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# 1 Introduction

## 1 Introduction

If one puts aside philosophical questions created by the perceived counterintuitive features of the quantum mechanics that are frequently discussed in the literature on the quantum measurement problem (an entry point to this literature is provided, e.g., by the collections of papers  or monographs ) it is easy to see that the physics of quantum measurements is fairly well understood by now at least on a qualitative level. The process of quantum measurement is dynamic interaction between a microscopic quantum system and a macroscopic detector that establishes correlations between the states of these systems. Although it is impossible to give a universal definition of “macroscopic” in this context, a reasonable working definition is that the macroscopic detector is a system with negligible quantum fluctuations. Such systems are quite abundant in nature and can be described quantitatively within the framework of quantum mechanics.

Since the description of quantum measurement process as an interaction between microscopic and macroscopic systems is quite broad, it is of interest to see whether there are any universal quantitative features of this process that are independent of specific physical realization of the detectors and the measured system. The purpose of this work is to show that one such universal characteristics of quantum measurements can be obtained from the linear response theory. This result was first pointed out in , and this work gives its more concise and accurate presentation.111 Note added in the electronic version. After this manuscript was submitted for publication, the author’s attention was drawn to Ref.  which presents similar development of Ref. .

An example of the area where a universal description of the quantum measurement process can be particularly useful is mesoscopic quantum dynamics of solid-state, in particular Josephson-junction, qubits. Recent widespread interest in the development of solid-state qubits for quantum information processing brought with it the discussion of a large number of different detectors for measurement of quantum dynamics of these qubits. These detectors include quantum point contacts , normal-metal  and superconducting  SET transistors operated in different regimes, resonant tunneling structures , generic mesoscopic conductors , SQUIDs . With such a variety of detectors (the list of references above is by no means complete), a possibility of giving a quantitative description of some detector characteristics independently of its physical realization is obviously very helpful for understanding of the process of quantum measurement of mesoscopic qubits.

## 2 Measurement model and basic relations

As was discussed in the introduction, the most essential feature of the model of the quantum measurement process considered in this work is its universality. The model applies to measurement with an arbitrary detector which has to satisfy only some basic conditions. Schematics of this model is shown in Fig. 1 and includes the measured system and the detector with the Hamiltonians $`H_S`$ and $`H_D`$, respectively. The detector and the system are coupled through an interaction Hamiltonian $`H_{int}`$ which almost without any loss of generality can be written as the product of some system “coordinate” $`x`$ and the detector “force” $`f`$:

$$H_{int}=xf.$$
(1)
The operator $`x`$ acts as the observable measured by the detector. In principle, one could imagine a situation when a detector couples to some system through a combination of the several product terms like (1), but the detector sensitive to several different dynamic variables of the system would be quite unusual.

The general structure of the Hamiltonian of the system:

$$H=H_S+H_D+H_{int},$$
(2)
is similar to the Hamiltonians studied in the discussions of the dissipative quantum dynamics based on the “system+reservoir” models (see, e.g., ) if the detector is identified with the reservoir. This analogy is not accidental, and many features of the dynamics of the measurement process are similar to the dissipative quantum dynamics of open systems. For instance, as will also be discussed below, coupling to the detector leads to the dephasing of the measured system, similar to the reservoir-induced dephasing.

There are, however, important differencies between the two situations. The main difference is that in the case of the dissipative quantum dynamics induced by a reservoir, changes in the reservoir caused by the system of interest are assumed to be unobservable, while the detector as a matter of principle should have an output observable $`o(t)`$ that provides some information about its state. To represent the complete measurement process, $`o(t)`$ should behave as a classical variable, i.e. magnitude of quantum fluctuations in it should be much smaller than its classical component. This condition implies that there is another difference between the detector and the dissipative reservoir. The detector should be able to convert weak quantum input signal $`x(t)`$ into the classical output signal $`o(t)`$ that is large on the scale of quantum fluctuations. Such a transformation requires amplification and can not be achieved in an equilibrium system, i.e., the detector, in contrast to the reservoir has to be driven out of the equilibrium.

In the case of the dissipative reservoirs, it is well known that the linear response theory is a powerful tool that produces a general quantitative statement, fluctuation-dissipation theorem, about the reservoir-induced relaxation. The theorem is independent of the specific microscopic model of the system. The analogy between the measurement and the environment-induced relaxation leads naturally to the question of whether some general relations characterizing quantum measurements can be derived from the linear response theory. As we will see below, the answer to this question is yes, and the linear response theory applied to the measurement problem enables one to derive generic restriction on the energy sensitivity of a general linear quantum detector. The obtained relation characterizes how close the detector is to being quantum-limited, i.e., how close the detector-induced back-action dephasing in the measured system is to the fundamental limit set by the quantum mechanics. While such a restriction on the energy sensitivity was known before in several specific detector models, linear response theory establishes it for an arbitrary detector weakly coupled to the measured system.

For the linear response theory to be applicable to the measurement set-up shown in Fig. 1, and to provide some meaningful information, the detector has to satisfy certain conditions. Two most important are:

* the detector is weakly coupled to the measured system so that its response to variations in this system is linear,
* the detector is in the stationary state.

Since the detector can not be in equilibrium, the second item on this list generalizes the equilibrium condition of the standard linear-response theory. Both of these conditions are not very restrictive, and are satisfied in many experimental situations.

Linearity of the response is not sufficient to specify the detector properties completely, since the linear response coefficient can have an arbitrary frequency dependence, i.e. one needs to assume some spectral characteristics of the detector. Here we consider the simplest case when the response time of the detector is much shorter that the characteristic time of the dynamics of the measured system. This means that the response coefficient $`\lambda `$ is constant in the relevant frequency range. Although this assumption is less fundamental that the previous two, and in principle can be avoided, it simplifies the discussion considerably.

Quantitatively, linearity of the detector response means that dynamics of the detector operators can be treated in the lowest order of the perturbation theory in the detector-system coupling $`H_{int}`$. Expanding the evolution operator $`U(t)=e^{iHt/\mathrm{}}`$ with the total Hamiltonian (2) upto the first order in $`H_{int}`$ we see that the detector output $`o(t)`$ can be written as:

$$o(t)=q(t)+\frac{i}{\mathrm{}}^t𝑑\tau [f(\tau ),q(t)]x(\tau ).$$
(3)
The first term $`q(t)e^{iH_Dt/\mathrm{}}o(0)e^{iHt/\mathrm{}}`$ in this expression can be interpreted as the output noise of the detector that exists even in the absence of the input signal, while the second term represents the detector’s linear response to measured system. In zeroth order in coupling, the detector and the system are independent, so the averages over their states in eq. (3) can be taken separately. Tracing out the detector variables in (3) we obtain the regular expression for the linear response, extended to the situation when the “driving force” $`x(t)`$ is a quantum operator. With the adopted assumption of instantaneous detector response:

$$\frac{i}{\mathrm{}}[f(t),q(t+\tau )]_D=\lambda \delta (\tau 0)$$
(4)
eq. (3) reduces to:

$$o(t)_D=\lambda x(t).$$
(5)
The infinitesimal shift in the argument of the $`\delta `$-function in (4) represents small but finite response time of the detector, and is needed to resolve the ambiguity in eq. (3). In equation (4), we used the assumption (introduced above) that the detector is in the stationary state and the $`q`$$`f`$ correlator depends therefore only on the difference of the time arguments, and $`\mathrm{}_D`$ denotes the average of the stationary detector density matrix. Since $`q(t)`$ represents the output noise, we took $`q(t)_D=0`$.

Similarly, if the detector produces some non-vanishing average force $`f(t)_DF0`$, it is natural to include it in the system Hamiltonian $`H_S`$, and one can therefore always assume that $`f(t)_D=0`$. Dynamics of the coupling force $`f`$ generated by the detector is characterized then by the correlation function $`ff(t)_D`$ and physically can be viewed as “back-action” noise that dephases the measured system. Following the assumption of the instantaneous response (4) we also take both the output noise and the back-action noise to be $`\delta `$-correlated:

$$q(t+\tau )q(t)_D=2\pi S_q\delta (\tau ),f(t+\tau )f(t)_D=2\pi S_f\delta (\tau ).$$
(6)
Here we introduced spectral densities of the output ($`S_q`$) and back-action ($`S_f`$) noise that are constant in the relevant low frequency range. Besides the infinitely small response time of the detector, eqs. (6) also imply that dynamics of both $`q(t)`$ and $`f(t)`$ is essentially classical, since the frequency-dependent part of the spectrum that corresponds to zero-point fluctuations gives negligible contribution to the correlators (6).

## 3 Back-action dephasing versus acquisition of information

Qualitatively, measurement dynamics defined by the total Hamiltonian (2) and assumptions (4) and (6) about the detector characteristics, includes two related processes. One is the dephasing and relaxation/excitation of the measured system by the back-action force $`f(t)`$. This part of the measurement is very similar to the dissipative quantum dynamics of a system weakly coupled to a reservoir. The second process is acquisition of information about the state of the measured system reflected in the evolution of the detector output $`o(t)`$. On the quantitative level, measurement dynamics depends on the Hamiltonian $`H_S`$ of the measured system and the operator structure of the measured observable $`x`$.

Probably the simplest situation which can be used to illustrate the two qualitative aspects of the measurement dynamics is the case of the stationary system, $`H_S=0`$, with an observable $`x`$ that has several discrete eigenstates $`|j`$: $`x|j=x_j|j`$ with eigenvalues $`x_j`$. Since under the assumption (6) the back-action force $`f(t)`$ can be treated as a classical random force generated by the detector, one can write the time-evolution equation directly for the density matrix $`\rho `$ of the measured system. From the Hamiltonian (2), this equation in the basis of $`x`$-eigenstates is:

$$\dot{\rho }_{j,j^{}}=\frac{i}{\mathrm{}}(x_jx_j^{})f(t)\rho _{j,j^{}}.$$

Solution of this equation averaged over different realizations of $`f(t)`$ using eq. (6) gives:

$$\rho _{j,j^{}}(t)=\rho _{j,j^{}}(0)e^{\mathrm{\Gamma }_dt},\mathrm{\Gamma }_d\pi (x_jx_j^{})^2S_f/\mathrm{}^2.$$
(7)
From this equation one can see that when the system is prepared in the initial state which is a superposition of the eigenstates of $`x`$, i.e. $`\rho _{j,j^{}}`$ has non-vanishing off-diagonal elements, interaction with the detector dephases the system and suppresses these off-diagonal elements. The suppression does not happen only if the states $`j`$ and $`j^{}`$ are degenerate with respect to $`x`$: $`x_j=x_j^{}`$, so that the detector does not distinguish them. Equation (7) shows also that the rate $`\mathrm{\Gamma }`$ of such a back-action dephasing is determined by the spectral density of the back-action force $`f(t)`$.

The dephasing (7) leads to diagonalization of the density matrix in the basis of the measured observable and coincides with the simplest instance of the environment-induced dephasing of an open quantum system. From the measurement perspective, it describes the dynamic side of the “wave-function collapse”, since when the measurement is completed, the measured system should find itself in one of the eigenstates of the observable being measured, i.e. $`x`$. The density matrix diagonal in the $`x`$ representation corresponds precisely to such a situation. This interpretation of the back-action dephasing is strengthened by the relation between the dephasing rate $`\mathrm{\Gamma }`$ and the rate of information acquisition - see, e.g., . Indeed, from this perspective, in the example of the preceding paragraph, the detector has to distinguish different eigenstates of the observable $`x`$ and to provide information in which eigenstate the system finds itself. According to the linear response relation (5), the difference between two eigenvalues of $`x`$, $`x_jx_j^{}`$, translates into the difference $`\delta o=\lambda (x_jx_j^{})`$ of the dc values of the detector output $`o`$. The characteristic time $`\tau _m`$ on which this difference in $`o`$ can be distinguished in the presence of the output noise is determined by the low-frequency spectral density $`S_q`$ of this noise. Averaging the $`\delta `$-correlated noise over the time interval $`\mathrm{\Delta }t`$ leaves characteristic noise amplitude $`\mathrm{\Delta }o=(2\pi S_q/\mathrm{\Delta }t)^{1/2}`$. The characteristic time $`\tau _m`$ of acquisition of the information about the dc value of the detector output, and therefore, about the eigenstate of the measured observable, is determined by the condition that the noise amplitude is reduced at least to half the distance $`\delta o`$ between the signal level. This condition gives

$$\tau _m=8\pi S_q/[\lambda (x_jx_j^{})]^2,$$
(8)
and shows that the relation between the back-action dephasing rate and the “measurement time” $`\tau _m`$ is independent of the eigenvalue difference $`x_jx_j^{}`$, and depends only on the linear-response parameters of the detector:

$$\tau _m\mathrm{\Gamma }_d=8(\pi /\mathrm{}\lambda )^2S_qS_f.$$
(9)
Now the final step is to show that the linear response theory relates parameters $`\lambda `$, $`S_q`$, $`S_f`$, in such a way that the dephasing rate is fundamentally linked to the measurement time:

$$\tau _m\mathrm{\Gamma }_d1/2.$$
(10)
To see this, we start by taking Fourier transform of eq. (4):

$$i\frac{\mathrm{}\lambda }{2\pi }=S_{fq}(\omega )S_{fq}^{}(\omega ),S_{fq}(\omega )=\frac{1}{2\pi }𝑑\tau e^{i\omega \tau }fq(\tau )_D.$$
(11)
Expanding expression for the correlator $`S_{fq}(\omega )`$ in the basis of the energy eigenstates $`|\epsilon `$ of the detector we obtain:

$$S_{fq}(\omega )=𝑑\epsilon \rho _D(\epsilon )\nu (\epsilon )\nu (\epsilon \mathrm{}\omega )\epsilon |f|\epsilon \mathrm{}\omega \epsilon \mathrm{}\omega |q|\epsilon ,$$
(12)
where $`\nu (\epsilon )`$ is the density of the detector energy states, and since the detector was assumed to be in the stationary state, its density matrix $`\rho _D(\epsilon )`$ in the energy basis is diagonal.

Making use of the expression (12) and similar expressions for noise spectral densities, we can establish an inequality relating them. To obtain it, we note that eq. (12) can be viewed from a somewhat artificial, but useful perspective as a scalar product of two functions of energy $`\epsilon `$, $`\epsilon \mathrm{}\omega |q|\epsilon `$ and $`\epsilon \mathrm{}\omega |f|\epsilon `$. Since both the density of states and the probability $`\rho _D(\epsilon )`$ are non-negative, the scalar product defined by eq. (12) satisfies all the usual requirements of the scalar product. Using the standard notation for this product, we can write (12) simply as

$$S_{fq}(\omega )=<f|q>.$$
(13)
Spectral densities of the back-action and the output noise can be also expressed in terms of this scalar product. The total spectral densities $`S_q`$, $`S_f`$ are defined as

$$S_q(\omega )=(S_{qq}(\omega )+S_{qq}(\omega ))/2,S_{qq}(\omega )=\frac{1}{2\pi }𝑑\tau e^{i\omega \tau }qq(\tau )_D,$$
(14)
with similar equations for $`S_f(\omega )`$. Writing the correlators $`S_{qq}(\omega )`$ and $`S_{ff}(\omega )`$ in the same way as $`S_{fq}(\omega )`$ (12) in the basis of the detector energy eigenstates one sees immediately that they again can be expressed very simply in the language of the introduced scalar product:

$$S_{qq}(\omega )=<q|q>,S_{ff}(\omega )=<f|f>.$$
(15)
Schwarz inequality for this scalar product gives, when applied to eqs. (13) and (15):

$$S_{ff}(\omega )S_{qq}(\omega )S_{fq}(\omega )^2.$$
(16)
Finally, combining eq. (11), inequality (16), similar inequality for components of the correlators at frequency $`\omega `$, and our assumption that the noise spectral densities $`S_q(\omega )`$ and $`S_f(\omega )`$ are constant at low frequencies, we see that

$$\lambda =4\pi \text{Im}S_{fq}/\mathrm{},$$

and therefore

$$|\lambda |\frac{4\pi }{\mathrm{}}[S_fS_q(\text{Re}S_{fq})^2]^{1/2},$$
(17)
where all spectral densities and the response coefficient are now taken at low frequencies. This inequality is the main result of application of the linear response theory to the measurement problem.

One consequence of the inequality (17) is the proof of the relation (10) between the back-action dephasing rate and the measurement time. It follows directly from eq. (17) that when the detector is “symmetric”, i.e. $`\text{Re}S_{fq}=0`$, so that there are no classical correlations between the back-action noise and the output noise, inequality (17) transforms eq. (9) directly into the (10). (The case of an asymmetric detector is discussed below.) In this derivation of (10), this inequality appears to be the consequence of some relation between the correlators appearing in the linear response theory. From the perspective of the measurement problem it can be interpreted in a much broader sense. Inequality (10) shows that in general the dephasing of the measured system by a detector can be arbitrary strong without providing any information on the system. However, acquisition of information about the state of the system creates some minimum dephasing that suppresses coherence between the eigenstates of the measured observable. The fact that such a minimum exists is dictated by the basic principle of quantum mechanics which requires the successful measurement of an observable to localize the system in one of the eigenstates of this observable. If the detector is such that it is causing only this minimum back-action dephasing dictated by quantum mechanics, it is typically referred to as “quantum-limited” or “ideal” detector.

Interplay between information acquisition by the detector and back-action dephasing of the measured system has a simple form of inequality (10) only in the situation of measurement of a static system. When the system Hamiltonian $`H_S`$ is non-vanishing, this interplay is affected by the dynamics of the system and in general manifests itself less directly. One studied example of this  is the measurement of a two-state system. Coherent quantum oscillations in this system are transformed by measurement into classical oscillations of the detector output. In this case, the trade-off between the back-action dephasing and information acquisition is reflected in the height of the oscillations peak $`S_m`$ in the output spectrum relative to the output noise $`S_q`$. Inequality (10) limits then the peak height: $`S_m/S_q4`$, with eaquality reached by measurement with a symmetric quantum limited detector.

Another system which has been studied in this context is harmonic oscillator . Similarly to the two-state system, dynamics of the measurement process is reflected in this case in the frequency spectrum of the detector output, which contains the detector output noise and a peak at the oscillator frequency. The trade-off between the detector back-action and information gain becomes relevant if one asks a question what is the minimum contribution of the detector noise to the spectrum. Qualitatively, there are two ways in which the detector noise contributes to the spectrum. The detector output noise gives direct contribution to the spectrum, while the back-action noise contributes to the output spectrum indirectly, by inducing additional oscillations at the detector input that are transformed to the output by the detector response. Minimization of the total noise contribution (reduced to the detector input and normalized to the zero-point spectrum of the oscillator in units of $`\mathrm{}/2`$) shows that the minimum total noise is given by the “energy sensitivity” $`ϵ`$:

$$ϵ=\frac{2\pi }{|\lambda |}[S_fS_q(\text{Re}S_{qf})^2]^{1/2}.$$
(18)
Energy sensitivity has the dimension of action, and relation (17) between the parameters of the linear response theory translates into the following limitation on $`ϵ`$:

$$ϵ\mathrm{}/2.$$
(19)
Inequality (19) can be expressed qualitatively as a statement that the detector, when measuring a harmonic oscillator, adds at least half an excitation quantum of this oscillator to the measured signal. This inequality was obtained for the first time in a different physical context of linear amplification of electromagnetic radiation, where this interpretation has direct meaning – see, e.g., the papers on quantum noise in linear amplifies reprinted in , also  and references therein. The magnitude of the signal in this context is described naturally by the number of photons in a mode and amplification is characterized by the dimensionless photon gain: the ration of these numbers in the output and input modes. Relation between such a linear amplifier and the linear detector considered in this work is established by the fact that in the limit of large gain, the input signal of the amplifier which in general can be quantum (i.e., contain only few photons) is transformed into the output signal which contains number of photons much larger than one and is in this sense classical. This means that the amplifier in this regime acts essentially as a detector, since after amplification of the signal to the classical level, it can be dealt with without any restrictions.

The last point to be made here concerns the case of an asymmetric detector. Such a detector is defined by the nonvanishing classical correlations between the output and back-action noises described by the real part of the spectral density $`S_{fq}`$. Comparison of eq. (9) for the trade-off between the measurement time and the back-action dephasing, and eq. (19) for the energy sensitivity shows that they behave differently in the case of non-vanishing $`\text{Re}S_{fq}`$. While the energy sensitivity (19) can reach its quantum limit even in asymmetric detectors with $`\text{Re}S_{fq}0`$, the $`\tau _m\mathrm{\Gamma }_d`$ product (9) in this situation can only be larger than its quantum limit $`1/2`$. The origin of this discrepancy is that in asymmetric detectors the output noise contains some information about the back-action noise which should be utilized to reach the optimum quantum-limited performance of the detector. In the simple treatment that lead to inequality (10), this information is lost, and as a result the dephasing is increased beyond the minimum required by the quantum mechanics. In the case of measurement of the harmonic oscillator, the noise minimization procedure implicitly makes use of this information, since the precise frequency where the noise is minimum depends on the correlation strength $`\text{Re}S_{fq}`$. In the case of information/dephasing trade-off, the information provided by the correlations contained in non-vanishing $`\text{Re}S_{fq}`$ can also be used to approach the quantum limit of dephasing. Conceptually (and probably also practically) the simplest way to use the information contained in the output noise of the detector to reduce the back-action dephasing is to apply the output noise with an appropriate transfer coefficient to the measured system together with the back-action noise. Although physically this procedure might require a rather complicated set-up that actually applies part of the detector output to the measured system, formally this is achieved by simply redefining the back-action force of the detector:

$$ff(\text{Re}S_{fq}/S_q)of^{}.$$

It is straightforward to see that the rate $`\mathrm{\Gamma }_d^{}`$ of back-action dephasing created by the redefined force $`f^{}`$ in measurement of a static system can indeed be equal to the quantum minimum of $`1/2\tau _m`$ even for asymmetric detectors with $`\text{Re}S_{fq}0`$, if the relation (17) between the linear response properties of this detector is satisfied as equality. The same conclusion can be reached for measurement of the two-state systems . This provides one more example of the fact that many physical characteristics of the measurement process can be understood conveniently as dynamics of information.

Acknowledgements

The author would like to thank E.V. Sukhorukov for useful discussion of the results and for drawing his attention to Ref. . This work was supported in part by AFOSR and ARDA.


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# Spatially Resolved 3 µm Spectroscopy of IRAS 22272+5435: Formation and Evolution of Aliphatic Hydrocarbon Dust in Proto-Planetary NebulaBased on data collected at Subaru Telescope, which is operated by the National Astronomical Observatory of Japan.

## 1 Introduction

IRAS 22272+5435 (= HD 285858, SAO 34504) is an extremely carbon-rich proto-planetary nebula (PPN) with peculiar infrared spectral features (Kwok, Volk, & Hrivnak, 1989; Geballe et al., 1992). A PPN is a transition object that has left the asymptotic giant branch (AGB) for a planetary nebula (PN), but it is not yet hot enough to ionize the surrounding AGB ejecta. The dust in a PPN is becoming optically thin, but has not been altered in the hard UV field of a PN. A carbon-rich PPN provides the best opportunity to study unprocessed solid carbon material immediately after the formation.

A classification of carbon dust in the interstellar medium (ISM) has been proposed by Geballe (1997) and Tokunaga (1997) based on the 3 $`\mu `$m infrared emission features (IEF). The class A sources are characterized by the intense and isolated aromatic features at 3.3 $`\mu `$m with an occasional association of weak and sharp peaks in the 3.4–3.5 $`\mu `$m region. They are the most common IEF observed toward young stellar objects (YSO), H II regions, PN, reflection nebulae, diffuse interstellar medium, and extragalactic sources (Tokunaga et al., 1991; Sloan et al., 1997; Jourdain de Muizon, D’Hendecourt, & Geballe, 1990; Sellgren, Werner, & Dinerstein, 1983; Tanaka et al., 1996; Moorwood et al., 1996). The class B sources are characterized by broad and prominent aliphatic features at 3.4 $`\mu `$m accompanied by the 3.3 $`\mu `$m aromatic features. The class B IEF has been found exclusively toward PPNs with extremely carbon-rich chemistry typified by IRAS 22272+5435 (Geballe & Van der Veen, 1990; Geballe et al., 1992). The simultaneous presence of aromatic and aliphatic features in class B sources makes a good laboratory for the study of the transition of the chemical composition of hydrocarbons.

Another advantage in observing a PPN is that the history of its dust formation is locked in the spatial distribution of the material. Since PPNs are less developed than PNs, most of them are spatially unresolved. However, the dust distribution around IRAS 22272+5435 has been well studied by subarcsecond mid-infrared imaging (Meixner et al., 1997; Dayal et al., 1998; Ueta et al., 2001), optical imaging with the Hubble Space Telescope/Wide Field Planetary Camera 2 (HST/WFPC2) (Ueta, Meixner, & Bobrowsky, 2000), and near-infrared polarimetric imaging (Gledhill et al., 2001). Ueta et al. (2000) classified IRAS 22272+5435 as a member of PPNs that are optically thin. It therefore ensures an unobscured view of the central part of the nebula.

Although observing at 3 $`\mu `$m is essential to assess the chemical composition of the carbon dust, a drawback is that the emitting region is physically more compact than at longer wavelengths. In addition, the contribution of the direct and scattered light from the central star is not negligible in the 3 $`\mu `$m region. Both to resolve the dust emission region and to achieve the high dynamic range required to distinguish the faint dust emission from the central star, an adaptive optics (AO) system must be integral part of the instruments used to make the spectroscopic observations. Our goal for this work is to use the high spatial resolution spectroscopy afforded by AO to better understand how hydrocarbon dust forms around a carbon-rich evolved star, and how it is processed before dissipating into the local ISM.

## 2 Observation

The spectroscopic observation was made on UT 2001 July 13 using the Infrared Camera and Spectrograph (IRCS; Tokunaga et al. 1998; Kobayashi et al. 2000) at the 8.2 m Subaru Telescope in conjunction with the AO system (Takami et al., 1998; Gaessler et al., 2002). The Subaru AO system is a 36-element curvature system installed at the front end of the telescope Cassegrain port. A medium-resolution grism was used with a 0$`\stackrel{}{\mathrm{.}}`$30 slit in the 58 mas camera section to provide spectra from 2.84 to 4.18 $`\mu `$m with a resolving power of 600–800. The visible central star was used as the wavefront reference source for the AO system. The position angle of the slit was 56 along the elongation in the mid-infrared image that corresponds to an equatorial density enhancement of the nebula (Ueta et al., 2001). The spectra were recorded by nodding the tip-tilt mirror inside the AO system by 2″ along the slit to subtract the sky emission and dark current images. The total on-source integration time was 720 s. A nearby F8V star HR 8472 was observed as a spectroscopic standard at similar airmass. The spectroscopic flat field was obtained at the end of the night with a halogen lamp.

## 3 Data Reduction and Results

We obtained the one-dimensional spectra of IRAS 22272+5435 using the IRAF111IRAF is distributed by the National Optical Astronomy Observatories, which are operated by the Association of Universities for Research in Astronomy, Inc., under a cooperative agreement with the National Science Foundation. aperture extraction package. The aperture width was about equal to the FWHM of the spatial profile (4-pixel or 0$`\stackrel{}{\mathrm{.}}`$23). We set the extraction apertures at the central star and another 14 locations along the slit (Figure 1). We found the spectra recorded at the nodding positions A and B to be slightly different. The most likely reason for this is that the mirror nodding axis was not precisely straight to the slit, and we observed slightly different parts of the nebula. The data obtained at positions A and B were reduced separately. The wavelength calibration was performed by fitting over 60 telluric absorption lines in the 3 $`\mu `$m region. The flux calibration relative to the standard star was made assuming the intrinsic spectrum of a F8V star is represented by a Planck function of $`T_{\mathrm{eff}}=`$ 6100 K (Tokunaga, 2000). The hydrogen recombination lines in the standard star spectrum were fit with a Gaussian function and subtracted before dividing. The details of the reduction can be found elsewhere (Goto et al., 2002).

The result is shown in Figure 2 after being normalized to the continuum at 3.5 $`\mu `$m. No hydrocarbon emission feature is seen at the position of the central star. Instead we observe absorption bands with the hydrocarbon emission bands becoming evident only at 0$`\stackrel{}{\mathrm{.}}`$35 from the central star. The integrated intensity of the hydrocarbon emission bands is consistent with that of 5″ aperture spectroscopy formerly reported by Geballe et al. (1992). The absence of hydrogen recombination lines at 3.74 $`\mu `$m (Pf$`\gamma `$) and 4.05 $`\mu `$m (Br$`\alpha `$) ensures that no H II region has developed at the center of the nebula. The spectrum continuum is approximately represented by a power law. The continuum flux around the central star is most likely the light scattered by large dust grains in the nebula superposed on the halo component of the point-spread function of the central star. The continuum subtracted spectra are shown in Figure 3.

## 4 Discussion

### 4.1 Molecular Absorption Features near the Center

A wealth of absorption features is found in the spectra of IRAS 22272+5435 close to the central star. The carbon atoms consisting of C-H bonds have one of $`sp`$, $`sp^2`$, or $`sp^3`$ hybridized orbitals, in which triple, double, and single bonds connect the carbon with adjacent atoms. The stretching vibration mode of different C-H bonds shows up as various band structures in the 3 $`\mu `$m region. The individual ro-vibrational transition lines are not resolved with the present spectral resolution, and higher resolution spectroscopy will be required to make a solid identification of the absorption lines. The only exception is the absorption bands at 3.0 $`\mu `$m, which are identified with the combination of $`P`$ and $`R`$ branches of $`sp`$ C-H bonds in C2H2 and HCN. Figure 4 shows the same molecular features in CRL 618 (Chiar et al., 1998) and those computed with the HITRAN database (Rothman et al., 1998).

The molecular absorption features are evident close to the central star, but they disappear abruptly at 0$`\stackrel{}{\mathrm{.}}`$47 or 750 AU ($`d`$ = 1.6 kpc is assumed based on a private communication with Nakashima 2002). The broad emission bands at 3.3 and 3.4 $`\mu `$m become strong in turn at 600 AU (Fig. 3). This is the first time that both the hydrocarbon gas and dust are observed in a circumstellar environment in clearly separated locations. It indicates the hydrocarbon molecules are indeed the source of the solid dust material, and that the molecular gas that failed to be involved with the grain formation is being observed near the central star.

### 4.2 Hydrocarbon Dust Emission at 3.3–3.4 $`\mu `$m

The most common IEF in the ISM is the class A type emission ubiquitously observed where the carbon dust is exposed to a hard UV field. The emission carrier has been attributed to aromatic species (Duley & Williams, 1981) such as neutral and ionized polycyclic aromatic hydrocarbons (PAH; Léger & Puget 1984; Allamandola, Tielens, & Barker 1985, 1989 and references therein). The 3.3 $`\mu `$m feature matches the ro-vibrational band of the stretching vibration of aromatic $`sp^2`$ C-H bonds. While the class A IEF is observed with hot excitation sources with $`T_{\mathrm{eff}}>`$ 20000 K, the central stars of class B sources are typically F–G type supergiants whose effective temperature is $`T_{\mathrm{eff}}`$ = 4500–7000 K. The radiation environment of class B sources is much more benign with less UV photons available. The aromatic molecules absorbs UV-visible photons with a long wavelength cut-off. The larger molecules have a longer cut-off wavelength (Desért, Boulanger, & Puget, 1990; Schutte, Tielens, & Allamandola, 1993). The soft radiation field yet strong emission of class B features implies larger hydrocarbons than those of class A sources are responsible.

What distinguishes class B spectra most clearly from class A IEF is broad and intense emission at 3.4 $`\mu `$m. It was once proposed that a hot band of anharmonic oscillation of aromatic C-H bonds is responsible (Barker, Allamandola, & Tielens, 1987). However, the weakness or absence of overtone bands at the 1.6–1.8 $`\mu `$m region makes this hypothesis unlikely (Magazzu, & Strazzulla, 1992; Siebenmorgen & Peletier, 1993; Geballe et al., 1994). Instead Schutte, Tielens, & Allamandola (1993) proposed that the aliphatic C-H bonds of superhydrogenated benzene rings account for the 3.4 $`\mu `$m emission. Hydrogenated PAH (Hn-PAH) is rich in $`sp^3`$ C-H bonds where the double bonds in the benzene rings are partially saturated by extra attachment of hydrogens. Bernstein, Sandford, & Allamandola (1996) have shown that some Hn-PAH have similar absorption peaks that agree well with 3.4–3.5 $`\mu `$m features of a class A source Orion bar. Joblin et al. (1996) argue that the aliphatic C-H bonds, in particular -CH2 in long chains or cyclic aliphatic hydrocarbons, best match the strong 3.42 $`\mu `$m features of class B source IRAS 05341+0852.

In the mid-infrared region, IRAS 22272+5435 shows two broad emission features near 8 $`\mu `$m and 12 $`\mu `$m (Buss et al., 1993), which contrasts with typical class A IEF (Sloan et al., 1999). Allamandola, Hudgins, & Sandford (1999) tried several laboratory compounds of PAH to reproduce IEF of class A and class B sources. They suggested that there is a systematic difference in the character of aromatic species required to fit the IEF in the two different environments. The class A IEF is most closely reproduced by compounds of cations of stable PAH species, while neutral and less stable PAH species are a better match to the broad features of class B sources.

Specific chemical materials have been proposed for the class B IEF carriers by many authors. Those substances are in a more solid form, and laboratory spectroscopy indicates they are rich in $`sp^3`$ hybridized bonds. These are the more common characteristics of amorphous carbons, totally fit in the above modifications required for the conventional aromatic species, namely, larger, more neutral, and more aliphatic materials for class B IEF. The possible carriers presented so far are all successful in reproducing the spectral shape from 3.3 to 3.4 $`\mu `$m. These include a mixture of PAH molecules fully reprocessed by energetic hydrogen plasma (Beegle, Wdowiak, & Arnoult, 1997; Arnoult, Wdowiak, & Beegle, 2000), carbon nanoparticles produced by laser pyrolysis of C2H4 and C4H6 (Herlin et al., 1998) or C2H2 (Schnaiter et al., 1999), hydrogenated amorphous carbon prepared by eximer laser ablation of graphite in a hydrogen rich atmosphere (Scott, Duley, & Jahani, 1997; Grishko & Duley, 2000), and quenched carbonaceous composite produced by the plasma deposition technique with CH4 (Sakata et al., 1990; Goto et al., 2000). Semianthracite coal grains (Guillois et al., 1996) are also successful in reproducing the aliphatic band at 3.4 $`\mu `$m and substructures in the mid-infrared feature and overall continuum shape. Since there is no unique laboratory analog, we refer the carrier of the class B emission features at 3.3–3.4 $`\mu `$m as “hydrocarbon dust” in the following text. The hydrocarbon dust is rich in both aromatic and aliphatic C-H bonds.

### 4.3 Variations of Aliphatic and Aromatic Abundance

Figure 5 shows the emission feature at 600 to 1300 AU from the central star at the northeast sector of the nebula. The relative intensity of the aliphatic feature at 3.4 $`\mu `$m to the aromatic feature at 3.3 $`\mu `$m decreases with the distance from the central star. We discuss two processes that could modify the relative abundance of the aliphatics to the aromatics.

First, we examine the formation of the aliphatic C-H bonds on the surface of carbon particles. Mennella et al. (1999) demonstrated that $`sp^3`$ hybridized C-H bonds are newly formed by exposing pure carbon particles to an atomic hydrogen atmosphere. The activated aliphatic band successfully reproduces the 3.4 $`\mu `$m absorption feature observed toward the Galactic center. They discuss that the carrier responsible for the 3.4 $`\mu `$m absorption ubiquitously observed toward highly reddened objects does not originate in cold dark clouds as has been proposed by Greenberg et al. (1995), but in the diffuse ISM where the destruction of C-H bonds by UV photolysis is equilibrated by rehydrogenation with ample atomic hydrogen (Mennella et al., 2001, 2002). Tielens et al. (1994) proposed a similar mechanism for the formation of aliphatic C-H bonds by hydrogenation of a graphite surface amorphized by the ion bombardment in the interstellar shocks. The process supposedly plays an important role in the production of the 3.4 $`\mu `$m absorption feature in the Galactic center sources (Schnaiter et al., 1999). Chiar et al. (1998) proposed that the shocks caused by the fast wind at the last stage of the post-AGB evolution is relevant to the formation of the 3.4 $`\mu `$m absorption carriers in CRL 618.

However, the freshly formed aliphatic bands do not match the emission feature we observed. In Figure 6 we compare the emission feature of IRAS 22272+5435 with the absorption features of carbon particles from Mennella et al. (1999), CRL 618 (Chiar et al., 1998) and the Galactic center (Chiar et al., 2000), as well as the laboratory analog of Goto et al. (2000). Indeed, the hydrogenated nano-size carbon particles of Mennella et al. (1999) reproduce the observed absorption band well; the discrepancy with IRAS 22272+5435 is obvious, indicating different carriers. Considering CRL 618 is a PPN more evolved than IRAS 22272+5435 with a compact H II region and a hot B0 star at the center of the nebula, the availability of UV might be critical to producing the particular chemical composition of the absorbing aliphatic hydrocarbons.

The thermal annealing of aliphatic material better fits the observed spectral variation. Figure 5 shows the 3 $`\mu `$m spectra of a laboratory analog of hydrocarbon dust subjected to thermal annealing at different temperatures (Goto et al., 2000). The model carbon dust produced by the plasma vapor deposition method of CH4 has rich $`sp^3`$ hybridized C-H bonds when it is deposited. As the annealing temperature becomes hotter in the postprocessing, the substance is dehydrogenated and graphitized. It gradually acquires strong continuum absorption, less prominent spectral features, and weak aliphatic features relative to the aromatic one. The thermal transformation of the aliphatic material is well studied in laboratory experiments with amorphous carbon films (Robertson, 1991; Bounouh et al., 1995). Similar spectral alterations have been also reported with hydrogenated amorphous carbons (Scott & Duley, 1996; Scott, Duley, & Jahani, 1997; Grishko & Duley, 2000; Mennella et al., 1996). The resemblance between the laboratory and the observed spectra indicates a similar process takes place in IRAS 22272+5435.

### 4.4 Thermal Process

#### 4.4.1 Heat Source

For the thermal annealing of aliphatic material to take place, we need an adequate heat source for the raw material. The chemical composition of the thermally processed material is sensitive to the annealing temperature. The aliphatic to aromatic ratio observed in IRAS 22272+5435 indicates that the hydrocarbon dust has undergone heating to about 760 K (Figure 5).

In the investigation of heating mechanisms, we first assumed the thermal annealing is currently in progress at $``$1000 AU away from the star, where the hydrocarbon emission is being observed. The equilibrium temperature at 1000 AU is too cool for annealing to happen. Ueta et al. (2001) solved the two-dimensional radiative transfer model to get $`T_{\mathrm{dust}}`$ = 200 K at 800 AU from the star, which is again too cool for the thermal annealing. Shock heating could be an alternative heat source; however, no sign of shock-induced molecular hydrogen emission has been observed in the 2 $`\mu `$m spectrum (Hrivnak, Kwok, & Geballe, 1994).

The heating mechanism is not necessarily a thermal equilibrium process. Thermal fluctuation or stochastic heating occurs when the energy of a single incident photon exceeds the total heat capacity of a grain. As no hydrogen recombination lines are detected in IRAS 22272+5435, no photons more energetic than Ly$`\alpha `$ or $`h\nu `$ = 10.2 eV are available. It is found that a grain should be smaller than 6 Å in radius ($`N_C<`$ 100) to be heated to 760 K by a single Ly$`\alpha `$ photon. We use the empirical specific heat of graphite measured at a low temperature (Touloukian & Buyco, 1970) and the graphite mass density 2200 kg m-3 in estimating the heat capacity. This is very small for a solid particle; however, grains of this size have been considered as a common constituent of reflection nebulae to account for the hot blackbody continuum of about 1000 K (Sellgren, 1984).

Alternatively, as a PPN is a mass-losing object, the observed spatial variation could be interpreted as a record of the history of grain production of the central star. The changing chemical composition at the outer circumstellar shell could represent the temporal transition of hydrocarbon output during the evolution of the PPN. The possible mode-switching in the production of dust has been proposed by Buss et al. (1993); Geballe (1997); Kwok, Volk, & Hrivnak (1999); and Kwok, Volk, & Bernath (2001) to account for the systematic difference of the IEF in PNs and their progenitor PPNs. Thus, the thermal processing is not necessarily a current ongoing event. Actually, the most obvious heat source in the nebula is the central star and the warm circumstellar shell close to it. The particular chemical composition, or a sign of thermal processing, would be acquired when a grain was still in the warm environment near the star. We will call the inhomogeneous chemical composition resulting from the temporal transition of grain formation the “old record” scenario. In the scenario, the thermal processing was completed close to the central star, and is being observed now when the dust grains with varying chemical compositions are blown off to 1000 AU away from the star.

We will consider two heating scenarios in the following discussion, (1) the ongoing stochastic heating of a very small grain, and (2) the old record scenario in which the spatial variation in the chemical compositions originates in the past at the time of grain formation in the warm region near the central star.

#### 4.4.2 Preserving Aliphatic Material

The immediate problem with the stochastic heating scenario is how the aliphatic material could survive through the warmer environment closer to the central star. The physical conditions are more favorable to active thermal annealing there; for instance, at the temperature of carbon condensation, the aliphatic material should be totally graphitized.

Before discussing the preservation of the aliphatic material, first we consider the location where the ultra-small grains could form. Because of the lack of an efficient destructive mechanism, a grain monotonically grows in the mass-loss wind as it travels through the circumstellar shell (Gail & Sedlmayr, 1988). Thus, a small grain can be formed only at the outer region of the envelope, where the grain growth is very inefficient; otherwise, the final dimension would be too large (Figure 7). Dominik, Gail, & Sedlmayr (1989) found that while most of the grains are nucleated at 1–2 $`R_{}`$ from the star and keep growing until they are as large as 0.01–0.1 $`\mu `$m, the population of small grains of carbon content $`N_C`$ = 100 should not be nucleated at 7 $`R_{}`$ or closer to the central star. The temperature there falls down well below 600 K (Gail & Sedlmayr, 1987). It is cool enough to allow the aliphatic C-H bonds to be preserved.

In the old record scenario, we do not have to assume the grains are ultra-small. Most of the grains are formed in a thin shell near the sonic point 1–2 $`R_{}`$ from the star. The nucleation and growth rates are very high there. However, grain formation is not an instantaneous event. Although the growth rate drops by orders of magnitude, a grain keeps growing even at tens of stellar radii from the star until the source gas is completely depleted or diluted (Dominik, Gail, & Sedlmayr, 1989). This means that the outermost layer of a grain particle is formed in the cool region where thermal processing no longer occurs. Thus, while the inner core formed in the warmer region is already graphitized, the fresh surface of a grain is most likely covered by the aliphatic C-H bonds (Figure 7). The growth of an “amorphous carbon mantle” in the cool ($`<`$1100 K) mass-loss wind has been discussed by Gail & Sedlmayr (1984).

#### 4.4.3 Mass-Loss History

We have heat sources, and the raw material is ready for the thermal treatment. Our observation shows less processed material inside, and more processed outside. We discuss how the observed spatial variation of hydrocarbon features could possibly be produced.

We start with a gradual annealing of a small grain when it travels outward in the circumstellar shell. The incidence of the Ly$`\alpha `$ photon per grain from a G5Ia central star at the distance of 1000 AU can be predicted using the stellar spectral model of Kurucz (1979). Assuming all photons of $`\lambda `$ $``$ 1215Å are converted to Ly$`\alpha `$ and the total luminosity of the central star to be 1.3$`\times 10^4L_{}`$ (Ueta et al., 2001), the photon rate to a 6 Å particle turns out to be about once in thousands of years. However, it critically depends on the wavelength range we consider. For instance, if we count the photons $`\lambda `$ $``$ 1500 Å, the incidence rate jumps up to once in every 5 yr. It drops by an order or two when visible extinction of AV = 1 is applied. At each incidence, a grain cools down in approximately 10-1 s while emitting as a blackbody. As a grain is blown off by roughly 1 AU per year if a 10 km s-1 mass-loss velocity is assumed; the region of our interest, 600–1300 AU from the star, corresponds to $``$700 yr for a grain to cross. The Ly$`\alpha `$ photon rate ($`\lambda `$ 1215Å) without extinction does not conflict with the grain traveling time. The higher fraction of the dust particles have experienced more energetic photon incidence in the outer region than in the inner region because they have been soaked in the radiation field longer. Hence, we would see more thermally annealed grains closer to the edge of the nebula. However, we have to be cautious about the coincidence of the timescale. First, we implicitly assumed the effective temperature of the central star does not significantly change during the relevant period of the time, which is not a trivial issue. Second, the reorganization of the carbon frameworks may not finish in an instant, but may take a finite period of time until the aliphatic to aromatic transformation is settled down. When the alteration timescale is longer than the cooling time, a single Ly$`\alpha `$ photon is insufficient to transform the chemical composition of the entire grain. Further discussion on the gradual annealing scenario would be premature until the microscopic processes of thermal annealing, as well as the effect of the evolution of the central star, is fully understood.

A size variation with distance from the star may provide a solution that accounts for the spatial variation in the chemical composition. Suppose that there is a dominant population of small grains farther away from the star; they are more processed than inner ones because a smaller grain reaches higher temperatures when heated with same energy input. Such a size variation with the distance from the star have been often observed in other PPN (e.g., Sahai et al. 1998). As the higher mass loss rate results in the larger grain size (Krüger & Sedlmayr, 1997), the accelerating mass loss at the end of AGB might be relevant to the production of the hypothetical grain size distribution.

On the other hand, in the old record scenario the assumed grain size is large enough to keep grains from thermal fluctuation. Thus, once the grain growth ceases near the star ($`<`$ 20 $`R_{}`$), the chemical composition of the grain surface remains unchanged during the traverse in the mass-loss wind. Then the variation of the spectral feature we observed at 1000 AU from the star simply reflects how the grain surface was composed near the star. If the timescale of grain growth is slow, it may keep growing in the cool region in the outer circumstellar shell, gradually building more aliphatic-rich mantles on the surface. By contrast, if the source gas quickly depletes closer to the star, a grain stops growing earlier in the warm region, and the surface composition remains mainly graphitic. The observed spatial variation implies a history of the gradual switching of these dust formation modes. However, dust formation models available at present are based on the stationary mass-loss wind, which is ineffective for predicting the temporal variation of chemical composition in dust production. The mass-loss rate is very sensitive to the stellar parameter at the end of the AGB phase (e.g., Willson 2000). In particular, in the superwind phase the mass loss shows complicated temporal variation strongly dependent on the initial mass of stars (Wachter et al., 2002; Schröder, Winters, & Sedlmayr, 1999). To fully understand how time-variable mass loss affects the chemical properties of dust, how those dust grains build up a heterogeneous spatial structure around the central star, and how eventually the spectrum of the chemical composition of dust becomes the carbon-rich late-type stars return to the ISM, further theoretical and observational studies are needed.

## 5 Summary

We presented spatially resolved 3 $`\mu `$m spectroscopy of the proto-planetary nebula IRAS 22272+5435 that reveals the different distribution of the hydrocarbon gas and dust. The main conclusions are follows:

1. The acetylene (C2H2) and hydrogen cyanide (HCN) absorption is found in the central star spectrum at 3.0 $`\mu `$m. The molecules are highly concentrated in the compact region at the center.

2. The 3.3 and 3.4 $`\mu `$m hydrocarbon dust emission is detected at 600–1300 AU from the star. The spatial separation of C2H2 and hydrocarbon dust is observed for the first time, and it reinforces the classical view of the dust formation.

3. We found the relative intensity of the aliphatic feature at 3.4 $`\mu `$m to the aromatic feature at 3.3 $`\mu `$m decreases with the distance from the star. The spatial variation of the spectral feature is well reproduced in the spectra of a laboratory analog of carbon dust. The thermal process is likely to account for the spectral variation.

4. We suggested the stochastic heating of very small grains ($`a<`$ 6 Å) or the grain surface composition at the end of grain growth would explain the changing aliphatic and aromatic spectral features. In both cases the time-dependent mass-loss profile should be the key to reproducing the spatial variation.

We thank all the staff and crew of the Subaru Telescope and NAOJ for their valuable assistance in obtaining these data and continuous support for IRCS and Subaru AO construction. Takashi Kozasa and Masao Saito are appreciated for their useful suggestions in the discussion. We are grateful to V. Mennella and collaborators for making their data available for use in Figure 6. We are also grateful to J. E. Chiar and collaborators for kindly allowing us to reproduce their data in Figures 4 and 6. Special thanks goes to A. T. Tokunaga for many inspiring discussions and enduring encouragement during the writing. We thank the anonymous referee for the helpful comments that make the manuscript more consistent and readable. M. Goto is supported by a Japan Society for the Promotion of Science fellowship. Last, but not least, we wish to express our appreciation to those of Hawaiian ancestry on whose sacred mountain we are privileged to be guests.


text:
# Quantum critical point in CuGeO3 doped with magnetic impurities

## Abstract

Using high frequency (up to 450 GHz) ESR and low temperature specific heat measurements we find that insertion of 1% Fe and 2% Co damps spin-Peierls and Neel transitions and for $`T`$$`<`$30K may give rise to onset of a quantum critical behaviour characteristic for a Griffiths phase.

, , , , , , , , ,

thanks: Corresponding author. E-mail: demis@lt.gpi.ru

Most of the available data for doped inorganic spin-Peierls compound CuGeO3 correspond to the limit of weak disorder when density of states have a pseudogap . In the oppposite case of a strong disorder the situation is expected to change dramatically: the ground state of CuGeO3 should be a Griffiths phase (GP) which thermodynamic properties are controlled by relatively rare spin clusters correlated more strongly than average . In this case density of states becomes gapless and diverges at $`ϵ`$$`=`$0: $`\rho (ϵ)`$$``$$`\left|ϵ\right|^\alpha `$ . As a consequence the temperature dependences of magnetic susceptibility $`\chi `$ and magnetic contribution to specific heat $`c_m`$ for Cu2+ spin-Peierls chains acquire the forms

$$\chi T^\alpha ;c_mT^{1\alpha }$$
(1)
where $`\alpha `$$`<`$1. As long as $`T`$$`=`$0 becomes singular or critical point, the aforementioned situation may be described in terms of quantum critical (QC) behaviour .

The experimental information about feasibility of the QC point in CuGeO3 is very limited . The aim of the present work consists in providing possible evidence of onset of the QC point in CuGeO3 doped with magnetic impurities Co and Fe.

Single crystals of CuGeO3 doped with 1% of Fe (S=1) and 2% of Co (S=3/2) impurities have been grown using self-flux method. The quality of crystals was controlled by X-ray and Raman scattering data . Magnetic properties of the samples in the temperature range 1.7-300K have been studied by high (up to 450 GHz) frequency ESR technique  for $`𝐁`$$``$$`𝐚`$ geometry. Specific heat for the temperature interval 6-20K was studied with the help of low temperature small sample relaxation calorimeter.

Doping of CuGeO3 with magnetic impurities causes (i) rapid damping of the spin-Peierls transition and (ii) onset of a strong paramagnetic background . Therefore the deriving of the effects of doping on Cu2+ S=1/2 chains in convenient magnetisation measurements requires ad hoc assumptions about background behaviour . This difficulty overcomes in ESR experiment, where magnetic impurity in CuGeO3 matrix and Cu2+ chains modified by impurity gives rise to a different absorption lines .

Typical magnetoabsorption spectra for CuGeO3:Co and CuGeO3:Fe at helium temperatures are shown in Fig.1. For the Co-doped sample spectrum is formed by two broad lines which becomes resolved for frequencies $`\nu `$$`>`$100 GHz. The spectrum of Fe-doped sample is characterised by a single resonance. The resonant fields $`B_{res}`$ for all modes presented in Fig.1 are found to vary linearly with frequency $`B_{res}`$$``$$`\nu `$. This result suggests that the observed magnetoabsorption features correspond to different ESR modes rather than coexistence of the ESR and antiferromagnetic resonance .

The analysis of the g-factor values together with the frequency and temperature dependences of the linewidth  have allowed to attribute the high field resonances with g$``$2.15 to ESR on disordered Cu2+ chains and the low field resonance with g$``$4.7 for CuGeO3:Co to ESR on Co2+ impurity in CuGeO3 matrix (Fig.1). A strong g-factor renormalisation for the Co-doped sample may reflect formation of the impurity spin clusters .

As long as the integrated intensity of the ESR line in the region of linear response is proportional to magnetic susceptibility it was possible to subtract contributions of Cu2+ chains and Co2+ impurities unambiguously and find $`\chi (T)`$ dependence for both contributions from the spectra taken at different temperatures (Fig.2). The correctness of the $`\chi (T)`$ evaluation from ESR spectra has been checked by measurements of the static susceptibility for Co-doped sample by vibrating sample magnetometer. We found that sum of $`\chi (T)`$ for Cu2+ and Co2+ resonances represents the integral static susceptibility of the sample within the error of less than 5%.

Quantitative analysis of $`\chi (T)`$ data for doped Cu2+ chains indicates that Eq.(1) holds for $`T`$$`<`$30K (curves 1 and 2 in Fig.2) and the power law provides reasonable description of experimental data. The best fit was obtained using index values $`\alpha =`$0.36$`\pm `$0.03 and $`\alpha =`$0.69$`\pm `$0.04 for Fe-doped and Co-doped crystals respectively. In contrast to the magnetic properties of Cu2+ chains, the susceptibility for Co2+ impurity is better fitted by Curie-Weiss law, $`\chi `$$``$1/(T-$`\mathrm{\Theta }`$), with characteristic temperature $`\mathrm{\Theta }=`$-2.8K (Fig.2, curve 3) corresponding to antiferromagnetically interacting Co2+ impurities. For doped Cu2+ chains it is visible that for magnetic impurities studied spin-Peierls and Neel transitions are already damped.

The observation of the power asymptotics of $`\chi (T)`$ in the absence of any type of long range magnetic order for the wide range 1.7$`<`$$`T`$$`<`$30K (where temperature varies more than 15 times) agrees with the theoretical predictions  for the QC point. An additional argument in favour of proposed interpretation follow from specific heat data for CuGeO3:Fe. It was found  that magnetic contribution $`c_m`$ follows power law with the index $`\alpha =`$0.37$`\pm `$0.03 which coincide within experimental error with the value obtained from magnetic susceptibility.

In conclusion, we provide possible experimental evidence that doping of CuGeO3 with magnetic impurities Co and Fe induces a strong disorder limit and low temperature $`T<`$30K ground state may become a GP. A magnetic structure of the clusters in GP, including the possibility of the predicted in  random dimer phase, is a subject of future investigations.

Authors acknowledge support from the INTAS project 00-807, programmes ”Physics of Nanostuctures” and ”Integration” of RAS and Venture Business Laboratory of Kobe University.


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# Long-lived memory for mesoscopic quantum bits

## Abstract

We describe a technique to create long-lived quantum memory for quantum bits in mesoscopic systems. Specifically we show that electronic spin coherence can be reversibly mapped onto the collective state of the surrounding nuclei. The coherent transfer can be efficient and fast and it can be used, when combined with standard resonance techniques, to reversibly store coherent superpositions on the time scale of seconds. This method can also allow for “engineering” entangled states of nuclear ensembles and efficiently manipulating the stored states. We investigate the feasibility of this method through a detailed analysis of the coherence properties of the system.

A broad effort is now underway to develop new techniques for coherently controlling quantum degrees of freedom in mesoscopic systems Awschalom et al. (2002). These efforts are stimulated in part by the proposals to use these systems as quantum bits in the context of quantum information science. The fast decoherence associated with solid-state environments proves to be the main obstacle for experimental realization of such control.

Spin degrees of freedom of electrons confined in semiconductor quantum dots are attractive qubit candidates Loss and DiVincenzo (1998); Burkard et al. (2000). Relatively long decoherence times are expected for such systems and techniques for the coherent manipulation and measurement of electron spins are now being developed. For the latter, coupling of spin and charge degrees of freedom is probably necessary. Experimental measurements of the spin relaxation times indicate sub-MHz rates Fujisawa et al. (2001), although it is not yet clear what will determine the ultimate coherence lifetimes.

This Letter describes a technique for greatly extending the lifetimes of electron-spin qubits in confined structures by coherently mapping an arbitrary spin superposition state into the spins of proximal, polarized nuclei. This is achieved by effective control of the spin-exchange part of hyperfine contact interaction. After the transfer is completed, the resulting superpositions could be stored for a very long time – up to seconds – and mapped back into the electron spin degrees of freedom on demand. We further show that the stored states can be manipulated using an extension of standard resonance techniques.

Although it is widely known that nuclear spins can possess exceptionally long coherence times due to their weak environmental coupling, single nuclear spins are very difficult to manipulate and measure in practice Kane (1998). In the present approach these problems are circumvented by using collective nuclear degrees of freedom, which do not require individual addressing and control. We demonstrate that such collective states are extremely robust with respect to realistic imperfections, such as partial initial polarization and spin diffusion, and decoherence As a result the present technique allows combines the strengths of electron spin (or charge) manipulation with the excellent long-term memory provided by nuclei.

When uncontrolled, the coupling of electronic spin degrees of freedom to nuclei may be considered an environmental decoherence process. Interesting features of this process arise from its non-Markovian nature Khaetskii et al. (2002a); Merkulov et al. (2002); Khaetskii et al. (2002b). The present paper shows that properly controlled coupling of electrons to nuclei can be used to greatly extend the effective coherence time of electron spins. This study parallels recent work involving the use of atomic ensembles as quantum information carriers Duan et al. (2001).

To illustrate the technique, consider a single electron localized in quantum dot. The effective Hamiltonian for the electron and $`N`$ spin-$`I_0`$ nuclei in a magnetic field $`B_0`$ along the $`z`$-axis is

$$\widehat{H}=g^{}\mu _BB_0\widehat{S}_z+g_n\mu _nB_0\underset{j}{}\widehat{I}_z^j+\widehat{V}_{HF};$$
(1)
The first two terms of Eq. 1 correspond to the Zeeman energy of the electronic and nuclear spins; the third term is the hyperfine contact interaction between the $`s`$-state conduction electrons and the nuclei in the dot, $`\widehat{V}_{HF}=_ja_j\widehat{\stackrel{}{I^j}}\widehat{\stackrel{}{S}}`$. The coefficients $`a_j=Av_0|\psi (\stackrel{}{r}_j)|^2`$ correspond to the one-electron hyperfine interaction with the nuclear spin at site $`\stackrel{}{r}_j`$, where $`A`$ is the hyperfine contact interaction constant, $`v_0`$ is the volume of a unit cell, and $`\psi (\stackrel{}{r})`$ is the envelope function of the localized electron. The hyperfine term can be written $`\widehat{V}_{HF}=\widehat{V}_D+\widehat{V}_\mathrm{\Omega }`$ where $`\widehat{V}_D=_ja_j\widehat{I}_z^j\widehat{S}_z`$ and $`\widehat{V}_\mathrm{\Omega }=_ja_j/2(\widehat{I}_{}^j\widehat{S}_++\widehat{I}_+^j\widehat{S}_{})`$. $`\widehat{V}_D`$ produces an effective magnetic field for the electron $`\widehat{B}_{\mathrm{eff}}=B_01/g^{}\mu _B_ja_j\widehat{I}_z^j`$, which results in the well-known Overhauser shift. However, when $`g^{}\mu _B\widehat{B}_{\mathrm{eff}}\widehat{V}_\mathrm{\Omega }`$, spin exchange becomes the dominate effect.

We start with a perfectly polarized nuclear ensemble $`|\mathrm{𝟎}_n=|I_0,\mathrm{},I_0_n`$, as shown in Fig. 1(a). Due to a total angular momentum conservation only a spin-down initial electron state can undergo non-trivial evolution. When the dynamics are governed by $`\widehat{V}_\mathrm{\Omega }`$ ($`\widehat{B}_{\mathrm{eff}}0`$), there is a coherent exchange of excitations between electronic and nuclear degrees of freedom. For the inital state $`|_e|\mathrm{𝟎}_n`$, spin-exchange couples this state to the collective nuclear excitation with one flipped spin $`|_e|\mathrm{𝟏}_n`$ with

$`|\mathrm{𝟏}_n({\displaystyle \underset{j}{}}|a_j|^2)^{1/2}{\displaystyle \underset{j}{}}a_j|I_0,\mathrm{},(I_01)_j,\mathrm{},I_0_n.`$
Hence the evolution is given by the two-level dynamics

$`\left[\begin{array}{c}||\mathrm{𝟎}\\ ||\mathrm{𝟏}\end{array}\right](t)=\left[\begin{array}{cc}\mathrm{cos}(\mathrm{\Omega }t/2)& i\mathrm{sin}(\mathrm{\Omega }t/2)\\ i\mathrm{sin}(\mathrm{\Omega }t/2)& \mathrm{cos}(\mathrm{\Omega }t/2)\end{array}\right]\left[\begin{array}{c}||\mathrm{𝟎}\\ ||\mathrm{𝟏}\end{array}\right](0),`$
The ensemble displays Rabi-oscillations with an effective Rabi rate:

$`\mathrm{\Omega }=\sqrt{2I_0{\displaystyle \underset{j}{}}|a_j|^2}.`$
At the same time, the spin-up electronic state $`|_e|\mathrm{𝟎}_n`$ is an eigenstate of both $`\widehat{V}_D`$ and $`V_\mathrm{\Omega }`$. Hence, by pulsing the applied field to go from $`g^{}\mu _B\widehat{B}_{\mathrm{eff}}\widehat{V}_\mathrm{\Omega }`$ to $`\widehat{B}_{\mathrm{eff}}0`$ for a time $`t=\pi /\mathrm{\Omega }`$ as diagramed in Fig. 1(b), an arbitrary superposition of electronic state will undergo the following evolution:

$$(\alpha |_e+\beta |_e)|\mathrm{𝟎}_n|_e(\alpha |\mathrm{𝟎}_n+i\beta |\mathrm{𝟏}_n),$$

demonstrating that an electronic spin state can be coherently mapped into nuclei.

The Rabi-flopping process can be controlled by removing the electron from the dot or by changing the effective magnetic field, $`B_0`$. Away from the resonance condition $`(|B_{\mathrm{eff}}|\mathrm{\Omega }/g^{}\mu _B)`$, the system is far detuned and no evolution will occur. For the perfectly polarized state the effective detuning is $`\delta =(g^{}\mu _Bg_n\mu _n)B_0+I_0A+(I_01)A/N`$. The Rabi frequency depends upon the distribution of the $`a_j`$ coefficients, $`\mathrm{\Omega }=\sqrt{2I_0}A/\sqrt{N}(1+\overline{(\mathrm{\Delta }a^2)}/\overline{a}^2)^{1/2}`$ with bars denoting averages over the set $`\{a_j\}`$. For a GaAs dot with $`10^4`$ nuclei and $`\overline{\mathrm{\Delta }a^2}\overline{a}^2`$, $`A90\mu `$eV and $`I_0=3/2`$, and the speed of transfer is determined by $`\mathrm{\Omega }/2\pi 0.6`$ GHz, which exceeds the expected spin coherence time by three orders of magnitude. The resonance condition is fulfilled for $`|B_{\mathrm{eff}}|50`$mT. Retrieval of the stored qubit can be implemented by reversing this process: we either inject a spin-polarized electron into the dot or change the effective magnetic field, bringing the levels into resonance, and Rabi oscillations pick up at the same point as before.

Before proceeding with a detailed description of the coherence properties and imperfections we note that the above results can be easily generalized to the preparation of complex collective nuclear states. For example, injection of a series of spin-down electrons into spin-up polarized nuclei will lead to a progressive increase of the nuclear spin. In the basis of collective angular momentum, $`\widehat{\stackrel{}{I}}=_i\widehat{\stackrel{}{I^i}}`$, we define the total angular momentum nuclear states $`|𝐦_n=|I=NI_0,I_z=Im_n`$. Each electron can effect the transfer $`|_e|𝐦_n|_e|𝐦+\mathrm{𝟏}_n`$. When injected electrons are prepared in different superposition states this process can be used to effectively “engineer” collective states of nuclear ensembles. In fact using a proper sequence of electrons an arbitrary state of the type $`|𝚿_n=_{m=0}^Ic_m|𝐦_n`$ can be prepared Footnote1 et al. (2002). We note in particular that the highly entangled states of the kind $`(|\mathrm{𝟎}_n+|𝐦_n)/\sqrt{2}`$, with large $`𝐦`$ could be used for high-resolution NMR spectroscopy in analogy with related atomic physics studies Bollinger et al. (1996); Huelga et al. (1997). Such states can also be prepared by manipulating one electron in the dot with fast electron-spin resonance (ESR) pulses.

Injection of polarized electrons, combined with ESR pulses, can also be used to perform manipulation of the stored nuclear state. For example, the qubit stored in nuclear spin could be mapped into the injected electron and an ESR pulse can be used to rotate it. Subsequently, it can be mapped back to nuclei. Alternatively virtual, off-resonant ($`|\delta |\mathrm{\Omega }`$) coupling of storage states to electron spin can be used to shift the resonance frequencies of transitions $`|𝐦_n|𝐦+\mathrm{𝟏}_n`$ relative to each other. For example in the case of two lowest states $`m=1,2`$ the differential shift is on the order of $`\mathrm{\Omega }^4/|\delta |^3`$. Whenever this shift is large compared to decoherence rate and the spectral width of excitation pulse, the lowest two states of collective manifold $`|\mathrm{𝟎}_n,|\mathrm{𝟏}_n`$ can be considered as an effective two level system and can be manipulated through NMR pulses and other means. These ideas could be extended to the spin-exchange coupled qubits proposal Loss and DiVincenzo (1998).

We now turn to the consideration of various decoherence mechanisms and imperfections that limit the performance of the storage technique. To evaluate the effects of spatial inhomogeneity we note that the collective state $`|_e|1_n`$ is not an eigenstate of $`\widehat{V}_D`$ unless the $`a_j`$’s are identical. The effect is determined by the distribution of eigenenergies under $`\widehat{V}_D`$ of the states $`|_e|I_0,\mathrm{},I_01_j,\mathrm{},I_0_n`$, given by

$`E_j=(g^{}\mu _B/2g_N\mu _NI_0)B_0+I_0A/2a_j/2`$
Since $`\overline{\mathrm{\Delta }E^2}\overline{\mathrm{\Delta }a^2}`$, the inhomogeneous linewidth is $`\overline{a}=A/N`$. Hence inhomogeneous broadening is smaller than the relevant time scale for Rabi-flopping by a factor of $`\sqrt{N}`$, and is negligible during transfer operation. After the mapping, its effect can be mitigated by either removing the electron from the dot, thereby turning off the hyperfine interaction entirely, or by using ESR spin-echo techniques to reverse the phase evolution Carr and Purcell (1954).

The leading decoherence process for the stored state is nuclear-spin diffusion, with dephasing rates in the kHz domain. However, techniques from NMR can be used to mitigate this effect Mehring (1976); Paget et al. (1977). By applying fast NMR pulse sequences Waugh et al. (1968) to rotate the nuclear spins the time average of the leading terms in the dipole-dipole Hamiltonian can be reduced to zero, leaving only residual dephasing due to second-order dipolar effects, pulse imperfections and terms due to the finite length of the averaging sequence. These phenomena have been studed for several decades for solid-state NMR systems and well-developed techniques routinely reduce $`T_2`$ by several orders of magnitude Mehring (1976), down to sub-Hz levels. Hence, coherent qubit storage on the time scale of seconds seems feasible.

To evaluate the effects of partial polarization on the storage fidelity, we use the Heisenberg picture. In the homogeneous case $`(a_i=a=A/N)`$, the Dicke-like collective operators defined above yield $`\widehat{I}^2`$ and $`\widehat{J}_z=\widehat{S}_z+\widehat{I}_z`$ as the constants of motion. We consider operator equations of motion $`\dot{\widehat{A}}=i[\widehat{A},\widehat{H}]`$, for the three operators $`\widehat{S}_z,\widehat{S}_+\widehat{I}_{}`$, and $`\widehat{S}_{}\widehat{I}_+`$, which commute with the constants of motion. We replace $`\widehat{I}_z`$ terms in the resulting equations with $`\widehat{J}_z\widehat{S}_z`$ and use the identity $`\widehat{I}_+\widehat{I}_{}=\widehat{I}^2\widehat{J}_z^2[\widehat{I}_{},\widehat{I}_+]/2`$ to put the equations in terms of constants of motion and the three operators we look to solve:

$`{\displaystyle \frac{d}{dt}}\widehat{S}_z`$ $`=`$ $`a{\displaystyle \frac{\widehat{S}_+\widehat{I}_{}(\widehat{S}_+\widehat{I}_{})^{}}{2i}}`$ (2)
$`{\displaystyle \frac{d}{dt}}(\widehat{S}_+\widehat{I}_{})`$ $`=`$ $`i[(g^{}\mu _Bg_n\mu _n)B_0+a(\widehat{J}_z1)](\widehat{S}_+\widehat{I}_{})`$ (3)
$``$ $`ia(\widehat{I^2}\widehat{J}_z^2+1/4)\widehat{S}_z.`$
It is convenient to choose new constants of motion, $`\widehat{\delta }=((g^{}\mu _Bg_n\mu _n)B_0+a(\widehat{J}_z1))`$ and $`\widehat{\mathrm{\Omega }}=a(\widehat{I^2}\widehat{J}_z^2+1/4)^{1/2}`$. These commute with each other and with $`\widehat{S}_z,\widehat{S}_+\widehat{I}_{}`$. As these equations are similar to those for two-level atoms in a field, we make the Bloch vector identifications:

$`\widehat{U}`$ $`=`$ $`a/\widehat{\mathrm{\Omega }}{\displaystyle \frac{\widehat{S}_+\widehat{I}_{}+(\widehat{S}_+\widehat{I}_{})^{}}{2}},`$
$`\widehat{V}`$ $`=`$ $`a/\widehat{\mathrm{\Omega }}{\displaystyle \frac{\widehat{S}_+\widehat{I}_{}(\widehat{S}_+\widehat{I}_{})^{}}{2i}},`$
$`\widehat{W}`$ $`=`$ $`\widehat{S}_z.`$ (4)
and Eqns. 3–4 become $`\dot{\widehat{\stackrel{}{M}}}=\widehat{\stackrel{}{M}}\times \widehat{\stackrel{}{\omega }}`$ with $`\widehat{\stackrel{}{\omega }}=(\widehat{\mathrm{\Omega }},0,\widehat{\delta })`$. The Bloch vector operator, $`\widehat{\stackrel{}{M}}`$, will rotate about the axis defined by $`\widehat{\stackrel{}{\omega }}`$ at a frequency $`\widehat{\omega }_0=\sqrt{\widehat{\delta }^2+\widehat{\mathrm{\Omega }}^2}`$. For no initial electron spin-nuclear spin correlation, we can easily solve for $`\widehat{S}_z`$ and find

$$\widehat{S}_z(t)=\frac{\widehat{\delta }^2+\widehat{\mathrm{\Omega }}^2\mathrm{cos}(\widehat{\omega }_0t)}{\widehat{\omega }_0^2}S_z(0).$$
(5)
For the perfectly polarized nuclear state, Eq. 5 gives $`\widehat{S}_z=1/2\mathrm{cos}(A\sqrt{2I_0/N}t)`$ for the spin-down species and $`1/2`$ for the spin-up species, exactly replicating the fully polarized behavior. In the case of partial polarization, even though we will set $`\widehat{\delta }=0`$, $`\widehat{\delta }^2`$ remains finite. The first part of Eq. 5 prevents complete transfer, to order $`\widehat{\delta }^2/\widehat{\omega }_0^2`$. For partial polarization $`P<1`$, $`\widehat{\omega }_0^2a^2N(2I_0+O(1P))`$. In a thermal state, all 2-particle expectation values factor, so $`\widehat{\delta }=0`$ and

$`\widehat{\delta }^2=a^2(\widehat{J}_z^2\widehat{J}_z^2)Na^2(1P)2I_0.`$ (6)
Accordingly, the error scales as

$`{\displaystyle \frac{\widehat{\delta }^2}{\widehat{\omega }_0^2}}1P.`$ (7)
Remarkably, this result demonstrates that efficient transfer is possible even with many nuclei in the “wrong” state as long as the average polarization per nuclei is high.

We modeled this system numerically with an initial thermal nuclear state. Oscillation of $`\widehat{S}_z`$ for several polarizations is shown in Fig. 2(a). The effect of partial polarization is immediately apparent; the transfer peak is less than 1/2, and the Rabi frequency decreases. The difference between the initial electron state and the state after once cycle of storage and retreival corresponds to the storage fidelity $`F`$. Fig. 2(b) shows that the analytical estimate is close to the numerically calculated values; thus, the transfer error can, to a large extent, be explained by the thermal uncertainty in $`\widehat{\delta }`$. The residual effect most likely stems from phase mismatching, as measured by the broadening of $`\omega _0`$, such that at $`t=(\pi \omega _0)^1,\mathrm{cos}(\omega _0t)=1O(1P)`$.

Inhomogeneous broadening for a thermal initial nuclear state is somewhat more pronounced than the fully polarized case first considered. The $`\widehat{V}_D`$ inhomogeneity causes slow dephasing of the stored state, and the inhomogeneous coupling in $`\widehat{V}_\mathrm{\Omega }`$ results in leakage in readout of the stored state into a set of states orthogonal to the original nuclear state. The results shown in Fig. 2(b) were calculated for a distribution of $`a_i`$’s corresponding to a gaussian $`|\psi (\stackrel{}{r})|^2`$. We plot the estimated fidelity for a complete storage and readout cycle as a function of the initial polarization of nuclear spins. The total expected fidelity, is approximated by the product of these two results (Fig. 2(b)). Hence, only modest nuclear polarizations are required to obtain a high fidelity of storage.

In summary, we have demonstrated that is possible to reliably map the quantum state of a spin qubit onto long-lived collective nuclear spin states. The resulting states have long coherence times, and can be retrieved on demand. Furthermore, the stored states can be efficiently manipulated and similar techniques can be used for quantum state engineering of collective nuclear states.

Experimental implementation of these ideas requires preparation of nuclear spin polarizations in the vicinity of confined electrons. Optical pumping of nuclear spins has demonstrated polarizations in GaAs 2D electron gases on the order of 90% Salis et al. (2001a) and 65% in self-assembled dots Gammon et al. (2001), and forced spin-flips through quantum hall edge states Dixon et al. (1997) has a claim of a similarly high polarization ability (85%). We anticipate that combining either of these techniques with electron localization in quantum dots would be a promising avenue of study. The methods outlined in this paper can be used to further increase the nuclear polarization. A current of spin-polarized electrons passing through the quantum dot with a dwell time $`\tau _{\mathrm{dwell}}<\pi /\mathrm{\Omega }_0`$ will result in spin transfer, thereby increasing nuclear polarization. By keeping $`B_{\mathrm{eff}}`$ tuned to zero with increasing nuclear polarization the spin flip-flop remains resonant and, when combined with dephasing to prevent saturation, leads to efficient cooling, similar to a recent proposal Eto (2002).

Coherence properties of the spin-exchange process could be probed in transport measurements. For example, sending spin polarized currents through the quantum dot in which the spin-exchange interaction is tuned to resonance will result in collapses and revivals of the electron spin polarization that will be a periodic function of the dwell time in the dot. Those can be measured using spin-filter techniques. For a given polarization $`P`$ and $`\tau _{\mathrm{dwell}}`$, the spin will be rotated by $`\mathrm{\Omega }(P)\tau _{\mathrm{dwell}}/\pi `$. Note that repolarization will be necessary after $`\sqrt{N}`$ nuclear spins have been flipped.

Practical applications of the storage and retrieval techniques and manipulation of stored states requires time-varying control over the spin-exchange coupling. This can be accomplished by using a pulsed magnetic field of order 50mT for a few ns, by engineering the electron $`g`$-factors Salis et al. (2001b); Matveev et al. (2000), or by optical AC Stark shifts Salis et al. (2001a) These techniques can be combined with a number of avenues for entanglement and manipulation of the electronic spin and charge states currently under exploration Awschalom et al. (2002); Loss and DiVincenzo (1998). Finally, quantum memory can facilitate implementation and reduce scaling problems for more ambitious tasks such as quantum error correction Steane (1999) or quantum repeaters Duan et al. (2001).

We thank J.A. Folk, Y. Yamamoto, and D. Loss for helpful discussions. This work was supported by ARO, NSF, and by David and Lucille Packard Foundation.


text:
# 1 Introduction

## 1 Introduction

The study of the reactions $`\gamma d\pi ^0d`$ and $`\pi ^{}d\pi ^{}d`$ near threshold has attracted continuous attention in the past few decades. Moreover the new experimental data appeared due to recent success of the accelerator technologies stimulate increasing theoretical interest in this field. In this paper we would like to concentrate on the rescattering effects (RE) and their role for these reactions. Indeed, these effects are found to be important in many of theoretical investigations of the reaction $`\gamma d\pi ^0d`$ (cf., e.g. Refs. ). However, recently in Ref.  the discussion about the role of these effects was renewed. In particular it was emphasized in  that the contribution from the two-step process $`\gamma d\pi ^{}pp\pi ^0d`$ (cf. Fig. 1a) is totally compensated by the loop corrections to the impulse approximation (LCIA) (cf. Fig. 1b). This was argued by the Pauli principle for the intermediate NN states. Thus, the rescattering effects in Ref.  do not contribute to the process of coherent $`\pi ^0`$ photoproduction on deuteron near threshold. Obviously, this conclusion of Ref.  disagrees with the results of other calculations performed, e.g., in Refs. .

Let us discuss the arguments of Ref.  in more detail:

* The final $`\pi ^0d`$ state has quantum numbers $`J^P=1^{}`$ at low energies where pion is in the $`S`$ wave with respect to the deuteron. However, the only possible state of the system $`pp\pi ^{}`$ with $`l_1=l_2=0`$ is $`0^{}`$ (here $`l_1`$ is the orbital angular momentum of the $`pp`$ system and $`l_2`$ is the orbital momentum of the pion relative to the $`pp`$ system). Therefore the S-wave intermediate state $`pp\pi ^{}`$ does not contribute to the process $`\gamma d\pi ^0d`$.
* In other words, the contribution of the diagram in Fig. 1a has to be compensated by the loop corrections to the impulse approximation (Fig. 1b) because of antisymmetry of the wave function for the pair of the intermediate nucleons.

Note, that the process $`\gamma d\pi ^0np\pi ^0d`$ is allowed by quantum numbers. However the amplitude $`\gamma n\pi ^0n`$ which contributes to this reaction is about factor of 20 smaller than the corresponding amplitude for the charged pion production.

In this remark we are going to discuss the role of rescattering effects for the process of pion-deuteron elastic scattering at low energies. The diagrams corresponding to RE and LCIA for the $`\pi d`$-scattering are very similar to the ones for the reaction $`\gamma d\pi d`$ (cf. Fig. 1 and Fig 2b and 2c). Therefore we will investigate the relevance of RE and the problem of the cancellation of RE and LCIA performing the calculation of the $`\pi d`$-scattering amplitude.

The $`\pi d`$-scattering length was measured with a high accuracy  and its value coincides with the theoretical predictions (cf., e.g., Refs. ). In all these theoretical calculations rescattering effects (including the two-step charge exchange process $`\pi ^{}p\pi ^0n\pi ^{}p`$) give significant contribution to the value of the pion-deuteron scattering length.

In what follows we will directly demonstrate that the real part of the rescattering diagram (cf. Fig.2c) gives non-negligible contribution to the pion-deuteron scattering length. It is not compensated by the real part of LCIA (cf. Fig.2b). However, the imaginary parts of RE and LCIA cancel each other. This cancellation means that there is no contribution to observables from the $`\pi NN`$ states forbidden by the Pauli principle.

## 2 Calculation of the $`\pi d`$ scattering amplitude

Below we use a simple potential approach for the calculation of the $`\pi N`$-scattering amplitude. This approach was already applied to the problem of the determination of the $`\pi N`$-scattering length in Ref. . The model utilizes a pion-nucleon potential $`V_{\pi N}(𝐩,𝐪)`$ which is required for solving the Lippman-Schwinger equation

$$T=V+VGT.$$
(1)
The S-wave $`\pi N`$-lengths $`b_0`$ and $`b_1`$ are related to the scattering length $`a_{\pi N}`$ by the equation

$$a_{\pi N}=b_0+b_1𝐈𝝉,$$
(2)
where I and $`𝝉`$ are isospin operators for pion and nucleon, $`b_0`$ and $`b_1`$ are isoscalar and isovector scattering lengths. The analyses  of the experimental data  show that the absolute values of $`b_0`$ and $`b_1`$ are small compared to the typical scale of the problem $`\mu ^1`$ (where $`\mu `$ is the pion mass). Note also that $`b_0b_1`$. Thus, the amplitude $`T`$ in eq. (1) may be perturbatively expanded in terms of the potential $`V_{\pi N}(𝐩,𝐪)`$.

Following Ref.  we choose $`V_{\pi N}`$ in the S-wave in the separable form:

$$V_{\pi N}(𝐤,𝐪)=\frac{(\lambda _0+\lambda _1𝐈𝝉)}{2m_{\pi N}}g(k)g(q),$$
(3)
where $`g(k)=(c^2+k^2)^1`$, $`m_{\pi N}=m\mu /(m+\mu )`$ and $`m`$ is the nucleon mass. The cut off parameter $`c`$ characterizes the range of the $`\pi N`$-forces, and usually it is varied in the range $`2.5\mu c5\mu `$ . The parameters $`\lambda _0`$ and $`\lambda _1`$ are chosen in such a way to reproduce the scattering lengths $`b_0`$ and $`b_1`$. In what follows we will calculate the pion-deuteron scattering amplitude up to the second order in terms of the potential $`V_{\pi N}`$. With this accuracy $`\lambda _0`$ and $`\lambda _1`$ are equal to

$`\lambda _0`$ $`=`$ $`{\displaystyle \frac{c^4}{2\pi ^2}}\left(b_0{\displaystyle \frac{c}{2}}(b_0^2+2b_1^2)\right),`$
$`\lambda _1`$ $`=`$ $`{\displaystyle \frac{c^4}{2\pi ^2}}b_1\left(1{\displaystyle \frac{c}{2}}(2b_0b_1)\right).`$ (4)
Corrections to these expressions are of the order of $`O(b_0^3,b_1^3)`$ which are negligible.

Let us calculate the pion-deuteron scattering length using the potential $`V_{\pi N}`$ (cf. eq. (3)).

i) Single scattering amplitude in the Born approximation

The diagram corresponding to this amplitude is shown in Fig. 2a. The expression for the $`\pi d`$ amplitude $`f_{\pi d}^{1(V)}`$ corresponding to the sum of two diagrams with the scattering of pion on proton and neutron has the form:

$$f_{\pi d}^{(1)V}=\frac{\mu }{(2\pi )(1+\mu /m_d)}𝑑𝐩\phi _d^2(𝐩)[V_{\pi ^{}p}+V_{\pi ^{}n}].$$
(5)
Here $`\phi _d(𝐩)`$ is the deuteron wave-function in the momentum space with the normalization condition $`𝑑𝐩\phi _d^2(𝐩)=(2\pi )^3`$. Neglecting by the small corrections of order of $`\mu /m`$, one may take out the potential $`V`$ in Eq. (5) of the integral and then get:

$$f_{\pi d}^{1(V)}=2\left[b_0\frac{c}{2}(b_0^2+2b_1^2)\right].$$
(6)
This contribution is real as it should be in the Born approximation. Note also that the value $`f_{\pi d}^{1(V)}`$ depends on the value of the parameter $`c`$.

ii) Single scattering in the one-loop approximation

The diagram for the one-loop correction to the Born approximation is shown in Fig. 2b. We have to calculate the sum of two diagrams with the scattering of pion on proton and neutron taking into account the sum over all intermediate states. The expression for the amplitude $`f_{\pi d}^{(1)VGV}`$ corresponding to this sum has the form:

$`f_{\pi d}^{(1)VGV}`$ $`=`$ $`{\displaystyle \frac{2\mu }{1+\mu /m_d}}\left[(\lambda _0^2+\lambda _1^2)I(\mathrm{\Delta }m=0)+\lambda _1^2I(\mathrm{\Delta }m)\right],`$
$`I(\mathrm{\Delta }m)=`$ $`{\displaystyle \frac{d𝐩}{2\pi }\frac{g^2\left(\frac{m𝐤\mu 𝐩}{m+\mu }\right)\phi _d^2(𝐩)}{(2m_{\pi N})^2}\frac{d𝐬g^2\left(\frac{m𝐤\mu 𝐩}{m+\mu }+{\displaystyle \frac{m\mu }{m+\mu }}𝐬\right)}{\text{}\left[{\displaystyle \frac{(𝐤+𝐬)^2}{2\mu }}+{\displaystyle \frac{p^2}{2m}}+{\displaystyle \frac{(𝐩𝐬)^2}{2m}}+\epsilon _d\mathrm{\Delta }m{\displaystyle \frac{k^2}{2\mu }}i0\right]}}.`$ (7)
Here $`𝐤`$ is the 3-momentum of the initial and final pion, $`\mathrm{\Delta }m=m_\pi ^{}+m_pm_{\pi ^0}m_n=3.3`$ MeV is the excess energy for the charge exchange process $`\pi ^{}p\pi ^0n`$ in the intermediate state. For the case of the elastic rescattering $`\mathrm{\Delta }m=0`$.

The integral in eq. (7) is calculated numerically for some values of the cut off parameter $`c`$. In the limit of large $`c`$, i.e. when $`c\mu `$ and for $`\mu /m1`$ this integral can be calculated analytically:

$$f_{\pi d}^{(1)VGV}=c(b_0^2+2b_1^2)+2i\left[k_0(\mathrm{\Delta }m=0)(b_0^2+b_1^2)+k_0(\mathrm{\Delta }m)b_1^2\right],$$
(8)
where we introduced the notation $`k_0^2=k^2+2\mu \mathrm{\Delta }m2\mu \epsilon _d`$. Note that $`kc`$ near the threshold.

Thus, in the limit of large $`c`$ the resulting contribution from the impulse approximation (cf. Fig. 2a and 2b) to the real part of the $`\pi d`$-scattering amplitude is

$$\mathrm{Re}f_{\pi d}^1=f_{\pi d}^{1(V)}+\mathrm{Re}f_{\pi d}^{(1)VGV}=2b_0.$$
(9)
This is a naive but expected result for the real part of the amplitude corresponding to the impulse approximation. The values of $`Ref_{\pi d}^{(1)VGV}`$ for the charge exchange process $`\pi ^{}d\pi ^0nn\pi ^{}d`$ are presented in Table 1 for the different values of parameter $`c`$. In contrary to the real part of the loop amplitude the imaginary part of $`f_{\pi d}^{(1)VGV}`$ (cf. eq. (8)) does not depend on $`c`$ as required by the unitarity.

Now let us discuss the contribution to the pion-deuteron scattering length from the double scattering process.

iii) Double scattering contribution

Double scattering diagram is shown in Fig. 2c. Performing the calculation we have the following integral for the doublescattering amplitude $`f_{\pi d}^{(2)}`$ (cf. Ref.  for details):

$`f_{\pi d}^{(2)}`$ $`=`$ $`{\displaystyle \frac{4c^4}{(2\pi )^5}}\left[(b_0^2b_1^2)J(\mathrm{\Delta }m=0)b_1^2J(\mathrm{\Delta }m)\right],`$
$`J(\mathrm{\Delta }m)`$ $`=`$ $`{\displaystyle \frac{d𝐪_1d𝐪_2\phi _d(𝐪_1)\phi _d(𝐪_2)g^2(𝐤+𝐪_1𝐪_2)}{(𝐤+𝐪_1𝐪_2)^2+(\mu /m)(q_1^2+q_2^2)+2\mu (\epsilon _d\mathrm{\Delta }m)k^2i0}}.`$ (10)
In the limit of large $`c`$ and for $`\mu /m1`$ this integral is reduced to the following expression:

$$f_{\pi d}^{(2)}=2(b_0^2b_1^2)\mathrm{\Psi }_d^2(r)\frac{e^{i\mathrm{𝐤𝐫}+ik_0(\mathrm{\Delta }m=0)r}}{r}𝑑𝐫2b_1^2\mathrm{\Psi }_d^2(r)\frac{e^{i\mathrm{𝐤𝐫}+ik_0(\mathrm{\Delta }m)r}}{r}𝑑𝐫,$$
(11)
where $`\mathrm{\Psi }_d(𝐫)`$ is the deuteron wave function in the coordinate space.

In the limit of small $`k`$ and $`k_0`$, i.e. near the threshold for the real part of $`f_{\pi d}^{(2)}`$ we get

$$Ref_{\pi d}^{(2)}=2(b_0^22b_1^2)\frac{1}{r}_d.$$
(12)
This expression is well known as a static limit for the doublescattering amplitude, see, e.g.  and references therein.

The imaginary part of the amplitude $`f_{\pi d}^{(2)}`$ (11) in the same limit is

$$\mathrm{Im}f_{\pi d}^{(2)}=2k_0(\mathrm{\Delta }m=0)(b_0^2b_1^2)2k_0(\mathrm{\Delta }m)b_1^2.$$
(13)
Note that this contribution is negative because $`b_1b_0`$.

iv) Total pion-deuteron amplitude

Let us discuss the value for total pion-deuteron scattering amplitude in the limit of large $`c`$ ($`c\mu `$) and for $`\mu /m1`$. For the imaginary part of the resulting amplitude in this limit from eqs. (8) and (13) we get

$$\mathrm{Im}f_{\pi d}4k_0(\mathrm{\Delta }m=0)b_0^2.$$
(14)
Thus, we obtain that the contributions from LCIA and RE to the imaginary part of the pion-deuteron scattering amplitude cancel each other in the leading order (i.e. terms $`b_1^2`$). The non-vanishing part of Im$`f_{\pi d}`$ is proportional to $`b_0^2`$ what corresponds to the elastic rescattering process $`\pi ^{}d\pi ^{}pn\pi ^{}d`$. Note, that the imaginary parts of both expressions (8) and (13) behave as two-particle phase space, i.e. proportional to $`k_0Q^{1/2}`$, where $`Q`$ is the kinetic energy of the intermediate $`\pi NN`$ system. However, three-particle $`\pi NN`$ phase space should behave as $`Q^2`$. This paradox can be resolved if we remind the reader that the approximation $`\mu /m1`$, which implies that the kinetic energies of the intermediate nucleons in Eqs. (7) and (10) are neglected, was used to obtain Eqs. (8) and (13). This approximation corresponds to the the rescattering of pion on the fixed centers. That is why the imaginary parts in Eqs. (8) and (13) behave as $`Q^{1/2}`$. Of course, one can avoid this unnecessary simplification and calculate Eqs. (7) and (10) with taking into account the terms of order of $`O(\frac{\mu }{m})`$. But it should not change the main result that the contributions from LCIA and RE to the imaginary part of the $`\pi d`$-scattering amplitude with intermediate charge exchange cancel each other. The result (14) means that the only possible final state which can be formed in the S-wave in the process of deuteron desintegration is $`pn\pi ^{}`$ (with $`S=1`$ and $`I=0`$ for pair of nucleons). The virtual charge exchange does not contribute to the imaginary part of the pion-deuteron amplitude. This conclusion is in agreement with the remark of Ref. .

At the same time we would like to stress that there is no complete cancellation between real parts of the amplitudes $`f_{\pi d}^{(1)VGV}`$ and $`f_{\pi d}^{(2)}`$, i.e. the resulting contribution from LCIA and RE to the real part of the pion-deuteron scattering amplitude is not small. This conclusion, which is also correct for the process $`\gamma d\pi ^0d`$, is in contrary to the arguments of Ref. . As can be seen from Eq. (8), the expression for Re$`f_{\pi d}^{(1)VGV}`$ depends linearly on the cut-off parameter $`c`$ for large values of $`c`$ and $`\mu /m1`$, whereas Re$`f_{\pi d}^{(2)}`$ in the same limit is totally determined by the deuteron wave function, i.e. independent of $`c`$ (c.f. Eq. (12)). Therefore the cancellation of the real parts of the amplitudes $`f_{\pi d}^{(1)VGV}`$ and $`f_{\pi d}^{(2)}`$ can not be achieved in this limit (the value $`c=2<|1/r|>_d1.2\mu `$ is obviousely not realistic).

In Ref.  we have calculated the sum of the real parts of the diagrams presented in Fig. 2 varying the parameter $`c`$ in the limits $`2.5\mu c3.5\mu `$. The results of the present numerical calculation are presented in Table 1 for the case when $`c`$ varies in a larger range and the terms $`O(\mu /m)`$ are taken into account. In the calculation we use the purely hadronic values for $`b_0`$ and $`b_1`$ presented in Ref. , i.e. $`b_0=2.2\times 10^3m_\pi ^1;b_1=90.5\times 10^3m_\pi ^1`$. This Table clearly confirmes the conclusion discussed above that the real parts of the diagrams of Fig. 2b and 2c do not cancel each other.

## 3 Summary

We developed a consequent potential approach to the problem of the calculation of the pion-deuteron scattering length. The $`\pi d`$ amplitude was calculated including terms of the second order with respect to the pion-nucleon potential $`V_{\pi N}`$. The proper symmetrization of the wave function for the intermediate nucleons is taken into account automatically in our approach.

We show that there is a significant cancellation of the contributions from the imaginary parts of LCIA (cf. Fig. 2b) and RE (cf. Fig. 2c). This cancellation is expected. It simply reflects the fact that the process $`\pi ^{}d\pi ^0nn`$ is strongly suppressed near threshold as required by the Pauli principle. However, no such cancellations take place between the real parts of these processes. The integrals for the real parts of the amplitudes (7) and (10) are quite different. In particular, they have different dependence on the cut off parameter $`c`$ in the formfactor. Therefore we see no reasons for the cancellation of Re$`f_{\pi ^{}d}^{(1)VGV}`$ and Re$`f_{\pi ^{}d}^{(2)}`$.

The situation for the reaction $`\gamma d\pi ^0d`$ is quite analogous to that discussed for the reaction $`\pi d\pi d`$. There is no any reasons for the cancellation of the real parts of the diagrams shown in Fig. 1a and 1b. This conclusion is in agreement with the results of papers  where rescattering effects are found to be important for the reaction $`\gamma d\pi ^0d`$ .

We would like to thank A. M. Gasparyan and V. G. Ksenzov for useful discussions. This work was partly supported by RFBR grant N0 02-02-16465, DFG-RFBR grant 436 RUS 113/652/0-1.