Laser control of free-carrier density in solids through field-enhanced multiphonon

tunneling recombination
A. M. Zheltikov, M. N. Shneider, A. A. Voronin, and R. B. Miles
Citation: Journal of Applied Physics 109, 033109 (2011); doi: 10.1063/1.3531571
View online: http://dx.doi.org/10.1063/1.3531571
View Table of Contents: http://scitation.aip.org/content/aip/journal/jap/109/3?ver=pdfcov
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JOURNAL OF APPLIED PHYSICS 109, 033109 2011

Laser control of free-carrier density in solids through field-enhanced

multiphonon tunneling recombination
A. M. Zheltikov,1,a M. N. Shneider,2 A. A. Voronin,1 and R. B. Miles2
1

Department of Physics, International Laser Center, M.V. Lomonosov Moscow State University,
Moscow 119992, Russia
2
Department of Mechanical and Aerospace Engineering, Princeton University, Princeton,
New Jersey 08544-5263, USA

Received 18 June 2010; accepted 25 November 2010; published online 10 February 2011
Enhancement of multiphonon tunneling recombination of free carriers in strong laser fields is shown
to offer a mechanism whereby ultrafast carrier-density dynamics in a semiconductor can be
controlled by properly shaped laser pulses. This regime of lasersolid interaction enables an ultrafast
switching of optical and electric properties of semiconductor materials, suggesting new strategies
for laser micromachining and nanomachining, optical data processing, and ultrafast plasmonics.
2011 American Institute of Physics. doi:10.1063/1.3531571

Electronic mail: zheltikov@phys.msu.ru.

0021-8979/2011/1093/033109/7/$30.00

30
20

10

14

10

2
d

15
10

Va

len

20

an

trap

multiphonon
transition

tunnel
e transition

ce
b

16

10

on

Energy

10

Co
b a ndu
nd cti

18

12

10

pump
pulse

Position

dump
pulse

10

10

-7.2

Intensity (GW/cm )

25

-3

Understanding laser-induced ionization phenomena in

solid-state materials is one of the long-standing problems of
optical physics. Research into the main mechanisms and scenarios of free-carrier generation in solids by the intense laser
radiation has helped reveal the general laws of laser-induced
breakdown in solids13 and has led to the discovery of new,
nonlinear-optical regimes of field-induced ionization.4,5
Analysis of laser-induced ionization of solids and related dynamics of free carriers is pertinent to the research aimed at
understanding ultrafast laser-induced phase transitions in
tailoring
ultrafast
carrier
dynamics
in
solids,6
semiconductors,7 and developing ultrafast chip-format semiconductor optical switching devices.8 The most recent relevant work in the area includes the examination of freecarrier
effects
in
semiconductor
nanophotonic
components,911 development of silicon-based Raman
lasers,12 frequency converters,13,14 slow-light devices,1517
and solid-state sources of broadband radiation
supercontinuum,18 and femtosecond micromachining,19,20
including micromodification and nanomodification of solidstate materials with few-cycle laser pulses.21
Ionization of solid-state materials by ultrashort laser
pulses involves a rich and complicated combination of processes, which gives rise to a broad diversity of scenarios. The
buildup dynamics of electron density t within an ultrashort laser pulse, however, usually follows a typical
switch-on-only pattern Fig. 1, controlled by the integral
t
wd, with the photoionization rate w
relation t
typically scaling as w IN, where I is the intensity
envelope of the laser pulse and the parameter N is understood as the number of photons required to promote an electron from the valence band to the conduction band in the
regime of multiphoton ionization or assigned a noninteger
effective, best-fit value in the regime of tunneling ionization.
Long lifetimes of free carriers then lead to pulse-to-pulse
accumulation of free carriers in a laser-irradiated medium,

which limits the performance of semiconductor photonic devices at high repetition rates and can eventually give rise to
an optical damage of the material. The monotonic increase in
the electron density t within the laser pulse translates into
a blue shift in spectral transformations of ultrashort laser
pulses in ionizing materials.22,23 Sign reversal of this frequency shift would suggest the way to reduce the carrier
density remaining in the material in the wake of the laser
pulse and would give a better control of the spectrum and,
hence, the temporal and spatial chirp of broadband field
waveforms produced in ionizing materials, thus helping to
synthesize extremely short light pulses and helping manipulate their phase profiles.

Electron density (cm )

I. INTRODUCTION

-7.0

-6.8

-4

-2

Retarded time (ps)

FIG. 1. Color online Laser control of free-carrier density in a semiconductor through field-enhanced multiphonon tunneling recombination. The fieldenhanced multiphonon recombination process diagram in the inset involves tunneling of conduction-band electrons and valence-band holes to a
recombination center site horizontal branches in the inset, assisted by the
emission of several phonons the vertical branch in the inset. The pump
pulse thin solid line induces ionization of a semiconductor, increasing the
density of free carriers solid line. A properly delayed dump pulse thin
solid line enhances recombination, thus reducing the electron density in a
medium. Variations in electron and hole densities in a semiconductor are
sketched in the upper part of the figure.

109, 033109-1

2011 American Institute of Physics

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033109-2

J. Appl. Phys. 109, 033109 2011

Zheltikov et al.

Here, we show that the enhancement of multiphonon

tunneling recombination of free carriers in strong laser
fields24,25 suggests the way to control ultrafast carrier-density
dynamics in a semiconductor material. The generic model of
electron-density dynamics adopted in this work includes
photoionization, avalanche ionization, and multiphonon tunneling recombination, described in terms of field-dependent
ShockleyReadHall SRH carrier lifetimes.26,27 Based on
this model, we demonstrate that, with properly optimized
parameters of laser pulses, field-enhanced multiphonon tunneling recombination of free carriers can enable an ultrafast
switching of optical and electric properties of semiconductor
materials Fig. 1, offering new strategies for laser micromachining, optical data processing, and ultrafast plasmonics.
II. MODEL

We model the dynamics of electron density in a semiconductor using a standard kinetic-equation approach28,29 assuming that electrons are generated through multiphoton or
tunneling photoionization and avalanche ionization and that
electron recombination is exponential with a well-defined
lifetime r:

= wI +
It .
t
U
r

Here, is the cross section of avalanche ionization, is the

laser frequency, and U is the effective ionization potential.5
For direct-band semiconductors, the photoionization rate
is calculated by using the Keldysh formalism.5 For indirectgap semiconductors, including silicon, where phonons are
required to pickup the crystal-momentum mismatch in ionizing transitions, the photoionization rate can be found by using the available experimental data on cross sections of multiphoton absorption see, e.g., Refs. 30 and 31. In particular,
in the range of wavelengths where photoionization is dominated by two-photon transitions 2PA, the photoionization
rate is defined as w2I 21I2, where is the cross
section of two-photon absorption. For longer wavelengths,
when three-photon transitions 3PA play the main role, the
photoionization rate is given by w3I 31I3, with
being the cross section of three-photon absorption.
To include avalanche ionization in our model, we use the
Drude formula for ,

c
e2
,
cn00m 1 + 22c

where c is the speed of light, n0 is the refractive index of the

material, e and m are the electron charge and effective mass,
respectively, and c is the Drude damping time,32 controlled
by electronphonon and electronelectron collisions in the
low-density and high-density regimes, respectively.
While in the earlier work see, e.g., Refs. 9, 21, and 28,
kinetic equations for the electron density have been solved
with an assumption of field-independent recombination time
r, here we extend this approach to include the dependence
of r on the field intensity I in the regime of trap-assisted
multiphonon tunneling recombination. This type of recombination involves tunneling of conduction-band electrons and

valence-band holes to a recombination center site horizontal

branches in the inset to Fig. 1, assisted by the emission of
several phonons the vertical branch in the inset to Fig. 1.
The probability of the multiphonon transition involved in
this process exponentially decreases with the growth in the
number of phonons needed to close the vertical part of the
recombination path. The tunneling probability, on the other
hand, is an exponentially decreasing function of the barrier
thickness. An electric field modifies the potential, thus
changing the most probable path of recombination, controlled by the exponential factors defining tunneling and
multiphonon transition probabilities. To include these mechanisms into the model of electron-density dynamics, we employ the generic Schenk formalism for SRH carrier
lifetimes,24,25

r rI =

0
,
gI

where 0 rI = 0 and gI is the field-enhancement factor.

For single-level recombination centers with a concentration Nt and a binding energy Et measured from the minimum of the conduction band, the field-enhancement factor
gI in the high-temperature regime including the roomtemperature range is given by the Schenk formula:24
gI = 1 +

1
2RkT
1+

3/2
3 i=x,y,z
i Et E0i1/2

a0 + Et i
kT
Et + R

1/2

3/2

exp

a0 ai
Et E0i
exp
kT
kT

exp

4 Et E0i
3 i

3/2

where k is the Boltzmann constant, T is the temperature, is

the Planck constant, R = S0 is the lattice relaxation
energy, 0 is the phonon energy, S is the HuangRhys
factor,
E0i = 2Fi1/2Fi + R + Et1/2 Fi1/2 R,
Fi
2
= 2RkT i3,
a0 = Et R24R1,
ai = E0i
R24R1, i = e2E21/32mi1/3, E is the field amplitude, mi = mt1 1 mt / mlE2i / E21 is the electron tunneling mass, Ei is the ith field component, and mt and ml are the
transverse and longitudinal effective masses, respectively.
The
Schenk
description
of
field-dependent
lifetimes24,25,33 is based on a combination of a standard
theory of multiphonon transitions34,35 and the theory of
Bloch electrons in a strong field.3639 Recombination centers
are assumed to have a single energy state with a deltafunction potential wave function and KosterSlater orbitals.
The model explicitly includes the anisotropy and the specific
multivalue shape of the conduction band of a semiconductor.
The phonon spectrum is assumed to consist of a single phonon mode with a frequency 0 the Einstein model, so that
the energy can be transferred only in portions multiple of
0. The phonon mode is assumed to stay decoupled from
the band states, and the frequency 0 is assumed to remain
constant during transitions. Finally, PoolFrenkel-type phe-

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J. Appl. Phys. 109, 033109 2011

18

10

-11

10

-13

10

0.000

0.003

0.006

10

10

0.020

1
2

0.009
2

Intensity (TW/cm )

3
0.015

17

10

16

10

0.010

15

10

14

10

13

10

20

0.025

0.005

a)

12

0.000

10

-6

-4

-2

0.025

10

Retarded time (ps)

19

10

0.020

18

10

10

-3

10

17

10

0.015

16

10

0.010

15

10

14

10

13

10

Intensity (TW/cm )

19

10

10

-9

10

electron density (cm )

10

-7

10

-3

electron density (cm )

20

Intensity (TW/cm )

21

10

Enhancement factor

Zheltikov et al.
Recombination time (s)

033109-3

0.005

b)

12

0.000

10

-2

Retarded time (ps)

FIG. 2. Color online Dynamics of electron density in a laser-irradiated semiconductor crystalline silicon with 1 r = 0 = 260 ns, 24 r given by Eq. 3
with 0 = 260 ns 2, 80 ns 3, and 26 ns 4. The laser pulse shown by the dashed-dotted line has a peak intensity of 10 GW/ cm2, a pulse width p
= 4 ps a and 2 ps b, and a central wavelength = 1500 nm a and 2350 nm b. The critical electron density is shown by the dotted line. The inset presents
the field-enhancement factor g solid line and the recombination time r = 0 / g with 0 = 260 ns dashed line as functions of the field intensity.

nomena, related to the lowering of the tail of the Coulomb

potential barrier in the presence of a strong electric field, are
neglected. The Schenk model is, rigorously speaking, applicable for static fields. However, because of the weak or no
frequency dependence of the tunneling probability, staticfield models often provide important and useful insights into
the scenarios of electron tunneling in alternating fields.5,40,41
Since it assumes a static field, the Schenk formula Eq. 4
predicts no resonant enhancement of lasersolid interaction
for field frequencies tuned to the frequency separating the
trap level from the band edges. However, when the field is
sufficiently strong so that tunneling dominates the recombination process, such an enhancement should be suppressed
even in the case of alternating fields, except for the leading
and trailing edges of a laser pulse, where the optical response
would be much more complicated. Although we mainly focus below on field-enhanced multiphonon tunneling in a
semiconductor with parameters of crystalline silicon with a
gold acceptor level, analysis can be generalized to other
types of practically significant semiconductor materials, including gallium arsenide.33
For the analysis of carrier-density dynamics in crystalline silicon, the frequency-dependent two- and three-photon
absorption coefficients and are defined in accordance
with the experimental data from Refs. 28 and 29, with
0.48 cm/ GW at the wavelength of 1500 nm and
0.025 cm3 / GW2 at 2350 nm. For the range of electron
densities studied in this work below 1021 cm3, the Drude
damping time for silicon can be estimated as c 10 fs.42,43
The effective ionization potential is calculated as5 U
= 21U01/2E, where E is the full elliptic integral of
the second kind, = K2 1 + K2 1, = 1 + K2 1, K
= meU01/2eE1 is the Keldysh parameter, and we take
U0 1.1 eV for silicon. Other parameters appearing in Eqs.
1, 2, and 4 are defined as Et 0.55 eV, mt = 0.19me,
ml = 0.92me, m = 0.18me me is the electron mass, 0
0.068 eV, S = 3.5, and T = 300 K
In agreement with the earlier calculations by Schenk,24
the growth in the field intensity enhances multiphonon tunneling recombination, reducing the relevant electron lifetime
in a semiconductor with the above-specified parameters from
0 100 s to r 100 ps at I 10 GW/ cm2, with the gI
profile as shown by the solid line in the inset to Fig. 2. The

dashed line in this inset presents a typical rI = 0 / gI dependence calculated by applying the same gI profile to a
sample with 0 = 260 ns, corresponding to an effective density of recombination centers Nt 3 1012 cm3. In the
presence of a field with I 10 GW/ cm2, the electron lifetime in a sample with such a density of recombination centers is estimated as r 0.9 ps.
III. RESULTS AND DISCUSSION

Figures 2a and 2b illustrate the influence of fieldenhanced multiphonon tunneling recombination on the dynamics of electron density t in a semiconductor with the
above-specified parameters irradiated by a laser pulse with a
peak intensity of 10 GW/ cm2, a pulse width p = 4 ps Fig.
2a and 2 ps Fig. 2b, and a central wavelength of 1500
nm Fig. 2a, the range where photoionization is dominated
by 2PA and 2350 nm Fig. 2b, the range where photoionization is mainly due to 3PA. Dashed curves 1 in Figs. 2a
and 2b present the t profiles calculated with a standard
assumption of a large field-independent recombination time
r p. Dynamics of the electron density in this regime has
been thoroughly studied in the earlier work see, e.g., Refs.
28 and 29 for review. Briefly, t displays a monotonic
growth due to ionization within the laser pulse with its decay
in the wake of the laser pulse t p, controlled by the fieldfree recombination time r p, being too slow to be visible
on the time scale of Figs. 2a and 2b.
Enhancement of multiphonon tunneling recombination
can radically change the character of t profiles. Curves
24 in Figs. 2a and 2b present the results of calculations
performed by using Eqs. 14 for different central laser
wavelengths and different values of 0. Ionization in the
leading edge of the laser pulse gives rise to a rising section of
the t profile. Field enhancement of multiphonon tunneling
recombination does not play an important role at this stage
because the field intensity is still low. However, closer to the
peak of the laser pulse, where the field provides the maximum enhancement of multiphonon tunneling, leading to
minimum carrier lifetimes, a clearly pronounced dip is observed in the t profile. In the trailing edge of the pulse, the
electron density increases again. Here, the decreasing laser
field does not provide a substantial enhancement of mul-

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J. Appl. Phys. 109, 033109 2011

Zheltikov et al.
0.030

0.030
20

0.020
16

10

0.015

14

10

0.010

12

a)

10

0.005

10

-4

-3

-2

-1

0.025
2

18

10

0.020
16

10

0.015

14

10

0.010

12

b)

10

0.005

10

0.000

10

10

-3

Intensity (TW/cm )

-3

electron density (cm )

0.025
18

10

electron density (cm )

20

10

Intensity (TW/cm )

033109-4

0.000

10

-4

-3

Retarded time (ps)

-2

-1

Retarded time (ps)

FIG. 3. Color online Dynamics of electron density in a semiconductor irradiated with a Gaussian laser pulse shown by the dashed-dotted line with a peak
intensity of 10 GW/ cm2, a pulse width p = 2.5 ps a and 3.5 ps b, and a central wavelength = 1500 nm a and 2350 nm b. The initial electron density
0, from bottom to top, is a 0, 1014, 1016, 1018, 5 1019 cm3 and b 0, 1014, 1016, 1018, 3 1018 cm3; 0 = 26 ns. The critical electron density is shown by
the dotted line.

tion, respectively. Such pulses, as can be seen from the results of calculations presented in Figs. 4a and 4b, can
lower the carrier density in a semiconductor material by
more than three orders of magnitude from the initial level of
0 = 5 1019 cm3 to w = 3.6 1016 cm3 in the wake of the
pulse for = 1500 nm in Fig. 4a.
Importantly, the stationary level of the electron density
s observed in t profiles in Figs. 3 and 4 is virtually independent of the initial carrier density 0. To explain this result,
we set / t = 0 in Eq. 1 and formally solve the resulting
equation for the stationary electron density as s wef f ,
1
with 1
ef f = r I / U. This approximate solution is presented
by open circles in Figs. 4a and 4b, showing an excellent
agreement with the results of simulations using Eq. 1.
In Figs. 5a5c, we plot the electron density w in the
wake of the laser pulse calculated as a function of the pulse
width Figs. 5a and 5b and central wavelength Fig. 5c
of a super-Gaussian laser pulse It = I0 expt10 / 10
0 with
I0 = 10 GW/ cm2 for semiconductor samples with different 0
with filled circles and rectangles and without open circles
and rectangles inclusion of avalanche ionization. These calculations demonstrate that semiconductors with shorter 0
higher densities of recombination centers are favorable for
the ultrafast switching of carrier density due to fieldenhanced multiphonon tunneling recombination. In samples
with shorter 0, the carrier density can be dumped, as can be
seen from Figs. 5a and 5b, by using shorter laser pulses,

tiphonon tunneling recombination, while the electron density

is high enough to give rise to efficient avalanche ionization.
In Figs. 3a and 3b, we show how the field enhancement of multiphonon tunneling recombination can be used to
lower the carrier density in a semiconductor material where
photoionization is dominated by 2PA Fig. 3a and 3PA
Fig. 3b. In these calculations, we assume that a certain
initial density of free carriers 0 below the critical electron
density c shown by the dotted line has been created in a
sample before the laser pulse. As can be seen from Figs. 3a
and 3b, with an appropriate choice of parameters of the
laser pulse, enhanced recombination around the peak of the
pulse can substantially reduce the electron density in a medium, which can be used for ultrafast switching of electric
and optical properties of semiconductor materials and can
help to increase the laser damage threshold at high repetition
rates of laser pulses.
Specifically shaped laser pulses can be used to reduce
the unwanted increase in the electron density in the trailing
edge of the pulse, which is caused by avalanche ionization,
facilitated by the high density of carriers generated by the
leading edge and the central part of the pulse. Figures 4a
and 4b present electron density profiles t calculated for a
semiconductor with different initial carrier densities 0 c
irradiated by a super-Gaussian pulse with 0.7 ps pulse edges
shown by the dashed-dotted line and a central wavelength
of 1500 nm Fig. 4a and 2350 nm Fig. 4b, corresponding to two-phonon and three-photon regimes of photoioniza-

0.030

16

10

14

10

12

0.015
0.7 ps
0.010
0.005

a)
10

Intensity (TW/cm )

0.020

10

-10

-8

-6

-4

-2

Retarded time (ps)

0.000
10

0.025
18

10

0.025

Intensity (TW/cm )

18

-3

10

20

10

electron density (cm )

20

-3

electron density (cm )

0.030
10

10

0.020
16

10

0.015
0.7 ps

14

10

0.010

12

10

0.005

b)
10

10

-10

-8

-6

-4

-2

0.000
10

Retarded time (ps)

FIG. 4. Color online Dynamics of electron density in a semiconductor irradiated with a super-Gaussian laser pulse shown by the dashed-dotted line with
a peak intensity of 10 GW/ cm2, a pulse width of 10 ps, and a central wavelength = 1500 nm a and 2350 nm b. The initial electron density 0, from
bottom to top, is a 0, 1014, 1016, 1018, 5 1019 cm3 and b 0, 1014, 1016, 1018, 2 1019 cm3; 0 = 26 ns. The critical electron density is shown by the dotted
line. Open circles present the approximate solution s wef f for the stationary electron density.

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033109-5

J. Appl. Phys. 109, 033109 2011

Zheltikov et al.
20

21

10

10
-3

Electron density (cm )

-3

Electron density (cm )

a)
19

10

18

10

17

10

b)

20

10

19

10

18

10

17

10

16

10

16

10

10

12

FWHM pulse width (ps)

-3

Electron density (cm )

10

2000

2500

2PA

c)

10

FWHM pulse width (ps)

1500
21

3000

3PA

21

10

20

10

19

10

18

10

17

10

16

10

15

10

20

10

19

10

18

10

17

10

16

10

15

10

1500

2000

2500

3000

Wavelength (nm)
FIG. 5. Color online The electron density w in the wake of the laser pulse calculated as a function of the FWHM pulse width a and b and central
wavelength c of a super-Gaussian laser pulse with a peak intensity of 10 GW/ cm2 with filled circles and rectangles and without open circles and
rectangles inclusion of avalanche ionization: a = 1500 nm; b = 2350 nm; c the dashed horizontal line separates the regions where photoionization is
dominated by 2PA and 3PA, the laser pulse width is 1.3 ps for the 2PA region and 1.6 ps for the 3PA region. The initial electron density is 5 1019 cm3 a
and 1019 cm3 b; for 0 = 80 ns rectangles and 26 ns circles. The critical electron density is shown by the dotted line.

making it possible to suppress effects related to avalanche

ionization. Indeed, with 0 = 26 ns, the minimum electron
density w in the wake of the pulse is achieved with a dump
pulse width of 1.3 ps. For such a pulse, the contribution of
avalanche ionization is reduced to about 10% of the overall
w value cf. filled-circle and open-circle lines in Fig. 5a.
When 0 = 80 ns, however, the optimal dump pulse width is
estimated as 4.5 ps in the regime where two-photon processes dominate photoionization Fig. 5a. The avalanche
ionization then generates more than 50% of carriers in the
trailing edge of the pulse cf. filled-rectangle and openrectangle lines in Fig. 5a. When photoionization is dominated by three-photon processes Fig. 5b, effect of the avalanche ionization is even more dramatic. With 0 = 80 ns, the
avalanche ionization then generates electron densities exceeding c, thus leading to a laser damage of the material, for
any sensible pulse width filled rectangles in Fig. 5b.
The Drude model of avalanche ionization cross section
Eq. 2 suggests that effects related to this type of ionization can be reduced by choosing shorter wavelengths of the
laser field. Indeed, with c2 1, which is the case studied
here, Eq. 2 yields 21
c . Since the rate of avalanche
ionization is proportional to the current value of carrier density t see Eq. 1, this recipe for the suppression of avalanche ionization should be corrected to include the spectral
dependences of the two-photon and three-photon absorption

coefficients. The net effect of avalanche ionization as a function of the laser wavelength is seen in Fig. 5c. The dashed
horizontal line in this figure separates the region where
photoionization is dominated by 2PA from the area where
photoionization is mainly due to 3PA. The full width at half
maximum FWHM pulse width in this figure is chosen in
such a way as to provide the minimum of w for given 0 and
central laser wavelength. For 0 = 26 ns, this is achieved with
a pulse width of 1.3 ps in the 2PA region corresponding to
the minimum of the filled-circle curve in Fig. 5a and 1.6
ps in the 3PA region filled circles in Fig. 5b. For 0
= 80 ns, the FWHM pulse width is set equal to 4.5 ps, which
corresponds to the minimum of the filled-rectangle curve in
Fig. 5a. It can be seen from Fig. 5c that the significance
of avalanche ionization rapidly increases with the growth in
the laser wavelength. For samples with a higher density of
recombination centers 0 = 26 ns, where shorter 1.31.6
ps laser pulses can be used to dump the carrier density, the
avalanche ionization tends to lower the efficiency of carrierdensity control but does not lead to dramatic consequences,
as w remains much lower than the critical electron density
within the entire wavelength range under study filled circles
in Fig. 5c. On the contrary, for lower-Nt samples 0
= 80 ns, where longer laser pulses are necessary to efficiently control the carrier density, the avalanche ionization

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J. Appl. Phys. 109, 033109 2011

Zheltikov et al.
0

-2

10

3.0x10

-2

3.0x10

10
2

Intensity (TW/cm )

-2

-3

10

2.0x10

-4

10

1.5x10

2
1

1.0x10

-5

10

-2

-2

-6

-3

5.0x10

-2

10

-7

-6

-4

-2

-2

1.5x10

2
1

1.0x10

-4

10

-5

10

-6

10

-2

-3

5.0x10

b)

-7

0.0
-8

-6

-4

-2

Retarded time (ps)

Retarded time (ps)

-1

-1

s (s )

-2

10

13

-2

10

3.0x10

12

s (s )

-2

3.0x10

12

2.5x10

-2

2.5x10

11

-2

10

2.0x10

10

10

1.5x10

2
1

1.0x10

10

-2

10

-2

-3

5.0x10

10

Intensity (TW/cm )

13

10

-2

2.0x10

10

0.0
-8

1
2

-3

10

a)

10

-2

2.5x10

-2

2.5x10
-2

10

10

dnp

-1

11

10

-2

2.0x10

10

10

10

10

c)

-2

1.5x10

2
1

1.0x10

-2

-3

5.0x10

d)

0.0

10

-8

Intensity (TW/cm )

dnp
-1

10

Intensity (TW/cm )

033109-6

-6

-4

-2

Retarded time (ps)

0.0

10

-8

-6

-4

-2

Retarded time (ps)

FIG. 6. Color online Temporal profiles of the correction to the refractive index n pt a and b and the electrical conductivity ct c and d induced
in a semiconductor by a super-Gaussian laser pulse shown by the dashed-dotted line with a peak intensity of 10 GW/ cm2, a central wavelength
= 1500 nm a and c and 2350 nm b and d, and the duration of pulse edges 1 3 ps, 2 0.7 ps, and 3 0.1 ps. The initial electron density is 5
1019 cm3 a and c and 1019 cm3 b and d; 0 = 26 ns.

generates electron densities exceeding the critical density c

shown by the dotted line in Figs. 5a5c already for laser
wavelengths 2.05 m filled rectangles in Fig. 5c. In
this regime, efficient laser control of electric and optical
properties of semiconductor materials is limited to a narrow
wavelength region, requiring a careful optimization of the
central wavelength of control laser pulses.
Generation and recombination of carrier density in a
semiconductor translate into a time-dependent change in the
1 1/2
refractive index, n pt n0 n20 t / c1 + 22
c ,
and
electric
conductivity,
ct t / 4cc1
1
+ 22
c . The solid lines in Figs. 6a6d present the
temporal profiles of n pt Figs. 6a and 6b and ct
Figs. 6c and 6d calculated for a semiconductor with
above-specified silicon-type parameters irradiated by flattop laser pulses shown by the dashed lines in Figs.
6a6d with different durations of pulse edges and central
wavelengths of the laser pulse corresponding to the regimes
of two-photon Figs. 6a and 6c and three-photon Figs.
6b and 6d photoionization. As can be seen from these
plots, laser pulses with steeper trailing edges help to avoid
the unwanted increase in the electron density within the field
turn-off time see also Figs. 4a and 4b, thus providing a
higher contrast of refractive-index and electric-conductivity
switching, defined as the ratio of stationary n p and c values before and after the laser pulse. In particular, refractiveindex and electric-conductivity switching contrasts as high as
3 103 can be achieved with a 0.1 ps edge pulse for a material with the above specified parameters curves 1 in Figs.
6a and 6c, suggesting an attractive strategy for ultrafast
optical switching, reversible micromachining and material

processing, reversible laser writing of reconfigurable photonic and plasmonic structures, as well as high-speed optical
information processing.
IV. CONCLUSION

We have shown in this work that the enhancement of

multiphonon tunneling recombination of free carriers in
strong laser fields suggests the way to control ultrafast
carrier-density dynamics in a semiconductor material. Laser
pulses with properly optimized parameters for fieldenhanced multiphonon tunneling recombination of free carriers have been demonstrated to enable an ultrafast switching
of optical and electric properties of semiconductor materials.
An intriguing new physical feature of the lasersolid interaction scenario identified in this work is that, instead of further increasing the density of free carriers in a laser-preexcited semiconductor, a properly shaped laser pulse with
carefully optimized parameters can significantly lower the
carrier density, thus realizing a new regime of lasermatter
interactions and offering new strategies for laser micromachining, optical data processing, and ultrafast plasmonics.
ACKNOWLEDGMENTS

Illuminating discussions with R. Kotlyar are gratefully

acknowledged. Research by A.A.V. and A.M.Z. was supported in part by the Russian Federal Science and Technology Program and International Science and Technology Center. A.A.V. also acknowledges the support of his work by the
Russian Foundation for Basic Research Project Nos. 08-0291756, 09-02-12359, and 09-02-12373.

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033109-7

Zheltikov et al.

E. Yablonovitch and N. Bloembergen, Phys. Rev. Lett. 29, 907 1972.

N. Bloembergen, IEEE J. Quantum Electron. 10, 375 1974.
3
Y. R. Shen, Rev. Mod. Phys. 48, 1 1976.
4
L. V. Keldysh, Zh. Eksp. Teor. Fiz. 33, 994 1957.
5
L. V. Keldysh, Zh. Eksp. Teor. Fiz. 47, 1945 1964 Sov. Phys. JETP 20,
1307 1965.
6
A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C.
Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D.
Weinstein, D. P. Lowney, T. K. Allison, T. Matthews, R. W. Falcone, A. L.
Cavalieri, D. M. Fritz, S. H. Lee, P. H. Bucksbaum, D. A. Reis, J. Rudati,
P. H. Fuoss, C. C. Kao, D. P. Siddons, R. Pahl, J. Als-Nielsen, S. Duesterer, R. Ischebeck, H. Schlarb, H. Schulte-Schrepping, T. Tschentscher, J.
Schneider, D. von der Linde, O. Hignette, F. Sette, H. N. Chapman, R. W.
Lee, T. N. Hansen, S. Techert, J. S. Wark, M. Bergh, G. Huldt, D. van der
Spoel, N. Timneanu, J. Hajdu, R. A. Akre, E. Bong, P. Krejcik, J. Arthur,
S. Brennan, K. Luening, and J. B. Hastings, Science 308, 392 2005.
7
S. Gupta, J. F. Whitaker, and G. A. Mourou, IEEE J. Quantum Electron.
28, 2464 1992.
8
R. Soref, IEEE J. Sel. Top. Quantum Electron. 12, 1678 2006.
9
Q. Lin, J. Zhang, P. M. Fauchet, and G. P. Agrawal, Opt. Express 14, 4786
2006.
10
B. Jalali, Nat. Photonics 1, 193 2007.
11
P. K. Kashkarov, L. A. Golovan, A. B. Fedotov, A. I. Efimova, L. P.
Kuznetsova, V. Y. Timoshenko, D. A. Sidorov-Biryukov, A. M. Zheltikov,
and J. W. Haus, J. Opt. Soc. Am. B 19, 2273 2002.
12
H. Rong, A. Liu, R. Jones, O. Cohen, D. Hak, R. Nicolaescu, A. Fang, and
M. Paniccia, Nature London 433, 292 2005.
13
M. A. Foster, A. C. Turner, J. E. Sharping, B. S. Schmidt, M. Lipson, and
A. L. Gaeta, Nature London 441, 960 2006.
14
L. A. Golovan, A. M. Zheltikov, P. K. Kashkarov, N. I. Koroteev, M. G.
Lisachenko, A. N. Naumov, D. A. Sidorov-Biryukov, V. Y. Timoshenko,
and A. B. Fedotov, JETP Lett. 69, 300 1999.
15
Y. A. Vlasov, M. OBoyle, H. F. Hamann, and S. J. McNab, Nature London 438, 65 2005.
16
Y. Okawachi, M. Foster, J. Sharping, A. Gaeta, Q. Xu, and M. Lipson,
Opt. Express 14, 2317 2006.
17
A. M. Zheltikov, Phys. Rev. A 76, 033825 2007.
18
I.-W. Hsieh, X. Chen, X. Liu, J. I. Dadap, N. C. Panoiu, C.-Y. Chou, F.
1
2

J. Appl. Phys. 109, 033109 2011

Xia, W. M. Green, Y. A. Vlasov, and R. M. Osgood, Opt. Express 15,
15242 2007.
19
D. Du, X. Liu, G. Korn, J. Squier, and G. Mourou, Appl. Phys. Lett. 64,
3071 1994.
20
R. R. Gattass and E. Mazur, Nat. Photonics 2, 219 2008.
21
M. Lenzner, J. Krger, S. Sartania, Z. Cheng, C. Spielmann, G. Mourou,
W. Kautek, and F. Krausz, Phys. Rev. Lett. 80, 4076 1998.
22
W. M. Wood, C. W. Siders, and M. C. Downer, IEEE Trans. Plasma Sci.
21, 20 1993.
23
A. J. Verhoef, A. Mitrofanov, A. Zheltikov, and A. Baltuka, Opt. Lett. 34,
82 2009.
24
A. Schenk, Solid-State Electron. 35, 1585 1992.
25
A. Schenk, Solid-State Electron. 36, 19 1993.
26
W. Shockley and W. T. Read, Jr., Phys. Rev. 87, 835 1952.
27
R. N. Hall, Phys. Rev. 87, 387 1952.
28
A. Couairon, L. Sudrie, M. Franco, B. Prade, and A. Mysyrowicz, Phys.
Rev. B 71, 125435 2005.
29
L. Berg, S. Skupin, R. Nuter, J. Kasparian, and J.-P. Wolf, Rep. Prog.
Phys. 70, 1633 2007.
30
Q. Lin, J. Zhang, G. Piredda, R. W. Boyd, P. M. Fauchet, and G. P.
Agrawal, Appl. Phys. Lett. 91, 021111 2007.
31
S. Pearl, N. Rotenberg, and H. van Driel, Appl. Phys. Lett. 93, 131102
2008.
32
M. L. Cohen and J. R. Chelikowski, Electronic Structure and Optical
Properties of Semiconductors Springer, Heidelberg, 1989.
33
A. Schenk, J. Appl. Phys. 71, 3339 1992.
34
K. Huang and A. Rhys, Proc. R. Soc. London, Ser. A 204, 406 1950.
35
C. H. Henry and D. V. Lang, Phys. Rev. B 15, 989 1977.
36
L. V. Keldysh, Sov. Phys. JETP 6, 763 1958.
37
E. O. Kane, J. Appl. Phys. 32, 83 1961.
38
D. E. Aspnes, F. A. Germano, and P. Handler, Phys. Rev. 166, 921 1968.
39
D. F. Blossey, Phys. Rev. B 2, 3976 1970.
40
F. Brunel, J. Opt. Soc. Am. B 7, 521 1990.
41
G. L. Yudin and M. Y. Ivanov, Phys. Rev. A 64, 013409 2001.
42
P. P. Pronko, P. A. VanRompay, C. Horvath, F. Loesel, T. Juhasz, X. Liu,
and G. Mourou, Phys. Rev. B 58, 2387 1998.
43
K. Sokolowski-Tinten and D. von der Linde, Phys. Rev. B 61, 2643
2000.

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