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# References

15 December 2003

hep-ph/0312180

Reply to “A remark on the “Theory of neutrino oscillations””
Carlo Giunti
INFN, Sezione di Torino, and Dipartimento di Fisica Teorica,

Università di Torino, Via P. Giuria 1, I–10125 Torino, Italy

Abstract

I refute the criticisms of Ref.  raised in Ref. .

With this short note I would like to answer the rather provocative note of Okun, Rotaev, Schepkin and Tsukerman (O.R.S.T.) in Ref. .

First, I would like to thank O.R.S.T. for their attention to my recent paper in Ref. , that is the object of their criticism.

The specific target of the O.R.S.T. criticism is the use of the substitution $`t=x`$ in the covariant derivation of the neutrino oscillation probability in the plane wave approach. Here $`x`$ is the distance traveled by the neutrino between production and detection and $`t`$ is the elapsed time.

Unfortunately, O.R.S.T. did not notice or mention that in Ref.  it is explained that in order to justify the substitution $`t=x`$ it is necessary to treat massive neutrinos as wave packets . I think that, if one accepts the assumption $`t=x`$, the covariant derivation of the neutrino oscillation probability in the plane wave approach presented in Ref.  does not present inconsistencies.

The physical reason why the substitution $`t=x`$ is correct can be understood by noting that the massive neutrino wave packets overlap with the detection process for an interval of time $`[t\mathrm{\Delta }t,t+\mathrm{\Delta }t]`$, with

$$t=\frac{x}{\overline{v}}x\left(1+\frac{\overline{m^2}}{2E^2}\right),\mathrm{\Delta }t\sigma _x,$$
(1)
where $`\overline{v}`$ is the average group velocity, $`\overline{m^2}`$ is the average of the squared neutrino masses, $`E`$ is the neutrino energy (neglecting mass contributions), $`\sigma _x`$ is given by the spatial uncertainties of the production and detection processes summed in quadrature  (the spatial uncertainty of the production process determines the size of the massive neutrino wave packets). I also assumed that massive neutrinos are ultrarelativistic and contribute coherently to the detection process in order to observe the oscillatory terms of the flavor transition probability, for which the substitution $`t=x`$ is needed in order to get the space-dependent phases

$$\varphi _{kj}(x)=\frac{\mathrm{\Delta }m_{kj}^2x}{2E}=2\pi \frac{x}{L_{kj}^{\mathrm{osc}}},$$
(2)
where $`\mathrm{\Delta }m_{kj}^2=m_k^2m_j^2`$ is the difference between two squared neutrino masses and $`L_{kj}^{\mathrm{osc}}=4\pi E/\mathrm{\Delta }m_{kj}^2`$ is the corresponding oscillation length. It is clear that the correction $`x\overline{m^2}/2E^2`$ to $`t=x`$ in Eq. (1) can be neglected, because it gives corrections to the oscillation phases which are of higher order in the very small ratios111 Since the neutrino masses are smaller than about one eV (see Ref. ) and only neutrinos with energy larger than about 100 keV can be detected (see Ref. ), we have $`m_k^2/E^210^{10}`$.  $`m_k^2/E^2`$. The corrections due to $`\mathrm{\Delta }t\sigma _x`$ are also negligible, because in all realistic experiments $`\sigma _xL_{kj}^{\mathrm{osc}}`$, otherwise oscillations could not be observed . One can summarize these arguments by saying that the substitution $`t=x`$ is correct because the phase of the oscillations is practically constant over the interval of time in which the massive neutrino wave packets overlap with the detection process and it is given by Eq. (2) plus negligible corrections of higher order in the neutrino masses.

Let me answer in detail to the two false problems raised by O.R.S.T.:

1. One is free to define “so-called space velocities $`\overline{v}=x/t`$” of massive neutrinos, which are trivially identical. However, I think that such definition is useless. Neutrinos are not classical objects, for which $`v=x/t`$. It is pretty clear that the uncertainty principle forbids any relation of such type.

Certainly, the “space velocities $`\overline{v}=x/t`$” have no relevance at all for the phase of a quantum wave function.

The judgment “But in this case the plane wave approximation is not valid.” does not seem to follow from any logical consideration.
2. The second remark does not apply to my paper in Ref. , where the substitution $`t=x`$ was adopted. Without any logic, O.R.S.T. write that since the different prescription $`x=v_kt`$ gives a wrong result, “the “theory” of ref.  is false.”

Both the two false problems claimed by O.R.S.T. stem from a confusion between phase velocity, group velocity and other fanciful velocities that continues to appear from time to time in the literature (see the references in Ref. ), in spite of the discussion in Ref.  and the fact that the difference between phase velocity and group velocity and their physical relevance are explained in several introductory books on Quantum Mechanics and Optics.

O.R.S.T. conclude their note claiming the validity of the so-called “equal-energy assumption”, which has been proved to be in general unrealistic in Refs.  on the basis of simple relativistic considerations.

O.R.S.T. write that “one has to assume that all three $`E_k`$ are equal”. However, physics is not made from arbitrary assumptions and one should justify them. O.R.S.T. reasoning seems to be: since (in their opinion) the substitution $`t=x`$ “is fraught with at least two problems”, the equal-energy assumption must be correct, because it is the only one that produces the standard phase in the plane wave approximation. This is clearly a circular reasoning: in order to get the standard phase one has to assume equal energies and in order to justify the equal-energy assumption one has to assume the correctness of the standard phase.

The physical reason why the equal-energy assumption is not realistic is that energy-momentum conservation in the production process in general implies that the energies of different massive neutrinos are different , as at least a subset of O.R.S.T. should know . Of course, energy and momentum are not exactly defined in the production process, in order to allow the coherent production of different massive neutrinos, but it is pretty unlikely that an uncertainty in energy and momentum could generate the equal-energy constraint. Indeed, the neutrino wave packets have been calculated in the framework of quantum field theory in Ref. , showing that in general the energies of different massive neutrinos are different.

In conclusion, I think that the covariant derivation of the neutrino oscillation probability in the plane wave approach presented in Ref.  is rather attractive, because it is simple, avoiding wave packet complications, and uses a minimum of well-motivated assumptions. In particular, it shows clearly that unrealistic assumptions about the values of the energies and momenta of massive neutrinos are not needed. Of course, I think that one is free to derive the neutrino oscillation probability in the plane wave approach through the equal-energy assumption (as well as the equal-momentum assumption used in the original derivation of the standard phase ), as long as one is aware of its limitations and does not claim that it describes reality.

Note added after hep-ph/0312280

The authors of hep-ph/0312280 seem to have problems with elementary logical reasoning and elementary calculations.

$`t=x`$ is justified by a wave packet treatment. Once this is accepted, wave packets are not needed for the calculation of the phase at leading order in the neutrino mass contribution.

$$\left(E_kE_j\right)x\frac{\overline{m^2}}{2E^2}\frac{\mathrm{\Delta }m_{kj}^2x}{2E}\frac{\overline{m^2}}{2E^2}\frac{\mathrm{\Delta }m_{kj}^2x}{2E}.$$
(3)
How is it possible that “As emphasized in ref., such corrections are of the same order as the standard oscillation phase and as such are used from time to time in the literature to modify the standard phase by the notorious factor of 2.” \[hep-ph/0312280\]?222 The factor of two mistake is not due to a correction to the time at which interference is calculated, but to a calculation of interference for different propagation times of the different massive neutrinos (see ).

Future comments will be posted at http://www.nu.to.infn.it/Neutrino\_Oscillations/.


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# Towards Automated Generation of Scripted Dialogue: Some Time-Honoured Strategies

## 1 Introduction

By a scripted dialogue we mean a dialogue which is performed by two or more agents on the basis of a description of that dialogue. This description, i.e., the script, specifies the actions which are performed in the course of the dialogue and their temporal ordering. We assume that the script is created in advance by an author. Automated generation of scripted dialogue involves a computer programme in the role of the author and execution of the script by software agents. André et al. (2000) coin the term ‘presentation team’ for such a collection of software agents. In their words, presentation teams ‘\[…\] rather than addressing the user directly–convey information in the style of performances to be observed by the user’ (André et al., 2000:220).

The plan of this paper is to first motivate why the study of scripted dialogues is interesting and useful, whilst also pointing out the limitations and complications of scripted dialogue. We then present a number of strategies for the automated generation of scripted dialogue. Our discussion is illustrated by means of some extracts from mainly scripted dialogues. The paper concludes with a brief overview of the ongoing neca project in which scripted dialogues are presented by embodied conversational agents.

## 2 Prospects and Problems

Scripted dialogues have interesting features, both from a theoretical and a practical point of view. Let us start by highlighting A theoretical issue. Scripted dialogues involves two layers of communication. First, in a scripted dialogue there is a layer at which the participants of the dialogue mimic communication with each other. The communication is not real because the actions of the participants are based on a script; the participants do not interpret the actions of the other participants in order to determine their own actions. Second, there is a layer of uni-directional communication from the author of the script to the audience of the dialogue. At this level, a scripted dialogue is very much like a monologue. Thus scripted dialogue presents a challenge because it requires simultaneous generation of a layer of real and one of pretended communication, each layer having its own participants with their (real or pretented) goals, beliefs, desires, personalities, etc.

Also from a practical point of view scripted dialogue has something to offer. Before we go into its advantages, let us, however, first discuss a feature of scripted dialogue which might be perceived as one of its limitations. There is a class of applications which requires the generation of dialogue about a subject matter that evolves in real-time. For such applications scripted dialogue is not possible. For instance, André et al. (2000)’s dialogues between two reporters about a live transmission of a Robocup soccer event cannot be implemented as scripted dialogue: the verbal reports of the agents are determined to a large extent by events which evolve in real-time. Hence it is impossible to script the verbal reports in advance. Similarly, automatically generated scripted dialogues do not lend themselves well to user involvement in the dialogue: because the script is created in advance there is no scope for reaction to the user’s contributions.

These limitations are, however, offset by a large number of benefits. Firstly, it should be noted that for large scale applications it has been argued that a combination of scripted and autonomous behaviours is required. For instance, in the mre project at usc111See, e.g., Rickel et al. (2002). a combination of autonomous and scripted virtual humans is used to create a realistic training environment. Thus applications do not necessarilly force a strict choice between autonomous and scripted behaviour (more specifically dialogue).

Secondly, staying within the education/training domain it should be noted that in the literature on Intelligent Tutoring Systems (its) a case has been made for so-called vicarious learning (e.g., Lee et al., 1998; Cox et al., 1999): learning by watching dialogues of other people being taught or engaged in a learning process. Various studies have been carried out in this area and some positive effects of vicarious learning by overhearing dialogue (as opposed to monologue) have been found (see Scott et al., 2000).

Thirdly, there is a large class of obvious applications for scripted dialogues. The dialogue in film scenes, commercials, plays, product demonstrations, etc. can be treated as scripted dialogue. These are examples of situations in which real-time interaction with the environment or a user are not required.

Finally, there is not only a wide range of potential applications for scripted dialogue, but applying scripted dialogues also has some distinct advantages over relying on dialogue generated by autonomous agents:

1. The generation of a scripted dialogue requires no potentially complicated and error-prone interpretation of the dialogue acts produced by other autonomous agents.
2. More time is available for the generation process, because scripted dialogue is not generated in real time.
3. Not only more time but also more information is available to the generation process of scripted dialogue. Whereas in spontaneous dialogue an individual action can only be constructed using information about the actions which temporally precede it, in scripted dialogue an action can be tailored to both the actions which precede and those which follow it.
4. It is much easier to create dialogues with certain global properties (e.g., a certain pattern of turn-taking), because the dialogue is constructed by a single author. In spontaneous dialogue, such properties emerge out of the autonomous actions of the participants, which makes it difficult to control them directly.

## 3 Strategies for Scripted Dialogue Generation

We have already pointed out that in one important respect scripted dialogue resembles monologue: information flows from a single author to an audience. Hovy (1988) was one the first to systematically consider how the (communicative) goals of an author can be related to various strategies for communicating information through a monologue. In particular, he describes a natural language generation (nlg) system (Pauline) which implements a number of such strategies. He thereby abandoned an assumption which was and still is implicit in many nlg systems, namely that a text is generated from a database of facts and that the task is mainly one of mapping these facts onto declarative sentences which express them. Hovy’s work on the influence of pragmatic factors on natural language generation is currently followed up by various researchers involved in building embodied conversational agents (for a bibliography of recent work in this newly emerging area of natural language generation see Piwek, 2002).

The new picture that emerges is one where an author uses a text as a device for influencing the attitudes of his or her audience. Amongst the attitudes which an author might want to influence are the beliefs, intentions (plans for action), goals, desires and opinions (judgements about whether something is good, bad or neutral) of the audience. All of the aforementioned attitudes are about something (that is, they are intentional; see, for instance, Searle, 1983). Roughly speaking, one can discern attitudes which are about the subject matter/topic of a text and those which pertain to the context (e.g., the author, the audience and the relation between the two). Attitudes about the context are normally communicated implicitly. Hovy discusses how style (formal, informal, forceful) can be used to do so. Generally speaking, everything that is discussed explicitly in a text is part of its subject matter. Thus, whenever contextual aspects are discussed explicitly (e.g., ‘I am your boss, therefore listen to what I have to say’), they become also part of the subject matter. This leaves us with a class of information that is neither discussed explicitly (and therefore not part of the subject matter) and is neither part of the context. For instance, take an opinion about a person which can be expressed explicitly as in ‘X is a bad guy’, but also implicitly as in ‘X killed John’.222Hovy (1988) discusses how reporting that a person is the actor of an action which is generally considered to be bad can be used to implicitly convey the opinion that the person is bad.

Scripted dialogue offers the same communicative opportunities (i.e., for communicating facts and influencing an audience in other ways) as ordinary text, plus a number of other ones in addition. To illustrate some of the issues, let us summarize one of the first dialogues written by the humanist philosopher Erasmus of Rotterdam in 1522 (Erasmus, 1522).333Large parts of the dialogue were omitted, reworded, or summarized, since we wil be focusing on a specific set of issues. The (very tentative) translation is our own.

| E1 | 1. | A: | Where have you been? |
| --- | --- | --- | --- |
|  | 2. | C: | I was off to Jerusalem on |
|  |  |  | pilgrimage. |
|  | 3. | A: | Why? |
|  | 4. | C: | Why do others go? |
|  | 5. | A: | Out of folly if I’m not mistaken. |
|  | 6. | C: | That’s right; glad I’m not the |
|  |  |  | only one though. |
|  | 7. | A: | Was the trip worthwhile? |
|  | 8. | C: | No. |
|  | 9. | A: | What did you see? |
|  | 10 | C: | Pilgrims causing mayhem. |
|  | 11. | A: | Were you morally uplifted? |
|  | 13 | C: | No, not at all. |
|  | 14 | A: | Did you get richer? |
|  | 15. | C: | No, quite the contrary. |
|  | 16 | A: | Was there nothing good about |
|  |  |  | the trip then? |
|  | 17 | C: | Yes, in fact there was. In |
|  |  |  | particular, I can now entertain |
|  |  |  | others with my lies, |
|  |  |  | like other pilgrims do. |
|  | 18. | A: | But that’s not very decent, |
|  |  |  | is it? \[…\] |
|  | 19. | C: | True. But I may also be able to |
|  |  |  | talk others out of the idea of |
|  |  |  | pilgrimage. |
|  | 20. | A: | I wish you had talked me out |
|  |  |  | of it. |
|  | 21. | C: | What? Have you been as stupid |
|  |  |  | as I? |
|  | 22. | A: | I’ve been to Rome and |
|  |  |  | Santiago de Compostela. |
|  | 23. | C: | Why? |
|  | 24. | A: | Out of folly I guess \[because …\] |
|  | 25 | C: | So why did you do it? |
|  | 26. | A: | My friends and I vowed to go |
|  |  |  | when we were drunk. |
|  | 27. | C: | Surely a decision worth taking |
|  |  |  | when you’re drunk \[…\] |
|  |  |  | Did everyone arrive back home |
|  |  |  | safely? |
|  | 28. | A: | All except three: Two died; |
|  |  |  | the third we left but he’s |
|  |  |  | probably in heaven now. |
|  | 29. | C: | Why? Was he so pious? |
|  | 30. | A: | No, he was a scoundrel. |
|  | 31. | C: | Then why is he in heaven? |
|  | 32. | A: | Because he had plenty of |
|  |  |  | letters of indulgence with |
|  |  |  | him \[…\] |
|  | 33. | A: | Don’t get me wrong: I’m |
|  |  |  | not against letters of indulgence |
|  |  |  | but I have more admiration for |
|  |  |  | someone who leads a virtuous |
|  |  |  | life. Incidentally, when do we |
|  |  |  | go to these parties that you |
|  |  |  | mentioned? |
|  | 34. | C: | Let’s go as soon as we can, |
|  |  |  | and add to other pilgrims’ |
|  |  |  | lies. |

The central question that we will start addressing in this paper is ‘what strategies for influencing the attitudes of the audience are specific to scripted dialogue?’ A number of these strategies will be introduced below. We will return to Erasmus’ dialogue at various points in our discussion and highlight parts of the dialogue which illustrate the aforementioned strategies.

### 3.1 Strategies of information distribution

As we have seen, the main difference between monologue and scripted dialogue is that the latter communicates with the audience via the (pretended) communication between the dialogue participants. This has a number of immediate effects:

1. The author can let a participant say something without being directly responsible for the content.
2. Each participant can represent a particular chunk of information, making the combined content more easily digestible.
3. In particular, the participants can represent different points of view on the same subject matter, which may even be inconsistent with each other.
4. One participant may express an opinion concerning something the other participant has raised.

Point 1 was clearly relevant to Erasmus, in whose case direct criticism of the Catholic church could have made him a target for the Inquisition. (A’s last utterance seems intended to further milden any criticism.) Point 2 is relevant because each of the two participants represents a particular journey. Both journeys could have been related in one monologue, but this might have led to confusion and would certainly have been less exciting to read. In fact, it is patently clear from reading the whole dialogue that one participant’s questions are used for making more lively what would otherwise have been a story with some rather boring parts.

Point 3 is not directly relevant in the case of the present dialogue but the very fact that both participants agree on all essentials can only reinforce the strengths of Erasmus’ implied position. (See also under Strategies of Emphasis.) Point 4 is relevant again, since both participants frequently express evaluative opinions concerning various elements of the two stories. In many cases, evaluative opinions are expressed in highly indirect fasion, and this brings us to a second class of strategies.

### 3.2 Strategies of association

One way to influence the attitude of the audience about, for instance, a person is to mention the person in combination with something else to which the audience already has the intended attitude. Hovy (1988) suggests, for example, that we can make somebody look good, bad or neutral by presenting him or her as the actor of an action which is generally (or specifically by the audience) perceived to be good, bad or neutral, respectively: “Mike killed Jim” makes Mike look bad, whereas “Mike rescued Jim” makes him look good.

In fact, this strategy seems to be an instance of a more generally applicable strategy: To convey that X has property P, one can present X in combination with something which has or implies property P. Thus, to convey that Mike is a clever guy we might say “Mike managed to solve this partial differential equasion in no time”, i.e., Mike is presented as being able to solve a difficult problem quickly, which implies being clever.

Information conveyed in a text is not only presented in the context of other information which can influence its interpretation but also by the author (and possibly speaker) of the text. If any properties of this author/speaker are known, these can rub off on the points s/he is trying to make. The appeal to this tendency in an argument is considered to be a fallacy (Argumentum ad Hominem). For instance, one might argue that Bacon’s philosophy is untrustworthy because he was removed from his chancellorship for dishonesty (Copi, 1972:72).

Scripted dialogue lends it particularly well to this type of association. The presence of the second layer of communication allows the author to distribute communicative acts over characters which were conceived by the author. These characters can be given certain traits which influence the interpretation by the audience of what they say in the dialogue. These traits can be conveyed by various means. In the case of Erasmus’ dialogue, the fact that the protagonists and their pilgrim friends are avid partygoers – evidently something Erasmus didn’t approve of – is used to discredit their pilgrimage. If the dialogue is enacted by a collection of embodied agents, their physical appearance can be used. Alternatively, certain characteristics of the dialogue can also suggest a particular property. For instance, Thomas (1989) discusses various ways in which a speaker can come across as dominant or an authority (interruptions, abrupt changes of topic, marking new stages in the interaction, metadiscoursal comments, etc.). The following is an example of a marking of a new stage in the interaction taken from Thomas (1989:146):
E2 A:   Okay that’s that part. The next part what I want to deal with is your suitability to remain as a CID officer.

### 3.3 Strategies of emphasis

For various reasons, an author might want to highlight certain information and suppress other information. In a monologue, repetition of information signals emphasis. For instance, de Rosis and Grasso (2000) analyse an explanation text about drug prescription and point out that certain information is rather redundant, i.e., repeated with identical or equivalent wording such as:
E3   “The good is news is that we do have tablets that are very effective for treating TB”, and “but it is something we can do something about”.
Here it seems that positive information is repeated intentionally. In dialogue, repetition can be achieved naturally due to the presence of two interlocutors at the second layer of communication. Consider the dialogue fragment below from Twain (1917:11) between a young man and an old man.

| E4 | 1. | y.m. | What detail is that? |
| --- | --- | --- | --- |
|  | 2. | o.m. | The impulse which moves a |
|  |  |  | person to do things – the |
|  |  |  | only impulse that ever moves |
|  |  |  | a person to do a thing. |
|  | 3. | y.m. | The only one! Is there |
|  |  |  | but one? |
|  | 4. | o.m. | That is all. There is only |
|  |  |  | one. |
|  | 5. | y.m. | Well, certainly that is a |
|  |  |  | strange enough doctrine. |
|  |  |  | What is the sole impulse that |
|  |  |  | ever moves a person to |
|  |  |  | do a thing? |
|  | 6. | o.m. | The impulse to content |
|  |  |  | his own spirit–the necessity |
|  |  |  | of contending his own spirit |
|  |  |  | and winning its approval. |

Here turns 3. and 4., which form a subdialogue, are both about the claim that there is only one impulse which moves a person to do things. Now imagine that we have an algorithm which has already distributed the information which it wants to get across to the audience amongst the dialogue participants. Let us call this step I. During step II, the algorithm will determine how this information can be conveyed through a sequence of turns. To generate E4, we might at this stage produce the sequence: 1., 2., 5., 6. Step III would involve the addition of further turns for the purpose of emphasizing information. During step III, such an algorithm could insert subdialogues like the one above (3., 4.), if there are any matters which need particular emphasis.

Note that Erasmus also employs this strategy. For instance, in Erasmus’ Dialogue (E1), the turns 4. and 5. form a subdialogue which a system like the one proposed here could insert during step III, after already having created the sequence 1., 2., 3., 6., …

Note that the sketched approach presupposes that realization (both verbal and non-verbal) is performed only after steps I – III; during steps I – III the algorithm manipulates abstract descriptions of the semantic and pragmatic content of the utterances. The reason for this is that before step III, the algorithm can not yet know whether to realize the beginning of turn 6. as ‘That’s right’ or ‘Out of folly’, since this depends on whether the subdialogue (4., 5.) is inserted or not.

## 4 Application in the NECA project

The work reported in this paper is carried out in the context of the neca project which started in October 2001 and has a duration of 2.5 years.444neca stands for Net Environment for Embodied Emotional Conversational Agents. The project is funded by the Ec. The partners in the project are: Dfki, Ipus (University of the Saarland), Itri (University of Brighton), öfai, Freeserve and Sysis ag. Further details can be found at http://www.ai.univie.ac.at/NECA/. In this project a system is being built that can generate scripted dialogues that are subsequently performed by animated human-like characters. One prototype to be delivered by neca is an electronic showroom (eShowroom).555This application builds on the work carried out at Dfki and reported in André et al. (2000). The idea is that a user/customer can select a class of cars and/or attributes (friendly for the environment, luxury, sportiness, etc.) in which s/he is interested. Furthermore, the user can set the personality traits of the characters which are to discuss this car (introverted, extroverted, agreeable, etc.). On the basis of these settings, the system then produces dialogues about specific cars and presents these to the user by means of embodied conversational agents which play out the dialogue. The strategies discussed in the present paper are highly relevant in the context of car sales. For example,

* Information about cars can be complex, so it can be useful to have one or more participants ask clarification questions (somewhat in the style of Conan Doyle’s Watson character, who triggers Sherlock Holmes into explanations that benefit us as readers).
* Not all customers are alike and it can be useful to let different types of customers be represented by different animated characters: one who is primarily interested in the performance off the car, one who is interested in chrome and gloss, one who is very aware of environmental and safety-related issues, etc.

Let us describe in more detail how one of the strategies of emphasis will be implemented in the neca system. The neca system generates the interaction between two or more characters in a number of steps, where information flows from a Scene Generator to a Multi-modal Natural Language Generator, to a Speech Synthesis component, to a Gesture Assignment component, and finally to a media player.

In the Scene Generator, the basic structure of the dialogue is determined. For this purpose, a top-down planning algorithm is used. The output of this module is a rrl Scene Description (see Piwek et al., 2002). Amongst other things, this Scene Description contains a set of dialogue acts. Individual dialogue acts are specified in terms of the dialogue act type, the speaker, the addressees, the semantic content, the actions which the act is a reaction to, and the and emotions (felt and expressed). The temporal ordering amongst the dialogue acts is represented separately and allows for underspecification.

A Scene Description is constructed stepwise. We might start by constructing the following dialogue fragment:666In reality, at this stage in the processing linguistic realization has not yet taken place; thus the texts in E5. should be understood as mere paraphrases of the abstract descriptions of the dialogue acts which are actually passed on.

| E5 | $`x_1`$ | B: | How fast is this car? |
| --- | --- | --- | --- |
|  | $`x_2`$ | S: | Its top speed is 180mph. |
|  | $`x_2`$ | B: | Wow, that’s great. |

At this point, further elaboration of the dialogue is possible. Assume, for example, that the positive information that the car has a top speed of 180mph is to be emphasized. For this purpose, the strategy of emphasis we discussed in section 3.3 can be employed: a subdialogue can be inserted after $`x_2`$ consisting of a question by the buyer (‘As much as 180mph?’) which provides the seller with the opportunity to repeat a positive piece of information. This procedure yields the following ‘enhanced’ dialogue:

| E6 | $`x_1`$ | B: | How fast is this car? |
| --- | --- | --- | --- |
|  | $`x_2`$ | S: | Its top speed is 180mph. |
|  | $`y_1`$ | B: | As much as 180mph? |
|  | $`y_2`$ | S: | Yes, no less than 180 mph. |
|  | $`x_2`$ | B: | Wow, that’s great. |

Note that the information which required emphasis has been mentioned no less than three times in the dialogue. This has been achieved by exploiting a very natural dialogue phenomenon: the occurrence of confirmation subdialogues.

The thus created abstract representation of the dialogue (the Scene Description) can subsequently be processed further by the Multi-modal Natural Language Generator, the Speech Synthesis component, and the Gesture Assignment component. The result is sent to a media player which displays the dialogue to the user by means of a collection of embodied conversational characters.

## 5 Conclusions

We are not aware of any work which lays out strategies for the automated generation of scripted dialogue. There is a rapidly growing body of work on (Embodied) Conversational Agents (see, e.g., Ball & Breeze, 1998; De Carolis et al., 2001; Loyall & Bates, 1997; Nitta et al., 1997; Prendinger & Ishizuka, 2001; Walker et al., 1996 and Zinn et al., 2002), but to the extent that language generation is discussed there777See Piwek (2002) for an overview of the literature in this area, specifically on affective natural language generation., it is from the perspective of the agents who participate in the conversation, rather than from the perspective of an author who produces a script for their interaction. The only exception we came across is André et al. (2000) which reports on implemented systems for both spontaneous and scripted dialogue. Our aim has been to take a step back from the domain-specific implementation which they propose and find out whether it is possible to first identify more general strategies which are valid for the automated generation of scripted dialogue. We have tried to find such strategies on the basis of examples of human-authored and naturally occurring dialogues. We hope that our tentative investigations will encourage further studies into this new topic. A topic which, in our opinion, harbours interesting research questions at the intersection between dialogue processing and text generation, and which also lends itself well for various types of practical applications.

## Acknowledgements

We would like to thank Alexandre Direne, Martin Klesen and Neil Tipper for comments on an earlier draft of this paper, and two anonymous reviewers for their comments and encouragement. This research is supported by the EC Project neca IST-2000-28580. The information in this document is provided as is and no guarantee or warranty is given that the information is fit for any particular purpose. The user thereof uses the information at its sole risk and liability.

## References

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Ball, G. & J. Breeze (1998). ‘Emotion and Personality in a Conversational Character’. In: Proceedings of the Workshop on Embodied Conversational Characters, Lake Tahoe, CA, 1998, 83–86.

Cox, R., J. McKendree, R. Tobin, J. Lee & T. Mayes (1999). ‘Vicarious learning from dialogue and discourse’. Instructional Science, 27, 431–458.

Copi, Irving M. (1972). Introduction to Logic: Fourth Edition. Macmillan, New York.

de Carolis, B., V. Carofiglio, C. Pelachaud & I. Poggi (2001). ‘Interactive Information Presentation by an Embodied Animated Agent’. In: Proceedings of the International Workshop on Information Presentation and Natural Multimodal Dialogue, Verona, Italy, 14–15 December 2001, 19–23.

Erasmus, Desiderius (1522). Colloquia.

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Lee, J., F. Dineen, J. McKendree (1998). ‘Supporting student discussions: it isn’t just talk’. Education and Information Technologies, 3, 217–229.

Loyall, A.B. & J. Bates (1997). ‘Personality-Rich Believable Agents That Use Language’. In: Proceedings of the first International Conference on Autonomous Agents, Marina Beach Marriott Hotel, Marina del Rey, California, February 5-8, 1997.

Nitta, K., O. Hasegawa, T. Akiba, T. Kamishima, T. Kurita, S. Hayamizu, K. Itoh, M. Ishizuka, H. Dohi, and M. Okamura (1997). ‘An Experimental Multimodal Disputation System’. In: Proc. of the IJCAI-97 Workshop on Intelligent Multimodal Systems, Nagoya, 1997.

Piwek, P. (2002). ‘An Annotated Bibliography of Affective Natural Language Generation’. ITRI Technical Report ITRI-02-02, University of Brighton. (available at: http://www.itri.bton.ac.uk/$``$Paul.Piwek)

Piwek, P., B. Krenn, M. Schröder, M. Grice, S. Baumann & H. Pirker (2002). ‘RRL: A Rich Representation Language for the Description of Agent Behaviour in NECA’. In: Proceedings of the AAMAS workshop “Embodied conversational agents – let’s specify and evaluate them!”, 16 July 2002, Bologna, Italy.

Prendinger, H. & M. Ishizuka (2001). ‘Agents That Talk Back (Sometimes): Filter Programs for Affective Communication’. Contribution to: Second Workshop on Attitude, Personality and Emotions in User-adapted Interaction (in conjunction with User Modeling 2001), Sonthofen, Germany, July 13, 2001.

Rickel, J., S. Marsella, J. Gratch, R. Hill, D. Traum & W. Swartout (2002). ‘Toward a New Generation of Virtual Humans for Interactive Experiences’. IEEE Intelligent Systems, July/August 2002.

de Rosis, F. & F. Grasso (2000). ‘Affective Natural Language Generation’. In: A.M. Paiva (Ed.), Affective Interactions, Springer Lecture Notes in AI 1814, 204–218.

Scott, D.C., B. Gholson, M. Ventura, A.C. Graesser and the Tutoring Research Group (2000). ‘Overhearing Dialogues and Monologues in Virtual Tutoring Sessions: Effects on Questioning and Vicarious Learning’. International Journal of Artificial Intelligence in Education, 11, 242–253.

Searle, John R. (1983). Intentionality. Cambridge University Press, Cambridge.

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text:
# Collective clusterization effects in light heavy ion reactions

## 1 INTRODUCTION

For A$`{}_{}{}^{}{}_{CN}{}^{}`$$``$48, the compound nucleus (CN) so formed decays subsequently by the emission of mainly the LPs (n, p, $`\alpha `$ and $`\gamma `$-rays), and a significant (5-10%) decay strength is observed for the complex IMFs. The measured angular distributions and energy spectra for IMFs are consistent with fission-like decays of the respective CN.

The statistical Hauser Feshbach (HF) analysis, given for LPs emission, is also used to include the IMFs emission (BUSCO code , or the Extended HF scission-point model (EHFM) ). For IMFs, a more accepted process is the binary fission of the CN (fusion-fission), worked out in the statistical scission-point fission model  or the saddle-point ”transition-state” model (TSM) , with the LPs still treated within the HF method.

The recently advanced dynamical cluster-decay model (DCM)  include the missing structure information of the statistical fission models, by taking each fragment (LP or IMF) preformed in the CN, which subsequently follows the dynamical cluster-decay process rather than the fission process of the statistical model. The structure information influences the observed yields strongly through the observed strong resonance behaviour in the measured excitation functions of large-angle elastic and inelastic scattering yields (see, e.g., ), which enters the DCM via the preformation probability of the fragments.

The DCM for hot and rotating compound systems is a reformulation of the preformed cluster model (PCM) of Gupta et al.  for ground-state decays, briefly developed in Section 2. The application of DCM to 32S+24Mg$``$56Ni is discussed in section 3. The 56Ni has a negative Q-value (Qout), with experimental mass distributions of both LPs and IMFs being available . The model has also been applied successfully for the positive Q-value $`{}_{}{}^{116}Ba^{}`$ system. A summary of our results is presented in section 4.

## 2 THE DCM FOR HOT AND ROTATING NUCLEI

The DCM uses collective coordinates of mass (charge) asymmetry $`\eta `$=(A1-A2)/(A1+A2) ($`\eta _Z`$=(Z1-Z2)/(Z1+Z2)), and relative separation R, characterizing, respectively, the nucleon-exchange between the outgoing fragments, and the incident channel kinetic energy (Ecm) transferred to internal excitation of outgoing channel (E$`{}_{}{}^{}{}_{CN}{}^{}`$+Qout(T)=TKE(T)+TXE(T); TXE and TKE as the total excitation and kinetic energy), since R$``$R(T,$`\eta `$). For decoupled R-,$`\eta `$-motions, in terms of partial waves, the fragment formation or CN decay cross-section

$$\sigma =\frac{\pi }{k^2}\underset{l=0}{\overset{l_c}{}}(2l+1)P_0P;k=\sqrt{\frac{2\mu E_{cm}}{\mathrm{}^2}}.$$
(1)
The preformation probability P0, refering to $`\eta `$-motion, is the solution of stationary Schröd- inger eqn. in $`\eta `$ (with T-dependent collective fragmentation potentials ), at a fixed

$$R=R_a=C_t(\eta ,T)+\overline{\mathrm{\Delta }R}(T).$$
(2)
Ci are Süsmann radii and T is from E$`{}_{}{}^{}{}_{CN}{}^{}`$=Ecm+Qin=$`\left(A/9\right)`$T2-T. $`\overline{\mathrm{\Delta }R}`$(T), the only parameter of model, simulating the two-centre nuclear shape, is similar to neck-length used in statistical models . The penetrability P, refering to R-motion, is the WKB integral, with V(Ra)=V(Rb)=Qeff. Rb is second turning point. Qeff, the effective Q-value or TKE(T,$`\mathrm{}`$=0), is Qeff(T)=B(T)-\[B1(T=0)+B2(T=0)\]=TKE(T)=V(Ra), for the CN at T to decay to two observed cold fragments (T=0). This transition occurs by emitting LPs of energy Ex=B(T)-B(0)=Qeff(T)-Qout(T=0). Instead, here we use Eq. (2). $`\mathrm{}_c=R_a\sqrt{2\mu [E_{cm}V(R_a,\eta _{in},\mathrm{}=0)]}/\mathrm{}`$, with $`\mu `$ and Ra referring to entrance channel $`\eta _{in}`$.

## 3 CALCULATIONS

Fig. 1 gives the variation of $`P_0`$ and $`P`$ with $`\mathrm{}`$ for both the LPs ($`A4`$) and IMFs (A$`>4`$) refering to energetically favoured fragments. Interestingly, the behaviour of LPs is different from that of the IMFs; whereas for LPs $`P_0`$ decreases with increase of $`\mathrm{}`$, for IMFs it increases as $`\mathrm{}`$ increases and then starts to decrease at a large $`\mathrm{}`$-value. Thus, LPs contribute to $`P_0`$ for smaller $`\mathrm{}`$-values whereas the same for IMFs is important for higher $`\mathrm{}`$’s ($`>18\mathrm{}`$). Similarly, the $`P`$’s for LPs are large at all $`\mathrm{}`$-values, whereas the same for $`\mathrm{}18\mathrm{}`$ is nearly zero for all IMFs. This means that the lower $`\mathrm{}`$’s contribute only towards LPs cross-section $`\sigma _{LP}`$ and the higher $`\mathrm{}`$’s ($`>18\mathrm{}`$) to fission-like, IMFs cross-section $`\sigma _{IMF}`$, as shown in Fig. 2(a). The total cross-section $`\sigma _{Total}=\sigma _{LP}+\sigma _{IMF}`$ is also plotted, and the summed up cross-sections are given in braces, to be compared with experiments.

Fig. 2(b) illustrates the contributions of individual IMFs. Apparently, the lighter IMFs contribute more than the heavier IMFs towards $`\sigma _{IMF}`$, pointing to the observed favourable asymmetric mass distribution. Interestingly, similar results, as presented by Figs. 2(a) and 2(b), are obtained by the statistical fission model  (see e.g. Fig. 14 in ).

Fig. 3(a) shows the summed up $`\sigma `$ for decay of 56Ni at $`E_{c.m.}=`$51.6 MeV to both the LPs and even-A, N=Z IMFs, along with the TSM and EHFM calculations, compared with the experimental data . The TSM and EHFM for LPs are the HF results, whereas the DCM treats both the LPs and IMFs emissions on similar footings. For the LPs emission, the measured $`\sigma _{LP}=1050\pm 100`$ mb but the separate yield for each emitted light particle is not available for a direct comparison. First of all, we notice in Fig. 3(a) that the unphysical discontinuity at the point between $`A_2=`$4 and 6 in TSM is not present in our DCM results. In DCM, $`\sigma _{LP}`$ is over-estimated by a large factor of $``$5, a discrepancy that gets removed if mass-one-particle (proton) is replaced with neutron, for example. This signifies the importance of the contributing particles to $`\sigma _{LP}`$. For the IMFs, the general comparison between the data and DCM is of similar quality as for the TSM or EHFM model, at least for $`A_222`$. The use of $`Q_{eff}`$ improves the comparison slightly.

Fig. 3(b) shows the average $`\overline{TKE}=_{\mathrm{}=0}^\mathrm{}_c\sigma _{\mathrm{}}(TKE)_{\mathrm{}}/\sigma `$, with $`\sigma =\sigma _{\mathrm{}}`$, compared with experimental data . Apparently, the comparisons are reasonably good. The maximum $`\mathrm{}`$-value is less than $`\mathrm{}_c`$-value, which may be due to the use of $`\overline{\mathrm{\Delta }R}`$ instead of actual $`\mathrm{\Delta }R(\eta )`$.

## 4 CONCLUSIONS

The dynamical collective clusterization is shown as an alternative good decay process for both the LPs and IMFs produced in low energy reactions. The IMFs are shown to be produced as clusters, like in cluster radioactivity, but from excited CN. The LPs are also considered to be of the same origin, without invoking any statistical evaporation process.


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# Oxygen and Strontium Codoping of 𝐋𝐚_𝟐𝐍𝐢𝐎_𝟒: Room Temperature Phase Diagrams

## I Introduction

In recent years $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_{4+\delta }`$ Rice93aN ; Tamura93aN ; Tranquada98e ; Tranquada94bN  has been studied intensively because of its close relationship with the isostructural high-$`T_c`$ superconductor $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{CuO}_{4+\delta }`$ Radaelli94a ; Wells97 ; Kastner98 . In both systems the transition-metal-oxide planes ($`\mathrm{NiO}_2`$, $`\mathrm{CuO}_2`$) can be doped with hole-like charge carriers resulting in a large number of different structural and electronic phases, in particular the superconducting phase in the case of the cuprates. Although the nickelate system does not exhibit superconductivity, its investigation is very helpful to understand many features of the cuprates, such as oxygen phase separation Radaelli94a ; Wells96 ; Khaykovich02a ; Chou93b  and stripe correlations. Tranquada95 ; Wells97 ; Tranquada95a  Nickelates are quite amenable to study for several reasons: 1) high $`x`$ and $`\delta `$ can be reached, 2) it is much easier to obtain homogeneously oxygen-charged samples, and 3) stripe correlations are more stable and therefore easier to detect than in the cuprates. In most experiments the intension is to introduce holes either by Sr substitution ($`x`$) or by excess oxygen ($`\delta `$). However, as-grown Sr-doped nickelates frequently contain a considerable amount of excess oxygen, which can have a strong impact on various properties. Lack of knowledge of $`\delta `$ can lead to misinterpretations of properties of these materials.

Substitution of $`\mathrm{Sr}^{3+}`$ for $`\mathrm{La}^{3+}`$ appears to be random and has a relatively weak effect on the lattice. The phase diagram of $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$ in Fig. 1(a) shows four structural phases: a high temperature tetragonal phase (HTT), a low temperature orthorhombic phase (LTO), a low temperature less orthorhombic phase (LTO2) and a low temperature tetragonal phase (LTT). LTT  At room temperature the structure changes at $`x0.12`$ from the LTO to the HTT phase, mainly due to the decrease of the sublattice mismatch between the (La,Sr)-O and the Ni-O bond lengths with increasing hole content.

Excess oxygen occupies interstitial lattice sites centered within the LaO

bilayers Jorgensen89aN  and results in the formation of several structurally and compositionally distinct phases separated by miscibility gaps. Rice93aN ; Tranquada94bN  The O-doping phase diagram has been studied by several groups with different techniques. Rice93aN ; Tamura93aN ; Tranquada94bN ; Tamura96aN ; Medarde97aN ; Poirot97aN ; Poirot98aN  Though there are some discrepancies between the various proposed phase diagrams, most features are captured by our schematic diagram in Fig. 1(b). Tranquada94bN  As a function of $`\delta `$ at room temperature the system shows a sequence of pure phases LTO$``$LTT$``$HTT separated by biphasic regions of LTO/LTT and LTT/HTT. These biphasic regions are the result of miscibility gaps which follow from the unmixing of interstitial oxygen defects into oxygen-poor and oxygen-rich phases. Strong interstitial oxygen correlations give rise to these miscibility gaps. For moderate oxygen concentrations the HTT phase transforms into a phase with one-dimensional (1D) stage order of the oxygen interstitials upon cooling below room temperature. Tranquada94bN  Onset of staged ordering may involve opening of additional miscibility gaps or intergrowth of stacking faults in the staging sequence, allowing for variation in average oxygen stoichiometry throughout this compositional range. Tranquada94bN  Finally, at very high $`\delta `$ three-dimensional (3D) oxygen order is observed. Hiroi90aN ; Chen93aN ; Tranquada95aN

In $`\mathrm{La}_2\mathrm{NiO}_4`$, the $`\mathrm{NiO}_2`$ planes form a two-dimensional (2D) spin $`S=1`$ Heisenberg antiferromagnet (AF) on a square lattice, with a Néel temperature of $`330`$ K. Rodriguez91aN ; Nakajima95  As the system is doped with an increasing concentration of holes $`p=x+2\delta `$, the commensurate AF order is destroyed and a phase of static charge and spin stripes forms. The stripe phase is the consequence of an electronic phase separation into hole-rich charge stripes acting as antiphase boundaries between hole-poor AF spin stripes. Tranquada95a  So far, for pure Sr doping stripe order has been observed for hole concentrations $`p=x0.135`$ and in the case of O doping for $`p=2\delta 0.22`$ (see Fig. 1). Tranquada94aN ; Sachan95aN ; Tranquada95aN ; Tranquada98e  In the latter case, the first appearance of stripe order might be connected to that of the 3D order of the O interstitials Tranquada94aN ; Wochner98aN ; Homes02aN .

The idea of an interplay between the electronic phase separation in the $`\mathrm{NiO}_2`$ planes, the structural phase separations, and the O interstitial ordering within the rock-salt bilayers has been a strong motivating factor behind this work. We are interested in the question of how additional doping by Sr affects the various phases and phase boundaries of the oxygen-content phase diagram. In particular, are the observed phases the result of purely steric effects of the interstitials or are they partially stabilized by electronic correlations? Beyond these questions it is desirable to map the structural phase diagram of (Sr,O)-codoped $`\mathrm{La}_2\mathrm{NiO}_4`$ so that in future, for a particular Sr content, the $`\delta `$ value of the sample can be determined simply by measuring its lattice parameters.

In the present paper, our focus is the study of specimens with fixed Sr concentrations in the range $`0.02x0.12`$ and variable interstitial oxygen concentrations in the range $`0\delta 0.13`$ at room temperature. Phase separation into oxygen-poor and -rich domains similar to $`x=0`$ was observed for all $`x0.06`$. Drastic changes occur only for higher Sr concentration $`x=0.08`$ and 0.12, where first the LTT/HTT miscibility gap and then also the LTO/LTT miscibility gap disappears. At such high Sr concentrations the tilt angle of the coherent octahedral tilts, with respect to $`x=0`$, is already considerably reduced and finally becomes zero for $`x=0.12`$. Our results rely on a precise adjustment of $`\delta `$, which we have accomplished by controlled atmosphere annealing under conditions of temperature and oxygen fugacity that depend on $`x`$fugacity  In fact, we find that for all samples with $`x0.08`$ an excess oxygen concentration smaller than $`\delta =0.01`$ is sufficient to induce an unmixing into oxygen-poor and oxygen-rich phases. Hence, to study the intrinsic properties of $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$ the oxygen content $`\delta `$ has to be zero, or at least $`0.01`$. We compare our data with results for $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$ prepared in air, Ca- and Ba-doped $`\mathrm{La}_2\mathrm{NiO}_4`$, $`\mathrm{Pr}_2\mathrm{NiO}_{4+\delta }`$, and $`\mathrm{Pr}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$Han95aN ; Sullivan91aN ; Sullivan92aN

## II Experimental

Several series of $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_{4+\delta }`$ powder samples with fixed Sr content ($`x`$) and variable excess oxygen content ($`\delta `$) have been prepared. The starting crystals with $`x=0`$, 0.02, 0.04, 0.06, 0.08, and 0.12 were obtained by congruent melt growth using radio frequency induction skull melting. Buttrey84aN  To adjust $`\delta `$, small crystal pieces were annealed at different temperatures in atmospheres with different oxygen fugacities $`\mathrm{f}_{\mathrm{O}_2}`$ ranging from $`\mathrm{log}(\mathrm{f}_{\mathrm{O}_2})=12`$ to 0. Samples with low $`\delta `$ were obtained by anneals at 1000 C and different $`\mathrm{f}_{\mathrm{O}_2}`$. Samples with medium and high $`\delta `$ were obtained by anneals at 900, 750, 600 and 450 C in Ar and pure $`\mathrm{O}_2`$ respectively. The oxygen fugacity was monitored electrochemically using a Y-stabilized $`\mathrm{ZrO}_2`$ cell against a 1 atm $`\mathrm{O}_2`$ reference. All anneals were terminated by a quench to room temperature. The oxygen content was determined by iodometric titration. Details of crystal growth, O-annealing, and chemical analysis are described in Ref. Buttrey91aN, ; Sullivan91aN, ; Rice93aN, ; Buttrey94a, ; Buttrey95a, . Synchrotron x-ray powder diffraction patterns at room temperature were collected at beamline X7A of the National Synchrotron Light Source at Brookhaven using a Ge(111) monochromator at wavelengths $`\lambda `$ of 0.66Å, 0.7Å, or 0.8Å. Photons were collected with a position-sensitive detector. Smith91a  Spectra were typically acquired in the range $`10^{}<2\theta <50^{}`$ by measuring in $`0.25`$ degree steps for 30-60 sec/step. Powder samples were contained in glass capillaries ($`\mathrm{}`$ 0.4mm) sealed under argon. To avoid potential long-term exposure to oxygen between annealing and measurement, capillaries were stored under mineral oil.

## III Results

### III.1 Excess oxygen content $`\delta `$ vs $`\mathrm{𝟐}𝐜/(𝐚+𝐛)`$

Essential for this study is the precise knowledge of $`\delta `$ for each specimen. In Fig. 2(a) we show the iodometrically determined $`\delta `$ values for the various sample series with fixed $`x`$ as a function of $`2c/(a+b)`$ determined by x-ray diffraction. Iodometric analyses were performed in triplicate under an inert atmosphere using de-aerated solutions and standardized thiosulfate. Buttrey91aN ; Rice93aN ; Buttrey94a ; Buttrey95a . All samples in this diagram are single-phase, as determined from the diffraction measurements. Within each of these series, $`\delta `$ increases super-linearly as a function of $`2c/(a+b)`$. With increasing $`x`$, curves are shifted systematically to higher $`2c/(a+b)`$. Anneals performed under the same conditions with specimens of different $`x`$ show a systematic decrease in $`\delta `$ with increasing $`x`$. The absolute random errors of $`\delta `$ and $`2c/(a+b)`$ were determined to be $`\pm 0.003`$ and $`\pm 0.0005`$, respectively. Note, that the relative error of $`2c/(a+b)`$ ($`\pm 0.02`$%) is much smaller than those of $`a`$, $`b`$, and $`c`$ ($`\pm 0.1`$%), since certain errors, as for example that from uncertainties in $`\lambda `$, cancel out in the ratio. To smooth and interpolate the results, we have applied empirical least-squares fits, indicated by the solid lines, to the $`\delta `$ vs. $`2c/(a+b)`$ data. Values of $`\delta `$ evaluated from these curves using the measured $`2c/(a+b)`$ were subsequently used to plot other quantities as a function of $`\delta `$ or $`p=x+2\delta `$. The fits, shown in Fig. 2 as solid lines, are power laws up to 3rd order, and were fitted simultaneously for all $`x`$. The coefficients of the nonlinear terms were varied independently for each curve. The coefficient of the linear term, i.e. the initial slope at $`\delta =0`$, as well as the value of $`2c/(a+b)`$ at $`\delta =0`$, were allowed to vary linearly as a function of $`x`$. Uncertainties in $`\delta `$ versus 2c/(a+b) are primarily due to the limited mass of sample used for the individual titrations of large numbers of specimens. In future, we plan to characterize this relationship more carefully using larger specimens. This is expected to also reveal any fine structure that may be obscured in the fits provided here.

### III.2 Distinction of structural phases

At high temperatures $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_{4+\delta }`$ is expected to have the ideal $`\mathrm{K}_2\mathrm{NiF}_4`$ HTT structure (space group $`I4/mmm`$) regardless of the oxygen stoichiometry. The crystal lattice consists of $`\mathrm{NiO}_2`$ monolayers separated by $`(\mathrm{La},\mathrm{Sr})\mathrm{O}`$ rock-salt bilayers. Each $`\mathrm{Ni}`$ site is coordinated by six oxygens, resulting in a network of corner-sharing $`\mathrm{NiO}_6`$ octahedra. The formal valence of the $`\mathrm{NiO}_2`$ planes is negative while that of the $`(\mathrm{La},\mathrm{Sr})\mathrm{O}`$ bilayers is positive. Doping with interstitial oxide ions or $`\mathrm{Sr}^{2+}`$ reduces the positive net charge in the rock salt bilayers. Similarly, the compensating holes serve to reduce the negative net charge in the $`\mathrm{NiO}_2`$ planes. Overall, doping decreases the charge separation inherent to the structure, providing a stabilizing effect.

With decreasing temperature different structural transitions are observed depending on $`x`$ and $`\delta `$. Most of these low temperature phases can be described by different patterns of slightly-tilted, almost rigid $`\mathrm{NiO}_6`$ octahedra. Tilt angles are of the order of a few degrees and depend on temperature and doping. It is convenient to index all phases on the basis of the $`\sqrt{2}a\times \sqrt{2}b\times c`$ supercell, relative to the parent $`\mathrm{K}_2\mathrm{NiF}_4`$ cell. In this supercell the interstitial $`\mathrm{O}^2`$ ions reside at positions near ($`\frac{1}{4},\frac{1}{4},\frac{1}{4}`$), i.e. centered within the positive $`(\mathrm{La},\mathrm{Sr})\mathrm{O}`$ bilayers. Jorgensen89aN  In the HTT phase ($`F4/mmm`$) the average octahedral tilt angle is zero. This means that the $`\mathrm{NiO}_2`$ planes are either flat or there is at least no coherent tilt pattern. Short-range correlations of octahedral tilts may exist due to local lattice distortion associated with O and Sr dopants. In the LTO phase ($`Bmab`$), the octahedra tilt along the  direction. In the LTT phase ($`P4_2/ncm`$) the octahedral tilt axis is rotated in-plane by an azimuthal angle of $`45^{}`$ with respect to the LTO phase. Since the direction of this rotation alternates in adjacent $`\mathrm{NiO}_2`$ layers, tilt axes in adjacent layers are perpendicular to each other. Often the LTO2 phase ($`Pccn`$) is observed, which is an intermediate phase between the LTO and LTT phases, since the tilt axis is rotated by an angle $`0^{}<\varphi <45^{}`$. At very high $`\delta `$ an orthorhombic phase was reported for pure $`\mathrm{La}_2\mathrm{NiO}_{4+\delta }`$, for which the symmetry is $`Fmmm`$Jorgensen89aN ; Rice93aN ; Tamura93aN  In the present study this phase was not observed, because in our Sr-doped samples $`\delta `$ is not high enough.

The powder diffraction spectra have been analyzed using the program Rietica to determine the lattice parameters.Rietica  The reflection conditions for the different phases are explained in Ref. Rice93aN, . In the following, we focus on a few characteristic reflections (see Fig. 3) that are very helpful in distinguishing between the different phases and in determining phase fractions in the case of biphasic samples. The LTO phase manifests itself by a split of certain reflections with $`hk`$ such as $`(200)/(020)`$ and $`(515)/(155)`$. In addition, one observes superlattice reflections such as $`(212)`$ or $`(032)`$, which indicate coherent octahedral tilts. In the case of the LTT phase, the split for reflections with $`hk`$ is absent, but the superlattice reflections $`(212)`$ and $`(032)`$ remain. Mixed LTO/LTT phases can be identified by the coexistence of split and non-split reflections as well as the presence of two of each of the superlattice reflections of $`(212)`$ or $`(032)`$, since the lattice constants of the LTO and LTT phases are different. Since the resolution at high angles is better than that at low angles, we have determined the LTO/LTT phase fractions from the $`(515)/(155)`$ reflections. The HTT phase does not show any superlattice reflections; hence, the (212) and (032) reflections are absent. Mixed LTT/HTT phases are most readily identified by a split of reflections such as $`(008)`$ and $`(11\overline{11})`$, as the $`c`$-axis of the LTT and HTT phases are different. The $`c`$-axis differs also for the LTO and LTT phases, but the difference is smaller and was not resolvable in our spectra. The LTO2 phase shows a similar but reduced orthorhombic splitting of the fundamental reflections as in the LTO phase as well as the superlattice reflections $`(122)/(212)`$ and $`(302)/(032)`$. It is well known that $`\mathrm{La}_2\mathrm{NiO}_4`$ at temperatures $`T70`$ K exhibits the LTO2 phase. Rodriguez88aN  In our room temperature spectra, no evidence of the LTO2 phase was observed for any combination of $`x`$ and $`\delta `$.

Representative spectra for the different phases of samples with fixed Sr content x=0.02 and 0.08 are presented in Fig. 3 along with the $`\delta `$ values. For $`x=0.02`$ (top) the two miscibility gaps LTO/LTT and LTT/HTT were clearly detectable. Pure phases were observed only for the LTO and the HTT phase. A pure LTT phase was not detected, most probably because none of our prepared samples matched the required $`\delta `$ value. For $`x=0.04`$ and 0.06 we have in fact observed single-phase LTT samples. Due to the narrow $`\delta `$-range of the LTT phase it is generally difficult to obtain LTT-type samples, which also explains the small number of reports on this phase.

With increasing hole concentration, the structural differences between the LTO, LTT and HTT phases generally decrease since the sublattice mismatch diminishes, making phase separations more difficult to detect. This is clearly the case for $`x=0.08`$ (bottom) where the orthorhombic strain in the stoichiometric sample ($`\delta 0`$) is already much weaker than for $`x=0.02`$ as one can see from the smaller splitting of the (155)/(515) reflections. With increasing $`\delta `$ we observed a mixed phase, but it was not possible to decide whether this phase is of the LTO/LTT or LTO/HTT type. Neither a pure LTT phase nor a mixed phase LTT/HTT was observed. Interestingly, for $`x=0.08`$ the ($`11\overline{11}`$) reflection of the biphasic samples show a significant asymmetry, indicating a majority LTO phase for $`\delta =0.004`$ and a majority LTT or HTT phase for $`\delta =0.023`$. Usually, LTO/LTT phase separation does not show up as clearly in a split of the ($`11\overline{11}`$) reflection as in the case of LTT/HTT phase separation. Therefore, the asymmetry of the ($`11\overline{11}`$) reflections for $`x=0.08`$ might indicate that the second phase is HTT. To solve this problem measurements at low temperatures are needed, where the tilt angles are larger.

### III.3 Lattice constants vs hole content p=x+2$`\delta `$

In Fig. 4 we show the lattice parameters as a function of the hole content $`p=2x+\delta `$. In this figure, only the data of single-phase samples or the majority phases of biphasic samples are included. \[We have also created plots (not shown) of the lattice parameters as a function of $`2c/(a+b)`$ and the excess oxygen $`\delta `$, but these provide no new insight.\] In plot (b) we show the average basal plane lattice constant $`(a+b)/2`$ versus hole content. At low hole doping $`p0.08`$ the branches for the different sample series with fixed $`x`$ almost coincide. In contrast, at higher hole doping the branches are clearly separated. The branch for the highest (lowest) Sr content shows the lowest (highest) values for $`(a+b)/2`$. All other branches for the various $`x`$ values fill in systematically. A closer look at the lattice constants in the LTO phase in Fig. 4(a) shows that $`a`$ and $`b`$ follow a nearly universal dependence on $`x`$ and $`\delta `$. Within each set of points having fixed $`x`$, the left most point has $`\delta 0`$, and then $`\delta `$ increases towards the right point. Accordingly, the orthorhombic strain also follows a universal curve as is shown in Fig. 4(d) where we plot the orthorhombic splitting in percent of $`(a+b)/2`$. Interestingly, the c-axis length shows a nearly unique dependence on $`p`$, as well \[plot (c)\]. As we will discuss later, this coincidence is not obvious. In fact, it turns out that the c-axis length not only depends on $`p`$ but also on the steric effects of the dopands. Furthermore, we observe a change in the slope $`dc/dp`$ at around $`p=0.12(2)`$. At roughly this hole content, pure $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$ as a function of $`p=x`$ crosses over from LTO to HTT (at room temperature). Fig. 4(e) shows the volume $`V`$ of the supercell, which reveals no significant new insights. For fixed $`x`$ the general trend is that, with increasing oxygen content, $`V`$ first shrinks then saturates and eventually increases. Obviously $`V`$ deviates from a linear dependence on oxygen doping, thereby violating Vegard’s rule. Deviations from Vegard’s rule are not uncommon among strongly anisotropic and/or non-stoichiometric crystal structures. Lee89a ; Ganguly93a

#### III.3.1 Pure Sr doping vs. pure O doping

The major differences between Sr and O doping become very clear when comparing the lattice parameters for pure Sr doping ($`\delta =0`$) and pure O doping ($`x=0`$). In Fig. 5 we show corresponding data as a function of $`p`$. For both types of hole doping, the average basal plane lattice constant $`(a+b)/2`$ decreases \[plot (a)\]. With increasing hole concentrations the oxygen-doped samples show significantly larger $`(a+b)/2`$ values as well as a tendency to saturate. For Sr doping $`(a+b)/2`$ decreases linearly, in agreement with Vegard’s rule. Since the dependence of $`c`$ on $`x`$ and $`\delta `$ is almost identical \[plot 5(b)\], the large differences observed for $`V`$ are mainly due to the in-plane effects \[plot 5(d)\]. The differences clearly show that the lattice parameters do not solely depend on the hole content but also on steric effects.

#### III.3.2 Comparision with as-prepared-in-air samples

In Fig. 6 we compare our results for pure Sr and pure O doping with the lattice parameters from Ref. Han95aN,  of Sr-doped samples prepared in air that were not post-annealed. Air-prepared samples frequently contain a considerable amount of excess oxygen. From Fig. 6 it is apparent that this excess oxygen causes huge differences between the lattice parameters of annealed and air-prepared samples, particularly at low Sr concentrations. It is known that the excess oxygen concentration in air-prepared (not post-annealed) samples decreases with increasing Sr content, typically reaching $`\delta 0`$ near $`x=0.3`$, and that for larger $`x`$ oxygen vacancies are generated ($`\delta <0`$). It is for this reason that in Fig. 6 the data points for pure Sr doping and those of the air-prepared samples for large $`x0.3`$ merge into a common Sr doping dependence. From the lattice parameter $`c`$ in Fig. 6(b) we estimate for the air-prepared sample with $`x=0`$ an excess oxygen content as high as $`\delta 0.11`$.

### III.4 Sr and O codoping phase diagrams

In Fig. 7 we present the individual oxygen-content phase diagrams for the various fixed Sr concentrations $`x`$ with regard to the lattice parameters $`a`$ and $`b`$. All data points stem from single-phase samples or the majority phase of biphasic samples. Pure phases are represented by shaded areas and miscibility gaps by white areas. The hatched areas were not covered in this study. As one can see, the maximum $`\delta `$ values obtained by anneals at 450 C in $`\mathrm{O}_2`$, systematically decrease with increasing Sr content. On the other hand the lowest $`\delta `$ values scatter around $`\delta 0`$ within the experimental error. In fact we assume that the most reduced samples are all very close to $`\delta =0`$. Note also, that the lattice parameters for $`x=0`$ and $`\delta 0.055`$ were taken from our earlier publication in Ref. Rice93aN, , but were refit according to section III.1. Hence, minor systematic differences between the phase diagram for $`x=0`$ in Fig. 7 and

those in Fig. 1(b) and Ref. Rice93aN,  are due to the fit procedure we have applied to all data sets (see Fig. 2). For $`x=0`$ one can clearly see the sequence of the pure LTO, LTT, and HTT phases, as well as the mixed LTO/LTT and LTT/HTT phases for intermediate $`\delta `$ values. The phase diagrams for $`x=0.02`$, 0.04 and 0.06 are qualitatively similar, but become increasingly difficult to resolve. According to our data, the $`\delta `$-range of the LTO phase slightly broadens from $`x=0`$ to $`x=0.06`$, while the LTT phase narrows. The pure LTO phase at room temperature never exists at $`\delta `$ values higher than 0.01. This means that $`\delta `$ has to be much smaller than 0.01 to be able to observe the intrinsic properties of $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$. The LTT phase is centered at about $`\delta =0.02`$, while the low $`\delta `$ phase boundary of the HTT phase systematically shifts to lower $`\delta `$ values.

Drastic changes of the phase diagram are observed for $`x0.08`$. For $`x=0.08`$ we were not able to detect the pure LTT phase, nor the second miscibility gap. Moreover, the $`\delta `$-range of the LTO phase again becomes narrower. To confirm these results we have prepared a second series of samples with $`x=0.08`$ which showed essentially the same behavior. At the end of section III.2 we argue that for $`x=0.08`$ the first miscibility gap might be of the LTO/HTT type rather than LTO/LTT. Measurements at low temperatures where the octahedral tilts are larger, are needed to verify this result. For $`x=0.12`$ all samples are in the HTT phase. Only the most reduced samples show traces of the LTO phase and measurements at low temperatures reveale that these samples are indeed close to the HTT/LTO transition which occurs at about 275 K. In conclusion, our results for $`x0.08`$ clearly indicate a suppression of oxygen phase separation. Possible reasons will be discussed below. Finally, we emphasize that we do not observe any evidence for staging order or 3D interstitial order at room temperature. Tranquada94bN ; Tranquada95aN

## IV Discussion

Our experiments have revealed several key results. First of all, all Sr-doped samples in general should be assumed to be codoped unless their oxygen content was determined to be $`\delta =0`$. Furthermore, our results show that one has to clearly distinguish between Sr and O doping at any level of $`x,\delta `$–codoping. As long as miscibility gaps appear, their $`\delta `$-ranges depend mainly on the amount of excess oxygen and not on the hole content. Other features, such as the orthorhombic strain $`2(ba)/(a+b)`$ and the $`c`$ lattice parameter depend mainly on the hole content $`p=x+2\delta `$, independent of whether holes were introduced by Sr or O doping. In contrast, the average basal plane lattice constant $`(a+b)/2`$ (and, therefore, also the unit cell volume) depends explicitly on the individual concentrations of Sr and O.

### IV.1 Oxygen-content phase diagrams

The microscopic mechanism of phase separation and the concomitant structural transitions is quite complex and not fully explored. The fact that the doubly negatively-charged oxygen interstitials are located within the positively charged rock-salt bilayers is consistent with the electrostatic environment. We assume that phase separation into oxygen-poor and -rich domains takes place by diffusion of the interstitials parallel to the rock-salt layers. Diffusion along the $`c`$-axis is assumed to be negligible. (The diffusion process seems to be driven by the free energy ($`\overline{G}_0`$) rather than by self-diffusion. JacobsonPriv ) The final ground state is a delicate balance between lattice distortions, Coulomb repulsion between the interstitial $`\mathrm{O}^2`$ ions, and screening effects by the charge carriers in the $`\mathrm{NiO}_2`$ planes. With increasing $`\delta `$ the LTT phase becomes energetically favorable over the LTO phase, though the stabilization of the initial LTT domains requires a minimum concentration of interstitials. Within the first miscibility gap it is obviously energetically favorable for the interstitials to separate into oxygen-poor LTO and oxygen-rich LTT domains, i.e., the overall gain in lattice distortion energy by forming $`\mathrm{O}^2`$ depleted LTO as well as $`\mathrm{O}^2`$ enriched LTT domains compensates the loss in Coulomb energy due to the enhanced charge inhomogeneity in the rock-salt layers and possibly also in the $`\mathrm{NiO}_2`$ planes. Evidence for a charge inhomogeneity in the $`\mathrm{NiO}_2`$ planes at this low level of O-doping comes from studies of the magnetic properties, which indicate the coexistence of domains with Néel temperatures typical for the pure phases, i.e. the coexistence of domains with different hole concentrations. Hosoya92aN ; Tranquada94bN  This is very similar to $`\mathrm{La}_2\mathrm{CuO}_{4+\delta }`$ where phase separation results in superconducting and antiferromagnetic domains, Cho93  indicating not only the formation of oxygen-rich and -poor domains, but also a corresponding charge inhomogeneity in the $`\mathrm{CuO}_2`$ planes.

The LTT phase exists only in a very narrow range of $`\delta `$. At higher $`\delta `$ the structure at room temperature eventually becomes HTT. The HTT phase is characterized by a disordered non-coherent octahedral tilt pattern. There are certainly several factors responsible for the doping dependent crossover from the LTT to the HTT phase. We assume that in HTT domains the reduction of the sublattice mismatch with increasing hole concentration has advanced to a degree, that no coherent tilt pattern is possible. The observation of orthorhombic staged phases at temperatures slightly below room temperature show that, in principle, a phase with a coherent tilt pattern can be induced at high hole and oxygen concentrations, as well.

Structural models proposed in Ref. Tranquada94bN,  suggest that the LTT structure is indeed more suitable to accommodate the interstitials than the LTO phase. However, the concentration of excess oxygen is not the only parameter that determines the phase diagram. In $`\mathrm{Pr}_2\mathrm{NiO}_{4+\delta }`$ for example, the $`\delta `$ range of the pure LTT phase is centered at $`\delta 0.06`$ in contrast to $`\delta 0.02`$ in $`\mathrm{La}_2\mathrm{NiO}_{4+\delta }`$ (see Fig. 8). Buttrey90aN ; Sullivan91aN  Moreover, no HTT phase is observed between the LTT and the orthorhombic high-$`\delta `$ phase ($`Fmmm`$). Since trivalent Pr is smaller than La, in $`\mathrm{Pr}_2\mathrm{NiO}_4`$ the sublattice mismatch is larger, i.e. the octahedral tilt angle is larger and the $`c`$-axis shorter. Buttrey90aN ; Sullivan91aN  The change of the local environment of the interstitial site obviously makes it more difficult to stabilize the LTT phase. It is worth mentioning that in a Pr based sample, annealed under identical conditions as a La based sample, the interstitial oxygen content is higher, which is also the reason for the larger accessible $`\delta `$ range in Fig. 8.

So far, we have considered the effects of oxygen doping. Additional doping with Sr, on one hand introduces random lattice defects, and on the other hand Coulomb repulsion between the relatively-negative (compared to La) Sr sites and the O interstitials. Furthermore, Sr doping increases the concentration of holes. The holes in the $`\mathrm{NiO}_2`$ planes might be expected to screen the $`\mathrm{O}^2`$ interstitials, as well as the Sr impurities in the rock-salt layers, which should result in a reduced O-O and Sr-O Coulomb repulsion. From our results, however, we have obtained no evidence that screening has a significant impact on the oxygen interstitials. On the other hand, our data yield clear signatures of an influence of Sr doping on the oxygen-content phase diagram: the suppression of oxygen phase separation for $`x0.08`$ as well as a weak change of the widths of the LTO and LTT phases for $`x0.06`$.

One possible explanation is that the Coulomb interaction between the O interstitials and Sr defects suppresses the tendency for phase separation into oxygen-rich and oxygen-poor domains. However, other factors can also cause the observed changes. As our comparison with $`\mathrm{Pr}_2\mathrm{NiO}_{4+\delta }`$ has shown, it might well be that with decreasing octahedral tilt angle (with increasing $`x`$) the phase boundaries shift in $`\delta `$ as well as in temperature. Since the cusp of a miscibility gap is rounded, the $`\delta `$ range of the gap depends on the temperature of the experiment relative to the upper consolute temperature. This can explain a broadening or narrowing of the pure phases, too. In this context, the successive disappearance of the miscibility gaps for $`x0.08`$ can occur if their upper consolute temperatures drop below room temperature.

We note that, though the structural differences between the LTO, LTT and HTT phases decrease with increasing Sr concentration, oxygen phase separation in principle should stay detectable. Even in the extreme case of a phase separation into oxygen-rich and oxygen-poor HTT domains, the lattice parameters of these two HTT phases would be different and therefore distinguishable. As we have no indication that this happens in our samples with $`x0.08`$, we assume that we have indeed observed a suppression of the phase separation, as mentioned above. Further measurements at variable $`T`$ to track the consolute temperature as a function of $`x`$ and $`\delta `$, as well as at low $`T`$ where the lattice distortions are usually larger, are necessary to confirm this point.

### IV.2 Structural anisotropy

In Fig. 9 we compare our results for the lattice parameters of $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_{4+\delta }`$ with data for Ba, Sr and Ca-doped $`\mathrm{La}_2\mathrm{NiO}_4`$ from Ref. Han95aN,  and references cited therein, as well as $`\mathrm{Pr}_2\mathrm{NiO}_4`$ from Ref. Sullivan92aN, . Note that in Ref. Han95aN,  a broad Sr range was covered ($`0x`$ 1). We limit our comparison to $`x0.3`$ since only around this Sr content does one obtain $`\delta 0`$ in typical air-prepared samples (section III.3.2). We assume a similar situation for Ca and Ba doping.

Let us focus first on the behavior of $`c`$ in Fig. 9(b). The coincidence of our data for $`\mathrm{La}_2\mathrm{NiO}_4`$ for pure O doping and pure Sr doping up to $`x=0.12`$ is confirmed by a point at $`x=0.3`$ taken from Ref. Han95aN, . In contrast, $`c`$ is significantly larger for a Ba-doped sample and shorter for a Ca-doped sample, both with $`x=0.33`$. In the case of $`\mathrm{Pr}_2\mathrm{NiO}_4`$ the $`c`$-axis is about 2.5% shorter than in $`\mathrm{La}_2\mathrm{NiO}_4`$, but it shows a similar Sr doping dependence as $`\mathrm{La}_2\mathrm{NiO}_4`$ at low $`x0.12`$. A comparison of the ionic radii of the substituting elements shows that $`c`$ qualitatively scales with the average ionic radii at the La site: $`\mathrm{Ba}^{2+}:\mathrm{Sr}^{2+}:\mathrm{La}^{3+}:\mathrm{Ca}^{2+}:\mathrm{Pr}^{3+}1.47\mathrm{\AA }:1.31\mathrm{\AA }:1.216\mathrm{\AA }:1.18\mathrm{\AA }:1.179\mathrm{\AA }`$Shannon76a  Therefore, we conclude that the coincidence of $`c`$ for Sr and O-doped $`\mathrm{La}_2\mathrm{NiO}_4`$ is accidental.

As shown in Fig. 9 (a), out of all dopants, interstitial oxygen shows the largest in-plane lattice constants. Even for Ba, the largest dopant, $`(a+b)/2`$ stays significantly smaller than for oxygen doping. We assume that this is due to a large chemical pressure of the intercalated oxygen ions. Interestingly, the Ca-doped sample is in line with the Sr data, and the data for $`\mathrm{Pr}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$ are just 0.2% lower than for $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{NiO}_4`$. The fact that, compared to $`c`$, $`(a+b)/2`$ barely depends on the average ionic radii at the La site shows that the chemical pressure for La site doping is highly anisotropic. Furthermore, we have to conclude that the decrease of $`(a+b)/2`$ upon Sr doping is largely due to the dependence of the Ni-O bond length upon hole doping. If this conclusion is correct, then the much weaker decrease of $`(a+b)/2`$ observed for oxygen doping effectively indicates an expansion of the $`ab`$-plane by oxygen interstitials. At a hole content of $`p0.3`$, this expansion amounts to $`1.1`$% which has to be compared to an expansion of the $`c`$ axis by 1.2% (see Fig. 9). Therefore, we conclude that interstitial oxygens cause an almost isotropic expansion. We note furthermore, that a strongly anisotropic lattice expansion has also been observed in the LTO phase of Nd-doped $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{CuO}_4`$BuechnerDiss

Finally we discuss the change of the slope $`dc/dp`$ in Fig. 4(c) at a hole content of $`p0.12`$ . This effect was also observed by Tamura et al. in $`\mathrm{La}_2\mathrm{NiO}_{4+\delta }`$ with $`x=0`$Tamura93aN  There are certainly several factors that contribute to the Sr and O doping dependence of $`c`$. One factor is the chemical pressure of the dopants, as was discussed above. Next, hole doping leads to a decrease of the sublattice mismatch, which causes the $`\mathrm{NiO}_6`$ octahedra to straighten up. This results in an increase of $`c`$, and further is an additional reason for the stabilization of the HTT phase. On the other hand, O and Sr doping lead to significant disorder within the octahedral tilts, because the surrounding apical oxygens are pushed away from the defect site (even in the HTT phase). Tilt disorder, therefore, effectively causes $`c`$ to decrease. Furthermore, it is assumed that the accompanying disruption of the coherent tilt pattern stabilizes the HTT phase, as well. A closer look at Fig. 4(c) shows that the slope $`dc/dp`$ becomes smaller at approximately the hole content where the samples enter the pure HTT phase. At the moment we cannot conclusively say whether this effect represents a distinct crossover or a gradual variation. However, one possible explanation involves the already mentioned contribution coming from a change of the octahedral tilt angle for the coherent tilt pattern. This contribution is zero in the HTT phase and therefore might cause the slower increase of $`c`$ with increasing $`p`$. We mention that in $`\mathrm{La}_{1.95}\mathrm{Bi}_{0.05}\mathrm{CuO}_{4+\delta }`$, as well, a change of $`dc/d\delta `$ at $`\delta 0.07`$ was observed. Kato96a  In $`\mathrm{La}_{2\mathrm{x}}\mathrm{Sr}_\mathrm{x}\mathrm{CuO}_4`$, a similar behavior might be related to an increasing concentration of oxygen vacancies for $`x0.25`$Radaelli94  Nevertheless, in this compound the feature occurs roughly at the Sr-doping-dependent crossover from the LTO phase to the HTT phase, as well.

## V conclusion

In summary, we have presented a detailed x-ray powder diffraction study of Sr and O codoped $`\mathrm{La}_2\mathrm{NiO}_4`$ at room temperature. From the lattice parameters we have constructed the oxygen-content phase diagram for each investigated Sr content. At low Sr concentrations $`x0.06`$ the phase diagrams are qualitatively similar to that for $`x=0`$. However, significant changes occur for $`x0.08`$ where phase separation progressively disappears. We have argued that both the Coulomb interaction between the oxygen interstitials and the Sr defects, and the reduction of the octahedral tilt angle by Sr doping contribute to this effect. A comparison of the lattice parameters of codoped samples reveals that one has to clearly distinguish between Sr and O doping. Furthermore, we have systematically characterized the differences between pure Sr and pure O doping, as well as Sr-doped samples prepared in air. A comparison with other dopants shows that the chemical pressure of the La site dopants is strongly anisotropic, while oxygen interstitials exhibit a more isotropic chemical pressure. Finally, this study provides a $`(x,\delta )`$-structure-map which can be used to determine the oxygen content of a Sr-doped sample with $`x0.12`$ by measuring the x-ray powder diffraction spectrum.

###### Acknowledgements.

We acknowledge experimental support from B. Noheda and Y. Lee and helpful discussions with P. DeSanto. We are grateful to L. Finger for implementation of GPLSFT for Windows XP. The work at Brookhaven and Delaware was supported by the Office of Science, US Department of Energy under Contract No. DE-AC02-98CH10886 and DE-FG02-00ER45800, respectively.


text:
# Physics of Relativistic Perfect Fluids

## 1 Physical fluids and energetic evolutions. The inverse problem

In the absence of nuclear or chemical reactions, and independent of the external constraints to which it may be submitted, a material medium is considered here as physically characterized by the specification of its molecular components.

In a domain $`\mathrm{\Omega }`$ of the space-time, and in the absence of exterior constraints, every initial configuration of a material medium gives rise to a particular evolution. And, to every one of these evolutions in $`\mathrm{\Omega }`$ an energy tensor  $`T_f`$ corresponds univocally. Due to the absence of exterior constraints, the energy tensors so obtained are divergence-free, $`T_f=0`$.

Thus, a set $`𝐓_f\{T_f\}`$ of energy tensors is associated to every medium $`f`$, namely those of all its possible unconstrained evolutions in the space-time domain $`\mathrm{\Omega }`$. We have the diagram of Figure 1.

The energetic description of a particular evolution of the medium $`f`$ by the energy tensor $`T_f`$, consists, and only consists, of the specification of the energy density $`\rho _f`$, the energy flow density $`q_f`$ and the stress tensor $`t_f`$ of this evolution of $`f`$ in $`\mathrm{\Omega }`$.

Consequently, the energetic description by $`T_f`$ does not explicitly contain the physical characterization of the medium, that is, the specification of its molecular components.

Thus, a given divergence-free energy tensor $`T_f`$ could describe the particular evolution of more than one medium. In other words, the sets $`𝐓_f`$ and $`𝐓_{\overline{f}}`$ of all possible unconstrained evolutions of two mediums $`f`$ and $`\overline{f}`$ are not necessarily disconnected as the diagram of Figure 2 shows.

On the other hand, divergence-free energy tensors $`T`$ may be generated theoretically in many ways, which may or may not correspond to particular evolutions of a physical medium. Thus, if $`𝐓`$ denotes the set of all divergence-free energy tensors $`T`$, $`𝐓`$ $`\{T/T=0\}`$, $`𝐅`$ the set of all mediums $`f`$, $`𝐅`$ $`\{f\}`$, and $`𝐓_𝐅`$ that of all divergence-free energy tensors $`T`$ describing all particular evolutions of all mediums $`f`$, $`𝐓_𝐅`$ $`\{T𝐓/f:T=T_f,f𝐅\}`$, we have the diagram of Figure 3.

Usually, in many (theoretical or experimental) physical situations one starts from known elements of $`𝐅`$ and looks for some of the corresponding elements of $`𝐓`$. Here we are interested in the inverse problem that inquires about the existence and characterization of mediums $`f`$ in $`𝐅`$ corresponding to a given energy tensor $`T`$ of $`𝐓`$ (see Figure 4).

In this paper we shall restrict the analysis of such an inverse problem to the subclass $`𝐓^{}`$ of $`𝐓`$ constituted by the set of perfect fluid energy tensors, that is to say, by those divergence-free energy tensors,

$$T=0_\alpha T^{\alpha \beta }=0$$
(1)
of the form

$$T=(\rho +p)uu+pg$$
(2)
In spite of its apparent clarity, it is worthwhile asking the following question: is this inverse problem physically meaningful?

In Section 2 we shall see that additional assumptions are necessary in order to obtain physically meaningful answers, and the assumption selected here will be that of local thermal equilibrium (l.t.e.). The necessary and sufficient condition for an energy tensor $`T`$ of $`𝐓^{}`$ to be in l.t.e. will be presented, and some important properties will be mentioned.

In Section 3 we shall show how our condition applies in a particular example: among the Szekeres-Szafron class II espace-time solutions, our condition easily allows us to obtain all the perfect fluid solutions which are in l.t.e. and gives the corresponding matter density, specific entropy and temperature.

Finally, in Section 4, as a further application, we shall present the necessary and sufficient conditions for a perfect fluid to be an ideal gas.

The proof of all our statements will be given elsewhere , where we will present a deeper analysis of the ideas related to the ”physical meaning” of perfect fluids.

## 2 Local thermal equilibrium

As described above, the set $`T_f`$ of energy tensors associated in $`\mathrm{\Omega }`$ to a fluid $`f`$ gives the energetic description of the set of unconstrained evolutions that correspond to the different initial configurations that the fluid may adopt. As a consequence, it is meaningless to try to find a physical interpretation to a perfect fluid energy tensor $`T`$ in $`\mathrm{\Omega }`$ submitted to the sole divergence-free condition. The reason is that the system $`\{(1),(2)\}`$ is not causal, so that not only one energy tensor corresponds to every initial configuration , but a partially arbitrary family of such tensors, which include arbitrarily advanced-retarded-like solutions as well as Maxwell’s demonds-like perturbations of the physical evolution . In order to select a physical (causal) evolution, one has to complete the above system conveniently . It is known  that its completion with a l.t.e. scheme is causal.

Here we shall choose to study the inverse problem for a divergence-free perfect fluid energy tensor under the hypothesis that its evolution takes place in l.t.e..

Let us remember that a perfect fluid is in l.t.e. if and only if i) the intensive variables of the fluid are related by equations of state, ii) these equations are compatible with the thermodynamic relation $`Tds=dϵ+pdv`$, iii) the matter density $`r1/v`$ is conserved, $`(ru)=0`$.

As already stated, the l.t.e. scheme thus defined is a causal completion for the system $`\{(1),(2)\}`$. But it is not a minimal causal completion in the sense that it introduces a clearly superabundant number, not only of equations, but also of unknowns. Because the system $`\{(1),(2)\}`$ consists of four equations for five unknowns, the following question can be asked: does an equivalent formulation of the l.t.e. scheme exits that is reduced to the addition to the system of a unique equation relating the five given unknowns?

This question is far from being academic. If the answer were positive, not only would we dispose of an easy deductive algorithm to detect whether or not a given divergence-free perfect fluid energy tensor evolves in l.t.e., but we would also dispose of an equational and conceptual simplified version of l.t.e.: a version that would show that, contrary to what is indicated by general opinion and historic development, the concept of l.t.e. does not need a thermodynamic, but only a dynamic, purely energetic background.

In fact, in a very different conceptual situation, we already answered this question positively some years ago . The result is the following theorem:
Theorem (Coll-Ferrando, 1989): A divergence-free perfect fluid energy tensor evolves in l.t.e. if, and only if, the space-time function

$$\chi \frac{\dot{p}}{\dot{\rho }}$$
(3)
called the indicatrix of l.t.e., depends only on the variables $`p`$ and $`\rho `$ :

$$d\chi dpd\rho =0$$
(4)
We believe that this simple result is very interesting from the physical point of view because of the following remarks:

i) This theorem says, in other words, that a relation of the form

$$\dot{p}=\chi (p,\rho )\dot{\rho }$$
(5)
is a minimal causal completion to the equations $`.T=0`$ for a perfect fluid.

ii) Condition (4), $`d\chi dpd\rho =0`$, is a deductive condition of l.t.e. for the hydrodynamic variables $`u`$, $`p`$ and $`\rho `$.

iii) The ”iff” character of the theorem implies that this condition constitutes an alternative definition of l.t.e.. And surprisingly enough at first glance, this alternative definition involves only hydrodynamic, energetic and evolutive concepts, but not thermodynamic ones.

iv) If the conditions of the theorem are verified, that is, if the perfect fluid evolves in l.t.e., then the indicatrix $`\chi `$ becomes a function of state, $`\chi (\rho ,p)`$, and it physically represents the square of the velocity of the sound in the fluid ,

$$\chi (\rho ,p)v_{sound}^2$$
(6)
v) From the above interpretation, one has the following necessary condition of physical reality:

$$0\chi 1$$
(7)
In the next Section we have selected a general (family of) perfect fluid space-time(s) to show how our theorem is applied in a particular case.

## 3 Class II Szekeres-Szafron space-times

The Szekeres-Szafron solutions to Einstein Equations constitute one of the largest families of perfect fluid exact solutions with no generic symmetries. A class of them, the so called class II, is given by a line element $`ds^2`$ of the form

$$ds^2=dt^2R^2\left\{(B+P)^2dx^2+\frac{dy^2+dz^2}{\left[1+\frac{k}{4}(y^2+z^2)\right]^2}\right\}$$
(8)
with

$$P\frac{\frac{1}{2}(y^2+z^2)U+yV_1+zV_2}{1+\frac{k}{4}(y^2+z^2)}$$
(9)
where $`R(t)`$, $`U(x)`$, $`V_1(x)`$, $`V_2(x)`$, $`V(x)`$ are arbitrary functions, $`k\{0,\pm 1\}`$, and $`B(x,t)`$ is a solution of the equation:

$$\ddot{B}+3\frac{\dot{R}}{R}\dot{B}\frac{kB+U}{R^2}=0$$
(10)
In these coordinates the perfect fluid is comoving, and its pression $`p`$ and energy density $`\rho `$ are given by

$$p=\frac{2R\ddot{R}+\dot{R}^2+k}{R^2}$$
(11)
$$\rho =\frac{2R\dot{R}\dot{B}+3(B+P)\dot{R}^2+k(B+3P)2U}{R^2(B+P)}$$
(12)
In order to characterize, among these fluids, all those that evolve in l.t.e., it is convenient to first detect the structure of the above function $`B(\rho ,p)`$. Such a structure is given by the following lemma:
Lemma 1: The general solution of the equation

$$\ddot{B}+3\frac{\dot{R}}{R}\dot{B}\frac{kB+U}{R^2}=0$$
(13)
is of the form

$$B=\alpha a+(k\beta +1)b+\beta U$$
(14)
where $`a(x)`$ and $`b(x)`$ are arbitrary functions and $`\alpha (t)`$ and $`\beta (t)`$ verify

$$\ddot{\alpha }=3\frac{\dot{R}}{R}\dot{\alpha }+\frac{k}{R^2}\alpha $$
(15)
$$\ddot{\beta }=3\frac{\dot{R}}{R}\dot{\beta }+\frac{1}{R^2}(k\beta +1)$$
(16)
The isobaric case $`\dot{p}=0`$, which according to expression (11) corresponds to particular choices of $`R(t)`$, obviously verifies our condition of l.t.e..

In order to select all other solutions that evolve in l.t.e., it is now easy, because $`p=p(t)`$, to develop expression (4) directly, and thus allows us to neglect time derivatives of $`\rho `$ and $`\chi `$. The result is
Theorem 1: The non isobaric class II Szekeres-Szafron perfect fluids that evolve in l.t.e. are those for which

$$a(x)=0\mathrm{𝑜𝑟}a(x)0,k=0,U(x)=0$$
(17)
For such fluids it is then easy, starting from the ”old” definition of l.t.e., to find their thermodynamic variables. One obtains:
Theorem 2: For the non isobaric class II Szekeres-Szafron perfect fluids that evolve in l.t.e., the matter density $`r`$ is given by

$$r=\frac{\varphi (u)}{R^3(\beta u+1)},u\frac{kb+U}{b+P}$$
(18)
for the case $`a(x)=0`$, and by

$$r=\frac{\varphi (u)}{R^3(\alpha +u)},u\frac{b+P}{a}$$
(19)
for the case $`a(x)0`$, $`k=0`$, $`U(x)=0`$. The specific entropy $`s`$ and the temperature $`T`$ are, respectively

$$s=s(u),T=\frac{1}{s^{}}\left(\frac{\rho +p}{r}\right)^{}$$
(20)
where the prime denotes derivative with respect to $`u`$.

We must note the relatively easy way, and the simple and compact general results that may be obtained by direct application of our above theorem on l.t.e.. It is worthwhile comparing them with the partial expressions obtained, only for a partial subclass of the class II Szekeres-Szafron solutions, with the method claimed by Quevedo and Sussman in reference 8.

## 4 When is a perfect fluid an ideal gas?

Results of the above type allow us to easily find all the families of perfect fluid solutions of a general class that evolve in l.t.e.. But, what does a family of perfect fluid solutions mean physically? Is it a family of physical fluids, every one of them in a particular evolution state?, is it a family of evolution states of one particular physical fluid?, or is it a hybrid family?

There are no known results that allow us to answer this question. Moreover, even for a unic given perfect fluid solution one does not dispose of simple criteria to detect its plausible physical meaning.

Here, to show how one can solve these problems, we present a simple criterion for a perfect fluid to be a conventional ideal gas.
Theorem 3: The necessary and sufficient condition for a divergence-free perfect fluid energy tensor, $`T=(\rho +p)uu+pg`$, to represent the l.t.e. evolution of a classical ideal gas,

$$pv=kT,k\frac{nR}{m},$$
(21)
with specific internal energy

$$ϵ=c_vT,$$
(22)
is that the indicatrix $`\chi `$ be of the form

$$\chi =\frac{\gamma p}{\rho +p}$$
(23)
with

$$1\gamma 2.$$
(24)
Then, the constants $`k`$ and $`c_v`$ are related by

$$\gamma =1+\frac{k}{c_v}$$
(25)
It is important to note the following points:

i) In practice, it is convenient to verify directly that one has

$$d\frac{(\rho +p)\dot{p}}{p\dot{\rho }}=0$$
(26)
ii) If it is the case, then the constant

$$\gamma \frac{(\rho +p)\dot{p}}{p\dot{\rho }}$$
(27)
fixes, but only fixes, the quotient $`k/c_v`$ of the gas. Thus, the values $`\gamma =5/3`$ and $`\gamma =7/5`$ correspond respectively to monoatomic and diatomic ideal gases.

Other gases, not necessarilly ideal ones, will be characterized elsewhere .