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Z. Phys.

B 93, 195 204 (1994)

ZEITSCHRIFT FORPHYSIKB
9 Springer-Verlag 1994

A dynamics-controlled truncation scheme for the hierarchy of density matrices in semiconductor optics
V.M. Axt, A. Stahl Institut ffir Theoretische Physik, RWTH Aachen, D-52056 Aachen, Germany
Received: 14 July 1993

Abstract. We discuss the interaction of coherent electromagnetic fields with the semiconductor band edge in a dynamic density matrix model. Due to the influence of the Coulomb-interaction the n-point density matrices are coupled in an infinite hierarchy of equations of motion. We show how this hierarchy is related to an expansion of the density matrices in terms of powers of the exciting field. We make use of the above results to set up a closed set of equations of motion involving two-, four- and sixpoint correlation functions, from which all third order contributions to the polarization can be calculated exactly. Comparison of our treatment of the hierarchy with the widely used RPA decoupling on the two-point level, gives interesting insight into the validity of the RPA. In particular we find, that a RPA-like factorization for two of the relevant density-matrices yields a solution of their respective equations of motion to lowest order in the electric field.
PACS: 42.65; 71.35; 71.45

1. Introduction
Under the influence of a strong coherent electromagnetic field semiconductor materials can be brought into a state far from equilibrium. The optical response of such systems reflects the many different kinds of correlations generated by the interaction of the field with the many-particle system and the interactions between the particles themselves. We shall present a description of these correlations using a dynamic density matrix theory in realspace representation. The most serious problem in manyparticle systems like the one considered here is that the Coulomb-interaction gives rise to an infinite hierarchy of equations of motion for the n-point density matrices. The lowest level of this hierarchy consists of the two-point density matrices representing transitions between valence and conduction bands and occupation densities of these bands. The two-point density matrices are of special in-

terest, because the relevant electrodynamic observables like the polarization and the charge densities can be expressed directly in terms of these quantities. It was considered therefore as a goal to set up a closed dynamics taking into account only two-point density matrices. In such a treatment higher order correlation functions are either fully neglected or factorized into sums of products of two-point functions according to a random phase approximation (RPA) decoupling scheme [1-7]. Although descriptions fully neglecting higher order contributions in many cases are in surprisingly good agreement with measurements [8-10], there is a growing number of experiments clearly marking the limits of such a treatment. Examples of the latter kind can be found in [11-14], where even to achieve a qualitative understanding of the experimental results it is necessary to include contributions from four-point density matrices at least in a RPA sense. Furthermore it is possible under certain conditions to excite selectively resonances specific to higher order correlation functions, the most prominent of which is the biexciton resonance [15-20]. Obviously there is no way to deal with those situations seriously using any kind of RPA decoupling. Therefore there is a need for a more systematic inclusion of higher order density matrices from both sides, the experimental and the theoretical. The nonlinear optical response of semiconductors can successfully be classified according to an expansion in powers of the applied electric field up 'to rather high intensities. In the present paper we shall demonstrate that such a classification can be used to systematically decouple the hierarchy of equations of motion for n-point density matrices. The paper is organized as follows: in Sect. 2 we describe the multi-band semiconductor model, introduce the density matrix elements on the two-point level and relate them to the relevant observables of the system. In Sect. 3 we set up equations of motion for the two- and four-point density matrices making explicit their coupling. In Sect. 4 we explain how to decouple systematically the hierarchy of equations of motion. Section 5 is devoted to a comparison with the corresponding RPA

196 approach. Furthermore we shall prove that for some of the n-point density matrices a factorization is exact to lowest order in the electric field. These factorization properties finally yield a closed set of equations only coupling two- and four-point density matrices, from which all third order contributions to the polarization can be calculated exactly. In Sect. 6 we summarfze our results and give an outlook on possible applications. In a forthcoming paper [21] we shall demonstrate how most of the equations relevant for the calculation of the third order susceptibility X3 can be solved analytically assuming a coherent system. Furthermore as an illustration of these solutions we shall discuss the case of the resonant excitation of the biexciton in the dynamical Stark effect. Finally H c represents the Coulomb interaction. Here we consider only the monopole-monopole part (cf. [22]):

Oe-~l Z V i j ( n i - h i ) ( n j - h j ); i~j
e2

(7)

V/j -= 4~ebeo Iri - rj [ ' where we have used the abbreviations"

n j - 2 c;*c;; h:-Z d;*a;.


c v

(8)

2. The model

In optical experiments the quantities of main interest are electromagnetic observables as polarization and charge densities. These quantities can be expressed in terms of two-point density matrices, which are defined as expectation values of two Fermion-operators: W - ( I P ~ ) -- (d~ cb) a exciton transition, (9) (10) (1l)

We consider a multi-band model of a semiconductor in real-space representation. Electrons located at lattice site j in conduction-band c will be described by creation and annihilation operators cf*, cf for the corresponding Wannier-states. The analogous operators for holes in valence-band v are denoted by d~*, d~. Further valence bands will be labeled by greek letters afl),fi, while latin letters abed are used for conduction bands. Our model Hamiltonian consists of three terms:

c ~ b - - ( C ~ ) =(c~*c~) ___"electronoccupation, D ~ =-(15~a a) --(d~*d~) -~ hole occupation.


Using these definitions the polarization is given by: P = 2~Re (r=r!--r2 d3r ~'c,M2~* Yl~*) ' and the charge density can be written a s

(12)

H = H o + g e m + H c.

(1)

H o stands for the Bloeh-energies in the various valenceand conduction-bands and describes intraband transport processes. It is given by:

Ho= ,
jl \'~

*'J ~' ~ J - Z
v

~J''

"JJ'

(2)

3. Equations of motion

where the transfer matrices Tl}; v ~ {c, v} are related to the band structure E~ (k) by:

a) The two-point level


The equations of motion for the two-point density matrices have been derived in several places [23-25]. The main steps to be carried out are: 9 setting up the Heisenberg equations of motion for the pair operators; 9 applying anticommutation rules for the Fermion operators c~ ,, el, d~ ~ and d~ to bring all operator products into normal order; 9 going over to expectation values; 9 using an interpolation procedure in order to get a continuum rather than a site formulation. In previous derivations [23-25] however these steps were followed by an application of the RPA decoupling scheme to factorize four-point density matrices. In contrast we shall leave the four-point contributions unfactorized and arrive at the following equation for the excitonic transition density:

TI} - ~

~ eik'(R~--RJ)E~(k).

(3)

Hem accounts for the interaction with the electromagnetic


field realized by interband dipole transitions between the valence- and conduction-bands:

M~l d, c j + h . c . .
jl cv

(4)

Ejl denotes the electric field at some point (usually midpoint) between site j and l and Mfy is the interband dipole matrix element between Wannier-states:

cv - - ~1 ~ e~k'(RJ--R1)M M), ~ ,(k~ ,,


with: M~o (k) - - e (q/~ (k)[r I ~u~( k ) ) ,

(5)

(6)

-- ih Y(2b + bY2 g Y~2 b = M2b~9E21 - E 1. ~, Mc~ (iV1) C(2b-- E2" ~, M b v ( - iVz) D ~


c v

where q/~ (k); v ~ {c, v} are the Bloch functions for the crystal.

197

+~ d3rj ( V i i - V~j)

(~ ~c-~_v o~) , :jj12 z: r+j~2


v

(14) (15)

four-point functions entering as sources in the above equations are:

hg2 y - Eb ( - iV2)-- E= ( i V 1 ) - Vn.

Na~Ya-1234 = (c~t df* dJ ca4) ^ excitonic occupation

(22)

The left hand side of (14) determines the propagation of Y;'2 b in time and configuration space. In particular it is the differential operator h f2r (essentially the Hamiltonian for a hydrogen-like problem) which is responsible for the well known excitonic structure of Y~. On the right hand side three different kinds of source terms can be identified. First there is the linear source, which is the only term independent of other density matrices. On the second line we find the 'blocking terms', which are known to lead to saturation effects. Finally there is the coupling to the four-point level via the Coulomb integral on the third line, where we have used the definitions:
1234 -- \t'l w2 '~3

Kabcd-1234 =

~C1 C2 C3 C4 )

a? bJ c d

A_.c o n d u c t i o n

b a n d densitydensity correlation (23)

L=aya * df df ) = ^ valence band density1234 =/d~* - - N~l ~ ~2 density correlation.

(24)

b) The four-point level


It is straightforward to extend the density matrix theory to the four-point level and to set up equations of motion for the quantities introduced in the previous section. These equations have the general structure:

-ihA +
(16)

hf2 AA
propagation (drift) in configuration space

QA ,
sources

(25)

electron-screened transition,
234 - - \~1 ~2 u3

"--hole-screened transition.

(17)

where A represents any of the four-point functions. The source terms contain contributions from two-, four- and six-point functions: Q __ f)II +
A HA QA

The above given interpretations of V:byd ~1234 and TaflYd * 1234 as screened transitons are based on the observation, that the corresponding operator contain as a factor the operator for the annihilation of an electron hole pair providing the transition character. The second factor is in the first case the operator for an electron density and in the second case the operator for a hole density, which are correlated with the respective transitions. The equations for the two point-densities C~[ and D~2 ~ including their coupling to the four-point level are given by:
ih +

IV

+Q"

vI

(26)

As it turns out besides the density matrices already introduced there is only one further four-point function coupled on the four point level, namely: B~b~d=/,4~ b d3 ~ c4 a) ~ biexciton transition. 1234 - - XUl c2 The drift operators hf~ A and sources Q~, @A v, QVi are listed in Appendix A.

4. Systematic decoupling of the hierarchy


=E2" ~,
v

M b ~ ( - i V 2 ) Y ~ * - - E 1 " Z mva(iV1) Y~2b


v

a) General considerations
Obviously we could continue writing equations of motion for the six-point functions occurring as sources for the four-point density matrices. Proceeding in this way we would build up an inifinite hierarchy of equations of motion. This kind of hierarchy is a common feature of manyparticle problems. In general situations the search for systematic strategies to deal with this hierarchy will impose serious problems. Systems however which are reasonably described by our model are rather special in that all correlations have their origin in the action of the electromagnetic field. Therefore in our model there is a close relation between the hierarchy of equations of motion and the susceptibility expansion in powers of the electric field. This relation finds its quantitative expression in the following theorem, the proof of which is given in Appendix B:

+ I d3rj(glj

g2j) ( ~ c *~ljj2 iuaecb -- 2 Nljj avvb) 2 '


u

(18)
(19)

hfa c - Eb ( - iVg) - E . (iV1) . -ihf){f


c /

+ hg2DD{2~
c

= E 2 . ~ ' Mc~(ii72 ) y ~ f * _ Ei . ~, M ~ ( _ iV1) y~c


+I
~ d 3 r j ( V l j - - V2j ) [ v~ r ~j 12j

2c : ' j l" 2j

]Vcocflc'~ " /,

(20)
(21)

hO D ----E: ( - i E ) - E p (iV2).

The operators hf2 c and hO D describe a drift in configuration space, while the source terms involving two-point density matrices represent the generation of electron and hole densities respectively by interband transitions. The

Theorem. Let An be a n-point operator in normal order


according to the electron hole representation and let nc (rid) denote the number of electron (hole) operators con-

198 tained in A. such that n = n~ + na. Consider now a system whose time evolution is determined by the Hamiltonian (1) and which is initially in the ground state consisting of filled valence bands and empty conduction bands. Then it follows for the expectation value of A~: (A~) = cY(E m) with: m>max{n~,nd}.
h 2

- ihY~2b + hf2r Y~2 b =Ma~OI2-E12-E 1.~, M ~ C ; ~ - E 2 . Z Mb~D2~~


c

+S d3rj ( V u - V2J) -(Z e c c ~ b X2 T,13~b'~ ~ /i ajjl2 / ,


c h 2 13

(27)

A direct consequence of the above theorem is that the nonlinear response of a semiconductor material calculated to a fixed order in the electric field is influenced only by a finite number of density matrices. This offers the possibility for a systematic truncation of the hierarchy according to the following recipe: 9 choose the order in the electric field up to which the response has to be calculated; 9 write down equations of motion for all density matrices which are according to the above theorem of lower than the desired order; 9 neglect all source terms which are a priori known to be of higher order in the electric field. As a result one arrives at a closed set of equations of motion which by construction allows the calculation of the system response exactly to a given order in the electric field.

hfay=-ha)b~ - 2 m ~ A2-- ~ - m a A1 -- Vl12,

(28)

where h a)cv = Ec (k) Ik = 0 - E, (k) Ik = o denotes the energy gap between the bands under consideration.

--ih d~2b+ hf2cC~ b


v

_j" d3rj (Vlj_ V2j) ~, ~r ,jj2 ,


v

(29)

h2 h2 hfa c - ha)ba + 2m,m, A 1 - 2 m ~ A2"

(30)

-- ihD~2P + hf2DD~
=E2. Z M~Z Y ? ; * - E 1 . Z M*~ Y ~
c r

b) ;g3-Relevant equations of motion


The most important application of the prescription just presented is the derivation of a closed set of equations of motion from which the third order susceptibility )~3 can be calculated exactly. Inspection of the density matrices and their equations of motion introduced in Sects. 2 and 3, shows that besides the two-point density matrices yc~b12, C1ab and D~2 '~ on the four-point level only the fourpoint functions B~b~4 d, N f f ~ d, ~1234K' abrd ~..~nclTff2B3~ d contribute to )~3. The correlations K1234aacd and ~123~" r~ara can be ruled out because they are at least of ~7r But analyzing the six-point sources of the relevant functions reveals that there is an additional contribution to X3 resulting from:
zal3ydef =/,,a+ AB rAY ,,d A~ C{) 123456 -- \~1 ~2 w3 ~ 4 ~ 5

-j" d3rj- (V~j - V2j) ~, ~,j~2j~rc=a~,


c

(31)

h2 h2 hDD=ha~P +~m~ A1--2rn~ A2"


__ i177O a b y d ~- 17,("} ~ a b y d

(32)

= -E23 "Mb~, a23 Cff+E43"Ma~, ~43 Cla2 b


+ g 2 9Z
v azr A;avyd__l~ " ~ 1At ATavyb "~WtbvZV1234 ~4"/, ~ ' ~ d v ~ ~ 1432 v

- - E l "Z ~'~ 7iAr* 17tvb7d av ~1234


v

+ j d ~ j ( V4j - V3j + Vv - V~j) ~ =1z23~7~


v

(33)

exciton-biexciton transition. The operator for this six-point density matrix annihilates two electron hole pairs and creates another pair. It therefore describes transitions between excitonic and biexcitonic states. In order to take into account all contributions to X3 we have to extend our theory to the six-point level to include the equation of motion for 7afl~'def ~123456 " We shall write down the x3-relevant equations in effective mass approximation assuming a direct gap semiconductor with parabolic bands. Furthermore we shall assume the transitions to be directly allowed and neglect the k-dependence of the transition dipole M~o (k) resulting in a real space structure of the transiton dipole given by: M~f=Mcv(~12 with M~,,--Mc~(k)I~= o. With these assumptions the )c3 relevant equations read:

h ~ s - h (~Oav + ~%~) h2 ~- ~ma Zl l -- ~mb A 2 -- ~ 2 m A 3 -- ~m d A ,


~- V24V34V23.

h2

h2

h2

(34)

; t a ' T a B Y d A- ~ r
- - *'* ~ 1 2 3 4 --'~

To~I3y d
T * 1234

= -- E24. MaB 1~24 D]'~' + E43" Md~, ~ 4 3 D ~

+E:.~
- E I "~,
c

~'~cfl ~ ' 2 1 3 4

~"~-E3"~M~
c

~"~

~' 3124

M*~ ~2~3~

l~flcrd

--I d3ry (V4J - V3J -- V2J + Vii ) ~' ~j12j347cuflc'd'


c

(35)

199

hO T = h (Ogdr + o9~) h2 h2 h 2 A3-2~md A4 +2m~ A ~ - 2 m ~ A ~ - 2 m ~ h2


.... . . . . . . . . . . . . . . . i

r2 t \ t \~+
1"~ .................... A

t
"f'4

I \\

~+

~< / \ I

,'i,.4

ra abed B1234

+
_ihB~3~4a + ~ ~ o ~

v 4- v34
B n~b~d ~1234
Yff2b - -

(36)

$1~34

abed

a~d T~2~4

Fig. 1. Illustration of the molecular character of the transition densities S, T and B E4~. M ~ 641 Y3)2b (37) is illustrated in Fig. 1. Similarly T represents transitions involving the annihilation of a positive ion similar to the H + -molecule and the creation of a free hole. As is characteristic for transitions, S and T have a gap between a conduction and a valence band. The biexciton transition B is another example having as expected two interband gaps. The molecular character of B can be read off from the operator t-2B, which coincides apart from the gaps with the Hamiltonian for a molecule consisting of two positively and two negatively charged particles. In contrast the configuration space propagation of the excitonic occupation N is determined by an operator, which is the difference between two exciton operators, one operating on the coordinates r3, r 4 and the other one operating on rl, r 2. N therefore exhibits resonances near or at frequency zero, which is a typical feature of density like quantities. Finally we discuss the propagation of the six-point function Z and note that the corresponding operator is the difference between an exciton operator operating on rl, r 2 and a biexciton operator operating on r3, r4, rs, r 6. In accordance with our interpretation of Z as transition between excitonic and biexcitonic states we thus find h ~2z having a spectrum consisting of differences between exciton and biexciton energies. It is important to remember that the actual character of a quantity being the solution of a driven differential equation is determined by both, the characteristics of the O-operator as discussed, and the spatial and spectral structure imposed by the corresponding sources.

= + E43. M~r 643

@ E 2 1 " M b e ~21 ~

- - E 2 3 " M b , ~ 2 3 Yl~4d ,

h ~ . - - h(O~dy + COb~)
h2 ----ZI h2
h2 h2

A 3 --

A4
(38)

- - g12 ~- V 1 3 -

Vii 4 -

V23-~- V 2 4 -

V34.

At 'N O a* - - ~ ;t~ z ~ z AraB~d ,1234 ~,,~ ~ , 1 2M 3 4a flYd-- - E34" M d ~ (~34 Y2flll

(39)
hON -- h (o)dy - a) ~,)
+2

ha h~ h~ Zll + ~ m ~ / 1 2 A3 ma 2 m~

h~

/14
(40)

+ V~2- V34.
__ i h T a f l y d e f A_ ~r
~'~123456 ~'~Z~123456

7aflydef

..~ AFaflY d __ 12' 7Ill ..g ATafl ed = "~E56.Mfe~56~,1234 z-,36 " ~,~f7 t~ 36 ~ 9 1254

+ E~4. Ma~ ~34 N ~ g ~ - E4s" Ma~ cY4eN~f3g~


-- El2"

M2~

~ 1 2 "~

(41)

hf2 z - h (COdy + e)s~ - o) ~,) h2


h2

h2
h2

h2
h2

5. Dynamics induced factorization


-~" g12-- V34+ V 3 5 - V 3 6 - V45-~- V 4 6 - V56.

(42)

The four- and six-point density matrices are dynamic variables each having its own specific characteristics as imposed by their respective equations of motion. Thus the propagation in configuration space of the screened transition S is determined by an operator hl2s, which is essentially the difference of the kinetic energy operator for an electron at r~ and the Hamiltonian for an atom consisting of two electrons at r 2 and r 4 and a hole at r 3. Therefore in the transitions represented by S effectively a negative ion similar to the H - - a t o m is annihilated and a free electron is created. As a consequence S reflects on the one hand the binding energies brought forth by the Coulomb interaction leading to the negative ion and on the other hand describes a charge transfer from the center of mass of the ion to the position of the free electron as

In this section we demonstrate that for some of the npoint density matrices the solution of their equation of motion coincides to lowest order in the electric field with the RPA factorization. We begin the discussion with the excitonic occupation N. The RPA factorization of N reads

[1]:
Naflrd~ 1234 ~'~ y ~ * yf4a + C ; f D~,

= y o. y d+ G(z4).

(43)

We shall now try the RPA result as an ansatz to solve equation (39) to lowest order. To lowest order y~a has to fulfill the linearized equation (27):

- i h Yf4d+ ho)dY--2m~ A 4 - - 2 m ~ A a - V34 Y~4 d


= E34" Mdy 034, (44)

200 while Y2Pll a* obeys the adjoint equation:


ihYff'*+

Ihogs/3 .

. .AI . 2 m ~ A 2 - V~2 Y~* 2m~

= El2" M~*a012 ,

(45)

Multiplying equation (44) by Y~* and subtracting (45) multiplied by Y3~ a we find:
-- ih ~
I

functions of hg2 N can be separated, it is not guaranteed, and in general it even will not be true, that N ~ 2 a can be factorized in higher than lowest order in the electric field. Finally we have to discuss the six-point function Z. The operator hf2 z being the difference between a biexcitonic and an excitonic operator suggests an ansatz for a factorization: g a B , d e f__ v l ~ a * ~ , d e f ~_ G ( E 5) (47) 123456" - - ~ 21 x'~3456 ~ Using (47) together with (37) and (45) in analogy to (43)-(46) we get:

( Y ~ * Yf4a)
. h2 . . h2 . Z 3 - - V34

+ ha)a"

2m a

A4 2 m ,

-- ih vfla* yf4 d -21

~f

(yfla* l~,def .~4_l~(.) (v~rfla* R,def ~


kx21 ~3456 ] . . . . . Z\*21 ~3456 ]

. . . . hog~p 2rn~ AI ih ~ @ h ~ N l ~t

2rn~ A 2 - V12

= E 56 . M f ~ 6 56 y~a * Y~a - E 36 . M f , 6 36 Y~a * y~4a

+ E34. Me , 634 y~a* yr f _ E4s. M a ,


: E34"

~45

Y2Pll a* Y~6f
(48)

r2flla* y~4d
(46)

E12. X~*~~ 12 B~4dse6 f

"~- ~ ( E 5 )"

g d , ~34 Z2f111 a* -- E l 2 " ga~/~ ~12 Z~4d"

Thus Y~a*Yf4 a solves the equation of motion for N~ , a t,, 1234 ~ lowest order. Because (39) is an inhomogeneous linear differential equation its most general solution is given by y ~ * y ~ d plus the general solution of the corresponding homogeneous equation. The homogeneous part has to be determined from appropriate boundary conditions for the asymptotic behavior at large distancies. These conditions are generally fulfilled by the RPA factorization. We therefore conclude, that the RPA treatment (43) of N is exact to lowest order. Although our analysis and the RPA approach both yield the same factorization for N, there are important differences : 9 The RPA factorization is usually motivated as the first step of a cumulant expansion, where the corresponding irreducible rest is neglected. Therefore from a traditional point of view in general there is no hint indicating the order in the electric field of the irreducible rest. This becomes particularly clear when analyzing the four-point densities S, T and B. The assumption that the corresponding irreducible rests would be of higher order in the electric field would lead to the conclusion, that all biexcitonic contributions to )C3 vanish, which is in contradiction to experiments as well as to our equations of motion. 9 In our treatment the factorization of N is not necessary to truncate the hierarchy. Instead it is a remarkable special property generated by the dynamics of the system. Another point to be emphasized is the difference between the inhomogeneous equation considered here and the corresponding eigenvalue problem. In the latter case the fact that hf2 u is the difference between operators operating on disjoint pairs of variables would be sufficient to allow for separated eigenfunctions. Indeed a complete set of eigenfunctions of hi2 N is given by products of excitonic wave functions. On the other hand in the inhomogeneous case in order to yield a factorized solution the source must have a very specific structure. Although the eigen-

Taking into account that we have already proved (43), the above equation (48) implies that indeed the relation z a123456 B e a e f - --- vBa*eeaef4_ G ( E 5) holds. This result can be ~ 21 ~3456 compared with the factorization proposed by the corresponding cumulant expansion [26-28]. Such a treatment in the RPA-spirit also leads to lowest order in E to the relation (47) as is demonstrated in Appendix C. In conclusion we have found that our model generates a dynamics such that the exact solutions for the density matrices N and Z coincide to lowest order in the exciting field with the results of a RPA like treatment. On the other hand such a decoupling is incorrect even to lowest order for the four-point density matrices S, T and B. These quantities therefore have to be determined directly from their respective equations of motion.

6. Concluding remarks
We have presented a description of semiconductors excited by coherent electric fields based on density matrix theory. Because correlations in such systems are generated mainly by the interaction with the driving field, a susceptibility expansion of the system response provides a relevant ordering scheme. We have shown how this expansion is related to the hierarchy of equations of motion for n-point density matrices. Our main result is a closed set of equations of motion allowing the calculation of the exact model response up to ff (E3). Furthermore we have shown that for some of the density matrices a RPA like factorization is exact to lowest order in the electric field. As a first application of our method we will present in a further paper [21] a calculation of the influence of the biexciton on the dynamical Stark effect as measured by Hulin et al. [ 15]. Apart from this special example we expect quite generally that the approach presented in this paper will give insight into the role of dynamic screening or collective resonances (like the biexciton resonance) in time resolved experiments.

201 Appendix A Drift operators of the equations of motion for four-point density matrices:
Plg2S(~na = _ E a (iV1) + E b ( - iV2) - E r (iV3) - E 3" ~ Mc v (iV3) N ~ c
o

+ E 4 Z M.o( - i V 4 ) -~-1 4 ~ 23
..... Q iv B1234 E,-~
c

M . (iV1) ~ ~4 cbyd
(iV3) ~c 3b 2~ 1d 4

+ E d( - iV4) + V24- V34- V23, ~- E3" 2 Mcy

ha~,;~:~ = E~ ( - iVO - Ep (iV9 - E . (iVy)


+ E a( -- iV4) + V23-- V24-- V34, hf2B,~:~ = - E~, (iV,) + Eb ( -- i v y )
--

-G'7,
/3

M ~ o ( - ;re ~ T.~,. ' 21 ~2134 Mdo( - i~7 ~~ 7-~.b ' 42 4132


v

+Ee'Z
IV __

Ey( i ~ 7 3 )

-k_ Z d ( __ i ~ 7 4 )

- v~ + v~3- v~4- v~ + v~4- ~ 4 ,


hs N,%~,,= -- E a ( iV~ ) + E I~ (iV2) - E , ( - iV3) + E d( - iV4) + V~2- V~4 , h~2 K~;~ = -- E~ ( i V 1 ) - E b (iV2) + E c ( - iV3) + E d( - iV4) - V~ + V34 , hs ~ = E~ ( -- i V , ) + E ,~ ( - iV2) - E r (iV3)

Q N~:~: ~ - + G " Z M ~ ( - ivy) ~1~4 c


--

E 3 . 2 M~y ( 1'% )
c

d~Z~* $43 21

Jc EI " 2 v
v IV

Mva(iV1)~t2134TflvYd
,

- E4"Z M d o ( - i V 4 ) T3421 .Pa*


= .

9 bcvd Mva(tVI)S2314 tl

~- E2" Z Mvb(iV2) ~acvd~'1324

- E6 (iV4) - Va2 1/34,


-E3" 2

Sources for the four-point density matrices involving twopoint functions:

Mcv( - i~73) ~ d b v a * o 4 2 3 1

+ E4" ~. M d o ( --lV4)~3241 ..... b~,* ,

Q ~}::~= -- E2~-M br C~4 d + E4~-M4d3 ~ C~?,


II Q o~ . TI234
. . .
c~y E4~-M~D,~ +E 4 ~ " M2 Dr~

a Ivp,o q~, = _ E l . ~. M~,c ( - iVO ~234t T Z~ac


c

QII __~ ;~ardy ..... z543"1v143 B1234

Y ; b - E4~. M ~

Y~2b

+E2"~
c

Mzc(-~

ii7

~ "1342 Ta~ dc "2J

+ E ~ . M ~ 7 Y~4d - E~3. M b ~
II __ *

Y~4 d,

--

E 39~ M<, (iV3) "4213T~~


c
9

QN,;~,~_ _ E12. M~2,e yf4d + E43. Md~, y ~ a * .

+ E4. ~. M c a ( i V 4 ) -t TrZ~c* 3214

Sources for the four-point density matrices involving fourpoint functions" ,v = _ E , . ~ , M , ~ (t" .~ra 171)B,~4 Qs,~
o

Sources for the four-point density matrices involving sixpoint functions'


VI __ Qs,~'J-~ d3rj (g4j - - g3j + ~j --

gu)

+ e~. ~ M ~ ( - iV9 ~ ~'~~34 v


-- E4"

Z
v

M dv

9 ( --/V4)

avyb N14 32

QV~ .... T1234


"3 ) (IV ~bu K13 24 ,

~ d3rj (V4j- V3j- V2j + VU )

+ E 3 9~, M ~
c

QT~BI231 ....
IV

El" Z Mac ( -- iW " 1] "~~ 2 1 3 4


c

+ E2" Z McZ (iV2) N f { ~ d c

202

d QVlb}, B~2~

- ~ d30 (V4j - V3j + V2j - Vlj)

<(
QVl~x~f~ = -I

2b3'

n--*n+l" Obviously we can write:

IP.+l,v>

=Ev(n+l) Yv(n+l)" P~,a>.


Yv(n + 1)" I P,~,,~>

dgrJ(V4J- V3]+ V2j- VIj)

Therefore it follows:

>
QK~[~ ~- --I d3rj (V4j
VI __

=Ev(n+l)[-d,

I?'v?(n+1)1 " ] P~,~>

27 V3j

__

W2j

__

Vlj )

+ ~,.2(,+, ) f : ( , + , ) . d . I P , , ~ .

(51)

)
Qz~e~o- - ~ d3r# (V~] + V2j
VI __ __

according to the induction hypothesis

v',n"

V3~

__

V4~)

Calculation of [A, Y;(.+I)] ~* yields:

[c,; , 317'] :a j
[Do. ,

02" m

r17*,

]~##t] = 6,+ 6=~, Yt~b* .

Appendix B
Proof of the theorem connecting the dynamic hierarchy of density matrices with the susceptibility expansion
In this appendix we apply the Schr6dinger picture. To facilitate the proof we introduce the notion of a n-pair state of order n denoted [P~,v>. [P.,v> represents a Fockspace state generated from the ground-state [0> (filled valence bands and empty conduction bands) by application of n creation operators for electron-hole pairs with a prefactor f.,v being proportional to a product of at least n components of the electric field, v specifies all spatial and band indices needed to identify the pair states involved. If v (1). 9 9v (n) are the indices of the n pairstates represented by v we can write: (49)
n factors

These equations imply our statement: In the case of d = ~yc the right hand side of (51) has the desired form, because Ev(n+l)- [Pn F> is obviously a n-pair state of order n and for Ev(~+i')~" ] P~,~> and E~(~+~)/)~. [P~,~> using the induction hypothesis proves our statement. In the other cases A = .dlf' and .d -D~j - ~ ~' we simply have to note that E v(, + 1) I?,*- [P,, F> is a n + 1-pair state of order n + 1. Therefore we have proved, that application of one of the operators Y~j " ~ ", C~ ~e~"; D~j ",~, on a n - p a i r state of order n yields a linear combination of such states having in general different n's. Next we shall show the following corollary: Corollary. Consider a system being at time t = t o in the ground state: [~u> [,=~o= [07 with a time evolution determined by the Hamiltonian H = H o + Hem + H~ according to (1). Then it follows that for all t > to the system is in a state [ r which is a linear superposition of npair states of order n.

where:

f~,v = const. E~(1) . . . . .

Ev(m)

Proof of the Corollary. As a consequence of the lemma we find that:

= ~Y(E m) with: m > n . In a first step we prove: Lemma. Let A be one of the operators ~ ; then it follows" C l f ' ; Jl~ ~"

/41L,v> = F, <.,.. Ie..,v.>.


n',v'

A[P,,v> = ~, av,,, IPo,,~,>


it',n"

with suitably choosen a~,,,.

(50)

Proof of the Lemma. We shall prove the lemma by induction with respect to n starting from n = 0:

A IPo, O = fo, v ' A [0) = 0 ,


which proves the induction hypothesis setting in (50) all
a~,,,, = 0 .

To see this we note that: a) Ho is a linear combination of operators Cu a n d / ) v ' Thus the lemma can be applied immediately, b) Hem is a linear combination of operators E~ L and E u I7"~.In the first case again direct application of the lemma is possible, while the statement is trivial in the second case. c) H e is a linear combination of operators which are of the form: Cl, J u , ; /J,, C,; C~ C~, or /J~,/},. Applying the lemma twice yields in all cases the desired result. Now we divide the time interval t - t o in N infinitesimal intervals of length A t = (t-- to)/N. If N is great enough the time evolution of the system from time tj =-jA t+ to to time tj + A t is given by:

203

I~,(tj+At))=

(l+7~-H(tj)I~'(tj)). )
g(tN_,) H(to)
. . . .

Appendix C Comparison with the RPA factorization on the six-point level


The factorization derived from a cumulant expansion for the six-point function Z neglecting the irreducible rest reads [26-28]'
z a fl),dz f 123456 v I 3 a * f R ) ' d e f -"21 t ~3456 (y~4dy~Z Y3Y6fy;d)}

Therefore the state of the system at time t can be approximated by:

I~(t))~ I~,N(t))-- 1 +/~


9 1+~

~'(to)),

which becomes exact in the limit N--+ oo. For fixed N the above considerations show that [ ~UN(t)) is a linear combination of n-pair states of order n. Taking the limit completes our proof of the corollary. We are now prepared for the actual proof of our theorem: Theorem. Let A. be a n-point operator in normal order according to the electron hole representation and let n~ (nd) denote the number of electron (hole) operators forming A~ such that n = nc + n~. In a system of the type considered in the above corollary it follows for the expectation value of A~ :

-~ ~34 I,~'1256 - - k * 2 1
-- v Y f f N' a f e d *36 i,*, 1254 ( V f a * Y~a/-~ C ~ : D ~ \*21 . e )}

-}- *56 I,~,1234


_

--\

21
YU+

,,,of),i_ *54 "txT 1236 k'~21

, osn a), ~'-'16 ~ 2 3

)}

"J- C ~ {
~16

,Tfl)'ef--2356 (D2f3)' Y5o f ~ ~2354 \~23

D2f15e ~Y3~Z)}
n fie ~25

-- t'~aff T f ) , e d FI fly S ~ a d e f - @ ~ 2 3 I.~1456

t l-} sl)' r e d "~54 ( C ad y e f _ _ \'~14 "56

y~4a)}

cla~fy;d)} Cl26 f yfd)}

-- 17 fie f ~ a d ) , f __ ( ( w a d v ) ' f - ~ 2 5 [~1436 \"J14 *36 (~ad 1 f~ l"i fl)' r 5 e l + ~14 23 ~- C ~6f { D 2f155 e ~Y )' d

(An) = ~ ( E m) with: m>=max{nc, na}.


As A. is in normal order we can write:

D~ e

r3rf)}

--23/) fly r5~4d)}

+ Y~=*{ YfJ Y H - r~6fY:4a)}

(52)

A.=A.+.A. ,
where A.+ - product of n~ + electron and n ] hole creation operators, and A._ = product of n~ electron and nff hole annihilation operators. The leading order contributions are as expected of order G (E 3). Inspection of (52) reveals that only the first five lines and the last line contain third order contributions. Taking into account that the factorization .NTafl)'d=, 1 2 3 4 Y2B1 ~* yf4d+ ~ ( E 4) has already been proved, it is found that all third order contributions on the second to fifth line cancel. Finally combining the first and the last line demonstrates that (52) coincides to lowest order with our result (47).

~ n o = n + +n~- ;
It follows: _d. [Pj,~) = 0

nd=n + +n a .

for all j < n2-

or

j < n~-,

References
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because for j < n~- (j < n2) An annihilates more electrons (holes) than contained in I Pj,~). Therefore we conclude from our corollary:

J. I~,(t))= ~ ' ( E m ' ) ;


Analogously we find:

m' >max{n~-,nff}.

(q/(t)iA,+ = G ( E m " ) ;
Finally arriving at:

m" >max{n+,nd+}.

( A . ) =(~u (t)[A,+ .A._ I ~, (t)) = O ( e ~ ) , with: m > max{n + , n ] } + max {n~-, n~- } > max{n o, na}. which was the statement to be proved.

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