibrated against an atomic cesium fountain clock. A frequency gap of 37 THz at the fourth harmonic of the HeNe standard was bridged by a frequency comb generated by a mode-locked femtosecond laser. The frequency of the In(+) clock transition was found to be 1,267,402,452,899.92 (0.23) kHz, the accuracy being limited by the uncertainty of the HeNe laser reference. This result represents an improvement in accuracy of more than 2 orders of magnitude over previous measurements of the line and now stands as what is to our knowledge the most accurate measurement of an optical transition in a single ion.s.