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# Correlations in interfering electrons irradiated by nonclassical microwaves

## I Introduction

Interference of electrons that encircle a magnetostatic flux has been studied for a long time since the pioneering work of Aharonov and Bohm . It has applications in various contexts, for example in conductance oscillations in mesoscopic rings , neutron interferometry , and ‘which-path’ experiments .

A further development is the replacement of the magnetostatic flux with an electromagnetic field. In this case, the electrons feel not only the vector potential but the electromagnetic field. Therefore, the objective in this ‘ac Aharonov-Bohm’ effect is very different from the ‘dc Aharonov-Bohm’ effect (with magnetostatic flux). In the latter case the physical reality of the vector potential has been demonstrated and the subtleties of quantum mechanics in non-trivial topologies have been studied. The former case constitutes a non-linear device, where the interaction between the interfering electrons and the photons leads to interesting non-linear phenomena  like amplification and frequency conversion. Indeed the non-linearity can be seen in the intensity of the interfering electrons which is a sinusoidal function of the time-dependent magnetic flux. Our study is related to recent work on the interaction of mesoscopic devices with microwaves .

One step further in this line of work is to use in these experiments non-classical microwaves, where the quantum noise is carefully controlled. In this case, we can quantify how the quantum noise destroys slightly the electron interference . More generally, we have here two coupled quantum systems (photons and electrons) and we can study how various quantum phenomena associated with the non-classical electromagnetic field cause corresponding quantum phenomena on the electrons. For example, we can study how the quantum statistics of photons affects the quantum statistics of the electrons; how the entanglement of two-mode non-classical microwaves affects the electron interference; etc.

In this paper we study how various types of non-classical microwaves affect both the average intensity and the spectral density of the interfering electrons. The results are compared with those for classical microwaves (Section II). We also consider two-mode microwaves with frequencies $`\omega _1`$ and $`\omega _2`$ in Section III, where we show that we get different results for rational and irrational values of $`\omega _1/\omega _2`$. We interpret these results in terms of emission and absorption of photons by the non-linear device of the interfering electrons. This discussion shows the potential use of the device for frequency conversion. Two-mode microwaves can be factorizable, separable or entangled . We study how such deep quantum phenomena in the microwaves can affect the electron interference. The problem is complex and it is approached through examples which demonstrate the effect. In particular, we compare and contrast the effect on electron interference, of an entangled microwave state with that of the corresponding separable microwave state. We conclude in Section IV with a discussion of our results.

## II One-mode microwaves

### II.1 Classical microwaves

Interfering electric charges in mesoscopic devices that follow two different paths $`C_0`$ and $`C_1`$ are considered. A magnetic flux $`\varphi `$ is threading the surface between the two paths. This is referred to as the dc or ac Aharonov-Bohm experiment, according to whether the magnetic flux is time-independent or time-dependent, correspondingly. In the dc Aharonov-Bohm experiment the electric charges feel only a vector potential. In the ac Aharonov-Bohm experiment the electric charges also feel an electric field, which is induced according to Faraday’s law. The ac Aharonov-Bohm effect can be realised experimentally: at low frequencies using a solenoid with a suitable time-dependent current; or at high frequencies using a waveguide, whose magnetic and electric fields are perpendicular and parallel to the plane of the two paths, respectively (Fig. 1).

Let $`\psi _0`$, $`\psi _1`$ be the electron wavefunctions with winding numbers $`0,1`$ correspondingly, in the absence of magnetic field. The effect of the electromagnetic field is the phase factor $`\mathrm{exp}[ie\varphi (t)]`$ and the intensity is

$$I(t)=|\psi _0+\psi _1\mathrm{exp}[ie\varphi (t)]|^2=|\psi _0|^2+|\psi _1|^2+2|\psi _0||\psi _1|\mathrm{}\{\mathrm{exp}[i(\sigma +e\varphi (t))]\}$$
(1)
where $`\sigma =\text{arg}(\psi _1)\text{arg}(\psi _0)`$. Units in which $`k_B=\mathrm{}=c=1`$ are used throughout. For simplicity we consider the case of equal splitting, in which $`|\psi _0|^2=|\psi _1|^2=1/2`$ and let $`\sigma =0`$. In this case we get

$$I(t)=1+\mathrm{cos}[e\varphi (t)].$$
(2)
In general, for a complex intensity $`I(t)`$ the autocorrelation function is defined as

$$\mathrm{\Gamma }(\tau )=\underset{T\mathrm{}}{lim}\frac{1}{2T}_T^TR(t,\tau )𝑑t;R(t,\tau )I^{}(t)I(t+\tau ).$$
(3)
The following properties of the autocorrelation function are well known:

$`\mathrm{\Gamma }(\tau )=\mathrm{\Gamma }^{}(\tau );\mathrm{\Gamma }(0)0;|\mathrm{\Gamma }(\tau )|\mathrm{\Gamma }(0).`$ (4)
It will be explained later that these relations are also true in the case of non-classical microwaves. The normalized autocorrelation function is defined as

$`\gamma (\tau )={\displaystyle \frac{\mathrm{\Gamma }(\tau )}{\mathrm{\Gamma }(0)}};\mathrm{\hspace{0.33em}\hspace{0.33em}\hspace{0.33em}\hspace{0.33em}\hspace{0.33em}0}|\gamma (\tau )|1.`$ (5)
For one-mode microwaves, the autocorrelation function $`\mathrm{\Gamma }(\tau )`$ for the charges will be periodic with a period $`2\pi /\mathrm{\Omega }`$, where $`\mathrm{\Omega }`$ is, by definition, the frequency associated with the periodic function $`\mathrm{\Gamma }(\tau )`$. An expansion of $`\mathrm{\Gamma }(\tau )`$ into a Fourier series gives the spectral density $`S_K`$:

$`S_K`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }}{2\pi }}{\displaystyle _0^{2\pi /\mathrm{\Omega }}}\mathrm{\Gamma }(\tau )\mathrm{exp}(iK\mathrm{\Omega }\tau )𝑑\tau `$
$`\mathrm{\Gamma }(\tau )`$ $`=`$ $`{\displaystyle \underset{K=\mathrm{}}{\overset{\mathrm{}}{}}}S_K\mathrm{exp}(iK\mathrm{\Omega }\tau ).`$ (6)
Equation (4) implies that the coefficients $`S_K`$ are real numbers, for both classical and non-classical microwaves.

We consider the case where the classical time-dependent flux is given by

$$\varphi (t)=\varphi _1\mathrm{sin}(\omega t)$$
(7)
and using Eqs.(2),(3) we find the autocorrelation function:

$$\mathrm{\Gamma }_{cl}(\tau )=\left[1+J_0(e\varphi _1)\right]^2+2\underset{K=1}{\overset{\mathrm{}}{}}\left[J_{2K}(e\varphi _1)\right]^2\mathrm{cos}(2K\omega \tau ),$$
(8)
where $`J_K`$ are Bessel functions. Comparison of Eqs.(II.1),(8) shows that $`\mathrm{\Omega }=2\omega `$ and

$$S_0=[1+J_0(e\varphi _1)]^2;S_K=[J_{2K}(e\varphi _1)]^2.$$
(9)
We note that $`S_K=S_K`$. This is because in the classical case considered in this section, $`I(t)`$ is real and consequently $`\mathrm{\Gamma }(\tau )`$ is real. Therefore Eq.(4) shows that $`\mathrm{\Gamma }(\tau )`$ is an even function, which implies that $`S_K=S_K`$. It is stressed that in the non-classical case considered next, $`\mathrm{\Gamma }(\tau )`$ is complex in general and $`S_KS_K`$.

### II.2 Non-classical microwaves

A monochromatic electromagnetic field of frequency $`\omega `$ is considered, at temperatures $`k_BT<<\mathrm{}\omega `$. In quantized electromagnetic fields the vector potential $`A_i`$ and the electric field $`E_i`$ are dual quantum variables. For a loop $`C=C_0C_1`$ (where $`C_0`$ and $`C_1`$ are the paths corresponding to 0,1 winding), which is small in comparison to the wavelength of the microwaves, the $`A_i`$ and the $`E_i`$ can be integrated around $`C`$ and yield the magnetic flux $`\varphi =_CA_i𝑑x_i`$ and the electromotive force $`V_{\mathrm{EMF}}=_CE_i𝑑x_i`$, correspondingly, as dual quantum variables. The size of a mesoscopic device is usually of the order of $`0.1\mu m`$ and is indeed much smaller than the microwave wavelength. The annihilation operator is now introduced as $`a=2^{\frac{1}{2}}\xi ^1\left(\varphi +i\omega ^1V_{\mathrm{EMF}}\right)`$ and the corresponding creation operator, where $`\xi `$ is a constant proportional to the area enclosed by $`C`$. The flux operator is consequently written as $`\varphi (t)=\mathrm{exp}(itH)\varphi (0)\mathrm{exp}(itH)`$, where $`H`$ is the Hamiltonian that contains the $`\omega a^{}a`$ term and an interaction term. In the ‘external field approximation’ the interaction term, which describes the back-reaction from the electrons on the electromagnetic field, is neglected. This is a good approximation for external fields which are strong in comparison to those produced dynamically by the currents in the mesoscopic device (back-reaction). In this approximation the interaction term can be ignored and we get

$$\widehat{\varphi }(t)=\frac{\xi }{\sqrt{2}}\left[\mathrm{exp}(i\omega t)a^{}+\mathrm{exp}(i\omega t)a\right].$$
(10)
The phase factor $`\mathrm{exp}(ie\varphi )`$ is now the operator

$$\mathrm{exp}\left[ie\widehat{\varphi }(t)\right]=D\left[iq\mathrm{exp}(i\omega t)\right],q=\frac{\xi e}{\sqrt{2}}$$
(11)
where $`D(\lambda )`$ is the displacement operator $`D(\lambda )=\mathrm{exp}(\lambda a^{}\lambda ^{}a)`$. The interference between the two electron beams is described by the intensity operator

$`\widehat{I}(t)=1+\mathrm{cos}\left[e\widehat{\varphi }(t)\right]=1+{\displaystyle \frac{1}{2}}D\left[iq\mathrm{exp}(i\omega t)\right]+{\displaystyle \frac{1}{2}}D\left[iq\mathrm{exp}(i\omega t)\right].`$ (12)
Let $`\rho `$ be the density matrix describing the external non-classical microwaves. We can now calculate the expectation value of the electron intensity

$$I(t)\text{Tr}\left[\rho \widehat{I}(t)\right]=1+\frac{1}{2}\stackrel{~}{W}(\lambda )+\frac{1}{2}\stackrel{~}{W}(\lambda );\lambda =iq\mathrm{exp}(i\omega t),$$
(13)
where $`\text{Tr}\left[\rho D(\lambda )\right]\stackrel{~}{W}(\lambda )`$ is the Weyl (or characteristic) function which has been studied by various authors including ourselves (e.g.  and references therein). The tilde in the notation reflects the fact that the Weyl function is related to the Wigner function through a two-dimensional Fourier transform. Physically the $`\mathrm{Tr}\left[\rho \widehat{I}(t)\right]`$ describes the exchange of photons between the electrons and the external electromagnetic field. Expansion of the exponentials in Eq.(13) gives an infinite sum of terms of the type $`\mathrm{Tr}\left[\rho (ae^{i\omega t})^N(a^{}e^{i\omega t})^M\right]`$ which describe processes in which the electrons emit $`M`$ photons to the external electromagnetic field and at the same time absorb $`N`$ photons from the external electromagnetic field. Summation of the appropriate coefficients leads to Bessel functions which appear in most of the calculations throughout the paper. We note that a similar expansion and a similar interpretation can also be made in the classical microwave case. However, in this case instead of creation and annihilation operators we have classical numbers and the interpretation is perhaps less convincing.

Ref. has considered several density matrices and presented results for $`\stackrel{~}{W}(\lambda )`$. Using them we have calculated $`I(t)`$ for various quantum states of the microwaves. We are also interested in the quantity

$$R(t,\tau )\text{Tr}\left[\rho \widehat{I}^{}(t)\widehat{I}(t+\tau )\right]$$
(14)
which is calculated for various density matrices, as well as $`\mathrm{\Gamma }(\tau )`$ using Eq.(3). The Fourier series of Eq.(II.1) leads to the coefficients $`S_K`$.

We note that using the relation

$$\mathrm{\Gamma }(\tau )=\underset{T\mathrm{}}{lim}\frac{1}{2T}_T^T\text{Tr}\left[\rho \widehat{I}^{}(t)\widehat{I}(t+\tau )\right]𝑑t$$
(15)
in conjunction with the fact that for any operator $`\widehat{O}`$, $`\text{Tr}\left(\widehat{O}^{}\right)=\left[\text{Tr}(\widehat{O})\right]^{}`$, we prove $`\mathrm{\Gamma }(\tau )=\mathrm{\Gamma }^{}(\tau )`$ and therefore the coefficients $`S_K`$ are real numbers. As we already pointed out, $`\mathrm{\Gamma }(\tau )`$ is in general complex. This is intimately related with the fact that the operators $`\widehat{I}^{}(t)`$ and $`\widehat{I}(t+\tau )`$ do not commute. In fact, the imaginary part of $`R(t,\tau )`$ is $`(1/2)\text{Tr}\{\rho [\widehat{I}(t),\widehat{I}(t,\tau )]\}`$. In the classical case, these quantities are not operators, they commute and consequently $`R(t,\tau )`$ is real.

#### II.2.1 Microwaves in coherent states

For coherent states $`|A=D(A)|0`$ the $`R(t,\tau )`$ is

$`R_{coh}(t,\tau )`$ $`=`$ $`1+\mathrm{exp}\left({\displaystyle \frac{q^2}{2}}\right)\mathrm{cos}\left[2q|A|\mathrm{cos}(\omega t\theta _A)\right]`$ (16)
$`+\mathrm{exp}\left({\displaystyle \frac{q^2}{2}}\right)\mathrm{cos}\left[2q|A|\mathrm{cos}(\omega t+\omega \tau \theta _A)\right]`$
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left\{q^2[1+\mathrm{exp}(i\omega \tau )]\right\}\mathrm{cos}\left[4q\mathrm{cos}\left({\displaystyle \frac{\omega \tau }{2}}\right)|A|\mathrm{cos}\left(\omega t+{\displaystyle \frac{\omega \tau }{2}}\theta _A\right)\right]`$
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left\{q^2[1\mathrm{exp}(i\omega \tau )]\right\}\mathrm{cos}\left[4q\mathrm{sin}\left({\displaystyle \frac{\omega \tau }{2}}\right)|A|\mathrm{sin}\left(\omega t+{\displaystyle \frac{\omega \tau }{2}}\theta _A\right)\right]`$
where $`\theta _A=\text{arg}(A)`$. Using Eq.(15) the electron autocorrelation function $`\mathrm{\Gamma }(\tau )`$ for microwaves in coherent states is found as

$`\mathrm{\Gamma }_{coh}(\tau )`$ $`=`$ $`1+2\mathrm{exp}\left({\displaystyle \frac{q^2}{2}}\right)J_0\left(2q|A|\right)`$ (17)
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left\{q^2\left[1\mathrm{exp}(i\omega \tau )\right]\right\}J_0\left[4q\mathrm{sin}\left({\displaystyle \frac{\omega \tau }{2}}\right)|A|\right]`$
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left\{q^2\left[1+\mathrm{exp}(i\omega \tau )\right]\right\}J_0\left[4q\mathrm{cos}\left({\displaystyle \frac{\omega \tau }{2}}\right)|A|\right].`$
In contrast to the case of classical microwaves, $`\mathrm{\Gamma }_{coh}(\tau )`$ is now a complex function and $`S_KS_K`$. This is a periodic function with period $`\pi /\omega `$ and a Fourier series analysis is performed numerically as in Eq.(II.1).

#### II.2.2 Microwaves in squeezed states

Squeezed states are defined as

$`|B;r\vartheta `$ $`=`$ $`S(r\vartheta )|B=S(r\vartheta )D(B)|0`$ (18)
$`S(r\vartheta )`$ $`=`$ $`\mathrm{exp}\left[{\displaystyle \frac{r}{4}}\mathrm{exp}(i\vartheta )a^2+{\displaystyle \frac{r}{4}}\mathrm{exp}(i\vartheta )a^2\right].`$ (19)
where $`S(r\vartheta )`$ is the squeezing operator. The expectation value for the electron $`R_{sq}(t,\tau )`$ is given by

$`R_{sq}(t,\tau )`$ $`=`$ $`1+\mathrm{exp}(Y_1)\mathrm{cos}(X_1)+\mathrm{exp}(Y_2)\mathrm{cos}(X_2)`$ (20)
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left[iq^2\mathrm{sin}(\omega \tau )\right]\mathrm{exp}(Y_3)\mathrm{cos}(X_3)`$
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left[iq^2\mathrm{sin}(\omega \tau )\right]\mathrm{exp}(Y_4)\mathrm{cos}(X_4)`$
where the $`Y_j`$ and $`X_j`$, are given in the Appendix. Using this result we have calculated the $`\mathrm{\Gamma }_{sq}(\tau )`$ numerically. It can easily be verified that for $`r=0`$ the squeezed states results reduce to the coherent states results. $`\mathrm{\Gamma }_{sq}(\tau )`$ is a periodic function with period $`\pi /\omega `$ and a Fourier series analysis is performed numerically as in Eq.(II.1).

#### II.2.3 Microwaves in thermal states

For thermal states, the $`R(t,\tau )`$ is

$`R_{th}(t,\tau )`$ $`=`$ $`1+2\mathrm{exp}\left[{\displaystyle \frac{q^2}{2}}\mathrm{coth}\left({\displaystyle \frac{\beta \omega }{2}}\right)\right]`$ (21)
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left[iq^2\mathrm{sin}(\omega \tau )2q^2\mathrm{sin}^2\left({\displaystyle \frac{\omega \tau }{2}}\right)\mathrm{coth}\left({\displaystyle \frac{\beta \omega }{2}}\right)\right]`$
$`+{\displaystyle \frac{1}{2}}\mathrm{exp}\left[iq^2\mathrm{sin}(\omega \tau )2q^2\mathrm{cos}^2\left({\displaystyle \frac{\omega \tau }{2}}\right)\mathrm{coth}\left({\displaystyle \frac{\beta \omega }{2}}\right)\right]`$
and clearly $`\mathrm{\Gamma }_{th}(\tau )=R_{th}(\tau )`$. The $`\mathrm{\Gamma }_{th}(\tau )`$ is a periodic function with period $`\pi /\omega `$ and its Fourier coefficients are calculated numerically.

### II.3 Results

Numerical results are presented for the four cases: classical microwaves and non-classical microwaves in coherent, squeezed and thermal states. For a meaningful comparison, we consider the case where the average number of photons $`N`$ in coherent, squeezed and thermal states is the same:

$`N=|A|^2`$ $`=`$ $`\left[\mathrm{sinh}\left({\displaystyle \frac{r}{2}}\right)\right]^2+\left[\mathrm{cosh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{sinh}\left({\displaystyle \frac{r}{2}}\right)\right]^2B^2`$ (22)
$`=`$ $`{\displaystyle \frac{1}{\mathrm{exp}(\beta \omega )1}}.`$
For the classical case we took $`\varphi _1^2=2|A|^2=2N`$. In all results of Figs. 2 to 5, $`\omega =10^4`$ (which in our units is $`eV`$), $`N=100`$, $`r=5.5`$.

Fig. 2 shows the $`I(t)`$ as a function of $`\omega t`$. In Fig. 3, the absolute value of the normalized autocorrelation function $`|\gamma (\tau )|`$ \[Eq.(5)\] is shown as a function of $`\omega \tau `$. The period of $`|\gamma (\tau )|`$ is $`\pi /\omega `$ (i.e., $`\mathrm{\Omega }=2\omega `$) and the plots are presented from $`0`$ to $`\pi `$. As explained earlier the $`\gamma (\tau )`$ is real in the case of classical microwaves, but it is complex in general in the case of non-classical microwaves. This is shown explicitly in Fig. 4, which includes the imaginary parts of $`\gamma (\tau )`$ for all cases, as a function of $`\omega \tau `$. Fig. 5 shows the Fourier coefficients $`S_K`$ ($`K=2,\mathrm{},2`$).

The results quantify the effect of quantum noise on interference. All microwaves that we have considered have the same average number of photons and they differ in the quantum noise. For the classical microwaves (where the concept of number of photons is not applicable) the amplitude is equal to the amplitude of the microwaves in the coherent state. These four types of microwaves lead to different electron interference results. Fig. 2 shows clearly that $`I(t)`$ is different in all these cases. Fig. 3 shows that the absolute normalized electron autocorrelations are different, with the exception of the classical result which is almost identical to the coherent result. The imaginary part of the electron autocorrelation (Fig. 4) distinguishes the classical from the non-classical microwave cases. It is zero for classical microwaves and takes various distinct non-zero values for different types of non-classical microwaves. The same effect can also be seen through the spectral density coefficients $`S_K`$ in Fig. 5 which are simply the Fourier transform of the electron autocorrelation function (Eq.(6)).

## III Two-mode microwaves

### III.1 Classical microwaves

The case of classical two-mode microwaves

$`\varphi (t)=\varphi _1\mathrm{sin}(\omega _1t)+\varphi _2\mathrm{sin}(\omega _2t).`$ (23)
is considered. In this case Eq.(2) gives the electron intensity

$$I(t)=1+\mathrm{cos}[e\varphi _1\mathrm{sin}(\omega _1t)+e\varphi _2\mathrm{sin}(\omega _2t)],$$
(24)
which is a periodic function. The autocorrelation function is different in the two cases where the ratio $`\omega _1/\omega _2`$ takes rational and irrational values. The physical reason for this is that in the rational case, where $`\omega _1/\omega _2=P/Q`$ and $`P,Q`$ are coprime integers, the non-linear system can act as a frequency converter by absorbing $`Q`$ photons of frequency $`\omega _1`$ and emitting $`P`$ photons of frequency $`\omega _2`$. The relation $`Q\omega _1=P\omega _2`$ expresses the conservation of energy. In the irrational case, the system cannot act as a frequency converter simply because there is no analogous relation for the conservation of energy.

Combining Eqs.(3),(24) it is found that in the case of irrational $`\omega _1/\omega _2`$, the autocorrelation is

$$\mathrm{\Gamma }_{ir}(\tau )=1+2J_0(e\varphi _1)J_0(e\varphi _2)+\underset{n,k=\mathrm{}}{\overset{\mathrm{}}{}}\mu (\tau )\left[J_n(e\varphi _1)\right]^2\left[J_{2kn}(e\varphi _2)\right]^2$$
(25)
where $`\mu (\tau )=\mathrm{exp}\{i[n\omega _1+(2kn)\omega _2]\tau \}`$. In the case that the ratio $`\omega _1/\omega _2=P/Q`$ (rational), the autocorrelation is

$`\mathrm{\Gamma }_{ra}(\tau )`$ $`=`$ $`1+{\displaystyle \underset{n=\mathrm{}}{\overset{\mathrm{}}{}}}J_{Qn}(e\varphi _1)J_{Pn}(e\varphi _2)+{\displaystyle \underset{n=\mathrm{}}{\overset{\mathrm{}}{}}}J_{Qn}(e\varphi _1)J_{Pn}(e\varphi _2)`$ (26)
$`+{\displaystyle \frac{1}{4}}{\displaystyle \underset{n,m,N=\mathrm{}}{\overset{\mathrm{}}{}}}\nu (\tau )J_n(e\varphi _1)J_m(e\varphi _2)J_{NQn}(e\varphi _1)J_{NPm}(e\varphi _2)`$
$`+{\displaystyle \frac{1}{4}}{\displaystyle \underset{n,m,N=\mathrm{}}{\overset{\mathrm{}}{}}}\nu (\tau )J_n(e\varphi _1)J_m(e\varphi _2)J_{NQn}(e\varphi _1)J_{NPm}(e\varphi _2)`$
$`+{\displaystyle \frac{1}{4}}{\displaystyle \underset{n,m,N=\mathrm{}}{\overset{\mathrm{}}{}}}\nu (\tau )J_n(e\varphi _1)J_m(e\varphi _2)J_{NQn}(e\varphi _1)J_{NPm}(e\varphi _2)`$
$`+{\displaystyle \frac{1}{4}}{\displaystyle \underset{n,m,N=\mathrm{}}{\overset{\mathrm{}}{}}}\nu (\tau )J_n(e\varphi _1)J_m(e\varphi _2)J_{NQn}(e\varphi _1)J_{NPm}(e\varphi _2)`$
where $`\nu (\tau )=\mathrm{exp}[i(NQn)\omega _1\tau +i(NPm)\omega _2\tau ]`$. It is interesting to explain the results of Eqs.(25),(26) taking into account the interpretation of the expansion of the exponentials in terms of emission/absorption of photons (discussed after Eq. (13)) in conjunction with the above comments about frequency conversion. For example, in the last term of Eq.(26) for the rational case, the system emits $`n`$ photons of frequency $`\omega _1`$ at time $`t`$ (related to an exponential $`\mathrm{exp}(in\omega _1t)`$); emits $`NQn`$ photons of frequency $`\omega _1`$ at time $`(t+\tau )`$ (related to an exponential $`\mathrm{exp}[i(NQn)\omega _1(t+\tau )]`$); absorbs $`m`$ photons of frequency $`\omega _2`$ at time $`t`$ (related to an exponential $`\mathrm{exp}(im\omega _2t)`$); and absorbs $`NPm`$ photons of frequency $`\omega _2`$ at time $`(t+\tau )`$ (related to an exponential $`\mathrm{exp}[i(NPm)\omega _2(t+\tau )]`$). Taking into account the relation $`\omega _1/\omega _2=P/Q`$ we see that the product of these exponentials is the factor $`\nu (\tau )`$. Similarly, in the last term of Eq.(25) for the irrational case the system emits $`n`$ photons of frequency $`\omega _1`$ at time $`t`$; absorbs $`n`$ photons of frequency $`\omega _1`$ at time $`(t+\tau )`$; absorbs $`(2kn)`$ photons of frequency $`\omega _2`$ at time $`t`$; and emits $`(2kn)`$ photons of frequency $`\omega _2`$ at time $`(t+\tau )`$. In this case there is no transfer of energy (frequency conversion) between the two frequencies. As previously, the factor $`\mu (\tau )`$ is related to the exponentials associated with the absorption/emission of photons. Clearly, the electron autocorrelation is a periodic function of $`\tau `$ only in the rational case.

### III.2 Entangled two-mode microwaves

We next consider non-classical two-mode microwaves. We are particularly interested to study how entangled two-mode microwaves affect the electron interference. For this reason we consider the entangled state $`|s=2^{1/2}(|01+|10)`$ where $`|01`$ , $`|10`$ are two mode number eigenstates. For comparison we also consider the separable (disentangled) state

$$\rho _{sep}=\frac{1}{2}(|0101|+|1010|).$$
(27)
Clearly, the density matrix of the entangled state $`\rho _{ent}=|ss|`$ can be written as

$$\rho _{ent}=\rho _{sep}+\frac{1}{2}(|0110|+|1001|).$$
(28)
In this case using Eq.(13) with

$`\widehat{I}(t)=1+{\displaystyle \frac{1}{2}}D_1(\lambda _1)D_2(\lambda _2)+{\displaystyle \frac{1}{2}}D_1(\lambda _1)D_2(\lambda _2);\lambda _j=iq\mathrm{exp}(i\omega _jt)`$ (29)
for two modes ($`j=1,2`$) we find that

$`I(t)_{sep}`$ $`=`$ $`1+\left(1q^2\right)\mathrm{exp}\left(q^2\right),`$ (30)
$`I(t)_{ent}`$ $`=`$ $`I(t)_{sep}q^2\mathrm{exp}\left(q^2\right)\mathrm{cos}[(\omega _1\omega _2)t].`$ (31)
These results are presented in Fig. 6. It is seen that for the example we considered, the $`I(t)_{sep}`$ is constant in time, while the $`I(t)_{ent}`$ is an oscillatory function of time. The $`R(t,\tau )`$ has also been calculated using Eq.(14). In the separable case, the result does not depend on $`t`$ and therefore

$`\mathrm{\Gamma }_{sep}(\tau )=R_{sep}(t,\tau )`$ $`=`$ $`1+\left(22q^2\right)\mathrm{exp}\left(q^2\right)`$ (32)
$`+{\displaystyle \frac{1}{2}}\left[12q^2(s_1^2+s_2^2)\right]\mathrm{exp}\left[iq^2(d_1+d_2)\right]\mathrm{exp}\left[2q^2(s_1^2+s_2^2)\right]`$
$`+{\displaystyle \frac{1}{2}}\left[12q^2(c_1^2+c_2^2)\right]\mathrm{exp}\left[iq^2(d_1+d_2)\right]\mathrm{exp}\left[2q^2(c_1^2+c_2^2)\right].`$
where $`d_j=\mathrm{sin}(\omega _j\tau )`$, $`s_j=\mathrm{sin}(\omega _j\tau /2)`$, $`c_j=\mathrm{cos}(\omega _j\tau /2)`$ and $`j=1,2`$. This is a periodic function of $`\tau `$ only if the ratio of $`\omega _1/\omega _2`$ is rational. Indeed, it can easily be verified that if $`\omega _1/\omega _2=P/Q`$ where $`P`$ and $`Q`$ are coprime integers, then the period is $`(2\pi P)/\omega _1=(2\pi Q)/\omega _2`$. The $`\mathrm{\Gamma }_{sep}(\tau )`$ is a quasi-periodic function of $`\tau `$, if the ratio of $`\omega _1/\omega _2`$ is irrational. In Fig. 7 we present the absolute value of $`\mathrm{\Gamma }_{sep}(\tau )`$ as a function of $`\omega _2\tau `$ for the case $`\omega _1=1.2\times 10^4,\omega _2=10^4`$.

In the entangled (non-separable) microwave case

$`R_{ent}(t,\tau )`$ $`=`$ $`R_{sep}(t,\tau )q^2\mathrm{exp}\left(q^2\right)\mathrm{cos}[(\omega _1\omega _2)t]q^2\mathrm{exp}\left(q^2\right)\mathrm{cos}[(\omega _1\omega _2)(t+\tau )]`$ (33)
$`2q^2s_1s_2\mathrm{exp}\left[iq^2(d_1+d_2)\right]\mathrm{exp}\left[2q^2(s_1^2+s_2^2)\right]\mathrm{cos}\left[(\omega _1\omega _2)\left(t+{\displaystyle \frac{\tau }{2}}\right)\right]`$
$`2q^2c_1c_2\mathrm{exp}\left[iq^2(d_1+d_2)\right]\mathrm{exp}\left[2q^2(c_1^2+c_2^2)\right]\mathrm{cos}\left[(\omega _1\omega _2)\left(t+{\displaystyle \frac{\tau }{2}}\right)\right]`$
With regard to the periodicity of $`R_{ent}(t,\tau )`$ as a function of $`\tau `$, similar comments can be made as for the $`\mathrm{\Gamma }_{sep}(\tau )`$. We note that $`R_{sep}(t,\tau )`$ is independent of $`t`$ while $`R_{ent}(t,\tau )`$ is equal to $`R_{sep}(t,\tau )`$ plus an extra term which is a periodic function of $`t`$ with period $`(2\pi )/(\omega _1\omega _2)`$. Therefore, integration with respect to $`t`$ leads to the result that $`\mathrm{\Gamma }_{ent}(\tau )=\mathrm{\Gamma }_{sep}(\tau )`$.

## IV Discussion

There has been a lot of work in the last few years on the interaction of mesoscopic devices with microwaves (e.g. ). In this paper we have considered non-classical microwaves which are carefully prepared in a particular quantum state and where the quantum noise is carefully controlled. We have studied how quantum phenomena in the microwaves, affect quantum phenomena in the interfering electrons.

We have quantified the effect of the quantum noise on electron interference. More specifically we have calculated both the average intensity and the spectral density of the interference electrons for several types of non-classical microwaves (Figs 2-5). A comparison of the results with the case of classical microwaves demonstrates clearly the influence of the quantum noise on the interference. The non-zero value of $`\mathrm{}[\gamma (\tau )]`$ in Fig 4 is a purely quantum mechanical result due to the non-commutativity of the quantum mechanical operators $`\widehat{I}(t)`$ and $`\widehat{I}(t+\tau )`$. This quantity is zero in the classical case.

We have also considered two-mode microwaves where we have shown that we get different results for rational and irrational values of the ratio $`\omega _1/\omega _2`$. We have interpreted these results in terms of emission and absorption of photons by the non-linear device of the interfering electrons. We have also considered both separable and entangled microwaves and quantified their effect on the interference (Figs 6-7). The different results in these two cases demonstrate how the deep quantum phenomenon of microwave entanglement affects electron interference.

## V Appendix

The terms entering the squeezed states result in Eq.(20) are

$`Y_1`$ $`=`$ $`{\displaystyle \frac{q^2}{2}}[\mathrm{cosh}(r)\mathrm{sinh}(r)\mathrm{cos}(2\omega t+\vartheta )]`$
$`X_1`$ $`=`$ $`2q|B|\left[\mathrm{cosh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{cos}(\omega t\theta _B)\mathrm{sinh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{cos}(\omega t+\theta _A+\vartheta )\right]`$
$`Y_2`$ $`=`$ $`{\displaystyle \frac{q^2}{2}}[\mathrm{cosh}(r)\mathrm{sinh}(r)\mathrm{cos}(2\omega t+2\omega \tau +\vartheta )]`$
$`X_2`$ $`=`$ $`2q|B|\left[\mathrm{cosh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{cos}(\omega t+\omega \tau \theta _B)\mathrm{sinh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{cos}(\omega t+\omega \tau +\theta _B+\vartheta )\right]`$
$`Y_3`$ $`=`$ $`2q^2\mathrm{cos}^2\left({\displaystyle \frac{\omega \tau }{2}}\right)[\mathrm{cosh}(r)\mathrm{sinh}(r)\mathrm{cos}(2\omega t+\omega \tau +\vartheta )]`$
$`X_3`$ $`=`$ $`4q|B|\mathrm{cos}\left({\displaystyle \frac{\omega \tau }{2}}\right)\left[\mathrm{cosh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{cos}\left(\omega t+{\displaystyle \frac{\omega \tau }{2}}\theta _B\right)\mathrm{sinh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{cos}\left(\omega t+{\displaystyle \frac{\omega \tau }{2}}+\theta _B+\vartheta \right)\right]`$
$`Y_4`$ $`=`$ $`2q^2\mathrm{sin}^2\left({\displaystyle \frac{\omega \tau }{2}}\right)[\mathrm{cosh}(r)+\mathrm{sinh}(r)\mathrm{cos}(2\omega t+\omega \tau +\vartheta )]`$
$`X_4`$ $`=`$ $`4q|B|\mathrm{sin}\left({\displaystyle \frac{\omega \tau }{2}}\right)\left[\mathrm{cosh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{sin}\left(\omega t+{\displaystyle \frac{\omega \tau }{2}}\theta _B\right)\mathrm{sinh}\left({\displaystyle \frac{r}{2}}\right)\mathrm{sin}\left(\omega t+{\displaystyle \frac{\omega \tau }{2}}+\theta _B+\vartheta \right)\right].`$
## VI References

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M. Peshkin and A. Tonomura, *The Aharonov-Bohm effect*, Lecture notes in Physics, Vol. 340 (Springer, Berlin, 1989).
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M. Pepper, Proc. Royal Soc. London A 420, 1 (1988).
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J. Summhammer, Phys. Rev. A 47, 556 (1993).
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E. Buks *et. al.*, Nature 391, 871 (1998).
G. Hackenbroich, Phys. Rep. 343, 464 (2001).
5. M.P. Silverman, Phys. Lett. A 118, 155 (1986); Nuovo Cimento B 97, 200 (1987).
M. Buttiker, Phys. Rev. B 46, 12485 (1992).
6. M. Buttiker, J. Low Temp. Phys. 118, 519 (2000).
R. Deblock *et. al.*, Phys. Rev. B 65, 075301 (2002).
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# Late stage kinetics for various wicking and spreading problems

## I Introduction

Wetting in complex geometries and on rough surfaces provides a wealth of fascinating non-linear hydrodynamics problems, as well as being of commercial importance in numerous industrial sectors. Perhaps the first kind of problem to be considered was the penetration of liquid into porous materials, where Washburn in 1921 demonstrated that the distance attained by the wetting front follows a $`t^{1/2}`$ law where $`t`$ is time Washburn (1921). Much later the spreading of droplets on flat surfaces was addressed by various workers, such as Tanner Tanner (1979) and Lopez et al Lopez et al. (1976), although it took some time for the subtleties of the physics at the wetting front to be resolved de Gennes (1985); Léger and Joanny (1992); Brenner and Bertozzi (1993); Oron et al. (1997). Generally, the wetting front advances with a $`t^\alpha `$ law where $`\alpha `$ is a small exponent which depends on the geometry of spreading and the origin of the driving force. For example, $`\alpha =1/10`$ for a drop spreading radially driven by surface tension (Tanner’s law), and $`\alpha =1/8`$ for a droplet spreading radially driven by gravity (see Oron et al Oron et al. (1997) for a summary of results).

The kinetics of wetting on rough surfaces has also been investigated experimentally and theoretically Cazabat and Stuart (1986); Gerdes et al. (1998); Rye et al. (1998). A paradigm for this problem is the spreading of a liquid in a wedge or V-shaped groove J. A. Mann et al. (1995); Romero and Yost (1996); Gerdes et al. (1997); indeed wetting in a network of V-shaped grooves has been invoked recently for oil spreading on skin Dussaud et al. (2003). Another kind of problem that has been considered is the wetting of hydrophilic strips Darhuber et al. (2001), as an example of wetting in a controlled microstructure that might be contemplated in a microfluidic device. In all these problems, a $`t^{1/2}`$ spreading law has been observed, but in the cases considered thus far, there has been a reservoir which provides liquid at essentially a constant pressure. In the present paper, the problems of spreading in a wedge, in a network of V-shaped grooves, and on a hydrophilic strip are revisited. It is found that in the absence of a reservoir, the spreading law changes to $`t^\alpha `$ with $`\alpha <1/2`$, similar to Tanner’s law and related problems.

These problems are first approached by scaling arguments developed in the next section. The bona fides of the scaling arguments is established by rederiving some known results for spreading on flat surfaces. In a further section, the scaling exponents are recovered by similarity analysis on the underlying partial differential equations which govern spreading. This also allows the scaling shape of the spreading drops to be computed.

## II Scaling arguments

The Washburn problem of a liquid being drawn into a capillary tube of internal dimension $`d`$ shown in Fig. 1(a) is considered first Washburn (1921). This is a model for penetration of liquid into a porous material for which $`d`$ interpreted as a mean pore size. The arguments here are very familiar, but form the basis for the more complex problems considered below.

Once the liquid has penetrated a sufficient distance $`Ld`$, a Poiseuille law obtains for the liquid velocity and the penetration rate, thus

$$\frac{dL}{dt}\frac{d^2}{\eta }\frac{\mathrm{\Delta }p}{L}$$
(1)
where $`\eta `$ is viscosity, and the pressure drop

$$\mathrm{\Delta }p\sigma /d$$
(2)
is due to the surface tension $`\sigma `$ of the curved surface at the wetting front, at a mean curvature $`1/d`$. All geometric factors associated with the shape of the tube and a finite contact angle have been dropped, although a contact angle $`\theta <\pi /2`$ is required for imbibition to take place. Combining Eqs. (1) and (2) gives

$$\frac{dL}{dt}\frac{\sigma }{\eta }\frac{d}{L}$$
(3)
which integrates to

$$L(\sigma td/\eta )^{1/2}.$$
(4)
This is the simplest form of the Washburn equation Washburn (1921). The result arises from a constant pressure drop acting over an increasing length of liquid, which responds by flowing according to the Poiseuille law. As we shall see below, this can be the case for many situations where a reservoir of liquid is present, but if a reservoir is absent, the rate of spreading can be much slower.

Next, the problem of a drop of liquid spreading on a flat surface is considered, as shown in Fig. 1(b). Usually the problem is approached by an appeal to the hydrodynamics in the vicinity of the moving contact line de Gennes (1985); Léger and Joanny (1992), but it can be analysed using similar concepts to the Washburn problem. Whilst only previously known results are recovered, the approach serves to illustrate further the arguments that will be used for the other problems.

Consider a drop of liquid spreading on a flat surface, in the case of complete wetting. Let a measure of the radius of the spreading drop be $`R`$ and the height in the centre be $`h`$. In the lubrication approximation, assuming a scaling shape of the droplet, all velocities will be proportional to $`(h^2/\eta )(\mathrm{\Delta }p/R)`$ (compare Poiseuille law above) where $`\mathrm{\Delta }p`$ is the pressure drop between the centre and the radius $`R`$. In particular the drop radius is expanding at a rate

$$\frac{dR}{dt}\frac{h^2}{\eta }\frac{\mathrm{\Delta }p}{R}.$$
(5)
First consider the capillary spreading case where the pressure gradient is due to surface tension $`\sigma `$. Simple geometry shows that the mean curvature at the centre of the droplet for $`hR`$ is $`h/R^2`$ therefore the pressure drop is

$$\mathrm{\Delta }p\sigma h/R^2$$
(6)
and hence

$$\frac{dR}{dt}\frac{\sigma }{\eta }\frac{h^3}{R^3}.$$
(7)
If $`h`$ were to be constant, as in the Washburn problem, this would be enough to determine the spreading rate. Here, though, a second relation connecting $`R`$ and $`h`$ must be sought. The desired relation follows from the conservation of drop volume $`\mathrm{\Omega }`$,

$$hR^2\mathrm{\Omega }.$$
(8)
Thus

$$\frac{dR}{dt}\frac{\sigma }{\eta }\frac{\mathrm{\Omega }^3}{R^9}$$
(9)
which integrates to

$$R(\sigma t\mathrm{\Omega }^3/\eta )^{1/10}.$$
(10)
This result is Tanner’s law Tanner (1979). The basic scaling $`R\mathrm{\Omega }^{3/10}t^{1/10}`$ is well documented and has been experimentally verified de Gennes (1985).

For the case where the spreading is driven by gravity, one has $`\mathrm{\Delta }p\rho gh`$ where $`\rho `$ is the mass density and $`g`$ is the acceleration due to gravity. Following the same line of argument as above, one obtains $`R(\rho gt\mathrm{\Omega }^3/\eta )^{1/8}`$ Lopez et al. (1976). The behaviour crosses over from capillary spreading to gravity spreading when the Bond number $`\rho gR^2/\sigma `$ increases. Since $`R`$ is increasing, this means that capillary spreading always crosses over to gravity spreading if one waits long enough. The weak increase in spreading rate has been observed experimentally Cazabat and Stuart (1986).

Another case that can be considered is planar or one-dimensional spreading. The only thing which changes is the volume conservation law which becomes $`hL\mathrm{\Omega }`$ where $`L`$ replaces $`R`$ as the measure of extent of spreading, and $`\mathrm{\Omega }`$ is a volume per unit length. This yields $`L(\sigma t\mathrm{\Omega }^3/\eta )^{1/7}`$ and $`L(\rho gt\mathrm{\Omega }^3/\eta )^{1/5}`$ for capillary Tanner (1979) and gravity Lopez et al. (1976) spreading respectively.

In the next problem, exactly analogous arguments are applied to the case of spreading in a wedge, shown in Fig. 1(c). In the case of spreading from a reservoir, this problem has been addressed by Romero and Yost Romero and Yost (1996). The basic idea is that one has scale invariance, with the depth $`h`$ of fluid being the only relevant length scale. Hence the transverse curvature of the interface $`1/h`$. Thus, provided the droplet has become sufficiently extended so that the contribution of the longuitudinal curvature to the mean curvature can be neglected, the pressure $`p()\sigma /h`$ where the negative sign obtains if the surface is convex into the liquid. This is the case if $`2\theta +\varphi <\pi `$ where $`\theta `$ is the contact angle and $`\varphi `$ is the wedge angle as in Fig. 1(c). In this case, the pressure becomes more negative as the amount of fluid is in the wedge gets smaller. This provides a pressure gradient which drives the liquid from regions of high loading to low loading.

Even though the liquid has a free surface, a Poiseuille-like law obtains,

$$\frac{dL}{dt}\frac{h^2}{\eta }\frac{\mathrm{\Delta }p}{L}$$
(11)
where $`L`$ is a measure of the extent of spread of the liquid drop. The pressure drop follows from the above arguments, $`\mathrm{\Delta }p\sigma /h`$, and therefore

$$\frac{dL}{dt}\frac{\sigma }{\eta }\frac{h}{L}$$
(12)
in perfect analogy to Eq. (3) in the Washburn problem. The difference here is that $`h`$ is a dynamic variable which, similar to the Tanner’s law derivation above, is found by a volume conservation law. In this case $`AL\mathrm{\Omega }`$ where $`Ah^2`$ is the cross section area occupied by the liquid, and $`\mathrm{\Omega }`$ is the volume of liquid. Thus $`h(\mathrm{\Omega }/L)^{1/2}`$. Substituting into Eq. (12) results in

$$\frac{dL}{dt}\frac{\sigma }{\eta }\frac{\mathrm{\Omega }^{1/2}}{L^{3/2}}$$
(13)
which integrates to

$$L(\sigma t\mathrm{\Omega }^{1/2}/\eta )^{2/5}.$$
(14)
This spreading law, $`L\mathrm{\Omega }^{1/5}t^{2/5}`$, is a new prediction. It can also be recovered by a more detailed analysis of the underlying partial diffential equations which will be given in a later section.

Note that if the liquid had been spreading along the wedge from a reservoir, this would correspond to $`h\mathrm{constant}`$. This leads to the Washburn result $`Lt^{1/2}`$ and is the origin of the scaling law obtained by previous workers J. A. Mann et al. (1995); Romero and Yost (1996).

The next case to be considered is the problem of a droplet spreading into a network of grooves. This has also been considered by various groups Cazabat and Stuart (1986); Gerdes et al. (1998); Dussaud et al. (2003). If spreading occurs from a reservoir, then the front advances with a $`t^{1/2}`$ Washburn-like law. However the case where the liquid is completely confined in the grooves is different. The scaling law in this case follows from arguments similar to those already applied to a drop spreading in a wedge. The analysis assumes that the grooves are rather sparse on the surface, in particular that the volume of liquid in the junction zones can be neglected compared to the volume contained in the grooves.

Consider therefore a drop of liquid spreading in a sparse random network of grooves. It will spread essentially radially. Suppose that the groove cross section is a V-shape, so that both the capillary pressure and the Poiseuille scaling laws can be taken over from the case of spreading in a wedge. The fact that the grooves are randomly inclined with respect to the radial pressure gradient only introduces an additional numerical prefactor Dussaud et al. (2003). Thus Eq. (12) above still holds (with $`L`$ replaced by $`R`$). What changes is the volume conservation law: as $`R`$ increases, more grooves become filled. If the length of grooves per unit area is $`l^1`$, where $`l`$ is a characteristic groove spacing on the surface, the total length of grooves occupied by the liquid $`R^2/l`$ and the volume $`\mathrm{\Omega }h^2R^2/l`$. Eliminating $`h`$ between this and Eq. (12) (with $`L`$ replaced by $`R`$) gives $`dR/dt(\sigma /\eta )(l\mathrm{\Omega })^{1/2}/R^2`$. This integrates to

$$R(\sigma t(l\mathrm{\Omega })^{1/2}/\eta )^{1/3}.$$
(15)
The basic prediction therefore is that the spreading rate should slow from the $`t^{1/2}`$ Washburn-like law for spreading from a reservoir, to an $`R\mathrm{\Omega }^{1/6}t^{1/3}`$ law as the liquid becomes confined to the grooves. The result is confirmed by a more detailed analysis of the underlying partial differential equations given later.

The final problem that is considered is spreading along a hydrophilic strip, shown in Fig. 1(d). The case where spreading occurs from a reservoir has been investigated both theoretically and experimentally, and it is found that the spreading front advances with a Washburn-like $`t^{1/2}`$ law Darhuber et al. (2001). The situation in the absence of a reservoir was not investigated though. Once again, the absence of a reservoir leads to a slower rate of spreading, and the scaling law can be determined using analogous arguments to those applied above.

Consider a drop of liquid which is completely wetting on a hydrophilic strip of width $`w`$. In the late stages, let the height of the liquid above the surface be $`hw`$, and a measure of the extent of spreading be $`Lw`$. The capillary pressure which drives the spreading is due to the transverse curvature of the interface, which for $`hw`$ is $`h/w^2`$. The pressure gradient is thus $`\mathrm{\Delta }p/L\sigma h/w^2L`$. In the lubrication approximation with $`hw`$, a Poiseuille-like law obtains for the fluid velocity with $`h`$ being the relevant length scale. Hence the rate of extension of the droplet obeys $`dL/dt(h^2/\eta )(\mathrm{\Delta }p/L)(\sigma /\eta )h^3/w^2L`$. Volume conservation indicates $`hwL\mathrm{\Omega }`$ and eliminating $`h`$ between this and the above spreading rate finds $`dL/dt(\sigma /\eta )\mathrm{\Omega }^3/w^5L^4`$. This integrates to $`L(\sigma t\mathrm{\Omega }^3/\eta w^5)^{1/5}`$. This is the predicted scaling law for the late stages of spreading in this problem, in the absence of a reservoir.

## III Similarity methods

The results obtained above can also be derived by using similarity methods to analyse the underlying partial differential equations (see for example Ref. Brenner and Bertozzi (1993)). Focus first on the problem of spreading in a wedge shown in Fig. 1(c). An equation which expresses local conservation of liquid in the wedge is

$$\frac{A}{t}+\frac{(A\overline{v})}{x}=0$$
(16)
where $`Ah^2`$ is the local cross section area occupied by liquid, $`\overline{v}`$ the mean velocity of the liquid, and $`x`$ is distance along the wedge. The Poiseuille law indicates that the mean velocity follows

$$\overline{v}\frac{h^2}{\eta }\frac{p}{x}.$$
(17)
The arguments above show that $`p\sigma /h`$ thus

$$\frac{p}{x}\frac{\sigma }{h^2}\frac{h}{x}.$$
(18)
Combining Eqs. (16)–(18) gives the following equation for the time evolution of the depth of liquid in the groove (compare Eqs. (8a)–(8c) of Romero and Yost Romero and Yost (1996))

$$\frac{(h^2)}{t}=K\frac{\sigma }{\eta }\frac{}{x}\left(h^2\frac{h}{x}\right).$$
(19)
The dimensionless coefficient $`K(\theta ,\varphi )`$ is given by Eq. (8c) in Romero and Yost Romero and Yost (1996) in terms of the static contact angle $`\theta `$ and the wedge angle $`\varphi `$. For spreading to occur, $`K>0`$ is required. This corresponds to $`2\theta +\varphi <\pi `$, or a liquid interface which is convex into the liquid. For the remainder of the discussion, the factor $`K\sigma /\eta `$ and other trivial numerical prefactors can be adsorbed into the units of time, and will be omitted.

Eq. (19) is basically a non-linear diffusion equation and one can seek similarity solutions of the form

$$h(x,t)t^\beta g(xt^\alpha )$$
(20)
where $`u=xt^\alpha `$ is the similarity variable and $`\alpha `$ is the exponent in the spreading law. Substituting this in Eq. (19) obtains both an exponent relation

$$2\alpha +\beta =1$$
(21)
which must be satisfied for the similarity solution to hold, and an ordinary differential equation (ODE) for the similarity function

$$gg^{\prime \prime }+2(g^{})^2+\alpha ug^{}+\beta g=0.$$
(22)
This is a non-linear second order ODE with boundary conditions $`g(0)=A`$ (which is set by the drop volume) and $`g^{}(0)=0`$ (required by symmetry).

A second exponent relation follows from the integrated conservation law. Volume conservation dictates that $`\mathrm{\Omega }_{\mathrm{}}^{\mathrm{}}h^2𝑑x`$ is constant. Inserting the similarity solution in this shows that $`\mathrm{\Omega }t^{\alpha 2\beta }\times _{\mathrm{}}^{\mathrm{}}g^2𝑑u`$ is constant, and therefore

$$\alpha =2\beta .$$
(23)
Solving Eqs. (21) and (23) gives

$$\alpha =2/5,\beta =1/5.$$
(24)
Thus the spreading law $`Lt^{2/5}`$ of the preceeding section is recovered. The dependence on $`\mathrm{\Omega }`$ and $`\sigma /\eta `$ can be determined by dimensional analysis.

To complete the discussion, the ODE for the similarity function $`g(u)`$ can be solved. Inserting Eq. (24) into Eq. (22) results in $`gg^{\prime \prime }+2(g^{})^2+2ug^{}/5+g/5=0`$, with $`g(0)=A`$ and $`g^{}(0)=0`$. Remarkably, this equation has an extremely simple closed form solution,

$$g=Au^2/10.$$
(25)
Note that $`g0`$ for $`uu_0=\sqrt{10A}`$, so the spreading drop in the groove has a finite extent. Some examples of the shape for different values of $`A`$ are shown in Fig. 2(a). The basic prediction is that the height profile of the liquid surface for a droplet spreading in wedge is a parabola in the distance along the wedge. To be specific, from Eqs. (20), (24) and (25),

$$h(x,t)=h_0[1(x/x_0)^2],(|x|<x_0)$$
(26)
where the height $`h_0t^{1/5}`$ and the maximum extent of spreading $`x_0t^{2/5}`$.

For the case of spreading in a network of grooves, Eqs. (19)–(22) remain the same (apart from numerical prefactors Dussaud et al. (2003)), but the integrated conservation law changes to $`\mathrm{\Omega }_0^{\mathrm{}}h^2\mathrm{\hspace{0.17em}2}\pi r𝑑r/l`$ (where $`r`$ should replace $`x`$ in Eq. (19)). Substituting the similarity solution shows that $`\alpha =\beta `$ must hold in this case. Combining this with Eq. (21) gives $`\alpha =\beta =1/3`$, thus the previous scaling exponent is recovered. Unfortunately the corresponding ODE does not have a closed form solution. Some examples of shapes obtained by numerical integration are shown in Fig. 2(b). Again $`g0`$ for $`uu_0`$ but in this case $`g`$ has a singularity: $`g(u_0u)^{1/3}`$ as $`uu_0`$ from below.

Finally, the problem of a liquid spreading along a hydrophilic strip shown in Fig. 1(d) is discussed. The governing partial differential equation has been obtained by Darhuber et al for this problem Darhuber et al. (2001). It is $`h/t[h^3(h/x)]/x`$ where the prefactor can be found from Eq. (7) in Ref. Darhuber et al. (2001). Substituting the similarity trial solution Eq. (20) in this yields an ODE $`g^3g^{\prime \prime }+3g^2(g^{})^2+\alpha ug^{}+\beta g=0`$ with $`g(0)=A`$ and $`g^{}(0)=0`$ being initial conditions, and an exponent relation $`2\alpha +3\beta =1`$. It follows from $`\mathrm{\Omega }_{\mathrm{}}^{\mathrm{}}wh𝑑x`$ that $`\alpha =\beta `$. Solving this together with the preceeding exponent relation gives $`\alpha =\beta =1/5`$, thus recovering the exponent of the preceeding section. Numerical integration of the ODE gives results which resemble those for the case of spreading in a network of grooves, shown in Fig. 2(b). Again $`g0`$ as $`uu_0`$ with $`g(u_0u)^{1/3}`$ as $`uu_0`$ from below (compare Fig. 3 of Ref. Darhuber et al., 2001).

In all these cases, the fact that $`g0`$ for $`uu_0`$ stands in contrast to the similarity solution for Tanner’s law for which there is no point where $`g0`$ Brenner and Bertozzi (1993). In that case one has to invoke an additional microscopic mechanism to account for the shape of the edge of the drop.

The case of spreading from a reservoir can also be treated with variant of the above analysis; in fact the essential arguments are already given by Romero and Yost Romero and Yost (1996), and Darhuber et al Darhuber et al. (2001). In the case of a reservoir, $`h`$ is constant at the reservoir edge which we define to be the point $`x=0`$. In terms of the similarity solution Eq. (20), this forces $`\beta =0`$. Combining this with the exponent relation in Eq. (21) or the analogous exponent relation for the strip problem shows $`\alpha =1/2`$ for all cases. Thus the Washburn-like spreading law is recovered for spreading from a reservoir, independent of whether spreading takes place in a wedge, in a network of grooves, or along a strip.

## IV Discussion

The main results concern the kinetics of spreading in various geometries. New predictions are made for the scaling laws governing the rate at which a droplet spreads in a wedge or V-shaped groove, in a network of such grooves, and on a hydrophilic strip. These are established both by simple scaling arguments and by similarity solutions of the underlying partial differential equations. The asymptotic shapes of the spreading droplets have also been considered.

Previous work on these problems has assumed the presence of a reservoir which supplies liquid at constant pressure. This results in spreading laws which are essentially the same as the Washburn law for penetration of a liquid into a porous material, or into a capillary. The analysis here complements this previous work by considering the problems in the absence of a reservoir. This will apply in the late stages of wetting when the reservoir becomes exhausted, or if there is only a small amount of liquid present.

These predictions could be tested by simulation or in experiments. The case of a droplet in a wedge would seem to be particularly simple, for instance a drop will spread in a right-angled corner provided the contact angle is less than $`45^{}`$. The prediction that the scaling shape of the droplet should be a parabola should also be tested.

I thank Alex Lips for discussions and encouragement.


text:
# Optimized time-dependent perturbation theory for pulse-driven quantum dynamics in atomic or molecular systems

## Abstract

We present a time-dependent perturbative approach adapted to the treatment of intense pulsed interactions. We show there is a freedom in choosing secular terms and use it to optimize the accuracy of the approximation. We apply this formulation to a unitary superconvergent technique and improve the accuracy by several orders of magnitude with respect to the Magnus expansion.

Perturbation theory when combined with a specific treatment for resonances is quite well understood in classical and quantum mechanics for time-independent systems. This includes also time-periodic driven systems for which the periodicity can be treated by Floquet theory in a way that yields a time-independent formulation . One knows that resonances yield divergent terms, that appear as small denominators, which have to be specifically removed. The counterpart of the concept of resonance for time-dependent systems is generally associated to secular terms whose size grows with time (see Ref.  and references therein).

With the advent of short ($`10`$ fs) and intense ($`10^{13}`$$`10^{15}`$ W/cm2) laser pulses, atomic or molecular systems can be strongly perturbed in a timescale shorter than characteristic times corresponding to the free evolution of the system and adiabatic theories are not applicable (see, e.g., Ref. ). The goal of this paper is to formulate a time-dependent perturbation theory well adapted for perturbations localized in time.

The conceptual framework of perturbation theory can be described as follows: The Hamiltonian of the considered system can be decomposed as the sum of two terms $`H_1=H_0+ϵV_1`$. The first term $`H_0`$ is assumed to have a structure simple enough to lead to explicitly known solutions for its associated propagator $`U_{H_0}(t,t_0)`$. The term $`ϵV_1`$ is supposed to be small with respect to $`H_0`$, in a sense specified below. Time-independent perturbation theories can be equivalently formulated at the level of eigenvectors or operators . A large class of these approaches amounts to construct a unitary transformation $`T`$ such that

$$T^{}H_1T=H^\mathrm{e}+ϵ^{}V^{}\text{,}$$
(1)
where $`H^\mathrm{e}`$ is still of simple structure \[i.e., its propagator $`U_{H^\mathrm{e}}(t,t_0)`$ can be explicitly computed\] and $`ϵ^{}V^{}`$ is a perturbation whose size is smaller than the original one. To compute the transformation $`T`$ explicitly, one represents it in general either (i) in terms of some power series

$$T=e^{iW},W=\underset{k}{}ϵ^kW_k,$$
(2)
or (ii) by an iterative construction as a composition of transformations

$$T=\underset{k}{}e^{iϵ_kW_k}.$$
(3)
These procedures generally differ. The former one is referred to as the time-independent Poincaré-Von Zeipel technique, which has been shown to be equivalent to the usual Rayleigh-Schrödinger perturbation theory . The latter procedure includes the Van Vleck technique (for which $`ϵ_k=ϵ^k`$) and the superconvergent Kolmogorov-Arnold-Moser (KAM) expansion (where $`ϵ_k=ϵ^{2^{k1}}`$ and $`W_k`$ is $`ϵ_k`$-dependent) . The perturbative procedure converges if the remaining perturbation $`ϵ^{}V^{}`$ can be made to go to zero, as the number of terms in the power series (2) or as the number of compositions in Eq. (3) goes to infinity.

In this description one has to state precisely what class of Hamiltonians $`H^\mathrm{e}`$ can be considered simple. For the first order or the first iteration, one considers $`H^\mathrm{e}=H_0+ϵD_1`$ with the condition that $`D_1`$ should be compatible with $`H_0`$ in the sense that if the propagator of $`H_0`$ is known, that of $`H_0+ϵD_1`$ can also be obtained explicitly. In the case of time-independent Hamiltonians the condition of compatibility is

$$[H_0,D_1]=0.$$
(4)
For the case of time-dependent Hamiltonians, we show that the condition of compatibility can be generalized to

$$[H_0(t),D_1(t)]=i\frac{D_1}{t}.$$
(5)
The construction of transformations of the type of Eq. (2) or (3) involves finding the generator $`iϵW_1(t)`$ of the transformation $`T_1(t)`$, that is the solution to

$$i[W_1(t),H_0(t)]+V_1(t)D_1(t)=\frac{W_1}{t}.$$
(6)
This equation, together with the constraint (5), are usually called cohomology equations in the time-independent case  and are here generalized to the time-dependent case. These cohomology equations have the same form for higher orders or successive iterations.

Here we formulate the time-dependent perturbation theory by transforming directly the evolution operator instead of considering the perturbed Hamiltonian as is usually done in time-independent theory. We obtain perturbative corrections to the full propagator in the form of a product of propagators which exhibit free parameters appearing through the general solutions of related differential equations. We recover in particular the Magnus expansion  as a special case of the time-dependent Poincaré-Von Zeipel theory. This extension also gives the precise correspondence between time-independent resonances and time-dependent secular terms. In the context of pulsed perturbations with a finite duration, the secular terms need not be eliminated. We show the remarkable result that they can be used to improve the convergence of the method at a given order. This optimization is achieved without any a priori knowledge of the solution by locating the minimum of a given eigenvalue as a function of the relevant free parameters that are identified. The efficiency of the method is illustrated on a two-level system driven by a short intense pulse.

Perturbation theory, resonances and secular terms. We consider the Hamiltonian $`H_1(t)=H_0(t)+ϵV_1(t)`$, where $`H_0(t)`$ is associated to a known propagator $`U_{H_0}(t,t_0)`$. The formulation is presented here for the KAM method, consisting in iterations of transformations which are exactly of the same form at each step. The first iteration involves a unitary operator $`T_1(t)`$ which transforms the propagator $`U_{H_1}(t,t_0)`$ according to

$$T_1^{}(t)U_{H_1}(t,t_0)T_1(t_0)=U_{H_2}(t,t_0),$$
(7)
into a propagator $`U_{H_2}(t,t_0)`$ associated with the sum $`H_2(t)`$ of an effective Hamiltonian $`H_1^\mathrm{e}(t)H_0(t)+ϵD_1(t)`$ which contains contributions up to order $`ϵ`$ and a remainder $`ϵ^2V_2(t)`$. This new propagator, generated by a sum of two Hamiltonians, can be written as the product

$$U_{H_2}(t,t_0)=U_{H_1^\text{e}}(t,t_0)R_2(t,t_0),$$
(8)
where $`R_2(t,t_0)`$ satisfies the Schrödinger equation whose Hamiltonian is $`ϵ^2U_{H_1^\text{e}}(t_0,t)V_2(t)U_{H_1^\text{e}}(t,t_0)`$. Similarly we can factorize $`U_{H_1^\text{e}}(t,t_0)=U_{H_0}(t,t_0)S_1(t,t_0)`$, where $`S_1(t,t_0)`$ is a unitary operator related to $`ϵD_1(t)`$:

$$i\frac{}{t}S_1(t,t_0)=ϵU_{H_0}(t_0,t)D_1(t)U_{H_0}(t,t_0)S_1(t,t_0).$$
(9)
The full propagator reads

$`U_{H_1}(t,t_0)=T_1(t)U_{H_0}(t,t_0)S_1(t,t_0)R_2(t,t_0)T_1^{}(t_0),`$ (10)
which yields the first order KAM approximation for $`R_2(t,t_0)`$ replaced by the identity. In this construction the only restriction on the self-adjoint operator $`ϵD_1(t)`$ is that it be of order $`ϵ`$. Hence we have the freedom to choose the Hamiltonian in Eq. (9) as $`t`$-independent, giving

$$D_1(t)=U_{H_0}(t,t_0)D_1(t_0)U_{H_0}(t_0,t),$$
(11)
with $`D_1(t_0)`$ arbitrary, which is the general solution of Eq. (5). This allows one to obtain the solution of Eq. (9) as

$$S_1(t,t_0)=\mathrm{exp}\left[i(tt_0)ϵD_1(t_0)\right].$$
(12)
Differentiating Eq. (10) and substituting $`T_1(t)=\mathrm{exp}\left(iϵW_1(t)\right)`$ leads to Eq. (6). The rest involves a series of $`k`$ nested commutators that reads $`ϵ^2V_2(t)=_{k=1}^{\mathrm{}}\frac{1}{(k+1)!}i^kϵ^{k+1}[W_1(t),\mathrm{}[W_1(t),kV_1(t)+D_1(t)]\mathrm{}]`$. It has exactly the same structure at each iteration which is useful for applications, particularly when high-order computations are needed.

Iterating the time-dependent KAM algorithm reduces the size of the remaining perturbation in a superconvergent way from order $`ϵ^{2^{n1}}`$ to $`ϵ^{2^n}`$ at step $`n`$. The time-dependent Van Vleck technique would allow one to reduce the size of the remainder from order $`ϵ^n`$ to $`ϵ^{n+1}`$. These methods, in the formulation presented here, are unitary upon truncation. The superconvergent character of the KAM algorithm has been shown numerically by applying the method to a two-level system perturbed by a short time-dependent interaction .

The time-independent problem, i.e., the problem of finding a transformation $`T_1`$ that enables one to simplify the time-independent Hamiltonian $`H_1`$ according to $`T_1^{}HT_1=H_0+ϵD_1+ϵ^2V_2`$, is recovered when one conveniently chooses $`T_1`$ as time-independent. In this case all the operators, and in particular $`D_1`$ and $`W_1`$, are time-independent and the standard cohomology equations are recovered: $`[H_0,D_1]=0`$ and $`V_1D_1+i[W_1,H_0]=0`$. Their solutions can be determined using the following key property : $`W_1`$ exists if and only if $`\mathrm{\Pi }_{H_0}(D_1V_1)=0`$, where $`\mathrm{\Pi }_{H_0}`$ is the projector in the kernel of the application $`A[A,H_0]`$ (for an operator $`A`$ acting on the same Hilbert space as $`H_0`$). The projector $`\mathrm{\Pi }_{H_0}`$ applied on an operator $`A`$ captures thus all the part $`B`$ of $`A`$ which commutes with $`H_0`$: $`[B,H_0]=0`$. The unique solution $`D_1`$ allowing $`W_1`$ to exist and satisfying Eq. (4) is thus

$$D_1=\mathrm{\Pi }_{H_0}V_1\underset{T\mathrm{}}{lim}\frac{1}{T}_0^Te^{itH_0}V_1e^{itH_0}.$$
(13)
The resonances are associated with terms of $`V_1`$ which commute with $`H_0`$. Application of Eq. (13) can be interpreted as an averaging of $`V_1`$ with respect to $`H_0`$ which allows one to extract resonances.

For the time-dependent problem, the general solution of Eq. (6) reads (up to a term $`U_{H_0}(t,t_0)B_1U_{H_0}(t_0,t)`$ with $`B_1`$ any self-adjoint operator that we set here to 0)

$`W_1(t)={\displaystyle _{t_1^{}}^t}𝑑sU_{H_0}(t,s)\left(V_1(s)D_1(s)\right)U_{H_0}(s,t),`$ (14)
with $`t_1^{}`$ any real number. Defining the average

$$\mathrm{\Pi }_{}V_1\underset{\tau \mathrm{}}{lim}\frac{1}{\tau }_{t\tau }^t𝑑sU_{H_0}(t,s)V_1(s)U_{H_0}(s,t),$$
(15)
one can show the following property: if $`W_1(t)`$ is bounded for negative infinite times, then $`\mathrm{\Pi }_{}(V_1D_1)=0`$. This is satisfied by $`D_1=\mathrm{\Pi }_{}V_1`$, the only solution compatible with Eqs. (5) and (15). Hence, the averaging $`D_1=\mathrm{\Pi }_{}V_1`$ allows one to remove secular terms at negative infinite times. This gives the precise correspondence between the resonances of stationary problems and the secular terms of time-independent problems. We remark that the definition (15) of the average can be in fact recovered from the formal calculation of the average $`\mathrm{\Pi }_{K_0}V_1`$ \[cf. Eq. (13)\] with respect to $`K_0=i\frac{}{t}+H_0`$ in an extended space, which includes time as a coordinate .

For a pulsed perturbation that is switched on at $`t_i`$ and off at $`t_f`$, Eq. (15) becomes  $`\mathrm{\Pi }_{}V_1=U_{H_0}(t,t_i)V(t_i)U_{H_0}(t_i,t)`$. This is a particular solution of Eq. (5) corresponding to the choice $`D_1(t_0)`$ $``$ $`U_{H_0}(t_0,t_i)V(t_i)U_{H_0}(t_i,t_0)`$ in Eq. (11). An alternate definition of the average: $`\mathrm{\Pi }_+V_1lim_\tau \mathrm{}\frac{1}{\tau }_t^{t+\tau }𝑑sU_{H_0}(t,s)V_1(s)U_{H_0}(s,t)`$ gives a different averaging $`\mathrm{\Pi }_+V_1=U_{H_0}(t,t_f)V(t_f)U_{H_0}(t_f,t)`$ and allows one to remove secular terms at positive infinite times.

Generally one cannot remove simultaneously the secular terms at negative and positive large times. This shows a conceptual difference between stationary resonances and secular terms associated with perturbations localized in time. Furthermore, it appears that the averaging such as Eq. (15) is not appropriate, but that a definition which combines the two definitions gives a new secular term that could improve the convergence of the algorithm. This suggests to work with the general solution (11) of Eq. (5), written with the perturbation evaluated at a free time $`t_1`$ as the arbitrary operator:

$$D_1(t)=U_{H_0}(t,t_1)V_1(t_1)U_{H_0}(t_1,t).$$
(16)
The free $`t_1`$ can then be chosen to minimize the rest after the first iteration, as we describe below. One has $`n`$ such free parameters $`t_k,`$ $`k=1,n`$ for $`n`$ iterations of the KAM algorithm. There is only one such free parameter for the time-dependent Poincaré-Von Zeipel and Van Vleck methods that are order by order techniques. An interesting result is that we recover the Magnus expansion from the time-dependent Poincaré-Von Zeipel in the particular case of $`D_k=0`$ and $`t_k^{}=t_0`$ for $`k=1,n`$.

Optimization of the perturbation theory. After one iteration, the rest $`R_2(t,t_0)`$ defined in Eq. (8) is associated with a second order operator through $`R_2(t,t_0)e^{iϵ^2G_2(t)}`$ with $`G_2(t_0)=0.`$ The closer $`R_2(t,t_0)`$ is to the identity, the smaller the correction terms are, i.e., the more accurate the approximation is. We evaluate the lowest order contribution to $`ϵ^2G_2(t)`$ as

$$ϵ^2G_2^{(2)}(t)=ϵ^2_{t_0}^t𝑑uU_{H_1^\text{e}}(t_0,u)V_2(u)U_{H_1^\text{e}}(u,t_0).$$
(17)
It is this operator that has to remain small for the algorithm to converge. The size of an operator $`A`$ can be characterized by the norm $`A=sup_{\psi =1}A\psi `$ with $`\psi `$ in the appropriate Hilbert space. For an Hermitian matrix this norm reduces to the largest of the absolute values of its eigenvalues.

In order to improve the accuracy we thus seek to minimize $`\lambda _2(t)`$, the largest of the absolute values of the eigenvalues of $`ϵ^2G_2^{(2)}(t)`$, with respect to the free parameters. To optimize the KAM algorithm, we have at our disposal two free parameters $`t_k`$ and $`t_k^{}`$ at each iteration. We expect the parameters $`t_k`$ to significantly affect the convergence, as they are related to secular terms.

Perturbation theory for short intense pulses. We consider a system described by the Hamiltonian $`\widehat{H}`$ (autonomous or not) and perturbed by a time-dependent Hamiltonian $`\widehat{V}(s)`$ whose characteristic duration is $`\tau `$. The perturbation is assumed to satisfy $`[\widehat{V}(s),\widehat{V}(s_0)]=0`$, $`s,s_0`$ which is realized in many situations of interest. We define a *sudden parameter* $`ϵ`$ as follows. A dimensionless time $`t`$ and dimensionless operators $`H`$ and $`V(t)`$ are defined through $`s\tau t,`$ $`\widehat{H}\mathrm{}\omega H,`$ and $`\widehat{V}(s)\frac{\mathrm{}}{\tau }V(t)`$, leading to the dimensionless Schrödinger equation $`i\frac{}{t}U(t,t_0)=\left\{V(t)+ϵH\right\}U(t,t_0)`$, where the sudden parameter is defined as $`ϵ\omega \tau `$. We then apply the perturbation theory described above with the identification $`H_0(t)V(t)`$ and $`V_1H`$. This formulation is suited to treat intense short pulses.

Illustration on a pulsed-driven two-level system.

We consider the case where $`H_0(t)=\mathrm{\Omega }(t)\sigma _1`$ and $`V_1=\sigma _3`$ with $`\mathrm{\Omega }(t)`$ a pulse that is switched on at $`t_i`$ and off at $`t_f`$, and $`\sigma _k`$ the Pauli matrices. Notice that, as discussed above, the role of the perturbation and reference Hamiltonian is interchanged. The pulse area $`A_{t_i}^{t_f}\mathrm{\Omega }(u)𝑑u`$ is a dimensionless parameter that can be fixed independently of the sudden parameter $`ϵ`$. The error between the numerical solution of the Schrödinger equation at the end of the pulse and the result of $`n`$ iterations is defined as $`\mathrm{\Delta }_nU_{H_1}(t_f,t_i)U_{H_1}^{(n)}(t_f,t_i)`$. We use the pulse shape $`\mathrm{\Omega }(t)=2A\mathrm{sin}^2\left(\pi t\right)`$ for $`0t1,`$ and $`0`$ elsewhere.

The upper panel of Figure 1 shows a comparison of the error $`\mathrm{\Delta }_1`$ for the first order Dyson, first order Magnus and one-iteration KAM methods as a function of $`t_1`$, for a non-perturbative area chosen to produce comparable errors $`\mathrm{\Delta }_1`$ for the Magnus and non-optimized ($`t_1=0`$) KAM techniques. The lower panel displays $`\lambda _2`$ the largest of the absolute values of the eigenvalues of $`ϵ^2G_2^{(2)}(t_\mathrm{f})`$ defined in Eq. (17). We clearly see that the error of the first KAM iteration is correctly estimated by this eigenvalue $`\lambda _2`$ and, in particular, minimized when $`\lambda _2`$ is minimized, i.e., for the value $`t_1^{}`$. It is worth noting that modifying $`t_1`$ covers more than one order of magnitude in the error, a situation that is not restricted to these values of the parameters. The optimized solution provides an improvement of the accuracy by almost one order of magnitude with respect to the Magnus calculation.

Figure 2 displays a comparison of the error $`\mathrm{\Delta }_2`$ for the second order Dyson, second order Magnus and two-iteration KAM methods as a function of $`t_2`$, for $`t_1=t_1^{}`$. It is seen that the Dyson approach is not applicable in this context of strong field as the second order performs worse than the first one.

Figure 2 also shows that the second KAM iteration can be enhanced by about two orders of magnitude with an appropriate choice of $`t_1`$ and $`t_2`$. This optimized second KAM iteration provides an improvement by two and a half orders of magnitude with respect to the second order Magnus technique. Higher iterations of the KAM technique can also be optimized and produce still better improvement owing to its superconvergent character.

In conclusion, we have presented an optimized perturbation theory for pulse-driven systems, which applies to a wide class of processes controlled by intense femtosecond laser pulses. The optimization reduces to the evaluation of eigenvalues and is therefore easy to implement. We anticipate that this approach will be usefull in the context of the laser control of atomic and molecular processes, such as the phase space localisation of Rydberg electron , or the alignment and orientation of molecules .

This research was supported in part by FNRS, ACI Photonique and Conseil Régional de Bourgogne.