A method for controlling the bandwidth of high energy, fewoptical-cycle

Ukr. J. Phys. Opt. 2015, Volume 16, Issue 4 147
A method for controlling the bandwidth of high-energy, few-
optical-cycle laser pulses tunable from the visible to the near-
infrared
Walid Tawfik
Department of Physics and Astronomy, College of Science, King Saud University,
Riyadh 11451, Saudi Arabia,
Department of Environmental Applications, National Institute of Laser NILES,
Cairo University, Cairo, Egypt Walid_tawfik@hotmail.com
Received: 30.06.2015
Abstract. In this work we report a new method for controlling the bandwidth of
few-cycle optical pulses, using another femtosecond laser pulses chirped in a neon-
filled hollow-core fibre. The observed bandwidth varies from 25 to 234 nm in the
optical wavelength region 600–950 nm. The pulse energy has for the first time
reached a sub-millijoule frontier at 1 kHz. The input pulses are positively chirped
using a chirped-pulse amplifier to acquire the widths 32–56 fs at the entrance of the
hollow fibre. Then the pulses are highly dispersed due to a self-phase modulation in
a nonlinear medium (a neon gas) followed by a pair of chirped mirrors that
compensate the dispersion. We have found that this scheme allows for direct tuning
of the output-pulse bandwidth while varying the chirping of the input pulses under
different neon-gas pressures. Our results can give an opportunity for controlling the
interactions in strong electric fields on the ultrafast time scales and are crucial for
regenerating attosecond X-ray pulses.
Keywords: ultrafast lasers, tunable femtosecond lasers, few-cycle lasers, self-phase
modulation
PACS: 78.47.jj
UDC: 535.37
1. Introduction
As long ago as in 1960s it has been realized that lasers should have strong impact on the
spectroscopy. To begin with, they offer intense light sources with high energy densities that
surpass, by many orders of magnitude, those achieved earlier with incoherent light sources.
Moreover, due to their bandwidth controlled from the vacuum UV to the far IR range, single-mode
lasers allow for a very high spectral resolution inaccessible in frame of the conventional methods
applied in the pre-laser epoch.
High intensity and spectral monochromatism of tunable lasers have initiated a new kind of
spectroscopic methods, allowing detailed exploration of structures of ‘large’ atoms and molecules
[1]. In many aspects, the laser absorption spectroscopy resembles the microwave spectroscopy,
where carcinotrons or klystrons represent tunable coherent radiation sources, analogues of tunable
lasers. In other words, the laser spectroscopy can transfer many advantages and techniques adopted
from the microwave spectroscopy into the UV, VIS or even the IR spectral ranges [2]. The bene-
fits of the absorption spectroscopy based on the tunable lasers include, in particular, the absence of
need in monochromators, because the absorption coefficient and its frequency dependence can be
determined directly from the difference between the intensities of the reference and transmitted
beams. The detector noises can be often ignored because of high spectral power densities of lasers,

Ukr. J. Phys. Opt. 2015, Volume 16, Issue 4148
as a consequence of laser-beam collimation. Furthermore, long absorption paths can be analyzed
using multiple back-and-forth reflections inside multiple-path absorption cells. Finally, it is
possible to tune the laser wavelength very fast over the whole spectral region to match the
molecular absorption. In this way rapid relaxation or transient absorption processes can be inves-
tigated, using short-pulse lasers with the time resolutions lying in the femtosecond domain [3, 4].
Novel developments of the femtosecond laser technology have enabled it to become a
powerful tool in the fields of materials diagnostics and ultrafast spectroscopy [5–8]. Combining
nonlinear optical techniques with the intense ultrashort pulses obtained from amplified solid-state
lasers, one can generate widely tunable femtosecond light pulses ranging from the near UV to the
IR [8–12]. Among many interesting developments, the nonlinear optical interactions with self-
phase modulation, which generate supercontinuum in the optical region using two gas-filled
microstructured hollow fibres, have attracted much attention of researchers [13–16]. Here
essentially nonlinear pulse compression relies on the interaction of Kerr nonlinearity and quadratic
dispersion [17]. These approaches are basically nonlinear and can produce increasing in the pulse
bandwidth, which cannot be directly obtained with purely linear schemes [18]. According to this
significant property, shorter transformation-limited pulses can be achieved, using a compression of
pulses with nonlinear pulse-compression techniques [19]. Being widely applied in the nonlinear
fibre optics, the pulse compression is based upon to the two different methods, a soliton effect and
a fibre grating effect [20]. The fibre compressors are typically preferred in the VIS and near-IR
optical ranges, while the compressors built on the soliton effect are often used in the IR range
(1.3–1.6 μm) [21]. Meanwhile, both of the compressor types can be united for the IR wavelengths
located in the vicinity of 1.3 μm, to yield high compressions that offer some prospects for
achieving the shortest possible pulses [22].
In 2008, Cirmi et al. [23] have used a complicated system to generate tunable few-optical-
cycle pulses via a non-collinear phase-matching geometry optical parametric amplifier (OPA).
Their construction contains two OPAs, the first of them delivering a phase-stable idler that
experiences spectral broadening through a 3 mm-thick sapphire plate to generate supercontinuum
spectra. The OPA is based on a BBO crystal enabling tunability of the output wavelength from 500
to 1600 nm by tuning the crystal angle. The main problem of the device is, however, that the pulse
energy does not exceed 5 J [24]. Three years later, the same authors have modified their system
and demonstrated a number of different OPA schemes which generate ultra-broadband pulses with
the tunable wavelength (1000–3000 nm) and the pulse duration 8.5 fs, although the pulse energy
has been 1–2 μJ only [25]. In 2012, J. Darginavicius et al. have demonstrated another
configurations with the tunable wavelength and the energy as high as 100 J. One of these
schemes works in the VIS range (530–720 nm) and the others can be tuned for the middle-IR and
the near-IR (λMIR = 1.6–7.2 μm and λNIR = 0.9–1.6 μm, respectively), depending on the operational
characteristics of the blue-pumped non-collinear phase-matching OPA. They have suggested using
different crystals (LiIO3, LiNbO3 or BBO) in the non-collinear phase-matching OPA systems to
enable differently tuned wavelength regions. Recently G. Cerullo et al. reported [26] on the
development of ultra-broadband tuneable few-optical-cycle lasers based on the other OPA
schemes. In this case the OPA system represents a so-called ‘degenerate’ OPA, in which the signal
and the idler have the same frequency, or a non-collinear OPA. These systems are pumped with
either fundamental frequency or second harmonics of an amplified Ti:sapphire laser (800 nm)
having the repetition rate of 1kHz. Tunability from the VIS to the IR is achieved with the crystals
having relatively high refractive indices (e.g., periodically poled stoichiometric lithium tantalate)

and different thicknesses (1–3 mm). Nonetheless, the authors of Ref. [27] have claimed that the
output pulse energy is still limited to the microjoule regime.
In this work, we suggest a new direct method for generating tuneable-bandwidth (from the
VIS to the near-IR) laser pulses of which energies reach a sub-millijoule range for the first time.
This is two orders of magnitude higher than the output of all the other complicated techniques
known up to date [23–27]. The characteristics reported above have been achieved by generating
super-continuum in a hollow fibre filled with neon gas. The wavelength tunability has been
controlled with the gas pressure. We have also studied the effect of varying chirping of the pulses
injected into the fibre on the bandwidth of the output pulses.
2. Experimental setup
An optical diagram of a table-top tunable ultrafast laser system is shown in Fig. 1. The
amplification stage includes a regenerative kHz amplifier that produces high-power femtosecond
pulses (2.5 W, 32 fs and the wavelength 800 nm). A 15 fs mode-locked Ti:sapphire seed oscillator
(400 mW and 75 MHz at 800 nm) generates femtosecond laser pulses in the TEM00 mode. The
basic oscillator setup consists of pump beam mirrors, folded cavity mirrors, a pump beam-focusing
lens, a pair of concave spherical mirrors aligned with the Ti:sapphire laser rod, an output coupler,
metal-coated mirrors, a set of prisms used for the dispersion compensation, and a slit as a spectral
tuning element.
The seed oscillator can be tuned from 780 to 820 nm. The oscillator is pumped by a green
CW diode-pumped solid-state laser Opus (4 W and 532 nm; available from Laser Quantum). Since
the output Ti:sapphire energy is limited to the nanojoule level, an additional amplification stage is
needed. We have selected the chirped-pulse amplification since it offers the pulse energies of the
order of millijoules at the kilohertz repetition rate [28]. It is worth noticing that the chirped-pulse
amplification applied to the ultrashort solid-state laser pulses can raise the powers of the generated
optical pulses up to gigawatt frontiers, thus making the technique favourite for the high-field lasers
and the ultrafast spectroscopy [29–32]. Before chirped-pulse amplifying, a stretcher is used for
stretching out the seed pulses temporally and spectrally in order to reduce the peak-power level
and avoid destruction of the gain medium [33]. A strongly dispersive element is employed in the
stretcher according to a standard two-path scheme, combining a single diffraction grating with a
telescope formed by a flat mirror and a spherical mirror equipped with broadband dielectric
coatings.
The chirped-pulse amplifier involves multiple passing through an amplifying gain medium
located within an optical resonator. The latter comprises an optical switch for controlling the
number of round trips and for reaching very high overall gains. The switch is composed of a
Pockels cell combined with a quarter-wave plate and a thin-film polarizer. A Faraday isolator is
used for separating the input and output pulses. It represents a passive optical device made of
magneto-optic material, which preserves the linear polarization of light and rotates its polarization
plane by 45° for the beam going in the forward direction and, due to a non-reciprocal character of
that rotation, by additional 45° for the backward direction.
After passing through a Faraday isolator and changing the polarization from horizontal to
vertical, the stretched pulses are injected into a regenerative amplifier at predetermined times,
using a Pockels cell as an optical switch. Then, after a necessary number of round trips in the
resonator, the energy of the laser pulse reaches its maximum value (higher than 3 mJ). The
amplified laser pulses are released from the regenerative-amplifier resonator by a second optical

switch (i.e., a second Pockels cell). That is done by applying short bell-shaped high-voltage pulses
to the Pockels cell that acts as a quarter-wave plate. The regenerative amplifier is pumped by a
diode-pumped Q-switched green pulse Nd:YLF laser (the wavelength 527 nm, the energy 20 mJ,
the duration 170 ns, and the repetition rate 1 kHz). It is a vertically polarized laser model DM20-
527 available from Photonics Industries.
Fig. 1. A schematic setup of our tunable ultrafast laser system: RTFP – thin-film polarizer, RW – Brewster
window, RPC – Pockels cells, RD – aperture, PD – photodiode, RC – Ti:sapphire crystal, GP – prism polarizer,
CG – compressor grating, and SG – stretcher grating.

Having passed the regenerative amplifier, the laser pulse is sent to a gate subsystem
consisting of two crossed polarizers and a third Pockels cell placed in between. This ‘pulse picker’
is employed to control the laser output by an external gate signal and to enhance the contrast.
Finally, the pulse is compressed back to the femtosecond regime via a compressor. To prevent any
damage of optical elements of the compressor, the beam is expanded by a telescope composed of
mirrors TT1 and TT2. The compressor itself involves an input mirror, a diffraction grating, a
mirror assembly, a ‘roof’ mirror assembly, and an output mirror CM4. The laser beam strikes the
grating four times inside the compressor. Behind the compressor, the laser pulses reach the
duration of 32 fs at the energy 2.5 mJ and the repetition rate 1 kHz. Then the amplified pulse is
directed to a final stage to produce the few-cycle pulse regime. We call this stage as a ‘hollow-
fibre compressor’. The mentioned compressor is composed of a one-metre hollow fibre filled with
a neon gas, followed by a multilayer chirped-mirror compressor. With the aid of a concave mirror
with the focal length f = 1.2 m, the laser radiation is focused into a fused-silica fibre with the inner
diameter 250 µm. The pulse spectrum gets broader via the self-phase modulation in the neon gas at
a controlled pressure (up to 2.5 atm). Finally, the output beam is collimated by a concave mirror
and then compressed after a six-path trip between the two chirped mirrors, thus reaching a few-
cycle regime.
3. Results and discussion
The oscillator beam has been optimized in a mode-locked regime at 95 nm and the bandwidth
52 nm. The full width at half maximum (FWHM) of the pulse is found to be 18 fs at the energy
4 nJ (see Fig. 2). The wavelength of the oscillator beam can be tuned in the wavelength region
750–850 nm, using a variable optical slit and a couple of prisms. The Ti:sapphire emission is
spread spatially and the wavelength can be tuned by varying the horizontal location and the width
of the slit. It is worthwhile that the narrow bandwidth of the gain medium used by us restricts
creating directly the few-cycle pulses. To avoid this fundamental limitation, we have employed an
external spectral broadening due to the hollow fibre and the consequent pulse compressor (see
Fig. 1). On the other hand, the amplified femtosecond pulses can be chirped in the compressor by
changing the separation distance between the gratings. Then the chirped output pulses have the
average power of 2.5 W at the repetition rate 1 kHz and the pulse energy 2.5 mJ.
-100 -80 -60 -40 -20 0 20 40 60 80 100
0
2
4
6
8
A(a.u.)
Delay time (fs)
Fig. 2. Autocorrelation data measured
for Ti:sapphire oscillator (18 fs at
795 nm, and the bandwidth 47 nm). A is
the intensity.

Reconstructed Pulse IAC
Delay (fs)
1000-100
A(a.u.)
8.0
7.5
7.0
6.5
6.0
5.5
5.0
4.5
4.0
3.5
3.0
2.5
2.0
1.5
1.0
0.5
0.0
9.36 fs
Fig. 3. Output-pulse profile estimated using the intensity autocorrelation function: the FWHM value measured
(9.36 fs) corresponds to the transformed limited pulses as short as 4.6 fs. IAC is the intensity autocorrelation
function.
The properties of the ultrafast pulses at the output of our system are affected by
many parameters, including the nonlinear phase shift due to generation of supercontinuum in
the hollow fibre filled with neon gas, the pressure of that gas, and the efficiency of
the regenerative-amplifier output. The final compressed pulses are found to reach the energies
as high as 0.6 mJ at the repetition rate 1 KHz. Fig. 3 shows the autocorrelated intensity
function for the ultrafast output, which has been measured with a so-called spectral
phase interferometry for direct electric-field reconstruction. As seen from Fig. 3, the FWHM
of the pulses is found to be 9.34 fs, which corresponds to the transformed limited pulses as short as
4.6 fs [34].
We have also studied the effect of varying amplified-pulse chirping (from 32 fs to
almost 56 fs) on the final output of the system, under conditions of different neon pressures. Fig. 4
shows the variations in the output-pulse bandwidth and the peak wavelength occurring when
the input-pulse chirping changes from 32to54 fs. Here the Ne pressure is kept fixed at
2.00atm. The peak intensities are observed at the wavelengths 701–728nm and the
bandwidth changes from 30.16 to 194.18nm. We have found that, under the given pressure, the
position of the peak intensity is approximately fixed at 710 nm, with only slight changes of the
order of ±2%. On the contrary, the bandwidth changes by almost 6.5 times when the incident-pulse
chirping increases from 32 to 54 fs.

Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 710 nm
30.16 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 701 nm
55.69 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 728 nm
137.85 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 702 nm
194.18 nm
Fig. 4. Output-pulse bandwidths and peak wavelength measured for the cases of different input-pulse chirping
(a neon-filled hollow-core fibre at the pressure 2.00 atm): (A) 32, (B) 44, (C) 47 and (D) 54 fs. S is the spectral
intensity.
Fig. 5 shows variations in the bandwidth of the output pulse and its peak wavelength, which
take place due to changing chirping of the input pulse (from 32 to 54 fs) under somewhat higher
neon pressure, 2.25 atm, inside the hollow fibre. The peak intensities are again located in the
wavelength region 701–728 nm and, as in case of the pressure 2.00 atm, the bandwidth changes
from 30.16 to 194.18 nm.
A
B
C
D

Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 718 nm
23.03 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 712 nm
27.29 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 701 nm
173.14 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 707.56 nm
184.5 nm
Fig. 5. Output-pulse bandwidths and peak wavelengths measured for the cases of different input-pulse chirping
(a neon-filled hollow-core fibre at the pressure 2.25 atm): (A) 32, (B) 47, (C) 50 and (D) 53 fs.
Finally, we have found that the bandwidths of the output pulses are much wider at still higher
neon pressure (2.50 atm), as compared with the parameters obtained at 2.00 or 2.25 atm. Fig. 6
shows that the output bandwidth starts with 72.75 nm at the input-pulse chirping 32 fs and
increases up to 234.2 nm at 54 fs. In this case the peak intensity is demonstrated to be
approximately fixed near 707 nm, with only a small relative variation (0.5%). Notice that the
bandwidth becomes very broad (almost 250 nm), beginning from the wavelength of 650 nm and
ending at 900 nm (see Fig. 6).
A
B
C
D

Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 707.56 nm
72.75 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 714 nm
161.25 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 702 nm
162.63 nm
Wavelength (nm)
950900850800750700650600
S(a.u.)
1.0
0.8
0.6
0.4
0.2
0.0 711 nm
234.22 nm
Fig. 6. Output-pulse bandwidths and peak wavelengths measured for the vases of different input-pulse chirping
(a neon-filled hollow-core fibre at the pressure 2.50 atm): (A) 32, (B) 37, (C) 47 and (D) 54 fs.
4. Conclusion
Summing up the main results of the present work, we have demonstrated a new table-top setup and
a corresponding technique that enable producing tunable, broad-band, ultrafast, few-cycle optical
pulses in the wavelength region 600–950 nm. The pulses achieve high enough energies close to the
sub-millijoule frontiers at the repetition rate 1 kHz. Notice that these characteristics have been
obtained for the first time and with relatively simple methods. Our scheme reveals the ability to
control the bandwidth from 23 to almost 250 nm. Our results seem to be very important since they
facilitate a sufficient wavelength tunability greatly needed while investigating the transient
A
D
C
B

interactions of ultrafast pulses with different molecular-energy states. Moreover, the ultrafast
tunable pulses can turn out to be very useful in generation of higher optical harmonics, which can
be further used to create shorter pulses in the attosecond regime with shorter wavelengths covering
the UV-to-X-ray range.
Acknowledgement
This project was funded by the National Plan for Science, Technology and Innovation
(MAARIFAH), King Abdulaziz City for Science and Technology, Kingdom of Saudi Arabia,
under the Award Number 12-ELE2628-02.
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Анотація. У цій роботі представлено новий метод керування шириною смуги пропускання
оптичних імпульсів тривалістю у кілька періодів із використанням додаткових частотно
модульованих фемтосекундних лазерних імпульсів, які поширюються крізь волокно з
серцевиною, заповненою неоном. Показано, що ширина смуги пропускання змінюється від
25 до 234 нм для оптичного діапазону 600–950 нм, а енергія імпульсу сягає суб-
міліджоулевої межі при 1 кГц. На вході волокна імпульси модулювали за частотою у
прямому напрямку від 32 до 56 фс. Після цього імпульси ставали суттєво диспергованими
самомодуляцією в нелінійному середовищі (газі неону), а після нього слідувала пара
модульованих дзеркал, які компенсували дисперсію. Виявлено, що ця схема дає змогу прямо
перестроювати ширину смуги пропускання вихідного імпульсу шляхом зміни модуляції
вхідних імпульсів при різних тисках газу. Одержані результати вказують на можливість
контролю взаємодій у сильних електричних полях за умови надшвидких процесів і мають
вирішальне значення для відновлення аттосекундних рентгенівських імпульсів.

A method for controlling the bandwidth of high energy, fewoptical-cycle

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A method for controlling the bandwidth of high energy, fewoptical-cycle