We investigate the linear optical properties of RbxK1xTiOPO4 alloy crystals (x = 0, 0.25, 0.5, 0.75, 1) in the framework of the Bethe–Salpeter approach and the second-order optical response of these crystals within the independent particle approximation. The independent particle spectrum of KTiOPO4 (KTP) shows that this crystal absorbs light in the near-UV region. By solving the full Bethe–Salpeter equation, it is seen that the excitonic effects lead to an overall increase of the intensity and a redshift of about 1.6 eV in the absorption onset from the near-UV region to the visible region, reflecting the significant role of the electron–hole (e)–(h) coulomb interaction. It is shown that the spatial distribution of the e–h pair dominating the absorption onset is very localized around the titanium atoms. The absorption spectra at different Rb substitutions indicate an insignificant variation in the energy of the absorption onset due to the small differences in the corresponding bandgaps. The second-harmonic susceptibility tensor components of KTP/RbTiOPO4 (RTP) alloys at λ=1064 nm are evaluated and compared with experimental results. We show that Rb substitution modifies the maximum values of deff in Rb0.5K0.5TiOPO4 and RTP. Our results provide a valuable theoretical framework for tuning the optical properties of the KTP based crystals through doping for optoelectronic applications.

1.
E.
Rafailov
,
W.
Sibbett
,
A.
Mooradian
,
J.
McInerney
,
H.
Karlsson
,
S.
Wang
, and
F.
Laurell
,
Opt. Lett.
28
,
2091
(
2003
).
2.
Y.
Zhang
,
L.
Tang
,
N.
Ji
,
G.
Liu
,
J.
Wang
,
H.
Jiang
, and
W.
Cao
,
J. Appl. Phys.
119
,
124104
(
2016
).
3.
J.
Huang
,
Z.
Huang
,
N.
Nikolaev
,
A.
Mamrashev
,
V.
Antsygin
,
O.
Potaturkin
,
A.
Meshalkin
,
A.
Kaplun
,
G.
Lanskii
,
Y. M.
Andreev
et al.,
Laser Phys. Lett.
15
,
075401
(
2018
).
4.
Y.
Zhang
,
N.
Hayashi
,
H.
Matsumori
,
R.
Mitazaki
,
Y.
Xue
,
Y.
Okada-Shudo
,
M.
Watanabe
, and
K.
Kasai
,
Opt. Commun.
294
,
271
(
2013
).
5.
J.
Gao
,
F.
Cui
,
C.
Xue
,
C.
Xie
, and
P.
Kunchi
,
Opt. Lett.
23
,
870
(
1998
).
6.
J.
Qiao
,
S.
Zhao
,
K.
Yang
,
J.
Zhao
,
G.
Li
,
D.
Li
,
T.
Li
,
W.
Qiao
,
H.
Chu
, and
C.
Luan
,
Opt. Laser Technol.
92
,
62
(
2017
).
7.
I.
Savatinova
,
I.
Savova
,
E.
Liarokapis
,
C.
Ziling
,
V.
Atuchin
,
M.
Armenise
, and
V.
Passaro
,
J. Phys. D: Appl. Phys.
31
,
1667
(
1998
).
8.
L.-L.
Wang
,
X.-J.
Cui
,
J.
Rensberg
,
J.-J.
Yin
,
S.
Creutzburg
,
K.
Ritter
,
W.
Wesch
, and
E.
Wendler
,
Opt. Mater.
66
,
374
(
2017
).
9.
N.
Dong
,
Y.
Yao
,
Y.
Jia
,
F.
Chen
,
S. K.
Vanga
,
A. A.
Bettiol
, and
Q.
Lu
,
Opt. Mater.
35
,
184
(
2012
).
10.
A.
Pugachev
,
N.
Surovtsev
,
V.
Voronkova
,
V.
Semenenko
,
V.
Yanovskii
, and
V.
Atuchin
,
J. Ceram. Process. Res.
4
,
101
(
2003
).
11.
L.
Cheng
,
L.
Cheng
,
R.
Harlow
, and
J.
Bierlein
,
Appl. Phys. Lett.
64
,
155
(
1994
).
12.
T. Y.
Losevskaya
,
O.
Alekseeva
,
V.
Yanovskii
,
V.
Voronkova
,
N.
Sorokina
,
V.
Simonov
,
S. Y.
Stefanovich
,
S.
Ivanov
,
S.
Eriksson
, and
S.
Zverkov
,
Crystallogr. Rep.
45
,
739
(
2000
).
13.
D.
Zhang
,
H.
Shen
,
W.
Liu
,
W.
Chen
,
G.
Zhang
,
G.
Zhang
,
R.
Zeng
,
C.
Huang
,
W.
Lin
, and
J.
Liang
,
J. Cryst. Growth
218
,
98
(
2000
).
14.
V.
Voronkova
,
V.
Yanovskii
,
T. Y.
Losevskaya
, and
S. Y.
Stefanovich
,
J. Appl. Phys.
94
,
1954
(
2003
).
15.
V.
Atuchin
,
O.
Alekseeva
,
V.
Kesler
,
L.
Pokrovsky
,
N.
Sorokina
, and
V.
Voronkova
,
J. Solid State Chem.
179
,
2349
(
2006
).
16.
S.
Sadhasivam
,
R. N.
Perumal
, and
P.
Ramasamy
,
J. Cryst. Growth
445
,
84
(
2016
).
17.
A. P.
Gazhulina
and
M. O.
Marychev
,
Cryst. Struct. Theory Appl.
2
,
106
(
2013
).
18.
Z.
Kecong
and
W.
Ximin
,
Chin. Sci. Bull.
46
,
2028
(
2001
).
19.
V.
Voronkova
,
V.
Yanovskii
,
I.
Leont’eva
,
E.
Agapova
,
E.
Kharitonova
,
S. Y.
Stefanovich
, and
S.
Zver’kov
,
Inorg. Mater.
40
,
1321
(
2004
).
20.
M.
Ghoohestani
,
A.
Arab
,
S. J.
Hashemifar
, and
H.
Sadeghi
,
J. Appl. Phys.
123
,
015702
(
2018
).
21.
Z.
Li
,
P.
Zhu
,
Y.
Chen
,
N.
Ji
,
J.
Liu
,
X.
Duan
, and
H.
Jiang
,
CrystEngComm
21
,
1570
(
2019
).
22.
Z.
Li
,
P.
Zhu
,
J.
Ding
,
N.
Ji
,
Y.
Chen
,
Z.
Wang
,
X.
Duan
, and
H.
Jiang
,
Cryst. Growth Des.
19
,
7143
(
2019
).
23.
J.
Liu
,
Z.
Li
,
P.
Zhu
, and
X.
Duan
,
Opt. Mater. (Amst)
75
,
38
(
2018
).
24.
M.
Landmann
,
E.
Rauls
, and
W.
Schmidt
,
J. Phys.: Condens. Matter
24
,
195503
(
2012
).
25.
L.
Chiodo
,
J. M.
García-Lastra
,
A.
Iacomino
,
S.
Ossicini
,
J.
Zhao
,
H.
Petek
, and
A.
Rubio
,
Phys. Rev. B
82
,
045207
(
2010
).
26.
W.
Kang
and
M. S.
Hybertsen
,
Phys. Rev. B
82
,
085203
(
2010
).
27.
E. K.
Chang
,
M.
Rohlfing
, and
S. G.
Louie
,
Phys. Rev. Lett.
85
,
2613
(
2000
).
28.
D. Y.
Qiu
,
H.
Felipe
, and
S. G.
Louie
,
Phys. Rev. Lett.
111
,
216805
(
2013
).
29.
J.
He
,
K.
Hummer
, and
C.
Franchini
,
Phys. Rev. B
89
,
075409
(
2014
).
30.
T. A.
Driscoll
,
H. J.
Hoffman
,
R. E.
Stone
, and
P. E.
Perkins
,
J. Opt. Soc. Am. B
3
,
683
(
1986
).
31.
T. Y.
Fan
,
C.
Huang
,
B.
Hu
,
R. C.
Eckardt
,
Y.
Fan
,
R. L.
Byer
, and
R.
Feigelson
,
Appl. Opt.
26
,
2390
(
1987
).
32.
A.
Arie
,
G.
Rosenman
,
V.
Mahal
,
A.
Skliar
,
M.
Oron
,
M.
Katz
, and
D.
Eger
,
Opt. Commun.
142
,
265
(
1997
).
33.
L.
Mayer
,
A.
Slablab
,
G.
Dantelle
,
V.
Jacques
,
A.-M.
Lepagnol-Bestel
,
S.
Perruchas
,
P.
Spinicelli
,
A.
Thomas
,
D.
Chauvat
,
M.
Simonneau
et al.,
Nanoscale
5
,
8466
(
2013
).
34.
W.
Ching
and
Y.-N.
Xu
,
Phys. Rev. B
44
,
5332
(
1991
).
35.
J.
Lowther
,
P.
Manyum
, and
P.
Suebka
,
Phys. Status Solidi B
242
,
1392
(
2005
).
36.
A. H.
Reshak
,
I.
Kityk
, and
S.
Auluck
,
J. Phys. Chem. B
114
,
16705
(
2010
).
37.
V.
Atuchin
,
V.
Kesler
,
G.
Meng
, and
Z.
Lin
,
J. Phys.: Condens. Matter
24
,
405503
(
2012
).
38.
S.
Neufeld
,
A.
Bocchini
,
U.
Gerstmann
,
A.
Schindlmayr
, and
W.
Schmidt
,
J. Phys.: Mater.
2
,
045003
(
2019
).
39.
P.
Puschnig
and
C.
Ambrosch-Draxl
,
Phys. Rev. B
66
,
165105
(
2002
).
40.
S.
Sagmeister
and
C.
Ambrosch-Draxl
,
Phys. Chem. Chem. Phys.
11
,
4451
(
2009
).
41.
S.
Sharma
,
J.
Dewhurst
, and
C.
Ambrosch-Draxl
,
Phys. Rev. B
67
,
165332
(
2003
).
42.
A.
Gulans
,
S.
Kontur
,
C.
Meisenbichler
,
D.
Nabok
,
P.
Pavone
,
S.
Rigamonti
,
S.
Sagmeister
,
U.
Werner
, and
C.
Draxl
,
J. Phys.: Condens. Matter
26
,
363202
(
2014
).
43.
J. P.
Perdew
,
A.
Ruzsinszky
,
G. I.
Csonka
,
O. A.
Vydrov
,
G. E.
Scuseria
,
L. A.
Constantin
,
X.
Zhou
, and
K.
Burke
,
Phys. Rev. Lett.
100
,
136406
(
2008
).
44.
P.
Thomas
,
S.
Mayo
, and
B.
Watts
,
Acta Crystallogr. B
48
,
401
(
1992
).
45.
N.
Sorokina
and
V.
Voronkova
,
Crystallogr. Rep.
52
,
80
(
2007
).
46.
S. T.
Norberg
,
P. A.
Thomas
, and
M. G.
Tucker
,
J. Phys.: Condens. Matter
23
,
175401
(
2011
).
47.
F.
Bechstedt
,
Many-Body Approach to Electronic Excitations
(
Springer
,
2016
).
48.
L. G.
Ferreira
,
M.
Marques
, and
L. K.
Teles
,
Phys. Rev. B
78
,
125116
(
2008
).
49.
L. G.
Ferreira
,
M.
Marques
, and
L. K.
Teles
,
AIP Adv.
1
,
032119
(
2011
).
50.
R. R.
Pela
,
U.
Werner
,
D.
Nabok
, and
C.
Draxl
,
Phys. Rev. B
94
,
235141
(
2016
).
51.
S.
Sharma
and
C.
Ambrosch-Draxl
,
Phys. Scr.
2004
,
128
.
52.
R.
DeSalvo
,
A. A.
Said
,
D. J.
Hagan
,
E. W.
Van Stryland
, and
M.
Sheik-Bahae
,
IEEE J. Quantum Electron.
32
,
1324
(
1996
).
53.
H.
Li
,
C.
Kam
,
Y.
Lam
, and
W.
Ji
,
Opt. Mater.
15
,
237
(
2001
).
54.
G.
Mann
and
S.
Seidel
,
Proc. SPIE
3098
,
582
590
(
1997
).
55.
A.
Zukauskas
,
V.
Pasiskevicius
, and
C.
Canalias
,
Opt. Express
21
,
1395
(
2013
).
56.
N.
Golego
and
M.
Cocivera
,
Thin Solid Films
322
,
14
(
1998
).
57.
A.
Dudelzak
,
P.-P.
Proulx
,
V.
Denks
,
V.
Mürk
, and
V.
Nagirnyi
,
J. Appl. Phys.
87
,
2110
(
2000
).
58.
R.
Leitsmann
,
W.
Schmidt
,
P.
Hahn
, and
F.
Bechstedt
,
Phys. Rev. B
71
,
195209
(
2005
).
59.
A.
Riefer
and
W.
Schmidt
,
Phys. Rev. B
96
,
235206
(
2017
).
60.
CASTECH
, See www.castech-us.com/casktp.htm for “Potassium Titanyl Phosphate” (2010).
61.
M. V.
Pack
,
D. J.
Armstrong
, and
A. V.
Smith
,
Appl. Opt.
43
,
3319
(
2004
).
62.
W. J.
Alford
and
A. V.
Smith
,
J. Opt. Soc. Am. B
18
,
524
(
2001
).
63.
I.
Shoji
,
T.
Kondo
,
A.
Kitamoto
,
M.
Shirane
, and
R.
Ito
,
J. Opt. Soc. Am. B
14
,
2268
(
1997
).
64.
A.
Anema
and
T.
Rasing
,
Appl. Opt.
36
,
5902
(
1997
).
65.
L.
Cheng
,
L.
Cheng
,
J.
Galperin
,
P. M.
Hotsenpiller
, and
J.
Bierlein
,
J. Cryst. Growth
137
,
107
(
1994
).
66.
H.
Vanherzeele
and
J. D.
Bierlein
,
Opt. Lett.
17
,
982
(
1992
).
67.
B.
Boulanger
,
J.
Feve
,
G.
Marnier
, and
B.
Menaert
,
Pure Appl. Opt.
7
,
239
(
1998
).
68.
R. C.
Eckardt
,
H.
Masuda
,
Y. X.
Fan
, and
R. L.
Byer
,
IEEE J. Quantum Electron.
26
,
922
(
1990
).
You do not currently have access to this content.