Bosonic Lasing From Collective Exciton Magnetic Polarons in Diluted Magnetic Nanowires and Nanobelts (ACS Photonics) (2016)

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Article
Bosonic Lasing from Collective Exciton Magnetic
Polarons in Diluted Magnetic Nanowires and Nanobelts
Shuangyang Zou, Muhammad Arshad Kamran, Li-Jie Shi,
Ruibin Liu, Shuai Guo, Alexey Kavokin, and Bingsuo Zou
ACS Photonics, Just Accepted Manuscript • DOI: 10.1021/acsphotonics.6b00289 • Publication Date (Web): 21 Sep 2016
Downloaded from http://pubs.acs.org on September 23, 2016
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Page 1 of 36 ACS Photonics
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7 Bosonic Lasing from Collective Exciton
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Magnetic Polarons in Diluted Magnetic
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12 Nanowires and Nanobelts
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16 Shuangyang Zou1#, Muhammad Arshad Kamran1#, Li-Jie Shi1#, Ruibin Liu1, Shuai
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18 Guo1, Alexey Kavokin2,3* and Bingsuo Zou1*
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22 Beijing Key Laboratory of Nanophotonics & Ultrafine Optoelectronic Systems,
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24 Beijing Institute of Technology, Beijing 100081, China; 2 Physics and Astronomy,
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27 University of Southampton, Highfield, Southampton, SO171BJ, UK; 3 CNR-SPIN,
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29 Viale del Politecnico 1, I-00133, Rome, Italy;
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33 ABSTRACT
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37 Exciton magnetic polarons (EMPs) are self-organized magnetic quasiparticles that
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40 can be formed by excitons in diluted magnetic semiconductors (DMSs). The optical
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42 response of EMPs in DMS microstructures is not yet well understood because it is
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45 affected by many competing factors, including spin-dependent exchange interactions,
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47 phonon coupling, collective and non-linear effects. Here, we report on lasing from
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50 collective EMP states in Co(II)-doped CdS nanowires (NWs) and nanobelts (NBs)
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52 that we interpret in terms of bosonic lasing – the spontaneous emission of radiation by
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55 a single quantum state macroscopically populated by bosonic quasiparticles. The
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57 lasing threshold coincides with the appearance of ferromagnetic domains, indicating
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ACS Photonics Page 2 of 36
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4 an important role of spin ordering in the formation of coherent collective EMPs.
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6 These results pave the way to the realization of a new type of bosonic laser, different
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9 from exciton-polariton lasers, where formation of the bosonic condensate is possible
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11 due to the coupling of EMPs via the exchange interaction of exciton and magnetic ion
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14 spins.
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18 KEYWORDS Exciton magnetic polarons, lasing ， nanobelts and nanowires,
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20 diluted magnetic semiconductors
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55 Formation of collective magnetic polarons and the onset of bosonic lasing in
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5 Carrier-spin interactions are generally considered as the source of ferromagnetism
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in narrow-bandgap diluted magnetic semiconductors (DMS).1, 2
In wide-bandgap
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10 DMS, the transition metal (TM) ions can arrange their spins ferromagnetically if
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sufficient concentrations of spin polarized carriers or excitons are present. The
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15 exchange interaction between carrier (exciton) spins and spins of magnetic ions is
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responsible for the magnetic polaron effect manifested by the self-trapping of carriers
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20 or excitons and formation of small ferromagnetic domains. Magnetic polaron
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23 formation strongly affects the optical properties of DMS. Most bulk DMS crystals do
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25 not exhibit a strong photoluminescence (PL) signal in the case of heavy doping.
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28 Low-dimensional structures, including quantum dots (QDs) and quantum wells
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30 (QWs), are usually better light emitters than are bulk crystals. In DMS QDs, the
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33 impurity ions and photo-induced excitons may couple to each other, forming exciton
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35 magnetic polarons (EMPs), which are manifested in PL spectra as strong resonances
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38 near the bandedge.3-5 EMPs localized at the static disorder fluctuations have also been
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40 observed in QW structures.6 The magnetic polaron effect is likely to be responsible
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43 for light-induced ferromagnetism in colloidal QDs.7 The ferromagnetic alignment of
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45 the localized magnetic ions in the vicinity of a carrier or an exciton is at the origin of
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48 this effect.8 The signatures of EMPs in QWs and bulk crystals are peaks at the lower
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50 energy side of free exciton (FX) emission lines. The red-shift of EMP lines compared
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53 to FX lines is due to the exchange interaction of TM ion spins with spins of excitons.9,
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EMP spectral lines are usually subject to a strong inhomogeneous broadening
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58 caused by the fluctuations in the concentration of impurity ions. Coupled localized
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4 EMPs (LEMPs) in bulk DMS form clusters that can generate coherent spin-polarized
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6 emission at high excitation densities.11, 12
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10 Here, we study diluted magnetic Co(II)-doped CdS nanowires (NWs) and nanobelts
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12 (NBs), where a very strong and broad emission band can be observed at
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15 approximately 540-800 nm. This band is caused by the 4T1(P) → 4A2(F) transition of
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17 Co2+ ions next to its bandedge emission at above-critical concentrations of the dopant.
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20 The temperature dependence of the emission of these structures appears to be
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22 correlated to their magnetic response, up to 373K. The bandedge emission can be
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25 divided into two bands composed of the individual free exciton (FX) band and the
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27 EMP band at low and room temperature, depending on the shape of the wire (belt)
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30 and the dopant concentration. The strong temperature dependences of PL and Raman
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32 scattering spectra indicate a strong longitudinal optical (LO) phonon Fröhlich
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35 coupling effect. The EMP emission band is circularly polarized, that is characteristic
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37 of the ferromagnetic spin alignment. A single-mode lasing at the frequency of the
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40 EMP is observed following optical excitation by ns laser pulses at room temperature.
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42 The lasing threshold is manifested by a dramatic line narrowing and the increase of
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45 the PL intensity at the critical pumping power. The non-linear enhancement of EMP
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47 photoluminescence, suppression of the inhomogeneous broadening of the EPM line
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50 and formation of an intense coherent polarized optical signal are manifestations of the
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52 bosonic lasing in domains of merged EMPs, as we show below.
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4 The exciton Bose-Einstein condensation (BEC) of excitons has been recently
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6 studied in coupled QW structures where a long exciton life-time is assured through
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9 the spatial separation of electrons and holes.13, 14 The spontaneous buildup of the
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11 excitonic coherence has been observed at cryogenic temperatures close to 1 K. On the
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14 other hand, polariton lasers showing non-equilibrium condensates of
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16 exciton-polaritons have been observed at room temperature15. Wide bandgap
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19 semiconductors such as GaN and ZnO are among the most suitable for polariton
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21 lasing at room temperature. Polariton lasing is a special case of bosonic lasing16,
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24 where light is emitted spontaneously by a condensate of bosonic quasiparticles of
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26 photon-excitons. We ever show that ZnO:Mn NWs, where EMPs can form
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29 non-equilibrium condensates even at room temperature in the absence of a magnetic
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31 field, which is why they are excellent candidates for the observation of bosonic lasing
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34 different from polariton lasing.11, 16 It is likely that other wide-gap DMS with large
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36 exciton binding energies may be suitable for bosonic lasing as well. Their
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39 characterization results proved the presence of this point.
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46 Results
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49 Morphology, structure and composition of Co-doped CdS NWs and NBs: The
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51 NWs and NBs were obtained using the VLS growth in CVD method discussed in the
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54 methods section. The morphology of the as-prepared Co-doped CdS NBs is shown in
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Figure 1a. The belt structures are mainly located in the high-temperature region of a
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4 silicon wafer, and the NWs are in the low temperature region. In Figure 1b, the
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6 magnified morphology shows that the surfaces of NBs are clean and smooth, without
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9 any nanoparticle impurities or contamination. The elementary composition of the NBs
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11 was S, Cd and Co according to the energy dispersive X-ray (EDX) analysis (inset of
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14 Figure 1b). The cobalt concentration (atomic %) can be identified by EDX for tuning
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16 from 0 to 4%. The element mapping images are shown in Figure 1c, 1d, 1e and 1f,
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19 which indicate that Co elements are not uniform in a single belt. The detailed XPS
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21 results, as shown in Figure S1, indicate the valence of Co (II) inside the CdS NBs.
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52 Figure 1. (a) low- and (b) high-magnification SEM images of as-prepared
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54 Co-doped CdS NBs. Inset in (b) is the EDX profile measured from a square marked in
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57 (b). (c) Typical SEM image of an individual Co-doped CdS NB, and the rectangular
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4 box indicates the selected area for EDX mapping. (d-f) the elemental mapping images
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6 of Co-doped CdS NBs for the detected elements: S, Cd and Co in figure 1(c).
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13 The XRD pattern of these NWs and NBs indicates a Wurtzite structure, as shown in
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Figure S2a. The Raman spectra of CdS powder，undoped and individual doped NBs
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18 (as shown in Figure S2b，c，d) also reflect the phonon modes of a Wurtzite CdS lattice.
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The intensity ratio of 2 LO of A1 mode to the 1 LO mode (in Table S1) usually
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23 represents the linear electron–phonon coupling strength in a Wurtzite lattice.17 This
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ratio, i.e., an overtone enhancement, can be observed in the NBs and NWs compared
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28 with the reference spectra of CdS powder. Co ion doping can lead to further
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enhancement of this overtone, inducing also a slight shift of the phonon modes. This
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33 indicates a clear enhancement of the Fröhlich electron-phonon coupling in the doped
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semiconductor nanostructures that might affect their electronic properties.
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39 Photoluminescence properties of NBs and NWs: Figure 2a shows room
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41 temperature PL spectra of Co-doped CdS NB excited by a 405 nm line of a CW
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44 semiconductor laser. The PL spectrum of pure CdS NB with a regular shape shows
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46 Upon Co (0.91%) incorporation, a bandgap peak centered at 513.6 nm (green) can be
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49 found with a reduced intensity, and a band centered at 606.5 nm (red) appears due to
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51 the d-d transition 4T1(P) → 4A2(F) between Co ions.18 As the doping concentration
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54 increases from 0.91% to 2.92%, the bandedge red shifts from 513.6 to 516.5 nm, and
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the red band shifts from 606.5 to 620.5 nm. This red shift in the green and red
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4 emission bands is related to the doped Co+2 cations and their coupling.18, 19
For
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6 comparison, pure CdS belt emission have also been measured. A very strong
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9 bandedge emission band centered at 508 nm was obtained. No obvious surface states
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11 related to or sulfur vacancy emissions within the gap could be found, indicating the
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14 high crystal quality. To confirm the origin of the red emission band in doped CdS NB,
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16 we use a 532 nm laser to excite the doped NB. Aan emission band centered at 620
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19 nm without the anti-Stokes band at the bandedge was obtained and shown in Figure
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21 S3a. So we conclude that the 620 nm band should be related to Co ions set in a CdS
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24 lattice because a 532 nm laser mode can only excite certain d levels of the Co ion in
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26 the sulfide lattice if the phonon-assisted anti-Stokes bandedge emission is not
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29 induced.
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32 Figure 2b shows the micro-PL spectra of single Co doped NW obtained using the
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35 405 nm laser excitation, the bandedge(green) and in-gap emissions(red) can also
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37 show up as that in NB. Its spectral profile is strongly related to the excitation location
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40 or doping uniformity under the same excitation power. The in-gap state emission can
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42 only be found in NWs or NBs with Co concentrations above 0.8% and could be
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45 enhanced with increasing Co ion concentration. The higher the Co concentration, the
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47 larger the redshift of the bandedge and Co d-d transitions.
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51 Ferromagnetic coupling between neighboring transition metal ions in a
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53 semiconductor lattice leads to a redshift of the d-d band 19 and it is also instrumental
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56 to the formation of localized EMP. In CdS:Mn NBs, a significant redshift d-d
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4 transition from 575 nm to even 800 nm was detected as a result of the ferromagnetic
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6 aggregates of (MnS)n ions forming inside CdS.20 For the CdS:Co belt, although this
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9 d-d transition in the visible light range occurs to a high d level but not the lowest
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11 excited level, the ferromagnetic coupling between neighboring Co ions can lead to a
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14 long-lifetime high d level, which can emit light due to its relaxed transition rule.
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16 This phenomenon is often termed “intrashell emission.” 21
The effect of this
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19 interaction can also be verified via ab initio calculation.22
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22 Low-temperature micro-PL spectra: The ferromagnetic interactions of Co2+
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25 dopants in the host CdS can produce EMP, whose emission band in bulk DMS can
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27 often show up parallel to FX and manifests at low temperature in past view.10 Thus,
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30 the low-temperature micro-PL of doped NBs are useful, and so obtained in Figure
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32 2c and 2d. This belt has a Co high doping concentration to 2.92%, in which the in-gap
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35 state emission (red) is dominant and bandedge emissions are minimal at room
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37 temperature. However, at the low-temperature its green PL band transform into a clear
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40 double bands, which is discussed in next section.
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25 Figure 2. The PL spectra of CdS:Co nanostructures under 405nm CW laser excitation.
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2a and 2b show the respective PL spectra of CdS:Co nanobelt and nanowire with
28 different doping concentration (0.89% and 1.96% ) under 405nm excitation(the inset
29 is the optical morphology and luminescence morphology). 2c shows the temperature
30 dependent PL spectra (peak locations) of FX and EMP at different temperatures
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32 (83-373K), and the separation and convergence of FX and EMP due to the phonon
33 contribution and polaronic nature. 2d shows the PL emission peak near 600nm due to
34 d-d transitions with ferromagnetic coupling, almost no shift in the temperature range
35 of 80-373K.
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41 The entire PL spectra can be classified into two parts: the green band around the
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44 bandedge and the red band for all doped NBs and NWs. In the green emission in
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46 fig.2c, the band can be reasonably assigned to the free exciton(FX) and related
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49 interactions with phonons and spins, which is called exciton magnetic polaron(EMP).
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51 Because of the crystal field and spin-orbit interaction, the valence band of CdS was
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54 split into three subbands, which form three exciton resonances characterized by
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different energies, namely, A-exciton (2.5535 eV), B-exciton (2.5675 eV), and
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4 C-exciton (2.629 eV). The emission peak at 486.6 nm in Figure 2c (83K), very close
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6 to the energy of the A-exciton of Wurtzite CdS structure, can be assigned to FX
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9 emission in this study. The next peak at 83K is located at 491.1 nm, with a
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11 separation to FX of 25 meV. This energy is less than that of the A1 LO phonon
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14 mode (38 meV) of Wurtzite CdS. Therefore, this emission peak cannot be assigned to
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16 a LO phonon replica emission, i.e., phonon scattering.23 To reveal its origin by
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19 Co-doping , we also did the temperature-dependent PL spectra of a pure CdS NB,
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21 which was shown in Figure S3b. The emission peak at 491.1 nm for Co doped one at
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24 low temperature did not show up for pure CdS NBs at the same temperature . Hence,
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26 it originates from Co(II) ion interactions with the exciton in CdS. For its lower
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29 energy and larger FWHM than that of FX we identified the 491.1 nm peak as an
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31 EMP, because only the ferromagnetic coupling of multi-Co ions can reduce the FX
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34 energy.10
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37 Based on the temperature dependent PL in Figure 2c, EMP and FX can coexist
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40 independently at 77 K and up to 233 K. Their temperature-dependent intensities are
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42 shown in Figure S3c and S3d, from which it is seen that the EMP have a different
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45 temperature dependent profile from that of the FX in doped and pure belts. This
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47 difference lies that the FX emission is related to phonon scattering, while the EMP
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50 emission has relations to the ferromagnetic couplings. Their temperature dependences
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52 differ, as well as their spatial distributions within the belt. Above a critical
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55 temperature(223K), the EMP in this belt combines with its FX (in Figure 2c) to
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57 produce a merged emission band (511-518 nm) that redshifts with increasing
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4 temperatures. Such double band emission characteristics can also be observed in
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6 ZnO:Mn NWs at room temperature,24 indicating a common profile in the diluted
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9 magnetic semiconductors, which have not been identified before. Moreover, such
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11 double-band(FX and EMP) emissions aound bandedge can be more easily detected
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14 in NBs doped with less than 0.8% Co(II) ions, even at room temperature. Clearly, the
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16 separation between EMP and FX is related to the aggregate number of Co ions. In the
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19 case of pure CdS belt, the PL peak becomes red -shifted from 487.5 nm to 514 nm
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21 as the temperature rises from 77 K to 323 K, accompanied by an decreasing
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24 intensities. This phenomenon is due to the well-known Fröhlich exciton-phonon
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26 coupling in wide bandgap semiconductors. The bulge in the EMP I-T profile is
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29 supposed due to the local magnetic phase transiton or FX-EMP transformation
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31 processes, which can be seen in the I-T profile of local EMP(d-d transition) in fig.s3d.
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34 The bandedge peak energy demonstrates that the PL of a pure CdS NB follows the
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36 Varshni-like temperature dependence, 23, 25
agree well with the result in fig.s3c. A
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39 composite FX-EMP-phonon state near the bandedge at high temperature also follows
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the Varshni-like temperature dependence, as shown in Figure S3c. In contrasting to
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44 the shift of EMP and FX, the energy of red PL band is blue shifted by only 12 nm as
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the temperature is decreased from 373 K to 77 K. This is also different from that of
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49 the deep defect emission. In addition, its PL intensities decrease non-uniformly from 77
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to 273K, as shown in Figure S3d. If this band originates from the defect-related
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54 emission, its intensity should rapidly decrease at some low temperature. In this case, a
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much stronger red emission band occurs at 77 K compared to at 373 K, similar to the
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4 magnetic response with temperature, from which one can conclude that this red
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6 emission band belong to ferromagnetically coupled Co d-d transitions in CdS NBs,
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9 identified as a localized EMP(LEMP).
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15 The PL lifetime decay profiles of Co-doped CdS NWs at 511.7 and 620.5 nm
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18 emissions are studied, as presented in Figure S4a and b，which show lifetimes of 0.51
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± 0.005 ns for emission at λem = 511.7 nm and of 0.53 ± 0.02 ns (17%) and
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23 45.03 ± 0.7 ns (83%) for emission at λem = 620.5 nm. The lifetime obtained at 511.7
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nm includes contributions from FX and EMP decays in Co(II)-doped CdS NWs. If the
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28 FX and EMP are separated in some belts, the EMP lifetime is 1.3-1.63 ns, longer than
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that of FX at 0.23-0.5 ns, like that in ZnO:Mn NW 24 and ZnMnSe/ZnSe QW 26. This
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33 indicates that EMP has a longer lifetime than FX. Both FX and EMP lifetimes are a
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little shorter than that of LEMP, indicating a d-d transition rate, but not long lifetime
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38 deep traps.
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41 Polarized EMP in PL spectra: Figure 3a shows the room-temperature emission
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44 spectra of the belt with a varied local Co concentration (0.1-0.8%). The coexistence of
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46 two bands (FX at 508 nm and EMP at 519 nm) can be observed even at room
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49 temperature. Note that the two separate bands have never been observed
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51 simultaneously in QD samples.5, 7
This indicates that FX and EMP are spatially
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54 separated in doped belts; they can coexist in a sufficiently large crystal system, like
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belts. This offers us an opportunity of studying their optical properties separately and
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4 independently. Under high doping conditions, they always merge into one band at
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35 Figure 3. (a) The room temperature PL spectra of a belt (The right inset is the
36 bandedge emission composed of FX and EMP and the left inset is their optical
37 morphology and luminescence images). (b) and (c): The polarized spectra of
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39 differently belts (the vertical axis is the relative intensity of PL to the FX PL intensity
40 under 0 angle polarization). The inset shows the intensity ratio of peak 2/ peak 1 with
41 polarization angle and the corresponding optical morphology image of doped belt, the
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polarization change depending on the angle and initial location, but not morphology.
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44 (d) The schematic of spatial distributions of the FX and EMP with fixed-spin and
45 dipole in the lattice of a CdS:Co belt. The green oval is FX distributed randomly on
46 the surface and inner belt. The red oval represents EMP with fixed spin direction
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exists in the belt.
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The polarized spectra of a Co-doped CdS NB with irregular shapes were shown in
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56 Figure 3b and 3c. There are several stripes can be seen in the optical images as shown
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4 in their insets. FX, emission is seen to be unpolarized at room temperature; but EMP
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6 exhibits a strong polarization at a special angle range(90-115°in fig.3b and
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9 60-170° in fig.3c). This angle change has no relation to the lattice orientation of
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11 the belt, and the angle range also varied with different belt, so these phenomena
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14 indicate the existence of fixed EMP dipole in the belt. Its dipole stays where
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16 theferromagnetic coupling of ions leads to the formation of ferromagnetic domains 12,
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19 in different belts, because the parallel spin orientation form ferromagnetic
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21 domains. Although no direct relationship between this polarization and the shape of
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24 NBs at a scale greater than micrometers is found, the EMP polarization, in contrast to
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26 FXs, can be easily identified experimentally.20 In the previous work, it was found that
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29 the ferromagnetically aligned spins of neighboring ions lead to the head-tail spin
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31 alignement of a chain of EMPs under photoexcitation, whose emission band redshifts
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34 in micrometer-sized DMS structures.30 The ferromagnetic spin alignment of
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36 neighboring doping ions can keep at room temperature. Therefore, based upon the
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39 change of emission polarization and wavelength location of the second emission peak,
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the EMP formation in in irregular belts can be identified.
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45 EMP lasing in NBs: The lasing experiment from a nano-belt has been carried out
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47 using a 2 ns laser excitation of 355 nm from a YAG:Nd laser. Exciting a CdS belt
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50 with 0.1-0.68% Co(II) doping concentrations we can observe a lasing line at
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52 approximately 518 nm at sufficiently high excitation power, as shown in Figure 4a.
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55 The line width and intensity have strong dependences on the excitation power (as
56
57 shown in Figure 4b). Beyond the threshold power of 7.4μj, we can see a superlinear
58
59 15
60
1
2
3
4 increase of the emission intensity. This coincides with a pronounced band narrowing.
5
6 Despite of the inhomogeneous distribution of the dopant in the belts, a single lasing
7
8
9 mode always occurs at the EMP location. The lasing line intensity at even high
10
11 excitation is not so large as shown in fig.4 over 16μj, that means there are other
12
13
14 effect may start to be involved, like exiton – carrier or phonon interactions.
15
16
17 The steady-state PL spectra of a belt include a two-band emission near the
18
19
20 band-edge, which are always located at the 508-510 nm zone for the first band (FX)
21
22 and at the 518-525 nm for the second band (EMP) at room temperature. In fig.4, the
23
24
25 EMP emission band gradually becomes dominant, single peaked and narrow and also
26
27 exhibits a small redshift with increasing excitation power produced by a ns laser pulse.
28
29
30 Their energy span is often close to the 2 LO A1 phonon energy or slightly higher,
31
32 which indicates that EMP formation requires phonon polarization involvement.31, 32
33
34
35 Moreover, these EMPs with definite spin orientation can polarize more FXs into
36
37 ordered EMP aggregates, which behave coherently to produce lasing line as well as
38
39
40 phonons. Clearly, Co ions with a ferromagnetic coupling order provide significant
41
42 carriers and drving forces to complete this collective emission processes, similar to
43
44
45 Mn ions in the ZnO:Mn NWs11, 24. The difference lies in the excitation pulse width
46
47 and morphology in ZnO:Mn NWs, whose EMP lasing line can only be excited by fs
48
49
50 laser pulses,24 whereas a CdS:Co belt can do by both ns and fs lasers. This
51
52 difference indicates that the EMP in the latter should have a larger coherence length
53
54
55 and coherence time because ns laser excitation can cover more microscopic
56
57 interactions, such as exciton-exciton, exciton-phonon, exciton-carrier and exciton-spin,
58
59 16
60
1
2
3
4 inside the excitation zone, while these interactions exist in variable timescales. If
5
6 exciton–carrier interaction is efficient as in fig.s4c, the PL emission is broad and the
7
8
9 lasing profile give multi-mode emissions due to the optical cavity mode selection,
10
11 which have been reported in early publications.33,34 If exciton–carrier interaction is
12
13
14 negligible at low TM ion doping, these interactions would only keep their bosonic
15
16 natures ; therefore, this EMP lasing due to spin correlation occurs not only in a CdS
17
18
19 NW of definite length but also in the irregular shapes of belts of several micrometers.
20
21 That is to say, EMP formation facilitates the bosonic interaction and coherence in a
22
23
24 micrometer DMS belt.
25
26
27
28
29
30
31
32
33
34
35
36
37
38
39
40
41
42
43
44
45 Figure 4a display the PL spectra from spontaneous emission to stimulated emission
46 when excited by nanosecond pulse laser (355 nm). The PL emission intensity and
47
FWHM is extracted and plotted as a function of pumping power (Figure 4b). When
48
49 the excitation intensity was below the threshold, a broad spontaneous emission band
50 was observed which shows a linear increase with excitation power (Figure 4b), while
51 the pumping power was larger than the threshold, the emission intensity showed a
52
superlinear increase with the excitation power. Moreover, the width at half maximum
53
54 (FWHM) become narrower when increasing the pumping power (Figure 4b).
55
56
57
58
59 17
60
1
2
3
4 Magnetic response of Co-doped NWs and NBs: Figure 5a shows the
5
6 magnetization (M) of Co-doped CdS NBs as a function of the applied magnetic field
7
8
9 (H) ranging from −10000 to 10000 Oe. The inset is the magnified area near zero
10
11 magnetic fields. In all cases, the diamagnetic response of the substrate Si wafer has
12
13
14 been removed. The M-H curves show good magnetic hysteresis loops, clearly
15
16 indicating the ferromagnetic behavior of these belts. From the M–H curves, the
17
18
19 coercive field (Hc) and remnant magnetization values are higher than those measured
20
21 at room temperature and reveal a temperature-dependent magnetization. Hc at 10 K is
22
23
24 210 Oe at ~2.92% Co doping, comparable with other DMS materials. To determine its
25
26 Curie temperature, we also measured the M-T curve by applying a magnetic field H =
27
28
29 150 Oe, as in Figure 5b. The magnetization slowly decreases with increasing
30
31 temperature, as expected for a ferromagnet with a Curie temperature above 350 K; It
32
33
34 is easily seen that the M-T profile has a similar profile of EMP emission intensity
35
36 versus temperature, proving the relations of ferromagnetism and EMP emissions in
37
38
39 the belt. It is difficult to extract the exact value as it falls beyond our measurement
40
41
range. For the spin-carrier interactions, one cannot obtain the Tc above room
42
43
44 temperature.30 Therefore, the ferromagnetic coupling between Co ions may represent
45
46
the origin of ferromagnetism above room temperature and can bind with excitons to
47
48
49 form EMP and LEMP after photoexcitation, thereby emitting light and producing
50
51
52
lasing.
53
54
55
56
57
58
59 18
60
1
2
3
4
4 8
5 (a) (b)
M a g n etiza tio n x 1 0 -5 (em u )

6 3
M agn etiza tion x10 -5 (em u )

7 2 10K
8 100K 7
1
9 300K
0
10
M a g n etiza tio n x 1 0 -5 (em u )

0.5
11 -1 6
0.0
12 -2
13 -3 -0.5
H=150 Oe
14 -200-150-100 -50 0 50 100 150 200
-4 Field (Oe)
5
15 -10000 -5000 0 5000 10000 0 50 100 150 200 250 300 350
16 Temperature (K)
Field (Oe)
17
18
19 Figure 5. Magnetic properties of the as-grown Co-doped CdS nanobelts measured by
20
21 SQUID. (a) The M-H curves of Co-doped CdS NBs at 10, 100, and 300 K. Inset is the
22
23
24 Magnified area near the zero magnetic field of M-H curve. (b) the M-T curve of
25
26 Co-doped CdS nanobelts.
27
28
29
30
31
32
33 Modelling
34
35
36
37
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54 Figure 6 the calculated DOS of bandedge and ingap d state (between 5 and -5eV) for the
55
56 CdS with single Co, two Co ferromagnetic coupling (FM), and two Co antiferromagnetic
57
58
59 19
60
1
2
3
4 coupling(AFM). The EMP formation has relation to that Co ferromagnetic coupling with FX in
5
6 the lattice and influence the bandedge of DMS (see red line).
7
8
9
10
11
12
13 The energy band structures and DOS of CdS:Co have been calculated by VASP
14
15 software. Figure S5 shows the unit cell, band structures and DOS of the NB
16
17
18 containing one Co ion in a CdS 332 cell(a)，two ferromagnetic (FM, (b))，and two
19
20
antiferromagnetic (AFM(b)) coupled and two Co ions at neighboring locations in the
21
22
23 CdS 332 cell, respectively. From the band structure in figure S5c，S5d, S5e and S5f,
24
25
the energy dispersion of d state is often narrow. In figure 6, the total DOS of the d
26
27
28 state of the two FM coupled Co ions in one unit cell below the Fermi level (at
29
30
approximately -0.5 eV) (red line) has a clear shift to the Fermi level, and the DOS of
31
32
33 the two AFM coupled Co ions (green line) shows a minimal shift further to the Fermi
34
35
36
level. The DOS of the two FM coupled Co ions above the Fermi level (at
37
38 approximately +0.5eV) has a strong shift to the Fermi level, and the DOS of the two
39
40
41
FM coupled Co ions and single Co ion remain nearly fixed; moreover, the two FM
42
43 coupled Co ions and the single Co ion show a one-band DOS profile in the +0-1 eV
44
45
46 range, whereas the FM Co-ion-doped CdS shows a three-peak profile. For the Co FM
47
48 coupled CdS, the magnitude of the s, p state components from S and Cd increased by
49
50
51 approximately one order of magnitude for the system with AFM coupled Co ions and
52
53 single Co-doped CdS (refer to table S2). This indicates an enhanced sp-d
54
55
56 hybridization in this energy area.22 These DOS variations near the Fermi level then
57
58
59 20
60
1
2
3
4 produced a significant modification of its optical transition, which may be reflected
5
6 by their optical emissions of d-d transitions.
7
8
9
10 The observed redshift of the bandedge and in-gap state emissions with the
11
12 increasing Co concentration and clear red emission in Co-doped CdS NBs is in a good
13
14
15 agreement with the above DOS calculation results. This reflects that fact that the Co
16
17 ions inside the CdS lattice prefer the ferromagnetic coupling in the DMS, and its EMP
18
19
20 formation brings the redshift of bandedge; during this type of coupling, sp-d
21
22 hybridization is strengthened. Based on the latter situation, the LO polarizability of
23
24
25 excitons acts in favor of the spin polarization of the magnetic environement.31, 32
26
27 Moreover, the ferromagnetic spin-spin coupling of doped Co ions stabilizes the EMP
28
29
30 and LEMP states in Co-doped CdS crystal.
31
32
33
34
35
36 Discussion
37
38
39
40 We have demonstrated the EMP formation due to the exchange interaction of FX
41
42 spin with Co ion spins with the ferromagnetic alignments. The EMP emission is
43
44
45 strongly amplified and it acquires coherence characteristic of laser emission above
46
47 some threshold excitation power. We interpret these phenomena in terms of bosonic
48
49
50 lasing. Coupling between partially delocalized EMPs through their exchange
51
52 interaction with the magnetic ions leads to the formation of a collective magnetic
53
54
55 polaron state, that is a bosonic state with the occupation number significantly over 1.12,
56
57 28
The phonon assisted scattering of exciton to this state is stimulated by the
58
59 21
60
1
2
3
4 occupation number, that leads to formation of a non-equilibrium Bose-Einstein
5
6 condensate similar to those observed in polariton lasers. Note that we are not working
7
8
9 with microcavities, and the system is not in a strong exciton-photon coupling regime.
10
11 Nevertheless, out of equilibrium bosonic condensates are formed in our system, and
12
13
14 they manifest themselves by a coherent spontaneous emission and magnetic ordering.
15
16
17 The formation of a collective EMPs and a bosonic lasing mode in a ferromagnetic
18
19
20 domain are illustrated in Figure 7. The factors that affect the collective EMP
21
22 formation in our structures are: 1) the presence of dopant Co ions enhances the
23
24
25 strength of exciton coupling with A1 phonons, that helps the exciton energy relaxation
26
27 and exciton orientation.12, 13 2) neighbouring Co ions are subject to ferromagnetic
28
29
30 coupling, which is at the origin of formation of ferromagnetic domains triggered by
31
32 the EMP formation and collective action.28, 29 3) Accelerating annihilation of FX
33
34
35 and stimulated scattering of the collective EMP states come from the growth of
36
37 ferromagnetic domains and non-equilibrium exciton condensates.35 4) The 2 LO
38
39
40 modes of A1 phonons polarized along the c-axis in Wurtzite CdS structures provide an
41
42 efficient coupling of FXs, facilitate the FX conversion into EMPs and formation of
43
44
45 the collective coherent emission states.32 5) II-VI semiconductors have high exciton
46
47 binding energies and even enhanced EMP. For example, Wurtzite CdS crystals have a
48
49
50 free exciton binding energy of 30 meV.36 The polaron energy from the combined 2
51
52 LO phonon and spin polarizations can reach >74 meV during EMP formation; hence,
53
54
55 the total binding energy of the EMP in CdS:Co can be greater than 104 meV,
56
57 substantially larger than kT at room temperature. Therefore, such stable and polarized
58
59 22
60
1
2
3
4 EMPs can be easily coupled and then dynamically become a condensate at high
5
6 density in a micrometer structure, fianlly for bosonic lasing.
7
8
9
10 We underline, that there is no Bose-Einstein condensation in our system: a critical
11
12 temperature for the equilibrium phase transition would be too low. In this respect, our
13
14
15 study strongly differs from the previous studies on the spontaneous coherence build
16
17 up in condensates of spatially indirect excitons and magneto-excitons37-39. In our
18
19
20 samples, primarily, classical condensates are formed in the real space. It is important
21
22 that in our belts, EMPs have a longitudinal polarization. The spin-spin coupled
23
24
25 head-tail-head-tail exciton connection provides an attraction force that is enhanced
26
27 due to the ferromagnetic ordering of the magnetic ion spins between individual
28
29
30 EMPs.40,41 This helps stability of EMPs and facilitates formation of collective states.
31
32 The classical condensation and a subsequent stimulated scattering of FX to the
33
34
35 collective EMP states lead to formation of bosonic condensates that emit a coherent
36
37 light spontaneously.42, 43
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55
56
57
58
59 23
60
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
25
26
27
28
29
30 Figure 7. Formation of collective magnetic polarons and the onset of bosonic
31
32 lasing in CdS:Co belts.
33
34
35
36
37
38
39 Conclusion
40
41
42 High-quality 1D-Co-doped CdS NBs have been prepared through a thermal
43
44
45 evaporation method. We observe three correlated effects in the belts: formation of a
46
47 exciton magnetic polaron state, exciton-induced ferromagnetic d-d transitions and
48
49
50 bosonic lasing from a collective EMP mode. We argue that the exchange interaction
51
52 between carrier and magnetic ion spins results in the formation of EMPs in our system.
53
54
55 The EMPs merge due to the overlapping tails of the carrier wavefunctions and form
56
57 large clusters at rising excitation power, which may be referred to as collective
58
59 24
60
1
2
3
4 magnetic polarons. Due to reduced dimensionality of the structures that we studied
5
6 (NWs and NBs), these clusters also merge, thereby forming quite large ferromagnetic
7
8
9 domains. We observe signatures of these domains both in the polarized
10
11 photoluminescence and in direct measurements of the magnetization of the samples
12
13
14 via SQUID. Most interestingly, the large collective exciton magnetic polaron states
15
16 formed in this way exhibit a pronounced bosonic behavior. We observe bosonic lasing
17
18
19 from EMP modes that is fed by the stimulated scattering of free excitons to these
20
21 modes mostly via exciton-2LO phonon interactions. The lasing is accompanied by a
22
23
24 dramatic narrowing of the PL line, whose intensity exhibits a strongly superlinear
25
26 increase as a function of the pump power. Because there is no external or internal
27
28
29 uniform optical cavity in the system that we studied, the stimulation could not
30
31 originate from the optical mode. The only possible mechanism of lasing in this case is
32
33
34 bosonic lasing collective EMPs, similar to the polariton lasing studied in
35
36 semiconductor microcavities. The stimulated scattering of excitons into the collective
37
38
39 EMP mode is followed by spontaneous emission of light by an exciton condensate,
40
41
therein producing monochromatic and coherent light. Bosonic lasing from collective
42
43
44 EMP states can be used as a coupling interface between magnetic memory and optical
45
46
circuits in computers and communication networks.
47
48
49
50 ：
Methods：
51
52
53 Co-doped NW and NB growths. Co-doped CdS NBs were prepared using a
54
55
56 CVD method in a horizontal tube furnace (HTF). A 1 g mixture of CdS (99.999%,
57
58
59 25
60
1
2
3
4 Alfa Aesar) and Co(OH)2 (99.5%, Alfa Aesar) powders used as precursors was loaded
5
6 in a ceramic boat and inserted into the central region of a quartz tube. First, some
7
8
9 silicon (001) pieces were ultrasonically cleaned in acetone, ethanol and deionized
10
11 water for 15 minutes. Then, a layer of Au (~5 nm thickness) thin film was deposited
12
13
14 onto silicon wafers using a sputtering method. Then, the silicon substrates were
15
16 placed in the downstream position 6–8 centimeters away from the center of the quartz
17
18
19 tube. After sealing the HTF, the tube was heavily flushed with high-purity Ar
20
21 premixed with 10% hydrogen for 1 hour. For the chemical reaction, the precursors
22
23
24 were heated to 750 °C at a rate of 70 °C/min, and synthesis proceeded at this
25
26 temperature for 30 min with a constant gas (90% Ar + 10% H2) flow of 10 sccm
27
28
29 (sccm: standard cubic centimeters per minute). After the reaction, yellow colored
30
31 Co-doped CdS NBs were deposited onto the silicon wafers.
32
33
34
35 Structural and morphological characterizations. The morphology and
36
37 composition of the samples were characterized via scanning electron microscopy (FEI,
38
39
40 QUANTA-250). The compositions and chemical bonding states of the samples were
41
42 determined by X-ray photoelectron spectroscopy (XPS; VG Scientific
43
44
45 ESCALAB-210 spectrometer, East Grinstead, UK) with monochromatic Mg Kα
46
47 X-rays (1,253.6 eV). The phase purity of the product was examined via XRD using an
48
49
50 X-ray diffractometer (Brucker D8-advance) with Cu Kα radiation, therein maintaining
51
52 the operating voltage and current at 40 kV and 40 mA, respectively. 2θ ranged from
53
54
55 30 to 55° with a step of 0.02° and a count time of 2 s.
56
57
58
59 26
60
1
2
3
4 Micro-Raman and PL spectra and imaging: Raman spectra were obtained using a
5
6 spectrometer (LABRAM-HR, JY, Horiba) with the 514.5 nm line of an Ar+ laser
7
8
9 with 30 mW of optical power for a single NW or NB using a laser cofocal optical
10
11 microscope system. Scattered radiations were collected at an angle of 90°with
12
13
14 respect to the excitation beam. The reported wavenumbers are believed to be
15
16 accurate to ±2 cm-1. The PL, polarized PL and lasing spectra were also measured
17
18
19 by the same laser confocal PL microscopy (Horiba JY iHR550, Olympus BX51 M)
20
21 device using a 405 and 532 nm continuous wave (CW) semiconductor laser as an
22
23
24 excitation source. The single nanowire or nanobelt are excited on the sample plate
25
26 in the Microscopy. For the low-temperature PL measurements, the sample was
27
28
29 placed in a microscope cryostat. Liquid nitrogen was used to cool the samples down
30
31 to 77 K. The PL lifetime decay profile was recorded by a time-correlated
32
33
34 single-photon counting (TCSPC) system (Picoquant ‘Timeharp 200’) along with
35
36 narrow-bandpass filters at 510 and 620 nm on the same optical microscope system.
37
38
39 A 405 nm pulsed diode laser (pulse width of tens of ps) was used (Picoquant ‘PDL
40
41
800-B’, 10 MHz-80 MHz) as the excitation source. All results are collected on
42
43
44 excitation on one nanowire or nanobelt. The data obtained in Figure 4e-f were fitted
45
46
by single exponential and biexponential decay functions using the Matlab
47
48
49 deconvolution function. The lasing spectra of the belts were obtained using a 2 ns
50
51
355 nm laser from a YAG laser for excitation, for the laser pulse is illuminated on
52
53
54 the belt on the objective table of the microscope in a tilt way, its excitation power is
55
56
57
scaled by the total energy of a pulse for simplicity.
58
59 27
60
1
2
3
4
5
6
7 Magnetization measurement: The measurements of the magnetization (M) as a
8
9
10 function of H were realized using a superconducting quantum interface device
11
12 (SQUID) magnetometer in the range −1 ≤ H ≤ 1 T. All magnetization
13
14
15 measurements were performed in the presence of an in-plane magnetic field on the
16
17 massive sample on the silicon wafer substrate. The measured magnetization data were
18
19
20 corrected by accounting for the diamagnetic contribution from the substrate. The
21
22 2.93% Co-ion-doped CdS NBs were used for this measurement.
23
24
25
Energy band and d-state calculation: VASP version 5.2 was used to calculate the
26
27
28 band structure and d-state energy dispersion in the Co-doped CdS crystal with varying
29
30
Co ion concentrations in a CdS unit cell.
31
32
33
34 ASSOCIATED CONTENT
35
36
37 Supporting Information
38
39
40
The Supporting Information is available free of charge on the ACS Publications website at
41
42
43 DOI:
44
45
46
47
48
49
50 ：
AUTHOR INFORMATION：
51
52
53 Corresponding Author，E-mail: zoubs@bit.edu.cn， phone： 86-10-68910204
54
55
56 ACKNOWLEDGMENTS
57
58
59 28
60
1
2
3
4 The authors thank the 973 project (2014CB920903) of MOST for financial support.
5
6 Some results on the structures, composition, physical properties and energy band
7
8
9 calculation of CdS:Co nanostructures are included in the supporting information file.
10
11
12 Notes
13
14
15 The authors declare no competing financial interests.
16
17
18
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Bosonic Lasing From Collective Exciton Magnetic Polarons in Diluted Magnetic Nanowires and Nanobelts (ACS Photonics) (2016)

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