DFG-based mid-IR laser system for muounic-hydrogen spectroscopy

Lyubomir I. Stoychev*a,b, Miltcho B. Danailovc, Alexander A. Demidovichc, Ivaylo P. Nikolovc,

Paolo Cinquegranac, Paolo Sigalottic, Dimitar Bakalovd, Andrea Vacchia
a
Istituto Nazionale di Fisica Nucleare, Padriciano 99, AREA Science Park, 34149 Trieste, Italy;
b
The Abdus Salam International Centre for Theoretical Physics, Strada Costiera 11, 34151 Trieste,
Italy; cElettra-Sincrotrone Trieste S.C.p.A., SS14, Km 163.5, 34149 Basovizza, Trieste Italy,
d
Institute for Nuclear Research and Nuclear Energy, 72 Tzarigradsko chaussee, 1784 Sofia, Bulgaria

ABSTRACT

The goal of this work is to prove the feasibility of building a laser system that can generate mid-infrared radiation with
the parameters required for the measurement of the hyperfine splitting in the ground state of the mounic hydrogen
spectroscopy.

The first experimental results of a very straightforward scheme that, to our knowledge, has not been considered in the
literature, are presented. We study a laser test bench system emitting nanosecond pulses of infrared tunable radiation in
the spectral range 6.78 m with high energy and narrow line-width, based on direct difference frequency generation
(DFG), in non-oxide nonlinear crystals, using as pump lasers a single-mode Nd:YAG laser and tunable narrow-
bandwidth Cr:forsterite laser.

The investigated system is based on lithium thioindate (LiInS2) and silver thiogallate (AgGaS 2) crystals cut for type II
difference frequency generation. The pulses of the Nd:YAG laser (1,064 m) are combined with the pulses at ~ 1.262
m of the Cr:forsterite laser through a dichroic mirror and sent to the nonlinear crystals in different optical geometries.
The generated radiation reaches an output energy up to 80 J in a single pass optical geometry, has 10 ns long pulses at
50 Hz frequency repetition rate and is tunable in the range 6595 6895 nm. These first results prove the suitability of
such an approach for building the laser system for the muonic-hydrogen experiment.

Keywords: DFG, tunable mid-infrared radiation, mounic-hydrogen, nonlinear optcis, nonlinear crystals, LiInS2 crystals.

1. INTRODUCTION

The so-called proton radius puzzle is among the challenging problems that fundamental physics is facing 1,2. A promising
approach based on high precision spectroscopy of muonic hydrogen 3, is to determine the proton Zemach radius. The
accurate knowledge of the Zemach radius of the proton provides an efficient tool for testing quantitatively the models of
the proton structure. In comparison to the r.m.s. proton charge radius the Zemach radius has the important feature to be
sensitive also to the magnetic dipole moment distribution. In particular the measurement of the Zemach radius with an
uncertainty less than 0.5 % would impose independent experimental bounds on the low momentum transfer limit of the
proton charge to magnetic form factors ratio4. Further on, comparing the values of Zemach radius obtained in normal and
muonic hydrogen might also help to resolve the puzzle with the apparent discrepancy between the values of the r.m.s.
charge radius of the proton2.

The basic outline of the muonic-hydrogen experiment is as follows. To produce the muonic hydrogen an intense, low
energy pulsed muon beam will be brought to stop in a pressurized hydrogen gas target. The muon beam pulses have a
repetition rate of 50 Hz and a pulse duration of 70 ns. Measuring the energy difference ( 3S1-1S0) in the muonic hydrogen
requires a pulsed nanosecond mid-IR laser source tunable around 67853 nm, with linewidth less than 0.07 nm and
energy output of about 1 mJ at the same repetition rate.
* lyubomir.stoychev@ts.infn.it

Laser Sources and Applications II, edited by Jacob I. Mackenzie, Helena Jelnkov, Takunori Taira, Marwan Abdou Ahmed,
Proc. of SPIE Vol. 9135, 91350J 2014 SPIE CCC code: 0277-786X/14/$18 doi: 10.1117/12.2052110

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 The rapid development of the mid-infrared lasers finds its motivations in the many potential applications that these
sources find in the fields of spectroscopy, remote gas sensing, medicine, etc. There are a numerous mid-infrared sources
available today like solid state lasers, gas lasers, laser systems using frequency conversion and quantum cascade lasers
(QCL). Among them the suitable candidates to produce tunable mid-infrered radiation are the QCLs and the frequency
conversion systems. While the QCLs are stable and simple to operate, tunable over the wavelength range ~ 6.8 m and
have very narrow linewidths5, their application for the muonic hydrogen experiment is limited by the insufficient energy
output. On the other side the frequency conversion based laser sources using parametric processes have the advantage of
high obtainable energies but the emitted radiation is very broad and usually spreads over several nanometers. Exception
is the radiation emitted through DFG schemes which have relatively lower output energies but can be with narrower line-
widths.

It is possible to find in the literature reports of pulsed DFG lasers reaching and even exceeding the requested 1 mJ in the
6.78 m range6,7,8,9, and others reporting line-widths not far from the requested 0.07 nm at the wavelength needed for the
muonic hydrogen experiment10,11. Though the generation of pulses having the combination of parameters needed for the
muonic hydrogen experiment has not been demonstrated, it seems to be within the reach by the present nonlinear optics
(NLO) sources and materials.

A rich variety of NLO based schemes can be used to generate 6.8 m light. The different approaches can be grouped in
one stage or two stage processes. An examples for one stage process is DFG generation in non-oxide crystals with pump
and signal coming from one narrow-band nanosecond fixed wavelength and one tunable solid state lasers emitting at
wavelengths below 2 m. Another possibility is an optical parametric oscillator (OPO) pumped in the 1m region using
non-oxide crystals with relatively low effective nonlinearity 12. Two stage process could be two-stage parametric
amplifier, pumped by a femtosecond Ti:Sapphire amplifier, based on travelling wave amplification in BIBO (nonlinear
crystal) generating signal wave at 1.399 m and idler at 1.763 m. Then, the 6.78 m will be generated by performing
DFG of the signal and idler, applying a strong phase-modulation leading to a stretching of the pulses and narrowing of
the spectrum. An other approach for two-stage scheme is nanosecond OPO (based on oxide crystals) with pump still in
the 1 m YAG region generating an idler wavelength above 2 m which is in the transparency range of nonlinear
crystals with higher nonlinearity13. The second stage then uses one of this crystals, like e.g. ZGP 7 for generating the mid-
IR pulses in the 6.78 m region based OPA/OPO pumped by the first OPA (seeded by a narrow-line QCL).

2. SETUP AND INSTRUMENTATION

The layouts of the tested system are shown on Fig.1 and Fig.2. These schemes are based on direct difference frequency
generation using a fixed wavelength (1.064 m) single-mode diode pump Nd:YAG laser (LS-2139DP - LOTIS TII), with
frequency repetition rate 50 Hz, 10 ns pulse length, 0.5 ns jitter and a tunable narrow line-width Cr:forsterite
(Mg2SiO4:Cr4+) laser (LT-2212G-100 - LOTIS TII) pumped by a second Nd:YAG synchronised to the first one. A lamp
pumped Q-switched Nd:YAG laser (LS-2138 - LOTIS TII) with output energy of 150 mJ, pulse duration 10 ns, pulse
repetition rate 50 Hz, jitter 1.2 ns is used to pump the Cr:forsterite laser. The latter contains a diffraction grating as an
output coupler, allowing to obtain tunable light in the 1.200-1.280 m range with an energy per pulse of up to 15 mJ and
a line-width of about 8-10 pm for 15 ns long pulses at 50 Hz frequency repetition rate. Its pulses are then combined with
the pulses at 1.064 m of the diode-pumped YAG (Nd:YAG2 on the figures) through a dichroic mirror and sent to the
nonlinear crystals in a single pass and double pass geometries respectively. The two lasers are triggered through a delay
generator - 4 channel, 1 ps resolution, less than 10 ps RMS typical jitter, (Highland Technology, P400) - allowing to
compensate the build-up time of the Cr:forsterite pulse and had a relative timing jitter below 1ns.

Among the big variety of non linear crystals suitable for the generation of infrared radiation tunable around 6.8 m our
first studies are concentrated on AgGaS 2 and LiInS2 crystals due to the relatively high damage thresholds and
nonlinearities of these two crystals. The nonliner crystals were studied in Type II DFG. The AgGaS 2 crystals are cut for
Type II difference frequency mixing of 1.064 m and 1.262 m for generation of 6.780 m, cutting angle Theta/=44.6
deg. The LiInS2 crystals are cut for Type II difference frequency mixing of 1.064 m and 1.262 m for generation of
6.780 m, cutting angle Theta/=90 deg, Phi/=35.5 deg, cut in the XY plane. All crystals studied are with anti-
reflection (AR) coatings at 1.06 m & 1.26 m on the front side and AR coating at 6.8 m on the back side,
respectively.

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 Pump BD
beams
M5 DC NL
BS Power
T2 Idler
Sync beam meter
Nd:YAG2 CaF2
device Prism
M4
Power Wavelength
meter
meter
WP Pol T1
M1 BS

Nd:YAG1 Cr:
BS M3
forsterite
M2
Spectro Power
graph meter

Figure 1. DFG scheme for generating 6.8m: WP - waveplate, Pol - polarizer, M1-M5 - mirrors, T1 and T2 - matching telescopes,
BS - beamsplitters, DC - dichroic mirror (reflecting 1.26m, transmitting 1.06m , NL - nonlinear crystal

T2 M6
M4
Sync NL
Nd:YAG 2
device DC 1
Power DC 2
meter M5
BS
WP Pol T1 Wavelength
M1 BS
meter
Nd:YAG 1 BS Cr:forsterite M3
Energy
M2 meter
Spectro Power
graph meter

Figure 2. Double pass DFG scheme: WP - waveplate, Pol - polarizer, M1-M6 - mirrors, T1 and T2 - telescopes, BS beamsplitters,
DC1 - dichroic mirror (reflecting 1.26m, transmitting 1.06m), DC2 - dichroic mirror(reflecting 1.06 and 1.26 m, transmitting
6.76m)

3. RESULTS AND DISCUSSION

The DFG schemes, though having relatively smaller conversion efficiency, have the advantage (compared to OPO, OPA
and OPG) of much narrower line-width which is of crucial importance for the final experiment. The nonlinear crystals
under study, AgGaS2 and LiInS2, are 5 mm long with different cross-section dimensions, all commercially available. The
purpose was to test the output energies and the crystals' damage thresholds.

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 In order to obtain generation at 6.78 m the radiation at 1.064 m from the single-mode Nd:YAG laser was mixed with
radiation from the Cr:forsterite at ~ 1.262 m. Initially the output beams of both lasers (Nd:YAG and Cr-forsterite) were
adjusted to a diameter 3.6 mm (~10 mm 2). The total energy applied on the crystals was 30 mJ (22 mJ from Nd:YAG and
8 mJ from Cr:forsterite, respectively), with total power density 29.48 MW/cm 2, (21.62 MW/cm2 for the 1.06 m and 7.86
MW/cm2 for 1.26 m). This was done in order to avoid damaging of the crystals, whose damage thresholds were found
to be over 30 MW/cm 2 at 1.06 m, and much higher (over 100 MW/cm 2) for the 1.26 m. Under these conditions from
the LiInS2 crystals an output energy of ~ 7.5 J at 6.76 m was generated with pulse length ~ 10 ns in the single pass
geometry configuration (Fig.1). Under the same working conditions for the AgGaS 2 crystal an output of 0.8 J was
reached. As a second step the same optical scheme geometry was used with two nonlinear crystals of the same type put
in sequence. In this configuration with the LiInS 2 crystals an energy up to 25 J was generated and 3 J from the
AgGaS2.

In a subsequent iteration the geometrical arrangement of the layout was modified in order to investigate the effect of the
double pass of the laser beams through the crystals on the energy generated at 6.78 m (see Fig.2). In such a
configuration with two LiInS2 crystals, each long 5 mm, the energy of the mid-infrared emission increased up to ~ 40 J,
which compared to the 25 J obtained in the single pass geometry under the same conditions is an increase of the 60% of
the energy at 6.78 m .

Keeping the same output energies of both lasers (Nd:YAG and Cr:forsterite) and decreasing both beam sizes to 3.3 mm,
thus increasing the power densities to 25.73 MW/cm 2 and 9.36 MW/cm2 respectively, an output of 35 J was reached in
the scheme with single pass geometry with LiInS 2 crystals. Further decreasing both beam diameters to 3.0 mm and thus
increasing the power densities to 31.12 MW/cm2 and 11.32 MW/cm2 respectively, an energy of 80 J was generated in
the single pass geometry. No damages were observed neither in the bilk of the crystals' nor on the coatings even at
prolonged exposures (for the cases when the diameters of the pumping beams were 3 mm).

Very big advantage of the configuration described here is that it allows us to obtain an easy and fast tuning of the mid-
infrered radiation in the spectral range 6.68 m 6.88 m without changing neither the triggering between the two pump
beams nor the angle of incidence of the beams on the nonlinear crystals. This tunability was achieved only by varying
the angle of the output diffraction grating of the Cr:forsterite laser and thus changing the output wavelength of the
Cr:forsterite emission from 1265.58 nm to 1268.65 nm. The change of the mid-infrared output energy with the
wavelength of the difference frequency generated emission is presented at Fig.3. Here the angle of incidence on the
LiInS2 crystals was optimized for maximum energy output at 6770nm.

40

35

30

25
E n e r g y , J

20

15

10

6680 6700 6720 6740 6760 6780 6800 6820 6840 6860 6880
W a v e le n g th , n m

Figure 3. Energy output of the emitted radiation from two LiInS 2 placed in sequence vs the wavelength.

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 4. SUMMARY AND CONCLUSIONS

We demonstrate a simple and robust scheme of optical system for generation of mid-infrared radiation in the spectral
region 6.78 m, that allows fast and easy tunning of the output emission wavelength. The laser system studied has been
based on difference frequency generation in LiInS 2 and AgGaS2 crystals by mixing fixed wavelength single-mode diode
pump Nd:YAG laser at 1.064 m with the radiation of tunable narrow linewidth Cr:forsterite (Mg 2SiO4:Cr4+) laser
emitting in at ~ 1.262 m. With two 5mm long LiInS 2 crystals put in sequence an output energy of up to 80 J was
obtained at wavelength 6.76 m, with pulse length ~ 10 ns and 50 Hz pulse repetition rate. The mid-infrared emission of
the system was tunable in the spectral range 6.68 m - 6.88 m by only changing the output wavelength of the
Cr:forsterite laser. Tested under identical conditions the energy generated using the AgGaS 2 crystals was much lower
than the one form the LiInS2 crystals. Using the nonlinear crystals in scheme with double pass geometry will allows to
obtain increase of the energy output of 60 %.

The results obtained show that through rather straightforward scaling of the laser system by keeping the power densities
at the present levels (below the damage thresholds of the crystals) and using multiple larger size nonlinear crystals of the
same type, it is possible to achieve laser generation of pulses with the combination of parameters requested for the
muonic hydrogen experiment. With commercially available laser systems (both Nd:YAG and Cr:forsterite) and LiInS2
crystals it is possible to obtained from single bulk crystal pulsed nanosecond laser light at 6.78 m with higher energies
than the requested 1 mJ and linewidths of the emitted mid-IR radiation in the order of 200 MHz. The possibility to use
more than one nonlinear crystal in optical sequence and the double pass scheme shall allow to reach even higher power
densities.

ACKNOWLEDGEMENTS

The authors are very grateful to the International Society for Optics and Photonics (SPIE) for the continuous support of
this work through its Anchor Research Program at ICTP. We would also like to thank to the The Abdus Salam
International Centre for Theoretical Physics (ICTP). The work presented was financed by the board 3 of the Italian
Natiional Institute for Nuclear Physics under the FAMU project.

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