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# 1 Introduction

## 1 Introduction

The HERA-B experiment is a hadronic B-factory at DESY, where B-mesons are produced via interactions of 920 GeV beam halo protons with an internal target . In order to reach the necessary production rate of $`b`$-quarks, the HERA-B detector must operate at an extremely high interaction rate of $``$ 40 MHz, corresponding to an average of 4 superimposed interactions per HERA proton bunch crossing. Such a high rate of inelastic interactions results in events with large charge and neutral multiplicities - up to several hundred particles every 96 ns - and a harsh radiation environment for the constituent detectors. The peak integrated doses in the HERA-B tracking system are about 1 Mrad/year for the Inner Tracker and 500 $`\frac{mC}{cmwire}`$ per year for the Outer Tracker.

The high irradiation levels in HERA-B led to several painful experiences with aging problems in gaseous detectors. Although irradiation of small area chambers with $`X`$-rays showed that the original Inner and Outer Tracker prototype chambers are able to tolerate very large X-rays doses, corresponding to several years of operation without visible aging effects, in the HERA-B environment both chambers died within hours. In a subsequent extended R$`\&`$D program these problems were solved, either by going to a revised design of the Inner Tracker (e.g. introducing GEM foils in the original diamond coated MSGC)  or by changing the original concept for the drift tubes of the Outer Tracker (surface conductivity, gas mixture, production materials) .

Strong restrictions on the gas choice are imposed by the operating conditions in the muon detector (the maximum accumulated charge on the wire can reach 200 $`\frac{mC}{cmwire}`$ per year). In a previous paper , studies of the aging performance of muon proportional chambers under sustained irradiation with $`Fe^{55}`$ and $`Ru^{106}`$ sources and in a 100 MeV $`\alpha `$-beam were presented. Despite the negligible gas gain loss measured after the long-term irradiation with radioactive source, rapid aging effects during irradiation with the 100 MeV $`\alpha `$-particles were observed in an $`Ar/CF_4/CH_4`$ (74:20:6) mixture. From these results it is evident that from the accumulated charge alone, it is difficult to combine the data from the different radiation sources into one consistent model. The difference between these results could be partially attributed to the type of ionization particles, the size of the irradiation area, gas gain, gas flow rate or some other variations in the operating parameters. As long as the data from different aging setups can not be combined properly, it is very difficult to give an extrapolation about the lifetime of the real detector. Therefore, we have tested the aging performance of muon proportional chambers filled with $`Ar/CF_4/CH_4`$ (74:20:6), $`Ar/CF_4/CH_4`$ (67:30:3) and $`Ar/CF_4/CO_2`$ (65:30:5), $`Ar/CF_4`$(70:30), $`CF_4/CH_4`$(90:10), $`CF_4/CH_4`$(80:20) mixtures in the HERA - B environment, under conditions as close as possible to the real ones. The results of these aging tests are summarized in this paper.

## 2  Aging Studies in a HERA-B Environment

### 2.1  Experimental Setup

Three different types of gas proportional chambers make up the muon system: tube, pad and pixel . In the following we report on aging studies performed with aluminum proportional tube chambers in the real HERA-B environment.

The main objective of these tests was to prove that muon chambers are capable of operating after exposure to an integrated charge of 600 $`\frac{mC}{cmwire}`$, which is expected after three years of operation in the hottest region, without loss in performance.

The tube chamber is a closed-cell proportional wire chamber made from an aluminum profile (wall thickness 2 mm) with a drift cell 14 $`\times `$ 12 mm2 in cross section. Fig. 1 shows a schematic drawing of a tube chamber. A gold-plated tungsten wire of 45 $`\mu `$m diameter and a length of nearly 3 m is stretched inside each cell and fixed mechanically with pins at the chamber endcaps.

In order to test the aging properties under conditions as close as possible to real ones, three tube chambers with 16 drift cells each and a cross section exactly as for the production version, but of a shorter length of 50 cm, were placed between the electromagnetic calorimeter and the muon absorber in the HERA-B experiment, where the charged and neutral particle fluxes are extremely high . Initially, two of the chambers filled with $`Ar/CF_4/CH_4`$ (67:30:3) and $`Ar/CF_4/CO_2`$ (65:30:5) mixtures were subdivided to allow groups of anode wires (zones) to be operated at five different high voltages. Fig. 2 shows a simple schematic representation of the experimental setup, numbering scheme for the wires, and summarizes the operating conditions. The applied voltages were chosen in a way to obtain comparable accumulated charges in zones 2,3,4,5. Between any two zones there was a reference wire for which high voltage was not applied. The total collected charge in each HV zone was determined by integrating the continuously recorded anode current. Due to variations in the rate of $`pN`$-interactions in the HERA-B experiment, the radiation intensity and thus the average current varied during the studies by a factor of 4, thus excluding a possibility to investigate the aging behavior as a function of rate. It should also be noted that tests with $`Ar/CF_4/CH_4`$ and $`Ar/CF_4/CO_2`$ mixtures have been done at about one order of magnitude higher radiation levels than expected in the muon detector (20 nA/cm), thus allowing a study of the aging properties of the gases in a more severe radiation environment. The third chamber was subdivided into 4 zones, each containing two or three wires, as shown in Fig. 2. Radiation studies with mixtures $`CF_4/CH_4`$ (90:10), $`CF_4/CH_4`$ (80:20), $`Ar/CF_4`$ (70:30) were performed on different chamber wires in order to investigate the influence of materials and possible trace contaminants in the gas system, as well as water addition and cathode cleanliness, on the aging performance.

For each chamber a pre-mixed gas was transported by a 150 m stainless steel tube followed by a polyamid tube connected directly to the chamber inlet. The addition of water to the gas was done indirectly, by varying the length of the polyamid tube, which is transparent to $`H_2O`$, for a fixed flow rate. The gas flow within the chamber was serial: the gas inlet was connected to chamber cell N1, and the gas outlet to cell N16. The gas outlet of the chamber was connected via a 50 m stainless steel tube to the input of a gas chromatograph, which was used to analyze the concentration of species ($`Ar`$, $`CF_4`$, $`CH_4`$, $`CO_2`$, $`N_2`$, $`O_2`$, $`H_2O`$) in the effluent gas stream. Usually, measured concentrations of $`N_2`$ and $`O_2`$ were at the level of 150-250 ppm.

Periodically (typically once/month) chamber characteristics were studied in a 3 GeV electron beam with an intensity $``$ 1 $`kHz/cm^2`$. A reduction in efficiency measured with electrons at different positions along the wire was used as the main information about the loss in performance. In addition, during irradiation in the HERA-B environment several other types of performance degradation with distinct symptoms also indicate the appearance of aging effects: dark current, special ’switch-on’ current behavior (decrease in the anode current after high voltage is applied, since a certain time is necessary to establish the equilibrium charge density on the aged wire surface). This phenomena has been widely described in the literature . And finally, an interesting phenomena was observed for all aged wires operated with an $`Ar/CF_4/CH_4`$ mixture: the operating current was dependent upon the gas flow rate (an increase of gas flow led to an increase in the anode current). We will come back to the experimental study of this specific aging phenomena in a subsequent paper . At the same time, for all wires without gain reduction, neither ’switch-on’ current behavior nor dependence of operating current upon the flow rate have been observed. Thus, the appearance of any type of performance degradation for a particular group of anode wires could also serve as a manifestation of aging effects.

Before the start of the aging run, tube chamber efficiency and singles counting rate as a function of high voltage were measured for different gas mixtures in the electron beam (see Fig. 3a,b). The readout of the chambers is based on the ASD-8 amplifier shaper discriminator chip . Therefore, real afterpulses and multiple hits coming from ASD-8 per signal both contribute to the rise in singles rate curves, above the nominal beam intensity, with increasing high voltage. According to results reported in , operating voltages for the tube chamber were chosen for the following: $`Ar/CF_4/CH_4`$ (74:20:6) - 2.25 kV, $`Ar/CF_4/CH_4`$ (67:30:3) - 2.45 kV, $`Ar/CF_4/CO_2`$ (65:30:5) - 2.4 kV, corresponding to the baseline gas amplification $`310^4`$.

### 2.2  Aging in an $`Ar/CF_4/CH_4`$(67:30:3) gas mixture

Radiation tests with an $`Ar/CF_4/CH_4`$ (67:30:3) mixture, which is similar to $`Ar/CF_4/CH_4`$ (74:20:6), have been carried out in the real HERA-B environment. Due to the reduced $`CH_4`$ content in $`Ar/CF_4/CH_4`$ (67:30:3), better aging properties of this mixture were expected. This was also confirmed during irradiation with a $`Ru^{106}`$ source, where stable operation up to a total collected charge of 2 $`\frac{C}{cmwire}`$ was achieved . Since water added to the mixture in small concentrations is believed to prevent polymerization of hydrocarbons, we used 500 $`ppm`$ of $`H_2O`$ from the beginning of the tests. Typically, a chamber was flushed at a flow rate of 3 liters/hour, corresponding to two volume exchanges per hour.

First results in the HERA-B environment showed that aging effects in the $`Ar/CF_4/CH_4`$(67:30:3) + 500 $`ppm`$ of $`H_2O`$ mixture depend on the gas amplification (high voltage) and the size of the irradiation area.

After 10 days of exposure which resulted in a collected charge of $``$ 25 $`\frac{mC}{cmwire}`$ electron beam tests showed gain reduction for two (N14,N15) from three wires operated at high voltage 2.65 kV. After an accumulated charge of $``$ 100 $`\frac{mC}{cmwire}`$ all three wires (N13,N14,N15) in zone 5 were already inefficient. A similar aging behavior has been observed for the wires irradiated at 2.6 kV, however their lifetime was slightly longer. After an accumulated charge of $``$ 80 $`\frac{mC}{cmwire}`$, gain reduction has been found for one wire N11 and approximately at a dose of 170 $`\frac{mC}{cmwire}`$ electron beam tests revealed efficiency loss in both cells (N10,N11). In addition to a gain reduction for the wires irradiated at 2.6 kV and 2.65 kV, operation of these cells in the HERA-B environment was accompanied by the ’switch-on’ current behavior and the appearance of the dependence of the operating current on the gas flow rate. Dark current (or Malter effect) in these zones also started to appear and could lead to a subsequent detector degradation.

It has to be noted that the efficiency loss for wires operated at 2.6 kV and 2.65 kV was more severe in the direction of the serial gas flow. Initially aging effects in zones 4 and 5 appeared on the last wires (N11,N15) in the serial gas flow, although the radiation intensity for these wires was the lowest in each zone. Fig. 4 shows an example of how the efficiency profile developed in the direction of gas flow for wire N11 with the accumulated charge. The loss in performance for cell N11 with increasing ’usage’ of the gas is obvious. Wires (N13,N14,N15) were irradiated up to a dose of $``$ 200 $`\frac{mC}{cmwire}`$, while aging tests in zones 2,3,4 were continued up to collected charge $``$ 400 $`\frac{mC}{cmwire}`$. Due to the smaller current density the total accumulated charge in zone 1 was only $``$ 100 $`\frac{mC}{cmwire}`$. We did not observe any onset of dark current in cells N1-N8 during the whole period of irradiation. After the aging run, the chamber performance was studied in an electron beam. All wires operated at 2.6 kV, 2.65 kV showed strong anode aging. At the same time, scanning along the wires N5,N7,N8 with an electron beam revealed several distinct spots with a typical size of several $`cm`$, where local inefficiencies were detected (measured efficiency at 2.4 kV was $``$ 90-98 $`\%`$). No change in performance was found for wires N1,N2 (2.25 kV), N4 (2.5 kV), and all reference wires.

In addition to measurements in the electron beam, at the conclusion of the run wires irradiated at 2.6 kV and 2.65 kV were taken for surface analysis at ‘Digital Analytical Scanning Microscope JSM-6400’. The scanning electron microscope (SEM) yields information on the morphology of the wire surface by imaging with scattered and secondary electrons, and energy dispersive X-ray spectroscopy (EDX) analysis gives the atomic composition of the surface material. Usually, micrographs of anode wires were taken at SEM accelerating voltage 20 kV (sometimes - 5 kV), while cathodes were analyzed at 5 kV. The increased sensitivity to surface deposits at 5 kV is due to the reduced penetration of the lower energy primary electrons. Fig. 5 shows SEM micrographs and EDX analysis of wire N13 specimen taken near the gas inlet and wire N15 specimen taken near the gas outlet (150 cm downstream from the beginning of zone 5 in the serial gas flow). EDX analysis of these specimens confirmed the presence of polymers on the wires, containing carbon and fluorine as the only detectable elements (SEM is insensitive to hydrogen) (see Fig. 5). Moreover, analysis of the wires (N13,N14,N15) have shown that the $`F/C`$ ratio in the surface deposit increases in the direction of the serial gas flow. SEM micrograph of wire N11 irradiated at 2.6 kV was also taken and is shown in Fig. 6. In the whisker emission ’EDX’ spectrum there were identified lines corresponding only to $`C`$ and $`F`$ elements.

At this point we decided to study the influence of water on aging performance and continued tests with an increased $`H_2O`$ content (1400 $`ppm`$), while using the previously irradiated wires in zones 1,2,3. During three monthes of operation, approximately 400 $`\frac{mC}{cmwire}`$ were accumulated for wires irradiated at 2.5 kV and 2.55 kV and $``$ 100 $`\frac{mC}{cmwire}`$ for wires at 2.25 kV in addition to those collected in the previous run, which resulted in a total radiation dose of $``$ 800 $`\frac{mC}{cmwire}`$ in zones 2,3 and $``$ 200 $`\frac{mC}{cmwire}`$ in zone 1. Further scanning along the wires with an electron beam have shown that small inefficient spots on wires N5,N7,N8 had vanished, and all wires became fully efficient again. No change in performance was also observed for wires N1,N4. At the same time, an efficiency drop was detected for one of the wires, N2, operated at 2.25 kV, being more severe near the chamber endcaps (measured efficiency at 2.4 kV was $``$ 85 $`\%`$) than in the center of the wire ($``$ 97 $`\%`$), where the radiation intensity was the largest. Upon completion of the beam studies, all wires from the chamber were analyzed under the electron microscope. EDX analysis of irradiated wires N1,N4,N5,N7,N8 and all reference wires revealed only $`Au`$ peaks thus confirming the absence of the polymer coating. Fig. 7 shows the SEM micrograph and EDX spectrum for wire N5. However, SEM imaging of wire N2 revealed a surface deposit consisting of traces of $`Si`$ and $`O`$ (see Fig. 7). The absence of $`Si`$-containing deposits on all other aged wires operated with $`Ar/CF_4/CH_4`$ indicates that $`Si`$-polymerization was not a dominant aging process in our tests, and particularly for cell N2 could be a result of contamination from chamber endcaps. Moreover, gaseous discharges in an $`Ar/CF_4/CH_4`$ mixture could provide additional resistance for $`Si`$-deposits, which react with fluorine radicals to form volatile $`SiF_4`$. In plasma polymerization, discharges of $`CF_4/H_2`$ mixtures are successfully used for $`SiO_2`$ etching, while $`CF_4/O_2`$ plasmas selectively etches $`Si`$ .

In order to study the influence of water on aging performance in $`Ar/CF_4/CH_4`$, we have carried out new radiation tests. For this all chamber cells were restrung with new wires. With an electron beam rate of 1 $`kHz/cm^2`$, no difference in efficiency between previously irradiated and reference cells was found. However, the dark current observed in the previous run from wires N10,N11,N13,N14,N15 indicates that surface deposits could be present on the cathodes in these cells. Although a subdivision of anode wires into 4 high voltages groups was slightly changed for this run: zone 1 (wires N1,N2) - 2.25 kV, zone 2 (wires N4,N5,N6) - 2.5 kV, zone 3 (wires N8,N9) - 2.6 kV, zone 4 (wires N14,N15,N16) - 2.65 kV, this did not affect significantly the average current density in each zone. Initially, radiation tests with the previously used mixture $`Ar/CF_4/CH_4`$ (67:30:3) \+ 1400 $`ppm`$ of $`H_2O`$ were performed up to radiation doses: 40 $`\frac{mC}{cmwire}`$ in zone 1, 80 $`\frac{mC}{cmwire}`$ in zone 2, 100 $`\frac{mC}{cmwire}`$ in zone 3, 120 $`\frac{mC}{cmwire}`$ in zone 4. During the whole period of irradiation, we observed dark current for the wires operated at 2.65 kV. At this point all polyamid tubes were exchanged with stainless-steel lines, thus excluding the presence of water in the chamber. Several types of performance degradation (dark current, steadily decreasing anode current) started to appear for wires operated at 2.5 kV, 2.6 kV, 2.65 kV at a level of an accumulated charge $``$ 15-30 $`\frac{mC}{cmwire}`$. These results were especially surprising for wires irradiated at 2.5 kV, since no gain reduction has been observed up to 800 $`\frac{mC}{cmwire}`$ in $`Ar/CF_4/CH_4`$ (67:30:3) mixture with 500 $`ppm`$ and 1400 $`ppm`$ of $`H_2O`$. At the end of the aging run without water, the following radiation doses were collected: 20 $`\frac{mC}{cmwire}`$ in zone 1, 70 $`\frac{mC}{cmwire}`$ in zone 2, 85 $`\frac{mC}{cmwire}`$ in zone 3, 65 $`\frac{mC}{cmwire}`$ in zone 4. (High voltage in zone 4 was switched off earlier than in other zones). It might be noted that in sharp contrast to wires in other zones no performance degradation for wires in zone 1 was observed up to the end of the run.

Studies of chamber efficiency in an electron beam confirmed significant gain reduction for all wires operated at 2.5 kV, 2.6 kV, 2.65 kV. Moreover, a strongly nonconductive polymer coating present on the wires complicated the measurement of efficiency due to the time-dependent amplitude suppression resulting from charging-up of aged wire surfaces . When the chamber was opened for inspection, dark whiskers randomly distributed on all irradiated wires in zones 2,3,4 were observed. Fig. 8 presents typical micrographs of the shaped growth deposits revealed by SEM on the wires N5 (2.5 kV) and N9 (2.6 kV), which are very similar to those observed after irradiation with $`Ar/CF_4/CH_4`$ (67:30:3) + 500 $`ppm`$ $`H_2O`$. The structure of these ’whiskers’ suggests that they are caused by debris attaching to the anode wire and could serve as nucleation points for further deposits. It is also important to note that the deposit thickness was clearly irregular, with some areas appearing relatively clean while others had ’whisker’ type deposits. Moreover, even in the ’whiskers’ free region, surface deposits consisting of $`C`$ and $`F`$ elements and masking the underlying gold signal, were identified (see Fig. 8). Scanning along wires N1,N2 irradiated at 2.25 kV, revealed a loss in efficiency for wire N1 with a maximum drop in the center of the wire (measured efficiency at 2.4 kV was $``$ 93 $`\%`$), where the radiation intensity was the largest. No change in performance was observed for wire N2. In contrast to results in other zones, these data demonstrate a dependence of the degree of aging on the irradiation intensity, and thus the accumulated charge, and not on the direction of the serial gas flow. SEM analysis at 20 kV of wire N1 revealed only gold, while the EDX spectrum at 5 kV is dominated by an intense $`C`$ peak masking the $`Au`$ signal. The different texture of the wire deposits at 5 kV and 20 kV, as a result of increased SEM sensitivity at 5 kV to the thin carbon layer, is clearly evident from Fig. 9. It is also notable that the deposits on the wire N1 are carbonaceous, without incorporation of $`F`$ into the polymer structure. This is in contrast to typical deposits detected after irradiation with higher voltages.

Unfortunately, the relatively small accumulated charge in zone 1, leaves us unable to conclude whether the difference in chemical composition of polymers in zone 1 and 2-4 can be attributed to the change in the polymerization mechanism as a result of increased plasma density in the avalanche for higher voltage, or simply indicates that the polymerization in an $`Ar/CF_4/CH_4`$ (67:30:3) mixture starts from the deposition of a carbon layer on the anode wire. Detailed discussion of the results presented here will be reported in a companion paper .

Several cathode pieces were also analyzed under the electron microscope. As can be seen from Fig. 10a, a thin deposit, consisting of $`C`$, $`F`$ and $`O`$, was detected on the irradiated $`Al`$ surfaces. Fig. 10 also shows that the maximum $`F`$ abundance was found on cathode cells N5 and N8, operated up to a dose $``$ 1000 $`\frac{mC}{cmwire}`$ in an $`Ar/CF_4/CH_4`$ (67:30:3) mixture with 500 $`ppm`$ of $`H_2O`$, 1400 $`ppm`$ of $`H_2O`$, and without water. Analysis of cathode cell N10, after irradiation with $`Ar/CF_4/CH_4`$ (67:30:3) + 500 $`ppm`$ of $`H_2O`$ up to 400 $`\frac{mC}{cmwire}`$ and cathode cell N6, after irradiation with $`Ar/CF_4/CH_4`$ (67:30:3) + 1400 $`ppm`$ of $`H_2O`$ up to 150 $`\frac{mC}{cmwire}`$, revealed a comparable $`F`$ abundance. Since the operating conditions for wires N5 and N6 were nearly identical during the last run, the difference in the $`F`$ abundance in these cells could be explained by the fact that polymer deposition on the $`Al`$ surface in cell N5 also occured in the previous run with water, when 800 $`\frac{mC}{cmwire}`$ were collected. Similar $`F`$ abundances on cathode cells N6 and N10, after different accumulated charges, indicates a larger rate of fluorocarbon deposition on $`Al`$ surfaces without water. However, it is not clear whether polymers deposited on the cathodes in the previous run (with 500 $`ppm`$ and 1400 $`ppm`$ of $`H_2O`$) could provoke extremely rapid aging effects during operation without water, or if such an aging rate is defined solely by the kinetics of $`Ar/CF_4/CH_4`$ wire avalanches without water, under particular discharge conditions.

Our results clearly demonstrate that the addition of water to the mixture $`Ar/CF_4/CH_4`$ (67:30:3) substantially increases the lifetime of the aluminum proportional chambers and decreases the rate of polymer deposition on the anode wires and cathode surfaces. Although under some conditions (gas gain $`<10^5`$, water addition $`>1000ppm`$, gas flow 3 l/h) tube chambers can be operated up to a nominal lifetime (600 $`\frac{mC}{cmwire}`$), the strong dependence of aging properties on high voltage and size of irradiation area completely ruled out the $`Ar/CF_4/CH_4`$ (67:30:3) mixture as a candidate for operation in the muon chambers at the HERA-B experiment.

### 2.3  Aging in an $`Ar/CF_4/CO_2`$(65:30:5) gas mixture

Our intensive aging studies have shown that both $`Ar/CF_4/CH_4`$ (74:20:6) and $`Ar/CF_4/CH_4`$ (67:30:3) mixtures failed to fulfill radiation hardness requirement and can not be used for operation in the muon detector. In order to test the suitability of the $`Ar/CF_4/CO_2`$ (65:30:5) + 1000 $`ppm`$ of $`H_2O`$ mixture, radiation studies were performed at five different high voltages (gas gain ranges from $`10^4`$ to $`310^5`$). We have employed a gas flow rate of 3 l/hour, corresponding to 2 volume exchanges per hour.

No change in performance of aluminum proportional chambers operated with $`Ar/CF_4/CO_2`$ (65:30:5) + 1000 $`ppm`$ mixture has been observed during the whole run up to collected charge $``$ 700 $`\frac{mC}{cmwire}`$ in zones 2-5. (The accumulated charge for the wires in zone 1 was $``$ 170 $`\frac{mC}{cmwire}`$). Fig. 11 shows efficiency profiles along wires N5,N10,N13 after an accumulated charge of 700 $`\frac{mC}{cmwire}`$ in the $`Ar/CF_4/CO_2`$ (65:30:5) + 1000 $`ppm`$ mixture.

At the conclusion of these tests, the tube chamber was opened for inspection. Fig. 12 shows typical SEM micrographs of the wires irradiated at high voltages: 2.5 kV (wire N5), 2.6 kV (wire N10), 2.65 kV (wire N13). Although SEM imaging revealed some local deterioration of the smooth wire surface after a long-term operation at high gain $`3\times 10^5`$ (see Fig. 12), the elemental composition of this wire is dominated by $`Au`$ peak (at 20 kV SEM voltage) and there is no evidence of other chemical elements. The appearance of a few wire specimens was slightly more black than that of a new one, however detailed SEM investigation of all irradiated wires have shown apparently clean surfaces with only a few point-like deposits ($`Si`$,$`Al`$) with typical size of 1-2 $`\mu m`$, that did not result in local inefficiencies.

While SEM demonstrated the absence of polymers on the anode wires, EDX analysis revealed trace amounts of $`C`$, $`O`$ and $`F`$ on the $`Al`$ cathodes in cells N13,N14,N15, irradiated at 2.65 kV (see Fig. 13). For cells N7 and N8, operated with a lower voltage of 2.55 kV, the relative abundances of $`C`$, $`O`$, $`F`$ on $`Al`$ cathodes were greatly reduced. Cathodes in cells N4 and N5, operated at 2.5 kV, were almost indistinguishable from the reference ones. Such fluorocarbon films on the cathode surfaces did not lead either to dark current or to efficiency loss. The appearance of fluorocarbon deposits on irradiated cathodes in $`CF_4`$-containing mixtures has been reported in the literature. As was shown in , trace fluorocarbon deposits formed on cathodes after irradiation in pure $`CF_4`$ resulted in a loss of gas gain, rather than in a self-sustaining discharge. Although in other tests an increased layer of fluorine and oxygen was observed on the cathode, no change in gas gain was observed during long-term irradiation .

Using $`Ar/CF_4/CO_2`$(65:30:5) + 1000 $`ppm`$ $`H_2O`$ mixture, no loss in performance of aluminum proportional chambers was observed up to collected charge $``$ 700 $`\frac{mC}{cmwire}`$, whilst irradiating with different gas gains. Analysis of cathode surfaces revealed trace amounts of $`C`$, $`O`$ and $`F`$ for tubes operated at high gas gain $`10^5`$, while for a baseline gain of $`310^4`$, exposed cathodes were almost indistinguishable from reference ones. Therefore, $`Ar/CF_4/CO_2`$(65:30:5) + 1000 $`ppm`$ $`H_2O`$ mixture is currently used for the muon chamber operation.


text:
# Dimensionality dependence of the wave function statistics at the Anderson transition

## Abstract

The statistics of critical wave functions at the Anderson transition in three and four dimensions are studied numerically. The distribution of the inverse participation ratios (IPR) $`P_q`$ is shown to acquire a scale-invariant form in the limit of large system size. Multifractality spectra governing the scaling of the ensemble-averaged IPRs are determined. Conjectures concerning the IPR statistics and the multifractality at the Anderson transition in a high spatial dimensionality are formulated.

A disordered electronic system in $`d>2`$ dimensions can be driven from the phase of extended states to that of localized states by increasing the strength of disorder. This transition, bearing the name of Anderson, is characterized by remarkably rich critical properties. In particular, the eigenfunctions at the critical point show strong fluctuations and represent multifractal distributions.

These fluctuations can be quantitatively characterized by a set of inverse participation ratios (IPR), $`P_q=d^dr|\psi (𝐫)|^{2q}`$. Using the renormalization group in $`d=2+ϵ`$ dimensions ($`ϵ1`$), Wegner found  that the ensemble-averaged IPRs, $`P_q`$, show at criticality an anomalous scaling with respect to the system size $`L`$, $`P_qL^{\stackrel{~}{\tau }_q}`$, where

$$\stackrel{~}{\tau }_q=(q1)dq(q1)ϵ+O(ϵ^4).$$
(1)
Equation (1) is written for the case of unbroken time-reversal symmetry corresponding to the orthogonal ensemble which we consider in the paper. According to Eq. (1), the fractal dimensions $`\stackrel{~}{D}_q=\stackrel{~}{\tau }_q/(q1)`$ are different from the spatial dimension $`d`$ and depend on $`q`$, manifesting the multifractal character of the wave function intensity $`|\psi (𝐫)|^2`$ . It is customary to characterize such a distribution by its singularity spectrum determined by the Legendre transform of $`\stackrel{~}{\tau }_q`$, yielding

$$\stackrel{~}{f}(\alpha )=d(d+ϵ\alpha )^2/4ϵ+O(ϵ^4).$$
(2)
In the present paper we study how the wave function statistics and, in particular, the multifractality spectrum evolve with increasing spatial dimensionality, when the transition shifts from the weak-disorder range (as in $`d=2+ϵ`$) to the strong-disorder one. A numerical study of the Anderson transition in higher-dimensional systems is of special interest since no analytical results for the critical behavior in high $`d`$ are available. In contrast to conventional second-order phase transitions for which the mean-field treatment becomes valid above the upper critical dimension $`d_c`$, so that the critical exponents are $`d`$-independent for $`dd_c`$, the usual mean-field approach fails in this case. The model has been solved on the Bethe lattice  which is believed to correspond to the limit $`d=\mathrm{}`$. While for the critical exponent of the localization length the conventional mean-field value $`\nu =1/2`$ was obtained, a very unusual non-power-like critical behavior of other quantities was found (namely, an exponential vanishing of the diffusion constant and a jump in the inverse participation ratios $`P_q`$ with $`q=2,3,\mathrm{}`$ at the mobility edge). It was, however, shown in  that these results are intimately related to the spatial structure of the Bethe lattice. On this basis, it was argued that although the symmetry-breaking description of the transition in terms of an order-parameter function  is of general validity, the peculiar critical behavior found in  is an artifact of the Bethe lattice and should take a power-law form for any finite $`d<\mathrm{}`$. Assuming that the critical indices should match at $`d\mathrm{}`$ the Bethe lattice behavior (which corresponds to $`\stackrel{~}{\tau }_q=0`$ for $`q2`$ and to the value $`s=\mathrm{}`$ for the conductivity exponent), one then concludes that the upper critical dimension is $`d_c=\mathrm{}`$  (see also ). While available numerical results for the value of $`\nu `$  and for the form of the critical level statistics  in four dimensions (4D) are consistent with this conjecture, its rigorous justification and a systematic analytical study of the transition for large $`d`$ are still missing.

To investigate the dimensionality dependence of the critical statistics of wave functions, we have performed numerical simulations of 3D and 4D tight-binding models with periodic boundary conditions and a box distribution of site energies. The critical values of the disorder are known to be $`W_c16.5`$ for 3D  and $`W_c35`$ for 4D . We have calculated wavefunctions with energy close to zero by diagonalizing the Hamiltonian using efficient numerical packages . Thereby we could average over an ensemble that contained typically $`10^3`$ samples. From every sample 128 wavefunctions with energy close to zero have been taken into account.

We begin by showing in Fig. 1 the evolution of the distribution $`𝒫(\mathrm{ln}P_2)`$ in 3D with the linear size $`L`$ of the system from $`L=8`$ to $`L=80`$. It is clearly seen that at large $`L`$ the distribution acquires a scale-independent limiting form and simply shifts along the $`x`$-axis without changing its shape. The scale-invariance of the IPR distribution at criticality was conjectured in . This conjecture was questioned in , where numerical simulations of the IPR distribution in 3D were performed, with the conclusion that the fractal dimension $`D_2`$ is not a well defined quantity but rather shows strong fluctuations with root mean square deviation $`\mathrm{rms}(D_2)1`$. In terms of the IPR distribution the statement of  would mean that the rms deviation $`\sigma _2[\mathrm{var}(\mathrm{ln}P_2)]^{1/2}`$ scales in the same way as $`\mathrm{ln}P_2\mathrm{ln}L`$ in the limit of large $`L`$. However, a detailed analytical and numerical study of the wave function statistics in a family of critical power-law random banded matrix (PRBM) ensembles has shown  that the IPR distribution $`𝒫(\mathrm{ln}P_q)`$ is scale-invariant, corroborating the conjecture of . It was argued that this is a general feature of the Anderson transition, and the conclusion of Ref.  was criticized as based on a not sufficiently careful numerical analysis of data obtained for too small systems. This expectation was supported by a very recent numerical study of the 3D Anderson transition  where a trend to saturation of the width of the distribution $`𝒫(\mathrm{ln}P_2)`$ with increasing length $`L`$ was found. Our data (Fig. 1a) demonstrate the scale-invariance of the limiting distribution even more convincingly, since we have reached considerably larger values of $`L`$. The same conclusion can be drawn from the inset of Fig. 2 where the saturation of the rms deviation $`\sigma _q(L)`$ of the distribution $`𝒫(\mathrm{ln}P_q)`$ at $`L\mathrm{}`$ is demonstrated. Qualitatively similar results are obtained for the IPR distribution in 4D (Fig. 1b). Though a tendency to the saturation with increasing $`L`$ is clear in this case as well, the full saturation has not been reached, in view of smaller linear sizes of the system as compared to 3D.

To visualize the strength of the IPR fluctuations, we show in the main panel of Fig. 2 the values of the rms deviations $`\sigma _q`$, which characterize the width of the distribution functions $`𝒫(\mathrm{ln}P_q)`$, extrapolated to $`L\mathrm{}`$. In $`d=2+ϵ`$ dimensions $`\sigma _q`$ can be calculated analytically following , with the result

$$\sigma _q^2=8\pi ^2a_2ϵ^2q^2(q1)^2,qq_c=(2/ϵ)^{1/2},$$
(3)
where $`a_2`$ = 0.00387 for the periodic boundary conditions. Here $`q_c`$ is the value of $`q`$ corresponding to the root $`\alpha _{}`$ of the singularity spectrum $`\stackrel{~}{f}(\alpha )`$, i.e. $`q_c=\stackrel{~}{f}^{}(\alpha _{})`$ and $`\stackrel{~}{f}(\alpha _{})=0`$. For $`qq_c`$ the IPR distribution is dominated by its slowly decaying power-law “tail”

$$𝒫(P_q/P_q^{\mathrm{typ}})(P_q/P_q^{\mathrm{typ}})^{1x_q},P_qP_q^{\mathrm{typ}},$$
(4)
where $`x_q=q_c/q`$ . This yields $`\sigma _q=q/q_c`$, or in $`2+ϵ`$ dimensions,

$$\sigma _q=(ϵ/2)^{1/2}q,q(2/ϵ)^{1/2}.$$
(5)
In addition to the numerical results for 3D and 4D, we present in Fig. 2 the result (3) of the $`ϵ`$-expansion for $`d=2.2`$. Furthermore, we show the small-$`q`$ and large-$`q`$ analytical asymptotics (3) and (5) with $`ϵ=1`$. Of course, the $`ϵ`$-expansion is only justified parametrically for $`ϵ1`$. Nevertheless, we see that it still describes very reasonably the IPR fluctuations at the Anderson transition in 3D.

Having demonstrated that the distributions of the IPRs $`P_q`$ are scale-invariant at criticality, so that the fractal dimensions are well defined, we are prepared to analyze the form of the multifractal spectra. We use the numerical procedure described in Ref. , where it was applied to the quantum Hall plateau transition. Specifically, we calculate the ensemble-averaged IPR $`P_q`$ for different system sizes $`L`$, extract $`\stackrel{~}{\tau }_q`$ and $`\stackrel{~}{f}(\alpha )`$ and extrapolate to the thermodynamic limit $`L\mathrm{}`$ in order to eliminate the finite-size corrections. We refer the reader to Ref.  for more details of the procedure and for a discussion of its advantages as compared to the box-counting calculations performed in earlier publications.

The obtained results for $`\stackrel{~}{f}(\alpha )`$ in 3D and 4D are shown in Fig. 3. To illustrate the evolution of the spectrum in the whole range from $`d=2`$ to $`d=4`$, the analytical results (2) for $`2+ϵ`$ dimensions with $`ϵ=0.2`$ and $`ϵ=0.01`$ are also shown. In Fig. 4 the corresponding results for the fractal dimensions $`\stackrel{~}{D}(q)`$ are presented. We see that with increasing dimensionality the singularity spectrum $`\stackrel{~}{f}(\alpha )`$ broadens. This is not surprising: with increasing $`d`$ the transition moves further in the region of strong disorder, implying stronger multifractality. What is much less obvious is that in the range $`\alpha 2`$ the $`\stackrel{~}{f}(\alpha )`$ curve shifts to the left with increasing $`d`$. This corresponds to the fact that the fractal exponents $`\stackrel{~}{D}_q`$ with $`q1`$ decrease with increasing $`d`$. In particular, for the exponent $`\stackrel{~}{D}_2`$ determining the spatial dispersion of the diffusion coefficient at criticality we find $`\stackrel{~}{D}_2=1.3\pm 0.05`$ in 3D and $`\stackrel{~}{D}_2=0.9\pm 0.15`$ in 4D . It is worth mentioning that the $`ϵ`$-expansion (2) with $`ϵ=1`$ describes the 3D spectrum remarkably well (though with detectable deviations, see inset of Fig. 3). In particular, the position of the maximum, $`\alpha _0=4.03\pm 0.05`$ is very close to its value $`\alpha _0=d+ϵ`$ implied by (2). As expected, in 4D the deviations from the parabolic shape are much more pronounced and $`\alpha _0=6.5\pm 0.2`$ differs noticeably from $`6`$.

The obtained value of $`\stackrel{~}{D}_2=1.3\pm 0.05`$ in 3D is considerably smaller than what was found in the earlier numerical studies  where the values in the range $`1.4÷1.8`$ were reported. The reasons for this are as follows. In the earlier works the spectrum $`f(\alpha )`$ of individual eigenstates was studied via the box-counting procedure. While in the limit $`L\mathrm{}`$ the spectrum $`f(\alpha )`$ defined in this way should reproduce the part of the $`\stackrel{~}{f}(\alpha )`$ curve lying above the $`x`$-axis, for a finite $`L`$ the finite-size effects affect $`f(\alpha )`$ strongly, especially in the region close to the zero $`\alpha _{}`$ of $`\stackrel{~}{f}(\alpha )`$. As a result, such a method not only fails to yield the exponents $`\stackrel{~}{D}_q`$ with $`q>q_c`$ but also leads to very large errors in determination of $`D_q`$ with $`q`$ smaller than but close to $`q_c`$. In particular, in 3D and 4D we find that $`q_c`$ is close to 2, explaining large errors in earlier results for $`q=2`$ in 3D. As to the 4D case, we are not aware of any previous studies of the wave function statistics at the Anderson transition.

Let us discuss now what our findings imply for the high-$`d`$ behavior of the critical wave function statistics. First of all, we notice that our numerical observation that $`\stackrel{~}{D}_q`$ with $`q1`$ decrease with increasing dimensionality confirms the above-mentioned expectation that they should tend to zero in the limit $`d\mathrm{}`$. In view of this, an analogy with the PRBM ensemble with the parameter $`b1`$ is very instructive. This ensemble can be considered as describing a 1D chain with random long-range hopping whose rms amplitude is $`b/r`$ where $`r`$ is the distance. The model is critical for arbitrary $`0<b<\mathrm{}`$ and can be studied analytically in both limits $`b1`$ and $`b1`$. The latter case is relevant to the issue under discussion, and we remind the reader of the key results  on the wave function statistics at $`b1`$. (The case $`b1`$ is to a large extent analogous to the Anderson transition in $`2+ϵ`$ dimensions with $`ϵ1`$.) Specifically, the scale-invariant critical distribution $`𝒫(P_q/P_q^{\mathrm{typ}})`$ becomes $`b`$-independent in the limit $`b1`$. Furthermore, the exponents $`\stackrel{~}{\tau }_q`$ with $`q>1/2`$ are proportional to $`b`$ in the small-$`b`$ limit,

$$\stackrel{~}{\tau }_q=2b\stackrel{~}{T}_q,\stackrel{~}{T}_q=2\mathrm{\Gamma }(q1/2)/\pi ^{1/2}\mathrm{\Gamma }(q1).$$
(6)
Correspondingly, the singularity spectrum $`\stackrel{~}{f}(\alpha )`$ acquires for $`\alpha 1`$ the form

$$\stackrel{~}{f}(\alpha )=2b\stackrel{~}{F}(\alpha /2b),$$
(7)
where $`\stackrel{~}{F}(A)`$ is the Legendre transform of $`\stackrel{~}{T}(q)`$, with the asymptotics $`F(A)1/\pi A`$ as $`A0`$ and $`F(A)A/2`$ as $`A\mathrm{}`$. The smallness of the fractal exponents, $`\stackrel{~}{\tau }_q1`$, reflects a very sparse structure of the eigenstates formed by resonances (spikes) with a hierarchy of distances between them, $`r_1r_2\mathrm{}`$, such that $`\mathrm{ln}r_{i+1}/r_i1/b`$ .

After this reminder we return to the Anderson transition in high dimensionality. The smallness of the fractal exponents, $`\stackrel{~}{D}_q1`$ at $`d1`$ implies, in close similarity to the PRBM model, that the corresponding critical eigenstates have the resonance structure with a hierarchy of scales $`\mathrm{ln}r_{i+1}/r_i1/b_d`$ and with a dimensionality-dependent parameter $`b_d`$ satisfying $`b_d0`$ as $`d\mathrm{}`$. (In contrast to the PRBM model, where the emergence of resonances was due to direct long-range hopping processes, now it should be determined by interference of all possible paths connecting two sites on a $`d`$-dimensional lattice.) The sparse resonance structure of eigenstates allows us to use the analogy with the PRBM model and to make the following conjectures: (i) The scale-invariant distribution $`𝒫(P_q/P_q^{\mathrm{typ}})`$ for $`q>1/2`$ becomes essentially $`d`$-independent at $`d1`$. (ii) The fractal exponents take at $`d1`$ and for $`q>1/2`$ the form $`\stackrel{~}{\tau }_q(d)=2b_d\stackrel{~}{T}_q`$, i.e. they depend on $`d`$ only through the overall factor $`b_d`$ (satisfying $`b_d0`$ as $`d\mathrm{}`$). Correspondingly, the singularity spectrum scales at large $`d`$ as $`\stackrel{~}{f}(\alpha )=2b_d\stackrel{~}{F}(\alpha /2b_d)`$. Though we are fully aware of a speculative character of these conjectures at the present stage, we expect that they will stimulate further numerical and analytical work, which should finally resolve the challenge posed by the Anderson transition in high $`d`$.

In conclusion, we have studied the statistics of critical wave functions at the Anderson transition in 3D and 4D. The distribution of the inverse participation ratio $`P_q`$ was demonstrated to acquire a scale-invariant form in the limit of large system size. As a convenient measure of the strength of the IPR fluctuations, we have evaluated the rms deviation $`\sigma _q`$ of $`\mathrm{ln}P_q`$ and found a result matching well analytical predictions for $`2+ϵ`$ dimensions with $`ϵ1`$. Calculating the ensemble-averaged IPR values, $`P_q`$, we have determined the spectrum of fractal dimensions $`\stackrel{~}{\tau }_q\stackrel{~}{D}_q(q1)`$ and the singularity spectrum $`\stackrel{~}{f}(\alpha )`$ characterizing the multifractal properties of the wave functions. In particular, we have found $`\stackrel{~}{D}_2=1.3\pm 0.05`$ in 3D and $`\stackrel{~}{D}_2=0.9\pm 0.15`$ in 4D. More generally, our results indicate that the dimensions $`\stackrel{~}{D}_q`$ with $`q1`$ decrease with increasing spatial dimensionality $`d`$. On this basis, we have formulated two conjectures concerning the wave function statistics at criticality in the large-$`d`$ limit.

It is a pleasure to acknowledge help with the implementation and usage of the Watson sparse matrix package by A. Gupta and M. Krauss. This work was supported by the SFB195 and the Schwerpunktprogramm “Quanten-Hall-Systeme” der Deutschen Forschungsgemeinschaft.


text:
# Electronic Structure of the c(2x2)O/Cu(001) System

## I Introduction

Oxygen adsorbtion on Cu(001) has been the subject of much discussion and debate in the past three decades mainly because of the illusive nature of the adsorption geometry. The history of the field is nicely summarized in a recent paper . Here we mention some of the essential points. Unlike the case of Ni(001) in which a true $`c(2\times 2)`$ phase is observed as the oxygen coverage approaches 0.5ML  in which the oxygen atoms occupy fourfold hollow sites at a distance about 0.8Å above the top Ni layer, the stable surface structure for similar oxygen coverage on Cu(001) has the periodicity $`(2\sqrt{2}\times \sqrt{2})R45^{}`$  and involves missing rows of Cu atoms according to LEED  and surface $`X`$ray diffraction  measurements. This conclusion was agreed upon after much debate and analysis of data from several complimentary experimental techniques, some of which indicated the presence of a $`c(2\times 2)`$ structure on an unreconstructed Cu(001) . Other experiments have indicated the presence of both of these phases  and still others have given evidences of disordered phases in the system . A more recent scanning tunneling microscopic (STM) study has also affirmed the presence of $`c(2\times 2)`$ overlayer of adsorbed oxygen on Cu(001) at low coverage, but only in nanometer size domains and not large well-ordered domains .

Currently, based on the above findings, the following picture can be built. If the adsorbate coverage is low, oxygen atoms adsorb on Cu(001) forming $`c(2\times 2)`$ islands. Increase in the coverage leads to the ordering of the $`c(2\times 2)`$ domains, forming $`c(4\times 6)`$ pattern. When the coverage approaches a critical value of 34% of monolayer, the $`(2\sqrt{2}\times \sqrt{2})R45^{}`$ structure made by a missing row type reconstruction is formed.

The competition between the observed O/Cu(001) phases and the subsequent reconstruction of the surface with the $`(2\sqrt{2}\times \sqrt{2})R45^{}`$ overlayer shows signs of a delicate balance in the surface electronic structure of the system which tilts in favor of one phase or the other depending on the coverage. A detailed description of the electronic states and chemical bonds formed when oxygen atoms adsorb on the Cu surface should thus provide much needed insight into the factors responsible for the observed variations in the surface structure.

A possible theoretical explanation follows from effective medium theory  which predicts a reconstructed stable state for the substrate. These researchers find that the O valence levels interact very strongly with the Cu $`d`$-bands such that the states can be shifted through the Fermi level. The difference in the total energy of the reconstructed and the unreconstructed Cu surface arises from dependence of the energetic location of the antibonding levels, derived from the O 2$`p`$ – Cu 3$`d`$ hybridization, on coordination. A missing row can force this level up, thereby pushing up the hybridized antibonding level which can straggle the Fermi level, leading to a reduced occupation and thus stronger net bonding. In the case of a Ni substrate the 3$`d`$ band straggles the Fermi level, and so its position is largely pinned by the need for charge neutrality.

The rationale for a reconstructed Cu surface with O as adsorbate has also been related to the instability of the unreconstructed surface due to the large charge transfer to the adsorbate . Calculations performed for oxygen on small clusters of Cu (2–25 atoms  and 5 atoms ) find a strong electronic charge transfer from the metal atoms to oxygen in the amount of 1.2e  or 1.5e . These two factors (the degree of the $`p`$O – $`d`$Cu hybridization and amount of the effective charge on O) have thus far been proposed as the driving forces for the phase instability of the $`c(2\times 2)`$ structure. The ab initio cluster calculations has also found the O–Cu bond to be mostly ionic with some participation of the $`d`$-electrons of Cu . It should be borne in mind, however that models like the effective medium theory are at best semi-empirical. Further none of the theoretical methods as far employed take into account the contribution of the Madelung potential for these two overlayer structures, which may significantly change the subband energetic positions and charge distribution. If indeed an appreciable charge transfer and details of $`p`$O – $`d`$Cu hybridization are responsible for the stability of a superstructure on Cu(001), a systematic calculation of these quantities is warranted. Such a calculation must also provide a comprehensive description of the relationship between the electronic and geometric structures of the system, including the contribution of the Madelung potentials. This paper is an effort in this direction.

We have carried out detailed calculations of the electronic structure of the O/Cu(001) system using a reliable method and by varying the separation between the oxygen overlayer and the Cu(001) surface. As we shall see, there continues to be a debate also on the height of the oxygen atoms above the Cu surface. Our calculational strategy allows us to compare the local charge redistribution, modifications of hybridization of various electronic states and variations of the local and long-range contributions to the potentials, as a function of the height of the oxygen overlayer above the surface. It is through such systematic studies and, in conjunction with experimental observations, that we expect to gain insights into the nature of the chemical binding between the O and Cu atoms and establish rationale for the formation of a particular overlayer. Since, both $`c(2\times 2)`$ and $`(2\sqrt{2}\times \sqrt{2})R45^{}`$ phases have been shown to exist , our focus in this paper is on the former. At a later stage we will undertake a study of the missing row reconstructed surface with the large surface unit cell to represent the $`(2\sqrt{2}\times \sqrt{2})R45^{}`$, which would require a much larger computational effort than the present one. It should be mentioned that Wiell et al.  have used a realistic full-potential LMTO method to examine the hybridization of orbitals of the N overlayer on Cu(001). These authors have also touched upon the O/Cu(001) system, but no details of the O – Cu electronic state hybridization or the charge transfer have been provided.

The structural studies of the $`c(2\times 2)`$ O/Cu(001) system performed with different techniques provide quite different results as the interlayer O–Cu spacing ($`d_{OCu1}`$) ranges from $`0`$ to $`1.5`$Å. However, a majority of results  gives $`d_{OCu1}`$ value in the range $`0.40.8`$Å. The SEXAFS measurements  suggest three different configurations. In one of them the O atoms are located at the fourfold hollow (FFH) sites with $`d_{OCu1}=0.5`$Å. Two other configurations represent the distorted FFH geometries with $`d_{OCu1}=0.8`$Å. The authors of recent photo-electron diffraction studies also propose a two-side model involving the O atoms at FFH positions with $`d_{OCu1}=0.41`$ and $`0.7`$Å. They associate these two values with the edge and center positions in small $`c(2\times 2)`$ domains, respectively. Our calculations are performed for the exact FFH geometry for a set of $`d_{OCu1}`$ including the values obtained from the different experiments. We use a computational method based on the theory of multiple scattering in real space. This allows us to explicitly obtain the local electronic structure of atoms with different locations. Our results show a general picture of the electronic state modification when oxygen atoms approach the Cu(001) surface and reveal the factors controlling charge transfer and chemical bond formation.

## II Computational Method

The calculations are based on the density functional theory within the local density approximation (LDA)  and multiple scattering theory. Our approach embodies the local self-consistent multiple scattering method , in which a compound is divided into overlapping clusters called local interaction zones (LIZs) centered around atoms in different local environments. For each LIZ, a system of equations for the $`T`$ scattering matrix in the lattice site – angular moment representation for the muffin-tin (MT) potential  is solved self-consistently. The solutions are used to determine the cluster Green’s functions and subsequently the local and total electronic densities of states and valence charge densities. An application of this method to materials related to the work here (copper oxides) has demonstrated its high efficiency and reliability .

In our model system, apart from the oxygen overlayer, the top four Cu layers (Cu1 – Cu4) were considered to be different from the bulk Cu. The fifth and lower Cu layers were supposed to have bulk properties. LIZ’s were built around nonequivalent atoms belonging to the five different layers and contained 71 to 79 atoms depending on the local configuration. The sizes of the LIZ’s were taken such that the calculated characteristics of the bulk system closely matched those obtained from other reliable methods.

At each iteration of the self-consistent process a new potential is built by solving the Poisson’s equation with the charge density obtained at the previous iteration. To take into account surface effects we follow the approach developed in Ref.  where the MT potential at the $`\alpha `$th atom belonging to the $`i`$th layer is given by

$$V(r_{i\alpha })=\frac{2Z_{i\alpha }}{r_{i\alpha }}+8\pi \left[\frac{1}{r_{i\alpha }}\underset{0}{\overset{r_{i\alpha }}{}}\rho _{i\alpha }(x)x^2𝑑x+\underset{r_{i\alpha }}{\overset{R_{i\alpha }}{}}\rho _{i\alpha }(x)x𝑑x\right]$$
(1)
$$+V^{xc}[\rho (r_{i\alpha })]V^{EC}V^{xc}(\rho ^0)4\pi \rho _i^0+V_{i\alpha }^{Mad}$$

The nuclear and the MT electronic charge density contributions to the potential (the first term and the terms in square brackets in (1), respectively) are of the same form as in the bulk calculations . The electrostatic $`(V^{EC})`$ and exchange-correlation $`(V^{xc}(\rho ^0))`$ parts of the MT constant are taken from the bulk. The last two terms in the above expression represent the distant part of the MT potential:

$$V_D=4\pi \rho _i^0+V_{i\alpha }^{Mad}$$
(2)
This part contains explicit information about the surface. The interstitial charge density $`\rho _i^0`$ is supposed to be layer-dependent reflecting the asymmetry of the system. In such an approach the space in the vicinity of the surface is divided by layers belonging to different atomic planes parallel to the surface. In the present calculations we keep the thickness of the oxygen layer independent of the interlayer O – Cu1 spacing such that the radius of the corresponding Wigner-Seitz sphere is equal to the O-II ionic radius $`R_O=1.24\AA `$. The thickness of the Cu2 and next Cu layers corresponds to the bulk lattice parameter. The Cu1 layer takes the rest of the space between the O and Cu2 layers. The $`\rho _i^0`$ values are obtained by averaging the interstitial charges. The latter are differences between Wigner-Seitz $`(Q_{i\alpha }^{WS})`$ and MT $`(q_{i\alpha }^{MT})`$ charges, which are calculated by integration of the electronic charge density over Wigner-Seitz and MT spheres, respectively. The $`Q_{i\alpha }^{WS}`$ values are multiplied by a coefficient to meet charge neutrality condition for the region disturbed by the surface. This coefficient approaches unity, with charge convergence. The Madelung potential includes monopole $`M_{i\alpha ,j\beta }^{00}`$, dipole $`M_{i\alpha ,j\beta }^{10}`$ and interstitial $`V_{ij}[\rho _j]`$ terms :

$$V_{i\alpha }^{Mad}=\underset{j,\beta }{}\left(q_{j\beta }M_{i\alpha ,j\beta }^{00}+d_{j\beta }M_{i\alpha ,j\beta }^{10}+V_{ij}[\rho _j]\right),$$
(3)
where $`d_{j\beta }`$ is a dipole moment of the MT charge density and

$$q_{j\beta }=Z_{j\beta }q_{j\beta }^{MT}+\frac{4\pi }{3}\rho _jR_{j\beta }^3$$

The $`M_{i\alpha ,j\beta }^{00}`$ and $`M_{i\alpha ,j\beta }^{10}`$ terms in (3) are calculated by an Ewald-like plane-wise summation, and explicit solution of one-dimensional (normal to the surface) Poisson’s equation, using the technique described in Ref. .

The exchange and correlation parts of the potential are determined within LDA using the technique described in Ref. .

To test the applicability of the method to surface problems, we have calculated the electronic structure of the clean Cu(001) surface and compared our results with ones obtained by means of TB-LMTO method , screened KKR Green’s function method  and self-consistent localized KKR scheme developed for the surface calculations . As we shall see in the next section, our projected densities of electronic states calculated for the $`c(2\times 2)`$ O/Cu(001) system are in good agreement with those obtained by full potential LMTO method

## III Results and Discussion

We have calculated the electronic structure of the O/Cu(001) surface with the c(2x2) symmetry for selected values of the O-Cu1 interlayer spacing $`d_{OCu1}`$. As already discussed, there is some discrepancy in the values of $`d_{OCu1}`$ obtained from different experiments. However a majority of experiments have found $`d_{OCu1}`$ to lie between $`0.4\AA `$ and $`0.8\AA `$ ($`0.11a0.22a`$, where $`a`$ is the lattice parameter of bulk fcc copper). With this in mind we have varied $`d_{OCu1}`$ from $`0.15a`$ to $`0.3a`$ in our calculations and examined its effect on the surface electronic structure. The local densities $`N_l^\alpha (E)`$ of electronic states, their projection $`N_{lm}^\alpha (E)`$ on the cubic harmonics, and the valence electron density $`\rho (r)`$ have been calculated for the oxygen overlayer and the four top Cu layers, for selected values of $`d_{OCu1}`$.

The densities of the $`p`$O- and $`d`$Cu-electronic states of the system are plotted in Fig. 1 for the longest and shortest interlayer spacings considered. As seen in Fig. 1, the $`N_d^{Cu}(E)`$ calculated for the Cu3 and Cu4 atoms (third and fourth layer) are hardly affected by the choice of $`d_{OCu1}`$ and differ slightly from the bulk values whereas the $`d`$Cu2-states are noticeably disturbed. The $`d`$Cu1 and $`p`$O state densities are found to have a rich structure and for both values of $`d_{OCu1}`$ the spectra show a clear signature of the $`p`$O – $`d`$Cu1 hybridization. Note the position of the peaks marked $`\mathrm{"}a\mathrm{"}`$ and $`\mathrm{"}b\mathrm{"}`$ for $`d_{OCu1}=0.3a`$ and $`\mathrm{"}a^{}\mathrm{"}`$ and $`\mathrm{"}b^{}\mathrm{"}`$ for $`d_{OCu1}=0.15a`$ in Fig. 1. When the oxygen overlayer approaches the Cu(001) surface ($`d_{OCu1}=0.15a`$), the splitting (the distance between $`a^{}`$$`b^{}`$ peaks in the figure) increases reflecting an enhancement of the hybridization, which even involves the second copper layer.

To examine the charge transfer in the vicinity of the surface we have calculated the Wigner-Seitz charges that allowed us to obtain the amount of charge deviation ($`\mathrm{\Delta }Q_i`$) from electric neutrality per $`2D`$unit cells belonging to the different layers. The results are shown in Fig. 2. One can see a strong charge transfer from the Cu1 layer to the O overlayer coupled with some increase in the electron charge in the Cu2 layer. The effect is significantly enhanced when the oxygen atoms approach the Cu1 layer. From this result one would conclude that the O – Cu1 chemical binding has an essentially ionic character and that the ionicity increases as oxygen atoms approach the Cu(001) surface. In Table 1, we present the amount of charge transfer for the five different heights of the oxygen overlayer that we considered. At the shortest O–Cu1 distance, the two Cu atoms in the unit cell of the first layer have a deficit of about one electron each, with 1.5 electron going to the O atom and 0.25 electron for each of the 2 atoms of the second layer. The amount of charge provided to the O atom drops to 1 electron when it’s height above Cu1 is doubled to 0.3a. The charge deviation $`\mathrm{\Delta }Q_O`$ of the O layer and the distant part $`V_D`$ of the potential in Eq. (2) at the O site are plotted versus $`d_{OCu1}`$ in the lower panel of Fig. 2. A clear correlation between $`\mathrm{\Delta }Q_O`$ and $`V_D`$ seen in the figure suggests that the long-range electrostatic interaction is a driving force for the charge transfer in the system.

In the system under consideration, each oxygen atom and its four nearest Cu1 neighbors form a pyramid. Such an atomic configuration is expected to cause a strong anisotropy in the electronic structure. Therefore an analysis of the $`N_{lm}^\alpha (E)`$ distributions for O and Cu1 is very useful for understanding the nature of the chemical bonds formed when oxygen adsorbs on the Cu surface. A simple symmetry consideration shows that only the O-$`p_x,p_y`$ –Cu1-$`d_{xz}`$ and O-$`p_z`$ – Cu1-$`d_{x^2y^2}`$ hybridization can be significant in the O – Cu1 subsystem. Therefore our focus is mainly on these electronic states. In Fig. 3, the densities of the O-$`p_z`$ and Cu1-$`d_{x^2y^2}`$ states are plotted for the values of $`d_{OCu1}`$ as labeled. Both projected densities are considerably modified with the decrease in $`d_{OCu1}`$. The band broadens and distinct new peaks appear as $`d_{OCu1}`$ takes the values $`0.2a`$ and $`0.15a`$. An energetic alignment of the O-$`p_z`$ and Cu1-$`d_{x^2y^2}`$ peaks in the $`a`$, $`b`$ and $`c`$ regions is a signature of hybridization of these states. An increase in the peak amplitudes and an extra splitting with the decrease in $`d_{OCu1}`$ reflect a strong enhancement of the hybridization as the oxygen atoms approach the surface. In contrast, the splitting of the O-$`p_x,p_y`$ and Cu1-$`d_{xz}`$ states is almost independent of the $`d_{OCu1}`$ value (see Fig. 4). This means that the hybridization of these states is not changed noticeably, when $`d_{OCu1}`$ is varied within the range that we considered. Such a difference in the response of the electronic states to variation of the O-Cu1 interlayer spacing can be explained on the basis of a simple geometric analysis. When the oxygen atoms approach the Cu1 layer, the O – Cu1 bond length decreases and the symmetry of the O-$`p_z`$ and Cu1-$`d_{x^2y^2}`$ cubic harmonics is such that their overlap increases enhancing the hybridization. On the other hand, the symmetry of the O-$`p_x,p_y`$ and Cu1-$`d_{xz}`$ states is such that the overlap of their cubic harmonics is diminished with decrease in $`d_{OCu1}`$ that compensates the effect of the O – Cu1 bond length reduction.

Thus, according to these results, a noticeable covalence $`p`$O – $`d`$Cu1 binding takes place in the system along with the strong ionic binding. If the O – Cu1 interlayer spacing is long enough ($`d_{OCu1}=0.3a`$), the covalence component of chemical binding is mostly determined by the O-$`p_x,p_y`$ – Cu1-$`d_{xz}`$ hybridization. When $`d_{OCu1}`$ is smaller, the O-$`p_z`$ – Cu1-$`d_{x^2y^2}`$ contribution to the covalence bond increases. This competition mostly controls modification of the electronic states when the oxygen atoms approach the surface.

The densities of O-$`p_x,p_y`$ and O-$`p_z`$ electronic states have also been calculated for O/Cu(001) by means of the full-potential LMTO method , which is considered to be one of the best approaches for electronic structure calculations. These authors considered an oxygen overlayer with a $`c(2\times 2)`$ structure with the oxygen atom occupying an FFH and a quasi-FFH sites. In Fig. 5 we have compared our results obtained for $`d_{OCu1}=`$ 0.15a (0.514Å) with the results of Ref.  at the FFH site at a height of 0.5Å, for O-$`p_z`$ and O-$`p_{x,y}`$. Both the splitting and peak amplitudes are in very good agreement attesting to the reliability of the method used here. We note from Fig. 5 that a shift the height between 0.15a and 0.2a produces a shift of about 1eV of the spectrum, again in good agreement with the results in Ref. .

We have calculated the radial dependence of the valence electron charge density around the O and Cu1 – Cu4 atoms along some symmetrical directions. The plot of the oxygen charge density in Fig. 6 displays it to be essentially anisotropic. We have also found that the anisotropy increases when $`d_{OCu1}`$ is reduced from $`0.3a`$ to $`0.2a`$ whereas further $`d_{OCu1}`$ reduction leads to a decrease in the anisotropy. This effect is illustrated in Fig. 7, in which the radial dependence of the difference between the densities along the (001) and (100) directions is plotted for systems with different values of $`d_{OCu1}`$. Such a non-monotonic behavior can be explained by the hybridization competition mentioned above. The change in the anisotropy of the oxygen charge density occurs because different amounts of charge flow to the O-$`p_x`$ and O-$`p_z`$ states, as $`d_{OCu1}`$ decreases. The stronger covalence binding, the larger an increase in the electron-electron repulsion caused by an extra electronic charge in the bond region. Therefore the charge tends to come to the states less involved in hybridization, which are the O-$`p_z`$ states when $`d_{OCu1}`$ is large. This leads to an increase in the anisotropy. The tendency is changed at short interlayer distances, when the hybridization of the O-$`p_z`$ and Cu1-$`d_{x^2y^2}`$ is enhanced significantly that can make preferable an occupation of the O-$`p_x,p_y`$ states.

We now turn to the implication of the results presented here to a simple model proposed for the adsorption of oxygen on Cu(001). To describe this phenomenon, the authors of Ref.  use a model isotropic potential based on the local part of the Madelung potential. At the same time they assume that not only the O and Cu1 layers are involved in charge transfer, but also deeper ones. Our results confirm the latter assumption (see Fig. 2) and imply that an accurate model potential should be based on the long range Coulomb interaction rather than on the local one. Furthermore, using the experimental data obtained for the $`c(2\times 2)`$ and $`(2\sqrt{2}\times \sqrt{2})R45^{}`$ phases the authors of Ref.  build the isotropic potential, which appears to have step-like dependence on the O – Cu1 bond length. To obtain this, these authors attribute a step-like behavior to the effective atomic charges. They assume that such a behavior can be induced by an increase in covalence, as the O – Cu1 bond length is reduced. Our results do not support these assumptions. We have found that the charges and covalence of the bonds are smooth functions of the interatomic distance. The $`c(2\times 2)`$ and $`(2\sqrt{2}\times \sqrt{2})R45^{}`$ phases are different in the symmetry of the oxygen local surrounding rather than in the interatomic distances. This suggests that the phase transition can be properly described only by means of an anisotropic potential. Moreover, a noticeable covalence of the O – Cu1 binding (even for relatively long bond lengths) and its anisotropy obtained in our study allows us to propose that an accurate modelling of the $`c(2\times 2)`$ phase itself requires an anisotropic potential.

## IV Conclusions

The electronic structure has been calculated for the O/Cu(001) system in the $`c(2\times 2)`$ with five different O – Cu1 interlayer spacings. We find that the oxygen and copper atoms form a mixed ionic-covalence chemical binding in the O/Cu(001) system for the whole range of the considered O – Cu1 interlayer spacings. The oxygen atom gains an extra charge varying between 1 and 1.5 electron when its height is varied between 0.3a and 0.15a. This charge comes solely from the atoms at the top layer of the substrate with a small enhancement of the second layer electronic charge. We also find that this charge transfer is controlled by variation of the long-range electrostatic interaction. The detailed analysis of the properties of the local electronic structure reveals that the electronic structure of the O/Cu(001) system is governed by a competition between the hybridization of Cu1-$`d_{xz}`$ – O-$`p_x,p_y`$ and Cu1-$`d_{x^2y^2}`$ – O-$`p_z`$ states, which depends on O – Cu1 spacing. The anisotropy of the oxygen valence electron charge density is found to be strongly and non-monotonically dependent on the interlayer spacing.

Acknowledgements.

This work was supported by the National Science Foundation (Grant No CHE9812397). The calculations were performed on the Origin 2000 supercomputer at the National Center for Supercomputing Applications, University of Illinois at Urbana-Campaign under Grant No DMR010001N. The work of TSR was also facilitated by the award of an Alexander von Humboldt Forschungspreis.


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# Untitled Document

Magnetoexcitons in quantum-ring structures: a novel magnetic interference effect

S. E. Ulloaa, A. O. Govorova,b, A. V. Kalameitsevb, R. Warburtonc, and K. Karraid

a Department of Physics and Astronomy, and CMSS Program, Ohio University,

Athens, OH 45701, USA; ulloa@helios.phy.ohiou.edu

bInstitute of Semiconductor Physics, RAS, Siberian Branch, 630090 Novosibirsk, Russia

c Department of Physics, Heriot-Watt University, Edinburgh, UK

d Sektion Physik der Ludwig-Maximilians-Universität and Center for Nano-Science, Geschwister-Scholl-Platz 1, 80539 München, Germany

Abstract

A novel magnetic interference effect is proposed for a neutral, but polarizable exciton in a quantum ring with a finite width. The magnetic interference effect originates from the nonzero dipole moment in the exciton. The ground state of exciton acquires a nonzero angular momentum with increasing normal magnetic field. This leads to the suppression of the photoluminescence in defined windows of the magnetic field.

When a quantum particle moves along a closed trajectory in external electric and magnetic fields, the Aharonov-Bohm and Aharonov-Casher effects can occur, caused by quantum interference between paths with different phases. As is well known, the Aharonov-Bohm (AB) effect is related to a charged particle trajectory enclosing a magnetic flux. Here we present a novel magnetic interference effect for a neutral, but polarizable quasi-particle. In particular, we show here theoretically that the wave function of a neutral polarizable exciton acquires a nonzero phase when it moves in a quantum ring pierced by a magnetic flux. The neutral exciton wave function becomes sensitive to the magnetic flux because of a net radial electric-dipole moment induced by asymmetries in the nanostructure potential. The transition to a finite phase and corresponding orbital momentum in the polarized exciton state strongly changes the photoluminescence (PL) spectrum of the system due to the optical selection rules for interband transitions.

We demonstrate this novel magneto-interference effect using a model of InAs self-organized quantum rings (QR’s) . The calculated single-particle wave functions of electrons and holes are peaked at different radii due to the potential asymmetries and the difference in effective mass of the particles; meanwhile, their mutual interaction correlates their motion around the ring. The dipole polarization of the exciton can be strongly enhanced due to a point/impurity charge in the ring center, or by a voltage applied to a metal nano-gate in the middle of a ring. In that case, the potential minimum for the electron is shifted from that for the hole, and the ground state of the exciton acquires a finite polarization. To qualitatively demonstrate the effect, we use a model of two nested one-dimensional (1D) rings with different radii, one for the electron and one for the hole (insert of Fig. 1). For rings with relatively large radii, the motion of particles is strongly correlated, whereas, in a small system, the state is nearly single-particle–like, as the relative weight of the Coulomb interaction decreases with respect to the confinement energies.

Since the vertical size of a QR is typically much smaller than the lateral one, we will discuss only the in-plane motion. The electron and hole in-plane potentials are approximated by $`U_{e(h)}(\rho )=m_{e(h)}\mathrm{\Omega }_{e(h)}^2(\rho R_{e(h)})^2/2`$, where $`\rho `$ is the in-plane distance to the ring center, and $`m_{e(h)}`$, $`\mathrm{\Omega }_{e(h)}`$, and $`R_{e(h)}`$ are effective masses, characteristic frequencies, and ring radius, respectively; the indices $`e`$ and $`h`$ indicate the electron and hole quantities. In the vertical, $`z`$-direction, the motion is strongly quantized.

In a magnetic field, the Hamiltonian of an exciton confined in a quantum ring reads $`\widehat{H}=\widehat{T}_e+\widehat{T}_h+U_e+U_h+U_C(|𝐫_e𝐫_h|)`$, where $`𝐫_{e(h)}`$ are the in-plane coordinates, $`\widehat{T}_{e(h)}`$ are the kinetic energies in the presence of a normal magnetic field, and $`U_C`$ is the Coulomb potential. Now we assume that the quantization in the radial direction is stronger than that in the azimuthal direction. It allows us to separate variables in the wave function, $`\mathrm{\Psi }(𝐫_e,𝐫_h)=f_e(\rho _e)f_h(\rho _h)\psi (\varphi _e,\varphi _h)`$. Here $`𝐫=(\rho ,\varphi )`$. The radial wave functions $`f_{e(h)}`$ are strongly localized near the radii, $`R_{e(h)}`$. The Hamiltonian describing the wave function $`\psi (\varphi _e,\varphi _h)`$ is (up to a $`B`$-independent constant term),

$$\widehat{h}=\frac{\mathrm{}^2}{2m_eR_e^2}\frac{^2}{\varphi _e^2}\frac{i\mathrm{}\omega _e}{2}\frac{}{\varphi _e}\frac{\mathrm{}^2}{2m_hR_h^2}\frac{^2}{\varphi _h^2}+\frac{i\mathrm{}\omega _h}{2}\frac{}{\varphi _h}+\frac{m_e\omega _e^2R_e^2+m_h\omega _h^2R_h^2}{8}+u_C(|\varphi _e\varphi _h|),$$
(1)
where $`\omega _{e(h)}=|e|B/[m_{e(h)}c]`$ are the cyclotron frequencies of the particles, $`B`$ is the normal magnetic field, and $`u_c`$ is the Coulomb potential averaged over the coordinate $`\rho `$ involving the radial wave functions. By introducing new variables, we can rewrite Eq. 1 as $`\widehat{h}=\widehat{h}_0(\varphi _0)+\widehat{h}_1(\mathrm{\Delta }\varphi )`$, where $`\mathrm{\Delta }\varphi =\varphi _e\varphi _h`$, $`\varphi _0=(a\varphi _e+b\varphi _h)/(a+b)`$, and $`a=m_eR_e^2`$ and $`b=m_hR_h^2`$. Then, the eigenfunctions and eigenvalues can be found in the form of $`\psi (\varphi _e,\varphi _h)=\psi _0(\varphi _0)\psi _1(\mathrm{\Delta }\varphi )`$ and $`E=E_0+E_1`$, respectively. Here, the $`\widehat{h}_0`$ operator is given by $`\widehat{h}_0(\varphi _0)=\epsilon _0\left[i\frac{}{\varphi _0}+\frac{\mathrm{\Phi }_{\mathrm{\Delta }R}}{\mathrm{\Phi }_0}\right]^2`$, where $`M=(m_eR_e^2+m_hR_e^2)/R_0^2`$, $`R_0=(R_e+R_h)/2`$, $`\epsilon _0=\mathrm{}^2/(2R_0^2M)`$, $`\mathrm{\Phi }_0=hc/e`$, and $`\mathrm{\Phi }_{\mathrm{\Delta }R}=\pi (R_e^2R_h^2)B=2\pi \mathrm{\Delta }RR_0B`$ is the magnetic flux penetrating the area between the electron and hole trajectories (insert of Fig. 1); and $`\mathrm{\Delta }R=R_eR_h`$. The eigenvalues of $`\widehat{h}_0`$ are $`E_0(l)=\epsilon _0[l+\mathrm{\Phi }_{\mathrm{\Delta }R}/\mathrm{\Phi }_0]^2`$, where $`l`$ is an integer which represents the total angular momentum of the exciton.

The relative motion in the exciton is described by the operator $`\widehat{h}_1(\mathrm{\Delta }\varphi )`$, which involves the Coulomb potential. The limit of strong Coulomb interaction implies the condition $`R_0a_0^{}`$, where $`a_0^{}`$ is the exciton Bohr radius. In this limit, the wave function $`\psi _1(\mathrm{\Delta }\varphi )`$ is strongly localized near the point $`\mathrm{\Delta }\varphi =0`$ and the ground-state energy for $`l=0`$ can be written as $`E_1(n=0)=E_b2V\mathrm{cos}[2\pi \mathrm{\Phi }_{eff}/\mathrm{\Phi }_0]`$, where $`V`$ is the amplitude of tunneling from $`\mathrm{\Delta }\varphi =0`$ to $`\mathrm{\Delta }\varphi =2\pi `$, $`\mathrm{\Phi }_{eff}\pi R_0^2B`$, and $`E_b`$ is the energy of a state localized near the angle $`\mathrm{\Delta }\varphi =0`$; $`n`$ is the index of a quantum state . In the strong-interaction limit, the tunneling amplitude $`V`$ becomes exponentially small, and the magnetic field dispersion of the exciton energy comes mostly from the motion of a dipole. The lowest energy branches are $`E(l,n=0)=E_1(0)+E_0(l)E_b+E_0(l)`$.

In the opposite case of $`R_0a_0^{}`$, we can neglect the Coulomb interaction and solve Eq. 1 using the original variables. The energy spectrum reads

$$E(l_e,l_h)=\frac{\mathrm{}^2}{2m_eR_e^2}\left[l_e+\frac{\mathrm{\Phi }_e}{\mathrm{\Phi }_0}\right]^2+\frac{\mathrm{}^2}{2m_hR_h^2}\left[l_h\frac{\mathrm{\Phi }_h}{\mathrm{\Phi }_0}\right]^2,$$
(2)
where $`\mathrm{\Phi }_{e(h)}=\pi R_{e(h)}^2B`$, and $`l_{e(h)}`$ are electron (hole) angular momenta.

In Figs. 1 and 2 we show the energy spectra and the PL intensity of an exciton in a QR (notice that $`E_{exc}=E_{gap}+E`$, where $`E_{gap}`$ is the semiconductor gap energy). For the strong-Coulomb-interaction limit (Fig. 1), we show the lowest states with $`n=0`$ and $`l=0,\pm 1,\pm 2,\mathrm{}`$, where $`l`$ is the total angular momentum of the exciton. We see that the ground-state momentum changes with increasing magnetic field from $`l=0`$ to $`l=1,2,\mathrm{}`$, according to the equation for $`E_0(l)`$. This arises as the electron and hole acquire different magnetic phases when they move along different closed trajectories (insert of Fig. 1). In the case of weak Coulomb interaction, the character of ground-state transitions in a magnetic field is a bit more complicated. The ground state $`(l_e,l_h)=(0,0)`$ changes to the states $`(1,0)`$, $`(1,+1)`$, $`(2,+1)`$, etc., as the field increases. The total momentum of the ground state, $`l=l_e+l_h`$, changes correspondingly.

According to the selection rules for optical transitions between the conduction and valence bands, only the zero-momentum excitons can emit a photon. At low temperatures, a photo-generated exciton relaxes within a short time to its ground state. Thus, in many cases the PL spectrum demonstrates mostly the line related to the ground state of an exciton. With increasing magnetic field, the exciton in its ground state acquires nonzero momentum and can not longer radiate. The darkness of the exciton in the ground state is seen as a suppression of the calculated PL in the magnetic-field intervals with the ground-state total momentum $`l=l_e+l_h0`$. The PL intensity shown in Fig. 2 was calculated from the relation $`I_{PL}(B)P(l=0,T)`$, where $`P(l=0,T)`$ is the probability to find an exciton in the states with $`l=0`$ at finite temperature $`T`$ . For the spacing $`\mathrm{\Delta }R`$ we have chosen $`2030`$ Å. As an example, an impurity charge $`+|e|`$ in the middle of a ring having $`R_0=85`$ Å, $`\mathrm{}\mathrm{\Omega }_e=35meV`$, and $`\mathrm{}\mathrm{\Omega }_h=25meV`$, induces a shift $`\mathrm{\Delta }R20`$Å. A similar $`\mathrm{\Delta }R`$ is obtained for the ring parameters of the system studied in Ref. .

A similar AB effect for a neutral exciton can occur in (spatially-indirect) type-II quantum dot embedded in a 2D quantum well . In such a system, the electron can move in a quantum-ring potential due to the joint action of the Coulomb force and the quantum-dot potential. This type-II geometry would correspond to that of GaSb/GaAs quantum dots, for example . Similarly, confinement asymmetries in a ring arising from mass differences or effective potential profiles could also give rise to a finite polarization of the exciton ground state. The details of the system would determine the strength of the magnetic field sensitivity such as shown in the figures.

It is important to emphasize that the predicted effect depends on the magnetic flux $`\mathrm{\Phi }_{\mathrm{\Delta }R}`$ through the area between the electron and hole trajectories (insert of Fig. 1) and does not include an exponentially-small factor due to electron-to-hole tunneling along the ring. This is in contrast to the AB effect for excitons in a 1D ring described recently in the literature . This difference would make the experimental detection of the effect discussed here much more likely. As single-dot spectroscopy  permits one to observe the PL energies with very high accuracy, it would be a suitable method to study the predicted magnetic-field interference effects.

Acknowledgements. We gratefully acknowledge financial support by Ohio University through the Rufus Putnam Visiting Professorship, by the Volkswagen-Foundation, the RFBR (Russia), and the US Department of Energy grant no. DE–FG02–87ER45334.

References

Figure captions
Fig.1 a) The energy spectrum and PL intensity of excitons confined in a quantum ring as a function of the normal magnetic field for the strong-Coulomb-interaction limit; here, $`m_e=0.07m_0`$ and $`m_h=0.2m_0`$. Insert: a sketch of the quantum ring system.
Fig.2 b) The energy spectrum and PL intensity of excitons confined in a quantum ring as a function of the normal magnetic field in the limit of weak Coulomb interaction.


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# Gravitational radiation from the 𝑟-mode instability

## 1 Introduction

This paper contains a portion of the material presented by Lee Lindblom in the talk “Relativistic Instabilities in Compact Stars” at the Fourth Amaldi Conference on Gravitational Waves. Most of the material presented in that talk has already been published, and so we limit our discussion here to that material which has not previously appeared in print. We direct those readers who might be interested in the wider range of subjects covered in the talk to the recent review Lindblom (2001), and the recent papers Lindblom, Tohline and Vallisneri (2001b) and Lindblom and Owen (2001).

Gravitational radiation (GR) is a de-stabilizing force on the $`r`$-modes of rotating neutron stars (Andersson 1998, Friedman and Morsink 1998). The first estimates of the timescales associated with this instability (Lindblom, Owen and Morsink 1998) showed that the GR driving force is much stronger than the stabilizing effects of the simplest forms of viscous dissipation in neutron stars. As a consequence there has been a great deal of interest in this instability as a potential source of observable GR, and as a mechanism for removing angular momentum from rapidly rotating neutron stars. During the past several years the effects of a number of additional dissipation mechanisms on the $`r`$-mode instability have been studied in some detail. A number of these mechanisms are much more effective in suppressing the $`r`$-mode instability than the simple viscosity considered in the initial estimates. In particular the effects of a solid crust (Bildsten and Ushomirsky 2000, Lindblom, Owen and Ushomirsky 2000, Wu, Matzner and Arras 2001), the effects of magnetic fields (Rezzolla, et al2001a, 2001b, Mendell 2001), the non-linear effects of mode-mode coupling (Schenk, et al2001), and the effects of hyperon bulk viscosity (Jones 2001a, 2001b, Lindblom and Owen 2001) make it appear less likely that the GR instability in the $`r`$-modes will play an interesting role in astrophysics. However, at the present time none of these mechanisms is understood well enough for us to conclude absolutely that the $`r`$-mode instability will never play a role in any neutron stars. Thus for the purposes of the present paper, we assume that the instability will occur in some rapidly rotating neutron stars. Our aim here is to present the best estimate of the GR that might be emitted during such an instability. To do this we analyze the GR emitted by the best currently available numerical simulation of the non-linear evolution of the $`r`$-mode instability. This paper is an update of the initial estimates of the GR emitted by the $`r`$-mode instability given by Owen, et al(1998).

## 2 r-Mode Evolution Model

We base our estimates of the GR produced by the non-linear evolution of an unstable $`r`$-mode, on the numerical simulations by Lindblom, Tohline and Vallisneri (2001a, 2001b). The evolution of a small amplitude $`m=2`$ $`r`$-mode subject to the current-quadrupole GR reaction force was studied numerically in a $`1.4M_{}`$ polytropic neutron star rotating at about 95% of its breakup angular velocity. Figure 1 illustrates the evolution of the current quadrupole moment $`|J_{22}|`$ (in cgs units) of this model as the simulation evolves. The current quadrupole moment is defined as

$$J_{22}=\rho r^2\stackrel{}{v}\stackrel{}{Y}_{22}^Bd^{\mathrm{\hspace{0.17em}3}}x,$$
(1)
where $`\rho `$ and $`\stackrel{}{v}`$ are the density and velocity of the fluid in the star, and $`\stackrel{}{Y}_{22}^B`$ is the magnetic type vector spherical harmonic (Thorne 1980). The time displayed along the horizontal axis of Fig. 1 is given in units of the initial rotation period of the star: $`P_0=1.18`$ms. During the first part of the evolution GR drives the growth of the $`r`$-mode, leading to the exponential growth in $`J_{22}`$ illustrated here. Once the amplitude of the mode becomes sufficiently large, however, non-linear hydrodynamic processes also become important. These lead to large surface waves which break and shock (see Lindblom, Tohline and Vallisneri 2001a, 2001b). The dissipation in these shocks damps the $`r`$-mode and leads to the rapid decrease in $`J_{22}`$ following its peak.

The timescale of the GR instability in the $`r`$-modes is much much longer than the hydrodynamic timescale. To perform the numerical simulation illustrated in Fig. 1 it was necessary to increase artificially the strength of the GR driving force so that the instability could proceed more rapidly. Fortunately tests have shown (see Lindblom, Tohline and Vallisneri 2001b) that the maximum amplitude which the $`r`$-mode achieves (and hence the maximum value of $`J_{22}`$) is relatively insensitive to the strength of the GR driving force. The amplitude grows until the velocities in the mode reach some critical value before the waves break and shock. The value of this critical velocity appears to be relatively insensitive to how rapidly the fluid velocity is increased to this critical level.

To determine the GR signal that would be emitted by the growth of an unstable $`r`$-mode, it is necessary to re-scale the time in the simulation. The early part of the simulation has been designed to proceed more rapidly than the physical case by the factor $`\tau _{GR}(\mathrm{physical})/\tau _{GR}(\mathrm{simulation})`$, where $`\tau _{GR}`$ represents the GR growth timescale of the instability. This ratio has the value 4488 in the simulation used here. Thus the early exponential growth phase of a physical $`r`$-mode evolution will last longer than this phase of the simulation by this factor. The late stages of the simulation are dominated by hydrodynamic forces which damp the $`r`$-mode within a few rotation periods. This final stage of the evolution therefore proceeds at the same rate in both the physical and the simulation cases. We (somewhat artificially) choose the dividing time between the early and late stages of the evolution to be the time at which the value of $`|J_{22}|`$ is maximum.

The time dependence of $`J_{22}`$ is found in the simulation to be nearly sinusoidal with a time dependent amplitude, $`J_{22}=|J_{22}|e^{i\psi (t)}`$, (with $`d\psi /dt=\omega `$ constant) because $`J_{22}`$ is dominated by the unstable $`r`$-mode in this case. The time dependence of $`|J_{22}|`$ is illustrated in Fig. 1. The frequency of the sinusoidal time dependence is conveniently determined numerically using the formula

$$\omega =\frac{1}{|J_{22}|}\left|\frac{dJ_{22}}{dt}\right|.$$
(2)
This approximation introduces errors of order $`(\omega \tau _{GR})^12\%`$ in our simulation. Figure 2 illustrates the evolution of the frequency, $`f=2\pi \omega `$, determined numerically in this way. Here we plot the frequency as a function of the re-scaled physical time (in seconds). We note that the frequency changes by only a few percent during the course of the evolution in which about 40% of the angular momentum of the star is radiated away as GR.

In general relativity theory an isolated object with time dependent current quadrupole moment radiates GR. The expression for the dimensionless GR amplitude $`h`$ (averaged over possible source and detector orientations) is given by

$$h(t)=\frac{16}{15}\sqrt{\frac{2\pi }{5}}\frac{\omega ^2G|J_{22}|}{c^5D}e^{i\psi (t)},$$
(3)
where $`G`$ and $`c`$ are Newton’s constant and the speed of light, and $`D`$ is the distance to the source. Figure 3 illustrates the time dependence of this dimensionless GR amplitude as a function of time as determined by the simulation. Since the frequency of these $`r`$-mode oscillations is essentially constant, the GR amplitude just grows in proportion to $`J_{22}`$. Once the amplitude peaks, non-linear hydrodynamic forces (i.e. shocks) quickly damp the mode and this is reflected in the sharp drop in $`h`$ (as a function of physical time) illustrated in Fig. 3. We have chosen $`D=20`$Mpc, the distance to the Virgo Cluster of galaxies, for the purposes of the illustration. Optimistic estimates of the event rate for these objects suggests that the nearest events expected during the time frame of the LIGO observations will be at this distance.

## 3 Optimal S/N

The optimal signal to noise ratio ($`S/N`$) for detecting a GR signal can be achieved with the use of an optimal filter, consisting of a template that matches the waveform of the signal. Let $`\stackrel{~}{h}`$ denote the Fourier transform of the GR signal:

$$\stackrel{~}{h}(f)=_{\mathrm{}}^{\mathrm{}}h(t)e^{2\pi ift}𝑑t.$$
(4)
The discrete Fourier transform of the gravitational wave signal from our numerical simulation is shown in Fig. 4. Here we have smoothed the resulting $`|\stackrel{~}{h}(f)|^2`$ with a windowing function of width $`0.5`$Hz. We see that the spectrum of the gravitational radiation is confined essentially to the band $`940f980`$Hz, which corresponds well with the evolution of the frequency of the $`r`$-mode as shown in Fig. 2. For a complex signal $`h(t)`$ the optimal value of $`S/N`$ is given by

$$\left(\frac{S}{N}\right)^2=2_0^{\mathrm{}}\frac{|\stackrel{~}{h}(f)|^2df}{S_h(f)},$$
(5)
where $`S_h(f)`$ is the one-sided power spectral density of detector noise. (For a real signal the 2 becomes a 4.) We approximate $`S_h(f)`$ for frequencies near $`960`$Hz by the Taylor expansion

$$S_h(f)S+S^{}\mathrm{\Delta }f+0.5S^{\prime \prime }(\mathrm{\Delta }f)^2,$$
(6)
where $`\mathrm{\Delta }f=f960`$Hz, and the three constants $`S`$, $`S^{}`$ and $`S^{\prime \prime }`$ are listed in Table 1 for three plausible LIGO II design options (see Buonanno and Chen 2001). Using these values for $`S_h`$ we find $`S/N1.2`$, 4.0 and 10.4 by performing the integral in Eq. (5) numerically for these three possible LIGO II configurations.

We can also make an analytical estimate of the optimal $`S/N`$ using an extension of a very general argument given originally by Blandford (1984, unpublished). For GR emitted by a multipole with azimuthal quantum number $`m`$ the angular momentum loss rate is

$$\frac{dJ}{dt}=\frac{5m\pi c^3}{2G}fD^2|h(t)|^2,$$
(7)
where $`|h(t)|^2`$ has been averaged over all possible orientations of source and detector (and over several wave periods for the case of a real signal). When a function such as $`h(t)`$ involves a rapid oscillation together with a much slower evolution of its amplitude and frequency, the Fourier transform $`\stackrel{~}{h}(f)`$ is well approximated by the stationary phase approximation,

$$|h(t)|^2=|\stackrel{~}{h}(f)|^2\left|\frac{df}{dt}\right|$$
(8)
for a complex signal $`h(t)`$. (For a real signal, the left-hand side is averaged over several periods and the right-hand side is multiplied by 2.) Since the angle-averaging affects both sides of Eq. (8) equally, we can use Eqs. (7) and (8) to re-express $`S/N`$ for a source at an “average” orientation from Eq. (5) as

$$\left(\frac{S}{N}\right)^2=\frac{4G}{5m\pi c^3D^2}\frac{dJ}{fS_h(f)}.$$
(9)
For GR sources such as the $`r`$-mode evolution the frequency of the radiation emitted is nearly constant, so $`fS_h(f)`$ can be treated as being essentially constant in Eq. (9). Thus, this integral becomes just the total amount of angular momentum $`\left|\mathrm{\Delta }J\right|`$ radiated away as GR:

$$\left(\frac{S}{N}\right)^2=\frac{4G}{5m\pi c^3D^2}\frac{\left|\mathrm{\Delta }J\right|}{fS_h(f)}.$$
(10)
The total amount of angular momentum radiated away as GR in the simulation was $`|\mathrm{\Delta }J|4.5\times 10^{48}`$ in cgs units. Using this value in Eq. (10) together with the values of $`S_h`$ from Eq. (6) and Table 1, we find $`S/N1.4`$, 4.5, and 12.0 in good agreement with our previous estimate based on the discrete Fourier transform and direct integration of the simulation waveform. We note that this argument can easily be extended to signals composed of multiple harmonics and multipoles so long as their frequencies are well-defined: Time-averaging of Eq. (8) eliminates cross-terms, so Eq. (10) is simply summed over each harmonic and $`m`$. We can also extend the argument to non-monotonically evolving frequencies by using Eq. (8) to express Eq. (5) as an integral over time and dividing $`f(t)`$ into piecewise monotonic parts.

It is not unreasonable to think that a realistic data analysis strategy could come within a factor of 2 of the optimal $`S/N`$. Due to the complexity of the physics involved it seems unlikely that matched filtering will ever be a viable option. However, cross-correlation of the output of two aligned interferometers (LIGO Hanford and LIGO Livingston) can in principle achieve $`1/\sqrt{2}`$ of optimal $`S/N`$ if the detectors’ noise is of comparable strength and uncorrelated—including non-Gaussian noise bursts (Anderson et al2001). This strategy relies on the supernova associated with the $`r`$-mode having been observed optically, allowing the appropriate time delay to be inserted between the interferometer data streams. Narrowing the search to a few minutes after the supernova (instead of continuous operation) also has the effect of greatly reducing the $`S/N`$ threshold for detection with reasonable false alarm statistics. Thus a cross-correlation with $`S/N4`$ might be considered enough for detection, implying a realistically detectable distance for $`r`$-modes of 5 Mpc for even the least optimal (for this type of source) LIGO II configuration—and up to 50 Mpc for the most optimal.

We thank Joel Tohline and Michele Vallisneri for allowing us to use the results of the non-linear $`r`$-mode simulations, Alessandra Buonanno for providing us with the latest LIGO II noise curves, and Jolien Creighton for conversations on data analysis. We also thank Kip Thorne for helpful comments and suggestions. This research was supported by NSF grants PHY-9796079, PHY-0071028, PHY-0079683, and PHY-0099568, and NASA grants NAG5-4093 and NAG5-10707.

## References