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# THE NEW COSMOLOGY

## 1 The New Cosmology

Cosmology is enjoying the most exciting period of discovery yet. Over the past three years a New Cosmology has been emerging. It incorporates the highly successful standard hot big-bang cosmology and may extend our understanding of the Universe to times as early as $`10^{32}`$sec, when the largest structures in the Universe were still subatomic quantum fluctuations.

This New Cosmology is characterized by

* Flat, critical density accelerating Universe
* Early period of rapid expansion (inflation)
* Density inhomogeneities produced from quantum fluctuations during inflation
* Composition: 2/3 dark energy; 1/3 dark matter; 1/200 bright stars
* Matter content: $`(29\pm 4)`$% cold dark matter; $`(4\pm 1)`$% baryons;
>0.3
>absent0.3\mathrel{\mathchoice{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\displaystyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\textstyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptstyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptscriptstyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}}0.3% neutrinos
* $`T_0=2.725\pm 0.001`$K
* $`t_0=14\pm 1`$Gyr
* $`H_0=72\pm 7\mathrm{km}\mathrm{s}^1\mathrm{Mpc}^1`$

The New Cosmology is not as well established as the standard hot big-bang cosmology. However, the evidence is growing.

### 1.1 Mounting Evidence: Recent Results

The position of the first acoustic peak in the multipole power spectrum of the anisotropy of the cosmic microwave background (CMB) radiation provides a powerful means of determining the global curvature of the Universe. With the recent DASI observations of CMB anisotropy on scales of one degree and smaller, the evidence that the Universe is at most very slightly curved is quite firm. The curvature radius of the Universe ($`R_{\mathrm{curv}}`$) and the total energy density parameter $`\mathrm{\Omega }_0=\rho _{\mathrm{TOT}}/\rho _{\mathrm{crit}}`$, are related:

$$R_{\mathrm{curv}}=H_0^1/|\mathrm{\Omega }_01|^{1/2}$$

The spatial flatness is expressed as $`\mathrm{\Omega }_0=1.0\pm 0.04`$, or said in words, the curvature radius is at least 50 times greater than the Hubble radius.

I will discuss the evidence for accelerated expansion and dark energy later.

The series of acoustic peaks in the CMB multipole power spectrum and their heights indicate a nearly scale-invariant spectrum of adiabatic density perturbations with $`n=1\pm 0.07`$. Nearly scale-invariant density perturbations and a flat Universe are two of the three hallmarks of inflation. Thus, we are beginning to see the first significant experimental evidence for inflation, the driving idea in cosmology for the past two decades.

The striking agreement of the BBN determination of the baryon density from measurements of the primeval deuterium abundance, $`\mathrm{\Omega }_Bh^2=0.020\pm 0.001`$, with those from from recent CMB anisotropy measurements, $`\mathrm{\Omega }_Bh^2=0.022\pm 0.004`$, make a strong case for a small baryon density, as well as the consistency of the standard cosmology ($`h=H_0/100\mathrm{km}\mathrm{sec}^1\mathrm{Mpc}^1`$). There can now be little doubt that baryons account for but a few percent of the critical density.

Our knowledge of the total matter density is improving, and becoming less linked to the distribution of light. This makes determinations of the matter less sensitive to the uncertain relationship between the clustering of mass and of light (what astronomers call the bias factor $`b`$). Both the CMB and clusters of galaxies allow a determination of the ratio of the total matter density (anything that clusters – baryons, neutrinos, cold dark matter) to that in baryons alone: $`\mathrm{\Omega }_M/\mathrm{\Omega }_B=7.2\pm 2.1`$ (CMB), $`9\pm 1.5`$ (clusters). Not only are these numbers consistent, they make a very strong case for something beyond quark-based matter. When combined with our knowledge of the baryon density, one infers a total matter density of $`\mathrm{\Omega }_M=0.33\pm 0.04`$.

The many successes of the cold dark matter (CDM) scenario – from the sequence of structure formation (galaxies first, clusters of galaxies and larger objects later) and the structure of the intergalactic medium, to its ability to reproduce the power spectrum of inhomogeneity measured today – makes it clear that CDM holds much, if not all, of the truth in describing the formation of structure in the Universe.

The two largest redshift surveys, the Sloan Digital Sky Survey (SDSS) and the 2-degree Field project (2dF), have each recently measured the power spectrum using samples of more than 100,000 galaxies and found that it is consistent with that predicted in a flat accelerating Universe comprised of cold dark matter. The SDSS will eventually use a sample of almost one million galaxies to probe the power spectrum. \[Interestingly enough, according to the 2dF Collaboration, bias appears to be a small effect, $`b=1.0\pm 0.09`$ \]

All of this implies that whatever the dark matter particle is, it moves slowly (i.e., the bulk of the matter cannot be in the form of hot dark matter such as neutrinos) and interacts only weakly (e.g., with strength much less than electromagnetic) with ordinary matter.

The evidence from SuperKamiokande for neutrino oscillations makes a strong case that neutrinos have mass (imν
>0.1
>subscript𝑖subscript𝑚𝜈0.1\sum_{i}m_{\nu}\mathrel{\mathchoice{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\displaystyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\textstyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptstyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptscriptstyle\hfil#\hfil$\cr>\crcr\sim\crcr}}}}0.1\,eV) and therefore contribute to the mass budget of the Universe at a level comparable to, or greater than, that of bright stars. Particle dark matter has moved from the realm of a hypothesis to a quantitative question – how much of each type of particle dark matter is there in the Universe? Structure formation in the Universe (especially the existence of small scale structure) suggests that neutrinos contribute at most 5% or 10% of the critical density, corresponding to imnu=imν/90h2eV
<5subscript𝑖subscript𝑚𝑛𝑢subscript𝑖subscript𝑚𝜈90superscript2eV
<5\sum_{i}m_{n}u=\sum_{i}m_{\nu}/90h^{2}\,{\rm eV}\mathrel{\mathchoice{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\displaystyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\textstyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptstyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptscriptstyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}}5\,eV.

Even the age of the Universe and the pesky Hubble constant have been reined in. The uncertainties in the ages of the oldest globular clusters have been better identified and quantified, leading to a more precise age, $`t_0=13.5\pm 1.5`$Gyr. The CMB can be used to constrain the expansion age, independent of direct measurements of $`H_0`$ or the composition of the Universe, $`t_{\mathrm{exp}}=14\pm 0.5`$Gyr.

A host of different techniques are consistent with the Hubble constant determined by the HST key project, $`H_0=72\pm 7\mathrm{km}\mathrm{s}^1\mathrm{Mpc}^1`$. Further, the error budget is now well understood and well quantified. \[The bulk of the $`\pm 7`$ uncertainty is systematic, dominated by the uncertainty in the distance to the LMC and the Cepheid period – luminosity relation.\] Moreover, the expansion age derived from this consensus Hubble constant, which depends upon the composition of the Universe, is consistent with the previous two age determinations.

The poster child for precision cosmology continues to be the present temperature of the CMB. It was determined by the FIRAS instrument on COBE to be: $`T_0=2.725\pm 0.001`$K. Further, any deviations from a black body spectrum are smaller than 50 parts per million. Such a perfect Planckian spectrum has made any noncosmological explanation untenable.

### 1.2 Successes and Consistency Tests

To sum up, we have determined the basic features of the Universe: the cosmic matter/energy budget; a self consistent set of cosmological parameters with realistic errors; and the global curvature. Two of the three key predictions of inflation – flatness and nearly scale-invariant, adiabatic density perturbations – have passed their first significant tests. Last but not least, the growing quantity of precision data are now testing the consistency of the Friedmann-Robertson-Walker framework and General Relativity itself.

In particular, the equality of the baryon densities determined from BBN and CMB anisotropy is remarkable. The first involves nuclear physics when the Universe was seconds old, while the latter involves gravitational and classical electrodynamics when the Universe was 400,000 years old.

The entire framework has been tested by the existence of the aforementioned acoustic peaks in the CMB angular power spectrum. They reveal large-scale motions that have remained coherent over hundreds of thousands of years, through a delicate interplay of gravitational and electromagnetic interactions.

Another test of the basic framework is the accounting of the density of matter and energy in the Universe. The CMB measurement of spatial flatness implies that the matter and energy densities must sum to the critical density. Measurements of the matter density indicate $`\mathrm{\Omega }_M=0.33\pm 0.04`$; and measurements of the acceleration of the Universe from supernovae indicate the existence of a smooth dark energy component that accounts for $`\mathrm{\Omega }_X0.67`$. \[The amount of dark energy inferred from the supernova measurements depends its equation of state; for a cosmological constant, $`\mathrm{\Omega }_\mathrm{\Lambda }=0.8\pm 0.16`$.\]

Finally, while cosmology has in the past been plagued by “age crises” – time back to the big bang (expansion age) apparently less than the ages of the oldest objects within the Universe – today the ages determined by very different and completely independent techniques point to a consistent age of 14 Gyr.

## 2 Mysteries

Cosmological observations over the next decade will test – and probably refine – the New Cosmology. If we are fortunate, they will also help us to make better sense of it. At the moment, the New Cosmology has presented us with a number of cosmic mysteries – opportunities for surprises and new insights. Here I will quickly go through my list, and save the most intriguing to me – dark energy – for its own section.

### 2.1 Dark Matter

By now, the conservative hypothesis is that the dark matter consists of a new form of matter, with the axion and neutralino as the leading candidates. That most of the matter in the Universe exists in a new form of matter – yet to be detected in the laboratory – is a bold and untested assertion.

Experiments to directly detect the neutralinos or axions holding our own galaxy together have now reached sufficient sensitivity to probe the regions of parameter space preferred by theory. In addition, the neutralino can be created by upcoming collider experiments (at the Tevatron or the LHC), or detected by its annihilation signatures – high-energy neutrinos from the sun, narrow positron lines in the cosmic rays, and gamma-ray line radiation.

While the CDM scenario is very successful there are some nagging problems. They may point to a fundamental difficulty or may be explained by messy astrophysics. The most well known of these problems are the prediction of cuspy dark-matter halos (density profile $`\rho _{\mathrm{DM}}1/r^n`$ as $`r0`$, with $`n11.5`$) and the apparent prediction of too much substructure. While there are plausible astrophysical explanations for both problems, they could indicate an unexpected property of the dark-matter particle (e.g., large self-interaction cross section, large annihilation cross section, or mass of around 1 keV). While I believe it is unlikely, these problems could indicate a failure of the particle dark-matter paradigm and have their explanation in a radical modification of gravity theory.

I leave for the “astrophysics to do list” an accounting of the dark baryons. Since $`\mathrm{\Omega }_B0.04`$ and $`\mathrm{\Omega }_{}0.005`$, the bulk of the baryons are optically dark. In clusters, the dark baryons have been identified: they exists as hot, x-ray emitting gas. Elsewhere, the dark baryons have not yet been identified. According to CDM, the bulk of the dark baryons are likely to exist as hot/warm gas associated with galaxies, but this gas has not been detected. \[Since clusters account for only about 5 percent of the total mass, the bulk of the dark baryons are still not accounted for.\]

### 2.2 Baryogenesis

The origin of quark-based matter is not yet fully understood. We do know that the origin of ordinary matter requires a small excess of quarks over antiquarks (about a part in $`10^9`$) at a time at least as early as $`10^6`$sec, to avoid the annihilation catastrophe associated with a baryon symmetric Universe. If the Universe underwent inflation, the baryon asymmetry cannot be primeval, it must be produced dynamically (“baryogenesis”) after inflation since any pre-inflation baryon asymmetry is diluted away by the enormous entropy production associated with reheating.

Because we also now know that electroweak processes violate $`B+L`$ at a very rapid rate at temperatures above $`100`$GeV or so, baryogenesis is more constrained than when the idea was introduced more than twenty years ago. Today there are three possibilities: 1) produce the baryon asymmetry by GUT-scale physics with $`BL0`$ (to prevent it being subsequently washed away by $`B+L`$ violation); 2) produce a lepton asymmetry ($`L0`$), which is then transmuted into the baryon asymmetry by electroweak $`B+L`$ violation; or 3) produce the baryon asymmetry during the electroweak phase transition using electroweak $`B`$ violation.

While none of the three possibilities can be ruled out, the second possibility looks most promising, and it adds a new twist to the origin of quark-based matter: We are here because neutrinos have mass. \[In the lepton asymmetry first scenario, Majorana neutrino mass provides the requisite lepton number violation.\] The drawback of the first possibility is the necessity of a high reheat temperature after inflation, $`T_{\mathrm{RH}}10^5`$GeV, which is difficult to achieve in most models of inflation. The last possibility, while very attractive because all the input physics might be measurable at accelerator, requires new sources of $`CP`$ violation at TeV energies as well as a strongly first-order electroweak phase transition (which is currently disfavored by the high mass of the Higgs).

### 2.3 Inflation

There are still many questions to be answered about inflation, including the most fundamental: did inflation (or something similar) actually take place!

A powerful program is in place to test the inflationary framework. Testing framework involves testing its three robust predictions: spatially flat Universe; nearly-scale invariant, nearly power-law spectrum of Gaussian adiabatic, density perturbations; and a spectrum of nearly scale-invariant gravitational waves.

The first two predictions are being probed today and will be probed much more sharply over the next decade. The value of $`\mathrm{\Omega }_0`$ should be determined to much better than 1 percent. The spectral index $`n`$ that characterizes the density perturbations should be measured to percent accuracy.

Generically, inflation predicts $`|n1|𝒪(0.1)`$, where $`n=1`$ corresponds to exact scale invariance. Likewise, the deviations from an exact power-law predicted by inflation, $`|dn/d\mathrm{ln}k|10^410^2`$ will be tested. The CMB and the abundance of rare objects such as clusters of galaxies will allow Gaussianity to be tested.

Inflationary theory has given little guidance as to the amplitude of the gravitational waves produced during inflation. If detected, they are a smokin’ gun prediction. Their amplitude is directly related to the scale of inflation, $`h_{\mathrm{GW}}H_{\mathrm{inflation}}/m_{\mathrm{Pl}}`$. Together measurements of $`n1`$ and $`dn/\mathrm{ln}k`$, they can reveal much about the underlying scalar potential driving inflation. Measuring their spectral index – a most difficult task – provides a consistency test of the single scalar-field model of inflation.

### 2.4 The Dimensionality of Space-time

Are there additional spatial dimensions beyond the three for which we have very firm evidence? I cannot think of a deeper question in physics today. If there are new dimensions, they are likely to be relevant for cosmology, or at least raise new questions in cosmology (e.g., why are only three dimensions large? what is going on in the bulk? and so on). Further, cosmology may well be the best means for establishing the existence of extra dimensions.

### 2.5 Before Inflation, Other Big-bang Debris, and Surprises

Only knowing everything there is to know about the Universe would be worse than knowing all the questions to ask about it. Without doubt, as our understanding deepens, new questions and new surprises will spring forth.

The cosmological attraction of inflation is its ability to make the present state of the Universe insensitive to its initial state. However, should we establish inflation as part of cosmic history, I am certain that cosmologists will begin asking what happened before inflation.

Progress in cosmology depends upon studying relics. We have made much of the handful we have – the light elements, the baryon asymmetry, dark matter, and the CMB. The significance of a new relic cannot be overstated. For example, detection of the cosmic sea of neutrinos would reveal the Universe at 1 second.

Identifying the neutralino as the dark matter particle and determining its properties at an accelerator laboratory would open a window on the Universe at $`10^8`$sec. By comparing its relic abundance as derived from its mass and cross section with its actual abundance measured in the Universe, one could test cosmology at the time the neutralino abundance was determined.

And then there may be the unexpected. Recently, a group reported evidence for a part in $`10^5`$ difference in the fine-structure constant at redshifts of order a few from its value today. I remain skeptical, given possible astrophysical explanations, other much tighter constraints to the variation of $`\alpha `$ (albeit at more recent times), and the absence of a reasonable theoretical model. For reference, I was also skeptical about the atmospheric neutrino problem because of the need for large-mixing angles.

## 3 Dark Energy: Seven Things We Know

The dark energy accounts for 2/3 of the stuff in the Universe and determines its destiny. That puts it high on the list of outstanding problems in cosmology. Its deep connections to fundamental physics – a new form of energy with repulsive gravity and possible implications for the divergences of quantum theory and supersymmetry breaking – put it very high on the list of outstanding problems in particle physics.

What then is dark energy? Dark energy is my term for the causative agent for the current epoch of accelerated expansion. According to the second Friedmann equation,

$$\frac{\ddot{R}}{R}=\frac{4\pi G}{3}\left(\rho +3p\right)$$
(1)
this stuff must have negative pressure, with magnitude comparable to its energy density, in order to produce accelerated expansion \[recall $`q=(\ddot{R}/R)/H^2`$; $`R`$ is the cosmic scale factor\]. Further, since this mysterious stuff does not show its presence in galaxies and clusters of galaxies, it must be relatively smoothly distributed.

That being said, dark energy has the following defining properties: (1) it emits/absorbs no light; (2) it has large, negative pressure, $`p_X\rho _X`$; (3) it is approximately homogeneous (more precisely, does not cluster significantly with matter on scales at least as large as clusters of galaxies); and (4) it is very mysterious. Because its pressure is comparable in magnitude to its energy density, it is more “energy-like” than “matter-like” (matter being characterized by $`p\rho `$). Dark energy is qualitatively very different from dark matter, and is certainly not a replacement for it.

### 3.1 Two Lines of Evidence for an Accelerating Universe

Two independent lines of reasoning point to an accelerating Universe. The first is the direct evidence based upon measurements of type Ia supernovae carried out by two groups, the Supernova Cosmology Project and the High-$`z`$ Supernova Team. These two teams used different analysis techniques and different samples of high-$`z`$ supernovae and came to the same conclusion: the expansion of the Universe is speeding up, not slowing down.

The recent serendipitous discovery of a supernovae at $`z=1.76`$ bolsters the case significantly and provides the first evidence for an early epoch of decelerated expansion. SN 1997ff falls right on the accelerating Universe curve on the magnitude – redshift diagram, and is a magnitude brighter than expected in a dusty open Universe or an open Universe in which type Ia supernovae are systematically fainter at high-$`z`$.

The second, independent line of reasoning for accelerated expansion comes from measurements of the composition of the Universe, which point to a missing energy component with negative pressure. The argument goes like this: CMB anisotropy measurements indicate that the Universe is nearly flat, with density parameter, $`\mathrm{\Omega }_0=1.0\pm 0.04`$. In a flat Universe, the matter density and energy density must sum to the critical density. However, matter only contributes about 1/3 of the critical density, $`\mathrm{\Omega }_M=0.33\pm 0.04`$. (This is based upon measurements of CMB anisotropy, of bulk flows, and of the baryonic fraction in clusters.) Thus, two thirds of the critical density is missing! Doing the bookkeeping more precisely, $`\mathrm{\Omega }_X=0.67\pm 0.06`$.

In order to have escaped detection, this missing energy must be smoothly distributed. In order not to interfere with the formation of structure (by inhibiting the growth of density perturbations), the energy density in this component must change more slowly than matter (so that it was subdominant in the past). For example, if the missing 2/3 of critical density were smoothly distributed matter ($`p=0`$), then linear density perturbations would grow as $`R^{1/2}`$ rather than as $`R`$. The shortfall in growth since last scattering ($`z1100`$) would be a factor of 30, far too little growth to produce the structure seen today.

The pressure associated with the missing energy component determines how it evolves:

$`\rho _X`$ $``$ $`R^{3(1+w)}`$
$`\rho _X/\rho _M`$ $``$ $`(1+z)^{3w}`$ (2)
where $`w`$ is the ratio of the pressure of the missing energy component to its energy density (here assumed to be constant). Note, the more negative $`w`$, the faster the ratio of missing energy to matter decreases to zero in the past. In order to grow the structure observed today from the density perturbations indicated by CMB anisotropy measurements, $`w`$ must be more negative than about $`\frac{1}{2}`$.

For a flat Universe the deceleration parameter today is

$$q_0=\frac{1}{2}+\frac{3}{2}w\mathrm{\Omega }_X\frac{1}{2}+w$$

Therefore, knowing $`w<\frac{1}{2}`$ implies $`q_0<0`$ and accelerated expansion. This independent argument for accelerated expansion and dark energy makes the supernova case all the more compelling.

### 3.2 Gravity Can Be Repulsive in Einstein’s Theory, But …

In Newton’s theory, mass is the source of the gravitational field and gravity is always attractive. In General Relativity, both energy and pressure source the gravitational field: $`\ddot{R}/R(\rho +3p)`$, cf., Eq. 1. Sufficiently large negative pressure leads to repulsive gravity.

While accelerated expansion can be accommodated within Einstein’s theory, that does not preclude that the ultimate explanation lies in a fundamental modification of Einstein’s theory. Lacking any good ideas for such a modification, I will discuss how accelerated expansion fits in the context of General Relativity. If the explanation for the accelerating Universe ultimately fits within the Einsteinian framework, it will be a stunning new triumph for General Relativity.

### 3.3 The Biggest Embarrassment in all of Theoretical Physics

Einstein introduced the cosmological constant to balance the attractive gravity of matter. He quickly discarded the cosmological constant after the discovery of the expansion of the Universe.

The advent of quantum field theory made consideration of the cosmological constant obligatory, not optional: The only possible covariant form for the energy of the (quantum) vacuum,

$$T_{\mathrm{VAC}}^{\mu \nu }=\rho _{\mathrm{VAC}}g^{\mu \nu },$$

is mathematically equivalent to the cosmological constant. It takes the form for a perfect fluid with energy density $`\rho _{\mathrm{VAC}}`$ and isotropic pressure $`p_{\mathrm{VAC}}=\rho _{\mathrm{VAC}}`$ (i.e., $`w=1`$) and is precisely spatially uniform. Vacuum energy is almost the perfect candidate for dark energy.

Here is the rub: the quantum zero-point contributions arising from well-understood physics (the known particles, integrating up to $`100`$GeV) sum to $`10^{55}`$ times the present critical density. (Put another way, if this were so, the Hubble time would be $`10^{10}`$sec, and the associated event horizon would be 3 cm!) This is the well known cosmological-constant problem.

While string theory currently offers the best hope for marrying gravity to quantum mechanics, it has shed precious little light on the cosmological constant problem, other than to speak to its importance. Thomas has suggested that using the holographic principle to count the available number of states in our Hubble volume leads to an upper bound on the vacuum energy that is comparable to the energy density in matter + radiation. While this reduces the magnitude of the cosmological-constant problem very significantly, it does not solve the dark energy problem: a vacuum energy that is always comparable to the matter + radiation energy density would strongly suppress the growth of structure.

The deSitter space associated with the accelerating Universe may pose serious problems for the formulation of string theory. Banks and Dine argue that all explanations for dark energy suggested thus far are incompatible with perturbative string theory. At the very least there is high tension between accelerated expansion and string theory.

The cosmological constant problem leads to a fork in the dark-energy road: one path is to wait for theorists to get the “right answer” (i.e., $`\mathrm{\Omega }_X=2/3`$); the other path is to assume that even quantum nothingness weighs nothing and something else with negative pressure must be causing the Universe to speed up. Of course, theorists follow the advice of Yogi Berra: “When you see a fork in the road, take it.”

### 3.4 Parameterizing Dark Energy: For Now, It’s $`w`$

Theorists have been very busy suggesting all kinds of interesting possibilities for the dark energy: networks of topological defects, rolling or spinning scalar fields (quintessence and spintessence), influence of “the bulk”, and the breakdown of the Friedmann equations. An intriguing recent paper suggests dark matter and dark energy are connected through axion physics.

In the absence of compelling theoretical guidance, there is a simple way to parameterize dark energy, by its equation-of-state $`w`$.

The uniformity of the CMB testifies to the near isotropy and homogeneity of the Universe. This implies that the stress-energy tensor for the Universe must take the perfect fluid form. Since dark energy dominates the energy budget, its stress-energy tensor must, to a good approximation, take the form

$$T_{X}^{}{}_{\nu }{}^{\mu }\mathrm{diag}[\rho _X,p_X,p_X,p_X]$$
(3)
where $`p_X`$ is the isotropic pressure and the desired dark energy density is

$$\rho _X=2.7\times 10^{47}\mathrm{GeV}^4$$

(for $`h=0.72`$ and $`\mathrm{\Omega }_X=0.66`$). This corresponds to a tiny energy scale, $`\rho _X^{1/4}=2.3\times 10^3`$eV.

The pressure can be characterized by its ratio to the energy density (or equation-of-state):

$$wp_X/\rho _X$$

Note, $`w`$ need not be constant; e.g., it could be a function of $`\rho _X`$ or an explicit function of time or redshift. ($`w`$ can always be rewritten as an implicit function of redshift.)

For vacuum energy $`w=1`$; for a network of topological defects $`w=N/3`$ where $`N`$ is the dimensionality of the defects (1 for strings, 2 for walls, etc.). For a minimally coupled, rolling scalar field,

$$w=\frac{\frac{1}{2}\dot{\varphi }^2V(\varphi )}{\frac{1}{2}\dot{\varphi }^2+V(\varphi )}$$
(4)
which is time dependent and can vary between $`1`$ (when potential energy dominates) and $`+1`$ (when kinetic energy dominates). Here $`V(\varphi )`$ is the potential for the scalar field.

### 3.5 The Universe: The Lab for Studying Dark Energy

Dark energy by its very nature is diffuse and a low-energy phenomenon. It probably cannot be produced at accelerators; it isn’t found in galaxies or even clusters of galaxies. The Universe itself is the natural lab – perhaps the only lab – in which to study it.

The primary effect of dark energy on the Universe is determining the expansion rate. In turn, the expansion rate affects the distance to an object at a given redshift $`z`$ \[$`r(z)`$\] and the growth of linear density perturbations. The governing equations are:

$`H^2(z)`$ $`=`$ $`H_0^2(1+z)^3\left[\mathrm{\Omega }_M+\mathrm{\Omega }_X(1+z)^{3w}\right]`$
$`r(z)`$ $`=`$ $`{\displaystyle _0^z}𝑑u/H(u)`$
$`0`$ $`=`$ $`\ddot{\delta }_k+2H\dot{\delta }_k4\pi G\rho _M\delta _k`$ (5)
where for simplicity $`w`$ is assumed to be constant and $`\delta _k`$ is the Fourier component of comoving wavenumber $`k`$ and overdot indicates $`d/dt`$.

The various cosmological approaches to ferreting out the nature of the dark energy – all of which depend upon how the dark energy affects the expansion rate – have been studied. Based largely upon my work with Dragan Huterer, I summarize what we now know about the efficacy of the cosmological probes of dark energy:

* Present cosmological observations prefer $`w=1`$, with a 95% confidence limit $`w<0.6`$.
* Because dark energy was less important in the past, $`\rho _X/\rho _M(1+z)^{3w}0`$ as $`z\mathrm{}`$, and the Hubble flow at low redshift is insensitive to the composition of the Universe, the most sensitive redshift interval for probing dark energy is $`z=0.22`$.
* The CMB has limited power to probe $`w`$ (e.g., the projected precision for Planck is $`\sigma _w=0.25`$) and no power to probe its time variation.
* A high-quality sample of 2000 SNe distributed from $`z=0.2`$ to $`z=1.7`$ could measure $`w`$ to a precision $`\sigma _w=0.05`$ (assuming an irreducible systematic error of 0.14 mag). If $`\mathrm{\Omega }_M`$ is known independently to better than $`\sigma _{\mathrm{\Omega }_M}=0.03`$, $`\sigma _w`$ improves by a factor of three and the rate of change of $`w^{}=dw/dz`$ can be measured to precision $`\sigma _w^{}=0.16`$.
* Counts of galaxies and of clusters of galaxies may have the same potential to probe $`w`$ as SNe Ia. The critical issue is systematics (including the evolution of the intrinsic comoving number density, and the ability to identify galaxies or clusters of a fixed mass).
* Measuring weak gravitational lensing by large-scale structure over a field of 1000 square degrees (or more) could have comparable sensitivity to $`w`$ as type Ia supernovae. However, weak gravitational lensing does not appear to be a good method to probe the time variation of $`w`$. The systematics associated with weak gravitational lensing have not yet been studied carefully and could limit its potential.

With the exception of vacuum energy, all the other possibilities for the dark energy cluster to some small extent on the largest scales. Measuring this clustering, while extremely challenging, could rule out vacuum or help to elucidate the nature of the dark energy. Hu and Okamoto have recently suggested how the CMB might be used to get at this clustering.

While the Universe is likely the lab where dark energy can best be attacked, one should not rule other approaches. For example, if the dark energy involves a ultra-light scalar field, then there should be a new long-range force.

### 3.6 The Nancy Kerrigan Problem

A critical constraint on dark energy is that it not interfere with the formation of structure in the Universe. This means that dark energy must have been relatively unimportant in the past (at least back to the time of last scattering, $`z1100`$). If dark energy is characterized by constant $`w`$, not interfering with structure formation can be quantified as: w
<12
<𝑤12w\mathrel{\mathchoice{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\displaystyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\textstyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptstyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}{\lower 3.6pt\vbox{\halign{$\mathsurround=0pt\scriptscriptstyle\hfil#\hfil$\cr<\crcr\sim\crcr}}}}-{1\over 2}. This means that the dark-energy density evolves more slowly than $`R^{3/2}`$ (compared to $`R^3`$ for matter) and implies

$`\rho _X/\rho _M`$ $``$ $`0\mathrm{for}t0`$
$`\rho _X/\rho _M`$ $``$ $`\mathrm{}\mathrm{for}t\mathrm{}`$
That is, in the past dark energy was unimportant and in the future it will be dominant! We just happen to live at the time when dark matter and dark energy have comparable densities. In the words of Olympic skater Nancy Kerrigan, “Why me? Why now?”

Perhaps this fact is an important clue to unraveling the nature of the dark energy. Perhaps not. I shudder to say this, but it could be at the root of an anthropic explanation for the size of the cosmological constant: The cosmological constant is as large as it can be and still allow the formation of structures that can support life.

### 3.7 Dark Energy and Destiny

Almost everyone is aware of the connection between the shape of the Universe and its destiny: positively curved recollapses, flat; negatively curved expand forever. The link between geometry and destiny depends upon a critical assumption: that matter dominates the energy budget (more precisely, that all components of matter/energy have equation of state $`w>\frac{1}{3}`$). Dark energy does not satisfy this condition.

In a Universe with dark energy the connection between geometry and destiny is severed. A flat Universe (like ours) can continue expanding exponentially forever with the number of visible galaxies diminishing to a few hundred (e.g., if the dark energy is a true cosmological constant); the expansion can slow to that of a matter-dominated model (e.g., if the dark energy dissipates and becomes sub-dominant); or, it is even possible for the Universe to recollapse (e.g., if the dark energy decays revealing a negative cosmological constant). Because string theory prefers anti-deSitter space, the third possibility should not be forgotten.

Dark energy is the key to understanding our destiny.

## 4 Closing Remarks

As a New Cosmology emerges, a new set of questions arises. Assuming the Universe inflated, what is the physics underlying inflation? What is the dark-matter particle? How was the baryon asymmetry produced? Why is the recipe for our Universe so complicated? What is the nature of the Dark Energy? Answering these questions will help us make sense of the New Cosmology as well as revealing deep connections between fundamental physics and cosmology. There may even be some big surprises – time variation of the constants of Nature, or a new theory of gravity that eliminates the need for dark matter and dark energy (though I for one am not betting on either!).

There is an impressive program in place, with telescopes, accelerators, and laboratory experiments, both in space and on the ground: the Sloan Digital Sky Survey; the Hubble Space Telescope and the Chandra X-ray Observatory; a growing number of large ground-based telescopes; the Tevatron and B-factories in the US and Japan; specialized dark-matter detectors; gravity-wave detectors; a multitude of ground-based and balloon-borne CMB anisotropy experiments; the MAP satellite (which is already taking data) and the Planck satellite (to be launched in 2007). Still to come are: the LHC; a host of accelerator and nonaccelerator neutrino-oscillation and neutrino-mass experiments; the Next Generation Space Telescope; gravity-wave detectors in space; cluster surveys using x-rays and the Sunyaev – Zel’dovich effect. And in the planning: dedicated ground and space based wide-field telescopes to study dark energy, the next linear collider and on and on. Any one, or more likely several, of these experiments will produce major advances in our understanding of the Universe and the fundamental laws that govern it.

The progress we make over the two decades will determine how golden our age of cosmology is.

## Acknowledgments

This work was supported by the DoE (at Chicago and Fermilab) and by the NASA (at Fermilab by grant NAG 5-7092).


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# Effect of CH4 addition on excess electron mobility in liquid Kr

## I Introduction

The study of electron conduction in nonpolar liquids is of great fundamental and technical interest holsch89 ; hatano97 . Non polar liquids are examples of simple disordered materials. Theoretical investigations of the electronic states in such media are connected to experiment by the low field behavior of the excess electron mobility finn86 . The properties of excess electrons in such media may also give useful information on the electronic states in noncrystalline solids doke ; yoshino76 ; sowada77 .

Non polar liquids are also used as sensitive media in high–energy physics ionization detectors. For such an application it is essential to know the behavior of excess electrons in the high–field region, where detectors are typically operated, in order to understand the basic electronic conduction mechanisms in that particular range for the goal of optimizing the detectors’ performances schmidt97 .

Liquified heavy noble gases, Ar, Kr, and Xe, are mainly used in ionization chambers because of the combination of large density and high values of the excess electron mobilities. At small electric fields mobilities exceeding several hundreds of $`cm^2/Vs`$ have been measured miller ; schnyders ; kf ; halpern ; freemanxe ; eibl ; lamp . In these so–called high–mobility liquids electrons are assumed to be quasifree because their mean free path is relatively long although they are moving in a very dense environment of atoms which are very effective scattering centers in the gas phase holsch89 .

At small electric fields electrons are in near thermal equilibrium with the atoms of the host medium. The electron mobility is determined by processes of elastic scattering and is approximately independent of the field strength. In this region the drift velocity increases linearly with the field strength. At higher values of the field the electron drift velocity increases less than proportionally with the field and, finally, it nearly saturates. This behavior is related to the increase of the mean electron energy with the field and to the dependence of the scattering rate on the electron energy.

It has been shown yoshino76 ; sakai ; rahm ; seguinot ; vuillemin ; BIC  that the addition of a molecular or atomic solute in small proportion influences the dependence of the mobility on the field strength, especially at high fields. In particular, the saturation drift velocity is largely increased above the value in the pure liquid. This effect is commonly explained as due to a reduction of the electron mean energy upon additional inelastic scattering with the impurities. These act as additional scattering centers that are very effective in thermalizing electrons even at quite large field strengths. In particular, for a spherical symmetric molecule like CH$`_4,`$ the inelastic processes are assumed to be due to the excitation of the main vibrational levels of the molecule (0.16 and 1.75 $`eV)`$ sakai ; sakai2  upon collisions with energetic enough electrons .

The search for the optimum combination of base liquid and impurity for the best detector performance is far from being concluded rahm ; seguinot ; vuillemin .

These mobility measurements are obviously important for detectors’ designers. However, from a fundamental point of view these data may give additional hints for the description of the electron mobility in liquids, which is not yet completely understood holsch89 . In fact, the theoretical treatment of the field behavior of the mobility in a pure liquid is far from being satisfactory.

The description of the electron mobility in the liquid can be approached from two completely opposite directions. The first approach is the so called single–scattering picture, essentially due to Lekner lek1 ; lek2 , in which electrons scatter off single atoms of the liquid or, more precisely, they undergo a binary collision with a single interaction potential that takes into account contributions from the potentials of nearby atoms. In this model, the two–term solution of the Boltzmann transport equation hux ; phelps  allows the calculation of an energy–dependent scattering cross section.

At the opposite extreme, the deformation potential theory of Basak and Cohen (BC) BC  represents the motion of the quasi–free electrons in the liquid as that of a wave in a quasi–periodic structure. In this model the electron mobility in a liquid is determined by the scattering produced by fluctuations of the bottom of the conduction band due to the intrinsic density fluctuations of the liquid.

In the latter model, the addition of a solute is assumed to enhance the disorder inherent to a fluid by introducing concentration fluctuations in addition to the usual density fluctuations. In the former one, many–body and multiple scattering effects are included in the cross sections, which have now to be determined by a fit to the experimental data.

On one hand, the BC model has been adapted with reasonable success to mixtures of liquid hydrocarbons, where both solvent and solute are liquid at the same temperature kengo . Unfortunately, its predictions have proven completely wrong when it is used for the description of the electron mobility in liquid mixtures of noble gases, namely Kr or Xe in liquid Ar BIC .

A further drawback of the BC model, and of its extension to mixtures, is that it makes predictions only on the zero–field mobility and does not describe its electric–field dependence, which, on the contrary, is very important from the point of view of detectors’ design.

On the other hand, the single–scattering (or gas–kinetic) approach has been succesfully used to describe the electric field dependence of the electron mobility in liquid Ar and methane kaneko ; kaneko2  by introducing two constant scattering cross sections, the momentum– and energy–transfer cross sections, in the wake of Lekner’s theory. In this model, the many–body and multiple scattering effects due to the combined effect of short interatomic distances and large electron wavelength are embodied in the effective cross sections. This dressing of the scattering cross section due to multiple scattering effects is also at the base of the heuristic kinetic model, developed for the successful description of the electron mobility in dense noble gases borg1 ; borg2 ; borg3 ; borg4 .

The same gas–kinetic approach has proven also quite succesful in the case of mixtures of liquified noble gases BIC . Although in pure Ar and CH4 the choice of two constant cross sections provides a quite nice agreement with the experimental data kaneko ; kaneko2 , an even better description of the electron mobility as a function of the electric field for all impurity concentrations in the mixtures of liquified noble gases is obtained by assuming a constant momentum transfer cross section $`\sigma _m`$ and an energy–transfer cross section $`\sigma _E`$ inversely proportional to the electron energy $`ϵ,`$ $`\sigma _E1/ϵ`$ BIC . This dependence has been chosen only on a phenomenological basis and its meaning is not clear yet. However, since in this gas–kinetic model the cross sections are treated as adjustable parameters, it can be only said that this energy–dependent energy–transfer cross section provides a much better fit to the experimental data than a constant cross section does.

In this work we have therefore more carefully investigated the effect of the addition of the molecular solute CH4 to pure liquid Kr, with emphasis on the low– and intermediate–field behavior of the mobility. Preliminary measurements, especially concerned with the mobility behavior at high fields, have been reported previously folegani , keeping in mind the application of such mixtures in ionization detectors. We report here a more complete study that includes new measurements at quite small electric field strengths aimed at a more physical goal.

This goal is twofold. On one hand, this mixture has never been studied before and might be promising as a medium for ionization detectors. On the other hand, it represents a different benchmark for the validation of the gas–kinetic model and the determination of the concentration dependence of the effective cross sections might contribute useful pieces of information on the effectiveness of elastic and inelastic electron scattering processes in the liquid.

## II Experiment

The experimental apparatus has been described elsewhere folegani  and we refer to literature for the details. We recall here only the essential features of the experiment. The cell is a typical double–gridded ionization chamber. Excess electrons are photoextracted from a Ni–coated brass cathode by a short pulse of ultraviolet light produced by a Xe flashlamp. The four electrodes, anode, cathode and the two grids, are kept at suitable voltages in order to ensure the maximum grid transparency bunne . Several guard rings are kept at the appropriate voltage by a resistor cascade in order to ensure the maximum field uniformity in the cylindrical drift space.

The electrodes are connected to charge amplifiers. The signal induced by the drifting electrons is recorded by a digital oscilloscope and analyzed by means of a personal computer. The drift time can be easily determined by analyzing the signal shape. To span a large region of electric fields in a single sweep both the drift times between the cathode and the first grid and between the first and the second grid are recorded simultaneously. The drift time in the region between the second grid and the anode, owing to the short distance and to the strong field between these two electrodes, cannot be measured reliably and has not been recorded. The two sets of drift mobility measured in the first and second region agree well with each other within the experimental accuracy where the field values overlap. The overall accuracy of the mobility measurements is better than 10 %.

Very pure, commercially available gaseous mixtures of CH4 in Xe of different and known composition are condensed in the cell through an Oxisorb purifier to remove oxygen and water vapor impurities. The cell is cooled down to the desired temperature by immersion in an isopentane bath cooled by liquid N$`_2.`$ Two thermoresistors located in the cell near the cathode and the anode, respectively, provide constant monitoring of the temperature. The temperature is stable within $`\pm 0.5K.`$

## III Experimental Results and Discussion

The excess electron mobility in liquid Kr has been measured as a function of the electric field strength up to $`E10kV/cm`$ at $`T130K`$ for several mixtures of different composition. The liquid density of pure Kr at the temperature of the experiment is $`N167\times 10^{26}m^3.`$ The CH4 concentration, $`x,`$ of the mixtures is $`x=`$ 0.01, 0.1, 0.5, 1, 2, 3, 5, and 10 %, respectively. As a calibration we have also measured the mobility in pure liquid Krypton. Our data in the pure liquid agree well with literature data finn86 .

We report the mobility as a function of the electric field strength $`E`$ for several of the mixtures under investigation in Figure 1 and Figure 2 in order to avoid overcrowding of the figures. All mixtures show similar features.

As usual, the electron mobility $`\mu `$ shows a low–field behavior where it is essentially independent of the electric field. In this region the excess electrons are in near thermal equilibrium with the atoms of the liquid, do not gain very much energy from the electric field, and mainly undergo elastic collisions that determine the mobility.

At higher fields, the mobility depends on the field strength and decreases sharply with increasing field. In this region the mean electron energy is greatly enhanced by the field and the net effect is a large increase of the scattering rate, leading to the observed decrease of the mobility. This behavior is common to all mixtures with some important differences.

At small concentration of methane the effect of the solute on the zero–field mobility $`\mu _0`$ is not very large. Only for the highest CH4 concentration $`(x10\%)`$, there is a significant reduction of $`\mu _0,`$ as shown in figure 3. Small concentrations, as evident from Figures 1 and 2, do mostly influence the high–field behavior of the mobility. An influence on momentum transfer is obtained only at high methane concentrations. This behavior is similar to that observed in mixtures of light alkanes in liquified noble gases yoshino76 . However, this is the first time for this behavior to be observed in the present mixture of CH4 in liquid Kr.

Moreover, it has to be noted that the situation in mixtures of liquified noble gases is completely different as far as $`\mu _0(x)`$ is concerned BIC . In fact, in the liquid Ar–Kr and liquid Ar–Xe mixtures, $`\mu _0`$ decreases rapidly with increasing solute concentration, especially in the Ar–Xe mixture. In the Ar–Kr mixture, where a concentration of $`30\%`$ is reached, $`\mu _0`$ eventually levels off and becomes nearly concentration independent. In the Ar–Xe mixture, for concentration up $`x5\%,`$ $`\mu _0`$ decreases linearly with large neative slope as $`x`$ is increased.

The sharp decrease of $`\mu `$ with increasing $`E`$ at larger fields (see Figures 1 and 2) is commonly attributed to the increase of the mean electron energy with increasing electric field. Between collisions, at higher fields, electrons pick up more energy from the field than they are able to share with the liquid upon collisions and thus become epithermal. The scattering rate is consequently enhanced and the mobility decreases.

The change of the electric field dependence of the mobility (see Figures 1 and 2) is therefore due to the increase of the mean electron energy above the thermal value because of the applied electric field. Upon increasing the methane concentration in the mixture, the region where the mobility is field independent spans a wider field range and the transition to the hot–electron behavior shifts to larger field strengths. Moreover, in the epithermal region, higher field strengths are required, upon increasing the impurity concentration, in order to achieve the same mobility value. Since $`\mu `$ depends on the mean electron energy only, provided that all other parameters are kept fixed, this fact means that electrons reach the same mean energy at larger fields for increasingly higher concentration of impurities.

These observations confirm the assumption that molecular impurities are very effective in thermalizing electrons at larger fields although they are not as effective as atomic impurities as far as momentum transfer is concerned. Molecular impurities act as additional scattering centers for electrons where they might lose energy in inelastic collisions more efficiently than in the pure liquid.

A similar behavior has been observed also in liquid mixtures of liquified noble gases BIC , where atomic impurities Xe and Kr were dissolved in liquid Ar. Also in that case, atomic impurities extend the range of the thermal behavior of electrons. However, a stronger dependence of $`\mu _0`$ on the impurity concentration was observed. This behavior is probably related to the fact that atomic impurities have fewer inelastic scattering channels for low–energy electrons than molecular impurities do and affect more effectively the momentum–transfer– rather than the energy–transfer processes.

At high fields the drift mobility is determined essentially by the relative magnitudes of elastic and inelastic energy loss rate. When inelastic losses become greater than the elastic ones the drift mobility increases above the value of the pure liquid.

In order to carry out a simple analysis of the experimental data, we adopt the gas–kinetic approach of Kaneko et al., based on the two–term solution of the Boltzmann transport equation kaneko ; kaneko2 . For a simple fluid of number density $`N,`$ the mobility $`\mu `$ is given by the usual formula lek1 ; lek2 ; hux

$$\mu =\left(\frac{e}{3}\right)\left(\frac{2}{m}\right)^{1/2}\underset{0}{\overset{\mathrm{}}{}}\frac{ϵ}{N\sigma _m\left(ϵ\right)}\left[\frac{\mathrm{d}g\left(ϵ\right)}{\mathrm{d}ϵ}\right]dϵ$$
(1)
where $`\sigma _m(ϵ)`$ is the energy–dependent momentum–transfer scattering cross section. $`e`$ and $`m`$ are the electron charge and mass, respectively. The Davydov–Pidduck electron energy distribution function $`g(ϵ)`$ is given by

$$g\left(ϵ\right)=A\mathrm{exp}\left\{\underset{0}{\overset{ϵ}{}}\frac{\mathrm{d}z}{k_\mathrm{B}T+\left(\frac{M}{6m}\right)\left(\frac{eE}{N}\right)^2\frac{1}{z\sigma _m\left(z\right)\sigma _E\left(z\right)}}\right\}$$
(2)
where $`M`$ is the atomic (molecular) mass, $`\sigma _E\left(ϵ\right)`$ is the energy–dependent energy–transfer scattering cross section. The constant $`A`$ is fixed by the normalization condition $`_0^{\mathrm{}}\sqrt{z}g\left(z\right)dz=1.`$

From Eqns. 1 and 2 it is evident that the mobility is primarily determined by the momentum–transfer cross section, but the energy–transfer cross section also affects the mobility because it influences the electron energy distribution function by controlling the rate at which energy is exchanged.

Strictly speaking, in order to account properly for the scattering of electrons off correlated atoms in the fluid lek3 , Eq. 1 should be divided by the long–wavelength limit $`S(0)`$ of the static structure factor, that takes into account the compressibility of the medium. However, according to Kaneko et al., we set $`S(0)=1`$ and every correlation effect is now accounted for by the effective cross section determined in this way.

By introducing constant values for the two relevant cross section $`\sigma _m`$ and $`\sigma _E100\sigma _m,`$ this model reproduces quite well the low–field limit of the experimental mobility in liquid Ar and CH$`_4,`$ but is not very accurate in the high–field region kaneko ; kaneko2 .

A great improvement for the description of the mobility in this region has been obtained by introducing an energy–dependent energy–transfer cross section of the form BIC

$$\sigma _E\left(ϵ\right)=\sigma _{E_0}\left(\frac{\pi k_\mathrm{B}T}{ϵ}\right)$$
(3)
where $`k_\mathrm{B}`$ is the Boltzmann constant and $`T`$ is the temperature.

This particular choice is heuristic and does not rely on any theory. However, it is interesting to note that $`\pi k_\mathrm{B}T/ϵ`$ is the square of the ratio of the de Broglie wavelength of an electron of energy $`ϵ,`$ $`\lambda =h/\sqrt{2mϵ},`$ to its thermal value, $`\lambda _T=h/\sqrt{2m\pi k_\mathrm{B}T}.`$ In other words, it seems that upon collisions the electron is exchanging energy with a cross section proportional to the cross sectional area of the associated quantum wavepacket. In order to test this view, mobility measurements should be carried out as a function of temperature. Anyway, we do not insist on this point since it is merely speculative.

With the introduction of the analytic form of $`\sigma _E`$ given in Eq. 3, the integrals in Eqns. 1 and 2 can be solved analytically, yielding

$$\mu =\mu _0\left[1+\left(\frac{M}{6\pi m}\right)\left(\frac{eE}{Nk_\mathrm{B}T}\right)^2\left(\sigma _m\sigma _{E_0}\right)^1\right]^{1/2}$$
(4)
with the usual expression for $`\mu _0`$

$$\mu _0=\frac{4e}{3N\sigma _m\sqrt{2\pi mk_\mathrm{B}T}}$$
(5)
It is easy to show that with this choice of $`\sigma _E,`$ at high–fields $`\mu E^1,`$ so that the drift velocity turns out to be approximately constant, as experimentally observed.

The extension of this model to binary mixtures is easily accomplished by introducing the concept of an equivalent one–component fluid with density $`N`$ and mass $`M`$ of the pure solvent (in this case, Kr) but described by effective scattering cross sections $`\sigma _m(x)`$ and $`\sigma _{E_0}(x),`$ which now depend on the solute concentration BIC .

We have therefore analyzed the present data according to Ref. BIC , by assuming, for each mixtures of concentration $`x,`$ that the momentum transfer cross section is energy independent $`\sigma _m(x,ϵ)\sigma _m(x),`$ and that the energy–transfer cross section is proportional to the inverse electron energy as described by Eq. 3 with $`\sigma _{E_0}\sigma _{E_0}(x).`$

Eq. 4 has been fitted to the present experimental data with $`\sigma _m`$ and $`\sigma _{E_0}`$ as adjustable parameters. In figure 4 we show the values of the parameters resulting from the fit.

The momentum transfer cross section strictly reflects the behavior of $`\mu _0`$ as a function of the methane concentration. This is obvious by inspecting Eq. 5. Its value is $`\sigma _m(6÷7)\times 10^2`$ Å2 and raises up to $`9\times 10^2`$ Å2 at the largest methane concentration. These values can be compared to the value $`(0.1÷0.4)`$ Å2 of the momentum transfer scattering cross section of atomic Kr at the Ramsauer minimum around $`0.5÷0.7eV`$ zecca .

In the present mixtures, $`\sigma _m`$ is approximately 3-4 times smaller than the value $`\sigma _m0.2`$ Å2 obtained for pure liquid Ar BIC , as a result of the fact that also in pure liquid Kr electrons are more mobile than in pure liquid Ar yoshino76 . The behavior of $`\sigma _{E_0}(x)`$ is very different in comparison with that of $`\sigma _m(x).`$ It shows a large and almost linear increase with increasing methane concentrations. At $`x=0,`$ $`\sigma _{E_0}2`$ Å$`^2,`$ to be compared to the value $`\sigma _{E_0}10`$ Å2 found in pure liquid Ar BIC . For $`x=10\%,`$ $`\sigma _{E_0}170`$ Å$`^2.`$ This confirms the fact that the increase of the concentration of methane in liquid Kr strongly enhances the inelastic processes leading to electron energy relaxation, while it has a nearly negligible effect on the processes of momentum transfer.

It is not completely surprising that the energy transfer cross section is much larger than the momentum transfer one because, as already pointed out in literature BIC ; lek1 ; lek2 , the efficiency of energy transfer for thermal electrons is larger than that of momentum transfer by a factor $`1/S(0)1.`$ In any case, we have to stress the fact that the behavior of the cross section with the concentration confirms the picture that the addition of a molecular solute increases the chance of an electron undergoing scattering.

In figure 5 we show the result of this kind of fit for the mixture with $`x5\%.`$ A similar behavior is found in all mixtures. It is easily observed that Eq. 4 correctly fits the data only up to intermediate field strengths, of the order of several hundreds of $`V/cm,`$ depending on the solute concentration. For larger values, $`\mu `$ decreases less rapidly with increasing $`E.`$ Its field dependence changes from the $`E^1`$ behavior, predicted by Eq. 4 with $`\sigma _E`$ given by Eq. 3, to a softer $`E^{1/2}`$ behavior. This effect is observed for all mixtures.

This new kind of field dependence at large fields is typical for constant cross sections. Therefore, at larger fields, hence at larger mean electron energies, the scattering events determining the mobility resemble those due to a gas of hard spheres. However, we have to recall that this kind of language is more pictorial than real, because we are considering effective cross sections dressed by many body and multiple scattering effects in a gas–kinetic model rather than real two–body collisions.

In the same Figure 5 we show the prediction of the gas–kinetic model where we have introduced a constant $`\sigma _E,`$ in order to simulate the results of hard–sphere scattering. The two curves in the figure have been obtained with $`\sigma _E=\sigma _{E_0}`$ (dashed line), with the value of $`\sigma _{E_0}`$ determined by the fit with Eq. 4, and with $`\sigma _E=(2\pi /3)\sigma _{E_0}`$ (dashed–dotted line), i.e., at thermal energy. In both cases, the calculated mobility at high fields is nearly parallel to the experimental data.

In any case, the deviation of the mobility from the $`E^1`$behavior towards the $`E^{1/2}`$one indicates that the processes of inelastic energy transfer are changing somewhat with the electron energy, as though different inelastic channels were opened by increasing the mean electron energy, leading to a different energy dependence of $`\sigma _E.`$

For the sake of completeness, it has to be noted that this change of behavior, though less relevant, is observed also in pure liquid Kr. A possible explanation of the effect in the pure liquid might be related to the possible existence of the Ramsauer minimum of the cross section also in the liquid, as argued by Christophorou et al. christo . In this case, at high fields, the electron energy distribution function is very broad and the cross section would be averaged across the Ramsauer minimum, thus yielding approximately a constant value.

A careful inspection of the $`\mu (E)`$ data shows that $`\mu `$ deviates from the $`E^1`$behavior when it approximately has the same value (within a factor of order unity) for each mixture. In other words, the deviation takes place when the mean electron energy is approximately the same in all mixtures, independently of the methane concentration. This confirms the hypothesis that new inelastic channels related to the molecular impurity open up when the mean electron energy exceeds a given threshold.

To give an estimate of the effect, in figure 6 we plot the value $`E^{}`$ of the field where $`\mu `$ takes on the value $`\mu ^{}`$ and starts deviating from the $`E^1`$ behavior. This threshold electric field has a nice square–root dependence on the CH4 concentration. This is easy to understand analytically if one inverts Eq. 4 with $`\mu ^{}/\mu _0(x)`$ and $`\sigma _m(x)`$ approximately constant, thus obtaining

$$E^{}=\left\{\frac{6\pi m}{M}\left[\left(\frac{\mu _0}{\mu ^{}}\right)^21\right]\left(\frac{Nk_\mathrm{B}T}{e}\right)^2\sigma _m\sigma _{E_0}\right\}^{1/2}$$
(6)
By inspecting figure 4 one observes that $`\sigma _{E_0}(x)`$ increases linearly, to a very good approximation, with $`x.`$ Hence, $`E^{}`$ is approximately proportional to $`x^{1/2}.`$ This observation is another confirmation of the fact that electrons are more efficiently thermalized by increasing the impurity content of the mixture.

Within this gas–kinetic model, the mean electron energy can be calculated as $`ϵ=_0^{\mathrm{}}z^{3/2}g(z)dz,`$ where $`g(z)`$ is given by Eq. 2. If the analytic form Eq. 3 for the energy–transfer cross section and a constant momentum–transfer cross sections are used, the mean electron energy turns out to be given by

$$ϵ=\frac{3}{2}\left[k_\mathrm{B}T+\left(\frac{M}{6\pi mk_\mathrm{B}T\sigma _m\sigma _{E_0}}\right)\left(\frac{eE}{N}\right)^2\right]$$
(7)
At the field $`E^{},`$ where the high–field dependence of the mobility changes from $`E^1`$ to $`E^{1/2},`$ the mean electron energy takes on the value $`ϵ^{}`$ shown in Figure 7. Beside a small decrease with increasing concentration, $`ϵ^{}`$ is close to 0.15 $`eV,`$ quite consistent with the value 0.16 $`eV`$ reported in literaturesakai ; sakai2  for the excitation of the main vibrational level of CH$`_4.`$ This result further confirms the conclusion that the change of the high–field behavior of the mobility is related to the opening of molecular inelastic channels of energy transfer.

## IV Conclusions

As observed in many other liquid mixtures, also in CH$`{}_{4}{}^{}`$doped liquid Kr the addition of molecular impurities increases the efficiency of electron thermalization. This fact permits to increase the drift velocity of electrons in the mixtures used as sensitive media in ionization detectors with respect to case of the pure liquid.

The use of the gas–kinetic approach also in liquid mixtures to describe the electric field dependence of the electron mobility gives very nice results. It is a very simple model that relies on a very easy physical picture to grasp, namely a binary–collisions picture. Nonetheless, in spite of its simplicity, the gas–kinetic model gives useful information about the relative strength of elastic and inelastic processes through the magnitude and concentration dependence of the effective cross sections, $`\sigma _m`$ for the momentum–transfer and $`\sigma _E`$ for the energy transfer.

In the case of CH$`{}_{4}{}^{}`$doped liquid Kr, the molecular solute has a relatively small influence on the momentum–transfer processes, as deduced from the fact that the zero–field mobility $`\mu _0`$ does not depend very much on the methane concentration. On the contrary, CH4 impurities originate an efficient energy relaxation of excess electrons. This fact has the consequence that collisional ionization of the liquid mixture should be more difficult to reach, yielding higher breakdown fields in the mixtures than in the pure liquid.

## Captions to the Figures

* Electron mobility in pure liquid Kr (closed circles) and in several liquid Kr–CH4 mixtures. Solid triangles: $`x=0.5\%.`$ Solid squares: $`x=5\%.`$ Open circles: $`x=10\%.`$ $`x`$ is the methane concentration. The error bars, of the order 5–10 %, are not shown for the sake of clarity.
* Electron mobility in several liquid Kr–CH4 mixtures. Closed diamonds: $`x=0.01\%.`$ Solid triangles: $`x=0.1\%.`$ Open squares: $`x=1\%.`$ Closed squares: $`x=2\%.`$ Open circles: $`x=3\%.`$ $`x`$ is the methane concentration. The error bars, of the order 5–10 %, are not shown for the sake of clarity.
* Zero–field electron mobility as a function of the concentration $`x`$ of CH4 in liquid Kr. The solid line is a parabolic fit to the data drawn to guide the eye.
* CH4 concentration–dependent behavior of the momentum–transfer cross section $`\sigma _m`$ (closed circle) and of proportionality constant $`\sigma _{E_0}`$ of the energy–transfer cross section $`\sigma _E.`$ The solid lines are only guidelines for the eye.
* Excess electron mobility as a function of the electric field in the mixture with $`x=5\%`$ of methane. Solid line: fit of the kinetic model with the energy–transfer cross section inversely dependent on the electron energy. Dashed– and dot–dashed lines: prediction of the kinetic model with two different values of an energy–independent energy–transfer cross section.
* Concentration–dependent behavior of the electric field values $`E^{}`$ beyond which the mobility data are no longer well described by an energy–transfer cross section inversely proportional to the electron energy. The solid line is a square–root fit to the data.
* Dependence on the CH4 concentration of the mean electron energy $`ϵ^{}`$ evaluated at the field $`E^{}`$ where the high–field behavior of the electron mobility changes from the $`E^1`$ to the $`E^{1/2}`$ dependence. The solid line is only a guide for the eye.


text:
# Holographic analysis of diffraction structure factors

## Abstract

We combine the theory of inside-source/inside-detector x-ray fluorescence holography and Kossel lines/x ray standing waves in kinematic approximation to directly obtain the phases of the diffraction structure factors. The influence of Kossel lines and standing waves on holography is also discussed. We obtain partial phase determination from experimental data obtaining the sign of the real part of the structure factor for several reciprocal lattice vectors of a vanadium crystal.

phase problem; standing waves; Kossel lines  preprint: LBNL

The phase determination of diffracted beams is the central problem of x-ray crystallography. Several methods exist to obtain this information, such as direct methods Sayre:1995 , 3-beam diffraction Shen:1987 , anomalous diffraction, heavy atom or molecular replacement Blundell:1976  and x-ray standing waves or Kossel lines von:1960 ; Batterman:1964 ; Cowley:1964 . Despite the many advances in these methods, not all problems can be solved. Direct methods fail when the unit cell contains a large number of atoms. Anomalous diffraction and related methods are among the most successful methods for biological crystallography, but they often require chemical modification of the molecules. Multiple beam diffraction, x-ray standing waves and Kossel lines have usually been applied only to high-quality crystals of relatively simple structures, or to the localization of dopants in high quality crystals Golovchenko:1974 .

Kossel lines are formed when a source of short wavelength radiation ($`1`$ Å) is located on a crystallographic site: they result from the Bragg scattering of outgoing fluorescent x-rays from various sets of planes in the lattice. In the notation of holography, this is an “inside-source” experiment. The fine structure of these lines has been explained by the dynamical theory of x-ray diffraction via the reciprocity theorem used in optics von:1960 . A proper analysis of the KL fine structure allows the determination of the phases of reflections Batterman:1964 ; Cowley:1964 ; Gog:1995 ; Vartanyants:2001 ; Lonsdale:1949 . In parallel to this work on KL, the x-ray standing wave (XSW) method has been developed Batterman:1964 ; Cowley:1964 ; Golovchenko:1974 ; Vartanyants:2001 . In this case, the source and the detector are interchanged as compared to the KL method: the atoms are subject to the changing wave-field in the crystal as the incident beam goes through a Bragg reflection, and fluorescent radiation proportional to the field at the atom is generated. This constitutes the ”inside-detector” configuration in holography Gog:1995 . Besides the fine structure of the KL or XSW produced when the crystal orientation satisfies a Bragg or Laue condition, tails are formed far from the Bragg angle. These coarse features, also formed by poorer-quality mosaic crystals provide information on the real and imaginary part of the structure factor Vartanyants:2001 ; Lonsdale:1949 .

Unlike standard imaging methods, holography offers the possibility of extracting both intensity and phase information. X-ray fluorescence holography (XFH) is thus a very promising new method for obtaining a direct image in real space of the local environments of different atomic species in reasonably well-ordered crystals or molecular ensembles. Long-range translational order is not required, and indeed one of the most important results obtained by XFH has been the imaging of the average local environment of a quasicrystal Marchesini:2000 . Despite this, with the exception of quasicrystals, all systems measured so far have been well-ordered crystals Tegze:1999 ; Hiort:2000 ; Tegze:2000 ; Kopecky:2001 .

In this paper we develop a theoretical method for analyzing the inside-source and inside-detector holograms of a periodic object using the kinematic approximation. By analyzing the holographic reconstruction in reciprocal space, we discuss how to obtain directly the phase of the structure factors. We also show how the standard holographic analysis is affected by diffraction, and discuss the solution to this problem.

A hologram is formed whenever an unknown object wave $`E_{obj}`$ is coherently added to a reference wave $`E_{ref}`$:

$`I\left(𝐤\right)`$ $`=`$ $`\left|E_{\text{ref}}+E_{\text{obj}}\right|^2`$ (1)
$`=`$ $`I_{\text{ref}}+I_{\text{obj}}+2\mathrm{R}\mathrm{e}\left\{E_{\text{ref}}^{}E_{\text{obj}}\right\}.`$
where $`I_{ref}`$ and $`I_{obj}`$ are the intensities of the reference and object waves respectively.

The hologram is extracted by subtracting the reference beam intensity $`I_{ref}`$ and normalizing. The object term $`I_{obj}`$ is usually assumed to be small and therefore neglected in order to permit a holographic analysis of the data in XFH. We will see later how this approximation can affect our analysis. When an atom located at the origin emits (inside source) or detects (inside detector) radiation, the resulting hologram (considering only the last term in eq. (1), i.e. the interference term) can be expressed as Hiort:2000 :

$$\chi \left(𝐤\right)=2\mathrm{R}\mathrm{e}\underset{𝐫}{}f(𝐤,𝐫)\chi _𝐫\left(𝐤\right),$$
(2)
where $`\chi _𝐫\left(𝐤\right)\frac{e^{i\left(kr𝐤𝐫\right)}}{r}`$ and $`f(𝐤,𝐫)`$ is the scattering factor (including the Thompson scattering factor Len:1997 ) of the atom located at $`𝐫`$. The summation is extended to all the atomic positions.

Ideally, when the object term can be neglected and the scattering factors are isotropic, the holograms $`\chi _𝐫\left(𝐤\right)`$, $`\chi _𝐫^{}\left(𝐤\right)`$ generated by two point scatterers located at $`𝐫`$ and $`𝐫^{}`$, are orthogonal. i.e. $`\chi _𝐫^{}\left(𝐤\right)\chi _𝐫^{}\left(𝐤\right)_𝐤`$$`\alpha \left(𝐫\right)\delta \left(𝐫𝐫^{}\right)`$. $`\alpha \left(𝐫\right)`$ is a normalization function and $`_𝐤`$ is the average on the measured k space. The two holograms are orthogonal because the relative phase oscillates when the infinite k-space is spanned. In normal situations, due in particular to the limited k-space sampling, $`\delta \left(𝐫𝐫^{}\right)`$ becomes a point spread function peaked in $`𝐫=𝐫^{}`$. The typical reconstruction algorithm is based on this orthogonality assumption. The holographic reconstruction is the projection of $`\chi \left(𝐤\right)`$ onto $`\chi _𝐫^{}\left(𝐤\right)`$:

$$U\left(𝐫^{}\right)=\chi \left(𝐤\right)\chi _𝐫^{}^{}\left(𝐤\right)_𝐤.$$
(3)
What happens if we now perform the reconstruction taking into account the long-range periodicity of the system? To answer this question, let us first examine the holographic reconstruction in the reciprocal space, by applying a Fourier transform to eq. (3). Since only the kernel $`\chi _𝐫^{}\left(𝐤\right)`$ depends on $`𝐫^{}`$ we can bring the FT inside the average and write:

$`G(𝐡^{})`$ $`=`$ $`\chi \left(𝐤\right){\displaystyle d^3𝐫e^{i𝐡^{}𝐫}\chi _𝐫^{}\left(𝐤\right)}_𝐤`$
$`=`$ $`\chi \left(𝐤\right)\stackrel{~}{\chi }_𝐡^{}^{}\left(𝐤\right)_𝐤,`$
$`\stackrel{~}{\chi }_𝐡\left(𝐤\right)`$ $`=`$ $`{\displaystyle d^3𝐫\frac{1}{r}e^{i\left\{kr(𝐤𝐡)𝐫\right\}}}=\frac{1}{\left(\left|𝐤𝐡\right|^2k^2\right)}.`$ (5)
The formal analogy between (3) and (Holographic analysis of diffraction structure factors) suggests we consider $`\stackrel{~}{\chi }_𝐡\left(𝐤\right)`$ as the hologram generated by a point structure factor, located at position $`𝐡`$ of the reciprocal space, $`i.e.`$ a sinusoidal charge density distribution with unitary scattering factor amplitude. Similarly to the discussion above, we expect the holograms $`\stackrel{~}{\chi }_𝐡^{}\left(𝐤\right),\stackrel{~}{\chi }_𝐡\left(𝐤\right)`$ generated by two points $`𝐡`$ and $`𝐡^{}`$ in the reciprocal lattice to be orthogonal in k-space, $`i.e.\stackrel{~}{\chi }_𝐡^{}^{}\left(𝐤\right)\stackrel{~}{\chi }_𝐡^{}\left(𝐤\right)\beta \left(𝐡\right)\delta (𝐡𝐡^{})`$. In real situations the Dirac delta function is replaced by a function peaked in $`𝐡`$.

We now examine the properties of the hologram $`\chi \left(𝐤\right)`$ in terms of the structure factors of the reciprocal lattice vectors. Following Adams:1998 , we rewrite (2) in terms of the electron density $`\rho \left(𝐫\right)`$:

$$\chi \left(𝐤\right)=2\mathrm{R}\mathrm{e}d^3𝐱\rho (𝐫)\frac{r_e}{r}e^{i(kr𝐤𝐫)},$$
(6)
where $`r_e`$ is the classical electron radius. For simplicity we have approximated the Thompson scattering factor to be a constant. If the system is periodic, the charge density distribution can be expressed in a Fourier series in terms of the reciprocal lattice vectors $`𝐡`$ and the relative structure factors $`F_𝐡`$, namely $`r_e\rho \left(𝐫\right)=_𝐡F_𝐡e^{i𝐡𝐫}`$, with $`F_𝐡=\frac{r_e}{V}\underset{V}{}\rho \left(𝐫\right)e^{i𝐡𝐫}d^3𝐫`$, where $`V`$ is the unit cell volume. The origin, which determines the phase shifts in the structure factors, is at the emitting atom in the unit cell.

The hologram (6) becomes, in analogy with (2):

$$\chi \left(𝐤\right)=2\mathrm{R}\mathrm{e}\underset{𝐡}{}F_𝐡\stackrel{~}{\chi }_𝐡\left(𝐤\right).$$
(7)
The divergence of $`\stackrel{~}{\chi }_𝐡\left(𝐤\right)`$ at the Bragg condition ($`𝐡^22𝐡𝐤=0)`$ in (5) is introduced as a consequence of neglecting extinction, mosaicity and the finite sample size. These effects can be approximated by writing $`k`$ as a complex number The:1 , i.e. $`k=k_r+ik_i`$, and $`\stackrel{~}{\chi }_𝐡\left(𝐤\right)=\mathrm{Re}\left\{\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right\}+i\mathrm{Im}\left\{\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right\}`$ then becomes:

$`\mathrm{Re}\left\{\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right\}`$ $`=`$ $`\left|\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right|^2\left(𝐡^22𝐡𝐤\right),`$
$`\mathrm{Im}\left\{\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right\}`$ $`=`$ $`\left|\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right|^2\left(2k_ik_r\right),`$
$`\left|\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right|^2`$ $`=`$ $`\frac{1}{\left(𝐡^22𝐡𝐤\right)^2+\left(2k_ik_r\right)^2}.`$ (8)
As the wave-vector $`𝐤`$ changes across the pole of $`\stackrel{~}{\chi }_𝐡\left(𝐤\right)`$, there will be a symmetric and an antisymmetric contribution dependent in different ways on the real and the imaginary part of the structure factor. Writing $`F_𝐡=\mathrm{Re}\left\{F_𝐡\right\}+i\mathrm{Im}\left\{F_𝐡\right\}`$, the hologram in (7) becomes:

$$\chi =2\underset{𝐡}{}\mathrm{Re}\left\{\stackrel{~}{\chi }_𝐡\right\}\mathrm{Re}\left\{F_𝐡\right\}\mathrm{Im}\left\{\stackrel{~}{\chi }_𝐡\right\}\mathrm{Im}\left\{F_𝐡\right\}.$$
(9)
Note that, at the Bragg condition, the object term cannot be neglected, it contributes with a second order divergence and therefore needs to be added to the interference term. The normalized object term can then be written as:

$$\frac{I_{obj}}{I_{ref}}=\underset{𝐡}{}\left|F_𝐡\right|^2\left|\stackrel{~}{\chi }_𝐡\right|^2+\underset{𝐡,𝐡^{}𝐡}{}F_𝐡^{}F_𝐡^{}\stackrel{~}{\chi }_𝐡^{}\stackrel{~}{\chi }_𝐡^{}.$$
(10)
Except when multiple Bragg conditions are satisfied simultaneously, the second term can be neglected. We recall that the object wave intensity is always smaller than that of the reference at a pole $`\frac{I_{obj}}{I_{ref}}\left|\frac{F_𝐡}{\left(2k_rk_i\right)}\right|^2<1`$, while the interference term (9), at a Bragg condition, is $`\frac{\mathrm{Im}F_𝐡}{k_rk_i}`$. The interference term (9) can still be the dominant one, depending on the phase of the structure factor.

Let us now consider the properties of the reconstructed image $`G`$, which can be viewed as the ‘hologram of the reciprocal lattice’, in relation to the structure factors. The real and imaginary parts of the reconstruction kernel $`\stackrel{~}{\chi }_𝐡^{}\left(𝐤\right)`$ (eq. (8)) are respectively antisymmetric and symmetric across the pole as $`\left(𝐡^22𝐡^{}𝐤\right)`$ changes from positive to negative. The product between an antisymmetric and a symmetric function is antisymmetric, and the integral across the pole cancels out:

$`\mathrm{Re}\left\{\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right\}\mathrm{Re}\left\{\stackrel{~}{\chi }_𝐡^{}\left(𝐤\right)\right\}_k`$ $`=`$ $`a\left(𝐡\right),`$
$`\mathrm{Re}\left\{\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right\}\mathrm{Im}\left\{\stackrel{~}{\chi }_𝐡^{}\left(𝐤\right)\right\}_k`$ $``$ $`0,`$
$`\mathrm{Im}\left\{\stackrel{~}{\chi }_𝐡\left(𝐤\right)\right\}\mathrm{Im}\left\{\stackrel{~}{\chi }_𝐡^{}\left(𝐤\right)\right\}_k`$ $`=`$ $`b\left(𝐡\right);`$ (11)
where the normalization functions $`a\left(𝐡\right)`$ and $`b\left(𝐡\right)`$, are positive functions. The resulting holographic reconstruction becomes:

$`\mathrm{Re}\left\{G\left(𝐡^{}=𝐡\right)\right\}`$ $``$ $`\mathrm{Re}\left\{F_𝐡\right\}a\left(𝐡\right),`$
$`\mathrm{Im}\left\{G\left(𝐡^{}=𝐡\right)\right\}`$ $``$ $`\left(2\mathrm{I}\mathrm{m}\left\{F_𝐡\right\}\frac{\left|F_𝐡\right|^2}{2k_rk_i}\right)b\left(𝐡\right).`$
The real part of the reconstructed hologram, with $`𝐡^{}`$ equal to a reciprocal lattice vector $`𝐡`$, is proportional to the real part of the structure factor. The characterization of $`\mathrm{Re}\left\{F_𝐡\right\}`$ reduces the phase problem of the structure factor from the possible $`(0,2\pi )`$ range to only two possible values of the phase, and in the centrosymmetric systems this correspond to the complete solution. This requires us to calculate the normalization function $`a\left(𝐡\right)`$, which is dependent on the measured k-space, polarization factors, extinction, sample boundaries, mosaic spread and angular resolution. Such calculation goes beyond the scope of this work; however the knowledge of the sign of $`\mathrm{Re}F_𝐡`$ reduces the range of the possible phases by half. The imaginary part of $`G`$ depends on the real and imaginary part of the structure factors. If the object term $`I_{obj}`$ in (1) cannot be neglected, the Fourier transform of $`G,`$ the “standard holographic reconstruction”, would have the wrong interpretation. It would be more some kind of Patterson function (the Fourier transform of $`|F_𝐡|^2)`$ rather than a hologram (Fourier transform of $`\mathrm{Re}F_𝐡+i\mathrm{Im}F_𝐡)`$. Only with the full knowledge of the normalization functions $`a\left(𝐡\right)`$ and $`b\left(𝐡\right)`$ can we separate and extract the values of the real and imaginary parts of the structure factors. The limitations on this straightforward analysis of the imaginary part of the structure factor apply to the standard holographic reconstruction as well. It is not surprising that a diffraction measurement interpreted as a hologram in a recent article Kopecky:2002  provides the correct structure, as the Patterson function peaks match the correct solution.

Analyzing the reconstruction in the reciprocal space allows extracting directly information on the real part of the structure factors, simplifying the problem to the calculation of the normalization functions. By including the knowledge of the absolute value of the structure factor, we can separate the contribution of the object intensity term to the imaginary part of the structure factor.

We performed the experiments on a bending magnet beamline (BL 9.3.1) at the Advanced Light Source. A schematic drawing of the experimental setup is shown in Figure 1. Inside the chamber, the sample, a vanadium bcc single crystal with (111) orientation, is mounted on a standard two-axis goniometer. The V $`K_\alpha `$ fluorescence radiation at 4.9 keV emitted by the sample was collected by a 4-channel high-speed solid state detector with single photon pulse analysis and a maximum of 4 MHz count rate Bucher:1996 . The measurement was performed by rotating the sample at high speed in a spiral motion Marchesini:2001 : the azimuth at 3600 degrees per second, and the polar at 2 degrees per second and varying from 0 (perpendicular to the surface) to 80 degrees. The detector was placed close to the sample to average the “inside source” hologram, resulting in an ”inside-detector” measurement in holographic terminology Gog:1996 . The azimuth stepper motor pulses were used to synchronize the data acquisition allowing us to collect a full pattern of 3.2 105 pixels in about 40 seconds. The measurement was repeated until the statistical noise and incident beam fluctuations have been reduced to a reasonable level; typically, several hundred separate patterns were thus summed in a final dataset.

The measured hologram at 6.3 keV incident energy is shown in Figure 2 and the real part of the reconstructed ‘reciprocal’ hologram $`\mathrm{Re}\left\{G\left(𝐡^{}\right)\right\}`$ as derived from Eqs. 4 and 5 is shown in Figure 3. The network of white lines connects the known positions of the reciprocal lattice positions in the V lattice. The image in reciprocal space shows its most intense yellow spots at the reciprocal lattice positions, which in turn correspond to the positive values of the real part of the structure factors. One can see that the height of these peaks is approximately constant. This is because the functions $`a\left(𝐡\right)`$ and $`b\left(𝐡\right)`$ are almost constant when $`\left|𝐡\right|`$ is not close to the wavenumber $`k`$, this can be true if the hologram is measured at a single energy in every direction, as was our case. The vanadium crystal is a special case in which the structure factors are real and positive. However the reconstructed image from a simulated Kossel line pattern of a PbSe single crystal which was chosen since it exhibit both positive and negative signs in the structure factors, correctly shows these different signs.

We have presented a method for the direct phase determination of the structure factors. This result has been obtained by analyzing the holographic reconstruction in reciprocal space and by combining the theory of inside-source/inside-detector holography and Kossel lines/x-ray standing waves. This method can be applied to any crystal possessing an atom which can be excited to emit radiation. We have shown how holograms and standard holographic reconstruction can be distorted in periodic objects by x-ray diffraction, and discussed the possible solution to this problem. By separating the real and imaginary parts of the reconstructed image, and by calculating the normalization function, we obtain the real part of the structure factor. By including the knowledge of the absolute value of the structure factor, one can separate the contribution of the object intensity term to imaginary part of the structure factor.

We have demonstrated this method experimentally on a simple test case, by measuring the full inside-detector XSW pattern and obtaining the real part of the structure factors for a vanadium crystal. In order to obtain the full phase determination, the calculation of the normalization functions $`a\left(𝐡\right)`$ and $`b\left(𝐡\right)`$. However even the qualitative direct image obtained provides the sign of the real part of the structure factor, which for centro-symmetric systems correspond to the complete solution. The information obtained by this technique can be used as input in a standard KL/XSW fitting analysis to obtain the full phase determination.

We would like to acknowledge M. R. Howells and J. C. H. Spence for useful discussions and L. Zhao for help during the experiment. This work was supported by the U.S. Department of Energy under Contract No. DE-AC03-76SF00098.