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# Coherent Phase Argument for Inflation

## 1 Overview

Over the last several years, we have gradually been accumulating evidence for a remarkable theory of the early universe. This theory now accounts for the observed structure in the universe by invoking new fundamental physics at very high energy scales. The theory is so elegant and simple that it contains just a handful of free parameters. It is outlined in Figure 1, which indicates how perturbations generated during inflation evolve with time. The observations today of anisotropies in the radiation and inhomogeneities in the matter therefore bear the imprint of:

* the potential of the field(s) which drive(s) inflation
* the abundances of different types of matter in the universe (baryons, which interact with radiation; dark matter, which does not; and neutrinos, which can freestream out of overdense region): $`\mathrm{\Omega }_b,\mathrm{\Omega }_m`$, and $`\mathrm{\Omega }_\nu `$
* late time phenomena such as dark energy (parametrized by abundance $`\mathrm{\Omega }_{de}`$ and equation of state $`w`$) and reionization

The most important observations confirming this model come from two segments of the electromagnetic spectrum. First, radio receivers have measured the cosmic microwave background (CMB) to exquisite precision. Second, optical telescopes have captured light from distant galaxies and quasars which tell us about the matter distribution both around those objects 2df ; sdss  and along the line of sight to us weaklensing . They have also received light from distant objects such as galaxies and supernovae, allowing us to measure distances and fill in a modern Hubble diagram wendy ; sn .

Here I will focus on one observation and one aspect of the model. Anisotropies in the CMB were first detected in 1992 by the COBE satellite cobe ; were probed extensively in the ensuing decade by more than thirty smaller scale experiments smallscale ; and have now been mapped exquisitely by the WMAP satellite bennett . These observations have been celebrated for measuring cosmological parameters to unprecedented accuracy (e.g. spergel ; mc ), and I will briefly describe the progress on this front in §5. But, for the most part, I want to focus on how the signal seen in the CMB is smoking gun evidence for the theory of inflation.

## 2 Inflation

The theory of inflation was introduced over twenty years ago guth  to solve some of the problems of the classical cosmology. For many years, progress was limited to theory and to addressing the question of whether the density in the universe is indeed equal to the critical density as inflation seems to predict. By far the most important, or at least the most testable, aspect of inflation though is its mechanism for producing small perturbations about a smooth background. These perturbations can be measured as long as we account for their (straightforward) evolution after inflation ends.

It is well known that inflation produces perturbations characterized by a Harrison-Zel’dovich spectrum mc ; inflper . This means that the amplitude of a particular Fourier mode is drawn from a distribution with mean equal to zero and variance given by

$$\stackrel{~}{\delta }(𝐤)\stackrel{~}{\delta }^{}(𝐤^{})=(2\pi )^3\delta ^3(𝐤𝐤^{})P(k)$$
(1)
where $`\delta `$ is the fractional overdensity with power spectrum $`P(k)`$ proportional to $`k^n`$. A Harrison-Zel’dovich spectrum corresponds to $`n=1`$, and most inflationary models predict something very close to this. You might think then that the shape of the power spectrum can be measured in observations, and this is what convinces us that inflation is right. Well, it is true that we can measure the power spectrum, both of the matter and of the radiation, and it is true that the observations agree with the theory. But this is not what tingles our spines when we look at the data.

Rather, the truly striking aspect of perturbations generated during inflation is that all Fourier modes all have the same phase. To understand what this means and how it develops, consider Fig. 2 which shows a cartoon view of the evolution of the amplitudes of two Fourier modes. Both oscillate quantum mechanically during inflation. Before inflation ends, though, both leave the horizon, that is, their wavelengths get stretched so much that no causal physics can alter them111Technically this occurs when the wavelength of the mode becomes greater than the Hubble radius, $`c/H`$.. Once this happens, their amplitudes remain constant. They stay constant up until the time much later on (for modes of interest this might typically happen when the universe is 100,000 years old) when the modes re-enter the horizon, at which time causal physics can once again affect their amplitudes. The crucial point here is that as the modes re-enter the horizon, $`\dot{\delta }`$ is small. If we think of each Fourier mode as a linear combination of a sin and a cos mode, inflation excites only the cos modes. It is difficult to envision any other theory with this striking feature.

## 3 Acoustic Oscillations

How do perturbations evolve once they re-enter the horizon? A cartoon version of the equation governing them is

$$\ddot{\delta }c_s^2^2\delta =F$$
(2)
where $`c_s`$ is the sound speed and $`F`$ is a forcing function due to gravity. The perturbations obey the wave equation as one expects physically: a region which is very overdense is driven by gravity to become more overdense, but driven toward the average density by pressure.

At this point, you might come to the conclusion that the spectrum of anisotropies in the radiation today will exhibit a series of peaks and troughs just as a guitar string produces a series of higher harmonics. In fact, the spectrum of the CMB looks remarkably like that of a guitar string. However, underlying the similarity is a pair of differences which are essential to the argument that inflation is the origin of the perturbations.

A guitar string produces a set of harmonics because it is tied down at its ends. So there are only a discrete set of frequencies at which it can oscillate. There is no such restriction for perturbations in the early universe, so why do we see anisotropies at certain frequencies but not at others?

To understand this, consider Fig. 3 which shows the evolution of four Fourier modes in the time leading up to recombination222After recombination, photons freestream though the universe, so we see their distribution today as it was at the time of recombination.. The mode with the largest wavelength cannot be affected by causal physics so its amplitude remains constant. Smaller scale modes have entered the horizon, and so have begun their acoustic oscillations. The smaller the wavelength of a mode, the earlier it will have entered the horizon, and the more oscillations it will have undergone by the time of recombination. Thus, the amplitude of the mode labeled “First Peak” is maximal at recombination, and we expect to see large anisotropies on angular scales which subtend this distance (roughly a degree). The mode labeled “First Trough” has oscillated for a longer time though, and its amplitude is zero at recombination. Therefore, we expect very small anisotropies on the corresponding angular scales. And on it goes, a succession of peaks and troughs present not because no excitations are allowed at the frequencies in the troughs (as is the case for the guitar string). Rather, perturbations are present at all wavelengths, but we happen to see only some of them, depending on the phase of the oscillation at recombination.

It is now very important to remember that there are many, many modes with nearly identical wavenumbers. Think of the number of arrows that can point from the center of a sphere to a fixed radius, keeping in mind that two arrows can be placed infinitesimally close to each other. In fact, since the universe is effectively infinite, there are an infinite number of modes for any wavenumber. All of these get excited during inflation and we must sum over all of them to compute the anisotropy amplitude at a given scale. Thus, when I drew the single line corresponding to the “First Peak” mode in Fig. 3, this was really shorthand for an infinite number of modes all with different amplitudes, as in Fig. 4. The amplitudes may differ, but as Fig. 4 shows, the phases are all the same. All modes enter the horizon with constant amplitude. Thus, all modes with the “First Peak” wavenumber have maximal amplitude (left panel in the figure) at recombination: they have all undergone half an oscillation, so their sign simply changes. Similarly, all modes corresponding to “First Trough” have gone through $`3/4`$ of an oscillation333You might expect the mode which has gone through $`1/4`$ of a full oscillation to be the first trough. However, there are other effects (the dipole and the Integrated Sachs-Wolfe effect) which fill in this trough.; since they all are cosine modes and $`\mathrm{cos}(3\pi /2)=0`$, all have zero amplitude at recombination (right panel).

Contrast this with the situation one might otherwise expect, random phases, as depicted in Fig. 5. If the phases were truly random, so that both the sine and cosine modes were excited, then at recombination, there would not be any difference at all between the rms amplitudes of the First Peak and First Trough wavenumbers. So we would not see a sequence of peaks and troughs in the anisotropy spectrum today. We would see simply a flat spectrum with no features. If not for inflation, we would see a flat spectrum. How else could the phases have been set well before the modes of interest entered the horizon?

Therefore, when we look at the anisotropy spectrum recently measured by WMAP bennett  and we see the first and second peaks and troughs very clearly (Fig. 6), we are really observing inflation doing the work of coordinating the phases of all Fourier modes. Without this coherence, there would be no peaks and troughs.

## 4 Polarization

The bottom panel of Figure 6 shows the cross-correlation between the temperature and polarization anisotropies. This cross-correlation was first detected by the DASI experiment in late 2002 kovac , so our measurements of polarization are much less established than those of temperature. Yet the WMAP results already are a crucial part of the coherence argument for inflation. The peaks and troughs in the anisotropy spectrum all are on angular scales smaller than a degree $`(l>200)`$; all of these scales were within the horizon at the time of recombination. So you might imagine that one could concoct a theory of structure formation which obeyed causality and still managed to produce only the cosine modes. If you could concoct such a theory turok ; hw , then you could explain the peaks and troughs without appealing to inflation. It seems unlikely, but it is at least logically possible.

This logical possibility evaporates when confronted with the polarization data. In particular, the negative cross-correlation between temperature and polarization on scales $`100<l<200`$ is also the result of phase coherence, as we will shortly see, and the scales involved were not within the horizon at recombination. So there is no causal mechanism that could have produced this anti-correlation: we must appeal to inflation to understand it.

To understand why the temperature and polarization are anti-correlated on scales of order a degree, we first must establish that polarization results from Compton scattering of a radiation field with a quadrupole moment. To see this consider Fig. 7 which depicts incoming radiation in the $`z=0`$ plane and shows the polarization of the outgoing radiation along the positive $`z`$-axis. Since the radiation has a quadrupole, incoming radiation along the $`x`$-axis is hotter than that along the $`y`$\- axis. Only the $`y`$-component of the polarization of the incoming $`x`$-ray gets transmitted (the $`z`$-component is parallel to the outgoing direction, and polarization is transverse to the direction of propagation) and only the $`x`$-component of the incoming $`y`$-ray gets transmitted. Hence the outgoing $`x`$-component is cooler than the outgoing $`y`$-component. A quadrupole in an unpolarized radiation field produces polarized radiation after Compton scattering.

Therefore, the polarization today should be proportional to the quadrupole at the time of recombination. The photons just before recombination are tightly coupled to the electrons. This tight coupling tends to suppress the quadrupole. Consider an observer measuring incoming photons, and for simplicity assume there is only a single plane wave perturbation. When the observer looks perpendicular to the direction along which the density is varying, he sees no perturbation. When he measures along this direction, he measures a Doppler shift, which can be Taylor expanded as

$$\frac{\delta T}{T}=v+v^{}\lambda _{\mathrm{mfp}}$$
(3)
where $`v`$ is the electron velocity; $`v^{}`$ its spatial derivative which is of order $`v/\lambda `$ with $`\lambda `$ the wavelength of the perturbation; and $`\lambda _{\mathrm{mfp}}`$ the distance the photon has traveled since it last scattered, the mean free path. The first term here represents the dipole seen by our hypothetical observer, the second the quadrupole. Hence the quadrupole is proportional to $`v\lambda _{\mathrm{mfp}}/\lambda `$. The quadrupole then is proportional to the electron velocity. The dipole of the radiation is equal to the electron velocity, so the quadrupole is proportional to the dipole right before recombination. The proportionality constant is small, since $`\lambda _{\mathrm{mfp}}`$ is much smaller than the typical wavelength. Collecting these arguments, we expect

$$PD\frac{\lambda _{\mathrm{mfp}}}{\lambda }$$
(4)
where $`P`$ is the polarization and $`D`$ the dipole. Incidentally, this explains why measurements of polarization have lagged behind those of temperature anisotropies: the polarization signal is a factor of ten smaller due to the $`\lambda _{\mathrm{mfp}}/\lambda `$ suppression.

The polarization of the CMB today then is determined by the dipole at recombination. The temperature anisotropies on the other hand are determined by the monopole at recombination444The monopole is what normally thinks of when speaking of the temperature in a given spot. It is the average temperature of all photons hitting that spot coming from all directions.. The cross-correlation between the temperature anisotropy and the polarization anisotropy then is proportional to the cross-correlation of the monopole and dipole at recombination. How is the monopole related to the dipole at recombination? We can answer this simply by recalling the continuity equation:

$$\frac{\rho }{t}+(\rho 𝐯)=0.$$
(5)
The velocity then (or equivalently the dipole) is proportional to $`\dot{\rho }`$, the time derivative of the monopole. This is shown explicitly in Fig. 8. At recombination, this phase difference causes the product of the two to be negative for $`100<l<200`$ and positive on smaller scales until $`l400`$. But this is precisely what WMAP has observed! We have clear evidence that monopole and dipole were out of phase with each other at recombination.

This evidence is exciting for the small scale modes ($`l>200`$). Just as the acoustic peaks bear testimony to coherent phases, the cross-correlation of polarization and temperature speaks to the coherence of the dipole as well. It solidifies our picture of the plasma at recombination. The evidence from the larger scale modes ($`l<200`$) though is positively stupendous. For, these modes were not within the horizon at recombination. So the only way they could have their phases aligned is if some primordial mechanism did the job, when they were in causal contact. Inflation is just such a mechanism.

## 5 Cosmological Parameters

I hope I have convinced you that we now have very good reason to believe in the basic framework of inflation as the seed of structure in the universe. Once we assume this framework, we can go ahead and determine the free parameters in the model. The first and most renowned is that the first peak appears where it should if the universe is flat, so let’s assume that the universe is flat. Three of the easiest parameters to measure then are the baryon density $`\mathrm{\Omega }_b`$, the matter density $`\mathrm{\Omega }_m`$, and the Hubble constant $`h`$. Actually, as indicated in Fig. 9, the CMB anisotropies are most sensitive to combinations of these parameters.

Here is a rough guide to the sensitivity of the anisotropies to these three cosmological parameters mc .

* Baryon density $`\mathrm{\Omega }_bh^2`$. The sound speed in Eq. (2) goes down as more baryons are added. The frequency of oscillation thus becomes smaller as the baryon density goes up. A reduced frequency accentuates the effectiveness of the driving force, making the oscillation more asymmetric. The result is that the height of the second peak is much smaller than the height of the first peak when the baryon density is high.
* Matter density $`\mathrm{\Omega }_mh^2`$. If there is a lot of radiation at recombination, the gravitational potential changes with time, inducing a larger driving force and hence boosting anisotropies.
* Cosmological constant $`\mathrm{\Omega }_\mathrm{\Lambda }`$. The cosmological constant555In a flat universe with constant $`\mathrm{\Omega }_mh^2`$ and $`\mathrm{\Omega }_bh^2`$, reducing $`\mathrm{\Omega }_\mathrm{\Lambda }`$ is equivalent to raising one of the other $`\mathrm{\Omega }`$’s and reducing the Hubble constant $`h`$ to keep the products $`\mathrm{\Omega }_ih^2`$ fixed. is a late time effect, so the only impression it leaves on the CMB relates to the way physical scales project onto angular scales; i.e. $`\mathrm{\Omega }_\mathrm{\Lambda }`$ changes the distance to the last scattering surface, so the curves simply shift horizontally if $`\mathrm{\Omega }_\mathrm{\Lambda }`$ changes.

The results from WMAP spergel  are shown in Fig. 10. We get a sense that the CMB has reduced parameter uncertainties by close to a factor of ten. And this improvement allows us to make several remarkable statements about our universe, based solely on observations of the CMB. First, if one assumes the universe is exactly flat, then the CMB tells us that Hubble constant is $`h=0.72\pm 0.05`$, in remarkable agreement with direct determinations wendy . The ratio of the total matter density to the baryonic density is about $`6\pm 1`$, which means the CMB alone requires significant non-baryonic dark matter. Finally, $`\mathrm{\Omega }_\mathrm{\Lambda }=1\mathrm{\Omega }_m`$ is equal to $`0.71\pm 0.07`$. The CMB, together with the flatness assumption, requires a cosmological constant, or some form of dark energy. No wonder parameter determination has received so much publicity!

## 6 Alternatives

It is perhaps not surprising that, as the evidence for inflation has firmed up, theoreticians have been working harder than ever to find alternatives to inflation. Here I want to focus on the question of what alternatives are viable in light of the coherent phase argument.

It is instructive to start with two models that don’t quite make it. The first is the well-known class of models with structure seeded by topological defects. The phases of the Fourier modes are not synchronized in defect models, so we do not expect a coherent series of peaks and troughs. This elegant argument was first first advanced by Albrecht et al. andy  as a way of distinguishing defect models from inflation and later confirmed in detailed numerical studies allen ; pst .

A second alternative has recently been proposed by Armendariz-Picon and Lim lim . They note that inflation works by producing perturbations when the modes of interest are sub-horizon and then driving these modes to be larger than the horizon. Once outside the horizon, the perturbations freeze-out, i.e. remain constant, until they re-enter the horizon much later around the time of recombination. They point out that really perturbations freeze out once they leave the sound horizon horizon ($`c_s/H`$ instead of $`H^1`$). Thus instead of the Hubble rate remaining roughly constant (as during inflation wherein $`c_s=1`$), freeze-out can also be accomplished if the sound speed drops rapidly. This is a clever idea, one that might ultimately be part of a viable alternative. At present though, it doesn’t quite work, because – as they point out – inflation is still needed (after perturbation production) to drive the scale beyond the horizon666However, the since scale-invariant perturbations have already been generated, the requirements on inflation are less severe than usual.. Another way of saying this is to notice that if not for inflation, the modes of interest would never have been sub-horizon, so nothing could have been effective in producing perturbations.

Indeed, the most basic requirement for coherent phases is that at some point is the distant past (well before recombination), the modes of interest had to be within the horizon. So, the coherent phases requirement is simply a strengthened version of the classical horizon problem. With that in mind, I come to a final class of alternatives which generate perturbations in a variety of ways, but all share the same innovative approach to the horizon problem.

One way to think of the horizon problem is in term of the comoving grid, wherein the wavenumber of any mode remains constant with time. The comoving Hubble radius is $`(aH)^1`$, which typically increases with time. The classical horizon problem is that, since the comoving Hubble radius monotonically increases in the standard cosmology, these modes must have all been outside the horizon before recombination. The inflationary solution is depicted in Fig. 11, which shows that the necessary requirement is that $`aH`$ must have increased sometime in the past. Mathematically then we would seem to require

$$\frac{d}{dt}\left(aH\right)=\frac{d^2a}{dt^2}>0$$
(6)
at some point in the distant past. That is, we seem to require inflation (which can be defined as a period in which $`\ddot{a}>0`$). The alternative models alternate  however evade this constraint by using a contracting phase. The requirement that the comoving radius decrease now is $`d[aH]/dt>0`$ (since the Hubble radius is $`H^1`$) or $`\ddot{a}<0`$. So the horizon problem can be solved and the necessary coherent phases generated if: (i) the universe accelerates while it is expanding (inflation) OR (ii) the universe decelerates while it is contracting.

These alternatives and others are honing in on the question of what we have really learned from the observations. That is, it is no longer sufficient to solve the classical horizon problem. While the scales of interest are sub-horizon, a mechanism is needed to generate perturbations with the proper amplitude and shape and to drive these perturbations beyond the horizon so they freeze out.

## 7 Conclusions

Detailed observations of the CMB have solidified our confidence in a model of structure formation based on inflation. The most striking evidence for inflation is the phase coherence of the primordial perturbations, which manifests itself in the peaks and troughs of the temperature anisotropies and in the cross-correlation between the temperature and the polarization. Once this framework has been accepted, it is possible to use it and extract cosmological parameters. This parameter estimation suggests that: the universe is flat; there is non-baryonic dark matter; and dark energy dominates the energy budget.

As the observations have improved, theorists have expanded the range of models which can account for them. and proposed new alternatives to inflation. The exciting development is that these alternatives must solve a much more demanding version of the horizon problem. And we are learning more about what precisely is necessary to generate the coherent phases we have so unambiguously observed.

This work was supported by the DOE, by NASA Grant NAG5-10842, and by NSF Grant PHY-0079251. I would also like to thank the organizers of the Fourth Tropical Workshop on Particle Physics and Cosmology: R. Volkas, S. Tovey, C. N. Leung, and J. Nieves.


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# CMS BARREL RESISTIVE PLATE CHAMBERS - TESTS AND RESULTS

## 1 Introduction

CMS (Compact Muon Solenoid) is a general purpose detector for the new coming LHC accelerator at CERN. Detailed description of CMS can be found elsewhere .
RPCs  are gaseous parallel-plate detectors with time resolution comparable to that of scintillators ($``$ 1 ns) and good spatial resolution ($``$ cm).
An RPC single gap consists of two parallel plates made of Bakelite and is filled with gas. The outer Bakelite surfaces are coated with graphite to form HV and ground electrodes. Two single gaps glued together form the double gap structure. The copper read-out strips are situated between the single gaps and are separated from the graphite coating by an insulating film.
A charged particle passing through an RPC initiates an electron avalanche due to ionisation in the applied electric field. The drift of electrons towards the anode induces a “fast” charge (signal) on the pick-up electrode. The developed more complex front-end electronics  allows to operate the RPCs in avalanche mode .
To increase the signal (at a fixed voltage) or to reduce the voltage (at a fixed signal), double gap design is implemented by CMS (two gas gaps are mechanically assembled together in one parallel double gap structure with common read-out strips) , .
Prototype RPCs have already been build and successfully tested , . The results presented in this paper refers to double gaps design.

## 2 Test Set-Up

The first 24 RPCs were tested using cosmic muons in Bari. The test set-up consists of the following systems:
Trigger System. The RPCs are situated between two upper and two lower large trigger scintillators. The trigger signal is formed by taking the logical “AND” of the four large scintillators. Two additional small “veto” scintillators are used in order to suppress the contribution from electromagnetic avalanches. The chambers under tests have two double gaps (“forward” and “backward”) which are tested separately.
HV System. Chamber’s up and down single gaps are supplied separately.
DAQ System. The front-end boards accepts signals from the chamber electrodes and after amplification and discrimination forms a LVDS signal for every strip. RPC signals are read-out at a fixed frequency of 40 MHz and are stored in a temporary memory. When the trigger arrives the information is passed to the PC for further processing.
Gas System. The gas system allow as to use up to four component gas mixture.

## 3 RPC tests and results

The efficiency, cluster size, noise rate and electric current were measured for different voltages in the range 9.0 - 9.8 kV. The chamber front-end electronics threshold was fixed during the tests to accept the charge above 125 fC. Temperature and atmospheric pressure corrections have been made. Freon-based gas mixture has been used (96.2% $`C_2`$$`H_2`$$`F_4`$, 3.5% i-$`C_4`$$`H_{10}`$, 0.3% i-S$`F_6`$).
Efficiency. The efficiency is defined as a ratio between the RPC responses (at least one fired strip) and the number of recorded triggers, with correction for spurious hits. All chambers have achieved desired efficiency of 95% and above (fig. 1). Long and stable efficiency plateaus are observed.
Cluster size. Cluster size is defined as the number of simultaneously fired adjacent strips. The average cluster size for the voltages in the range 9.4-9.6 kV is between 1.5 and 3 (fig. 1). This is higher than expected, but is still acceptable. The cluster size can be reduced by changing the front-end electronics thresholds to optimal value.
Noise rate. Noise rate is defined as the total chamber noise normalised to its active surface. A noise rate of up to 10 Hz/$`cm^2`$ is considered acceptable within the detector specifications. However, the test results show an even improved noise rate of less than 5 Hz/$`cm^2`$, (fig. 1). Only one chamber has unacceptable noise rate (CH 9) and will be reassembled.

## 4 Conclusions

The first 24 RPC chambers for muon station RB3 were produced and tested. All of them reach the desired high efficiency (above 95%). The cluster size and noise rate at high voltages 9.4-9.6 kV fully satisfy CMS requirements (except CH 9).


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# Metastable level lifetimes from electron-shelving measurements with ion clouds and single ions

## I Introduction

High-precision atomic lifetime measurements are a challenge for experimental and theoretical atomic physics. Increasing volume and precision of astrophysical observations have generated a growing need for precise atomic lifetime data Traebert (2000). Among all the interesting atomic systems, atoms with a closed inner shell and a single additional valence electron offer the possibility to accurately compare the results of atomic data modeling and experimental values.

There have been various theoretical approaches to the low-lying metastable doublet levels of 40Ca+ which have generated somewhat dispersed metastable lifetime predictions Osterbrock (1951); Warner (1968); Ali and Kim (1988); Zeippen (1990); Guet and Johnson (1991); Vaeck et al. (1992); Brage et al. (1993); Liaw (1995); Biemont and Zeippen (1996). In the past decade the lifetimes of the metastable D-levels of the singly-ionized calcium have also been measured several times Urabe et al. (1992); Arbes et al. (1993); Urabe et al. (1993); Arbes et al. (1994); Knoop et al. (1995); Gudjons et al. (1996); Ritter and Eichmann (1997); Block et al. (1999); Lidberg et al. (1999); Barton et al. (2000); Staanum et al. (2003). Most of these measurements have been carried out in rf traps, showing a clear evolution towards longer lifetimes throughout the years, as error sources have been identified. In particular, before 1999, the coupling of the metastable D-levels to the P-state due to off-resonant excitation by the repumper laser Block et al. (1999), had not been taken into account at all. As will be shown in this paper, ion-ion collisions in a relative hot and dense ion cloud ($`k_BT1eV`$, $`n10^8cm^3`$) may also contribute a few percent to the lifetime reduction. These two effects explain the gap between the earlier ion-cloud measurements and recent single-ion measurements. The experiments which have been carried out on single laser-cooled ions show a typical error bar of the order of 2%, with the exception of one experiment Barton et al. (2000), where the announced uncertainty is inferior to 0.6% and which gives the highest value ever measured for the $`3D_{5/2}`$-lifetime. In this article, we present our new measurements of the lifetime of the $`3D_{5/2}`$-state which have been carried out in a different way. In fact, we achieve population of the metastable level by direct pumping of the electric quadrupole transition which connects the ground state to the $`3D_{5/2}`$-state. We have also been able to establish a connection between the different published values, the discrepancy being mainly due to differing data analysis.

Single trapped ions are now extensively used for metrology and quantum information Gill (2002). Storage times can exceed days, and the control of the trapping environment along with the degree of laser stabilization have been improved to access linewidths of optical transitions down to the Hz-level Rafac et al. (2000). Our experimental project aims to propose a frequency standard in the optical domain, based on the interrogation of the $`4S_{1/2}3D_{5/2}`$ electric quadrupole transition of a single laser-cooled Ca+-ion. The measurement of the metastable $`3D_{5/2}`$-level lifetime is an important step in this direction, allowing to identify and to control effects which may reduce this lifetime, and which could thus contribute to the broadening of the clock transition.

In this paper, we briefly present our experimental device, and introduce the technique we have used to measure metastable lifetimes in ion clouds and single ions. We then present the different data processing methods. The fourth part of this article is devoted to the discussion of the uncertainties of our measurements. We finally present and discuss our results in the context of previous experiments.

## II Experimental Setup

We use a miniature ion trap to confine single ions and ion clouds up to approximately 500 particles. The trap is a modified Paul trap, a so-called Paul-Straubel trap Schrama et al. (1993) consisting of a cylindrical molybdenum ring with an inner diameter of $`2r_0=1.4`$ mm and a total ring height of $`2z_1=0.85`$ mm (Figure 1). Two circular mesh electrodes at 5.5 mm on each side from the trap center, allow the definition of well controlled electrical boundary conditions. Two copper tip electrodes in the plane of the trapping ring are used as positioning electrodes to correct for imperfections and asymmetries in the trapping potential and thus to reduce the micromotion of the confined ions. The applied trapping frequency $`\mathrm{\Omega }/2\pi =11.6`$ MHz with an rf voltage amplitude of 300 V, gives rise to a total pseudo-potential well depth of $`1.9`$ eV and motional frequencies around $`\omega _i/2\pi =1.5`$ MHz. The trap has been fully characterized and is described in detail in Champenois et al. (2001). The trapping setup is mounted into an ultra-high vacuum vessel and baked out at $`150^{}`$C during a couple of days. Vacuum conditions can be controlled by the ion pump current, a Bayard-Alpert gauge and a mass spectrometer operating up to 64 a.m.u.. Ions in the trap are created from a calcium oven heated by a direct current of 3 A. The effusive atom beam is crossed with a low-energy electron beam in the center of the trap producing singly-ionized calcium ions.

Laser-cooling is carried out on the $`4S_{1/2}4P_{1/2}`$ electric dipole transition at 397 nm using an intracavity frequency-doubled TiSa-laser \[Coherent 899\]. The output intensity of this laser is stabilized by a single-pass acousto-optical modulator (AOM), the error signal is fed back from a beam pick-up photodiode after crossing the trap. The optical power used for laser-cooling is about 50 $`\mu `$W in the case of an ion cloud, and an order of magnitude lower for a single ion, focussed in a 20$`\mu `$m-diameter waist (measured at 1/e2 power level). The linewidth of this laser has been found to be below 10 MHz in the course of our experiments. Due to a branching ratio to the $`3D_{3/2}`$-level larger than 5%, repumping from this level is required, and is assured by a single-mode diode laser at 866 nm mounted in a Littrow-configuration external cavity (ECDL). This diode laser is stabilized to a low finesse ($``$=200) reference cavity reducing its linewidth to about 1 MHz and improving its frequency stability. Stable operation during a whole day is achieved by locking the length of the reference cavity to a hyperfine transition of neutral caesium making use of an additional ECDL at 852 nm and a standard saturated-absorption setup. Typical power for the 866 nm-diode is about 200 $`\mu `$W focussed into a 70 $`\mu `$m-diameter waist. A broad-area laser diode is used to probe the electric quadrupole transition $`4S_{1/2}3D_{5/2}`$ at 729 nm . The nominal output power of this laser diode is 100 mW and its free-running linewidth is as large as 2 nm. This diode has been set up in an external cavity in Littrow configuration and pre-stabilized by electronic feedback onto a low-finesse reference cavity ($``$=200) . We thus obtain a laser linewidth in the MHz-range and a laser intensity of approximately 350 $`\mu `$W per 60 $`\mu `$m-diameter waist size in the trap Houssin et al. (2003).

Two mechanical shutters in the 729 nm-beam line allow to cut the light from this laser completely. Their closing time is in the ms-range, inferior to the smallest measurement interval used throughout the experiment. All the laser beams used in this experiment are brought to the ion trap by single-mode optical fibers. This ensures the spatial filtering of the laser beams and gives rise to well controlled waist sizes at the position of the ion. However, the main advantage of these fibers is to increase the pointing stability of the laser beams, which improves the day-to-day reproducibility of the measurements essential for trapping single ions.

Detection of the fluorescence of the ions at 397 nm is made outside the vacuum vessel (Figure 1). The fluorescence signal is spatially filtered by a small diaphragm (diameter below 500 $`\mu `$m) and then projected onto an intensified CCD camera (ICCD) and a photomultiplier (PM) in photon counting mode. A variable beamsplitter between these two devices allows to choose the fraction of signal sent to the photomultiplier between 10 and 100 %. The maximum fluorescence count is about 10000 counts/sec for a single ion. Data is collected and stored by a personal computer, that also controls the ion creation process and actuates the laser shutters. Excellent temporal synchronization is assured by buffer-controlled read-out on the data acquisition board. The typical duration of a measurement bin is 50 ms for the ion cloud measurements and 30 ms for the single-ion measurements.

## III electron shelving

All our lifetime measurements have been performed in the same trap, in a very similar way for a small ion cloud or a single ion. In both cases, ions have been laser-cooled on the strong $`4S_{1/2}4P_{1/2}`$ electric dipole transition and detected by the scattered 397 nm-photons. We have used the technique of electron-shelving proposed by H.G. Dehmelt Dehmelt (1975) for the whole set of measurements. This method allows to observe transitions on the forbidden electric quadrupole line via the switching of the strong laser-cooling transition at 397 nm. In our experiment the $`3D_{5/2}`$-state has been populated by direct optical pumping of the dipole-forbidden $`4S_{1/2}3D_{5/2}`$ transition, technique which has not yet been applied in the lifetime measurements with single trapped Ca+-ions. The direct excitation of this electric quadrupole transition allows an unambiguous definition of initial conditions.

### III.1  measurements in an ion cloud

A typical ion cloud contains 50 to 100 Ca+-ions which are laser-cooled to a temperature of about 50 K, temperature which is defined as a measure of the kinetic energy of the trapped particles. This temperature value stands for an equilibrium between the heating of the ions by the trapping field and the laser-cooling.

To measure the $`3D_{5/2}`$-level lifetime in an ion cloud we use approximately 350 $`\mu `$W of 729 nm-power. Once the resonant laser beam is admitted onto the ions, a fraction of the ions is pumped into the $`3D_{5/2}`$-state and the observed fluorescence signal at 397 nm decreases. The experimental signal is shown in figure 2. When the population of the $`3D_{5/2}`$-state has reached an equilibrium state which is represented by a constant fluorescence level, we shut off the 729 nm diode laser. The ion population then decays to the ground state with a time constant governed by the $`3D_{5/2}`$-state natural lifetime. This decay can be observed on the 397 nm fluorescence signal as the decaying ions return into the laser-cooling cycle and scatter blue photons. The revival function of the 397 nm fluorescence is fitted with a least-squares method (LSF) by the function $`F(t)=S_0+S(1exp(t/\tau _m))`$ where $`\tau _m`$ is the measured lifetime for a given set of experimental parameters, $`S`$ the net ion signal and $`S_0`$ the low-level signal being composed by the fluorescence signal of the ions remaining in the laser-cooling cycle and the background signal due to stray light. Actually, the measured lifetime $`\tau _m`$ is the natural lifetime of the $`3D_{5/2}`$-level affected by different de-shelving effects as will be discussed in section IV. The result for the measured lifetime in an ion cloud is $`\tau _{nat}=1095`$ ms with an 1$`\sigma `$-statistical uncertainty of 7.5 ms.

We have made simulations in an ion cloud of the population of all the atomic levels involved ($`S_{1/2}`$, $`P_{1/2}`$, $`D_{3/2}`$, $`D_{5/2}`$) with the use of the density matrix formalism taking into account the ion motion in the trap. The oscillatory movement of the ion cloud is described by a distribution of the velocity amplitudes at a single frequency Schubert et al. (1989). In this coupled four-level system, the fraction of ions which are pumped into the metastable $`D_{5/2}`$-state depends on the relative detuning of the three lasers used for cooling, repumping and probing of the clock transition, a phenomenon comparable to the occurrence of dark resonances. The simulation shows, that it is possible to pump almost the entire ion population into the metastable state if the ions are nearly at rest Champenois et al. (2004). The second parameter which is critical for the reproduction of the shelving curves is of course the laser power. The lines in figure 2 visualize the simulated fluorescence curves for a cloud of 50 ions with a temperature of 100 K, assuming that the fluorescence is directly proportional to the $`P_{1/2}`$-population. In the plotted simulations the relative laser detuning has been fixed while the power levels of the probing laser at 729 nm are varied. The right choice of relative laser detunings and absolute laser power levels enables us to reproduce accurately both the speed of the decrease of the fluorescence as ions leave the laser cooling cycle (t=4-9 sec) and the fraction of the ions being pumped into the $`D_{5/2}`$-level. As a matter of course, the revival of the fluorescence depends only on the lifetime of the 3$`D_{5/2}`$-state for the given set of experimental parameters.

### III.2  measurements with a single ion

Experiments with single ions have been carried out during twelve 6h-runs with single ions laser-cooled to temperatures below 1K. As the temperature of the ion is estimated from the asymmetric Doppler profile which is largely depending on the optical power used for laser-cooling, this value is an upper limit to the estimate of the kinetic energy.

When the electron-shelving technique is applied to a single ion, the observed fluorescence signal becomes binary. Actually, while the ion is in the laser-cooling cycle, a large number of blue photons is scattered giving rise to a high photon count rate (”bright” level), see figure 3. When the 729 nm laser diode is admitted onto the ion, it will be pumped into the $`3D_{5/2}`$-level. The fluorescence rate at 397 nm will then abruptly fall to the low level, which corresponds to the background light (”dark” level). As soon as we detect a ”dark” level signal, the 729-nm laser is shut off to avoid any coupling between the levels, as discussed in detail in section IV. The sudden changes in fluorescence due to transitions between atomic levels are called quantum jumps. Figure 3 shows the good distinction between the bright and the dark level. This allows to define an unambiguous threshold value for the determination of the duration of the quantum jumps. Typically, we have set the threshold value at the half of the net signal value, which is the difference between the mean upper trace and the mean lower trace. The timebase of the data acquisition has been chosen to give a maximum separation of bright and dark level together with best temporal resolution. Thus, variation of the threshold value separating dark and bright level between one third and two third of the net signal did not result in variations of the quantum jump length distribution.

The duration of the dark intervals have been processed by two different methods. First, they have been binned in a histogram and fitted by a least-squares method (LSF) using an exponential decay curve ($`F(t)=Aexp(t/\tau _m)`$) with two free parameters (A and $`\tau _m`$) at a 95% confidence level (figure 4). Taking into account the de-shelving by the 866 nm-diode as discussed in section IV, the obtained lifetime value is $`\tau _{nat}`$ = 1088 ms with a fitting uncertainty of 15 ms. This fitting procedure assumes that the measured number of events for each bin spreads around the fitted equation with a Gaussian probability distribution. Actually, the probability of very long events is in most cases very low (see figure 4), suggesting that deviations from the mean are not governed by a Gaussian distribution. It is then appropriate to apply the most general evaluation method, assuming a multinomial distribution, and calculating the lifetime by a maximum likelihood estimate (MLE). Recent measurements Barton et al. (2000); Staanum et al. (2003) have evaluated the metastable lifetime by using the method of the MLE obtaining values larger than 1150 ms. We have used the following formula Staanum et al. (2003) to calculate the lifetime by

$$\tau _m=\frac{\mathrm{\Delta }t}{ln(1+\frac{\mathrm{\Delta }t}{\overline{t}})},with\overline{t}=\frac{1}{N}\underset{i=1}{\overset{N}{}}n_it_i$$
(1)
where $`\mathrm{\Delta }t`$ is the bin size of the histogram, $`\overline{t}`$ is the mean value of the $`n_i`$ measured dark intervals of duration $`t_i`$, and $`N`$ is the total number of measured events. The statistical uncertainty for each data set can be exactly computed by

$$\sigma =\sqrt{\frac{\tau ^2}{N}\left[1+\frac{1}{12}\left(\frac{\mathrm{\Delta }t}{\tau }\right)^2+𝒪\left(\frac{\mathrm{\Delta }t}{\tau }\right)\right]}$$
(2)
Depending on the number of quantum jumps per run, the statistical uncertainty has been found to be below 3%. Extrapolation to zero 866nm-intensity gives a value for the natural lifetime of $`\tau _{nat}`$ = 1152 ms, with a fitting uncertainty of 19 ms, which is discussed in section IV.2.

To determine the appropriate method for the evaluation of the quantum jump data, we have simulated quantum jump events using the Monte-Carlo method, governed by a fixed input lifetime $`\tau _{in}`$ and with the same time base as in our experiment. These quantum jump lengths have been allotted randomly in files of different size starting at about 500 quantum jumps up to about 100 000. Each file has been processed by a least-squares fit to an exponential decay curve of the histogram of durations and by the maximum-likelihood estimate for the whole data set. The two data processing methods have been carried out in a totally identical way to the treatment of the experimental data. The obtained values are plotted in figure 5 as a function of the number of quantum jump events contained in the processed file. As can be seen, LSF data are more widely scattered around the input lifetime of the simulation. At about 10000 events the scattering of the MLE data is roughly a factor of three smaller than for LSF, values for both methods converge on a 2%-level only for runs with more than 40000 valid quantum jumps. Actually, the MLE method is well known in mathematics as a precise unbiased estimator, it reaches asymptotically the Cramér-Rao bound which describes the best attainable error Kendall (1961). In general, as the average time needed to record one quantum jump is of the order of two or three seconds including the preparation time, a few-hour run of data acquisition yields several thousands quantum jumps. In this range the difference between both methods may easily reach 10% of the absolute values, the 5.5%-discrepancy of our experimental results largely fits into this window. In summary, the number of quantum jump events we acquire in the course of a one-day run, imposes the use of MLE to reach minimum statistical uncertainties.

## IV Evaluation of uncertainties

Among the uncertainties on the measured lifetimes of the metastable $`3D_{5/2}`$-level of Ca+ we distinguish between the ones which are due to physical effects which may affect the apparent lifetime of the state and those due to data analysis.

### IV.1 De-shelving effects

The lifetimes we measure in the course of our experiments are function of the experimental parameters as various physical effects tend to shorten the observed lifetimes. The major de-shelving effects are collisions with the residual gas, heating or loss of the ions, and coupling of the atomic levels by laser light. The measured lifetime $`\tau _m`$ can therefore be expressed as

$$\frac{1}{\tau _m}=\frac{1}{\tau _{nat}}+n_B(\mathrm{\Gamma }_{quench}+\mathrm{\Gamma }_{mix})+\gamma _{heat}+\gamma _{loss}+\gamma _{coupling}.$$
(3)
with $`n_B`$ the residual particle density in the trapping device. We will discuss the influence of these de-shelving effects in detail in the following, their quantitative influence on the measured lifetimes is summarized in table 1.

We have looked for an eventual effect of the trapping potential and of the detuning of the 397 nm laser. Both parameters could influence the temperature of the trapped ions and eventually give rise to an increased amount of collisions. Nevertheless, we could not evidence any variation of the measured lifetime in the limit of the announced error bars.

#### IV.1.1 Collisional effects

The apparent lifetime of the metastable state can be reduced by inelastic collisions with (neutral) particles from the residual gas background. The base pressure of the ultra-high vacuum vessel is below $`5\times 10^{10}`$ mbar as measured by the ion pump current and the two gauges. From our previous measures of quenching and j-mixing reaction rates in hot ion clouds Knoop et al. (1995, 1998) and from the measured composition of the residual gas background by the mass spectrometer, we can deduce that the only non-negligible component giving rise to inelastic collisions is hydrogen. In fact, the partial hydrogen pressure for ion cloud experiments is inferior to $`2\times 10^9`$ mbar, and below the resolution of the mass spectrometer ($`1\times 10^9`$ mbar) for single ion experiments. The difference in the pressure values for both types of experiments is due to the duration and frequency of the ion creation process.

For the ion cloud experiments the residual hydrogen pressure results in a value of $`n_B\mathrm{\Gamma }_{quench}(1.8\pm 0.7)\times 10^3`$ s-1 due to quenching while the contribution of the fine-structure mixing collisions is $`n_B\mathrm{\Gamma }_{mix}(14\pm 10)\times 10^3`$ s-1.

The observation of quantum jumps in a single ion allows the direct measurement of the collision rate in the absence of the 729-nm laser. Every once in a while, the ion undergoes a quantum jump due to an inelastic collision with a particle from the residual gas. We have recorded these quantum jumps which are the result of collisional transfer between the fine-structure levels and from the ground-state. At a base pressure of $`2\times 10^{10}`$ mbar we have measured an average of 1 quantum jump every 5 minutes resulting in a collision rate of $`n_B\mathrm{\Gamma }_{coll}3\times 10^3`$ s-1.

#### IV.1.2 Ion heating

Temperature changes in the ion cloud could play a role in the determination of lifetimes due to changing collision rates and to varying frequency overlap (and therefore varying excitation efficiency) between the ions and the applied lasers. In the ion cloud experiments we have adjusted the 729-nm laser power to make sure that not more than one half of the ion cloud is pumped into the metastable state. As the laser-cooling is permanently applied to the rest of the ion cloud, sympathetic cooling of the dark ions prevents these from heating Larson et al. (1986). We can yet estimate the influence of ion heating from the signal variations at fixed laser frequencies, the upper limit is $`\gamma _{heat}1\times 10^3`$ s-1.

As for the single ions, heating becomes visible if the laser-cooling parameters (mainly the frequency and the power of the 397-nm laser) are largely detuned. After a dark interval the ion will then slowly return to the ”bright” fluorescence level over several measurement bins. In our lifetime measurements, we have made sure that the laser-cooling parameters are optimized and that the ion signal returns to the upper fluorescence trace in a time shorter than one measurement bin (30 ms), even for dark times which are superior to 10 seconds. Moreover, to ensure efficient cooling of the ion, we maintain it in the laser-cooling cycle for at least 600 ms before the 729 nm laser is again admitted to the trap.

#### IV.1.3 Ion loss

The revival function of the fluorescence in the ion cloud could be biased by competing decay processes, in particular ion loss. Ion loss is not visible on a single revival function but it will be detectable on the over-all fluorescence signal after a one-hour run. The upper limit for the influence of ion loss on the lifetime measurements in an ion cloud is given by $`\gamma _{loss}<7\times 10^3`$ s-1.

If the ion is lost, while we are observing quantum jumps, we have to reload a new ion. To make sure, that the vacuum conditions are identical throughout the whole set of experiments, we wait for about half an hour before we restart data acquisition.

#### IV.1.4 Level coupling by laser light

All the laser beams used in this experiment may couple the different atomic levels due to the Stark effect induced by their electromagnetic field. However, atomic level coupling by the 397 nm laser is negligible in our experiment, laser power at this wavelength being around 50 $`\mu `$W for an ion cloud and below 10 $`\mu `$W for the experiments with a single ion.

##### 729 nm

One important factor for the reduction of the metastable lifetime is coupling by the 729-nm laser. In fact, even at low laser powers, this radiation may induce transitions to the ground state by stimulated emission on the $`4S_{1/2}3D_{5/2}`$ line. We have taken precautions to avoid any coupling by this laser.

In any case we have to shut off the laser by a mechanical shutter in front of the trap for the observation of the revival function in the ion cloud measurements. The applied power at 729 nm is measured by a beam pick-up photodiode at the entrance of the trap. The instant when the power falls to zero is used to fix the starting point for the fit of the revival function.

In the single ion experiments complete extinction of the laser at 729 nm is essential to avoid reduction of the length of the dark intervals. We use a system of two synchronized mechanical shutters, one at the entrance of the optical fiber and one at its output, to guarantee maximum isolation from this radiation. When both shutters are closed, the 729-nm light level is inferior to the detection limit. For the excitation of quantum jumps, the 729-nm laser is applied to the laser-cooled ion, when the fluorescence level falls below threshold, the shutters are immediately closed. During the first measurement bins the 729-nm radiation is thus still present in the trap and we have to remove these earliest points to make sure that the decay conditions are well defined. In our evaluation of the distribution of the quantum jumps, we use data starting only at the fifth bin, which means that we do not take into account the first 120 ms of a quantum jump, and that quantum jumps whose duration is equal or inferior to that value are completely omitted. As a consequence, low-signal bins due to noise, which are typically of the length of one bin are also eliminated.

##### 866 nm

The main effect which reduces the lifetime of the metastable state is the coupling by the repumper laser at 866 nm Block et al. (1999), which is necessary for laser-cooling. We insist on this point, as this ”helper” laser is often applied with optical power levels largely beyond saturation to compensate for spatial and spectral instabilities.

The determination of the laser intensities seen by the ions is difficult to realize with high precision. On the one hand, absolute calibration of a power meter is in general not constant in time. More delicate still is the measure of the waist size in the ultrahigh-vacuum vessel. We have measured the waist sizes on different days by a commercial instrument (Melles Griot BeamAlyzer) just in front of the entrance of the trap by deviation with a high-quality mirror. This measurement is just an estimate of the waist dimension, as the position and shape of the focal point after the vacuum windows are certainly distorted. Additionally, the trajectory of the ion may be smaller than the waist of the laser. As a consequence, the error bar on the laser intensity seen by a single ion is difficult to estimate and may easily reach 10%, and up to 30 % for very low power levels (below 1$`\mu W`$).

We have checked our lifetime measurements versus the intensity of the repumper laser (see figure 6), observing a reduction of the apparent lifetime of the $`3D_{5/2}`$-level due to the AC Stark effect which couples the $`3D_{5/2}`$\- and $`4P_{3/2}`$-states. Data points are somewhat scattered, due to the finite number of quantum jumps per run (cf section IV.2) and the above discussed uncertainty in the power measurement. The extrapolation to zero is made by a weighted least-squares fit to all the measured data points taking into account errors in both coordinates Press (1988). On a 2$`\sigma `$-scale, all points but one fall into the confidence level limits of the fit. As a matter of fact, the points at lower power levels have a larger intensity error bar, and do thus contribute less than may be expected from the linear representation. The measured lifetime of the ions varies as $`\tau _m^1=\tau _{nat}^1+(3.0\pm 0.6)\times 10^3I`$ where I is the intensity of the laser at 866 nm in mW/mm2, and $`\tau _m`$ and $`\tau _{nat}`$ are the measured and natural lifetimes, respectively. The quantitative dependence of the lifetime on the 866 nm-intensity we have found is of the same order of magnitude as in previous measurements Block et al. (1999); Barton et al. (2000).

### IV.2 Data analysis effects

To determine the $`3D_{5/2}`$-level lifetime from the ion-cloud experiments we fitted more than 1700 revival graphs using a least-squares fitting method. Because we could not evidence any dependence of the lifetime on any experimental parameter, the complete set of decay constants has been taken into account to establish the final value. It has been found for these values that different methods of data analysis gave slightly different results. Actually, the mean value of the fitted time constants is not identical to the fit of the sum of the revival curves. Furthermore, harmonic and geometric mean are not identical. We have simulated shelving data of the ion cloud at a given decay rate having the same Gaussian noise pattern as our experimental data. These generated data are free from experimental bias such as ion loss or laser instabilities. Fitting these data demonstrated the variations from the different evaluation approaches, which could be as large as 1.6 % and forms the major contribution to the total error bar.

For a single ion, the total number of quantum jumps taken into account is superior to 40000. As has been discussed in section III.2 the number of quantum jumps which can be acquired in a one-day run is limited to roughly 10000. For measurement times longer than this, temperature drifts start to play a role in our actual experimental set-up, and ion loss may also occur. For the experimental points in figure 6 the mean quantum jump number per set of experimental parameters is of the order of 4000, giving a statistical uncertainty of about 2-3% per data set. These individual uncertainties together with the uncertainties on the power measurements are then used to weight the data points in the extrapolation of the lifetime values to zero repumper power, resulting in an overall statistical uncertainty of 1.8%.

Table 1 summarizes the quantitative influence of the different effects which define the precision of our measurements. Data analysis effects play a major role in the evaluation of the electron-shelving curves in a small ion cloud, whereas the main error contributions in single-ion measurements come from the limited number of quantum jumps and the estimation of the applied laser intensity independent of the data processing method. The total error bars represent an uncertainty on the measurement of the lifetimes of 2.5% in the case of the ion cloud and 1.5% and 1.8% for the single-ion experiments.

## V Discussion and conclusions

From the described measurements, the natural lifetime of the $`3d^2D_{5/2}`$-level lifetime has been found to be $`\tau _{IC}=(1095\pm 27)`$ ms in an ion cloud and $`\tau _{QJ}=(1152\pm 20)`$ ms in a single ion. These two values are very close, though their 1$`\sigma `$ error bars do not overlap. This discrepancy could be an evidence that ion-ion-collisions in the trap eventually contribute to the reduction of the lifetime. In the laser-cooled ion cloud the particle density of the Ca+-ions is roughly $`10^8cm^3`$. If we suppose an eventual lifetime reduction on the 1%-level, we can estimate the upper limit of the contribution of ion-ion collisions to be $`\mathrm{\Gamma }_{iic}1.2\times 10^{10}`$ cm3s-1.

As has been discussed in section III.2, we consider that the estimation of the lifetime in single ion measurements is optimal when made by the method of maximum likelihood. Nevertheless, we have also evaluated our data by using the least-squares minimization of the exponential fitting curve and have found (1088 $`\pm `$ 16) ms. This value is in very good agreement with experimental values which have been determined in the past by least-squares methods Block et al. (1999); Lidberg et al. (1999) with comparable number of events and probability distributions. One of the causes generating the discrepancy between these earlier values and recent measurements Barton et al. (2000); Staanum et al. (2003) as well as our value $`\tau _{QJ}=(1152\pm 20)`$ ms could thus possibly be the choice of the data processing method, which may account for differences of a couple of percent depending on the number of considered quantum jumps per run.

Figure 7 shows all the measurements and calculations that have been carried out on the Ca+-ion over the last years. A wide variety of theoretical models has been used to calculate the lifetime of the metastable state. If we consider only the more recent publications, the values still span over more than 20% of the average lifetime value. Since 1999, experimental measurements are converging towards a value around 1100 ms. Usually, lifetimes are given with a 1$`\sigma `$ error bar, which corresponds to a poor confidence level. We have plotted the most recent measurements with a $`2\sigma `$ error bar standing for a 95% confidence level (see inset on figure 7). Values obtained in the storage ring Lidberg et al. (1999) suffer from a strong collisional background and thus exhibit the largest error bars. The other values have been obtained on laser-cooled single ions in linear and spherical traps. In the figure, a graphical distinction has been made between values obtained by a least-squares fit of the exponential decay curve or maximum likelihood estimates.

In general, the overlap of the recent experimental results is very good, and in particular, the agreement of our value with the one from the Åarhus group Staanum et al. (2003) is excellent. The all-over precision of the experimental determination of the metastable lifetime measurement is very high, making the Ca+-ion an ideal candidate for the comparison with theoretical models.

In conclusion, we have measured the lifetime of the metastable state to a 2.0%-level and shown the influence of the data processing method on the obtained value. Measurement of the $`3d^2D_{3/2}`$-level lifetime would be interesting to allow direct comparison of the fine-structure levels. The actual experimental protocol does not allow such a measurement due to the coupling by the repumper laser. A comparable metastable-level lifetime has been measured in the Ba+-ion Yu et al. (1997). We plan to apply this latter technique for the measurement of the $`3D_{3/2}`$ lifetime in Ca+.

The high degree of control of our experimental parameters, that we need for the preparation of the metrological project, has now been achieved . The next step will be the localization of the ion in the trap to better than a fraction of the emitted wavelength, giving access to the Lamb-Dicke regime, where the first-order Doppler broadening can be eliminated Dicke (1953). Stabilization of the clock laser to an ULE cavity will be required to make the laser linewidth compatible with the observed ion features.

###### Acknowledgements.

This work has benefitted from fruitful discussions with Peter Staanum, David Lucas and Bruno Torrésani. Our project has been financially supported by the Bureau National de Métrologie.


text:
# Magnetization plateaus in frustrated antiferromagnetic quantum spin models

## 1 Introduction

Geometrically frustrated quantum spin systems constitute a class of systems exhibiting interesting quantum phenomena like different (unusual) quantum phases (see e.g.  for reviews of two-dimensional models). An external magnetic field may further enhance this frustration since it competes with the antiparallel alignment of spins favoured by antiferromagnetic exchange. This leads to interesting quantum phenomena in the high-field magnetization process of geometrically frustrated quantum spin systems. In particular, a spin gap may be opened by the external magnetic field, giving rise to a plateau in the $`T=0`$ magnetization curve. Although no complete review of the subject exists so far, different aspects are summarized e.g. in . In this article we will illustrate the status of the field by pointing out and presenting selected recent and new results.

Specifically we consider the $`XXZ`$ model in an external magnetic field $`h`$

$$H=\underset{i,j}{}J_{i,j}\left(S_i^xS_j^x+S_i^yS_j^y+\mathrm{\Delta }S_i^zS_j^z\right)h\underset{i}{}S_i^z,$$
(1)
where the $`\stackrel{}{S}_i`$ are spin-$`S`$ operators at site $`i`$ and the $`J_{i,j}`$ are the exchange constants between pairs of sites $`i,j`$ connected in the lattice topology under consideration. The special case of (1) where the $`XXZ`$ anisotropy satisfies $`\mathrm{\Delta }=1`$ corresponds to the Heisenberg model. Below we will concentrate on the extreme quantum limit $`S=1/2`$ and antiferromagnetic coupling $`J_{i,j}0`$ although some of the results can be generalized e.g. to $`S>1/2`$.

An important observable is the magnetization

$$M=\frac{1}{NS}\underset{i}{}S_i^z$$
(2)
which we normalize to saturation value $`M=1`$ (here $`N`$ is the total number of spins in the system). Note that the magnetization (2) is a conserved quantity for the Hamiltonian (1). This is technically useful for computing the magnetization curve e.g. by exact diagonalization (ED) using the Lanczos method.

## 2 One dimension

In one dimension, Oshikawa, Yamanaka and Affleck proposed the following condition on the magnetization $`M`$ at a plateau in the $`T=0`$ magnetization curve

$$SV\left(1M\right).$$
(3)
Here $`S`$ is the size of the local spin and $`V`$ is the number of spins in a translational unit cell of the ground state. The condition (3) can be understood easily starting from a limit where the system decouples into clusters with $`V`$ sites (see e.g. ) and in this case $`V`$ is the number of spins in a unit cell of the Hamiltonian. However, in particular in frustrated spin systems one finds that translational symmetry is spontaneously broken in the ground state (c.f. examples in the following sections) and then $`V`$ is larger than (namely an integer multiple of) the unit cell of the Hamiltonian. Nevertheless, the quantization condition (3) implies that the magnetization $`M`$ always has a rational value on a plateau.

### 2.1 Frustrated $`S=1/2`$ Heisenberg chain

Let us start by discussing some selected aspects of the $`S=1/2`$ frustrated Heisenberg chain (see inset of Fig. 1). Majumdar and Ghosh noticed more than 30 years ago  that one can explicitly write down the ground state if the next-nearest neighbour coupling $`J_2`$ and the nearest neighbour coupling $`J_1`$ are related by $`J_2=J_1/2`$. This so-called ‘Majumdar-Ghosh’ state is a two-fold degenerate dimer product state and has become a paradigm for the frustration-induced opening of a spin gap accompanied by spontaneous breaking of translational symmetry by a period two.

In the presence of a magnetic field, the spin gap leads to an $`M=0`$ plateau in the magnetization curve. Starting with , many authors have studied the magnetization process of this model by ED (see e.g.  and references therein) and no plateaus with $`M0`$ were found. Finally, a recent density-matrix renormalization group (DMRG) study of the $`S=1/2`$ frustrated Heisenberg chain exhibited a clear plateau at $`M=1/3`$ in the region of strong frustration $`J_1J_2`$ , as is illustrated by the main panel of Fig. 1 which reproduces the magnetization curve for $`J_2=0.8J_1`$ (the step on the $`M=1/3`$ plateau in the DMRG curve is due to the open boundaries). The state of this $`M=1/3`$ plateau spontaneously breaks translational symmetry by a period three. Two points are worthwhile noticing here. First, this period three is higher than the period two appearing in the Majumdar-Ghosh state  at $`h=0`$. Second, the very presence of this plateau was missed for a long time.

With hindsight, this $`M=1/3`$ plateau can be observed also in the ED results for $`L=12`$ and $`24`$ sites and periodic boundary conditions (reproduced for $`J_2=0.8J_1`$ in Fig. 1 after  – this figure also includes a new $`L=36`$ curve). It may be instructive to consider the reasons for missing it nevertheless. First, the excited states at $`h=0`$  and correspondingly the ground states in a magnetic field $`h0`$ have in general incommensurate momenta  which leads to oscillating finite-size effects. Second, one should concentrate on system sizes that can accommodate the known antiferromagnetic ground states in the limit of two decoupled chains $`J_10`$, implying that $`L`$ should be a multiple of 4. In addition, only those values of the magnetization can be studied which are realized for a given system size. In particular, $`M=1/3`$ is realized only if $`L`$ is a multiple of 3. These considerations restrict the system sizes that should be used for the discussion of an $`M=1/3`$ plateau in the frustrated Heisenberg chain to multiples of 12. The first cases are $`L=12`$, $`24`$ and $`36`$. These are used in Fig. 1 and are in good agreement with the DMRG results of .

### 2.2 Orthogonal dimer chain

Now we wish to draw the reader’s attention to the $`S=1/2`$ orthogonal dimer chain (also known as dimer-plaquette chain)  shown in the inset of Fig. 2, a further one-dimensional model where some remarkable properties were missed originally. This model attracted renewed attention recently since it can be regarded as a one-dimensional version of the two-dimensional Shastry-Sutherland model .

A first study  of the magnetization process of the $`S=1/2`$ orthogonal dimer chain found plateaus with $`M=1/4`$ and $`1/2`$. However, this study missed further plateaus and thus the remarkable property of the orthogonal dimer chain that it gives rise to a magnetization curve with (probably infinitely) many plateaus for some values of the parameters . At least some steps in the derivation can be carried out exactly exploiting the special property of the orthogonal dimer chain that the total spin on each vertical dimer is conserved. A plateau-state can then be characterized as follows : $`k`$ consecutive vertical dimers form triplets ($`S=1`$), separated by singlets ($`S=0`$). Covering the chain periodically with such ‘fragments’ of length $`k`$ each in the sector $`S^z=k`$ yields

$$M=\frac{k}{2k+2}.$$
(4)
At $`J^{}=0.7J>0`$ and for $`M<1/2`$ only precisely these states consisting of fragments of length $`k`$ with $`S^z=k`$ appear as ground states in a magnetic field , whereas for $`M>1/2`$ the ground state is in a sector where all vertical dimers form triplets $`S=1`$ (one difference between the present Fig. 2 and the original Fig. 3 of  is in the system sizes that have been used for extrapolating the magnetization curve in the region $`M1/2`$). As long as $`M<1/2`$, fragments of increasing length become ground states with increasing field, leading to a magnetization curve with infinitely many plateaus at the magnetization values given by (4) and jumps in between, compare the main panel of Fig. 2. This infinite series accumulates at $`M=1/2`$, where one finds a further pronounced plateau before a smooth transition to saturation follows.

The infinite sequence of plateaus arises in the orthogonal dimer chain because the ground states manifestly break translational symmetry with arbitrarily long periodicity $`k+1`$, implying that at least in one dimension there is no general upper bound on the possible periods for spontaneous breaking of translational symmetry.

## 3 Two dimensions

To the best of our knowledge there are no rigorous arguments why the condition (3) should hold in dimensions higher than one. Furthermore, starting from two dimensions one may have true long-range order in the spin components at $`T=0`$. Accordingly, an external magnetic field can induce transitions between different ordered and disordered states.

In one dimension, a plateau at a given $`M`$ already requires a detailed analysis of the specific model. And, even more so the presence and nature of a plateau state must be discussed case by case in two dimensions. Some selected examples are presented in the following sections.

### 3.1 Square lattice

Let us start with a brief discussion of the magnetization process of the square lattice which is a non-frustrated model and well understood. Fig. 3 shows the magnetization curve of the $`S=1/2`$ square-lattice Heisenberg model ($`\mathrm{\Delta }=1`$) obtained by different approaches. First, the thin full line shows the result obtained by ED for a finite lattice with $`N=40`$ sites (see also  for earlier ED studies – in the particular case $`N=40`$, the largest dimension to be treated was 554 596 326 and occurred in the sector $`S^z=3`$). The full bold line denotes an extrapolation of the ED data to the thermodynamic limit which is obtained by connecting the midpoints of the finite-size steps at the largest available system size. One observes a smooth magnetization curve with no peculiar features (in particular no plateaus) for $`\left|M\right|<1`$. Note that close to saturation the extrapolated curve includes data at large system sizes, which is not shown explicitly in Fig. 3. More precisely, for $`M0.84375`$, the curve is based exclusively on finite lattices with at least $`8\times 8`$ sites. The high-field part of the magnetization curve is therefore particularly well controlled by ED.

Second, a second-order spinwave result  is also available and shown by the bold dashed line in Fig. 3. Third, the magnetization process of the square lattice can also be studied by quantum Monte Carlo (QMC) since this lattice is not frustrated. The diamonds in Fig. 3 show available stochastic-series-expansion QMC results .

The quantitive differences of the results of all three approaches are small, i.e. each approach yields a good description of the $`S=1/2`$ square lattice. Since the spinwave approach  is based on a Néel state, we may therefore conclude that Néel order prevails in the transverse components for $`\left|M\right|<1`$ (see also  for a discussion from the point of view of ED).

### 3.2 Triangular lattice

The $`S=1/2`$ $`XXZ`$ model on the triangular lattice is among the first models whose magnetization process was studied by ED . These early studies already found a plateau with $`M=1/3`$, at least for Ising-like anisotropies $`\mathrm{\Delta }>1`$. Due to the restriction to at most 21 sites, it was first not completely clear whether the plateau persists in the isotropic regime $`\mathrm{\Delta }1`$. The magnetization process of the isotropic model was analyzed further using spinwave theory . This study provided evidence that the $`M=1/3`$ plateau exists also at $`\mathrm{\Delta }=1`$ and estimates for its boundaries were obtained.

Fig. 4 shows the magnetization curves obtained by ED for $`\mathrm{\Delta }=1`$ on finite lattices with $`N=27`$ and $`36`$ sites (thin lines). Both curves exhibit a clear plateau at $`M=1/3`$ in an otherwise smooth magnetization curve. These two curves overlap with previous ED results . Note, however, that for $`N=36`$ only the sector $`\stackrel{}{k}=0`$ was studied previously for $`M1/3`$ , but it turns out that the ground state is not always in this sector. Inclusion of sectors with $`\stackrel{}{k}0`$ for $`N=36`$, a different shape of the $`N=27`$ system and a previously incomplete $`N=36`$ curve lead to small differences of our Fig. 4 as compared to Fig. 4 of . The first-order spinwave results for the magnetic fields at the lower and the upper boundaries of the $`M=1/3`$ plateau  are smaller by about $`0.13J`$ (lower boundary) and $`0.01J`$ (upper boundary) than the ED results presented here for $`N=36`$ and $`S=1/2`$.

The full bold line in Fig. 4 denotes an extrapolation of the ED data to the thermodynamic limit which is obtained by connecting the midpoints of the finite-size steps at the largest available system size (except for the boundaries of the $`M=1/3`$ plateau where corners were used). Close to saturation this includes again bigger system sizes than those explicitly shown in Fig. 4.

The state of the $`M=1/3`$ plateau can be easily understood in the Ising limit $`\mathrm{\Delta }1`$ . Quantum fluctuations are completely suppressed in the limit $`\mathrm{\Delta }\mathrm{}`$ and the $`M=1/3`$ state is a classical state where all spins on two of the three sublattices of the triangular lattice point up and all spins on the third sublattice point down, as is sketched in the inset of Fig. 5. This state corresponds to an ordered collinear spin configuration. It breaks translational symmetry by a period three and accordingly is threefold degenerate. One can then use perturbation theory in $`1/\mathrm{\Delta }`$ to study the $`M=1/3`$ plateau of the $`XXZ`$ model . Here we numerically compute the overlap of the appropriate linear combination $`|\text{Ising}`$ of the three Ising states and the $`M=1/3`$ wave function $`|\text{full }XXZ`$ of the full $`XXZ`$ model with $`S=1/2`$ in order to show that this description remains qualitatively valid even in the isotropic region $`\mathrm{\Delta }1`$. Fig. 5 shows results for the overlap $`\left|\text{full }XXZ|\text{Ising}\right|`$ on finite lattices with $`N=18`$, $`27`$ and $`36`$ sites (for $`N=36`$ we have computed the overlaps by considering only the wave function within the $`\stackrel{}{k}`$-subspace that contains the ground state for $`\mathrm{\Delta }1`$). One observes that this overlap remains large even in the vicinity of the Heisenberg model $`\mathrm{\Delta }=1`$ and drops sharply around $`\mathrm{\Delta }=0.75`$. Accordingly, this $`M=1/3`$ plateau state is a stable phase for $`\mathrm{\Delta }>\mathrm{\Delta }_c`$ with $`\mathrm{\Delta }_c0.75`$. Remarkably, this estimate for $`\mathrm{\Delta }_c`$ is close to the estimate $`\mathrm{\Delta }_c0.85`$ for the vanishing point of the $`M=1/3`$ plateau which was obtained in  by comparing the plateau widths on $`3\times 6`$ and $`3\times 9`$ systems. Note that the location of the sharp drop in Fig. 5 is almost independent of system size although the absolute values of the overlaps $`\left|\text{full }XXZ|\text{Ising}\right|`$ do depend on $`N`$. We can thus locate the point $`\mathrm{\Delta }_c`$ where the $`M=1/3`$ plateau disappears quite accurately at $`\mathrm{\Delta }_c=0.76\pm 0.03`$.

### 3.3 Kagomé lattice

Finally, Fig. 6 shows magnetization curves for the Kagomé lattice (see inset) with $`N=27`$  and $`36`$ sites. Note that the $`N=36`$ curve in Fig. 6 differs slightly from the corresponding curve in  for $`M1/3`$. The reason is that due to the computational effort only selected $`\stackrel{}{k}`$-sectors were investigated in  and in some cases the correct symmetry of the ground state was in fact missed. Our new $`N=36`$ curve agrees with unpublished results of Waldtmann and Everts .

The Kagomé lattice is famous for a disordered ground state at $`h=0`$ accompanied by a small spin gap with many singlets inside this gap (see  and references therein). The spin gap should give rise to a narrow $`M=0`$ plateau even if it is difficult to recognize in Fig. 6.

A plateau at $`M=1/3`$ can be recognized better in Fig. 6. In fact, the presence of this plateau at $`M=1/3`$ in the $`S=1/2`$ Heisenberg model on the Kagomé lattice has been established previously by considering also system sizes different from those shown in Fig. 6 . Nevertheless, the state of this plateau is still an interesting issue. For the classical Heisenberg model at $`M=1/3`$, thermal fluctuations select collinear states, but due to the huge degeneracy of this space, there appears to be no real order on the classical level at $`M=1/3`$  (see also ). For $`S=1/2`$, it is useful to consider the $`XXZ`$ model. In the Ising limit $`\mathrm{\Delta }\mathrm{}`$ one can then first establish  a relation to a quantum dimer model on the hexagonal lattice which was argued  to give rise to a valence bond crystal ground state with a $`\sqrt{3}\times \sqrt{3}`$ order indicated by the circles in the hexagons in the inset of Fig. 6. Furthermore, like for the triangular lattice one can compute the overlap (see Fig. 5) of the $`M=1/3`$ wave function of the $`XXZ`$ model with that of the quantum dimer model as a function of $`\mathrm{\Delta }`$ and one finds no evidence for a phase transition for $`\mathrm{\Delta }1`$ . This implies that also the $`M=1/3`$ state of the $`S=1/2`$ Heisenberg model on the Kagomé lattice is a three-fold degenerate valence bond crystal, i.e. an ordered state with many low-lying non-magnetic excitations, but still a small gap to all excitations .

There may be a further plateau at $`M=5/9`$ in Fig. 6 although it is difficult to draw unambiguous conclusions from the available numerical data in this region of magnetization values.

Finally, one can see a pronounced jump of height $`\delta M=2/9`$ just below saturation in Fig. 6. This jump arises due to local magnon excitations which can be constructed in the spin-$`S`$ $`XXZ`$ model on the Kagomé lattice . These local magnon excitations give rise to an exact degeneracy at the saturation field and thus a macroscopic jump in the magnetization curve of height $`\delta M=1/(9S)`$. In the state just below the jump, magnons are localized on the hexagons marked by circles in the inset of Fig. 6. Since this is a crystalline ordered state, general arguments (see e.g. ) predict a gap and consequently a plateau in the magnetization curve at $`M=11/(9S)`$. Indeed, a plateau at $`M=7/9`$ can be seen clearly in the magnetization curve of the $`S=1/2`$ Heisenberg model on the Kagomé lattice in particular when one considers also lattices with $`N=45`$ and $`54`$ sites .

## 4 Conclusions and outlook

In this article we have discussed examples of plateaus in one- and two-dimensional quantum spin models. In one dimension, the appearance of a plateau is controlled by the quantization condition (3) which implies in particular that the magnetization $`M`$ on a plateau must be rational. This condition can be interpreted as a commensurability condition for the ground state. Hence, it is important to observe that translational symmetry can be spontaneously broken in frustrated quantum spin models. Even in well-studied examples such as the frustrated $`S=1/2`$ Heisenberg chain, an $`M=1/3`$ plateau with a spontaneously broken period three was discovered only recently . Furthermore, an infinite sequence of plateaus in the orthogonal dimer chain  shows that there is no upper bound on the possible periodicity of spontaneous breaking of translational symmetry.

It is less clear if the condition (3) is also applicable to two and higher dimensions. Nevertheless, it works for most examples discussed here: The state of the $`M=1/3`$ plateau in the $`S=1/2`$ triangular lattice has a unit cell with $`V=3`$ spins (see section 3.2) and for the Kagomé lattice the plateaus with $`M=1/3`$ in the $`S=1/2`$ model as well as the one with $`M=11/(9S)`$ in the spin-$`S`$ model both have unit cells with $`V=9`$ spins (see section 3.3, in particular the inset of Fig. 6). These cases fit well with the quantization condition (3). However, the disordered ground state at $`h=0`$ in the $`S=1/2`$ Kagomé lattice (see  and references therein) is not covered by the condition (3) since it gives rise to an $`M=0`$ plateau without the appropriate breaking of translational symmetry.

From the point of view of experiments, the exchange constants $`J_{i,j}`$ dictate the scale of magnetic fields needed to access the high-field region. SrCu<sub>2</sub>(BO<sub>3</sub>)<sub>2</sub> is an $`S=1/2`$ system with sufficiently small $`J`$’s that permit the observation of plateaus at $`M=1/8`$, $`1/4`$ and $`1/3`$ in pulsed-field magnetization experiments . SrCu<sub>2</sub>(BO<sub>3</sub>)<sub>2</sub> is believed to be a good realization of the two-dimensional Shastry-Sutherland lattice . Because of its relation to SrCu<sub>2</sub>(BO<sub>3</sub>)<sub>2</sub>, this frustrated spin model has been analyzed theoretically in detail (see  for a recent review). We hope that the examples discussed in this article will stimulate further theoretical and experimental research on the magnetization process of frustrated quantum spin models.

We would like to thank D.C. Cabra, M.D. Grynberg, P.C.W. Holdsworth and P. Pujol for useful discussions. The more complicated computations presented in this article have been performed on the compute-servers cfgauss and wildfire at the computing centers of the TU Braunschweig and Magdeburg University, respectively. We are particularly grateful to J. Schüle of the Rechenzentrum at the TU Braunschweig for technical support. This work was partly supported by the DFG (project Ri615/10-1).

## References