text:
# Evidence for non-linear quasiparticle tunneling between fractional quantum Hall edges

## Abstract

Remarkable nonlinearities in the differential tunneling conductance between fractional quantum Hall edge states at a constriction are observed in the weak-backscattering regime. In the $`\nu `$ = 1/3 state a peak develops as temperature is increased and its width is determined by the fractional charge. In the range $`2/3\nu 1/3`$ this width displays a symmetric behavior around $`\nu `$ = 1/2. We discuss the consistency of these results with available theoretical predictions for inter-edge quasiparticle tunneling in the weak-backscattering regime.

Under the application of intense perpendicular magnetic fields, the kinetic energy spectrum of the two dimensional electron gas (2DEG) becomes quantized and breaks into a sequence of macroscopically degenerate Landau levels. The properties of electron states in this regime are largely driven by Coulomb interactions. At some “magic” fractional values of the filling factor $`\nu `$, in particular, the 2DEG condenses into collective phases: the fractional quantum Hall (FQH) effect is the most remarkable fingerprint of such incompressible quantum fluids aron ; prange . Laughlin showed laug  that the emergence of such collective states implies the existence of new quasiparticles carrying fractional charge. Additionally, at the strong magnetic fields characteristic of the FQH effect the lowest-energy charged excitations are confined at the edge of the sample in one-dimensional branches whose excitations are forced to propagate only in one direction. Wen Wen1  was the first to describe such one-dimensional modes in terms of a chiral Luttinger liquid. Wen’s proposal stimulated a considerable amount of work aimed at understanding the properties of this non-Fermi liquid state kane .

The departure from the Fermi-liquid behavior is predicted to show up in many properties of an interacting one-dimensional system kane92 . Most of the experiments in quantum Hall systems concentrated on the observation of the power-law behavior of the electron tunneling from a metal to the FQH edge chang1 ; chang2 ; Grayson  and between two FQH edges Milliken ; glattli  in the strong backscattering limit. Resonant tunneling in this regime was also explored Grayson2 . The inter-edge tunneling process, in particular, can be experimentally induced at a quantum point contact (QPC) constriction. In the strong backscattering regime one observes the tunneling of electrons between two quantum Hall fluids separated by the QPC. For simple fractions (i.e. $`\nu =1/q`$, where $`q`$ is an odd integer), this leads to a dc tunneling current at temperature T=0 given by $`I_TV_T^{(2/\nu 1)}`$. Notably $`I_T`$ vanishes when the bias voltage $`V_T`$, with $`V_T`$ labeling the potential difference between the two edges, tends to zero kane .

In the opposite limit of weak backscattering the quantum Hall fluid is weakly perturbed by the QPC constriction. In this case the inter-edge tunneling current (again, at $`\nu =1/q`$) consists of Laughlin quasiparticles of charge $`e^{}=\nu e`$ that scatter between the edges through the quantum Hall fluid (see Fig.1 panel $`(a)`$). At T=0 the quasiparticle tunneling rate is predicted to grow at low voltages as $`I_TV_T^{(2\nu 1)}`$ in contrast to the electron-tunneling case discussed above. This remarkable nonlinear behavior is removed at finite temperature. When $`V_T`$ falls below a critical value $`V_{T,max}`$ of the order of $`k_BT/e^{}`$, the tunneling current reverts to the linear ohmic behavior $`I_TV_T`$. In the differential tunneling characteristics ($`dI_T/dV_T`$) this leads to a peak centered at $`V_T=0`$ with a width $`\mathrm{\Delta }V_T2V_{T,max}`$. This phenomenology was first predicted by Wen Wen  who showed, in particular, that the width of the finite-temperature peak is related to the fractional charge of the quasiparticle. The complex phenomena associated to non-linear quasiparticle tunneling, however, are still largely experimentally unexplored. During recent years magneto-transport experiments in the weak backscattering regime were reported and concentrated on shot noise measurements aimed at detecting the fractional charge of the quasiparticle noise .

In this Letter we report the observation of non-linear inter-edge tunneling in the weak backscattering regime. We present the differential tunneling conductance as a function of bias voltage in a wide range of temperatures and filling factors. In the FQH regime our data cannot be described by electron tunneling but display the features of Wen’s theory of quasiparticle tunneling. We demonstrate that while the differential tunneling characteristic shows the tendency towards a diverging behavior as the temperature is lowered at $`\nu =1/3`$, it develops a peak centered at $`V_T`$ = 0 as the temperature is increased. Width and shape of this zero-bias peak are determined by the fractional charge of the quasiparticle, consistently with Wen’s predictions. We also discuss the results obtained for filling factors between $`\nu `$ = 2/3 and $`\nu `$ = 1/3 where the zero-bias peak is observed even at the lowest probed temperature of 30 mK. Finally, we show that the evolution of the width of the differential conductance peak displays an unexpected symmetry around $`\nu `$ = 1/2 not explained by current theories. We believe that these results combine to provide the first evidence of non-linear quasiparticle tunneling in FQH systems.

The devices here studied were realized starting from a high-mobility GaAs/Al0.3Ga0.7As two-dimensional electron gas (2DEG) with low-temperature mobility $`\mu 1\times 10^6\mathrm{cm}^2/\mathrm{Vs}`$ and two-dimensional electron density $`n5\times 10^{10}\mathrm{cm}^2`$. The 2DEG was located $`140\mathrm{nm}`$ from the surface. The measurements discussed below were preformed in a dilution refrigerator. The QPC constriction was nanofabricated on Hall-bar mesas (width of 80 $`\mu m`$) using e-beam lithography and Al metallization. The width and length of the QPC constriction were $`300\mathrm{nm}`$ and $`600\mathrm{nm}`$, respectively.

Differential inter-edge tunneling conductance as a function of bias voltage $`V_T`$ was controlled by exploiting the QPC (see Fig.1 panel $`(a)`$) in order to force edge states to flow close to each other in the constriction. In the measurements presented here the split-gate was biased at $`V_g=0.4\mathrm{V}`$ which is just below the 2DEG depletion leading to 2D-1D threshold at zero magnetic field. At these bias conditions therefore the conduction takes place through the point contact only. This ensures that edge states indeed propagate inside the QPC while they are still separated enough to avoid strong interactions. A current $`I`$ with both dc and ac components was supplied to the Hall bar. This current causes a Hall voltage drop $`V_H=\rho _{xy}I`$ (with dc and ac components) between the counter-propagating edge channels within the constriction footnote1 . In the weak backscattering regime $`V_H`$ coincides with the tunneling bias i.e., $`V_T=V_H`$. Four-wire differential-resistance measurements were carried out using an ac lock-in technique (see Fig.1 panel $`(a)`$) with $`0I_{dc}45`$ nA and $`I_{ac}`$ = 250 pA. The latter value was chosen in order to have an acceptable signal-to-noise ratio without introducing unphysical nonlinearities in the tunneling current. The quantity that is measured in our configuration is the resistivity drop at the constriction (the differential longitudinal resistance $`dV/dI`$). In the weak backscattering regime $`dV/dI`$ is directly related to the differential tunneling conductance by:

$$dV/dI=\rho _{xy}^2dI_T/dV_T.$$
(1)
The presence of residual backscattering outside the constriction leads to a background signal superimposed to (1). In the present devices this background is significant at $`\nu =1/3`$. Even away from the constriction the longitudinal resistivity is around $`4k\mathrm{\Omega }`$, i.e. about $`30\%`$ of the value measured at the constriction in the bias range of interest for the weak backscattering regime. However it does not display a sizeable variation as a function of the tunneling bias (data not shown) at least for low values of the tunneling bias. This and additional control experiments carried out at lower values of $`V_g`$ allow us to unambiguously attribute the observed structures in $`dV/dI`$ to quasiparticle tunneling at the QPC.

Panel $`(b)`$ in Fig.1 shows the longitudinal resistance $`\rho _{xx}`$ at $`I_{dc}=0`$ as a function of magnetic field at $`V_g`$ = -0.4 V. This measurement displays Shubnikov-de-Haas oscillations associated to the quantum Hall states in the presence of the constriction. At $`I_{dc}0`$ marked nonlinearities are observed in the FQH regimes. An example is reported in the main panel of Fig.1 where two representative differential conductance curves at filling factors $`2`$ and $`1/3`$ are shown. As expected, the behavior in the integer regime is linear even at the lowest temperatures explored. In order to emphasize the differences observed in the fractional regime, the marked nonlinear behavior measured in the case $`\nu `$ =1/3 is shown at the comparatively high temperature of T = 400mK.

Figure 2 (panel a) shows the temperature evolution at $`\nu =1/3`$ for temperatures up to 900 mK. At this FQH state, the lowest-temperature curve (at 30 mK) shows a minimum at zero bias. The zero-bias peak, however, is recovered at higher temperatures. It develops above $`400\mathrm{mK}`$ and tends to disappear as temperature is increased above $`900\mathrm{mK}`$. We can understand the data in Fig. 2 in the framework of the weak-backscattering theory for inter-edge tunneling originally proposed by Wen Wen . We recall that in the weak-backscattering regime the constriction is a small perturbation for edge-state propagation and induces a limited and localized backscattering. This limit can be quantified comparing the tunneling current ($`I_T`$) to the total current ($`I`$) flowing through the device. We define the scattering to be weak when $`I_TI`$ (this condition could also be stated as $`dV/dIh/\nu e^275k\mathrm{\Omega }`$). In this regime we expect,

$`I_T\left(V_T\right)={\displaystyle \frac{2\pi \left|t\right|^2}{\mathrm{\Gamma }(2g)}}\left|{\displaystyle \frac{2\pi T}{T_0}}\right|^{2g1}\left|\mathrm{\Gamma }\left(g+{\displaystyle \frac{ix}{2\pi }}\right)\right|^2\mathrm{sinh}\left({\displaystyle \frac{x}{2}}\right),`$ (2)
where $`g=e^2/\nu e^2`$, $`x=e^{}V_T/k_BT`$, $`\mathrm{\Gamma }`$ is the Euler Gamma-function, and $`t`$ is the inter-edge tunneling amplitude. Note that in Wen’s original theory the chiral Luttinger liquid was assumed to exist only at the filling factors of the fractional quantum Hall effect. In (2) however, the filling factor $`\nu `$ is allowed to vary continuously. Such an extension of the original formulation can be justified on the basis of a hydrodynamic model, which allows us to derive a continuum of Luttinger liquids with continuously varying $`\nu `$ Dagosta .

The behavior of $`I_T`$ depends crucially on the relative size of $`e^{}V_T`$ and $`k_BT`$. At low temperatures (2) predicts the nonlinear behavior $`I_TV_T^{2g1}`$, which, for $`g<1/2`$, leads to a growing current with decreasing bias: this is the signature of the overlap catastrophe. At higher temperatures (2) predicts an ohmic behavior $`I_TV_T`$. The crossover between the two regimes occurs at $`V_T=V_{T,max}`$, where $`I_T`$ reaches a maximum. Figure 2 (panel $`b`$) shows the calculated differential tunneling conductance (the derivative of (2)) at $`\nu =1/3`$ ($`g=1/3`$) at different temperatures. The peak at zero bias arises from the ohmic region of the $`I_TV_T`$ relation. As the temperature lowers this peak is expected to grow in intensity without saturation and to shrink in size. Indeed the width of this peak (defined here as the distance between the two zeroes of the differential conductance) is $`2V_{T,max}4.79k_BT/e^{}`$ and is directly related to the effective charge of the quasiparticle involved in the tunneling process Wen . For $`V_T>V_{T,max}`$ the differential conductance becomes negative, and eventually tends to zero as $`V_T^{2g1}`$.

Figure 2 (panel $`c`$) reports the experimental results obtained for temperatures higher than $`400\mathrm{mK}`$. The tunneling conductance in this range of temperatures is characterized by a zero bias enhancement and the observed overall trend is in good agreement with the calculated behavior shown in Fig.2 (panel $`b`$) and discussed above. The agreement is particularly satisfactory for what concerns the width of the conductance peak. At higher temperatures the peak broadens and its amplitude decreases following qualitatively the theory. At temperatures higher than $`1K`$ the tunneling is completely linear in this voltage range. The data also show evidence of a negative contribution to the tunneling conductance at larger values of the bias voltage: again this is in qualitative agreement with the theory although the large background rises the average value of the conductance above zero.

At temperatures lower than $`400\mathrm{mK}`$ (see Fig.2, panel $`a`$), however, a crossover to a completely different behavior is observed. The tunneling conductance exibits a minimum at zero bias. The disappearance of the peak can be related to its progressive shrinking with temperature: for a given current modulation intensity a threshold temperature can be estimated below which the peak cannot be detected. In the weak backscattering limit $`V_{T,ac}\rho _{xy}I_{ac}0.02mV100\mathrm{mK}`$. This value is not in agreement with our experimental finding and suggests that the system by lowering the temperature may evolve into the strong backscattering regime nota28 . A further mechanism for the zero-bias suppression can be associated to negative interference between spatially separated tunneling events within the QPC constriction. This effect gets stronger with decreasing temperature and can contribute to the suppression at zero bias chamon .

Next we examine the dependence of tunneling current on filling factor. Experimental results are summarized in the color plots of Fig.3 for different temperatures (here higher values of the tunneling conductance are in yellow, lower values in black). The measured $`I_TV_T`$ relation was linear at integral filling factor (data not shown) and for temperatures above 900 mK. Otherwise, above 400 mK, the zero-bias peak is visible in the whole range $`1/3\nu 2/3`$, and presents an interesting evolution: the peak is strongest and narrowest at $`\nu =1/3`$ and $`\nu =2/3`$ (the two most prominent QHE fractions) and rapidly broadens and loses its strength as $`\nu =1/2`$ is approached from either side. Notably its width evolves symmetrically about $`\nu =1/2`$. This is shown in more detail in Fig.4 where the differential tunneling conductance is plotted at three representative values of the magnetic field. The inset of Fig.4 reports the width of the zero-bias peak as a function of magnetic field at T=400 mK (filled circles) and T = 500 mK (open circles). A similar behavior was found also at T = 700 mK (data not shown).

At the moment, a convincing theory of this is not available. Equation 2 is not particle-hole symmetric under any reasonable assumption. Setting $`g=\nu `$ yields a tunneling conductance curve with a peak at zero bias: however the width of the peak increases monotonically with $`\nu `$, while its amplitude decreases. It should be pointed out that, at $`\nu =2/3`$ (and more generally at filling factors of the Jain sequence $`np/(np+1)`$), the result of (2) with $`g=\nu `$ is in agreement with the weak backscattering theory of composite edge states developed by Kane and Fisher aron . Finally, we should like to point out that also the width of the zero-bias peak observed at $`\nu >1/3`$ and low temperature is not compatible with (2). One is tempted to associate the non-monotonic behavior of the peak with the different structure of the zero-temperature fixed points controlling the charge mode for the Jain sequences with positive and negative $`p`$. However, additional theoretical analysis of quasiparticle tunneling at non-quantized filling factor values is needed footnote2 .

In conclusion, we reported a marked non-linear behavior in the inter-edge tunneling in the fractional quantum Hall regime in the weak-backscattering limit. The observation of a zero-bias peak in the differential tunneling conductance has been interpreted as evidence for quasiparticle tunneling between fractional edge states. In selected ranges of temperatures and filling factors our data are consistent with Wen’s theory of quasiparticle tunneling. Results as a function of filling factors reveal intriguing feautures not predicted by currrent theories.

We acknowledge R. D’Agosta, M. Grayson and V. Piazza for useful discussions. This work was supported in part by INFM


format: text

text:
# Evidence for Unconventional Strong-coupling Superconductivity in PrOs4Sb12 : An Sb Nuclear Quadrupole Resonance (NQR) Study

## Abstract

We report Sb-NQR results which evidence a heavy-fermion (HF) behavior and an unconventional superconducting (SC) property in the filled-skutterudite compound PrOs4Sb12 revealing a SC transition temperature $`T_c=1.85`$ K. The temperature ($`T`$) dependence of nuclear-spin-lattice-relaxation rate $`1/T_1`$ and NQR frequency unravel a low-lying crystal-electric-field splitting below $`T_010`$ K, associated with Pr3+($`4f^2`$)-derived ground state. The emergence of $`T_1T`$=const. behavior below $`T_F4`$ K points to the formation of heavy-quasiparticle state. In the SC state, $`1/T_1`$ shows neither a coherence peak nor a $`T^3`$like power-law behavior observed for HF superconductors to date. The isotropic energy-gap with a size of gap $`\mathrm{\Delta }/k_B=4.8`$ K begins to already open up at $`T^{}`$ 2.3 K without any coherence effect just below $`T_c=1.85`$ K. We highlight that the superconductivity in PrOs4Sb12, which is in an unconventional strong-coupling regime, differs from a conventional s-wave type and any unconventional ones with the line-node gap.

preprint: PrOsSb

A class of Ce- and U-based intermetallic compounds reveal a crossover from high-temperature localized to low-temperature heavy-fermion (HF) state in which $`f`$ electrons are delocalized with enormous effective mass, and are remarkable to undergo an unconventional superconducting (SC) transition with line-node gap, indicative of the Cooper pairing of heavy fermions with an angular momentum greater than zero. It is widely believed that the superconductivity in these materials is mediated by magnetic fluctuations.

Recently, the HF-like behavior or a quadrupolar ordering has been reported in PrInAg2 Yatskar  and PrFe4P12 Sugawara ; Matsuda ; Aoki ; Nakanishi  and PrPb3 Bucher ; Morin ; DAoki ; Tayama . In these compounds, the ground state of a Pr3+ with $`4f^2`$ in a crystal electric field (CEF) scheme is believed to be the $`\mathrm{\Gamma }_3`$ nonmagnetic doublet with the electric quadrupolar moments for a total angular momentum $`J=4`$ state. The quadrupolar moments interact with the charges of conduction electrons, leading to the HF-like behavior or the quadrupolar ordering in these Pr-based compounds. In fact, PrPb3 shows an antiferro-quadrupolar ordering in the $`\mathrm{\Gamma }_3`$ ground state at 0.4 K Bucher ; Morin ; DAoki ; Tayama . In PrInAg2, a broad peak in specific heat is identified as a Kondo anomaly, having an enhanced electronic specific heat coefficient $`\gamma 6.5\mathrm{J}/\mathrm{molK}^2`$ Yatskar . Likewise, the filled-skutterudite compound PrFe4P12 shows the HF-like behavior with a large mass of $`m^{}70m_e`$ Sugawara  under a magnetic field and undergoes an anomalous transition at 6.4 K at zero field, indicative of a quadrupolar ordering Matsuda ; Aoki ; Nakanishi . Note that the large values in $`C/T`$ for these compounds are not always ascribed to such low-energy degrees of freedom as either magnetic or quadrupolar fluctuations, but also to the Schottky anomaly originating from some low lying CEF splitting.

Meanwhile, Bauer et al. reported the observation of HF behavior and superconductivity at $`T_c=1.85`$ K in the filled-skutterudite compound PrOs4Sb12 that is the first case of Pr-based HF superconductor Bauer . Its HF state was inferred from the jump in the specific heat at $`T_c`$, the slope of the upper critical field near $`T_c`$, and the electronic specific heat coefficient $`\gamma 350500`$ mJ/mole K2. The magnetic susceptibility, thermodynamic measurements, and recent inelastic neutron scattering experiments revealed the ground state of the Pr3+ ions in the cubic CEF to be the $`\mathrm{\Gamma }_3`$ nonmagnetic doublet Bauer ; Woodward . In the Pr-based compounds with the $`\mathrm{\Gamma }_3`$ ground state, the quadrupolar interactions play important role. In analogy with the quadrupolar Kondo model Cox , it was suggested that the HF-like behavior exhibited by PrOs4Sb12 may be relevant to a quadrupolar Kondo lattice. An interesting issue to be addressed is what role of Pr3+-derived quadrupolar fluctuations are relevant with the onset for the superconductivity in this compound.

In this letter, we report the observation of unconventional SC property probed by the measurement of nuclear-spin-lattice-relaxation time $`T_1`$ in PrOs4Sb12 through 121,123Sb nuclear quadrupolar resonance (NQR) experiments at zero field. Single crystals of PrOs4Sb12 were grown by the Sb-flux method as described elsewhere Sugawara2 . Measurements of electrical resistivity and ac-susceptibility confirmed a superconducting (SC) transition at $`T_c=1.85`$ K. The observation of the de Haas-van Alphen (dHvA) oscillations ensures high-quality of the samples Sugawara2 . For the 121,123Sb NQR measurements, the single crystals were crushed into powder.

Fig. 1(a) displays 121,123Sb-NQR spectra for two Sb isotopes at 4.2 K. Note that 121Sb(123Sb) with natural abundance 57.3 (42.7) % has the nuclear spin $`I=5/2`$ (7/2) and the nuclear gyromagnetic ratio $`\gamma _N=10.189(5.5175)`$ \[MHz/T\], and exhibits two (three) NQR transitions. The ratio of nuclear quadrupolar moment, $`{}_{}{}^{123}Q/^{121}Q`$ was reported as $``$1.275 from the NQR measurement of the pure Sb metal Hewitt . From these spectra, the values of nuclear quadrupole frequency, $`{}_{}{}^{121}\nu _{Q}^{}`$ 44.2 MHz and $`{}_{}{}^{123}\nu _{Q}^{}`$ 26.8 MHz, are deduced for PrOs4Sb12 along with an asymmetric parameter $`\eta 0.46`$. Note that the nuclear electric quadrupole interaction is represented as

$`_Q={\displaystyle \frac{e^2qQ}{4I(2I1)}}\{[3I_z^2I(I+1)]+\eta (I_x^2I_y^2)\},`$ (1)
where $`eq`$ gives the component along the principle $`z`$-axis of electric field gradient (EFG), which is determined by the charge distribution of conduction electrons around the Sb nuclei.

Fig. 1(b) indicates the $`T`$ dependence of the 123Sb-NQR spectrum arising from the 2$`\nu _Q`$ transition where $`\nu _Q`$ is defined as $`\frac{e^2qQ}{4I(2I1)}`$. A peak in the spectrum shifts to a high frequency below $`T_0`$ 10 K that is shown later to be a characteristic temperature in $`1/T_1`$. Since the transitions of $`2\nu _Q`$ and $`3\nu _Q`$ are not sensitive to the change in $`\eta `$, almost the same relative variation of EFG, $`[qq_0]/q_0`$ against the value $`q_0`$ at 10 K is obtained from the $`2\nu _Q`$ for 123Sb and the $`2\nu _Q`$ and $`3\nu _Q`$ for 121Sb, using a relation of $`[\nu _Q(T)\nu _0]/\nu _0`$ as shown in Fig. 1(c). Here $`\nu _0`$ is the value of $`\nu _Q`$ at 10 K. The rapid increase in EFG at the Sb site is evident below $`T_010`$ K. Such the distinct shift is never seen in the isostructual LaOs4Sb12. It is natural to ascribe this increase in EFG to the Pr3+-derived change. This is because the electronic contribution in specific heat divided by $`T`$, $`\mathrm{\Delta }C/T`$ revealed a similar $`T`$ variation to the EFG. It was reported that the rapid increase in $`\mathrm{\Delta }C/T`$ is consistent with the energy scheme of the $`4f^2(J=4)`$ state of Pr3+ in the CEF, that is, the $`\mathrm{\Gamma }_3`$ nonmagnetic doublet is a ground state and the $`\mathrm{\Gamma }_5`$ magnetic triplet is first excited state. The magnetic susceptibility, inelastic neutron scattering, and specific heat revealed the CEF energy splitting of $`\mathrm{\Delta }_{CEF}=711`$ K between these two levels Bauer ; Woodward ; Aoki2 ; Vollmer . We remark, therefore, that the electric quadrupole moments of this $`\mathrm{\Gamma }_3`$ ground state interact with the charges of the conduction electrons in the $`T`$ range below $`T_0`$ 10 K because of $`T<\mathrm{\Delta }_{CEF}`$. Thus the significant increase below $`T_0`$ in both $`\mathrm{\Delta }C/T`$ and the EFG at the Sb site is indicative of a low-lying CEF splitting below $`T_010`$ K, associated with Pr3+($`4f^2`$)-derived ground state.

Fig. 2 indicates the $`T`$ dependence of $`1/T_1`$ measured at $`2\nu _Q48.9`$ MHz for 123Sb along with the result in LaOs4Sb12 ($`T_c=0.75`$ K). In the normal state, a relation of $`T_1T=`$ const. is valid in LaOs4Sb12, characteristic for conventional metallic materials. By contrast, the $`1/T_1`$ at the normal state for PrOs4Sb12 is strongly enhanced than for LaOs4Sb12, showing a relaxation behavior similar to Ce-based HF systems reported thus far. Since $`1/T_1`$ stays a constant in $`T=`$10-20 K, the $`4f`$-electron-derived moments behave as if localized. With decreasing $`T`$ below $`T_010`$ K, $`1/T_1`$ seems to be decreased because of $`T<\mathrm{\Delta }_{CEF}`$. In the localized regime at high $`T`$, note $`1/T_1T\chi (T)`$ where $`\chi (T)`$ is a Curie-Weiss-like magnetic susceptibility in the normal state. As a matter of fact, the $`T`$ dependence of $`1/T_1T`$, which is shown in Fig. 3, resembles the measured susceptibility, which suggests that the $`\mathrm{\Gamma }_3`$ is the ground state and the $`\mathrm{\Gamma }_5`$ is the first excited state Bauer . The relaxation behavior is thus consistent with the other experiments suggesting $`\mathrm{\Delta }_{CEF}=711`$ K Bauer ; Woodward ; Aoki2 ; Vollmer . In $`T`$ lower than $``$ 4 K, however, this CEF model is not valid.

The inset presents the $`T`$ dependencies of $`(1/T_1)/\gamma _N^2`$ at the $`2\nu _Q48.9`$ MHz and the $`3\nu _Q78.6`$ MHz for 123Sb, and the $`2\nu _Q85.0`$ MHz for 121Sb. All the data are consistently on a curve, demonstrating that the relaxation process is magnetic in origin throughout the measured $`T`$ range. This result indicates that the ground state is not always in a nonmagnetic regime where the quadrupolar degree of freedom of nonmagnetic doublet $`\mathrm{\Gamma }_3`$ becomes dominant, but it might be hybridized with conduction electrons, making magnetic relaxation channel open even for $`T<<\mathrm{\Delta }_{CEF}`$. In such the case, the relaxation process at low $`T`$ may be described in terms of the CEF channel and the quasiparticle’s one as follows,

$`1/T_1=A\times \mathrm{exp}(\mathrm{\Delta }_{CEF}/k_BT)+B\times 0.7T`$ (2)
where $`0.7`$ is the value of $`1/T_1T`$ const. for LaOs4Sb12. The first term is the CEF contribution arising from the first excited $`\mathrm{\Gamma }_5`$ triplet state and the second one the quasiparticle’s one due to the hybridization between the $`\mathrm{\Gamma }_3`$ state and conduction electrons. The dotted line in the inset of Fig. 3 is a best fit obtained by assuming $`\mathrm{\Delta }_{CEF}/k_B=8`$ K Aoki2  and $`B=26.7`$ below $`T_F`$ 4 K. The latter value allows us to estimate that the effective density of state (DOS) for PrOs4Sb12 is $`5.2`$ times larger than that for LaOs4Sb12, because $`1/T_1T`$ is proportional to the square of the DOS. This value is quite consistent with the result of $`\gamma =313350`$ mJ/mol K2 for PrOs4Sb12 Bauer ; Vollmer  being five times larger than $`\gamma =56`$ mJ/mol K2 for LaOs4Sb12 Aoki3 . It is expected that the heavy-quasiparticle state is realized through mixing between the nonmagnetic $`\mathrm{\Gamma }_3`$ doublet state and conduction electrons.

Next we deal with the SC property. Fig. 4(a) shows the $`T`$ dependence of the quasiparticle part $`(1/T_1T)_{qp}`$ which is the second term in Eq. (2). Here the data are normalized by the value of $`(1/T_1T)_{qp}`$=const. in $`T=2.34.2`$ K. $`(1/T_1T)_{qp}`$ does not show any coherence peak just below $`T_c=1.85`$ K, and yet starts to be already decreased below $`T^{}`$=2.3 K far above $`T_c`$. Note that this $`T^{}`$ is close to the temperature at which $`C/T`$ has a peak Vollmer . These results point to the unconventional nature of the superconductivity in PrOs4Sb12. Most Ce- or U-based HF superconductors show the power-law behavior of $`1/T_1T^3`$ at low temperatures, consistent with the line-node SC gap Kitaoka ; Mac . However, the $`T`$ dependence of $`(1/T_1T)_{qp}`$ in PrOs4Sb12 does not show a $`T^3`$ dependence ($`T^2`$ dependence in $`1/T_1T`$) as indicated by the solid line in Fig. 4(a). Instead, as presented in Fig. 4(b), it follows an exponential decrease with $`\mathrm{\Delta }/k_B=4.8`$ K over three orders of magnitude in $`T^{}2.3`$ K$`0.3T_c`$ across $`T_c=1.85`$ K. Recent $`\mu `$SR experiment also suggests an isotropic energy gap MacLaughlin . It is unconventional that the isotropic SC gap for PrOs4Sb12 begins to already open up below $`T^{}2.3`$ K far above $`T_c=1.85`$ K. Unconventional strong-coupling effect seems to give rise to preformed pairs around $`T^{}`$ before a bulk SC transition takes place. This also seems to be relevant with the observation of the large jump $`\mathrm{\Delta }C/\gamma T_c3`$ in the specific heat at $`T_c`$ Vollmer . Apparently, the anomalous relaxation behavior in PrOs4Sb12 contrasts with a conventional one for an s-wave case that is actually seen in the $`T`$ dependence of $`1/T_1`$ for LaOs4Sb12 with $`T_c=0.75`$ K in Fig. 2. Remarkably, in this SC state, $`1/T_1`$ shows the large coherence peak just below $`T_c`$, followed by the exponential dependence with the gap size of $`2\mathrm{\Delta }/k_BT_c3.2`$ at low $`T`$. This clearly evidences that LaOs4Sb12 is the conventional weak-coupling BCS $`s`$-wave superconductor.

Although, in a strong-coupling regime, a significant suppression in the coherence peak was reported Ohsugi , it is unexpected that the gap emerges below $`T^{}2.3`$ K that is far above $`T_c=1.85`$ K in PrOs4Sb12. Although the recent thermal-conductivity experiment suggests point-nodes gap Izawa , evidence for the existence of any node in the SC gap is absent down to 0.3$`T_c`$. Unexpectedly, $`1/T_1`$ shows a saturation below 0.3$`T_c`$, remaining issue to conclude any precise argument on some gap structure. It is, however, evident as unraveled in this work that the novel superconductivity takes place under such the situation that the quadrupolar degree of freedom plays vital role for the formation of quasiparticle at temperatures lower than $`\mathrm{\Delta }_{CEF}=711`$ K. We also remark that $`T_c=1.85`$ K for PrOs4Sb12 is more enhanced than $`T_c`$=0.75 K for LaOs4Sb12 and furthermore, the Pr-based superconductor PrRu4Sb12 ($`T_c`$=1.3 K), which is characterized by a singlet CEF ground state, is the weak coupling s-wave superconductor with $`2\mathrm{\Delta }/k_BT_c3.1`$ Yogi . Therefore, it raises a question what type of pairing interaction is possible in mediating the Cooper pair to cause the unconventional strong-coupling superconductivity in PrOs4Sb12.

In summary, the temperature dependence of $`1/T_1T`$ in the new HF superconductor PrOs4Sb12, which is well scaled to the magnetic susceptibility, have revealed that the $`4f`$-derived moments behave as if localized at the higher $`T`$ than $`T_0`$ 10 K. At temperatures below $`T_0`$, the marked increase in NQR frequency at the Sb site and the decrease in $`1/T_1`$ unraveled a low-lying crystal-electric-field splitting, associated with Pr3+($`4f^2`$)-derived ground state. These results are consistent with other experiments that have led to an estimation of $`\mathrm{\Delta }_{CEF}=711`$ between the first excited $`\mathrm{\Gamma }_5`$ magnetic triplet and the $`\mathrm{\Gamma }_3`$ nonmagnetic doublet ground state. In the lower $`T`$ than $`T_F`$ 4 K, the relaxation process is well accounted for by incorporating both the CEF contribution arising from the first excited $`\mathrm{\Gamma }_5`$ triplet state and the $`T_1T`$=const. contribution from the heavy quasiparticle state. The latter is due to the hybridization of the nonmagnetic CEF doublet state with conduction electrons, that is, responsible for the onset of the superconductivity.

In the SC state, $`1/T_1`$ shows neither the coherence peak nor the $`T^3`$ like power-law behavior observed for the HF superconductors to date. Rather, the isotropic energy-gap model with $`\mathrm{\Delta }/k_B=4.8`$ K is consistent with the data below $`T^{}`$ 2.3 K across $`T_c=1.85`$ K. Most remarkably, the novel superconductivity in PrOs4Sb12 differs from the conventional s-wave type and any unconventional ones with the line-node gap. The opening of the large isotropic SC gap 2$`\mathrm{\Delta }/k_BT_c5.2`$ suggests the unconventional strong-coupling effect due to the pairing formation along with the lack for any anomaly across $`T_c`$. Importantly, the present work provides clue to gain insight into the $`4f^2`$-based superconductivity in PrOs4Sb12. We believe that the HF superconductor PrOs4Sb12 is in a new type of unconventional strong-coupling regime, closely relevant to the quadrupolar degree of freedom. The present work hence opens a new research field of superconductivity in strongly correlated electron systems.

We are grateful for fruitful discussions with Kazumasa Miyake and Hisatomo Harima on $`f^2`$-based HF systems. One of authors (H.K.) thanks Y. Tokunaga, @and K. Ishida for valuable discussions and comments. This work was supported by the COE Research (10CE2004) in a Grant-in-Aid for Scientific Research from the Ministry of Education, Sports, Science and Culture of Japan. One of authors (H.K.) has been supported by JSPS Research Fellowships for Young Scientists.


text:
# Rapid Determination of Multiple Reaction Pathways in Molecular Systems: The Soft-Ratcheting Algorithm

## 1 Introduction

Reaction paths in large molecular systems, such as biomolecules, provide critical information regarding structural intermediates (transitions states) and barrier heights. The search for these paths has a long history in the applied math research commnity (e.g., ), as well as in the field of biomolecular computation . Many approaches must start from an initial guess for the reaction path (such as a straight line between two states), effectively limiting the search to a single pathway. On the other hand, “targeted” and “steered” MD approaches  are capable of finding multiple pathways by repeated simulation (from differing initial conditions) forced to reach the desired end state.

The recently-introduced soft-ratcheting approach  is also capable of “blindly” determining multiple reaction pathways. It differs from the targeted and steered approaches in the following ways: (i) monotonic progress toward the target state is not enforced, permitting a wider range of reaction pathways; (ii) soft-ratcheting is applied in the context of stochastic dynamics, although this does not prevent the inclusion of explicit solvent molecules; and (iii) a probability weight (“score”) is associated with each trajectory generated, which in principle also permits estmates of the reaction rates within the dynamic importance sampling (DIMS) formulation discussed by Woolf  and by Zuckerman and Woolf . We note that reaction-rate estimates have not yet been produced by the soft-ratcheting algorithm, because such estimates require trajectories sampled with a near-optimal distribution (i.e., as would occur in unbiased dynamics; see below).

The soft-ratcheting procedure is simple and is motivated by the Metropolis algorithm  and the “exponential transformation” used in nuclear importance sampling (e.g., ). Related methods include the “weighted-ensemble Brownian dynamics” approach of Huber and Kim  and the “CONTRA MD” scheme of Harvey and Gabb . The process is: (a) generate an unbiased step; (b) if the step moves toward the target state, accept it; (c) if it moves away, accept it with a probability (i.e., “softly”) that increases in the forward direction; (d) repeat, while estimating the probability score for all accepted steps. We emphasize that the non-monotonicity embodied in (b) and (c), and the existence of the score in (d) distinguish this method from previous multiple-pathway methods. The guiding concept behind soft-ratcheting is *not* to force the system (which necessarily perturbs the dynamics) but to try to allow the system to proceed in a possible, if unlikely, way. Of course, rare stochastic events are just what we seek!

Note too that, unlike the trajectory sampling methods introduced by Pratt  and pursued by Chandler and coworkers  as well as those of Eastman, Grønbech-Jensen and Doniach , the *overall* effect of the soft-ratcheting algorithm is non-Metropolis in nature (despite the motivation): *trajectories do not evolve from one another and are statistically independent*. The Metropolis idea is only used to ensure that a given trajectory successfully reaches the target state. In this important sense, the soft-ratcheting algorithm comes under the independent-trajectory rubric of the DIMS method .

## 2 Theory

### 2.1 Generating Paths

In essence there is no more theoretical underpinning to producing soft-ratcheted trajectories than that already sketched in the Introduction: using a physically-but-arbitrarily chosen *acceptance probability function* for step increments, one accepts all forward steps, and backward steps are accepted with a probability which decreases the more “negative” the increment. See Fig. 1. Here, the forward direction is simply some vector in configuration space that points from the initial to the target state — perhaps a dihedral angle in a dihedral transition. The algorithm is sufficiently robust (see Results section) that advance knowledge of the reaction path and the true reaction coordinate is not necessary.

When generating a series of soft-ratcheted crossing events in a single long trajectory, it is convenient to use a simple *threshold* device . This means only that trajectories are permitted to perform unbiased dynamics in small regions near the “centers” of the beginning and end states, and biased (i.e., soft-ratcheted) dynamics begin only when the threshold is reached. The idea is to allow the trajectory to explore different parts of the stable states, with an eye toward finding exit points to different pathways. Such exploration, of course, must take place within the limits of available computer time! As noted below, our use of the threshold requires further investigation and optimization, though it appears to perform the task of permitting exploration of alternative exit points from a stable state.

### 2.2 Scoring Paths

It is only when one wishes to associate a score with a trajectory that some analysis must be undertaken. The dynamic importance sampling (DIMS) approach requires the probability score for use in rate estimates, moreover. Specifically, the probability score used in DIMS calculations is the ratio of two quantities : (i) the probability that the given trajectory would occur in an unbiased simulation — a known quantity; and (ii) the probabilty that the given trajectory was produced in the biased (e.g., soft-ratcheting) simulation. Further details of the full DIMS formulation may be found in Refs.  and are beyond the scope of the present report. Here we focus solely on computing the probability that the soft-ratcheting algorithm produced a given trajectory (ii), which unfortunately does not follow directly from the simple acceptance probability used to generate the trajectory.

This section gives full details of generating the probability score (i.e., ratio) required by DIMS. Briefly, however, assume progress towards the target is measured in terms of a scalar “distance,” $`\phi `$, which is larger at the target state than the initial: each step corresponds to an increment $`\mathrm{\Delta }\phi `$, with positive increments moving toward the target. From any starting configuration $`𝐱_{n1}`$, one can define the *unbiased* distribution of $`\mathrm{\Delta }\phi `$ increments $`p_{\mathrm{\Delta }\phi }(\mathrm{\Delta }\phi ;𝐱_n|𝐱_{n1})`$, which is simply the projection of the more fundamental distribution of configurations, $`𝐱_n`$, onto the $`\mathrm{\Delta }\phi `$ coordinate. The distribution of $`\mathrm{\Delta }\phi `$ increments typically is nearly Gaussian with a mean which may be either positive or negative. However, once certain backward steps are rejected due to the acceptance function in the soft-ratcheting procedure (specified below), the $`\mathrm{\Delta }\phi `$ distribution is shifted forward in a non-trivial way to become the biased distribution, $`b_{\mathrm{\Delta }\phi }(\mathrm{\Delta }\phi ;𝐱_n|𝐱_{n1})`$. Estimating the ratio of values of these two distributions for every accepted step (though not the entire distributions) is the task at hand.

The multi-dimensional case reduces to a simple scalar description in terms of $`\mathrm{\Delta }\phi `$ increments, but we include it for completeness. We assume (although it is not necessary for the formalism) that the initial and final states of interest in our molecule do not require the full all-atom configuration $`𝐱`$, but rather a subset of coordinates, say, $`\{\varphi _1,\varphi _2,\mathrm{}\}`$. If the target point is the “center” of state B, say, $`\{\varphi _i^B\}`$, then one can always measure the distance to that point,

$$d_B(\{\varphi _i\})=\left[\underset{i}{}\left(\varphi _i\varphi _i^B\right)^2\right]^{1/2},$$
(1)
where it may be necessary to consider the closest distance if the $`\varphi _i`$ coordinates represent true angles. For a step from $`𝐱_{n1}`$ to $`𝐱_n`$, one can then define a one-dimensional change in distance by

$$\mathrm{\Delta }\phi (n1n)=d_B(\{\varphi _i^{(n)}\})d_B(\{\varphi _i^{(n1)}\}).$$
(2)
In essence, since distance from the target is always a scalar quantity, one need only consider a one-dimensional description to estimate probability scores.

The acceptance function for $`\mathrm{\Delta }\phi `$ increments is very simple and is specified by the simulator. The function used in the present work is illustrated in Fig. 1 and is written

$$p_{\mathrm{acc}}(\mathrm{\Delta }\phi )=\{\begin{array}{cc}1\hfill & \text{if }\mathrm{\Delta }\phi >0\hfill \\ \mathrm{exp}\left[|\mathrm{\Delta }\phi /\mathrm{\Delta }\phi _0|^2\right]\hfill & \text{if }\mathrm{\Delta }\phi <0,\hfill \end{array}$$
(3)
where $`\mathrm{\Delta }\phi _0`$ is a parameter which controls the width of the (backwards) decay depicted in Fig. 1. The gradual decay to zero is the “softness” of soft-ratcheting: many backwards steps will be accepted.

With $`p_{\mathrm{acc}}`$ specified, the final task toward generating the required probability score is to consider the relation between the unbiased and soft-ratcheted (biased) distribution. The probability (density) that the soft-ratcheting algorithm will generate a given $`\phi `$ increment, $`b_{\mathrm{\Delta }\phi }`$, is proportional to the product of the unbiased probability of generating the increment, $`p_{\mathrm{\Delta }\phi }`$, and the acceptance probability, $`p_{\mathrm{acc}}`$:

$$b_{\mathrm{\Delta }\phi }(\mathrm{\Delta }\phi )=𝒩^1p_{\mathrm{\Delta }\phi }(\mathrm{\Delta }\phi )p_{\mathrm{acc}}(\mathrm{\Delta }\phi ),$$
(4)
where $`𝒩<1`$ is the required normalization factor, given by the fraction of steps initiated at $`𝐱_{n1}`$ which would be accepted by the soft-ratcheting procedure. As noted, the biased distribution, $`b_{\mathrm{\Delta }\phi }`$, has been shifted forward in the $`\phi `$ direction because the acceptance function $`p_{\mathrm{acc}}`$ partially suppresses backward steps.

The desired probability score for a single step is then the ratio deriving from (4), namely,

$$\text{single-step ratio}=\frac{p_{\mathrm{\Delta }\phi }(\mathrm{\Delta }\phi )}{b_{\mathrm{\Delta }\phi }(\mathrm{\Delta }\phi )}=\frac{𝒩}{p_{\mathrm{acc}}(\mathrm{\Delta }\phi )}.$$
(5)
To truly calculate the normalization factor $`𝒩`$, one would have to initiate a large number of steps from the point $`𝐱_{n1}`$ and compute the fraction accepted by the soft-ratcheting acceptance function. As that procedure would be very computationally expensive, we instead use the sequence of nearby *attempted* steps, both accepted and rejected, to estimate the probability that soft-ratcheted steps were accepted in a given local region of configuration space. The final score is simply the product of the single-step scores (5).

## 3 Results

The results of this preliminary report may be summarized in three points: (i) the soft-ratcheting algorithm is capable of generating reaction pathways *rapidly* — in a fraction of the time which would be required by unbiased simulation: see Fig. 2; (ii) the scores associated with each crossing trajectory permit the generation of a most-important *ensemble* of events as in Fig. 3, which can give more detailed information about the full “valley” of the pathway; and (iii) the associated scores, in principle, permit *rate estimates* within the dynamic importance sampling formulation .

In Figure 2, one sees the rapidity with which the soft-ratcheting algorithm generates crossing trajectories. The same three pathways are found in 1/70th of the simulation time. In absolute terms, the 10 nsec. of simulation time used in generating the soft-ratcheting trajectories appears quite long; however, this time may be significantly reduced by adjusting the threshold level (see Sec. 2) from the preliminary value used to generate the depicted results.

Figure 3 illustrates the capacity of the soft-ratcheting algorithm to generate an “important” (highly weighted) ensemble of crossing events. The large set of trajectories shown in the figure clearly gives a better description of the pathway valleys than the sparse events generated by unbiased simulation.

Figure 3 also demonstrates the agreement between the weight estimate discussed previously (used to select the depicted trajectories) and the unbiased results. The higher-weighted trajectories coincide strongly with the unbiased events. The large cluster of soft-ratcheted trajectories in the region $`110<\varphi <180`$ deserves comment. Because there is only a single unbiased event in that region, it is not obvious whether the relatively widely dispersed soft-ratcheted trajectories are “correct” — i.e., whether such an ensemble of trajectories would be found in a long unbiased simulation, with many events in the region. Examination of the adiabatic energy surface (not shown) does indicate that the channel in question is indeed significantly wider than the two pathways crossing $`\varphi =0`$, though perhaps not quite to the extent suggested by the soft-ratcheting trajectories of Fig. 3.

## 4 Future Research

Several means of improving the soft-ratcheting procedure are possible, of which we mention two. First, to increase the speed with which transition trajectories are generated — really, to decrease the waiting interval between crossing events — one can reduce the size of the threshold region (Sec. 2) in which purely *unbiased* dynamics are performed. The threshold region was intended to permit trajectories to explore a multiplicity of potential “exit points” from the stable state. However, the “softness” of the soft-ratcheting algorithm should, by itself, permit a substantial degree of this kind of exploration, and it may be possible to use a very small threshold region.

Second, a more optimal (i.e., higher-scoring) ensemble of trajectories presumably can be obtained by systematic estimation of parameter $`\mathrm{\Delta }\phi _0`$. In fact, the promising preliminary results presented in Sec. 3 were based on an *ad-hoc* choice. It is a simple matter to study in more detail an unbiased distribution of $`\mathrm{\Delta }\phi `$ increments, and then use this data to systematically inform the choice of $`\mathrm{\Delta }\phi _0`$. Moreover, one can imagine attempting to bias trajectories forward in a focussed conical region of dihedral angles , rather than simply according to (hyper)planes of constant $`\mathrm{\Delta }\phi `$.

Ultimately, it will also be important to compare the soft-ratcheted paths (which presumably represent the stochastic dynamics in a faithul way) with those generated by explicitly-solvated molecular dyanmics simulation. That is, how does the addition of explicit solvent alter the paths? Of course, this comparison will only be possible in small molecules like the alanine dipeptide and other small peptides, but it will provide a crucial validation of the technique.

## 5 Summary and Discussion

We have given motivation and details for the “soft-ratcheting” algorithm  for determining reaction pathways in molecular systems governed by stochastic dynamics. The method generates independent transition trajectories which will not be trapped in a single channel (pathway), and hence is capable of finding multiple channels. Although a final state is always targeted on average, the algorithm permits “backward” steps with a suppressed probability. The trajectories are thus ratcheted forward, but only softly: see Fig. 1. The capacities of the approach were demonstrated in Figs. 2 and 3 for an all-atom model of the alanine dipeptide molecule evolving according to overdamped Langevin dynamics with the AMBER potential .

Beyond rapidly generating multiple pathways, as other existing approaches are presently able to do , the soft-ratcheting algorithm has the potential also to estimate reaction rates and free energy differences via the dynamic importance sampling (DIMS) framework . The soft-ratcheting algorithm associates a score (see Sec. 2) with each transition trajectory it generates. The scores, in turn, may be used in principle to estimate kinetics and free energy differences. At present, however, we note that initial results showed that further parameterization and/or refinement of the algorithm are necessary before efficiency can be obtained in rate and free energy calculations.

## Acknowledgments

We gratefully acknowledge funding provided by the NIH (under grant GM54782), the AHA (grant-in-aid), the Bard Foundation, and the Department of Physiology. Jonathan Sachs offered many helpful comments on the manuscript.


text:
# One-dimensional continuum and exciton states in quantum wires

## Abstract

High-quality T-shaped quantum wires are fabricated by cleaved-edge overgrowth with the molecular beam epitaxy on the interface improved by a growth-interrupt high-temperature anneal. Characterization by micro-photoluminescence (PL) and PL excitation (PLE) spectroscopy at 5 K reveals high uniformity, a sharp spectral width, and a small Stokes shift of one-dimensional (1-D) excitons. The PLE spectrum for 1-D states shows a large peak of ground-state excitons and a small absorption band ascribed to 1-D continuum states with an onset at 11 meV above the exciton peak.

In semiconductor quantum wires, strong one-dimensional (1-D) Coulomb interactions Loudon ; OgawaPRB91 ; PKMpp242  cause 1-D excitons to have a large binding energy WegscheiderPRL ; SomeyaPRL ; many ; SzymanskaPRB  and strong absorption intensity in the ground state AkiyamaPRB96c . Moreover, it has been predicted that absorption intensity of continuum states at the band edge should be reduced from electronic joint density of states, which is proportional to inverse square root of energy $`1/\sqrt{E}`$ in 1-D systems OgawaPRB91 ; PKMpp242 . The ratio of the absorption intensity of the continuum states against electronic joint density of states is called the Sommerfeld factor. Thus, the Sommerfeld factor should be less than one in 1-D systems.

In 2-D and 3-D systems, on the other hand, the Coulomb interaction makes the absorption intensity of the continuum states at the band edges enhanced from the joint density of states PKMpp242 ; MillerPRB . In other words, the Sommerfeld factor is more than one in 2-D and 3-D systems. Such a striking contrast has long been an issue of fundamental interest in low-dimensional structures.

However, a major problem of practical quantum wires for experimental study of the above effect has been the large energy broadening due to structural inhomogeneities such as interface roughness, which disturbs the subtle detail inherent in 1-D systems. Over the past ten years the cleaved-edge-overgrowth method of molecular beam epitaxy (MBE) has been developed PfeifferAPL  to fabricate high-quality quantum wires (T-wires) formed at the right angle T-shaped intersection of two quantum wells (QWs) WegscheiderPRL ; SomeyaPRL ; GoniAPL ; HasenNAT ; AkiyamaJP ; WegscheiderAPL ; RubioSSC , in which the atomic precision of the quantum wire is determined entirely by the atomic precision of the individual intersecting wells. Moreover we have recently-developed an annealing technique YoshitaJJAP  that has dramatically improved the (110) interface uniformity. A doped T-wire sample formed with this method has shown an order of magnitude sharper photoluminescence (PL) linewidth compared to previous T-wires AkiyamaSSC .

In this work, we fabricate high-quality non-doped T-wires in a T-wire laser structure, and demonstrate striking improvement in uniformity, spectral width, and Stokes shift by micro-PL, PL excitation (PLE), and scanning micro-PL characterizations. The observed PLE spectrum of the T-wires has shown an isolated strong single peak and a small continuous absorption band with an onset at 11 meV above the peak. Experiments indicate that the peak and the continuous band are intrinsic to quantum wires, so that they are interpreted as the 1-D exciton ground state and 1-D continuum states, or 1-D inonized electron-hole excited states with continuous energy spectrum. In fact, the observed PLE spectrum of T-wires agrees qualitatively with theoretically predicted features inherent to 1-D excitonic systems Loudon ; OgawaPRB91 ; PKMpp242 .

Figure 1 shows a schematic of our T-wire sample, which is embedded in a T-wire laser structure fabricated by the following procedures. First, on a non-doped (001) GaAs substrate we successively grew a 50 nm GaAs buffer layer, a 1 $`\mu `$m cladding layer of 50 % digital alloy (GaAs)4(AlAs)4, 1.16 $`\mu `$m thick multiple QW layer composed of 20 periods of 14.15 nm Al0.073Ga0.927As QWs (stem well) and 41.88 nm Al0.35Ga0.65As barriers, a 3 $`\mu `$m cladding layer of 50% digital alloy (GaAs)4(AlAs)4, and a 10 nm GaAs cap layer. The substrate growth temperature was 600 C, and growth was interrupted for 15 seconds after each Al0.073Ga0.927As stem well and each GaAs layer in the 50% digital alloy.

Then, in a separate MBE growth on an in-situ cleaved (110) edge of this structure, we grew at 490 C by the cleaved-edge overgrowth method, a 6 nm GaAs QW (arm well) layer, a 10 nm Al0.5Ga0.5As barrier layer, a 167nm Al0.1Ga0.9As core layer, a 0.96 $`\mu `$m cladding layer of 50 % digital alloy (GaAs)6(AlAs)6, and a 10 nm GaAs cap layer. Right after the growth of the GaAs arm well layer, growth was interrupted for a 10 minute anneal at 600 C. This anneal is based on our recently-developed growth-interruption annealing technique YoshitaJJAP .

Substrate rotation was performed by 10 revolutions per minute during the MBE growths both in the (001) and the (110) directions. Our fabrication method is similar to that in our previous work WegscheiderPRL ; RubioSSC  except for the anneal step, that dramatically reduces interface roughness on (110)-GaAs surfaces.

Twenty periods of highly uniform T-wires are thus formed at the T-shaped intersections of 7%-Al-filled 14nm stem wells and a 6 nm arm well, and embedded in the core of T-shaped optical waveguide. A laser bar with 500$`\mu `$m cavity length was cut from the wafer by cleavage, attached on a copper block with silver paint, and cooled down to 5K on the cold finger of a helium-flow-type cryostat. Lasing properties of the sample will be reported elsewhere AkiyamaPRL2 .

Micro-PL and PLE measurements on the T-wires were performed with a cw titanium-sapphire laser via the overgrowth (110) surface in the geometry of point excitation into a 0.8 $`\mu `$m spot YoshitaJAP  centered at the T-wire region with a 0.5 numerical aperture objective lens. A 0.6m triple spectrometer with a 600 grooves/mm grating and a back-illumination-type liquid-nitrogen-cooled charge-coupled-device camera were used to detect PL. Spectral resolution was 0.3 meV.

Figure 2 (a) shows scanning micro-PL spectra by 1 $`\mu `$m steps over 30 $`\mu `$m along T-wires at 5 K. The excitation light had intensity of 2 $`\mu `$W and photon energy of 1.653 eV. Well-resolved sharp peaks are observed for the T-wires (1.578 eV) and the stem well (1.630 eV). PL of arm well is not observed, because carriers created in the arm well quickly flow into T-wires. The full-width-of-half-maximum (FWHM) of the T-wire peak is 1.5 meV, far smaller than those reported in previous work WegscheiderPRL ; SomeyaPRL ; AkiyamaPRB96c ; GoniAPL ; HasenNAT ; AkiyamaJP ; WegscheiderAPL ; RubioSSC , showing the high flatness of the interfaces.

PL peak of stem wells and the main peak of T-wires are very uniform over 30 $`\mu `$m. Intensities of small peaks in the lower energy side of the main peak of T-wires vary from place to place. Thus, these peaks are ascribed to localized excitons in T-wires. The PL energy positions of the localized excitons are discrete with separation of 2.4meV. This is consistent with thickness fluctuation of arm well by integer monolayers. Atomic force microscope study of arm well surfaces has shown the existence of islands with specific shape and 1-3 monolayer heights YoshitaJJAP . Small intensities of the localized exciton peaks indicate that such islands are very rare.

Figure 2 (b) shows scanning micro-PL spectra by 10 $`\mu `$m steps over 500 $`\mu `$m along T-wires at 5 K, which is the whole region of the T-wire laser cavity. The 30 $`\mu `$m region shown in Fig. 2 (a) is represented by the central three spectra indicated by the side arrows. The whole spectra show that PL of T-wires is uniform over 500 $`\mu `$m.

Figure 3 (a) shows PL spectrum at 5 K for a spot at the central region of Fig. 2 (a). Figure 3 (b) shows PLE spectrum of the T-wire PL, which reveals the absorption spectrum of the T-wires. The excitonic absorption peaks of T-wire (1.578 eV), arm well (1.599 eV), and stem well (1.632 eV) are clearly observed. The two peaks at 1.599 eV and at 1.605 eV are due to the arm well in the core region on 35% barrier and the adjacent arm well in the cladding region on 50% barrier, respectively, which is confirmed by a separate PL imaging experiment.

The Stokes shift of ground state excitons in T-wires, that is the peak shift energy of PL and PLE peaks for T-wires, is found to be 0.5meV, whereas the FWHM width of T-wire PLE peak is 2.5meV. The Stokes shift is small compared with the width, so that the PL peak is well overlapped with the PLE peak. This demonstrates that the PL of T-wires has a free-exciton nature. This is the first such demonstration for quantum wires.

Note that a continuous absorption band is observed in the PLE spectrum with an onset at 1.589 eV, as magnified in the inset of Fig. 3. It is 11 meV above the PL peak of the ground-state free exciton in T-wires. Such an absorption band was observed in all of several different pieces of samples that we measured. In particular, a single quantum wire sample with only one wire instead of 20 wires showed a continuous absorption band with a similar shape but with significantly smaller intensity than the present 20 wire sample. The reproducibility and the correlation of its intensity with wire numbers suggest that the continuous absorption band is not caused by extrinsic low energy states in the arm well but originates from intrinsic states in quantum wires.

In general, an exciton peak should accompany a continuous absorption band separated by an exciton binding energy, because excitons not only have a bound ground state but also have ionized continuous excited states of an electron and a hole. Thus, a continuous absorption band should be observed together with an exciton peak in a PLE measurement with high resolution and sensitivity. Therefore, the observed continuous absorption band in Fig. 3 is expected to correspond to ionized continuous excited states of an electron and a hole in T-wires, namely 1-D continuum states. A similar measurement of the excited levels of 2-D excitons in quantum wells was reported in 1981 by Miller and coworkers MillerPRB , in which they resolved the 1s-like ground-state exciton and the 2-D continuum states with a line shape close to the step-function-like 2-D density of state. Our work is the first such observation of 1-D continuum states in quantum wires enabled by improvement in spectral sharpness of the wires.

It is remarkable that the 1-D continuum states do not appear to have a $`1/\sqrt{E}`$-like singularity at the onset as would be expected from a 1-D joint density of states. Moreover, the peak intensity of the 1-D exciton ground state is much stronger than the intensity of the onset of the 1-D continuum states in quantum wires. In fact, it has been theoretically predicted Loudon ; OgawaPRB91 ; PKMpp242  for 1-D excitonic systems that the exciton ground state has strong absorption intensity in the ground state. Instead, absorption intensity of continuum states at the band edge should be reduced, and singularity in 1-D electronic joint density of states proportional to $`1/\sqrt{E}`$ should be removed.

To discuss this predicted effect, we made, in Fig. 4, combined plots of absorption spectra of 1-D excitons and continuum states calculated by Ogawa and Takagahara in 1991 OgawaPRB91 . Neglecting real confinement potential, they solved an 1-D schrödinger equation for the Coulomb potential $`e^2/(z+z_0)`$, where $`z`$ and $`z_0`$ are the electron-hole distance and an artificial cutoff length. Two thick vertical lines in the region of negative photon energy represent positions and relative intensity for absorption peaks of the ground and second exciton bound states for $`z_0/a_B=0.2`$, where $`a_B`$ shows the 3-D exciton Bohr radius. A thick curve in the region of positive photon energy represents absorption profile due to 1-D continuum states for $`z_0/a_B=0.2`$. In comparison, 1-D density of states proportional to $`1/\sqrt{E}`$ are shown by a dashed curve, which reveals that the absorption intensity of the 1-D continuum states is suppressed at the band edge. For smaller choice of $`z_0`$, the ground-state-exciton peak become stronger in intensity and lower in energy (not shown), while 1-D continuum states become smaller as shown by dotted curves for $`z_0/a_B`$=2.0, 1.0, 0.5, and 0.05. The second exciton peak is not sensitive to $`z_0`$. The physics suggested by this theory is that strong 1-D Coulomb interactions move the oscillator strength out of the low energy edge of the continuum states into the stabilized ground-state excitonPKMpp242 . Thus, the $`1/\sqrt{E}`$ singularity of the 1-D free-particle density of states is completely suppressed in the line shape for 1-D continuum states, and the shape becomes very similar to a step function.

Our result in Fig. 3 is the first experimental data in semiconductor quantum wires to be compared with such theoretical predictions Loudon ; OgawaPRB91 ; PKMpp242 , where the 1-D ground state exciton peak and a continuum absorption band are completely resolved.

For more quantitative discussion, we need to compare our result with more practical calculations. Though there are many theoretical papersmany  on 1-D exciton binding energies in T-wires, calculation of absorption spectra as well as binding energies to be compared with our present experiment has been reported only by Szymanska and coworkers SzymanskaPRB ; RubioSSC . The calculated spectrum SzymanskaPRB ; RubioSSC  shows a strong peak of the 1-D exciton ground state, a weaker peak of the second exciton state, and a series of continuously populated small states. The continuous states have onset at 11 meV above the ground states and have fairly flat intensity, which are in good agreement with our experimental results. On the other hand, the peak of the second exciton states appeared in the calculated spectrum at 6 meV above the ground state is not observed in our experiment. It suggests that further work both in measurements and theoretical calculations is necessary.

In summary, we achieved dramatic improvement in uniformity, spectral width, and Stokes shift in T-shaped quantum wires by growth interrupt anneal with cleaved edge overgrowth in MBE. The observed PLE spectrum of the T-wires shows the strong ground-state-exciton peak and a small continuous absorption band with an onset at 11 meV above the peak, which is ascribed to 1-D continuum states. The observed PLE spectrum of T-wires agrees qualitatively with theoretically predicted features inherent to 1-D excitonic systems meaning that the $`1/\sqrt{E}`$ singularity of the 1-D free-particle density of states is suppressed in the line shape for 1-D continuum states as a result of the strong 1-D Coulomb interaction effect.

We thank Professor P. B. Littlewood and Dr. M. Szymanska in University of Cambridge for valuable discussion, and Prof. T. Ogawa in Osaka University for discussion and permission for using his published results. One of the authors (H. A.) acknowledges the financial support from the Ministry of Education, Culture, Sports, Science and Technology, Japan.


text:
# Statistical hadronization of charmed quarks at SPS and RHIC

##

The interest to charmed quarks in heavy ion physics was initially motivated by the suggestion of Matsui and Satz  to use charmonia as a probe of the state of matter created at the early stage of the collision.

The standard picture of charmonium production in nucleus-nucleus collisions assumes that charmonia are created exclusively at the initial stage of the reaction in primary nucleon-nucleon collisions. During the subsequent evolution of the system, the number of hidden charm mesons is reduced because of (a) absorption of pre-resonance charmonium states in the nuclei (normal nuclear suppression), (b) interactions of charmonia with secondary hadrons (comovers), (c) dissociation of $`c\overline{c}`$ bound states in the deconfined medium. It was found that the $`J/\psi `$ suppression with respect to Drell-Yan muon pairs measured in proton-nucleus and nucleus-nucleus collisions with light projectiles can be explained by the normal nuclear suppression alone . In contrast, the NA50 experiment with a heavy projectile and target (lead-lead) revealed essentially stronger $`J/\psi `$ suppression for central collisions . This anomalous $`J/\psi `$ suppression was attributed to formation of quark-gluon plasma .

Despite of quite successful agreement with the $`J/\psi `$ data, the standard scenario seems to be in trouble explaining the $`\psi ^{}`$ yield. The recent lattice simulations  suggest that the temperature of $`\psi ^{}`$ dissociation $`T_d(\psi ^{})`$ lies far below the deconfinement point $`T_c`$: $`T_d(\psi ^{})0.1`$$`0.2T_c`$ . Therefore, not only the quark-gluon plasma, but also a hadronic co-mover medium should completely eliminate $`\psi ^{}`$ charmonia in central Pb+Pb collisions at SPS. However, the experiment revealed a sizable $`\psi ^{}`$ yield (see, for instance, ). It was observed  that $`\psi ^{}`$ to $`J/\psi `$ ratio decreases with centrality only in peripheral lead-lead collisions, but remains approximately constant at sufficiently large number of participants $`N_p100`$.

A completely different picture of charmonium production was proposed in Ref. : hidden charm mesons are supposed to be created at the hadronization stage. Similar to all other hadrons, their abundancies can be described within the thermal model . However, production of heavy quarks in soft processes is expected to be negligible. Most likely, they are produced exclusively at the hard stage. Their number, therefore, can, generally speaking, deviate from the thermal equilibrium value. This fact was taken into account by the statistical coalescence model (SCM), which was proposed in Ref.. Soon, it was realised that, when the average number of heavy quark pairs per collision is small ($`1`$), exact conservation of this pairs in the hadronization process appears to be crucial .

In this talk, I present the results  obtained within the statistical coalescence model:

* $`c`$ and $`\overline{c}`$ are created at the initial stage of the reaction in primary hard parton collisions;
* their number remains approximately unchanged during the subsequent evolution;
* they are distributed over open charm hadrons and charmonia at the hadronization stage in accordance with laws of statistical mechanics.

Within its applicability domain ($`N_p100`$), the model demonstrates excellent agreement ($`\chi ^2/\text{dof}=1.06`$) with the NA50 data on $`J/\psi `$ production (see Fig. 2).

The so-called ‘second threshold of anomalous $`J/\psi `$ suppression’ at large transverse energy ($`E_T100`$ GeV) naturally appears in SCM due to two effects: (i) fluctuations of the transverse energy at fixed number of participant nucleons and (ii) $`E_T`$-losses in the dimuon event sample with respect to the minimum bias one (see Ref.  for details).

The agreement with the data is reached assuming a rather strong enhancement of the open charm production in central Pb+Pb collisions: up to a factor of about $`3.5`$ within the rapidity window of the NA50 spectrometer. This is consistent with the indirect experimental result .

A possible mechanism of open charm enhancement was proposed in Ref. . Calculations in the leading order of perturbative quantum chromodynamics (QCD) show that, assuming factorization (i.e. independence of the hard QCD process on the subsequent soft stage), a great fraction of $`c\overline{c}`$ pairs is created with invariant masses $`M_{c\overline{c}}`$ below the corresponding meson threshold $`2m_D`$. In vacuum, these subthreshold pairs would not be able to form observable hadrons. In reality, however, some part of these pairs may hadronize due to interaction with spectator partons. Nevertheless, there is no reason to assert that all subthreshold pairs result in final state hadrons with open or hidden charm. It is quite reasonable to assume that a great part of them has to annihilate into lighter hadrons, or, alternatively, the final state interactions prevent formation of such pairs (factorization is broken).

In presence of a deconfined medium (quark-gluon plasma or its precursor), the subthreshold quark pairs can hadronize due to interactions with the medium, or, alternatively, the medium can modify the final state interactions making possible creation of the subthreshold pairs and their subsequent hadronization. This should lead to enhanced production of the total charm in nucleus-nucleus collisions in comparison to the standard result obtained within the direct extrapolation of nucleon-nucleon data.

We have estimated the upper bound of the open charm enhancement. At SPS energies, one can expect maximal enhancement by a factor of about 6, which is consistent with our above fit for the $`J/\psi `$ to Drell-Yan ratio.

It is interesting to note, that the statistical coalescence model does not always lead to $`J/\psi `$ suppression. Predictions of the statistical coalescence model for RHIC are shown in Fig. 2 (see also Ref.). As is seen, $`J/\psi `$ suppression is still expected at the lowest RHIC energy. In contrast, relative $`J/\psi `$ enhancement (e.g. growth of the $`J/\psi `$ to open charm111It should be stressed that, due to possible nuclear shadowing, the open charm multiplicity has not to be proportional to the number of binary nucleon-nucleon collisions. Therefore the ratio of $`J/\psi `$ multiplicity to the number of binary collisions may decrease even if $`J/\psi `$ to open charm ratio increases. ratio with the number of participants at $`N_p>100`$) is predicted for the top RHIC energy.

In conclusion, the NA50 data for not very peripheral lead-lead collisions are consistent with the following scenario:

Formation of deconfined medium leads to enhanced production of charmed hadrons. Charmonia as well as other hadrons are formed at the hadronization stage. The distribution of charm quarks and antiquarks over open and hidden charm hadrons follows laws of statistical mechanics.

A relative $`J/\psi `$ enhancement is expected at the top RHIC energy.

I am indebted to M. Gorenstein, W. Greiner, L. McLerran and H. Stöcker for fruitful collaboration. I wish to thank A. Andronic, F. Becattini, P. Bordalo, P. Braun-Munzinger, L. Bravina, A. Capella, Yu. Dokshitzer, J. Cleymans, W. Florkowski, A. Frawley, L. Grandchamp, A. Kaidalov, B. Kämpfer, J. Kapusta, F. Karsch, D. Kharzeev, V. Koch, K. Redlich, D. Rischke, M. Rosati, H. Satz, E. Shuryak, Yu. Sinyukov, J. Stachel, J. Wambach, A. Zhitnitsky and G. Zinovjev for interesting discussions.