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# Chirality effects in carbon nanotubes.

## I Introduction

Since the discovery of carbon nanotubes  the physical properties of these nanostructures have attracted a lot of attention . Usually carbon nanotubes (CNs) are visualized as a layer of graphene sheet rolled-up into a cylinder. Depending of the way of the rolling up the cylinder can be chiral or non-chiral.

In media with chiral symmetry it is impossible to distinguish between polar and axial vectors. This leads to the existence of the natural optical activity , including the optical rotatory power and circular dichroism in the absence of magnetic fields, and any other effect of chirality where a polar vector and an axial vector (or a pseudovector) are interrelated by some phenomenological equation. The circular photogalvanic effect (CPGE) is among them. In this effect a dc current induced by an electro-magnetic wave of the complex amplitude E is proportional to components of the axial vector $`i(𝐄\times 𝐄^{})`$ and thus depends on the sign of the circular polarization of light. The CPGE was predicted in  and then studied in bulk gyrotropic crystals  and semiconductor quantum-well structures .

Theoretically, achiral magnetic properties and optical absorption spectra of CNs were investigated by Ajiki and Ando in the effective-mass approximation  (see also ). The theory of the optical activity of CNs has been considered by Tasaki et al.  in the framework of the microscopic tight-binding model.

In the present paper we consider effects of chirality in CNs by extending the effective-mass theory . We show that these effects appear due to terms in the electron Hamiltonian describing the coupling between the orbital momentum around the circumference of a chiral CN and the linear electron momentum along the tube. This is quite different from the case of bulk materials and semiconductor quantum wells where these effects are attributed to spin-orbit terms $`\sigma _\alpha k_\beta `$ in the electron effective Hamiltonian ($`\sigma _\alpha `$ and $`𝐤`$ are the Pauli spin matrices and the electron wave vector; $`\alpha ,\beta `$ are the cartesian coordinates)  (see also ).

The paper is organized as follows. In Sec. II we briefly review properties of the single particle electron spectrum of CNs and derive an expression for the matrix element of the electron-photon interaction. In Secs. III and IV we present the theory of photogalvanic effects in chiral CNs. We show that the circularly polarized light generates a dc current through CN and the current direction depends on the sign of polarization, i.e. on the photon spirality. In the presence of an external magnetic field $`B`$ parallel to the nanotube principal axis, the linearly polarized light generates a dc current whose direction changes upon the inversion of $`B`$. In Sec. V we develop a theory of the magneto-chiral anisotropy in the dc charge transport through a CN, which is the existence of a dc current proportional to $`B`$ and quadratic in the applied electric field $`E`$. In Sec. VI we give analytical estimates for the optical anisotropy and optical activity of CN. In Sec. VII we discuss limitations of our approach and mention other effects which are similar to those considered in this article.

## II Electron band structure and electron-photon matrix elements in carbon nanotubes.

Usually carbon nanotubes (CNs) are visualized as a conformal mapping of a graphene sheet onto a cylindrical surface where one of the two-dimensional (2D) Bravais lattice vectors, L, maps to the cylinder circumference . The structures specified by the vectors L directed along one of the two-fold rotation axes $`u_2`$ or $`u_2^{}`$ are called respectively armchair and zigzag CNs, where the axis $`u_2`$ is parallel and the axis $`u_2^{}`$ is perpendicular at least to one side of the 2D lattice hexagon. These particular tubes are achiral. Except for them all others are chiral with their principal axis $`z`$ being the screw axis.

Following  we write the circumferential vector as

$$𝐋=n_a𝐚+n_b𝐛,$$
(1)
where $`n_a,n_b`$ are integers and $`𝐚,𝐛`$ are the 2D basis vectors with the angle 120 between them. Choosing the coordinate system $`x_1,x_2`$ in such a way that $`x_1𝐚`$, $`x_2𝐚`$ we have for the components of a and b

$$𝐚=a(1,0),𝐛=a(\frac{1}{2},\frac{\sqrt{3}}{2}),$$
(2)
where the lattice constant $`a`$ is equal to $`\sqrt{3}`$ times the interatomic distance $`d=1.44`$ Å . The electron effective Hamiltonian for a graphene sheet,

$$H=\left(\begin{array}{ccc}0& & h^{}\\ h& & 0\end{array}\right),$$
(3)
is expanded in the vicinity of the points

$$𝐊=\frac{4\pi }{3a}(1,0),𝐊^{}=\frac{4\pi }{3a}(1,0)$$
(4)
at the corners of the 2D Brillouin zone shown in Fig. 1. In the following we define k and $`𝐤^{}`$ as wavevectors referred respectively to the points $`𝐊`$ and $`𝐊^{}`$ and assume the products $`ka,k^{}a1`$ to be small. Then, in the second order in $`ka`$ or $`k^{}a`$, the matrix element $`h`$ in Eq. (3) is given by (see )

$$h(𝐤,𝐊)=\gamma e^{i\theta }\left[k_{}ik_z+\frac{a}{4\sqrt{3}}e^{3i\theta }\left(k_{}+ik_z\right)^2\right]$$
(5)
near the K point and

$$h(𝐤^{},𝐊^{})=\gamma e^{i\theta }\left[k_{}^{}ik_z^{}+\frac{a}{4\sqrt{3}}e^{3i\theta }\left(k_{}^{}ik_z^{}\right)^2\right]$$
(6)
near the $`𝐊^{}`$ point. Here $`\gamma =\frac{\sqrt{3}}{2}\gamma _0a`$, $`\gamma _0`$ ($`3`$ eV ) is the transfer integral between neighboring $`\pi `$ orbitals, $`\theta `$ is the angle between the vector L and the basis vector a. The subscripts $`z,`$ indicate components of a vector referred to the axes lying in the graphene plane and related to the vector L so as $`z𝐋`$ and $`k_z𝐋`$, $`k_{}𝐋`$.

In the same approximation the energy spectrum near the K point is given by

$$E_{c,v}(𝐤,𝐊)=\pm |h|\pm \gamma \left\{|𝐤|+\frac{a}{4\sqrt{3}|𝐤|}\left[\left(k_{}^33k_{}k_z^2\right)\mathrm{cos}3\theta +\left(k_z^33k_{}^2k_z\right)\mathrm{sin}3\theta \right]\right\},$$
(7)
where $`|𝐤|`$ = $`\sqrt{k_{}^2+k_z^2}`$, the upper and lower signs represent the conduction (subscript $`c`$) and valence (subscript $`v`$) bands respectively. The similar spectrum near the $`𝐊^{}`$ point is obtained by changing $`k_{}k_{}^{}`$, $`k_zk_z^{}`$, $`\theta \theta `$ in agreement with the time inversion symmetry requirement $`E_{c,v}(𝐤,𝐊^{})`$ $`=E_{c,v}(𝐤,𝐊)`$.

In a CN specified by the vector L the electron wave function satisfies the cyclic boundary condition $`\mathrm{\Psi }(𝐫)=\mathrm{\Psi }(𝐫+𝐋)`$. This enables one to find the allowed discrete values of $`k_{}`$ as

$$k_{}=\frac{2\pi }{L}\left(n\frac{\nu }{3}\right);k_{}^{}=\frac{2\pi }{L}\left(n+\frac{\nu }{3}\right),$$
(8)
where $`n`$ is an integer $`0,\pm 1,\pm 2\mathrm{}`$ characterizing the angular momentum component of an electron, $`L=|𝐋|=a\sqrt{n_a^2+n_b^2n_an_b}`$, and $`\nu `$ equals to one of three integers: $`0,\pm 1`$ determined by the presentation of the sum $`n_a+n_b`$ as $`3N+\nu `$ with integer $`N`$. The dispersion in the conduction and valence subbands is obtained by substituting Eq. (8) into Eqs. (5,6) or Eq. (7). In the following we focus on the nanotubes characterized by finite band gap and assume $`\nu 0`$. According to Eq. (7), for small values of $`k_z`$ satisfying the condition $`|k_z||k_{}|`$ in the $`K`$ valley and similar condition in the $`K^{}`$ valley, the electron spectrum has a parabolic form with terms linear in $`k_z`$

$`E_{c,v}(n,k_z;K)`$ $`=`$ $`\pm \left({\displaystyle \frac{\mathrm{\Delta }_n}{2}}+{\displaystyle \frac{\mathrm{}^2k_z^2}{2m_n}}+\beta _nk_z\right),`$ (9)
$`E_{c,v}(n,k_z^{};K^{})`$ $`=`$ $`\pm \left({\displaystyle \frac{\mathrm{\Delta }_n^{}}{2}}+{\displaystyle \frac{\mathrm{}^2k_z^{}_{}{}^{}2}{2m_n^{}}}+\beta _n^{}k_z^{}\right),`$ (10)
where

$$\mathrm{\Delta }_n=2\gamma |k_{}|,\mathrm{\Delta }_n^{}=2\gamma |k_{}^{^{}}|,$$
(11)
$$m_n=\frac{\mathrm{}^2|k_{}|}{\gamma },m_n^{}=\frac{\mathrm{}^2|k_{}^{}|}{\gamma },$$
(12)
$$\beta _n=\frac{\sqrt{3}}{4}\gamma a|k_{}|\mathrm{sin}3\theta ,\beta _n^{}=\frac{\sqrt{3}}{4}\gamma a|k_{}^{}|\mathrm{sin}3\theta ,$$
(13)
and $`k_{},k_{}^{}`$ are defined in Eq. (8). Note that the identity $`E_{c,v}(n,k_z;K^{})`$ $`=E_{c,v}(n,k_z;K)`$ follows directly from the time inversion symmetry.

In the presence of an external magnetic field $`𝐁`$, the electron energy is modified just by changing $`k_{},k_{}^{}`$ from Eq. (8) into

$$k_{}=\frac{2\pi }{L}\left(n\frac{\nu }{3}+\frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}\right);k_{}^{}=\frac{2\pi }{L}\left(n+\frac{\nu }{3}+\frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}\right),$$
(14)
where $`\mathrm{\Phi }`$ is the magnetic flux passing through the cross section of a CN, $`\mathrm{\Phi }=B_zL^2/(4\pi )`$, and $`\mathrm{\Phi }_0`$ is the magnetic flux quantum, $`ch/e`$. Now the consequence of the time inversion symmetry takes the form $`E_{c,v}(n,k_z;\mathrm{\Phi };K^{})`$ $`=E_{c,v}(n,k_z;\mathrm{\Phi };K).`$

Chirality (or spirality) of a nanotube manifests itself in a particular coupling between the angular momentum as described by $`n`$ and the directed translational motion as described by $`k_z`$: due to the terms linear-$`k_z`$ in Eq. (9) or, in general, due to odd-in-$`k_z`$ terms in Eq. (7) the energy has a contribution which depends both on the $`sign`$ of $`k_z`$ and the $`sign`$ of $`n`$.

It is interesting to analyze how this particular coupling disappears for zigzag and armchair tubes which are achiral from the symmetry point of view. In zigzag tubes, the angle $`\theta `$ between the circumferential vector L and the vector a is an integer multiple of 60, $`\mathrm{sin}3\theta `$ is zero and odd-in-$`k_z`$ terms in Eqs. (7,9) vanish. In armchair tubes, the angle $`\theta `$ equals to $`\theta =30^{}+N60^{}`$ with $`N`$ integer leading to one of the following three relations between $`n_a`$ and $`n_b`$: $`n_a=2n_b`$ or $`n_b=2n_a`$ or $`n_b=n_a`$. This means that the sum $`n_a+n_b`$ is an integer multiple of 3 and the parameter $`\nu `$ is zero. As a result values of $`|k_{}|`$ become independent of the sign of $`n`$ and the coupling between signs of $`n`$ and $`k_z`$ in the terms odd-in-$`k_z`$ terms. This follows also from the symmetry considerations and is an important check point. In the following sections we will show that the odd-in-$`k_z`$ terms in the electron energy spectrum govern the chirality effects in CNs.

Let us now turn to the calculation of the matrix element, $`V_{fi}`$, for the electron optical transition between the initial state $`i`$ and the final state $`f`$. The electron envelope functions can be written in the form

$$\psi _{c,v}(z;n,k_z)=\frac{e^{in\phi }}{\sqrt{2\pi }}\frac{e^{ik_zz}}{\sqrt{L_{CN}}}\widehat{C}_{c,v}(n,k_z),$$
(15)
where $`L_{CN}`$ is the nanotube length and $`\phi `$ is the azimuth angle. The two-component columns $`\widehat{C}_{c,v}`$ are eigenvectors of the 2$`\times `$2 matrix Hamiltonian (3), given by

$$\widehat{C}_c=\frac{1}{\sqrt{2}}\left[\begin{array}{c}h^{}/|h|\\ 1\end{array}\right],\widehat{C}_v=\frac{1}{\sqrt{2}}\left[\begin{array}{c}1\\ h/|h|\end{array}\right]$$
(16)
with $`h`$ defined by Eq. (5) for the $`K`$ valley and by Eq. (6) for the $`K^{}`$ valley where $`K,K^{}`$ are the $`z`$-components of the vectors $`𝐊,𝐊^{}`$.

We remind that the electron interaction with the electromagnetic field is described by the perturbation $`(e/c)\{\widehat{𝐯}𝐀\}_s`$, where A is the vector potential of the field, $`e`$ is the electron charge, $`\widehat{𝐯}`$ is the electron velocity operator $`\mathrm{}^1dH/dk_z`$ and the symbol $`\{\mathrm{}\}_s`$ means a symmetrized product of operators. If $`|k_z||k_{}|`$ then one can neglect the second-order terms in the expansion Eq.(5), the symmetrization symbol can be omitted and the scalar product of $`\widehat{𝐯}`$ and the light unit polarization vector e has the form

$$\widehat{𝐯}𝐞=\frac{i\gamma }{2\mathrm{}}\left[\begin{array}{cc}0& e^{i\theta }f_{12}\\ e^{i\theta }f_{21}& 0\end{array}\right].$$
(17)
Here

$`f_{12}=e^{i\phi }e_{}e^{i\phi }e_++e_z,f_{21}=e^{i\phi }e_{}e^{i\phi }e_+e_z,`$

$`e_\pm =e_x\pm ie_y`$ and $`x,y`$ are rectangular axes perpendicular to the principal axis $`z`$ of the tube. The selection rules for matrix elements of the operator taken between the envelope functions Eq.(16) are in agreement with the conservation law for $`z`$-components of the angular momenta: $`n_f=`$ $`n_i+n_{phot}`$, where $`n_{phot}=\pm 1`$ for the circular polarization $`\sigma _\pm `$ of a photon propagating along the $`z`$ axis and $`n_{phot}=0`$ for the light linearly polarized along $`z`$. In particular, the transitions $`(c,0,K)(c,1,K)`$, $`(c,0,K^{})(c,1,K^{})`$ occur respectively under the $`\sigma _+`$ and $`\sigma _{}`$ photoexcitation. The squared moduli of the corresponding matrix elements are given by

$$|(\widehat{𝐯}𝐞)_{fi}|^2=\frac{1}{8}\left[\frac{\gamma }{\mathrm{}}k_z\left(\frac{1}{k_{,0}}\frac{1}{k_{,1}}\right)\right]^2=\frac{1}{32}\left(\frac{\gamma }{\mathrm{}}\frac{k_z}{k_{,0}}\right)^2,$$
(18)
where we took into account that $`k_{,1}=2k_{,0}`$. The transitions under consideration are forbidden at the $`𝐊`$ and $`𝐊^{}`$ points but become allowed for $`k_z,k_z^{}0`$. The squared moduli of the optical matrix element is given by

$$|V_{fi}|^2=\left(\frac{e}{c}A\right)^2|(\widehat{𝐯}𝐞)_{fi}|^2=\frac{2\pi e^2I}{\omega ^2cn_\omega }\frac{1}{32}\left(\frac{\gamma }{\mathrm{}}\frac{k_z}{k_{,0}}\right)^2,$$
(19)
where $`A=|𝐀|`$, $`I`$ is the light intensity and $`n_\omega `$ is the refractive index of the medium. In the following we consider a free-standing nanotube and assume $`n_\omega =1`$.

It should be stressed that the linear-optics approximation is valid as long as $`\mathrm{}^1|V_{fi}|(2\tau _p)^1`$, otherwise one has to take into account the saturation of the absorption. Another important point is that the depolarization effect  can be neglected provided

$$\left|\frac{4\pi \sigma _{}}{L\omega }\right|1,$$
(20)
where $`\sigma _{}`$ is the conductivity at the frequency $`\omega `$ defined as

$`\mathrm{}\omega W=2\sigma _{}\left({\displaystyle \frac{\omega }{c}}A\right)^2`$

with $`W`$ being the optical transition rate.

## III Circular photogalvanic effect

Physically, the CPGE can be considered as a transformation of the photon angular momenta into a translational motion of free charge carriers. It is an electron analog of mechanical systems which transmit rotatory motion to linear one like a screw tread or a plane with a propeller. Phenomenologically, in the case of chiral CNs it is described by

$$j_{CPGE,z}=\mathrm{\Gamma }i(𝐄\times 𝐄^{})_z,$$
(21)
where $`j_{CPGE,z}`$ is the dc photocurrent, $`\mathrm{\Gamma }`$ is a real coefficient, E is the complex amplitude of the electric field of the electromagnetic wave and, for the transverse wave,

$$i(𝐄\times 𝐄^{})=P_{circ}E_0^2\widehat{o}$$
(22)
with $`E_0,P_{circ}`$, $`\widehat{o}`$ being respectively the electric field amplitude $`|𝐄|`$, the degree of the circular polarization of light and the unit vector pointing in the direction of light propagation. The photocurrent (21) reverses its direction under inversion of the light circular polarization and vanishes for linearly-polarized excitation.

Usually the microscopic theory of natural optical activity in bulk semiconductors  as well as the theory of CPGE  is based on allowance of spin-dependent linear in $`𝒌`$ terms $`\beta _{lm}\sigma _lk_m`$ in the electron effective Hamiltonian, where $`𝒌`$ is the electron wavevector and $`\sigma _l`$ are the Pauli spin matrices. The real coefficients $`\beta _{lm}`$ form a pseudotensor subjected to the same symmetry restriction as the pseudotensors describing the optical activity and CPGE. In CNs the spin-orbit interaction is negligible and the similar role is played by the coupling between the orbital angular momentum $`n`$ and the wave vector $`k_z`$ as described by Eqs. (7,9).

The transfer of photon angular momenta into an electric current along the principal axis of a chiral CN can be described by the standard equation for the current

$$j_{CPGE,z}=e\underset{n,k_z,s}{}v_c(n,k_z,s)f_c(n,k_z,s)+e\underset{n,k_z,s}{}v_h(n,k_z,s)f_h(n,k_z,s),$$
(23)
where $`e`$ is the elementary charge ($`e>0`$), the index $`s`$ labels the valleys $`K`$ and $`K^{}`$, $`v_c(n,k_z,s)=\mathrm{}^1(dE_c(n,k_z,s)/dk_z)`$ is the group velocity and $`f_c(n,k_z,s)`$ is the nonequilibrium steady-state distribution function for electrons in the conduction band. The similar quantities for holes in the valence band $`v`$ have the subscript $`h`$. Note that they are related with the corresponding quantities in the electron representation of the valence states by $`v_h(n,k_z,K)=v_v(n,k_z,K^{})`$, $`f_h(n,k_z,K)=1f_v(n,k_z,K^{})`$.

In the following we will consider the case where elastic scattering processes are more effective than the inelastic ones. Then one can apply the standard procedure of solving the kinetic equation and decompose the distribution function $`f_m`$ $`(m=c,h)`$ into the contributions

$$f_m^\pm (n,k_z,s)=\frac{1}{2}[f_m(n,k_z,s)\pm f_m(n,\stackrel{~}{k}_z,s)]$$
(24)
that are even and odd with respect to the change of $`k_z`$ by $`\stackrel{~}{k}_z`$ where $`\stackrel{~}{k}_z`$ belongs to the same valley and satisfies the equation $`E_m(n,\stackrel{~}{k}_z,s)`$ $`=E_m(n,k_z,s)`$. Since the even contribution in Eq. (24) is in fact a function of the electron energy, it nullifies the elastic scattering integral and also makes no contribution to the current. Introducing the momentum relaxation times $`\tau _p^{(f,i)}`$ we can present the photocurrent as

$$j=e\underset{n_f,n_i,k_z,s}{}\left[v_c(n_f,k_z,s)\tau _p^{(f)}v_c(n_i,k_z,s)\tau _p^{(i)}\right]W_{cc}(n_f,n_i,k_z,s)$$
(25)
for optical transitions $`(c,n_i,s)`$ $`(c,n_f,s)`$ between the conduction subbands and in a similar way for transitions between the valence subbands or for interband transitions, where $`n_f,n_i`$ are the angular momentum components in the final and initial states. The transition rate is given by

$`W_{cc}(n_f,n_i,k_z,s)={\displaystyle \frac{2\pi }{\mathrm{}}}|V_{fi}|^2f_c^0[E_c(n_i,k_z,s)]\delta [E_c(n_f,k_z,s)E_c(n_i,k_z,s)\mathrm{}\omega ].`$

Here $`f_c^0`$ is the equilibrium distribution function and we assume that in equilibrium the upper subband $`(c,n_f,s)`$ is unoccupied.

In this section we take a chiral CN with the parameter $`\nu =1`$, assume that the tube is $`n`$-doped and consider the intersubband photoexcitation of electrons from the lowest conduction subbands $`(c,n=0,s)`$ to the first higher subbands $`(c,n=1,K)`$ and $`(c,n=1,K^{})`$ (see Fig. 2). In order to obtain compact analytical results we consider near-edge optical transitions with the light frequency $`\omega `$ satisfying the condition

$$|\mathrm{}\omega \mathrm{\Delta }_{10}|\mathrm{\Delta }_{10},$$
(26)
where $`\mathrm{\Delta }_{10}`$ is the energy separation between the subbands $`(c,0,K)`$ and $`(c,1,K)`$ given by, see Eqs. (8,11),

$`\mathrm{\Delta }_{10}={\displaystyle \frac{1}{2}}(\mathrm{\Delta }_1\mathrm{\Delta }_0)={\displaystyle \frac{2\pi \gamma }{3L}}.`$

In this case $`|k_z||k_{}|`$ and one can use the approximate equations (9)–(13). Rewriting Eq. (9) in the form

$$E_c(n,k_z;K)=\frac{\mathrm{\Delta }_n}{2}\frac{m_n\beta _n^2}{2\mathrm{}^2}+\frac{\mathrm{}^2(k_z+\kappa _n)^2}{2m_n}$$
(27)
with $`\kappa _n=m_n\beta _n/\mathrm{}^2`$ we conclude that $`\stackrel{~}{k_z}`$ entering Eq. (24) equals to $`k_z2\kappa _n`$. We ignore the small frequency region where the terms linear-in-$`k_z`$ exceed or are comparable with the quadratic terms in-$`k_z`$ in Eq. (9) and assume the ratios $`\ae _n(k_z)`$ $`=\beta _nk_z/(\mathrm{}^2k_z^2/2m_n)`$ for $`n=0,1`$ to be small which is valid if

$`|k_z|2m_n\beta _n/\mathrm{}^2\text{or}|\mathrm{}\omega \mathrm{\Delta }_{10}|2m_n\beta _n^2/\mathrm{}^2.`$

Taking into account Eq. (18) and retaining the first-order terms in $`\ae _n`$ we can write the photocurrent as a sum of four contributions

$$j_{CPGE}=eW_{1,0}(l_v+l_m+l_\tau +l_f).$$
(28)
Here $`W_{1,0}`$ is the transition probability rate per unit length calculated neglected the terms linear-$`k`$:

$$W_{1,0}=\frac{2\pi }{\mathrm{}}\frac{2\pi e^2I}{\omega ^2cn_\omega }\frac{1}{32}\left(\frac{\gamma }{\mathrm{}}\frac{k_z}{k_{,0}}\right)^2f_c^0(E_0)g_{10}(\mathrm{\Delta }_{10}\mathrm{}\omega ),$$
(29)
$`I`$ is the light intensity in units $`energylength^1time^1`$, the one-dimensional reduced density of states equals to

$`g_{10}(E)=2\times {\displaystyle \underset{k_z}{}}\delta ({\displaystyle \frac{\mathrm{}^2k_z^2}{2\mu _{10}}}E)={\displaystyle \frac{1}{\pi }}\left({\displaystyle \frac{2\mu _{10}}{\mathrm{}^2E}}\right)^{1/2}\theta (E),`$

the factor of two makes allowance for the spin degeneracy, $`\theta (x)`$ is the step function equal to 0 if $`x<0`$ and 1 if $`x>0`$, $`\mu _{10}^1`$ is the inverse reduced effective mass $`m_1^1m_0^1`$, (since $`m_1=2m_0>m_0`$ a value of $`\mu _{10}=2m_0`$ is positive and $`g_{10}(E)`$ is defined for negative values of $`E`$), and $`f_c^0(E_0)`$ is the value of the equilibrium distribution function at the energy $`E_0=`$ $`(\mathrm{}^2k_z^2/2m_0)`$ $`=(\mu _{10}/m_0)(\mathrm{\Delta }_{10}\mathrm{}\omega )`$ $`=2(\mathrm{\Delta }_{10}\mathrm{}\omega )`$. The lengths $`l_v,l_m,l_\tau ,l_f`$ in Eq. (28) are related to the photoexcitation asymmetry arising due to the $`k_z`$-dependence of the velocity and density of states ($`l_v`$), of the squared matrix element ($`l_m`$), of the momentum relaxation time ($`l_\tau `$) and of the equilibrium distribution function ($`l_f`$). For the optical transitions under consideration the straightforward derivation results in

$$l_v=\frac{3\beta _0}{\mathrm{}}(\tau _p^{(1)}\tau _p^{(0)}),l_m=\frac{2\beta _0}{\mathrm{}}(\tau _p^{(1)}2\tau _p^{(0)}),$$
(30)
$`l_\tau ={\displaystyle \frac{6\beta _0}{\mathrm{}}}\left(\tau _p^{(1)}{\displaystyle \frac{d\mathrm{ln}\tau _p^{(1)}}{d\mathrm{ln}E_1}}\tau _p^{(0)}{\displaystyle \frac{d\mathrm{ln}\tau _p^{(0)}}{d\mathrm{ln}E_0}}\right),l_f={\displaystyle \frac{3\beta _0}{\mathrm{}}}(2\tau _p^{(0)}\tau _p^{(1)}){\displaystyle \frac{\mathrm{\Delta }_{10}\mathrm{}\omega }{k_BT}}[1f_0(E_0)].`$

Obviously, the momentum relaxation time $`\tau _p^{(1)}`$ is shorter than $`\tau _p^{(0)}`$ because a photoelectron excited to the subband ($`(c,n=1`$) can be readily scattered to the subband ($`(c,n=0`$).

The circular photocurrent can be estimated as

$$j_{CPGE}eW_{1,0}\frac{\beta _0}{\mathrm{}}\tau _pP_{circ}$$
(31)
and for intensities at the absorption saturation

$`j_{CPGE}{\displaystyle \frac{2\pi \mathrm{sin}3\theta }{\sqrt{3}}}{\displaystyle \frac{e}{\tau _p}}{\displaystyle \frac{a}{L}}\left({\displaystyle \frac{\mathrm{\Delta }_{10}}{\mathrm{\Delta }_{10}\mathrm{}\omega }}\right)^{1/2}.`$

Taking $`\gamma =`$ 6.5 eV$``$Å, $`a`$ = 2.5 Å, $`\nu =1`$, $`L=`$ 135 Å, $`\mathrm{sin}3\theta =`$ 0.7 we have $`\mathrm{\Delta }_{10}=0.1`$, $`m_0=0.017m`$, where $`m`$ is the bare electron mass, $`\beta _0/\mathrm{}=`$ 1.1$`\times `$10<sup>6</sup> cm/s. Then for $`\tau _p=`$ 10<sup>-11</sup> s, $`\mathrm{\Delta }_{10}\mathrm{}\omega =0.1\mathrm{\Delta }_{10}`$, and $`f_c^0(E_0)1`$ we obtain $`j_{CPGE}10^9`$ A. While making this estimation we assumed the difference $`\tau _p^{(0)}\tau _p^{(1)}`$ and the electron-electron scattering time $`\tau _{ee}`$ to be comparable with $`\tau _p^{(0)}`$. It is worth to mention that a value of the photocurrent in recently discovered crystals of CNs  will be significantly enhanced compared to a single CN.

We conclude the section by comparing the CPGE described by Eq. (31) with the photon drag (PD) effect which exists in crystals of arbitrary symmetry and is independent on the sign of the circular polarization. The PD current is estimated as

$$j_{PD}eW_{1,0}\frac{\mathrm{}q}{m_0}\tau _p,$$
(32)
where $`q`$ is the photon wave vector (in vacuum $`q=\omega /c`$). Thus, for $`\mathrm{}\omega =`$ 0.1 meV we have $`j_{CPGE}/j_{PD}\beta _0m_0/(\mathrm{}^2q)3`$.

In this section we presented both the detailed calculation and estimation by an order of magnitude for the CPGE. In the next chapters we restrict ourselves only to analytical estimations of other effects while their detailed consideration can be given elsewhere.

## IV Magneto-induced linear photogalvanic effect.

In addition to the circular PGE, in noncentrosymmetric media a photocurrent of another kind can be induced by the electro-magnetic wave. This is called the linear photogalvanic effect (LPGE) and described by a third-rank tensor, $`\chi _{ijk}`$, symmetrical with respect to the interchange of the indices $`j`$ and $`k`$. Thus, for the LPGE one has

$$j_{LPGE,i}=\chi _{ijl}I(e_je_l^{}+e_j^{}e_l)/2.$$
(33)
Ideal CNs are unpolar with their principal axis, $`z`$, being two-sided which forbids the photocurrent (33). In B<sub>x</sub>C<sub>y</sub>N<sub>z</sub> nanotubes (BNs) the symmetry is reduced, the axis $`z`$ is polar and the LPGE becomes allowed . We show here that the linear photocurrent can be induced in an ideal CN in the presence of an external magnetic field $`𝐁z`$. Phenomenologically the magneto-induced LPGE can be written as

$$j_{M\text{-}LPGE,z}=IB_z[\mathrm{\Lambda }_{}|e_z|^2+\mathrm{\Lambda }_{}(|e_x|^2+|e_y|^2)]$$
(34)
and determined by two linearly independent coefficients $`\mathrm{\Lambda }_{},\mathrm{\Lambda }_{}`$.

For the interband transitions $`(v,0)(c,0)`$ excited in an undoped CN by the linearly polarized light, $`𝐞z`$, one has the following estimation

$$j_{M\text{-}LPGE,z}eW_{0,0}\frac{\beta _0}{\mathrm{}}\tau _p\nu \frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}.$$
(35)
The estimation follows if we take into account the quadratic term in the expansion of $`h`$ in powers of $`ka`$. Due to this term the squared matrix element of the optical transition has an odd contribution, the ratio of the odd contribution to the main even contribution being proportional to $`ak_z\mathrm{sin}3\theta `$. In the magnetic field the band gaps $`\mathrm{\Delta }_{00}(K),\mathrm{\Delta }_{00}(K^{})`$ differ due to the difference of $`|k_{}|`$ and $`|k_{}^{}|`$ at $`n=0`$ (See Eq. (14) and Fig.3 where the scheme of the optical transitions is shown. The different thickness of lines in Fig.3, which correspond to the transitions of electrons with different momenta indicate that they probabilities are different). This leads to the relative difference in the transition rates for the $`K`$ and $`K^{}`$ valleys proportional to

$`{\displaystyle \frac{\mathrm{\Delta }_{00}}{\mathrm{}\omega \mathrm{\Delta }_{00}}}\nu {\displaystyle \frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}}.`$

Thus the linear magneto-photocurrent induced by the light polarized along the principal axis $`z`$ can be estimated as

$`j_{MLPGE,z}eW_{0,0}ak_z\mathrm{sin}3\theta {\displaystyle \frac{\mathrm{}k_z}{m_0}}{\displaystyle \frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}}{\displaystyle \frac{\mathrm{\Delta }_{00}}{\mathrm{}\omega \mathrm{\Delta }_{00}}}\tau _p.`$

Since

$`k_z{\displaystyle \frac{\mathrm{}k_z}{m_0}}{\displaystyle \frac{\mathrm{}\omega \mathrm{\Delta }_{00}}{\mathrm{}}}`$

and $`\mathrm{\Delta }_{00}\gamma k_{,0}`$, $`\beta _0a\gamma \mathrm{sin}3\theta `$ we obtain

$`j_{MLPGE,z}eW_{0,0}{\displaystyle \frac{\mathrm{\Delta }_{00}a}{\mathrm{}}}\tau _p\mathrm{sin}3\theta {\displaystyle \frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}}`$

and finally arrive at Eq. (35). The same order of magnitude for $`j_{MLPGE,z}`$ is obtained if we ignore the quadratic terms in $`h(𝐤)`$ but include the cubic-$`k_z`$ terms in the energy dispersion Eq. (7). Above we assumed $`\mathrm{\Phi }`$ to be much smaller than $`\mathrm{\Phi }_0`$. For large values of $`\mathrm{\Phi }`$ the linear magneto-photocurrent is a periodic function of the ratio $`\mathrm{\Phi }/\mathrm{\Phi }_0`$. While preparing the manuscript we learned about a similar work  on the magneto-induced linear photovoltaic effect.

## V Magneto-induced dc electric current <br>quadratic in the electric field

Eq.(35) for magneto-induced linear PGE holds at high frequencies $`\omega >\tau _p^1`$. This effect, however, does not vanish even in the case $`\omega =0`$: the chiral symmetry allows existence of a current which is quadratic in the electric field and linear in the external magnetic field. In the case of bulk metals this effect has been observed in .

In the case of chiral CN a general expression for dc current has the form

$$j_z=\sigma E_z+\mathrm{\Lambda }E_z^2B_z,$$
(36)
where $`\sigma =e^2n\tau _p/m_0`$ is the linear Drude conductivity, $`\tau _p`$ is the momentum relaxation time and $`m_0`$ is the effective mass in the lowest conduction subband, and we assume the Fermi level lies below the bottom of the subbands $`(c,\pm 1)`$. Note that the magneto-chiral coefficient $`\mathrm{\Lambda }`$ is nonzero only in chiral CNs.

Qualitatively, the nature of the magneto-chiral correction can be understood as follows: the electric field accelerates electrons (in $`n`$-doped samples) and creates a nonequilibrium electron distribution. In this section we assume that the elastic electron relaxation rate is much larger than the inelastic one , which is associated with the electron-phonon scattering. Than in the first approximation in the ratio between these rates the electron distribution function depends only on the electron energy. It should be determined from the balance of the energy supplied to the electron system by the electric field and the energy transfered by electrons to the acoustic phonons. It is important that the distribution functions which depend only on the electron energy correspond to zero current. To get a nonzero value of the dc current we have to take into account that in the case of chiral CN the electron-phonon inelastic scattering rate depends on the direction of the electron momentum. As a result, there is a correction to the electron distribution function which is odd-in-$`k_z`$, the value of which is proportional to the ratio between the inelastic and elastic relaxation rates. In other words, the electron-phonon inelastic processes convert a currentless distribution of the electron gas into a distribution characterized by a nonzero electric current, proportional to $`E^2`$.

An antisymmetric part of the probability rate for the electron inelastic scattering can be found if we use the symmetry considerations and write, in addition to the 2$`\times `$2 Hamiltonian (3), the operator of the electron-phonon interaction for a graphen sheet near the point K

$$V_{ephon}=\left(\begin{array}{cc}\mathrm{\Xi }_0u& \mathrm{\Xi }u_+\\ \mathrm{\Xi }u_{}& \mathrm{\Xi }_0u\end{array}\right).$$
(37)
Here $`u=u_{11}+u_{22}`$, $`u_\pm =u_{11}u_{22}\pm iu_{12}`$, $`u_{lm}`$ is the in-plane strain tensor in the axes $`x_1,x_2`$ and $`\mathrm{\Xi }_0,\mathrm{\Xi }`$ are the deformation potential constants. In the tight-binding model $`\mathrm{\Xi }=\mathrm{\Xi }_0/2`$. Let $`u_{zz}`$ be a uniform strain in a single CN. Then the strain-induced shift of the electron energy in the subband $`(c,0)`$ in the $`K`$ valley is equal to

$$\epsilon _u(\theta ;K)=\left[\mathrm{\Xi }_0\frac{\sqrt{3}}{2}\mathrm{\Xi }\left(\frac{k_{,0}}{k_0}\mathrm{cos}3\theta +\frac{k_z}{k_0}\mathrm{sin}3\theta \right)\right]u_{22}$$
(38)
and $`\epsilon _u(\theta ;K^{})=\epsilon _u(\theta ;K)`$. Here $`k_0=\sqrt{k_{,0}^2+k_z^2}`$. It follows from the above equation that the ratio of the part odd-in-$`k_z`$ to the part even-in-$`k_z`$ for the rate of electron scattering by a phonon can be estimated as

$$\eta (k_z)\frac{W^{()}}{W^{(+)}}\frac{k_z}{k_0}\mathrm{sin}3\theta .$$
(39)
At zero magnetic field the asymmetry induced by inelastic processes in the $`k_z`$ distribution in the valley $`K`$ is compensated by the asymmetry in the $`K^{}`$ valley and the quadratic-in-$`E_z`$ current is zero. The magnetic field shifts the bottoms of the $`K`$ and $`K^{}`$ valleys relative to each other (See Eqs. (9,13)), the equilibrium electron densities in these valleys become different leading to a current contribution proportional to $`E_z^2B_z`$.

In contrast to the previous consideration of free-standing CNs we consider here a CN that lies on a solid surface and is effected by 3D acoustic phonons of the solid. It allows to uncouple the momentum and energy conservation laws in electron-phonon scattering processes. Then the correction to the dc current proportional to $`E^2B_z`$ is estimated as

$$\delta j_zeW^{(+)}\eta (\overline{k}_z)\zeta [\tau _p(k_{f,z})v(k_{f,z})\tau _p(k_{i,z})v(k_{i,z})],$$
(40)
where $`\delta j_z`$ in the part of the current proportional to $`E_z^2`$,

$$\zeta \frac{\gamma k_{,0}}{E_F}\frac{\mathrm{\Phi }}{\mathrm{\Phi }_0},$$
(41)
is the relative difference of the electron equilibrium densities in the valleys $`K`$ and $`K^{}`$ induced by the magnetic field, see Eqs. (11,14), $`E_F`$ is the Fermi energy referred to the conduction band bottom, $`\tau _p`$ is the momentum relaxation time, $`v(k_z)=\mathrm{}k_z/m^{}`$ is the electron velocity, $`k_{f,z}`$ and $`k_{i,z}`$ are the initial and final values of $`k_z`$ in the inelastic scattering process, we assume the difference $`k_{f,z}k_{i,z}`$ to be much smaller than $`\overline{k}_z=(k_{f,z}+k_{i,z})/2`$; the angle brackets mean the averaging over $`k_z`$. A value of $`W^{(+)}`$ is estimated from the balance of energy as

$$k_BTW^{(+)}=\sigma E_z^2,$$
(42)
where $`k_B`$ is the Boltzmann’s constant and we take into account that the typical electron energy change under scattering is of the order of the thermal energy or, analytically,

$`\mathrm{}^2\overline{k}_z(k_{i,z}k_{f,z})/m^{}k_BT.`$

Here we consider the degenerate electron gas and assume $`k_BT`$ to be much smaller than the Fermi energy $`E_F`$. Then Eq. (40) can be reduced to

$$\delta j_ze\sigma E^2\mathrm{sin}3\theta \tau _p\frac{\gamma }{\mathrm{}E_F}\frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}$$
(43)
or

$$\frac{\delta j_z}{j_z}\mathrm{sin}3\theta \frac{eE\tau _p}{\mathrm{}}\frac{\gamma }{E_F}\frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}.$$
(44)
We would like to mention that in the approximation of purely elastic scattering $`\delta j_z`$ is zero. Nevertheless Eqs. (43,44) is independent of inelastic scattering rate. This is because we considered the case when the sample length is larger than the inelastic diffusion length, $`\sqrt{D_p\tau _{in}}`$, where $`D_pv_F^2\tau _p`$ is the elastic diffusion coefficient and $`v_F`$ is the Fermi velocity, and we used the equation (42). In the opposite limit the value of the current is proportional to $`\tau _{in}^1`$.

Assuming, for example, that the voltage bias on the sample is $`U0.01V`$, $`E_F0.1eV`$, $`\tau _p\gamma /\mathrm{}L_{CN}`$ and, hence, $`E_z\tau _p\gamma /\mathrm{}U`$, $`\mathrm{\Phi }/\mathrm{\Phi }_010^2`$ (for $`B_z=`$ 10 T, $`L=70\AA `$), we get the estimate $`\delta j_z/j_z10^3`$.

## VI Chirality effects in optical spectroscopy

In this section we presen estimates for two other effects of chirality in optical spectroscopy of CNs: the natural circular dichroism and the magneto-chiral dichroism.

Let us start with the natural circular dichroism appearing as a difference in the interband or intersubband optical transition rates for the $`\sigma _+`$ and $`\sigma _{}`$ light polarizations. As mentioned above, in bulk semiconductors the theory of natural optical activity is based on allowance for coupling between the electron spin and wavevector. Contrary to the approach , we ignore the spin-orbit interaction in CNs because it is negligible for C atoms and take into account the coupling between the angular momentum $`n`$ and the wavevector $`k_z`$. We assume the circularly polarized light to propagate along the principal axis $`z`$ of a chiral nanotube with $`\nu =1`$ and consider the interband optical transitions $`(v,0,K)`$ $`(c,1,K)`$, $`(v,1,K^{})`$ $`(c,0,K^{})`$ allowed for the $`\sigma _+`$ polarization and $`(v,1,K)`$ $`(c,0,K)`$, $`(v,0,K)`$ $`(c,1,K)`$ allowed for the $`\sigma _{}`$ polarization. The energy conservation law reads $`E_c(n_f,k_z+q;K)`$ $`E_v(n_i,k_z;K)=\mathrm{}\omega `$, $`E_c(n_f,k_z^{}+q;K^{})`$ $`E_v(n_i,k_z^{};K^{})=\mathrm{}\omega `$. Due to the presence of the light wavevector $`q`$ in these equations and the linear-in-$`k_z`$ terms in the energy dispersion given by Eq. (9), the absorption probability rates $`W(\sigma _\pm )`$ for the $`\sigma _\pm `$ polarization differ and the relative difference is given by

$$\frac{W(\sigma _+)W(\sigma _{})}{W(\sigma _+)+W(\sigma _{})}\frac{\beta q}{\mathrm{}\omega \mathrm{\Delta }_{10}^{cv}},$$
(45)
where $`\mathrm{\Delta }_{10}^{cv}`$ is the band gap between $`(c,1,K)`$ and $`(v,0,K)`$ subbands. For comparison we present also an estimation for the circular dichroism due to the Faraday effect in the magnetic field $`𝐁z`$:

$$\frac{W(\sigma _+)W(\sigma _{})}{W(\sigma _+)+W(\sigma _{})}\frac{\mathrm{\Delta }_{10}^{cv}}{\mathrm{}\omega \mathrm{\Delta }_{10}^{cv}}\frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}.$$
(46)
If the condition (20) is not satisfied the depolarization effect can substantially renormalize the dichroism, however the ratio of the relative differences given by Eqs. (45,46) holds unchanged.

Let us now turn to an estimate of the magnitude of the magneto-chiral dichroism which manifests itself in the dependence of the light absorption coefficient on the product $`q_\alpha B_\beta `$. Here $`q_\alpha `$ and $`B_\beta `$ are components of the light wavevector q and the magnetic field B , (see also  and references therein). In chiral CNs the magneto-chiral dichroism can be described by the following contribution to the absorption or emission probability rate

$$\delta W=B_zq_z[Q_{}|e_z|^2+Q_{}(|e_x|^2+|e_y|^2)].$$
(47)
For the interband transitions $`(v,0,s)(c,0,s)`$ ($`s=K,K^{}`$) one has $`Q_{}0`$, $`Q_{}=0`$ and $`\delta W_{00}`$ $`B_zq_z|e_z|^2`$ $`=B_z\mathrm{cos}\theta _0\mathrm{sin}^2\theta _0`$, where $`\theta _0`$ is the angle between the nanotube axis $`z`$ and the propagation direction of the light linearly polarized in the plane containing the vector $`𝐪_0`$ and the axis $`z`$. For the transitions $`(v,0)(c,0)`$ in one valley, say the valley $`K`$, the ratio $`\delta W_{00}/W_{00}`$ is given by $`\beta q_z/(\mathrm{}\omega \mathrm{\Delta }_{00})`$ similarly to the previous consideration. At zero magnetic field the transitions in the valley $`K^{}`$ lead to a contribution to $`\delta W_{00}`$ of the opposite sign and the net value of $`\delta W_{00}`$ vanishes. An external magnetic field breaks the compensation, and the imbalance in contributions from the $`K`$ and $`K^{}`$ valleys is governed by a value of $`[\mathrm{\Delta }_{00}/(\mathrm{}\omega \mathrm{\Delta }_{00})]`$$`(\mathrm{\Phi }/\mathrm{\Phi }_0)`$. As a result we obtain

$$\frac{\delta W_{00}}{W_{00}}\frac{\beta q_z\mathrm{\Delta }_{00}}{(\mathrm{}\omega \mathrm{\Delta }_{00})^2}\frac{\mathrm{\Phi }}{\mathrm{\Phi }_0}.$$
(48)
## VII conclusion

All chirality induced effects considered above are not specific for chiral CN. In principle they should be present in any mesoscopic system lacking the mirror-reflection symmetry. In particular they should be present in mesoscopic disordered metallic samples where all possible symmetries are broken. Some of these effects have been already discussed .

Another system where the effects considered above can manifest themselves is a DNA molecule, which electron transport properties have been investigated recently . Although usually DNA have large resistance, we would like to mention in this connection that the photoinduced electron transport effects can be measured even in diamond .

The photogalvanic effects should also exist in Josephson junctions with no mirror-reflection symmetry. For example, it could be either superconductor-carbon nanotube-superconductor or superconductor-disordered metal-superconductor junctions. The qualitative difference of the photogalvanic effects in metals is that the circularly polarized light will induce both the normal and superfluid components of the current through the junctions.

The theory presented above neglects effects of electron-electron interaction including the excitonic and Luttinger-liquid effects. In this respect we would like to mention that $`\mathrm{\Phi }`$-dependent terms in the electron spectrum will suppress the dip in the energy dependence of the density of states for interacting electrons in one dimension . In disordered samples the magnitude of this effect should match results  for diffusive quasi-one-dimensional conductors.

Finally we would like to mention an effect which is inverse to the circular and linear photogalvanic effects. Namely, in the absence of magnetic field the dc electric current in a CN should induce the circular polarization of the photoluminescence. In the presence of an external magnetic field parallel to a CN, the electric current $`j_z`$ should induce a change in the photoluminescence intensity proportional to $`j_zB_z`$.

The work of B.Spivak was supported by Division of Material Sciences, U.S. National science foundation under contract No. DMR-9205144. The work of E.L.Ivchenko was supported by programmes of Russian Academy and Ministry of Sciences. We would like to acknowledge useful discussions with D. Cobden, C. Kane, L. Levitov and C. Markus.


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# Contents

## 1 Introduction

Let $`SmCor(k)`$ be the category of smooth finite correspondences over a field $`k`$. Denote by $`𝐆_m`$ the scheme $`𝐀^1\{0\}`$. One defines the sheaf with transfers $`S_t^1`$ by the condition that $`𝐙_{tr}(𝐆_m)=S_t^1𝐙`$ where $`𝐙`$ is split off by the projection to the point and the point $`1`$. For any scheme $`X`$ consider the sheaf with transfers

$$F_X:YHom(S_t^1𝐙_{tr}(Y),S_t^1𝐙_{tr}(X))$$

We prove that the obvious map $`𝐙_{tr}(X)F_X`$ defines a quasi-isomorphism of singular simplicial complexes

$$C_{}(𝐙_{tr}(X))C_{}(F_X)$$

as complexes of presheaves i.e. for any $`Y`$ the map of complexes of abelain groups

$$C_{}(𝐙_{tr}(X))(Y)C_{}(F_X)(Y)$$

is a quasi-isomorphism. We then deduce from this result the cancellation theorem which asserts that if $`k`$ is a perfect field then for any $`K,L`$ in $`DM_{}^{eff}(k)`$ the map

$$Hom(K,K^{})Hom(K(1),K^{}(1))$$

is bijective.

This result was previously known in two particular situations. For varieties over a field $`k`$ with resolution of singularities it was proved in . For $`K^{}`$ being the motivic complex $`𝐙(n)[m]`$ and any field $`k`$ it was proved in . Both proofs are very long.

The main part of our argument does not use the assumption that we work with smooth schemes over a field and we give it for separated schemes of finite type over a noetherian base. To be able to do it we define in the first section the category of finite correspondences for separated schemes of finite type over a base. The definition is a straightforward generalization of the definition for schemes over a field based on the constructions of  and can be skipped. In the second section we define intersection of relative cycles with Cartier divisors and prove the properties of this construction which we need. In the third we prove our main theorem 4.6 and deduce from it the cancellation theorem over perfect fileds 4.10.

In this paper we say “a relative cycle” instead of “an equidimensional relative cycle”. All schemes are separated. The letter $`S`$ is typically reserved for the base scheme which is assumed to be noetherian. All the standard schemes $`𝐏^1`$, $`𝐀^1`$ etc. are over $`S`$. When no confusion is possible we write $`XY`$ instead of $`X\times _SY`$.

## 2 Finite correspondences

For a scheme $`X`$ of finite type over a noetherian scheme $`S`$ we denote by $`c(X/S)`$ the group of finite relative cycles on $`X`$ over $`S`$. In  this group was denoted by $`c_{equi}(X/S,0)`$. If $`S`$ is regular or if $`S`$ is normal and the characteristic of $`X`$ is zero, $`c(X/S)`$ is the free abelian group generated by closed irreducible subsets of $`X`$ which are finite over $`S`$ and surjective over a connected component of $`S`$. For the general definition see \[3, after Lemma 3.3.9\]. A morphism $`f:S^{}S`$ defines the pull-back homomorphism $`c(X/S)c(XS^{}/S^{})`$ which we denote by $`cycl(f)`$.

For two schemes $`X,Y`$ of finite type over $`S`$ we define the group $`c(X,Y)`$ of finite correspondences from $`X`$ to $`Y`$ as $`c(XY/X)`$.

Let us recall the following construction from \[3, §3.7\]. Let $`X^{}XS`$ be morphisms of finite type, $`𝒲`$ a relative cycle on $`X^{}`$ over $`X`$ and $`𝒵`$ a relative cycle on $`X`$ over $`S`$. Then one defines a cycle $`Cor(𝒲,𝒵)`$ on $`X^{}`$ as follows. Let $`Z_i`$ be the components of the support of $`𝒵`$ present with multiplicites $`n_i`$ and $`e_i:Z_iX`$ the corresponding closed embeddings. Let $`e_i^{}:Z_i\times _XX^{}X^{}`$ denote the projections. We set

$$Cor(𝒲,𝒵)=\underset{i}{}n_i(e_i^{})_{}cycl(e_i)(𝒲)$$

where $`(e_i^{})_{}`$ is the (proper) push-forward on cycles.

Let $`X`$, $`Y`$ be schemes of finite type over $`S`$ and

$$fc(X,Y)=c(XY/X)$$

$$gc(Y,Z)=c(YZ/Y)$$

finite correspondences. Let

$$p_X:XYY$$

$$p_Y:XYZXZ$$

be the projections. We define the composition $`gf`$ by the formula:

$$gf=(p_Y)_{}Cor(cycl(p_X)(g),f)$$
(2.1)
This operation is linear in both arguments and thus defines a homomorphism of abelian groups

$$c(X,Y)c(Y,Z)c(X,Z)$$

The lemma below follows immediately from the definition of $`Cor(,)`$ and the fact that the (proper) push-forward commutes with the $`cycl()`$ homomorphisms (\[3, Prop. 3.6.2\]).

###### Lemma 2.1

Let $`YXS`$ be a sequence of morphisms of finite type, $`p:YY^{}`$ a morphism over $`X`$, $`𝒴Cycl(Y/X,r)𝐐`$ and $`𝒳Cycl(X/S,s)𝐐`$. Assume that $`p`$ is proper on the support of $`𝒴`$. Then

$$p_{}Cor(𝒴,𝒳)=Cor(p_{}(𝒴,𝒳)).$$

###### Lemma 2.2

For any $`fc(X,Y)`$, $`gc(Y,Z)`$, $`hc(Z,T)`$ one has

$$(hg)f=h(gf).$$

Proof: Consider the following diagram

$$\begin{array}{ccccccccc}XT& \stackrel{4}{}& XYT& & YT& & & & \\ 7& & 8& & 2& & \\ XZT& \stackrel{9}{}& XYZT& & YZT& & ZT& & T\\ & & & & & & & & & & \\ XZ& \stackrel{5}{}& XYZ& \stackrel{9}{}& YZ& \stackrel{1}{}& Z& & \\ & & & & & & & & & & \\ & & XY& \stackrel{3}{}& Y& & & & \\ & & & & & & & & & & \\ & & X\end{array}$$

where the morphisms are the obvious projections. Note that all the squares are cartesian. We will also use the projection $`6:XZZ`$.

We have $`fc(XY/X)`$, $`gc(YZ/Y)`$ and $`hc(ZT/Z)`$. The compositions are given by:

$$gf=5_{}Cor(cycl(3)(g),f)$$

$$hg=2_{}Cor(cycl(1)(h),g)$$

$$(hg)f=4_{}Cor(cycl(3)(hg),f)=4_{}Cor(cycl(3)(2_{}Cor(cycl(1)(h),g)),f)$$

$$h(gf)=7_{}Cor(cycl(6)(h),gf)=7_{}Cor(cycl(6)(h),5_{}Cor(cycl(3)(g),f))$$

We have:

$$4_{}Cor(cycl(3)(2_{}Cor(cycl(1)(h),g)),f)=$$

$$=4_{}Cor(8_{}cycl(3)Cor(cycl(1)(h),g),f)=$$

$$=4_{}8_{}Cor(cycl(3)Cor(cycl(1)(h),g),f)=$$

$$=4_{}8_{}Cor(Cor(cycl(19)(h),cycl(3)(g)),f)$$

where the first equality holds by \[3, Prop. 3.6.2\], the second by Lemma 2.1 and the third by \[3, Th. 3.7.3\]. We also have:

$$7_{}Cor(cycl(6)(h),5_{}Cor(cycl(3)(g),f))=$$

$$=7_{}9_{}Cor(cycl(65)(h),Cor(cycl(3)(g),f))$$

by \[3, Lemma 3.7.1\]. We conclude that $`(hg)f=h(gf)`$ by \[3, Prop. 3.7.7\].

We denote by $`Cor(S)`$ the category of finite correspondences whose objects are schemes of finite type over $`S`$, morphisms are finite correspondences and the composition of morphisms is defined by (2.1).

For a morphism of schemes $`f:XY`$ let $`\mathrm{\Gamma }_f`$ be its graph considered as an element of $`c(XY/X)`$. One verifies easily that $`\mathrm{\Gamma }_{gf}=\mathrm{\Gamma }_g\mathrm{\Gamma }_f`$ and we get a functor $`Sch/SCor(S)`$. Below we use the same symbol for a morphism of schemes and its graph considered as a finite correspondence.

The external product of cycles defines pairings

$$c(X,Y)c(X^{},Y^{})c(XX^{},YY^{})$$

and one verifies easily using the results of  that this pairing extends to a tensor structure on $`Cor(S)`$ with $`XY:=XY`$.

## 3 Intersecting relative cycles with divisors

Let $`X`$ be a noetherian scheme and $`D`$ a Cartier divisor on $`X`$ i.e. a global section of the sheaf $`^{}/𝒪^{}`$. One defines the cycle $`cycl(D)`$ associated with $`D`$ as follows. Let $`U_i`$ be an open covering of $`X`$ such that $`D_{U_i}`$ is of the form $`f_{i,+}/f_{i,}^{}(U_i)`$. Then $`cycl(D)`$ is determined by the property that

$$cycl(D)_{|U_i}=cycl(f_{i,+}^1(0))cycl(f_{i,}^1(0))$$

where on the right hand side one considers the cycles associated with closed subschemes (). One defines the support of $`D`$ as the closed subset $`supp(D):=supp(cycl(D))`$.

We say that a cycle $`𝒵=n_iz_i`$ on $`X`$ intersects $`D`$ properly if the points $`z_i`$ do not belong to $`supp(D)`$. Let $`Z_i`$ be the closure of $`z_i`$ considered as a reduced closed subscheme and $`e_i:Z_iX`$ the closed embedding. If $`𝒵`$ and $`D`$ intersect properly we define their intersection $`(𝒵,D)`$ as the cycle

$$(𝒵,D):=n_i(e_i)_{}(cycl(e_i^{}(D)))$$

If $`p:XS`$ is a morphism of finite type and $`𝒵`$ is a relative cycle of relative dimension $`d`$ over $`S`$, we say that $`D`$ intersects $`𝒵`$ properly relative to $`p`$ (or properly over $`S`$) if the dimension of fibers of $`supp(D)supp(𝒵)`$ over $`S`$ is $`d1`$. This clearly implies that $`𝒵`$ intersects $`D`$ properly and $`(𝒵,D)`$ is defined.

###### Proposition 3.1

Assume that $`S`$ is reduced and $`D`$ and $`𝒵`$ intersect properly over $`S`$. Then:

1. $`(𝒵,D)`$ is a relative cycle of relative dimension $`d1`$ over $`S`$
2. let $`p:S^{}S`$ be a morphism and $`p^{}:XS^{}X`$ the projection, assume that $`(p^{})^{}(D)`$ is defined, then one has

$$p^{}(cycl(Z),D)=(p^{}(cycl(Z)),(p^{})^{}(D)).$$
(3.1)

Proof: One can easily see that $`D`$ intersects $`𝒵`$ properly relative to $`p`$ if and only if for any $`i`$ and any point $`x`$ of $`X`$ there exists a neighborhood $`U`$ of $`x`$ such that $`D_{|U}=f_+/f_{}`$ where $`f_+`$ and $`f_{}`$ are not zero divisors on the fibers of the maps $`Z_iS`$. Since the problem is local in $`X`$ we may assume that $`D=D(f)`$ where $`f`$ is a regular function on $`X`$ which is not a zero divisor on fibers of the maps $`Z_iS`$. We write $`(𝒵,f)`$ instead of $`(𝒵,D(f))`$.

To prove both statements of the proposition it is clearly sufficient to show that for any fat point $`Spec(k)\stackrel{x_0}{}Spec(R)\stackrel{x_1}{}S`$ one has

$$(x_0,x_1)^{}((𝒵,f))=((x_0,x_1)^{}(𝒵),fx_1^{}x_0^{})$$

where $`x_0^{},x_1^{}`$ are the projections

$$XSpec(k)\stackrel{x_0^{}}{}XSpec(R)\stackrel{x_1^{}}{}X$$

Let $`j:Spec(K(R))Spec(R)`$ be the generic point of $`R`$ and

$$pr:Spec(K(R))XX$$

the projection. Since $`S`$ is reduced, $`Z_i`$ are flat over a dense open subset of $`S`$ and $`(x_1j)^{}((𝒵,f))=m_jw_j`$ is defined and by Lemma 3.3 we have

$$(x_1j)^{}((𝒵,f))=((x_1j)^{}(𝒵),fpr)$$

For a cycle $`𝒲=m_jw_j`$ over the generic point of $`Spec(R)`$ denote by $`cl𝒲`$ the same cycle considered over $`Spec(R)`$. Since $`cl(x_1j)^{}(𝒵)`$ is a formal linear combination of cycles of flat subschemes, Lemma 3.3 applies and we conclude that:

$$(x_0,x_1)^{}((𝒵,f))=x_0^{}(cl(x_1j)^{}((𝒵,f)))=x_0^{}(cl(x_1j)^{}(𝒵),fx_1^{})=$$

$$=(x_0^{}cl(x_1j)^{}(𝒵),fx_1^{}x_0^{})=((x_0,x_1)^{}(𝒵),fx_1^{}x_0^{})$$

###### Lemma 3.2

Let $`Z`$ be a noetherian scheme and $`f`$ a regular function on $`Z`$ which is not a zero divisor. Let further $`e_i:Z_iZ`$ be the connected components of $`Z`$ and $`n_i`$ their multiplicities. Then one has:

$$cycl(f^1(0))=n_i(e_i)_{}(cycl(f_{|Z_i}^1(0)))$$
(3.2)
Proof: (P.Deligne) Replacing $`Z`$ by the local scheme of a generic point of $`f^1(0)`$ we may assume that $`Z=Spec(A)`$ is local of dimension $`1`$. By definition of the cycle associated to a closed subscheme (3.2) is equivalent to

$$l(A/(f))=l(A/p_i)l(A/(p_i+(f)))$$

where $`p_i`$ are the minimal ideals of $`A`$ and $`l(M)`$ is the length of an $`A`$-module. The function $`Ml(M)`$ extends to an additive function on the $`K_0`$ of the abelain category of $`A`$-modules of finite length. Consider the function $`l_f:Ml(cone(M\stackrel{f}{}M))`$. Equivalently we have $`l_f(M)=l(M^LA/f)`$ which shows that it is an additive function on $`K_0(Amod)`$. In $`K_0(Amod)`$ one has

$$A=(l(A/p_i)A/p_i)+M$$

where $`M`$ is a module of finite length. This implies:

$$l(A/f)=l_f(A)=l(A/p_i)l_f(A/p_i)=l(A/p_i)l(A/(p_i+(f))).$$

###### Lemma 3.3

Let $`Z`$ be a closed subscheme of $`X`$ which is flat and equidimensional over $`S`$ and $`f`$ be a regular function on $`Z`$ such that $`f^1(0)Z`$ is equidimensional over $`S`$. Then $`(cycl(Z),f)`$ is a relative cycle and for any morphism $`p:S^{}S`$ one has:

$$p^{}(cycl(Z),f)=(p^{}(cycl(Z)),fp^{})$$

where $`p^{}:XS^{}X`$.

Proof: Lemma 3.2 implies that

$$(cycl(Z),f)=cycl(f_{|Z}^1(0)).$$

Our condition on $`f`$ implies that, for any $`sS`$, $`f`$ restricted to the fiber $`Z_s`$ is not a zero divisor. Since $`Z`$ is flat over $`S`$ this implies that $`f_{|Z}^1(0)`$ is flat over $`S`$ (see e.g. ). Since $`Z`$ is equidimensional of relative dimension $`d`$, $`f_{|Z}^1(0)`$ is equidimensional of relative dimension $`d1`$. We conclude by  that $`cycl(f_{|Z}^1(0))`$ is a relative cycle.

For $`p;S^{}S`$ we have:

$$p^{}((cycl(Z),f))=p^{}(cycl(f_{|Z}^1(0)))=cycl((fp^{})_{|ZS^{}}^1(0))=$$

$$=(cycl(ZS^{}),fp^{})=(p^{}(cycl(Z)),fp^{}).$$

###### Corollary 3.4

Let $`X^{}\stackrel{f}{}XS`$ be morphisms of finite type, $`𝒵`$ a relative cycle on $`X`$ over $`S`$ and $`𝒲`$ a relative cycle on $`X^{}`$ over $`X`$ of dimension $`0`$. Let further $`D`$ be a Cartier divisor on $`X^{}`$ which intersects $`𝒲`$ properly over $`X`$. Then $`D`$ intersects $`Cor(𝒲,𝒵)`$ properly over $`S`$ and one has:

$$(Cor(𝒲,𝒵),D)=Cor((𝒲,D),𝒵)$$
(3.3)
Proof: It is a straightforward corollary of the definition of $`Cor(,)`$ and (3.1).

###### Lemma 3.5

Let $`f:X^{}X`$ be a morphism of schemes of finite type over $`S`$, $`𝒵`$ a relative cycle on $`X^{}`$ such that $`f`$ is proper on $`supp(𝒵)`$ and $`D`$ a Cartier divisor on $`X`$. Assume that $`f^{}(D)`$ is defined and $`𝒵`$ intersects $`f^{}(D)`$ properly over $`S`$. Then $`f_{}(𝒵)`$ intersects $`D`$ properly over $`S`$ and one has:

$$f_{}(𝒵,f^{}(D))=(f_{}(𝒵),D)$$
(3.4)
Proof: Let $`d`$ be the relative dimension of $`𝒵`$ over $`S`$. To see that $`f_{}(𝒵)`$ intersects $`D`$ properly over $`S`$ we need to check that the dimension of the fibers of $`supp(D)supp(f_{}(𝒵))`$ over $`S`$ is $`d1`$. This follows from our assumption and the inclusion

$$supp(D)supp(f_{}(𝒵))supp(D)f(supp(𝒵))=$$

$$=f(f^1(supp(D))supp(𝒵))=f(supp(f^{}(D))supp(𝒵))$$

To verify (3.4) it is sufficient to consider the situation locally around the generic points of $`f(supp(f^{}(D))supp(𝒵))`$. Therefore we may assume that $`D=D(g)`$ is the divisor of a regular function $`g`$ and $`𝒵=z`$ is just one point with the closure $`Z`$. Replacing $`X^{}`$ by $`Z`$ and $`X`$ by $`f(Z)`$ we may assume that $`X`$, $`X^{}`$ are integral, $`f`$ is surjective and $`X`$ is local of dimension $`1`$. Let $`A=𝒪(X)`$, $`B=𝒪(X^{})`$. As in the proof of 3.2, consider the function $`l_g:Ml_A(M^LA/g)`$ on $`K_0(Amod)`$. This function vanishes on modules with the support in the closed point which implies that

$$l_g(B)=deg(f)l_g(A)=deg(f)l_A(A/g)$$

On the other hand $`l_g(A)=l_A(B/(f^{}(g)))`$. Let $`x_i^{}`$ be the closed points of $`X^{}`$, $`k_i^{}`$ their residue fields and $`k`$ the residue field of the closed point of $`X`$. Let further $`M_i`$ be the part of $`B/(f^{}(g))`$ supported in $`x_i^{}`$. One can easily see that $`l_A(B/(f^{}(g)))=_i[k_i^{}:k]l_B(M_i)`$. Combining our equalities we get:

$$deg(f)l_A(A/g)=\underset{i}{}[k_i^{}:k]l_B(M_i)$$
(3.5)
which is equivalent to (3.4).

## 4 Cancellation theorem

Consider a finite correspondence

$$𝒵c(𝐆_mX,𝐆_mY)=c(𝐆_mX𝐆_mY/𝐆_mX).$$

Let $`f_1,f_2`$ be the projections to the first and the second copy of $`𝐆_m`$ respectively and let $`g_n`$ denote the rational function $`(f_1^{n+1}1)/(f_1^{n+1}f_2)`$ on $`𝐆_mX𝐆_mY`$.

###### Lemma 4.1

For any $`𝒵`$ there exists $`N`$ such that for all $`nN`$ the divisor of $`g_n`$ intersects $`𝒵`$ properly over $`X`$ and the cycle $`(𝒵,D(g_n))`$ is finite over $`X`$.

Proof: Let $`\overline{f}_1\times \overline{q}:\overline{C}𝐏^1X`$ be a finite morphism which extends the projection $`supp(𝒵)𝐆_mX`$. Let $`N`$ be an integer such that the rational function $`\overline{f}_1^N/f_2`$ is regular in a neighborhood of $`\overline{f}_1^1(0)`$ and the rational function $`f_2/\overline{f}_1^N`$ is regular in a neighborhood of $`\overline{f}_1^1(\mathrm{})`$. Then for any $`nN`$ one has:

1. the restriction of $`g_nf_2`$ to $`supp(𝒵)`$ is regular on a neighborhood of $`\overline{f}_1^1(0)`$ and equals $`1`$ on $`\overline{f}_1^1(0)`$
2. the restriction of $`g_n`$ to $`supp(𝒵)`$ is regular a neighborhood of $`\overline{f}_1^1(\mathrm{})`$ and equals $`1`$ on $`\overline{f}_1^1(\mathrm{})`$

Conditions (1),(2) imply that the divisor of $`g_n`$ intersects $`𝒵`$ properly over $`X`$ and that the relative cycle $`(𝒵,D(g_n))`$ is finite over $`X`$.

If $`(𝒵,D(g_n))`$ is defined as a finite relative cycle we let $`\rho _n(𝒵)c(X,Y)`$ denote the projection of $`(𝒵,D(g_n))`$ to $`XY`$.

###### Remark 4.2

Note that we can define a finite correspondence $`\rho _g(𝒵):XY`$ for any function $`g`$ satisfying the conditions (1),(2) in the same way as we defined $`\rho _n=\rho _{g_n}`$. In particular, if $`n`$ and $`m`$ are large enough then the function $`tg_n+(1t)g_m`$ defines a finite correspondence $`h=h_{n,m}:X𝐀^1Y`$ such that $`h_{|X\times \{0\}}=\rho _m(𝒵)`$ and $`h_{|X\times \{1\}}=\rho _n(𝒵)`$, i.e. we get a canonical $`𝐀^1`$-homotopy from $`\rho _m(𝒵)`$ to $`\rho _n(𝒵)`$.

###### Lemma 4.3

1. \[(i)\]
2. For a finite correspondence $`𝒲:XY`$ and any $`n1`$ one has $`\rho _n(Id_{𝐆_m}𝒲)=𝒲`$
3. Let $`e_X`$ be the composition $`𝐆_mX\stackrel{pr}{}X\stackrel{\{1\}\times Id}{}𝐆_mX`$. Then $`\rho _n(e_X)=0`$ for any $`n0`$.

Proof: The cycle on $`𝐆_mX𝐆_mY`$ over $`𝐆_mX`$ which represents $`Id_{𝐆_m}𝒲`$ is $`\mathrm{\Delta }_{}(𝐆_m\times 𝒲)`$ where $`\mathrm{\Delta }`$ is the diagonal embedding $`𝐆_mXY𝐆_mX𝐆_mY`$. The cycle $`(\mathrm{\Delta }_{}(𝐆_m\times 𝒲),g_n)`$ is $`\mathrm{\Delta }_{}(D𝒲)`$ where $`D`$ is the divisor of the function $`(t^{n+1}1)/(t^{n+1}t)`$ on $`𝐆_m`$. The push-forward of $`\mathrm{\Delta }_{}(D𝒲)`$ to $`XY`$ is the cycle $`deg(D)𝒲`$. Since $`deg(D)=1`$ we get the first statement of the lemma.

The cycle $`𝒵`$ on $`𝐆_mX𝐆_mX`$ representing $`e_X`$ is the image of the embedding $`𝐆_mX𝐆_mX𝐆_mX`$ which is diagonal on $`X`$ and of the form $`t(t,1)`$ on $`𝐆_m`$. This shows that the restriction of $`g_n`$ to $`supp(𝒵)`$ equals $`1`$ and $`(𝒵,D(g_n))=0`$.

###### Lemma 4.4

Let $`𝒵:𝐆_mX𝐆_mY`$ be a finite correspondence such that $`\rho _n(𝒵)`$ is defined. Then for any finite correspondence $`𝒲:X^{}X`$, $`\rho _n(𝒵(Id_{𝐆_m}𝒲))`$ is defined and one has

$$\rho _n(𝒵(Id_{𝐆_m}𝒲))=\rho _n(𝒵)𝒲$$
(4.1)
Proof: Let us show that (4.1) holds. In the process it will become clear that the left hand side is defined. We can write $`\rho _n(𝒵)𝒲`$ as the composition

$$X^{}\stackrel{𝒲}{}𝒳\stackrel{(𝒵,𝒟(_𝓃))}{}𝐆_𝓂𝐆_𝓂𝒴\stackrel{𝓅𝓇}{}𝒴$$

and $`\rho _n(𝒵(Id_{𝐆_m}𝒲))`$ as the composition

$$X^{}\stackrel{𝒴}{}𝐆_𝓂𝐆_𝓂𝒴\stackrel{𝓅𝓇}{}𝒴$$

where $`𝒴=(𝒵(Id_{𝐆_m}𝒲),D(g_n))`$. Consider the diagram

$$\begin{array}{ccccc}𝐆_mX^{}𝐆_mY& \stackrel{p_1}{}& 𝐆_mX^{}X𝐆_mY& & 𝐆_mX𝐆_mY\\ & & & & & & \\ & & X^{}X& \stackrel{p_2}{}& X\\ & & & & & & \\ & & X^{}\end{array}$$

where the arrows are the obvious projections. If we consider $`𝒵`$ as a cycle of dimension $`1`$ over $`X`$ then the cycle $`𝒵(Id_{𝐆_m}𝒲)`$, considered as a cycle over $`X^{}`$, is $`(p_1)_{}Cor(cycl(p_2)(𝒵),𝒲)`$ and we have

$$((p_1)_{}Cor(cycl(p_2)(𝒵),𝒲),D(g_n))=$$

$$=(p_1)_{}(Cor(cycl(p_2)(𝒵),𝒲),D(g_n))=(p_1)_{}Cor((cycl(p_2)(𝒵),D(g_n)),𝒲)=$$

$$=(p_1)_{}Cor(cycl(p_2)(𝒵,D(g_n)),𝒲)$$

where the first equality holds by (3.4), the second by (3.3) and the third by (3.1).

The last expression represents the composition $`𝒲(𝒵,D(g_n))`$ and we conclude that

$$\rho _n(𝒵)𝒲=\rho _n(𝒵(Id_{𝐆_m}𝒲))$$

###### Lemma 4.5

Let $`𝒵:𝐆_mX𝐆_mY`$ be a finite correspondence such that $`\rho _n(𝒵)`$ is defined. Then for any morphism of schemes $`f:X^{}Y^{}`$, $`\rho _n(𝒵f)`$ is defined and one has

$$\rho _n(𝒵f)=\rho _n(𝒵)f$$
(4.2)
Proof: Consider the diagram

$$\begin{array}{ccccc}𝐆_mXX^{}𝐆_mYY^{}& \stackrel{p_1}{}& 𝐆_mXX^{}𝐆_mY& & 𝐆_mX𝐆_mY\\ & & & & & & \\ & & XX^{}& \stackrel{p_2}{}& X\end{array}$$

where $`p_1`$ is defined by the embedding $`X^{}\stackrel{f\times Id}{}X^{}Y^{}`$ and the rest of the morphisms are the obvious projections. Consider $`𝒵`$ as a cycle over $`X`$. Then $`\rho _n(𝒵f)`$ is given by the composition

$$𝐆_mXX^{}\stackrel{𝒴_1}{}𝐆_m𝐆_mY\stackrel{pr}{}YY^{}$$

where $`𝒴_1=((p_1)_{}cycl(p_2)(𝒵),g_n)`$ and $`\rho _n(𝒵)f`$ by the composition

$$𝐆_mXX^{}\stackrel{𝒴_2}{}𝐆_m𝐆_mY\stackrel{pr}{}YY^{}$$

where $`𝒴_2=(p_1)_{}(cycl(p_2)((𝒵,g_n)))`$. The equality $`𝒴_1=𝒴_2`$ follows from (3.4) and (3.1).

For our next result we need to use presheaves with transfers. A presheaf with transfers on $`Sch/S`$ is an additive contravariant functor from $`Cor(S)`$ to the category of abelian groups. For $`X`$ in $`Sch/S`$ we let $`𝐙_{tr}(X)`$ denote the functor represented by $`X`$ on $`Cor(S)`$. One defines tensor product of presheaves with transfers in the usual way such that $`𝐙_{tr}(X)𝐙_{tr}(Y)=𝐙_{tr}(X\times Y)`$. To simplify notations we will write $`X`$ instead of $`𝐙_{tr}(X)`$ and identify morphisms $`𝐙_{tr}(X)𝐙_{tr}(Y)`$ with finite correspondences $`XY`$. Note in particular that $`𝐆_m`$ denotes the presheaf with transfers $`𝐙_{tr}(𝐆_m)`$ not the presheaf with transfers represented by $`𝐆_m`$ as a scheme. To preserve compatibility with the notation $`XY`$ for the product of $`X`$ and $`Y`$ we write $`FG`$ for the tensor product of presheaves with transfers $`F`$ and $`G`$.

Let $`S_t^1`$ denote the presheaf with transfers $`ker(𝐆_mS)`$. We consider it as a direct summand of $`𝐆_m`$ with respect to the projection $`Ide`$ where $`e`$ is defined by the composition $`𝐆_mS\stackrel{1}{}𝐆_m`$. In the following theorem we let $`fg`$ denote that the morphisms $`f`$ and $`g`$ are $`𝐀^1`$-homotopic.

###### Theorem 4.6

Let $`F`$ be a presheaf with transfers such that there is an epimorphism $`XF`$ for a scheme $`X`$. Let $`\varphi :S_t^1FS_t^1Y`$ be a morphism. Then there exists a unique up to an $`𝐀^1`$-homotopy morphism $`\rho (\varphi ):FY`$ such that $`Id_{S_t^1}\rho (\varphi )\varphi `$.

Proof: Let us fix an epimorphism $`p:XF`$. Then the morphism $`\varphi `$ defines a finite correspondence $`𝒵:𝐆_mX𝐆_mY`$ and for $`n`$ sufficiently large we may consider $`\rho _n(𝒵):XY`$. Lemma 4.4 implies immediately that $`\rho _n(𝒵)`$ vanishes on $`ker(p)`$ and therefore it defines a morphism $`\rho _n(\varphi ):FX`$.

Consider a morphism $`\varphi `$ of the form $`Id_{S_t^1}\psi `$. Then $`𝒵`$ is of the form $`(Id_{𝐆_m}e)𝒲`$ where $`𝒲:XY`$ corresponds to $`\psi `$. By Lemma 4.3 we have $`\rho _n(𝒵)=𝒲`$ and therefore $`\rho _n(Id_{S_t^1}\psi )=\psi `$ for any $`n1`$. If $`\rho ,\rho ^{}`$ are two morphims such that $`Id_{S_t^1}\rho \varphi `$ and $`Id_{S_t^1}\rho ^{}\varphi `$ then for a sufficiently large $`n`$ we have

$$\rho =\rho _n(Id_{S_t^1}\rho )\rho _n(Id_{S_t^1}\rho ^{})=\rho ^{}$$

This implies the uniqueness part of the theorem.

To prove the existence let us show that for a sufficiently large $`n`$ one has $`Id_{S_t^1}\rho _n(\varphi )\varphi `$. Let $`\stackrel{~}{\varphi }`$ be the morphism $`𝐆_mF𝐆_mY`$ defined by $`\varphi `$ and let

$$\stackrel{~}{\varphi }^{}:F𝐆_mY𝐆_m$$

be the morphism obtained from $`\stackrel{~}{\varphi }`$ by the obvious permutation.

###### Lemma 4.7

The morphisms $`\stackrel{~}{\varphi }(Id_{𝐆_m}e)`$ and $`(Id_{𝐆_m}e)\stackrel{~}{\varphi ^{}}`$ are $`𝐀^1`$-homotopic.

Proof: One can easily see that these two morphisms are obtained from the morphisms

$$\varphi Id_{S_t^1},Id_{S_t^1}\varphi ^{}:S_t^1FS_t^1S_t^1YS_t^1$$

by using the standard direct sum decomposition. One can see further that $`\varphi Id_{S_t^1}=\sigma _Y(Id_{S_t^1}\varphi ^{})\sigma _F`$ where $`\sigma _F`$ and $`\sigma _Y`$ are the permutations of the two copies of $`S_t^1`$ in $`S_t^1FS_t^1`$ and $`S_t^1YS_t^1`$ respectively. Lemma 4.8 below implies now that $`\varphi Id_{S_t^1}Id_{S_t^1}\varphi ^{}`$.

###### Lemma 4.8

The permutation on $`S_t^1S_t^1`$ is $`𝐀^1`$-homotopic to $`\{1\}IdId`$ where $`\{1\}:S_t^1S_t^1`$ is defined by the morphism $`𝐆_m\stackrel{xx^1}{}𝐆_m`$.

Proof: The same arguments as the ones used in \[2, p.142\] show that for any scheme $`X`$ and any pair of invertible functions $`f,g`$ on $`X`$ the morphism $`X\stackrel{fg}{}S_t^1S_t^1`$ is $`𝐀^1`$-homotopic to the morphism $`gf^1`$. This implies immediately that the permutation on $`S_t^1S_t^1`$ is $`𝐀^1`$-homotopic to the morphism $`Id(\{1\}Id)`$ where $`\{1\}Id:S_t^1S_t^1`$ is the morphism defined by the map $`𝐆_m\stackrel{xx^1}{}𝐆_m`$.

For a sufficiently large $`n`$ we have

$$\rho _n(\varphi (Id_{𝐆_m}e))=\rho _n(\varphi )(Id_{𝐆_m}e)$$

by Lemma 4.5. On the other hand

$$\rho _n((Id_{𝐆_m}e)\varphi ^{})=\varphi ^{}$$

by Lemma 4.3. By Lemma 4.7 we conclude that

$$\varphi ^{}\rho _n(\varphi )(Id_{𝐆_m}e)$$

which is equivalent to $`Id_{S_t^1}\rho _n(\varphi )\varphi `$. Theorem 4.6 is proved.

###### Corollary 4.9

Denote by $`F_Y`$ the presheaf

$$XHom(S_t^1X,S_t^1Y)$$

and consider the obvious map $`YF_Y`$. Then for any $`X`$ the corresponding map of complexes of abelian groups

$$C_{}(Y)(X)C_{}(F_Y)(X)$$

is a quasi-isomorphism

Proof: Let $`\mathrm{\Delta }^n𝐀^n`$ be the standard algebraic simplex and $`\mathrm{\Delta }^n`$ the subpresheaf in $`\mathrm{\Delta }^n`$ which is the union of the images of the face maps $`\mathrm{\Delta }^{n1}\mathrm{\Delta }^n`$. Then the n-th homology group of the complex $`C_{}(F)(X)`$ for any $`F`$ is the group of homotopy classes of maps from $`X(\mathrm{\Delta }^n/\mathrm{\Delta }^n)`$ to $`F`$. Our result now follows directly from 4.6.

###### Corollary 4.10

Let $`k`$ be a perfect field. Then for any $`K,L`$ in $`DM_{}^{eff}(k)`$ the map $`Hom(K,L)Hom(K(1),L(1))`$ is a bijection.

Proof: Since $`DM_{}^{eff}`$ is generated by objects of the form $`X`$ it is enough to check that for smooth schemes $`X,Y`$ over $`k`$ and $`n𝐙`$ one has

$$Hom(S_t^1X,S_t^1Y[n])=Hom(X,Y[n])$$

By Corollary 4.9 we know that the map

$$YF_Y=\underset{¯}{Hom}(S_t^1,S_t^1Y)$$

is an isomorphism in $`DM`$. Let us show now that for any sheaf with transfers $`F`$ and any $`X`$ one has

$$Hom_{DM}(S_t^1X,F[n])=Hom_{DM}(X,\underset{¯}{Hom}(S_t^1,F)[n])$$
(4.3)
The left hand side of (4.3) is the hypercohomology group $`𝐇^n(𝐆_mX,C_{}(F))`$ modulo the subgroup $`𝐇^n(X,C_{}(F))`$. The right hand side is the hypercohomology group $`𝐇^n(X,C_{}\underset{¯}{Hom}(𝐆_m,F))`$ modulo similar subgroup. Let $`p:𝐆_mXX`$ be the projection. It is easy to see that (4.3) asserts that $`𝐑p_{}(C_{}(F))C_{}(p_{}(F))`$. There is a spectral sequence which converges to the cohomology sheaves of $`𝐑p_{}(C_{}(F))`$ and starts with the higher direct images $`R^ip_{}(\underset{¯}{H}^j(C_{}(F)))`$. We need to verify that $`R^ip_{}(\underset{¯}{H}^j(C_{}(F)))=0`$ for $`i>0`$ and that $`p_{}(\underset{¯}{H}^j(C_{}(F)))=\underset{¯}{H}^j(C_{}(p_{}(F)))`$. Both statements follow from \[5, Prop. 4.34, p.124\] and the comparison of Zariski and Nisnevich cohomology for homotopy invariant presheaves with transfers.


text:
# Temporal and Spectral Properties of Gamma-Ray Flashes

## 1 Introduction

Intense $`\gamma `$-ray bursts of atmospheric origin were detected by the Burst and Transient Source Experiment (BATSE) detectors, located on the Compton Gamma Ray Observatory (CGRO) (Fishman et al., (1994)). All the observed TGFs were of short duration (a few milliseconds) and had extremely hard energy spectra consistent with bremsstrahlum radiation from energetic (MeV) electrons. Since they were spatially correlated with regions of high thunderstorm activity and in two cases have been correlated with individual lightning flashes (Inan et al., (1996)), they are thought to be caused by high-altitude discharges produced by runaway air breakdown. Several theoretical calculations have been done to explain the origins of TGFs under the runaway air breakdown mechanism (Chang and Price, (1995); Taranenko and Roussel-Dupre, (1996); Lehtinen et al., (1996); Lehtinen et al., (1997)). The calculated $`\gamma `$-ray fluxes and duration of the bursts are comparable to those measured by the BATSE detector on the CGRO satellite.

As the runaway air breakdown is a fundamental new process in plasma, it is interesting to understanding more the physics of the process through studying TGFs, if they were truly caused by such a mechanism. Besides the total fluxes, durations and time-averaged spectra, the energy dependence of temporal profiles and spectral evolution of TGFs can give more information about their production process. For this purpose we analyze the time-tagged event (TTE) data for TGFs observed by BATSE. For 4 energy channels with boundaries 25-55 keV, 55-110 keV, 110-320 keV, and $`>320`$ keV, the TTE data contains the arrival time ($`2\mu s`$ resolution) of each photon from a triggered event up to $`3.3\times 10^4`$ photons. Of 47 TGFs observed on CGRO in $`4`$ years and published by NASA in their details, 15 bursts with high signal to noise ratio are used in our analysis, which are selected by the criterion of $`F_m/T_{90}>4`$ ph/cm-2/0.1ms/ms, where $`F_m`$ is the peak rates of the counting series with time step 0.1 ms, $`T_{90}`$ (ms) the burst duration which contains $`\%90`$ burst photons.

## 2 Energy Dependence of Temporal Profiles

To study the energy dependence of temporal profiles, which is important to diagnose the emission mechanism, we construct two counting series $`f_1(t)`$ and $`f_2(t)`$ for each burst for the energy band 25-110 keV and $`>110`$ keV, respectively. The average pulse widths in the low and high energy bands and the relative time delays between the two bands can be calculated by a modified correlation analysis technique used in studying X-ray rapid variability of the black hole binary Cyg X-1 (Li et al., (1999); Li, (2001)).

The cross-correlation function of two time series $`f_1`$ and $`f_2`$ at time lag $`\tau `$ is defined as

$$\text{CCF}(\tau )=\underset{i}{}v_1(i\mathrm{\Delta }t+\tau )v_2(i\mathrm{\Delta }t)/\sigma (v_1)\sigma (v_2)$$
(1)
where $`v(t)=f(t)\overline{f}`$, $`f(t)`$ is the number of photons in the time interval $`(t,t+\mathrm{\Delta }t)`$, $`\mathrm{\Delta }t`$ is the time step. If the function CCF($`\tau `$)/CCF($`0`$) has maximum at $`\tau =\mathrm{\Lambda }`$, the time lag of the energy band 1 relative to the band 2 at the time scale $`Deltat`$ is then defined as $`\mathrm{\Lambda }`$. Monte Carlo simulations have been done and the results show that with this technique we can measure the relative time delay between two bands over a wide range of time scale $`\mathrm{\Delta }t`$ with high time resolution. At large scales one usually can get enough signal photons in a time bin and desirable correlation values from finite time bins. And at small scales the effect of serious Poisson fluctuation of signal counts in a time bin can be compensated by the large amounts of time bin and accurate correlation values can also be derived with Eq. (1). A distribution of time lag vs. time scale can reflect the character of the physical process to produce the delay better than a single value of lag at only one time scale. A physical process usually occurs in a range of time scale, the spectral delay caused by the process should appear at different time scales, smoothly distributed in the range. On the other hand apparent delays from statistical fluctuation will fluctuate between positive and negative values.

For each studied burst and $`m=25`$ different values of time step $`\mathrm{\Delta }t`$ which are logarithmically uniformly placed in the region of $`10^510^3`$ s, we calculate the time lags $`\mathrm{\Lambda }`$ of $`f_1`$ relative to $`f_2`$. All obtained time lags $`\mathrm{\Lambda }_i(i=1,\mathrm{},m)`$ of each burst with high signal to noise ratio are always positive. We average each 5 successive $`\mathrm{\Lambda }_i`$ and show the distribution of average time lag vs. time scale in Fig. 1. The global average $`\overline{\mathrm{\Lambda }}=_{i=1}^m\mathrm{\Lambda }_i/m`$ and the standard deviation $`\sigma (\mathrm{\Lambda })=\sqrt{(\mathrm{\Lambda }_i\overline{\mathrm{\Lambda }})^2/(m1)}`$ for each selected TGF is listed in Table 1. The total counting profile and profiles in 4 energy bands of a TGF with BATSE trigger number 2955 are plotted in Figure 2, where the delay of lower energy photons relative to higher energy ones is apparent.

The width $`W_l`$ of a temporal profile in a band $`l`$ can be defined as the FWHM of the autocorrelation function

$$\text{ACF}(\tau )=\underset{i}{}v_l(i\mathrm{\Delta }t+\tau )v_l(i\mathrm{\Delta }t)/\sigma ^2(v_1)$$
(2)
The widths $`W_1`$ and $`W_2`$ of studied TGFs in the low and high energy bands are calculated and their ratios $`W_1/W_2`$ are presented in Table 1, from which we can see that the lower energy pulses are wider than higher energy ones for most studied bursts.

## 3 Spectral Evolution

For two counts $`c_1`$ in 25-110 keV band and $`c_2`$ in $`>110`$ keV band recorded in the same time segment, we defined the hardness ratio as

$$h=\frac{c_2c_1}{c_2+c_1}$$
(3)
To show the spectral evolution, a TGF’s pulse is divided into 5 time segments, each segment contains approximately the same number of photons and the hardness ratio is calculated by Eq. (3). Figure 3 shows the spectral hardness variation vs. time (indicating by the segment number) with four panels grouped by the shape of temporal evolution of hardness. Although the shapes are various, a general trend of hardness that decreases with time appears in Fig. 3, which confirms the claim by Nemiroff et al.  with earlier TGF data.

## 4 Discussion

For all the bursts with high signal to noise ratio we find that in comparison with high energy band of $`>110`$ keV, $`\gamma `$-ray variations in the low energy band of 25 - 110 keV are always late in the order of $`100`$ $`\mu `$s, pulses are usually wide, and the energy spectra have a general trend to softening with time. The above features of energy dependence of time profiles and spectral revolution observed in TGFs support models of runaway breakdown as they are naturally expected for $`\gamma `$-rays produced by explosive discharges in plasmas. Monte Carlo calculations show that large-voltage and high-temperature pinch plasma columns can generate observed $`\gamma `$-ray flashes with energy spectra and spectral evolution characteristics, including the magnitude of soft lags, consistent with those observed in $`\gamma `$-ray bursts (Li and Wu, (1997); Li, (1998)).

Alternative mechanisms have been proposed to explain the origin of TGFs, e.g. Fargion  claimed that TGFs originated from $`10^{15}10^{17}`$ eV neutrinos of astrophysical nature induced air showers and take TGFs as first evidences for discovering ultra high energy (UHE) neutrinos. Our Monte-Carlo simulations show that up-going air showers are hard to produce the observed time lags between hard and soft energy photons in TGFs. In our simulations a geometrical model of the earth, atmosphere and BATSE detector is set. High energy $`\gamma `$-rays initiated by UHE neutrinos are produced from the earth’s surface, following with the up-going air showers. We tracked the secondary photons and electrons and record the arriving time and energy of all $`\gamma `$-rays reaching the detector, with deposition energy in the BATSE’s region. Simulations were made with the Monte-Carlo package GEANT3 from CERN. In more than one thousand simulated bursts no time lag between hard and soft photons larger than 10 $`\mu `$s has been found.

Quantitative comparison between observed features and expectations from models are needed to further confirm the mechanism and to study physics of the production process.

We thank Prof. Y. Muraki and the reviewers for helpful comments and suggestions. This study was supported by the Special Funds for Major State Basic Research Projects and by the National Natural Science Foundation of China and made use of data obtained through HEASARC Online Service, provided by NASA/GSFC.

Table 1 Selected TGFs    Trig No. $`T_{90}`$ (ms) $`F_m(10^3`$ ph/cm2/0.1ms) $`F_m/T_{90}`$ $`\overline{\mathrm{\Lambda }}\pm \sigma (\mathrm{\Lambda })(\mu `$s) $`W_1/W_2`$    106 1.3 6.74 5.19 102 $`\pm `$ 28 1.19  1433 1.5 7.15 4.77 71 $`\pm `$ 31 1.64  2144 0.7 9.62 13.74 115 $`\pm `$ 40 1.03  2348 1.1 7.15 6.50 88 $`\pm `$ 29 1.04  2370 0.7 8.14 11.63 151 $`\pm `$ 29 1.16  2465 1.0 7.89 7.89 157 $`\pm `$ 25 1.38  2754 0.9 7.65 8.50 120 $`\pm `$ 29 2.10  2808 1.0 5.67 5.67 105 $`\pm `$ 45 0.88  2955 0.7 7.89 11.28 125 $`\pm `$ 21 1.00  3377 1.0 10.11 10.11 373 $`\pm `$ 31 1.47  5577 0.6 5.18 8.63 81 $`\pm `$ 33 0.91  5587 1.2 6.41 5.34 163 $`\pm `$ 46 1.16  5598 1.1 6.17 5.61 117 $`\pm `$ 20 0.94  5665 1.4 7.65 5.46 265 $`\pm `$ 43 1.54  6773 0.9 3.82 4.25 278 $`\pm `$ 61 0.74


text:
# On the nature of the spin-singlet ground state in CaCuGe2O6

## Abstract

We investigate by means of ab initio electronic structure analysis and Quantum Monte Carlo calculations the scenario where longer-ranged magnetic interactions dominate over short-ranged interactions in the physical description of compounds. This question is discussed, in particular, for the case of CaCuGe2O6 which shows a spin-singlet behavior induced by third nearest neighbor copper pairs.

PACS numbers: 75.30.Gw, 75.10.Jm, 78.30.-j

There are a few low-dimensional materials which show, contrary to initial intuitive arguments, longer-ranged dominated exchange couplings. Examples include systems like the most discussed 1/5-depleted Heisenberg system CaV4O9 or the alternating chain compound (VO)2P2O7. CaV4O9 which was originally viewed as an array of weakly coupled square plaquettes of V4+ ions, each in a singlet in the ground state, is found to be a system with strongest coupling between next nearest neighbor vanadiums as revealed by a recent electronic structure study. In (VO)2P2O7 the strongest exchange path is found to be that between two V4+ ions through two phosphate groups PO4 and not between nearest neighbor vanadium ions V-O-V as was initially thought. From these examples, we learn that the subtle competition between the various interactions can lead to surprises and a microscopic study is needed. The detailed investigation of these systems often unveils interesting properties. One such a system is CaCuGe2O6, a system related to the spin-Peierls compound CuGeO3.

Susceptibility measurements on CaCuGe2O6 show the existence of a spin-singlet ground state with an energy gap of 6 meV. But, contrary to CuGeO3 where the spin-gap opens at the spin-Peierls phase transition, in CaCuGe2O6 the spin gap is intrinsic and there is no phase transition between 4.2K and 300K. Also, inelastic neutron scattering (INS) measurements were carried out on CaCuGe2O6 powder and the existence of a finite spin-gap was confirmed.

A question which neither INS nor susceptibility measurements could clarify was which Cu-pairs form the singlets in this material. This issue is of great importance since it determines the magnetic properties of the system. The structure of this material shows an obvious zig-zag 1D chain of spin=1/2 Cu2+ ions along the c-axis (see Fig. 1). Nevertheless, the magnetization and susceptibility data of Sasago et al. are in disagreement with a spin=1/2 Heisenberg chain model. These authors proposed that the spin-gap behavior of the system should be due to longer-distance-formed Cu-pairs and considered possible scenarios depending on which Cu-pairs were taken into account. Also the analysis of INS powder data led Zheludev et al. to conclude that this compound should be described as a weakly interacting dimer system in spite of the fact that the material shows a pronounced 1D arrangement of magnetic ions. Which Cu ions form the pairs, however, couldn’t be strictly defined from the analysis of the above experiments.

It is the purpose of this letter to investigate in detail the singlet nature of this system and why it shows such a behavior. In order to do that we have performed (i) ab initio calculations which give us information on the chemical bonding and the electronic structure and (ii) Quantum Monte Carlo computations which are used in order to calculate thermodynamical quantities like the susceptibility and magnetization in this material.

Crystal structure.- CaCuGe2O6 crystallizes in the monoclinic space-group P21/c with lattice parameters $`a`$ = 10.198 $`\AA `$, $`b`$ = 9.209 $`\AA `$, $`c`$= 5.213 $`\AA `$, $`\beta `$ = 105.73o, and it contains four formula units per primitive unit cell. The copper ions are all equivalent and form Jahn-Teller distorted octahedra with the surrounding oxygens and they build zig-zag chains along the c-direction (see Fig. 1(a)) by sharing an edge of the octahedra. Intercalated between these chains are the Ge and Ca ions. The distances between two nearest neighbor (NN) Cu within the same chain is 3.072 $`\AA `$ and the Cu-O-Cu angles in these chains are 92o for the Cu-O1A-Cu angle and 98o for the Cu-O1B-Cu angle (see Fig. 3 and Ref.  for the oxygen notation). The Cu-Cu distance within the 2nd NN pair which are also located in the same zig-zag chain is 5.213 $`\AA `$. The 3rd and 4th NN are formed by Cu atoms belonging to neighboring $`bc`$ planes (see Fig. 1). The distance between two neighboring $`bc`$ planes alternate between $`d=4.462\AA `$ and $`d^{}=5.354\AA `$ giving rise to 3rd NN and 4th NN distances of 5.549 $`\AA `$ and 6.213 $`\AA `$ respectively.

Band-structure.- We have performed an ab initio study based on the density-functional theory (DFT) in the generalized gradient approximation (GGA) in order to derive the electronic properties of CaCuGe2O6. Calculations have been performed within the frame-work of both the full-potential linearized augmented plane wave (LAPW) method based on the WIEN97 code and the linearized muffin tin orbital (LMTO) method based on the Stuttgart TBLMTO-47 code. The results of the band-structure calculations show four narrow bands close to the Fermi level with a bandwidth of $``$ 0.5 eV, having predominant Cu $`d_{x^2y^2}`$ character (in the local frame) admixed with oxygen contributions. These bands are half-filled and strong correlation effects should explain the insulating groundstate in this compound. These bands are separated by an energy gap of about 0.3 eV from the valence-band set and a gap of about 2 eV from the conduction bands (see Fig. 2).

Effective model.- We have performed LMTO-based downfolding and tight-binding analysis to derive the (single-particle) tranfer integrals of an effective model for this system.

In recent years a new form of the LMTO method has been proposed and implemented  which allows to derive few-orbital effective Hamiltonians by keeping only the relevant degrees of freedom and integrating out the irrelevant ones. This procedure amounts to putting the inactive orbitals by downfolding in the tails of the active orbitals kept in the basis. As a result, this takes into account the proper renormalization in the effective interactions between the active orbitals. The effective interactions obtained are therefore unique and given by the intervening interaction paths. Application of the downfolding procedure to CaCuGe2O6 to derive one orbital (namely $`d_{x^2y^2}`$ per Cu atom) effective model leads to the unambiguous result that the singlet pairs are formed by 3NN Cu-pairs. The next important interactions are the 1NN providing a picture of two-dimensional interacting dimers in agreement with susceptibility data and INS. It is to be noted here that a simple-minded tight-binding fitting method with one-band model is unable to distinguish the relative importance between 3NN and 4NN pairs. Either of the choice of dimer pairs would lead to similar band dispersions though not to the same magnetic behavior. This dominant effect of the 3NN Cu-Cu interaction over the 4NN Cu-Cu interaction is originated from the specific orientation of the intervening oxygen atoms between the Cu pairs and their relative hybridization with Cu $`d_{x^2y^2}`$ orbital guided by the magnitude of Cu-O-Cu bond angles and the bond lengths. This is supported by the 3D electron density plot shown in Fig. 3 near the Fermi level in a plane perpendicular to the c-axis. As it can be seen, the exchange paths connecting two 3NN coppers are not equivalent to the exchange paths connecting two 4NN coppers. For the considered 3NN Cu-Cu pair the intervening oxygens (predominantly O2A and O3A) provide a well-defined interaction path while for the 4NN Cu-Cu pair the contribution of the intervening oxygens (predominantly O2B and O3B) is much smaller leading to almost disconnected Cu2+ ions. This fact is also supported by the partial density of states (DOS) analysis at the Fermi level of the oxygens’ contribution where we observe that the contribution coming from O2B and O3B orbitals is almost negligible compared to that of O2A and O3A.

The downfolded-TB bands are represented by a Hamiltonian of the form:

$`H_{TB}={\displaystyle \underset{(i,j)}{}}t_{ij}(c_i^{}c_j+h.c.)`$ (1)
where the $`t_{ij}`$ are hopping matrix elements between Cu neighbors $`i`$ and $`j`$. We have considered hopping matrix elements up to fourth nearest neighbor (see Fig. 1) $`t_1`$, $`t_2`$, $`t_3`$ and $`t_4`$ (the subindex denotes 1NN, 2NN, 3NN and 4NN respectively). The values derived for this effective model were found to be $`t_1`$=0.068eV, $`t_2`$=0.008eV, $`t_3`$=0.088eV and $`t_4`$=0.004eV. In the inset of Fig. (2) we show the comparison of the DFT-bands to the downfolded-TB bands considering $`t_1`$, $`t_2`$, $`t_3`$ and $`t_4`$ hoppings only. The band-splitting along the path $`DZ`$ is reproduced by considering longer-ranged hopping matrix elements.

An estimate of the exchange integral related to the most dominating 3NN interaction parameter $`t_3`$ can be obtained by using the relation $`J_34t_3^2/U`$ where $`U`$ is the effective on-site Coulomb repulsion. A value of $`U`$ $``$ 4.2eV was proposed for CuGeO3 by mapping experimental data onto one-band description. Assuming that this value is similar for CaCuGe2O6, we get a value of $`J_386`$K.

Susceptibility and Magnetization.- The description for CaCuGe2O6 obtained from the previous first principle calculation is that of a system of interacting dimers. In order to check this result we have analyzed both the susceptibility as well as the magnetization behavior of this material by considering the following model:

$$H_{eff}=J_3\underset{}{}S_iS_j+J_1\underset{(i,j)}{}S_iS_j,$$
(2)
where $`J_3`$ and $`J_1`$ are the exchange integrals between 3NN and 1NN as illustrated in Fig. (1). The analysis of the model has been done by Quantum-Monte-Carlo (QMC) simulations (stochastic series expansion ) on $`20\times 40`$ lattices. We found an optimal value for $`J_3=67\mathrm{K}`$, very close to the value $`68\mathrm{K}`$ proposed by Sasago et al. . We find clear evidence for a weak ferromagnetic inter-dimer coupling $`J_1<0`$, as shown in Fig. (4). The optimal value is $`J_1=0.2J_3`$. The $`g`$-factor was determined by fitting the QMC-results for the susceptibility, $`\chi ^{(th)}=\left(S^zS^z\right)^2`$ with the experimental susceptibility $`\chi `$ (in \[emu/mol\]) at high temperatures via  $`\chi 0.375(g^2/J)\chi ^{(th)}`$. The optimal $`g`$-factor was found to be $`g=2.032`$, close to the value $`2.07`$ proposed earlier .

Sasago et al. measured the magnetization curve for CaCuGe2O6 as a function of an applied magnetic field at $`T=4.2\mathrm{K}`$. With the stochastic series expansion QMC-method it is possible to simulate quantum-spin models in an external field , although these simulations become very hard near saturation. We present the results of this simulation in Fig. (5), for the same parameters we used for evaluating the susceptibility, together with the experimental results. It is very reassuring that $`J_1=0.2J_3`$ is again the optimal parameter set.

The phase diagram of model Eq. (2) is very interesting by itself. In the limit $`J_3=0`$ it consists of decoupled $`J_1`$-chains (see Fig. (1(a))) either antiferro- or ferromagnetic for $`J_1>0`$ or $`J_1<0`$ respectively. In both cases the excitation spectrum is gapless, while it shows a gap in the limit $`J_1=0`$ $`J_30`$ (dimer phase). We therefore expect two quantum critical points connecting these two regions. We have investigated the phase-diagram and found the critical coupling strength to be $`J_10.55J_3`$ and $`J_10.9J_3`$ respectively. The parameter range for CaCuGe2O6 is away from these two critical points.

Discussion and Conclusions.- the analysis of the electronic structure of CaCuGe2O6 by first principles calculations as well as the examination of susceptibility and magnetization data by the QMC method leads to a unique description of this material as a system of dimers formed by 3NN magnetic spin=1/2 Cu2+ ions with ferromagnetic (1NN) interdimer couplings. The ferromagnetic nature of the 1NN coupling is more subtle to understand than in other edge-sharing Cu-O systems since due to the strong distorsion of the Cu octahedron, this coupling proceeds through two pathes with angles 92o and 98o. These two pathes can provide in principle competing ferro- and antiferromagnetic couplings respectively. The analysis of the susceptibility and magnetization behavior shows nonetheless a clear effective ferromagnetic coupling. In this system, since the primary role is played by the 3NN Cu-pairs, the role of the possible frustrating 2NN term to the 1NN interaction is secondary, unlike the case of the related spin-Peierls material CuGeO3. The strength of the magnetic exchange integrals has been obtained from the analysis of the susceptibility and the magnetization data with very good agreement between these two measurements. DFT calculations overestimate the value of $`J_1`$, which is not surprising, nonetheless the physical picture of this material is correctly provided by DFT+downfolding-TB analysis.

In conclusion, by analizing the electronic and magnetic properties of CaCuGe2O6 we have been able to provide a physical picture of the system as well as a microscopic description of the singlet nature in this material. The combination of ab initio techniques with many-body methods (QMC) can unambigously determine the microscopic behavior of a system as has been shown for CaCuGe2O6 in particular.

CaCuGe2O6 shows an interesting spin-gap behavior and we believe that experiments under the application of a magnetic field would be desirable to investigate the possible appearance of long-range order in the system. Moreover, the 2D interaction model provided by this system Eq. (2) is interesting per se since it shows two quantum critical points as a function of the strength quocient $`J_1/J_3`$.