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Ultraviolet polarized light emitting and detecting dual-functioning device based on nonpolar n-ZnO/i-ZnO/p-AlGaN heterojunction JIANGNAN DAI, 1, *JINGWEN CHEN, 1 XIAOHANG LI, 2 JUN ZHANG, 1 HANLING LONG, 1 HAOCHUNG KUO, 3 YUNBIN HE, 4 AND CHANGQING CHEN 1 1 Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, China 2 King Abdullah University of Science and Technology (KAUST), Advanced Semiconductor Laboratory, Thuwal 23955, Saudi Arabia 3 Department of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung University, 1001 Ta Hsueh Road, Hsinchu 300, Taiwan 4 Hubei University, Wuhan, 430062, China *Corresponding author: [email protected] Received 9 January 2019; revised 1 March 2019; accepted 4 March 2019; posted 12 March 2019 (Doc. ID 356963); published 5 April 2019 We report on the demonstration of a 386 nm light emission and detection dual-functioning device based on nonpolar a-plane n-ZnOi-ZnOp-Al 0.1 Ga 0.9 N heterojunction under both forward and reverse bias. The electroluminescence in- tensity under reverse bias is significantly stronger than that under forward bias, facilitated by carrier tunneling when the valence band of p-AlGaN aligns with the conduction band of i-ZnO under reverse bias. Also amid reverse bias, the photodetection was observed and applied in a duplex optical communication device. Optical polarization of the light emission is studied for potential polarization- sensitive device applications. The proposed device provides an important pathway for the multifunctional devices op- erating in a UV spectrum. © 2019 Optical Society of America https://doi.org/10.1364/OL.44.001944 Luminescence and photodetection can be achieved in two sep- arate devices; yet each often requires a more complex circuit construction and fabrication process. Therefore, it is desirable to integrate both functions in a single monolithic device and enable technically important multifunctional electronics. The dual-functioning device operating in a visible spectrum has been fabricated with a light-responsive double-heterojunction nanorod based on CdS, CdSe, and ZnSe nanocrystal materials [1]. Benefitting from a high exciton binding energy (60 meV) and large direct bandgap (3.37 eV) [2], ZnO is a promising candidate for UV light emitting diodes (LEDs), detectors, and sensors [3]. Considering the unavailability of the p-type ZnO [4], as well as the small lattice mismatch (1.8%) and similar band structure between ZnO and GaN [5], p-GaN has been widely employed to fabricate heterojunction devices with n-type ZnO. As for LEDs based on n-ZnO/p-GaN, the emission from the p-GaN layer generally dominates the spec- trum, because the majority of the depletion region lies in p-GaN [6], causing a low carrier injection efficiency in ZnO. In this Letter, we propose a feasible solution to improve the carrier injection and radiative recombination efficiencies by inserting an intrinsic ZnO (i-ZnO) layer between the n-ZnO and p-AlGaN, all on the nonpolar 11 ¯ 20 a-plane, where the depletion region almost entirely resides in the i-ZnO layer [7]. By increasing the conduction band offset ΔE c , the proposed heterojunction with p-AlGaN can greatly hinder the electron leakage to the p-type layer, thus localizing electrons and im- proving carrier injection efficiency in i-ZnO [8]. Moreover, compared to polar ZnO, nonpolar ZnO can realize polarized emission or detection, arising from modification of the valence band structure caused by anisotropic in-plane strains and the hexagonal unit cells distortions [9]. This unique property makes nonpolar ZnO feasible to fabricate polarization-sensitive optoelectronic devices, such as polarized sensors and detectors. In previous reports, the luminescence under forward bias and detection under reverse bias of a p-AlGaN/i-ZnO/n-ZnO (PIN) structure device were reported [10]. As for luminescence under reverse bias, only avalanche-mechanism-based lumines- cence under reverse bias was explained in detail [8]. In this Letter, luminescence mechanisms based on a tunneling effect, as well as a light detection mechanism, were studied in detail through experiments and simulation. Furthermore, the polar- ized luminescence of the heterojunction UV-LEDs was studied by angle-resolved electroluminescence (EL) and photolumines- cence (PL) measurements. To form PIN heterojunction, a 2.2 μm p-type AlGaN layer was first grown by metal organic chemical vapor deposition at 1030°C on a-plane aluminum nitride (AlN) templates on r -plane sapphire. The concentration and mobility of a hole in the p-Al 0.1 Ga 0.9 N layer are 3.8 × 10 17 cm -3 and 8.0 cm 2 Vs, determined by Hall measurements, respectively. The nonpolar 200 nm i-ZnO and 150 nm n-ZnO (Al-doped ZnO, i.e., AZO) layers were grown on the p-AlGaN layer by using pulsed laser deposition at 700°C. The layer thickness and growth ori- entation were verified by a transmission electron microscope (TEM), as shown in Fig. 1(d). The unintentional doping 1944 Vol. 44, No. 8 / 15 April 2019 / Optics Letters Letter 0146-9592/19/081944-04 Journal © 2019 Optical Society of America

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Page 1: Ultraviolet polarized light emitting and detecting dual-functioning … · 2019. 7. 14. · similar band structure between ZnO and GaN [5], p-GaN has been widely employed to fabricate

Ultraviolet polarized light emitting and detectingdual-functioning device based on nonpolarn-ZnO/i-ZnO/p-AlGaN heterojunctionJIANGNAN DAI,1,* JINGWEN CHEN,1 XIAOHANG LI,2 JUN ZHANG,1 HANLING LONG,1 HAOCHUNG KUO,3

YUNBIN HE,4 AND CHANGQING CHEN1

1Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, China2King Abdullah University of Science and Technology (KAUST), Advanced Semiconductor Laboratory, Thuwal 23955, Saudi Arabia3Department of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung University, 1001 Ta Hsueh Road, Hsinchu 300, Taiwan4Hubei University, Wuhan, 430062, China*Corresponding author: [email protected]

Received 9 January 2019; revised 1 March 2019; accepted 4 March 2019; posted 12 March 2019 (Doc. ID 356963); published 5 April 2019

We report on the demonstration of a 386 nm light emissionand detection dual-functioning device based on nonpolara-plane n-ZnO∕i-ZnO∕p-Al0.1Ga0.9N heterojunction underboth forward and reverse bias. The electroluminescence in-tensity under reverse bias is significantly stronger than thatunder forward bias, facilitated by carrier tunneling whenthe valence band of p-AlGaN aligns with the conductionband of i-ZnO under reverse bias. Also amid reverse bias,the photodetection was observed and applied in a duplexoptical communication device. Optical polarization ofthe light emission is studied for potential polarization-sensitive device applications. The proposed device providesan important pathway for the multifunctional devices op-erating in a UV spectrum. © 2019 Optical Society of America

https://doi.org/10.1364/OL.44.001944

Luminescence and photodetection can be achieved in two sep-arate devices; yet each often requires a more complex circuitconstruction and fabrication process. Therefore, it is desirableto integrate both functions in a single monolithic device andenable technically important multifunctional electronics. Thedual-functioning device operating in a visible spectrum hasbeen fabricated with a light-responsive double-heterojunctionnanorod based on CdS, CdSe, and ZnSe nanocrystal materials[1]. Benefitting from a high exciton binding energy (60 meV)and large direct bandgap (3.37 eV) [2], ZnO is a promisingcandidate for UV light emitting diodes (LEDs), detectors,and sensors [3]. Considering the unavailability of the p-typeZnO [4], as well as the small lattice mismatch (∼1.8%) andsimilar band structure between ZnO and GaN [5], p-GaNhas been widely employed to fabricate heterojunction deviceswith n-type ZnO. As for LEDs based on n-ZnO/p-GaN, theemission from the p-GaN layer generally dominates the spec-trum, because the majority of the depletion region lies inp-GaN [6], causing a low carrier injection efficiency in ZnO.

In this Letter, we propose a feasible solution to improve thecarrier injection and radiative recombination efficiencies byinserting an intrinsic ZnO (i-ZnO) layer between the n-ZnOand p-AlGaN, all on the nonpolar �112̄0� a-plane, where thedepletion region almost entirely resides in the i-ZnO layer [7].By increasing the conduction band offset ΔEc , the proposedheterojunction with p-AlGaN can greatly hinder the electronleakage to the p-type layer, thus localizing electrons and im-proving carrier injection efficiency in i-ZnO [8]. Moreover,compared to polar ZnO, nonpolar ZnO can realize polarizedemission or detection, arising from modification of the valenceband structure caused by anisotropic in-plane strains and thehexagonal unit cells distortions [9]. This unique propertymakes nonpolar ZnO feasible to fabricate polarization-sensitiveoptoelectronic devices, such as polarized sensors and detectors.In previous reports, the luminescence under forward bias anddetection under reverse bias of a p-AlGaN/i-ZnO/n-ZnO(PIN) structure device were reported [10]. As for luminescenceunder reverse bias, only avalanche-mechanism-based lumines-cence under reverse bias was explained in detail [8]. In thisLetter, luminescence mechanisms based on a tunneling effect,as well as a light detection mechanism, were studied in detailthrough experiments and simulation. Furthermore, the polar-ized luminescence of the heterojunction UV-LEDs was studiedby angle-resolved electroluminescence (EL) and photolumines-cence (PL) measurements.

To form PIN heterojunction, a 2.2 μm p-type AlGaN layerwas first grown by metal organic chemical vapor depositionat 1030°C on a-plane aluminum nitride (AlN) templates onr-plane sapphire. The concentration and mobility of a hole inthe p-Al0.1Ga0.9N layer are 3.8 × 1017 cm−3 and 8.0 cm2∕Vs,determined by Hall measurements, respectively. The nonpolar200 nm i-ZnO and 150 nm n-ZnO (Al-doped ZnO, i.e.,AZO) layers were grown on the p-AlGaN layer by using pulsedlaser deposition at 700°C. The layer thickness and growth ori-entation were verified by a transmission electron microscope(TEM), as shown in Fig. 1(d). The unintentional doping

1944 Vol. 44, No. 8 / 15 April 2019 / Optics Letters Letter

0146-9592/19/081944-04 Journal © 2019 Optical Society of America

Page 2: Ultraviolet polarized light emitting and detecting dual-functioning … · 2019. 7. 14. · similar band structure between ZnO and GaN [5], p-GaN has been widely employed to fabricate

concentration of i-ZnO is 5.6 × 1015 cm−3. The electron con-centration and mobility of n-ZnO are 3.2 × 1020 cm−3 and16.5 cm2∕Vs, respectively. The surface morphology of thePIN heterojunction wafer was characterized by atomic forcemicroscopy (AFM), as shown in Fig. 1(a). The RMS surfaceroughness over 5 × 5 μm2 is 1.94 nm. The crystallinity ofthe deposited films was probed by a high-resolution x-ray dif-fraction system (λ � 1.5406 Å). As shown in Fig. 1(b), only�112̄0� peaks at 56.5° and 57.9° belonging to the a-planeZnO and AlGaN can be observed, confirming the nonpolarstructure. The threading and stacking fault dislocation densi-ties of the ZnO layer were estimated [11] to be about 1 ×1011 cm−2 and 1 × 106 cm−1, according to Fig. 1(c).

The heterojunction devices with dimensions of 400 ×400 μm2 were fabricated and shown in Fig. 1(c). Ti/Al (20/40 nm) and Ni/Au (30/60 nm) were deposited on n-ZnO andp-AlGaN, respectively, and further annealed at 500°C for 1 minin the N 2 ambient to form ohmic contact, verified by Fig. 1(d).The large forward turn-on voltage of 10 V is due to the extraseries resistance caused by the intrinsic ZnO layer, as presentedin Figs. 2(a) and 2(b). The EL exhibits an obvious UV emissionpeak at 386 nm with a broad defect-related emission located ataround 505 nm. As shown in Fig. 2(a), for the device underforward bias, slight UV emission peak blueshift due to a band-filling effect [12,13] and redshift due to a raised junction tem-perature at a higher current can be found with increasinginjection current. The competition between the band-fillingand thermal excitation effects was also observed for the deviceunder reverse bias. However, the redshift happened earlier(about j−8j mA) than the forward bias mode (16 mA), becausecarriers are less likely to be confined at the p-AlGaN/i-ZnOand i-ZnO/n-ZnO, which led to a weaker band-filling effect.Notably, the intensity of UV emission under reverse biasis nearly 10 times larger than that under forward bias at thesame injection current, and the FWHM of the emission peakis almost reduced by half. Figure 2(d) shows the room temper-ature (RT) EL spectra of reverse-biased PIN heterojunction at20 mA with the fitted peaks. Considering that the EL spectracannot be fitted well by only two peaks, three peaks are set toresolve the spectra. The Peak i at around 386 nm is confirmedto be from the near-band-edge (NBE) emission of the i-ZnO

layer [8]. The inset image of Fig. 2(d) showed uneven illumi-nation because the carrier mobility of p-type and i-typelayer materials is not high, resulting in uneven current spread-ing. Using built-in potential ∅i � 0.521 eV, applied voltageV a � −40 V, d � 200 nm, εsn � 7.9 × 10−12 F∕m, andεsp � 10.274 × 10−12 F∕m, the total depletion layer widthxd is

xd � xn � xp � xi

�ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffid 2 � 2εsnεsp

q�Na � Nd �2�ϕi − V a�NaN d �Naεsp � Nd εsn�

s� 231 nm:

(1)

Then the depletion width in p-AlGaN was calculated to benearly 31 nm, which is much lower than 200 nm of i-ZnO,inferring that the majority of the depletion region lies in i-ZnO.

Figure 3 illustrates the light emitting and detecting mech-anisms of the reverse-biased device. Some of the injected

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Fig. 3. Energy band diagram of the proposed dual-functioningdevice under large reverse bias for dual-mode operation.

Letter Vol. 44, No. 8 / 15 April 2019 / Optics Letters 1945

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electrons drift across the p-AlGaN arriving at the AlGaN/ZnOinterface, and others from shallow donors recombine with holesin the Mg deep acceptor levels in the p-AlGaN to producePeak ii at 407 nm, consistent with Refs. [12,13]. For the elec-trons arriving at the interface, part of them may be captured bythe oxygen vacancy-related deep-level states near the interface,yielding the broad Peak iii at around 505 nm [14]. Meanwhile,valence electrons in p-AlGaN can tunnel to the conductionband of i-ZnO and recombine with holes, producing the sharpPeak i at 386 nm (ZnO NBE emission). The electrons fromp-AlGaN can tunnel through the thin barrier to i-ZnO,because the Fermi levels of p-AlGaN and i-ZnO gradually sep-arate, and the occupied valence band of the p-AlGaN is at thesame level or higher than the unoccupied conduction band ofthe i-ZnO with the increasing of reverse voltage. Under forwardbias, holes and electrons are concentrated at the interface ofp-AlGaN/i-ZnO and i-ZnO/n-ZnO, respectively, leading toa low overlap ratio of electron-hole wave function and lowradiative recombination efficiency, since the i-ZnO layer isthick. Under reverse bias, holes can tunnel through the i-ZnO/n-ZnO interface into i-ZnO and be amplified by the impactionization [15], which greatly improves the EL intensity by∼10 times, indicating higher external quantum efficiency, whichwas notmeasured, but expected to be lowwhich deserves furtherimprovement.

To clarify the carrier tunneling behavior, the band diagramand carrier concentration at −127 V were simulated byCrosslight APSYS. Since a perfect semiconductor was usedin the model, the reverse operating voltage of the device wasmuch higher than the experimental value which was basedon the semiconductor material with a lot of defects. The wideinterface gap between p-AlGaN and n-ZnO made the electronand hole concentrations in i-ZnO almost zero, while the carriertunneling happened when the voltage decreased to −127 V 0 theconcentrations of the electron and hole increased to a scale of1011 cm−3. Considering that the carriers were injected fromelectrodes at p-AlGaN and n-ZnO, the carriers in i-ZnO couldonly be explained as the tunneling effect, where the electronstunneled from p-AlGaN, and the holes from tunneled fromn-ZnO. The 378 nm NBE emission shown in the inset imageof Fig. 4(b) can also prove the carrier tunneling and recombi-nation behavior. To clarify the impact ionization amplificationof the carrier, the simulation result not considering the impactionization (light on only) was carried out. Under the influence

of impact ionization, the light emission intensity was signifi-cantly enhanced [Fig. 4(d)]. Figure 4(e) showed that the holeconcentration in i-ZnO has increased by more than 1000 timesand should be responsible to the emission enhancement.

Considering the wide bandgap of ZnO and AlGaN, anextremely large reverse bias (normally >500 V) is requiredto have the impact ionization effect for a reverse-biased PN di-ode, which is accompanied with very large current flow. In thiscase, significant current flow and light emission were obtainedwhen the reverse bias exceeds 5 V [see Fig. 1(d)], indicating thatthe interband tunneling process occurred, and this promotedthe carrier multiplication. The numerical calculations alsopresented that the impact ionization effect was essential tothe current flow at reverse bias.

As shown in Fig. 5(a), an obvious photocurrent was ob-served when the heterojunction was excited by 365 nm light.94.2% of the excited light was absorbed by n-ZnO [16], andthe others were absorbed by i-ZnO. Although a low electricfield existed in the n-ZnO layer, the photo-generated electron-hole pairs could be collected and amplified because of thetunneling and impact ionization effect. The photocurrent is0.946 mA at −50 V, while the dark current was 14.748 mA,and obvious light emission can be observed. This emission anddetection dual-function make this heterojunction be able torealize duplex optical communication. Through definition ofthe binary 0 and 1 of emission and detection, as shown inFig. 5(b), the heterojunction can also decode the received illu-mination information while transmitting the information inreal time, completely free of crosstalk. This demo of duplexcommunication can be viewed and experienced in the supple-mental material Code 1, Ref. [17]. Compared to normal for-ward-biased LEDs, this proposed reverse-biased LED can workas a photodetector simultaneously and shows a wider applica-tion scenario.

During EL and PL measurements, a Glan–Taylor prism wasplaced between the sample and the photodetector to resolvethe optical polarization anisotropy [18], showing the resultin Figs. 5(c) and 5(d). Usually, emitted light with an electricvector perpendicular (E⊥c) and parallel (Ekc) to the c-axis of

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Fig. 4. Under reverse bias, (a) the band diagram at −127 V with aninset image about the emission spectrum, and the carrier concentrationdistributions at (b) −30 V and (c) −127 V. (d) Emission spectrum, and(e) electron and (f) and hole concentration of the PIN heterojunctionunder light considering or not considering the impact ionization effect.

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1946 Vol. 44, No. 8 / 15 April 2019 / Optics Letters Letter

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the a-ZnO crystal is defined as transverse electric (TE) andtransverse magnetic (TM) modes, respectively [19]. The TEand TM modes originate from transitions between the conduc-tion band and the heavy-hole band, as well as the crystal fieldsplitting band. When the angle between the prism polarizationdirection and the c-axis of a-ZnO was changed from 0° to 90°,∼3 nm redshifts of the EL and PL emission peak are observed,indicating that the peak wavelength of the TE modes areconsistently larger than those of the TM modes, because thetopmost valence band has not switched to the crystal field split-ting band. The degrees of polarization (DOPs, i.e., ρ) [20] ofthe EL and the PL are 0.23 and 0.33, respectively. Similar tothe Al(In)GaN material, the DOP of the LED with ZnO activelayer decreases as the temperature rises, because the holesincreasingly occupy deeper split-off valence bands, leading tostronger TM light [21]. The lower DOP of EL than that ofPL in this Letter results from the heating caused by electricalinjection. Ascribed to the polarized emission and detectioncharacteristics, through modulation of the polarized informa-tion of the incident light, it is possible to double the bandwidthof data receiving of this duplex optical communication device.

In summary, the nonpolar a-plane n-ZnO∕i-ZnO∕p-Al0.1Ga0.9N dual-functioning heterojunction was fabricatedand investigated. A sharp UV emission peak at around 386 nmfor the PIN heterojunction was observed in the EL spectraunder both forward and reverse bias. The EL emission underthe reverse bias results from the recombination of electron tun-neling from p-AlGaN to i-ZnO and holes ionized in i-ZnOlayer. Photoresponse to the 365 nm light was observed indicat-ing the possible duplex optical communication device. Thepolarized luminescence of the PIN was also studied, and weobtained the polarized light with the DOPs of 0.23 and0.33 for the EL and the PL spectra, respectively. The proposeddual-functioning nonpolar heterojunction device under reversebias provides a valuable basis for the structural design of multi-functional electronics.

Funding. Key Project of Chinese National DevelopmentPrograms (2016YFB0400804); Key Laboratory of InfraredImaging Materials and Detectors; Shanghai Institute ofTechnical Physics, Chinese Academy of Sciences (CAS)(IIMDKFJJ-17-09); National Natural Science Foundation ofChina (NSFC) (11574166, 61377034, 61675079,61774065); KAUST Baseline (BAS/1/1664-01-01); KAUSTCompetitive Research (URF/1/3437-01-01); GCC ResearchCouncil (REP/1/3189-01-01); Director Fund of WNLO.

Acknowledgment. The authors acknowledge thenumerical calculations conducted by Prof. Zi-Hui Zhang atthe Hebei University of Technology.

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Letter Vol. 44, No. 8 / 15 April 2019 / Optics Letters 1947