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Dieter Meschede · Thomas Udem
Tilman Esslinger Editors

Exploring the
World with
the Laser
Dedicated to Theodor Hänsch on his
75th birthday
Exploring the World with the Laser
Dieter Meschede • Thomas Udem •
Tilman Esslinger
Editors

Exploring the World

with the Laser
Dedicated to Theodor Hänsch
on his 75th birthday
Editors
Dieter Meschede Thomas Udem
Institute for Applied Physics Max-Planck-Institute for Quantenoptik (MPQ)
University of Bonn Garching, Germany
Bonn, Germany

Tilman Esslinger
ETH Zurich
Institute for Quantum Electronics
Zurich, Switzerland

ISBN 978-3-319-64345-8 ISBN 978-3-319-64346-5 (eBook)

https://doi.org/10.1007/978-3-319-64346-5

Library of Congress Control Number: 2017951119

© The Editor(s) (if applicable) and The Author(s) 2018

The chapters “New Avenues for Matter-Wave-Enhanced Spectroscopy”, “From Quantum Transitions
to Electronic Motions”, “Measuring and Imaging Nanomechanical Motion with Laser Light”,
“Quantum Regime of a Free-Electron Laser: Relativistic Approach”, “Atomic “Bomb Testing”:
The Elitzur–Vaidman Experiment Violates the Leggett–Garg Inequality”, “High-Accuracy Deep-UV
Ramsey-comb Spectroscopy in Krypton”, “Phase-Stable, Multi-μJ Femtosecond Pulses from a
Repetition-Rate Tunable Ti:Sa-Oscillator-Seeded Yb-Fiber Amplifier”, “High-Precision Spectroscopy
of the HD+ Molecule at the 1-p.p.b. Level”, “Orientational Dependence of Optically Detected
Magnetic Resonance Signals in Laser-Driven Atomic Magnetometers”, “All Polarization-Maintaining
Fiber Laser Architecture for Robust Femtosecond Pulse Generation”, “Topological Spin Models
in Rydberg Lattices”, “Ultrafast Optomechanical Pulse Picking”, “Shifting the Phase of a Coherent
Beam with a 174Yb+ Ion: Influence of the Scattering Cross Section”, “A Compact Echelle Spectrograph
for Characterization of Astro-Combs”, “Mode Locking Based on the Temporal Talbot Effect”,
“Single-Slit Focusing and Its Representations”, “Ultracold Metastable Helium: Ramsey Fringes and
Atom Interferometry”, “Cavity Ring-Up Spectroscopy for Dissipative and Dispersive Sensing in a
Whispering Gallery Mode Resonator”, “Sensitivity and Resolution in Frequency Comb Spectroscopy
of Buffer Gas Cooled Polyatomic Molecules”, “Precision Measurements and Test of Molecular Theory
in Highly Excited Vibrational States of H2 (v ¼ 11)”, “Ranging with Frequency-Shifted Feedback
Lasers: From μm-Range Accuracy to MHz-Range Measurement Rate”, and “Extraction of Enhanced,
Ultrashort Laser Pulses from a Passive 10-MHz Stack-and-Dump Cavity” are licensed under the terms of
the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/
4.0/). For further details see license information in the chapters.
This work is subject to copyright. All rights are reserved by the Publisher, whether the whole or part of
the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations,
recitation, broadcasting, reproduction on microfilms or in any other physical way, and transmission or
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The registered company address is: Gewerbestrasse 11, 6330 Cham, Switzerland
“Enlightening the World with the
Laser”—Honoring T. W. Hänsch1

As guest editors of the T. W. Hänsch special issue of Applied Physics B, we are

delighted to introduce you to a series of articles authored in honor of Professor
Theodor W. “Ted” Hänsch, by colleagues, co-workers and (former) students of his.
The occasion is Ted’s 75th birthday, but the issue celebrates some 50 years of
cutting-edge research that he performed first at the University of Heidelberg in the
late 1960s, then at Stanford University, and since 1986 at the Max Planck Institute
of Quantum Optics in Garching and the Ludwig-Maximilian University of Munich.
Applied Physics B is a natural venue for such a Festschrift, given that Ted is serving
on its Editorial Board since 1983.
How Ted Hänsch has influenced the way we think about lasers, and how we use
them, is truly remarkable. His 75th birthday marks a great occasion to pause and
reflect on his achievements. Ted Hänsch’s passion is precision measurements and
the study of the hydrogen atom. Yet, even if the Nobel Prize came for the ingenious
frequency comb, “precision” and “hydrogen” do not quite cover his approach to
physics. More generally, Ted keeps teaching us how we can use laser light,
sometimes for rather playful applications, sometimes for fundamental break-
throughs—and from time to time also for commercial devices. His unique way of
doing physics, however, goes much further. In addition to leading the way with
groundbreaking research on topics from precision laser spectroscopy to ultracold
quantum gases, Ted has motivated an entire generation of physicists to pursue
related goals. He has generated a lasting impact in several communities, not least
thanks to the large number of alumni from his research group who have gone on to
develop careers of their own, inspired by Ted’s example.
The esteem in which Ted is held by colleagues, collaborators and friends from
around the world is reflected in the large number of excellent articles in this volume.
We are grateful to the many authors who contributed such interesting papers. As

1
This article is part of the topical collection “Enlightening the World with the Laser” - Honoring
T. W. Hänsch guest edited by Tilman Esslinger, Nathalie Picqué, and Thomas Udem.

v
vi “Enlightening the World with the Laser”—Honoring T. W. Hänsch

you browse this issue, you will find papers by outstanding scientists who are
working in the broad, interdisciplinary field of atomic, molecular and optical
physics. Most contributions highlight the influence of Ted’s scientific activities,
current and past. Exciting new findings regarding precision spectroscopy of atoms
and molecules are reported, alongside intriguing contributions in the areas of opto-
mechanics, ultracold atomic and molecular quantum gases and matter-wave optics,
as well as works on the development and application of novel laser sources,
including frequency combs. Other articles provide insightful perspectives and
reviews dedicated to various aspects of quantum and optical sciences.
We hope you will join us in celebrating Ted’s achievements and enjoy this
collection of papers.
Congratulations on your 75th birthday, Ted! We look forward to many more
ideas on how to explore the world with laser light.

Swiss Federal Institute of Technology Tilman Esslinger

Switzerland
Max Planck Institute of Quantum Optics Nathalie Picqué
Germany
Max Planck Institute of Quantum Optics Thomas Udem
Germany
Zurich and Garching
October 19, 2016
Contents

Unexpectedly Large Difference of the Electron Density at the Nucleus

in the 4p 2P1/2,3/2 Fine-Structure Doublet of Caþ . . . . . . . . . . . . . . . . . 1
C. Shi, F. Gebert, C. Gorges, S. Kaufmann, W. N€ortershäuser, B.K. Sahoo,
A. Surzhykov, V.A. Yerokhin, J.C. Berengut, F. Wolf, J.C. Heip,
and P.O. Schmidt
New Avenues for Matter-Wave-Enhanced Spectroscopy . . . . . . . . . . . 21
Jonas Rodewald, Philipp Haslinger, Nadine D€orre, Benjamin A. Stickler,
Armin Shayeghi, Klaus Hornberger, and Markus Arndt
Yb Fiber Amplifier at 972.5 nm with Frequency Quadrupling
to 243.1 nm . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 35
Z. Burkley, C. Rasor, S.F. Cooper, A.D. Brandt, and D.C. Yost
Optical Autler–Townes Spectroscopy in a Heteronuclear Mixture
of Laser-Cooled Atoms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45
C. Bruni, F. Münchow, and A. G€orlitz
From Quantum Transitions to Electronic Motions . . . . . . . . . . . . . . . 59
Ferenc Krausz
Measuring and Imaging Nanomechanical Motion with Laser Light . . . 71
Andreas Barg, Yeghishe Tsaturyan, Erik Belhage, William H.P. Nielsen,
Christoffer B. Møller, and Albert Schliesser
Quantum Regime of a Free-Electron Laser: Relativistic Approach . . . 87
Peter Kling, Roland Sauerbrey, Paul Preiss, Enno Giese, Rainer Endrich,
and Wolfgang P. Schleich
Playing Tricks to Ions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 117
Dietrich Leibfried

vii
viii Contents

Coherence in Laser-Driven Electrons at the Surface and in the

Volume of Solid Matter . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 129
Peter Hommelhoff
Atomic “Bomb Testing”: The Elitzur–Vaidman Experiment
Violates the Leggett–Garg Inequality . . . . . . . . . . . . . . . . . . . . . . . . . . 141
Carsten Robens, Wolfgang Alt, Clive Emary, Dieter Meschede,
and Andrea Alberti
Adjacency Graphs and Long-Range Interactions of Atoms
in Quasi-degenerate States: Applied Graph Theory . . . . . . . . . . . . . . . 159
C.M. Adhikari, V. Debierre, and U.D. Jentschura
Frequency-Comb Referenced Collinear Laser Spectroscopy of Be+
for Nuclear Structure Investigations and Many-Body QED Tests . . . . 175
A. Krieger, W. N€
ortershäuser, Ch. Geppert, K. Blaum, M.L. Bissell,
N. Fr€
ommgen, M. Hammen, K. Kreim, M. Kowalska, J. Krämer,
R. Neugart, G. Neyens, R. Sánchez, D. Tiedemann, D.T. Yordanov,
and M. Zakova
High-Accuracy Deep-UV Ramsey-comb Spectroscopy in Krypton . . . . 207
Sandrine Galtier, Robert K. Altmann, Laura S. Dreissen,
and Kjeld S.E. Eikema
Phase-Stable, Multi-μJ Femtosecond Pulses from a Repetition-Rate
Tunable Ti:Sa-Oscillator-Seeded Yb-Fiber Amplifier . . . . . . . . . . . . . 225
T. Saule, S. Holzberger, O. De Vries, M. Pl€otner, J. Limpert,
A. Tünnermann, and I. Pupeza
Quantum Electrodynamics, High-Resolution Spectroscopy
and Fundamental Constants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237
Savely G. Karshenboim and Vladimir G. Ivanov
High-Precision Spectroscopy of the HD+ Molecule
at the 1-p.p.b. Level . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 267
J. Biesheuvel, J.-Ph. Karr, L. Hilico, K.S.E. Eikema, W. Ubachs,
and J.C.J. Koelemeij
Orientational Dependence of Optically Detected Magnetic Resonance
Signals in Laser-Driven Atomic Magnetometers . . . . . . . . . . . . . . . . . 309
Simone Colombo, Vladimir Dolgovskiy, Theo Scholtes, Zoran D. Grujić,
Victor Lebedev, and Antoine Weis
All Polarization-Maintaining Fiber Laser Architecture for Robust
Femtosecond Pulse Generation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 331
Wolfgang Hänsel, Heinar Hoogland, Michele Giunta, Sebastian Schmid,
Tilo Steinmetz, Ralf Doubek, Peter Mayer, Sven Dobner, Carsten Cleff,
Marc Fischer, and Ronald Holzwarth
Contents ix

A >2-MJ, 1014-W Laser System for DT Fusion—NIF: A Note

in Celebration of the 75th Birthday of Prof. Theodore Haensch . . . . . 341
John F. Holzrichter and Kenneth R. Manes
Topological Spin Models in Rydberg Lattices . . . . . . . . . . . . . . . . . . . 351
Martin Kiffner, Edward O’Brien, and Dieter Jaksch
Ultrafast Optomechanical Pulse Picking . . . . . . . . . . . . . . . . . . . . . . . 371
Nikolai Lilienfein, Simon Holzberger, and Ioachim Pupeza
Shifting the Phase of a Coherent Beam with a 174 Ybþ Ion: Influence
of the Scattering Cross Section . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 389
Martin Fischer, Bharath Srivathsan, Lucas Alber, Markus Weber,
Markus Sondermann, and Gerd Leuchs
Thirty Years of Hydrogen Spectroscopy in Paris . . . . . . . . . . . . . . . . . 401
François Biraben, Lucile Julien, and François Nez
A Dense Gas of Laser-Cooled Atoms for Hybrid
Atom–Ion Trapping . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 417
Bastian H€
oltkemeier, Julian Glässel, Henry López-Carrera,
and Matthias Weidemüller
A Compact Echelle Spectrograph for Characterization
of Astro-Combs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 433
Rafael A. Probst, Tilo Steinmetz, Yuanjie Wu, Frank Grupp,
Thomas Udem, and Ronald Holzwarth
Mode Locking Based on the Temporal Talbot Effect . . . . . . . . . . . . . . 447
Thomas Udem and Akira Ozawa
T3-Interferometer for Atoms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 457
M. Zimmermann, M.A. Efremov, A. Roura, W.P. Schleich,
S.A. DeSavage, J.P. Davis, A. Srinivasan, F.A. Narducci, S.A. Werner,
and E.M. Rasel
Double-Electron Ionization Driven by Inhomogeneous Fields . . . . . . . 491
A. Chacón, L. Ortmann, F. Cucchietti, N. Suárez, J.A. Pérez-Hernández,
M.F. Ciappina, A.S. Landsman, and M. Lewenstein
Parity-Nonconserving Interaction-Induced Light Shifts in the
7S1=2 –6D3=2 Transition of the Ultracold 210 Fr Atoms to Probe
New Physics Beyond the Standard Model . . . . . . . . . . . . . . . . . . . . . . 509
T. Aoki, Y. Torii, B.K. Sahoo, B.P. Das, K. Harada, T. Hayamizu,
K. Sakamoto, H. Kawamura, T. Inoue, A. Uchiyama, S. Ito, R. Yoshioka,
K.S. Tanaka, M. Itoh, A. Hatakeyama, and Y. Sakemi
Single-Slit Focusing and Its Representations . . . . . . . . . . . . . . . . . . . . 529
Manuel R. Gonçalves, William B. Case, Ady Arie,
and Wolfgang P. Schleich
x Contents

Nonadiabatic Molecular Alignment of Linear Molecules Probed

by Strong-Field Ionization Yields of Photoelectrons . . . . . . . . . . . . . . . 577
G. Kaya, N. Kaya, J. Strohaber, N.A. Hart, A.A. Kolomenskii,
and H.A. Schuessler
Ultracold Metastable Helium: Ramsey Fringes and Atom
Interferometry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 597
W. Vassen, R.P.M.J.W. Notermans, R.J. Rengelink,
and R.F.H.J. van der Beek
Monolayer Graphene as Dissipative Membrane in an Optical
Resonator . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 617
Hendrik M. Meyer, Moritz Breyer, and Michael K€ohl
Cavity Ring-Up Spectroscopy for Dissipative and Dispersive Sensing
in a Whispering Gallery Mode Resonator . . . . . . . . . . . . . . . . . . . . . . 629
Yong Yang, Ramgopal Madugani, Sho Kasumie, Jonathan M. Ward,
and Sı́le Nic Chormaic
Sensitivity and Resolution in Frequency Comb Spectroscopy of Buffer
Gas Cooled Polyatomic Molecules . . . . . . . . . . . . . . . . . . . . . . . . . . . . 647
P. Bryan Changala, Ben Spaun, David Patterson, John M. Doyle,
and Jun Ye
Laser Phase Spectroscopy in Closed-Loop Multilevel Schemes . . . . . . 665
Ennio Arimondo
Precision Measurements and Test of Molecular Theory in Highly
Excited Vibrational States of H2 (v ¼ 11) . . . . . . . . . . . . . . . . . . . . . . . 679
T. Madhu Trivikram, M.L. Niu, P. Wcisło, W. Ubachs,
and E.J. Salumbides
Ranging with Frequency-Shifted Feedback Lasers: From μm-Range
Accuracy to MHz-Range Measurement Rate . . . . . . . . . . . . . . . . . . . . 701
J.I. Kim, V.V. Ogurtsov, G. Bonnet, L.P. Yatsenko, and K. Bergmann
Absorption Spectroscopy of Xenon and Ethylene–Noble Gas Mixtures
at High Pressure: Towards Bose–Einstein Condensation of Vacuum
Ultraviolet Photons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 729
Christian Wahl, Rudolf Brausemann, Julian Schmitt, Frank Vewinger,
Stavros Christopoulos, and Martin Weitz
Extraction of Enhanced, Ultrashort Laser Pulses from a Passive
10-MHz Stack-and-Dump Cavity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 741
Sven Breitkopf, Stefano Wunderlich, Tino Eidam, Evgeny Shestaev,
Simon Holzberger, Thomas Gottschall, Henning Carstens,
Andreas Tünnermann, Ioachim Pupeza, and Jens Limpert
Contents xi

External Cavity Diode Laser Setup with Two Interference Filters . . . . 753
Alexander Martin, Patrick Baus, and Gerhard Birkl
Bose–Einstein Condensates in an Optical Cavity with Sub-recoil
Bandwidth . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 765
J. Klinder, H. Keßler, Ch. Georges, J. Vargas, and A. Hemmerich
Ted’s Stanford Days . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 791
David H. McIntyre and Allister I. Ferguson
From Laser Cooling to the Superfluid Mott Insulator . . . . . . . . . . . . . 805
Tilman Esslinger
Unexpectedly Large Difference of the Electron
Density at the Nucleus in the 4p 2P1/2,3/2
Fine-Structure Doublet of Caþ

C. Shi, F. Gebert, C. Gorges, S. Kaufmann, W. N€ortershäuser, B.K. Sahoo,

A. Surzhykov, V.A. Yerokhin, J.C. Berengut, F. Wolf, J.C. Heip,
and P.O. Schmidt

Abstract We measured the isotope shift in the 2 S1=2 ! 2 P3=2 (D2) transition in
singly ionized calcium ions using photon recoil spectroscopy. The high accuracy of
the technique enables us to compare the difference between the isotope shifts of this
transition to the previously measured isotopic shifts of the 2 S1=2 ! 2 P1=2 (D1) line.
This so-called splitting isotope shift is extracted and exhibits a clear signature of
field shift contributions. From the data, we were able to extract the small difference
of the field shift coefficient and mass shifts between the two transitions with high

This article is part of the topical collection “Enlightening the World with the Laser” - Honoring
T. W. Hänsch guest edited by Tilman Esslinger, Nathalie Picqué, and Thomas Udem.

C. Shi • F. Gebert • F. Wolf • J.C. Heip

Physikalisch-Technische Bundesanstalt, 38116 Braunschweig, Germany
C. Gorges • S. Kaufmann • W. N€ ortershäuser
Institut für Kernphysik, Technische Universität Darmstadt, 64289 Darmstadt, Germany
B.K. Sahoo
Atomic, Molecular and Optical Physics Division, Physical Research Laboratory, Navrangpura,
Ahmedabad 380009, India
A. Surzhykov
Physikalisch-Technische Bundesanstalt, 38116 Braunschweig, Germany
Technische Universität Braunschweig, 38106 Braunschweig, Germany
V.A. Yerokhin
Physikalisch-Technische Bundesanstalt, 38116 Braunschweig, Germany
Center for Advanced Studies, Peter the Great St. Petersburg Polytechnic University,
St. Petersburg, Russia, 195251
J.C. Berengut
School of Physics, University of New South Wales, New South Wales 2052, Sydney, Australia
P.O. Schmidt (*)
Physikalisch-Technische Bundesanstalt, 38116 Braunschweig, Germany
Institut für Quantenoptik, Leibniz Universität Hannover, 30167 Hannover, Germany
e-mail: [email protected]

© The Editor(s) (if applicable) and The Author(s) 2018 1

D. Meschede et al. (eds.), Exploring the World with the Laser,
https://doi.org/10.1007/978-3-319-64346-5_1
2 C. Shi et al.

accuracy. This J-dependence is of relativistic origin and can be used to benchmark

atomic structure calculations. As a first step, we use several ab initio atomic
structure calculation methods to provide more accurate values for the field shift
constants and their ratio. Remarkably, the high-accuracy value for the ratio of the
field shift constants extracted from the experimental data is larger than all available
theoretical predictions.

1 Introduction

The study of isotopic shifts in atomic systems has a long history [1], and a profound
understanding of the isotope shift and theoretical calculations of the atomic prop-
erties is important in many applications. These reach from the extraction of nuclear
properties from atomic spectra to applications in astronomy and fundamental
physics. The spectrum of atoms and ions encodes information that provides a key
to the ground-state properties of nuclei [2, 3], small parity-violating effects caused
by the weak interaction [4], for unitarity tests of the Cabibbo–Kobayashi–Maskawa
(CKM) matrix [5], or for probing the Higgs coupling between electrons and
quarks [6].
Light appearing on earth from stars at large distances is red-shifted and can
provide information about the spectra of atoms in ancient times and whether there
have been changes, for example, from a variation of the fine-structure constant α.
However, isotopic composition can also contribute to the observed shifts since the
isotopes have different resonance frequencies, but this so-called isotope shift is
usually not resolved [7–9]. In this respect, isotope shift calculations became
recently an important topic with the goal to either determine the influence of the
isotopic abundance of the observed species on the analysis for a change in α [7, 10]
or to provide information of the isotopic composition in the ancient times of the
universe. Calcium is an element of considerable interest for many of the cases
mentioned above. For example, the isotope shift information in the 3d 2 DJ ! 4p 2
PJ infrared triplet [11] led to the discovery of an anomalous isotopic composition in
mercury-manganese (HgMn) stars, in which the isotopic Ca ratio in the stellar
atmosphere is dominated by 48Ca [12, 13]. Isotope shifts in other calcium transitions
have been studied, e.g., to extract nuclear charge radii along the long chain of
isotopes [14–17] or to perform ultra-trace analysis using isotope selective reso-
nance ionization [18]. Moreover, the calcium ion is a workhorse in the field of
quantum-optical applications and transition frequencies and isotope shifts of stable
isotopes were measured with high accuracy [19–22] and supported on-line studies
of exotic isotopes since they serve as calibration points [17, 23].
The calcium isotopic chain is quite unique since it contains two stable
doubly magic isotopes 40, 48 Caþ that have practically identical mean-square charge

40, 48
radii (δ r 2c ¼ 0:0045ð60Þ [22]) even though they are 20% different in mass.
This has been established using a variety of techniques, i.e., elastic electron
scattering [24], muonic atom spectroscopy [25] as well as optical isotope shift
Unexpectedly Large Difference of the Electron Density at the Nucleus in the. . . 3

data, e.g. [15] (for a synopsis see, e.g. [26] and references therein). The negligible
change in nuclear charge radius between the two isotopes allows for a cleaner
separation of mass and field shifts than in most other multi-electron systems. The
high-precision data presented here will provide important benchmarks for improved
calculations of this reference system.
The extraction of nuclear parameters from atomic spectra is strongly facilitated
by atomic structure calculations. Despite being a lighter system with only 19 elec-
trons, isotope shifts in the singly ionized calcium (Ca þ ) have not been studied
rigorously. High-precision calculations of magnetic dipole and electric quadrupole
hyperfine-structure constants have been performed in this ion using an all order
relativistic many-body theory in the coupled-cluster (RCC) theory framework
[27]. However, calculations of field shift and mass shift constants that are required
to estimate isotope shifts have not been performed at the same level of accuracy yet.
Here we present a high-precision absolute frequency measurement of the D2 line
of 40Caþ with 100 kHz accuracy, representing a fivefold improvement over previous
results [20]. Isotope shift measurements of this transition with the same resolution
are compared with a measurement of the D1 line [22]. A clear signature of field shift
contributions to the splitting isotope shift is observed. To explain this finding, we
have also performed several ab initio calculations of field shift constants employing
a hydrogenic method, a mean-field method using Dirac-Fock (DF) equation, and
state-of-the-art atomic structure calculations.

2 Experimental Setup

The isotope shift in the 2 S1=2 ! 2 P3=2 (D2) transition of even calcium isotopes was
measured by photon recoil spectroscopy, as described in detail in references
[21, 22]. In brief, we trap a singly charged 25 Mg þ ion together with the calcium
isotope under investigation in a linear Paul trap. The 25 Mg þ ion is used to
sympathetically cool the axial normal mode of the two-ion crystal to the ground
state [28]. To probe the transition, a series of 70 pulses of the spectroscopy laser
with a pulse length of 125 ns, synchronized to one of the motional frequencies of the
two-ion crystal, are applied. Each spectroscopy laser pulse is followed by 200 ns
short repump pulses on the 2 D3=2 ! 2 P1=2 and 2 D5=2 ! 2 P3=2 transitions at 866 and
854 nm, respectively. Recoil kick upon photon absorption on the spectroscopy
transition results in excitation of nearly coherent motion. This motional excitation
is mapped into an electronic excitation using a stimulated rapid adiabatic passage
(STIRAP) pulse on the 25Mgþ ion [29]. The high photon sensitivity of this technique
provides a large signal-to-noise ratio, resulting in a resolution of about 100 kHz in
less than 15 min of averaging time. As a consequence of the smallness of systematic
effects, the accuracy of absolute frequency measurements is also about 100 kHz.
Isotope shift measurements benefit from further suppression of systematic effects,
since most of them are common to all isotopes.
4 C. Shi et al.

Spectroscopy is performed using a cw single-mode Ti:Sa laser (Sirah, Matisse

TS) which is frequency doubled in an enhancement cavity (Spectra-Physics,
WaveTrain). The frequency of the laser is locked to an erbium-fiber-laser-based
frequency comb. The comb is stabilized in its offset and repetition frequencies to a
H-maser frequency which is calibrated by a cesium fountain at PTB (German
National Metrology Institute) as shown in Fig. 1. A beat signal between the
spectroscopy laser and the nearest comb tooth of a narrow-band frequency-doubled
output of the frequency comb is detected with a fast photo diode. The nearest comb
tooth is identified by measuring the frequency of the spectroscopy laser with a
wavemeter (High Finesse, model WS-7).
The RF signal is monitored by a spectrum analyzer (Rohde & Schwarz, FSL3)
and mixed down to 10 or 35 MHz using an rf synthesizer. The band-pass-filtered
signal is used as the input signal of a self-build phase frequency comparator (PFC)
operating at 10 or 35 MHz, which produces an error signal that is tailored by a
proportional-integral (PI) controller. The generated control signal is used to correct
the frequency of the Ti:Sa laser by changing the length of the laser cavity with a fast
piezo-electric actuator. By adjusting the frequency of the rf synthesizer, the fre-
quency of the spectroscopy laser can be adjusted to the resonances of the different
isotopes. Figure 2 shows the in-loop beat signal between the Ti:Sa laser and the
frequency comb, indicating an upper bound for the linewidth of the spectroscopy
laser below 260 kHz. The long-term frequency instability is determined by counting

Fig. 1 Simplified experimental setup. The left part of this figure indicates the configuration of all
optical beams and bias magnetic field with respect to the ions in the trap. The right part shows the
optical setup for the spectroscopy beam and the calcium repump beam. For details, see text. All RF
sources are referenced to a 10-MHz signal from the H-maser (HM). AOM acousto-optical
modulator, CCD electron-multiplication charge-coupled device, CSF cesium fountain clock, DC
Doppler cooling beam, ECDL external-cavity diode laser, FC frequency counter, FS frequency
synthesizer, P Parabolic mirror, PFC phase and frequency comparator, PI proportional-integral
controller, PI Mg=Ca photo-ionization beam for Mg/Ca, PMT photomultiplier tube, SA spectrum
analyzer, SHG second harmonic generation
Unexpectedly Large Difference of the Electron Density at the Nucleus in the. . . 5

Fig. 2 In-loop beat signal

of the Ti:Sa laser and the
nearest frequency comb
tooth. The data recorded by
the spectrum analyzer with
10 kHz resolution
bandwidth (blue circles) is
fit with a Gaussian profile
(red curve) that gives an
upper bound of 260 kHz for
the linewidth of the
spectroscopy laser. The
black squares present the
residuals of the fit

Fig. 3 Allan deviation of

the Ti:Sa laser frequency as
measured by the frequency
counter. The long-term
instability of the locked
spectroscopy laser is 14 kHz
pffiffiffiffiffiffiffi
= τ=s for integration times
longer than 1 s as derived
from a fit to the data (red
line)

the mixed-down RF signal with a frequency counter pffiffiffiffiffiffiffi(Kramer+Klische FXE). We

derive a frequency instability of about 14 kHz/ τ=s from an Allan deviation of
these measurements as shown in Fig. 3. The linewidth and the frequency instability
both fulfil the requirements for the anticipated resolution and accuracy of below
100 kHz. The spectroscopy beam is intensity stabilized and frequency scanned by
an acousto-optical modulator (AOM), while another AOM is used for switching.
The 866 and 854 nm repump beams depopulating the two D-states are generated
by two external-cavity diode lasers. The combined beam consisting of the two
repumpers is intensity stabilized by an AOM which is also used for fast switching.
The left part of Fig. 1 shows the direction of the beams together with the magnetic
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