Lanthanum titanate glasses (17 La2O3-83 TiO2) are fabricated via aerodynamic levitation melting. Nonlinear refraction and absorption were measured with the Z scan technique using 550 ps optical pulses at 532 nm wavelength with peak intensities in the range of 0.25–2.5 GW/cm2. The two-photon absorption coefficient (β) and the effective nonlinear refraction coefficient ( n 2 eff) are found to be, respectively, 2.19 cm/GW and 152 × 10−16 cm2/W (85 × 10−13 esu). The Raman gain is measured to be 106 × 10−11 cm/W. The nonlinearity strength is found to be nearly 60 times larger in lanthanum titanate glasses relative to silica.

1.
R.
Weber
,
S. K.
Wilke
, and
C. J.
Benmore
, “
Containerless techniques for in-situ X-ray measurements on materials in extreme conditions
,”
J. Phys. Soc. Jpn.
91
,
091008
(
2022
).
2.
J.
Weber
,
C.
Benmore
,
L.
Skinner
,
J.
Neuefeind
,
S.
Tumber
,
G.
Jennings
,
L.
Santodonato
,
D.
Jin
,
J.
Du
, and
J.
Parise
, “
Measurements of liquid and glass structures using aerodynamic levitation and in-situ high energy X-ray and neutron scattering
,”
J. Non-Cryst. Solids
383
,
49
51
(
2014
).
3.
A.
Masuno
, “
Functionalities in unconventional oxide glasses prepared using a levitation technique
,”
J. Ceram. Soc. Jpn.
130
,
563
574
(
2022
).
4.
D.
Möncke
,
B.
Topper
, and
A. G.
Clare
, “
Glass as a state of matter-the ‘newer’ glass families from organic, metallic, ionic to non-silicate oxide and non-oxide glasses
,”
Rev. Mineral. Geochem.
87
,
1039
1088
(
2022
).
5.
D.
Moncke
,
F.
Lind
,
B.
Topper
, and
E. I.
Kamitsos
, “
Anomalous deformation behavior in ULE glass upon microindentation: A vibrational spectroscopic investigation in the induced structural changes of a Ti-silicate glass
,”
J. Phys. Chem. C
125
,
4183
4195
(
2021
).
6.
H.
Kozuka
,
R.
Ota
, and
N.
Soga
, “
Preparation and properties of binary oxide glasses containing rare earth oxides
,”
J. Soc. Mater. Sci., Jpn.
35
,
73
79
(
1986
).
7.
O. L.
Alderman
,
C. J.
Benmore
,
A.
Tamalonis
, and
R.
Weber
, “
Rare-earth titanate melt structure and glass formation
,”
Int. J. Appl. Glass Sci.
10
,
463
478
(
2019
).
8.
S.
Wilke
,
A.
Al-Rubkhi
,
C.
Koyama
,
T.
Ishikawa
,
H.
Oda
,
B.
Topper
,
E.
Tsekrekas
,
D.
Möncke
,
O. L.
Alderman
,
V.
Menon
,
J.
Rafferty
,
E.
Clark
,
A. L.
Kastengren
,
C. J.
Benmore
,
J.
Ilavsky
,
J.
Neuefeind
,
S.
Kohara
,
M.
SanSoucie
,
B.
Phillips
, and
R.
Weber
, “
Microgravity effects on nonequilibrium melt processing of neodymium titanate: Thermophysical properties, atomic structure, and glass formation
” Micrograv. (in press) (
2023
).
9.
A.
Masuno
,
Y.
Watanabe
,
H.
Inoue
,
Y.
Arai
,
J.
Yu
, and
M.
Kaneko
, “
Glass-forming region and high refractive index of TiO2-based glasses prepared by containerless processing
,”
Phys. Status Solidi C
9
,
2424
2427
(
2012
).
10.
B.
Topper
,
S. K.
Wilke
,
M.
Pettes
,
A.
Alrubkhi
,
V.
Menon
,
A.
Neumann
,
D.
Möncke
,
R.
Weber
, and
A.
Mafi
, “
Mid-infrared luminescence properties of erbium and dysprosium doped lanthanum titanate glasses
,”
Opt. Mater. Express
13
,
2857
2868
(
2023
).
11.
X.
Pan
,
J.
Yu
,
Y.
Liu
,
S.
Yoda
,
H.
Yu
,
M.
Zhang
,
F.
Ai
,
F.
Jin
, and
W.
Jin
, “
Thermal, mechanical, and upconversion properties of Er3+/Yb3+ co-doped titanate glass prepared by levitation method
,”
J. Alloys Compd.
509
,
7504
7507
(
2011
).
12.
A.
Darafsheh
,
G. F.
Walsh
,
L.
Dal Negro
, and
V. N.
Astratov
, “
Optical super-resolution by high-index liquid-immersed microspheres
,”
Appl. Phys. Lett.
101
(
14
),
141128
(
2012
).
13.
S.
Yoda
,
W.-S.
Cho
, and
R.
Imai
, “
Aerodynamic levitator for large-sized glassy material production
,”
Rev. Sci. Instrum.
86
(
9
),
093906
(
2015
).
14.
J. R.
Weber
,
J. J.
Felten
,
B.
Cho
, and
P. C.
Nordine
, “
Glass fibres of pure and erbium or neodymium-doped yttria-alumina compositions
,”
Nature
393
,
769
771
(
1998
).
15.
Z.
Mao
,
C.
Wang
,
X.
Zheng
,
J.
Yu
, and
L.
Xiong
, “
Optical properties, thermal stability, and forming region of high refractive index La2O3-TiO2-Nb2O5 glasses
,”
J. Am. Ceram. Soc.
101
,
1500
1507
(
2018
).
16.
V.
Dimitrov
and
T.
Komatsu
, “
Electronic polarizability, optical basicity and non-linear optical properties of oxide glasses
,”
J. Non-Cryst. Solids
249
,
160
179
(
1999
).
17.
Z.
Shi
,
N.
Dong
,
D.
Zhang
,
X.
Jiang
,
G.
Du
,
S.
Lv
,
J.
Chen
,
J.
Wang
, and
S.
Zhou
, “
Transparent niobate glass-ceramics for optical limiting
,”
J. Am. Ceram. Soc.
102
,
3965
3971
(
2019
).
18.
B.
Topper
,
N. S.
Tagiara
,
D.
Palles
,
F.
Lind
,
M.
Baazouzi
,
M. T.
Soltani
,
L.
Wondraczek
,
D.
Möncke
, and
E. I.
Kamitsos
, “
Second-harmonic generation and structural rearrangements in multicomponent antimonite glasses by electrothermal poling
,”
J. Am. Ceram. Soc.
106
,
4163
4180
(
2023
).
19.
C.
Strutynski
,
F.
Calzavara
,
T.
Guerineau
,
L.
Loi
,
R.
Laberdesque
,
J.-M.
Rampnoux
,
S.
Morency
,
Y.
Ledemi
,
Y.
Petit
,
M.
Dussauze
et al, “
Heavy-oxide glasses with superior mechanical assets for nonlinear fiber applications in the mid-infrared
,”
Opt. Mater. Express
11
,
1420
1430
(
2021
).
20.
A.
Masuno
,
Y.
Kikuchi
,
H.
Inoue
,
J.
Yu
, and
Y.
Arai
, “
Giant second harmonic generation from metastable BaTi2O5
,”
Appl. Phys. Express
4
,
042601
(
2011
).
21.
F.
Miyaji
,
K.
Tadanaga
, and
S.
Sakka
, “
Third harmonic generation from MOx-PbO-GaO1.5 ternary glasses
,”
Appl. Phys. Lett.
60
,
2060
2061
(
1992
).
22.
S.
Le Boiteux
,
P.
Segonds
,
L.
Canioni
,
L.
Sarger
,
T.
Cardinal
,
C.
Duchesne
,
E.
Fargin
, and
G.
Le Flem
, “
Nonlinear optical properties for TiO2 containing phosphate, borophosphate, and silicate glasses
,”
J. Appl. Phys.
81
(3),
1481
1487
(
1997
).
23.
M.
Dussauze
and
T.
Cardinal
, “
Nonlinear optical properties of glass
,” in
Springer Handbook of Glass
(
Springer Nature
,
2019
), pp.
193
225
.
24.
J.
Sabadel
,
P.
Armand
,
D.
Cachau-Herreillat
,
P.
Baldeck
,
O.
Doclot
,
A.
Ibanez
, and
E.
Philippot
, “
Structural and nonlinear optical characterizations of tellurium oxide-based glasses: TeO2-BaO-TiO2
,”
J. Solid State Chem.
132
,
411
419
(
1997
).
25.
X.
Feng
,
Z.
Shi
,
J.
Chen
,
T.
Yu
,
X.
Jiang
,
G.
Du
,
J.
Qiu
, and
S.
Zhou
, “
All-inorganic transparent composite materials for optical limiting
,”
Adv. Opt. Mater.
8
,
1902143
(
2020
).
26.
R.
Adair
,
L.
Chase
, and
S. A.
Payne
, “
Nonlinear refractive-index measurements of glasses using three-wave frequency mixing
,”
J. Opt. Soc. Am. B
4
,
875
881
(
1987
).
27.
M.
Lines
, “
Influence of d orbitals on the nonlinear optical response of transparent transition-metal oxides
,”
Phys. Rev. B
43
,
11978
(
1991
).
28.
Y.
Watanabe
,
M.
Ohnishi
, and
T.
Tsuchiya
, “
Measurement of nonlinear absorption and refraction in titanium dioxide single crystal by using a phase distortion method
,”
Appl. Phys. Lett.
66
,
3431
3432
(
1995
).
29.
S. K.
Wilke
,
O. L.
Alderman
,
C. J.
Benmore
,
J.
Neuefeind
, and
R.
Weber
, “
Octahedral oxide glass network in ambient pressure neodymium titanate
,”
Sci. Rep.
12
,
8258
(
2022
).
30.
K.
Maruyama
,
Y.
Arai
,
S.
Sato
,
M.
Sanada
,
T.
Otomo
,
K.
Suzuya
, and
K.
Itoh
, “
Neutron diffraction study of isotope enriched glassy Sm4Ti9O24
,” in
Proceedings of the 2nd International Symposium on Science at J-PARC-Unlocking the Mysteries of Life, Matter and the Universe
(The Physical Society of Japan,
2015
), p.
031007
.
31.
Y.
Arai
,
K.
Itoh
,
S.
Kohara
, and
J.
Yu
, “
Refractive index calculation using the structural properties of La4Ti9O24 glass
,”
J. Appl. Phys.
103
(
9
),
094905
(
2008
).
32.
J. R.
Weber
, “
The containerless synthesis of glass
,”
Int. J. Appl. Glass Sci.
1
,
248
256
(
2010
).
33.
M.
Sheik-Bahae
,
A. A.
Said
, and
E. W.
Van Stryland
, “
High-sensitivity, single-beam n2 measurements
,”
Opt. Lett.
14
,
955
957
(
1989
).
34.
S.
Divya
,
V.
Nampoori
,
P.
Radhakrishnan
, and
A.
Mujeeb
, “
Electronic and optical properties of TiO2 and its polymorphs by Z-scan method
,”
Chin. Phys. B
23
,
084203
(
2014
).
35.
N.
Vermeulen
,
D.
Espinosa
,
A.
Ball
,
J.
Ballato
,
P.
Boucaud
,
G.
Boudebs
,
C. L.
Campos
,
P.
Dragic
,
A. S.
Gomes
,
M. J.
Huttunen
et al, “
Post-2000 nonlinear optical materials and measurements: Data tables and best practices
,”
J. Phys.: Photonics
5
,
035001
(
2023
).
36.
G.
Tsigaridas
,
M.
Fakis
,
I.
Polyzos
,
P.
Persephonis
, and
V.
Giannetas
, “
Z-scan technique through beam radius measurements
,”
Appl. Phys. B
76
,
83
86
(
2003
).
37.
G.
Boudebs
,
V.
Besse
,
C.
Cassagne
,
H.
Leblond
, and
C. B.
de Araújo
, “
Nonlinear characterization of materials using the D4σ method inside a Z-scan 4f-system
,”
Opt. Lett.
38
,
2206
2208
(
2013
).
38.
E. W.
Van Stryland
and
M.
Sheik-Bahae
, “
Z-scan
,” in
Characterization Techniques and Tabulations for Organic Nonlinear Optical Materials
(
Routledge
,
2018
), pp.
671
708
.
39.
E.
Van Stryland
,
M.
Sheik-Bahae
,
A.
Said
, and
D.
Hagan
, “
Characterization of nonlinear optical absorption and refraction
,”
Prog. Cryst. Growth Charact. Mater.
27
,
279
311
(
1993
).
40.
M.
Sheik-Bahae
,
A. A.
Said
,
T.-H.
Wei
,
D. J.
Hagan
, and
E. W.
Van Stryland
, “
Sensitive measurement of optical nonlinearities using a single beam
,”
IEEE J. Quantum Electron.
26
,
760
769
(
1990
).
41.
S.
Solin
and
A.
Ramdas
, “
Raman spectrum of diamond
,”
Phys. Rev. B
1
,
1687
(
1970
).
42.
Y.
Zhao
,
K.
Kita
,
K.
Kyuno
, and
A.
Toriumi
, “
Band gap enhancement and electrical properties of La2O3 films doped with Y2O3 as high-k gate insulators
,”
Appl. Phys. Lett.
94
(
4
),
042901
(
2009
).
43.
D. N.
Christodoulides
,
I. C.
Khoo
,
G. J.
Salamo
,
G. I.
Stegeman
, and
E. W.
Van Stryland
, “
Nonlinear refraction and absorption: Mechanisms and magnitudes
,”
Adv. Opt. Photonics
2
,
60
200
(
2010
).
44.
S.
Santran
,
L.
Canioni
,
L.
Sarger
,
T.
Cardinal
, and
E.
Fargin
, “
Precise and absolute measurements of the complex third-order optical susceptibility
,”
J. Opt. Soc. Am. B
21
,
2180
2190
(
2004
).
45.
R. H.
Stolen
,
C.
Lee
, and
R.
Jain
, “
Development of the stimulated Raman spectrum in single-mode silica fibers
,”
J. Opt. Soc. Am. B
1
,
652
657
(
1984
).
46.
J.
Jackson
,
C.
Smith
,
J.
Massera
,
C.
Rivero-Baleine
,
C.
Bungay
,
L.
Petit
, and
K.
Richardson
, “
Estimation of peak Raman gain coefficients for Barium-Bismuth-Tellurite glasses from spontaneous Raman cross-section experiments
,”
Opt. Express
17
,
9071
9079
(
2009
).
47.
C.
Rivero
,
R.
Stegeman
,
M.
Couzi
,
D.
Talaga
,
T.
Cardinal
,
K.
Richardson
, and
G.
Stegeman
, “
Resolved discrepancies between visible spontaneous Raman cross-section and direct near-infrared Raman gain measurements in TeO2-based glasses
,”
Opt. Express
13
,
4759
4769
(
2005
).
You do not currently have access to this content.