Excitation of a three-level Si:P donor by a Gaussian pulse

I. DONOR WAVEFUNCTIONS FROM KL VARIATIONAL CALCULATION

()
Notations used in this report: |0i is the 1sA state, 2p , , = x, y, z, is the 2p- wavefunction for the valley
(including the cos(k .r) term). The explicit forms of these wavefunctions are
" s ! #
1 1 x2 + y 2 z2
|0i = p 2 exp + 2 cos(kz) + cyclic permutations , (1)
3 a0 b0 a20 b0

where a0 = 2.4 nm, b0 = 1.4 nm, k 0.85 a2

Si
, and 0.8 is the shrink factor due to the central-cell correction (as
discussed in Thomass paper). The ground state energy is E0 = 45 meV.
The 2p0 wavefunction for the z valley is
s s !
2 x 2 + y2 z 2
|2p(z)
z i= exp + 2 z cos(kz) (2)
a21 b31 a21 b1
(x)
with a1 = 3.7 nm, b1 = 2.2 nm. The energy of the 2p0 level is E1 = 11 meV. The 2p0 wavefunctions |2px i for the
(y)
x valley and |2py i for the y valley have the same form with cyclic permutations of x, y, z.
()
The 2p wavefunctions are |2p i with 6= . An example is
s s !
(z) 2 x2 + y 2 z2
|2px i = exp + 2 x cos(kz) (3)
a42 b2 a22 b2

with a2 = 5.5 nm and b2 = 3.4 nm. The energy of the 2p levels is E2 = 6.1 meV.

II. INTERACTION OF DONOR ELECTRON WITH GAUSSIAN PULSE

The time-dependent electric field of a Gaussian pulse with a duration tp is

E(t) = (t) cos(L t), (4)
where
"  2 #
20 t
(t) = exp . (5)
tp /2

The Hamiltonian for a donor in a magnetic field is H = H0 (B) + H1 where

H0 (B) = Hdonor + B B.L (6)
and H1 is the dipole coupling
H1 = e(t) cos(L t)(.r). (7)
Assume that the interaction starts at ti = tp and ends at tf = tp ; this duration covers more than 99% of the pulse.

A. Transition from 1sA to 2p0

(x) (y) (z)

The relevant states for this transition is the ground state |0i and the 2p0 states |2px i , |2py i , |2pz i. Neglecting
the shift due to magnetic field for the 2p0 states, we have
0

~1
H0 = , (8)

~ 1
~1
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where 1 = (E1 E0 )/~ and (as in Bens report),

H1 = e(t)l1 (|0ihe1 | + h.c.) cos(L t) (9)
(x) (y) (z) (x) (y) (z)
where |e1 i = x |2px i + y |2py i + z |2pz i and l1 = h0|x|2px i = h0|y|2py i = h0|z|2pz i. The dimension of H0
can be reduced by switching to the basis of |0i and |e1 i, with which one obtains
 
0 0
H0 = . (10)
0 ~1
and
 
0 2~(t)
H = H0 + H1 = . (11)
2~(t) ~1
where
"  2 #
20 t
(t) = e(t)1 /(2~) = exp (12)
tp /2
with 0 = e0 l1 /(2~). Note that
Z
(t)dt = 0 tp . (13)

We expand the wavefunction as follows

(t) = c0 (t) |0i + c1 (t)eiL t |e1 i . (14)
The Schrodingers equation leads to the following differential equation for c0 (t) and c1 (t) (after making the rotating
wave approximation):
   
d c0 (t) c (t)
= iHrot (t) 0 , (15)
dt c1 (t) c1 (t)
where
 
0 (t)
Hrot (t) = . (16)
(t)
Here = 1 L is the detuning. At resonance when = 0, Hrot (t) at different times commute, and a simple
analytical solution exists
   Z t  
c0 (t) 0 0 c0 (ti )
= exp i Hrot (t )dt (17)
c1 (t) ti
c1 (ti )
  
cos(S(t)) i sin(S(t)) c0 (ti )
= ,
i sin(S(t)) cos(S(t)) c1 (ti )
Rt
where S(t) = ti (t0 )dt0 . For the initial condition (0) = |0i we have
(t) = cos(S(t)) |0i + i sin(S(t))eiL t |e1 i . (18)
At the end of the pulse (at time tf  tp )
f (tf ) = cos(Sf ) |0i + i sin(Sf )eiL t |e1 i , (19)
where
Z
Sf = (t)dt = 0 tp (20)

is the area under the Gaussian curve of (t).

When the field is off resonance, 6= 0, Hrot (t) at different times do not commute and hence the above analytical
solution is no longer valid. Now (tf ) can be obtained by numerical methods. One example is the following second
order method: Divide the interaction duration to N small time steps, tf ti = N t. The time grid is tn = ti +nt, n =
0, 1, . . . , N , then
  NY1  
c0 (tf ) c0 (ti )
= exp[it Hrot (tn + t/2)] . (21)
c1 (tf ) c1 (ti )
n=0
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B. Transition from 1sA to 2p

The dipole coupling Hamiltonian for this transition is

H1 = e(t)l2 (|0ihe2 | + h.c.) cos(L t) (22)

where
1 h i
|e2 i = x (|2p(y)
x i + |2p(z)
x i) +  y (|2p(x)
y i + |2p(z)
y i) +  z (|2p (x)
z i + |2p(y)
z i) (23)
2
(y)
and l2 = 2 h0|x|px i. The magnetic field-split 2p states for the x, y, z valleys are

(x) 1  
|2p i = |2py(x) i i |2pz(x) i , (24)
2
(y) 1  (y) 
|2p i = |2pz i i |2p(y)x i ,
2
(z) 1  (z) 
|2p i = |2px i i |2p(z)y i .
2
One can write |e2 i as the superposition
1
|e2 i = (|2p+ i + |2p i) , (25)
2
where
1 h  (z) (y)
 
(x) (z)
 
(y) (x)
i
|2p i = x |2p i i |2p i + y |2p i i |2p i + z |2p i i |2p i . (26)
2
For the rest of the report we assume that the magnetic field is directed along the [1,1,1] direction so that the energy
shift for the 2p levels are the same for all valleys. We denote this energy shift .
Delta pulse approximation: Assuming that the split 2 between the |2p+ i and |2p i states satisfy 2(tf ti ) 
0 tp , we can neglect this energy split during the pulse. Then we can proceed with the calculation in the basis of |0i
and |e2 i in the same way as in the previous section with |e1 i |e2 i. The final wavefunction is

f (tf ) = cos(Sf ) |0i + i sin(Sf )eiL tf |e2 i , (27)

where Sf is the pulse area given in Eq. (20). The excited state population at the end of the pulse is pe = 1
2
[cos (0 tp )] .
In the general case when tp is not negligible we need to work in the basis of |0i , |+i , |i. We expand the
wavefunction as

(t) = c0 (t) |0i + c+ (t)eiL t |2p+ i + c (t)eiL t |2p i . (28)

In the rotating wave approximation, the coefficients vector c(t) = [c0 (t), c+ (t), c (t)] obeys the differential equation

c(t) = iHrot (t)c(t), (29)

where

0 (t)

2
(t)

2
(t)
2
Hrot (t) = 0
, (30)

(t)

2
0 +

Square pulse: We can approximate the Gaussian pulse by a square pulse with the same pulse area
(
0 if tp /2 < t < tp /2.
(t) = (31)
0 otherwise.
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If initially the donor electron is in the ground state, the final wavefunction at resonance ( = 0) is
!
c0 (tp ) Z tp /2 1
c+ (tp ) = exp i Hrot (t0 )dt0 0 (32)
c (tp ) tp /2 0
2 2
+ cos(1 tp )

0
1 2
0 [(cos(1 tp )1)+i1 sin(1 tp )]

2
=
21 ,
0 [(1cos(1 tp )))+i1 sin(1 tp )]
2
21

p
where 1 = 2 + 20 . The excited state population at the end of the pulse is
2
2 + 20 cos (1 tp )

2
pe = 1 [c0 (tf )] = 1 . (33)
21

Numerical solution for the Gaussian pulse: For the Gaussian pulse in Eq. (12) we solve for the final wavefunction
(at resonance, =0) using the numerical method of Eq. (21). We fix 0 = 0.01 THz, so that the period of the Rabi
oscillation is TRabi = 2/0 628 ps, and consider two different cases: (1) When the energy shift is = 0.001 THz 
0 ; the period of the beat is Tbeat = 2/(2) = 3140 ps, and (2) when = 0 ; the period of the beat is Tbeat = 314
ps. Case 2 is closer to the experimental values of the quantum beat paper. The excited state population as a function
of the pulse duration tp is plotted in Fig. 1 and Fig. 2. The time evolution of the excitation probability during the
interaction window with a Gaussian pulse is also plotted in Fig. 3. The same graph for square pulse is given in Fig. 4
for comparison.
Remarks on the figures: When is comparable to 0 , as in Fig. 2, it is surprising that the result for the square
pulse and the Gaussian pulse are very different. In this regime there is no sustained Rabi oscillation with the Gaussian
pulse no matter how long the pulse duration is. We can also see that sustained Rabi oscillation exists for  0
with the Gaussian pulse (see Fig. 3), and for all values of with the square pulse (see Fig. 4). Im not sure why a
large beat frequency suppresses Rabi oscillation in the case of the Gaussian pulse.

FIG. 1. Excitation probability at the end of the pulse as a function of the pulse duration tp for 0 = 0.01 THz and = 0.001
THz.
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FIG. 2. Excitation probability at the end of the pulse as a function of the pulse duration tp for 0 = = 0.01 THz.

FIG. 3. Time evolution of the excitation probability during a Gaussian pulse with tp = 1500 ps for 0 = 0.01 THz and various
values of .

FIG. 4. Time evolution of the excitation probability during a square pulse with tp = 1500 ps for 0 = 0.01 THz and various
values of .