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Enhancement of second harmonic generation by wavefront shaping in the scratch of BaMgF 4 nanocrystal powder film HAOYING WU, ZHUO WANG, HAIGANG LIU, YANQI QIAO, YUANLIN ZHENG, AND XIANFENG CHEN* The State Key Laboratory on Fiber Optic Local Area Communication Networks and Advanced Optical Communication Systems, School of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240, China *[email protected] Abstract: During the exploration of nonlinear crystal, such as BaMgF 4 crystal for all-solid- state lasers in the vacuum ultraviolet region, many problems emerged in the scattering centers. These were caused by immature crystal-growth technology, which may bring difficulties to the periodic poling process for quasi-phase-matching. In previous studies, research has shown that nonlinear random materials can also be used for frequency conversion. In this paper, a random nonlinear process was observed when the fundamental wave is illuminated onto the scratch of the BaMgF 4 nanocrystal powder film. Then, the second-harmonic waves scattered from the nonlinear turbid media are re-collected to a forward direction using feedback wavefront shaping. The method shows a repeated way to improve the conversion efficiency, which may be viable to improve the second order conversion efficiency of BaMgF 4 at other wavelengths, especially in the VUV regime. Additionally, more interesting applications in random nonlinear material, such as nanocrystal ceramics, can be expected in the future. © 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement 1. Introduction All-solid-state lasers (ASSLs) have a lot of advantages, such as narrow bandwidth, high beam quality and compact setup compared with currently used excimer laser [1]. Due to these advantages, ASSLs in the vacuum ultraviolet (VUV) have been required for optical lithography, photoelectron spectroscopy and medical uses [2,3]. In 2007, C. Chen et.al. obtained watt-level average-power from 185 nm to 200 nm by using KBe 2 BO 3 F 2 (KBBF) crystal [3]. Compared with KBBF, a new ferroelectric crystal BaMgF 4 (BMF) was found to be another candidate for ASSLs in the VUV and mid-IR region because of its transparency from 125 nm to 13 μm [4,5]. The second-order nonlinear optical coefficient of BMF was reported to be d 31 = 0.15 pm/V, d 32 = 0.36 pm/V, d 33 = 0.12 pm/V [2]. Several years ago, E.G. Villora et al. obtained the shortest frequency-doubling emission at 368 nm by quasi phase matching in BMF crystal [5,6]. Nonetheless, scattering centers are always present in the BMF crystal grown by the temperature gradient technique or the Czochralski method [7,8]. These scattering centers may bring difficulties to the periodic poling process for quasi-phase- matching, and restrict device performance [9]. Besides, the birefringence in these materials was too small to birefringently phase match any interactions to generate VUV [10]. The random nonlinear system has emerged as a new research interest because it does not have strict requirement of crystals. It was demonstrated that the purposeful focusing of a second harmonic generated and scattered from superfine lithium niobate nanocrystal powder via feedback wavefront shaping method [11]. In this paper, the second harmonic generation (SHG) scattered from BMF nanocrystal powders was enhanced by feedback wave-front shaping, and the efficiency can be enhanced Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3593 #345315 Journal © 2018 https://doi.org/10.1364/OME.8.003593 Received 7 Sep 2018; revised 20 Oct 2018; accepted 22 Oct 2018; published 29 Oct 2018

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Page 1: Enhancement of second harmonic generation by wavefront …olab.physics.sjtu.edu.cn/papers/2018/25. Haoying Wu_OME_2018.pdf · ding to the tre-based wave-front illustrated in as the

Enhancement of second harmonic generation by wavefront shaping in the scratch of BaMgF4 nanocrystal powder film HAOYING WU, ZHUO WANG, HAIGANG LIU, YANQI QIAO, YUANLIN ZHENG, AND XIANFENG CHEN* The State Key Laboratory on Fiber Optic Local Area Communication Networks and Advanced Optical Communication Systems, School of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240, China *[email protected]

Abstract: During the exploration of nonlinear crystal, such as BaMgF4 crystal for all-solid-state lasers in the vacuum ultraviolet region, many problems emerged in the scattering centers. These were caused by immature crystal-growth technology, which may bring difficulties to the periodic poling process for quasi-phase-matching. In previous studies, research has shown that nonlinear random materials can also be used for frequency conversion. In this paper, a random nonlinear process was observed when the fundamental wave is illuminated onto the scratch of the BaMgF4 nanocrystal powder film. Then, the second-harmonic waves scattered from the nonlinear turbid media are re-collected to a forward direction using feedback wavefront shaping. The method shows a repeated way to improve the conversion efficiency, which may be viable to improve the second order conversion efficiency of BaMgF4 at other wavelengths, especially in the VUV regime. Additionally, more interesting applications in random nonlinear material, such as nanocrystal ceramics, can be expected in the future.

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

1. Introduction All-solid-state lasers (ASSLs) have a lot of advantages, such as narrow bandwidth, high beam quality and compact setup compared with currently used excimer laser [1]. Due to these advantages, ASSLs in the vacuum ultraviolet (VUV) have been required for optical lithography, photoelectron spectroscopy and medical uses [2,3]. In 2007, C. Chen et.al. obtained watt-level average-power from 185 nm to 200 nm by using KBe2BO3F2 (KBBF) crystal [3]. Compared with KBBF, a new ferroelectric crystal BaMgF4 (BMF) was found to be another candidate for ASSLs in the VUV and mid-IR region because of its transparency from 125 nm to 13 μm [4,5]. The second-order nonlinear optical coefficient of BMF was reported to be d31 = 0.15 pm/V, d32 = 0.36 pm/V, d33 = 0.12 pm/V [2]. Several years ago, E.G. Villora et al. obtained the shortest frequency-doubling emission at 368 nm by quasi phase matching in BMF crystal [5,6]. Nonetheless, scattering centers are always present in the BMF crystal grown by the temperature gradient technique or the Czochralski method [7,8]. These scattering centers may bring difficulties to the periodic poling process for quasi-phase-matching, and restrict device performance [9]. Besides, the birefringence in these materials was too small to birefringently phase match any interactions to generate VUV [10].

The random nonlinear system has emerged as a new research interest because it does not have strict requirement of crystals. It was demonstrated that the purposeful focusing of a second harmonic generated and scattered from superfine lithium niobate nanocrystal powder via feedback wavefront shaping method [11].

In this paper, the second harmonic generation (SHG) scattered from BMF nanocrystal powders was enhanced by feedback wave-front shaping, and the efficiency can be enhanced

Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3593

#345315 Journal © 2018

https://doi.org/10.1364/OME.8.003593 Received 7 Sep 2018; revised 20 Oct 2018; accepted 22 Oct 2018; published 29 Oct 2018

Page 2: Enhancement of second harmonic generation by wavefront …olab.physics.sjtu.edu.cn/papers/2018/25. Haoying Wu_OME_2018.pdf · ding to the tre-based wave-front illustrated in as the

by 30 times. obviously whreason is that also played an

2. ExperimeThe BMF nashown in Figwith maximufabricated by m× m30 mmin Fig. 1(d).

Fig. 1μm). sampl

The feedbcharacterize sin Fig. 2 [15](SLM), then tSLM were dMeanwhile, tserved as a fesome phase malgorithm choSH intensity amutagenic facthe optimizatigeneration. Fi

Additionally,hen the pump p

the rough frinn important rol

ent and resulanocrystal powg. 1(a), the scaum size of ~10

electrophoretic× 0.2 mm as s

1. (a) A SEM imag(b)the Electropho

le. (d) an SEM ima

back wavefronscattering medi]. The fundamthe SH can bedivided into sthe SH intensiteedback to opt

masks were genose half of segat the target, actor into the neion process wainally, the rand

, we found thposition was atge of the scratle in the surfac

lts wders were preanning electron0 μm. As depic deposition mhown in Fig. 1

ge of the BMF paoretic Deposition age of the film sam

nt shaping woria is the key of

mental wave (Fe focused to onseveral segmety at one chartimize the SLMnerated randomments from tw

and composed ext generationas repeated, andom speckle wa

hat the SHG ct the scratch ofch not only proe localization o

epared by the n microscope icted by Fig.

method [14]. Th1(c), and the S

articles with maximMethod (c) the

mple (scale bar, 2 μ

rking as a phaf this study. ThW) was reshap

ne point. Durinents, which crge coupled deM phase mask

mly as the primwo masks whic

the next gener, there came a

nd the spot couas focused into

conversion efff the BMF powovided additionof fundamenta

chemical synt(SEM) picture1(b), the BMF

he layer sampleSEM image of

mum size of ~10 picture of BMF μm).

ase-control hohe concept of tped using the ng the optimizcan reshape thevice (CCD) pks via genetic mal generation.ch were the moration. After in

a new set of SLuld be increasino one point.

ficiency was pwder film. Thenal scattering e

al light [12].

thesis method e of the BMF F nanocrystal e had a dimensthat sample w

μm (scale bar, 50nanocrystal film

olographic techthis technique spatial light m

zation, the pixehe FW indeppixel was recoalgorithm [11] Then, the optost effective rancorporating 1LM phase masngly clearer af

promoted e possible effect but

[13]. As particles

film was sion of 30 as shown

0 m

hnique to is shown

modulator els on the pendently. orded and ]. Firstly, imization

anking by 0%~30%

sks. Next, fter every

Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3594

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The schemdiode-pumpedof 1064 nm, aa Glan-Taylorpump light tcollimating ashaped wave another lens-transmission awas monitorespectral resolmeasured by filter of 1064computer base

Fig. 3bloomL3(a\b

When thewhich could bdiscussed in tpoints on the 1080 pixels oshown in Figonly one segmby 15 times, a

Fig. 2. The con

matic diagram d all-solid-statea pulse width or Prism were uto fit the inteand beam-bloo

went throughsystem and anand reflection

ed and analyzedlution 1/4 0.09an optical ins

4 nm. All the ed on the gene

3. the schematic ming lens system: b), f2(a\b) = 100, 4

FW was illumbe observed inthe next part. CCD. Then, t

on the SLM w. 4(b), after 20ment in size. Bas shown in Fi

ncept of SHG focu

of the experime Q-switched l

of 10 ns and repused to controlnsity thresholming lens sys

h a dichroic mn ocular glassdirection. In thd by a high-res9 nm). The imstrument CCD

SLM, CCD atic algorithm.

diagram of the pL1(a\b), f1(a\b) =40 mm, f3(a\b) = 2

minated onto tn all directionsAt the beginn

the SH signal were divided in00 generations Besides, the intig. 5(a). Accor

using via feedback-

mental setup islaser was usedpetition freque the optical pod and phase stem, the FW mirror and focs. The scatterehe transmissionsolution spectrmage of SH si

(DAHENG Mand spectrome

primary optical se 40, 200 mm; bea200, 50 mm; M, m

the scratch of s, and the possning, the speckwas focused b

nto 160× 90 seoptimization,

tensity of SH arding to the tre

-based wave-front

s illustrated ind as the FW souency of 500 Hzower and the prequirement owas expanded

cused into the ed SH signal n direction, therometer (AUaSignal in the re

MER-131-210Ueter were real-

etup. / 2λ , half-wam-scaling lens sy

mirror; DM, dichro

the film, we gsible reason ofkle patterns weby wavefront segments to resa SH focus wat the focused

end of the curv

t shaping.

n Fig. 3. A higurce with a wa

z. A half-wave olarization sta

of the SLM. d to fit the S

BMF film sawas collected

e intensity of SSpec 2048-FT, eflection direc

U3M/C) after p-timely monito

wave plate; beam-ystem: L2(a\b) andic mirror; F, filter.

got the brightef this phenomeere a group of

shaping. Firstlyshape the SH w

was observed wlocation was

ve, further impr

gh-energy avelength plate and tes of the Across a LM. The ample by d in both SH signal Avantes,

ction was passing a

ored by a

-d .

est signal enon was f discrete y, 1920×wave. As

which was enhanced rovement

Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3595

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of optimizatioenhancement get a clearer Swere set to 3estimated to b

The enhanchosen positioOne is the qoptimization. enhancement As shown in Fintensity at thvalue for gene

The possiscattered SH on the scratcha possibly per

Fig. 4optimgenerafocus segme

on was possiblwas similar to

SH speckle pat300. Finally, be 8 pixels, as sncement factoron before and

quantity of segThe other is factor has a th

Fig. 5(c), after he focused locetic algorithm. ible reason fosignal was focu

h of the film sarfect-focusing p

4. (a)(c)(e) picturmization while the p

ations of optimizaafter 300 genera

ents.

le. Thus, the go the previous ottern, the segmthe speckle pshown in Fig. 4r η was used tafter optimiza

gments, becauthat η increas

hreshold with th300 generation

cation was estim

or the SH focuused outside th

ample might plprocess [16].

res before optimipixels were divideation while the pixations of optimiza

generations weone, as shown

ments were refiatterns turned 4(f). to describe theation. There ar

use image thinses with the ghe definite genns optimizationmated to be 3

using based ohe surface [11]lay an importan

zation (b) The Sed into 160 × 90 sexels were divided ation while the p

ere increased toin Fig. 4(d) an

ined to 240× 1d into a focal

e relative intenre two main innning can impgenerations untneration and thn, the enhancem0, which migh

on this techno]. Additionallynt role in this o

SH focus after 20egments. (d) The Sinto 160 × 90 segmixels were divide

o 300, but thend Fig. 5(b). In35, and the gepoint, and th

nsity of the sinfluencing factprove the effictil saturation [

he quantity of sment factor η oht be a local m

ology is that r, the multiple soptimization, l

00 generations ofSH focus after 300ments. (f) The SHed into 240 × 135

result of n order to enerations he size is

ignal in a tors of η. ciency of [11]. The segments. of the SH maximum

randomly scattering leading to

f 0 H 5

Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3596

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Fig. 5after estima(c) η wsegme

This expenonlinear matbe realized ingeneration, fo

3. DiscussioDuring the exabout several influenced bypulse intensitbecause of thmW/mm2. Howhen the pumspectrometer, moved the fofilm, as shown

Fig. 6part oFW mfigure

. (a) The enhancem200 generations ated to be 15 afterwas estimated to bents.

riment is belieterials, nanotubn other nonlineour-wave mixin

on xperiment, the S

nW/mm2. Besy the intensity ty, but found he thermal effowever, duringmp position fo

a typical enhcus point fromn in Fig. 6.

6. The blue line shof the BMF nanocrmoves to a scratch e (scale bar, 100 μm

ment factor η of thwhile the pixels

r 300 generations wbe 30 after 300 gen

eved to be repebe materials anear processes wng and stimulat

SH signal coulsides, the efficof the incidenthat the surfa

fect accumulag the experimecused at the s

hancement in om the temper pa

hows the intensity rystal film. The reof this film. The mm).

he SHG at the focuwere divided in

while the pixels wnerations while the

eatable in othend other nanocwith proper coted Raman sca

ld be measuredciency of wavent light. Thereace of the BMtion [17]. Theent, it was foucratch of the Bour experimenart of the BMF

of the SH signal wed line shows the microscopic image

used location was nto 160 × 90 segmwere divided into 1e pixels were divid

er nonlinear macrystal materialonfigurations, attering, etc.

d at the film, buefront shapingefore, we triedMF film sample damage threund that the SBMF powder

nts was estimatF nanocrystal f

when the FW focuintensity of the SHe of the scratch is

estimated to be 15ments. (b) η was60 × 90 segments

ded into 240 × 135

aterials, such als. It is also exsuch as third h

ut the intensityg technology isd to increase thle would be deshold was abSH signal wasfilm. Monitoreted to be 100 film to a scratc

uses on the temperH signal when thealso shown in this

5 s . 5

as porous xpected to harmonic

y of it was s strongly he pump-destroyed bout 22.1 s stronger ed by the after we

ch of this

r e s

Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3597

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To undersMultiphysics.intensity waspowder accumfocus on this s

Fig

Theoreticathe rough surfAs the studyproportion to

where Ipoly is coherent feedat the accumusurface may a22].

4. ConclusioIn conclusiondeposition meilluminated onrough surfacewhich is in dishaping methThe enhancemAt last, the SHorders of maefficiency basrepeated in Btowards VUV

Funding National KeyFoundation oTechnology o

References 1. L.J. Cox, Sol2. J. J. Chen, X

second-order3. T. Kanai, X.

KBBF prism

stand the defec As shown in

s randomly enmulated and fstructure, and i

. 7. The intensity o

ally, there werface caused mu

y on random the effective o

the total SH idback was moreulating area coalso help form

on n, the BMF nethod. The SHnto the scratche caused multiirect proportionod based on th

ment factor at HG efficiency agnitude. Thissed on the ran

BMF nanocrysV.

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lid-State Laser EnX. F. Chen, Y. Z. M

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of both the FW wa

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I

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er, 1997). A. H. Wu, H. J. Li,aMgF4,” J. Opt. Sod C. Chen, “Watt-l10), 8696–8703 (2

imulated the prhe simulation scratch where

rthermore, the as shown in F

randomly enhance

phenomenon.effective opticthe total SH

equation can be

sity; L is the oh the help of lort of the samplegating both F

s prepared usy nearly 100 timason of this pheffective opticensity. Using t

H signal was foproximately 30r film can be enble way to inhe experiment prove the SHG

0303700); Nattion for Devel

, L. W. Jiang, and oc. Am. B 29(4), 6level tunable deep2009).

rocess using Cof the SH sig

e the BMF na FW was sim

Fig. 7(b).

ed at the scratch.

The first onecal path becam

H intensity is e written as:

optical path. Tonger interactile. Secondly, t

FW and SH po

ing the electrmes when the

henomenon wacal path becamthe feedback wocused to a brig0 after 300 gennhanced by neancrease the co

is also expecG conversion e

tional Naturallopment of Sci

J. Xu, “Measurem665–668 (2012). p ultraviolet light s

COMSOL gnal. The anocrystal

mulated to

was that me longer.

in direct

Therefore, on length the rough

ower [20–

ophoretic FW was

as that the me longer wave-front ght point. nerations. arly three onversion ted to be efficiency

Science ience and

ment of

ource by a

Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3598

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Vol. 8, No. 11 | 1 Nov 2018 | OPTICAL MATERIALS EXPRESS 3599