liu.seSearch for publications in DiVA
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • harvard1
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • oxford
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Exciton Fine-Structure Splitting in Self-Assembled Lateral InAs/GaAs Quantum-Dot Molecular Structures
Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0001-7155-7103
Show others and affiliations
2015 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 9, no 6, p. 5741-5749Article in journal (Refereed) Published
Abstract [en]

Fine-structure splitting (FSS) of excitons in semiconductor nanostructures is a key parameter that has significant implications in photon entanglement and polarization conversion between electron spins and photons, relevant to quantum information technology and spintronics. Here, we investigate exciton FSS in self-organized lateral InAs/GaAs quantum-dot molecular structures (QMSs) including laterally aligned double quantum dots (DQDs), quantum-dot clusters (QCs), and quantum rings (QRs), by employing polarization-resolved microphotoluminescence (μPL) spectroscopy. We find a clear trend in FSS between the studied QMSs depending on their geometric arrangements, from a large FSS in the DQDs to a smaller FSS in the QCs and QRs. This trend is accompanied by a corresponding difference in the optical polarization directions of the excitons between these QMSs, namely, the bright-exciton lines are linearly polarized preferably along or perpendicular to the [11̅0] crystallographic axis in the DQDs that also defines the alignment direction of the two constituting QDs, whereas in the QCs and QRs, the polarization directions are randomly oriented. We attribute the observed trend in the FSS to a significant reduction of the asymmetry in the lateral confinement potential of the excitons in the QRs and QCs as compared with the DQDs, as a result of a compensation between the effects of lateral shape anisotropy and piezoelectric field. Our work demonstrates that FSS strongly depends on the geometric arrangements of the QMSs, which effectively tune the degree of the compensation effects and are capable of reducing FSS even in a strained QD system to a limit similar to strain-free QDs. This approach provides a pathway in obtaining high-symmetry quantum emitters desirable for realizing photon entanglement and spintronic devices based on such nanostructures, utilizing an uninterrupted epitaxial growth procedure without special requirements for lattice-matched materials combinations, specific substrate orientations, and nanolithography.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2015. Vol. 9, no 6, p. 5741-5749
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-118007DOI: 10.1021/acsnano.5b01387ISI: 000356988500013PubMedID: 25965972OAI: oai:DiVA.org:liu-118007DiVA, id: diva2:812751
Available from: 2015-05-20 Created: 2015-05-20 Last updated: 2018-09-05
In thesis
1. Micro-photoluminescence and micro-Raman spectroscopy of novel semiconductor nanostructures
Open this publication in new window or tab >>Micro-photoluminescence and micro-Raman spectroscopy of novel semiconductor nanostructures
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Low-dimensional semiconductor structures, such as one-dimensional nanowires (NWs) and zerodimensional quantum dots (QDs), are materials with novel fundamental physical properties and a great potential for a wide range of nanoscale device applications. Here, especially promising are direct bandgap II-VI and III-V compounds and related alloys with a broad selection of compositions and band structures. For examples, NWs based on dilute nitride alloys, i.e. GaNAs and GaNP, provide both an optical active medium and well-shaped cavity and, therefore, can be used in a variety of advanced optoelectronic devices including intermediate band solar cells and efficient light-emitters. Self-assembled InAs QDs formed in the GaAs matrix are proposed as building blocks for entangled photon sources for quantum cryptography and quantum information processing as well as for spin light emitting devices. ZnO NWs can be utilized in a variety of applications including efficient UV lasers and gas sensors. In order to fully explore advantages of nanostructured materials, their electronic properties and lattice structure need to be comprehensively characterized and fully understood, which is not yet achieved in the case of aforementioned material systems. The research work presented this thesis addresses a selection of open issues via comprehensive optical characterization of individual nanostructures using micro-Raman ( -Raman) and micro-photoluminescence ( -PL) spectroscopies.

In paper 1 we study polarization properties of individual GaNP and GaP/GaNP core/shell NWs using polarization resolved μ-PL spectroscopy. Near band-edge emission in these structures is found to be strongly polarized (up to 60% at 150K) in the orthogonal direction to the NW axis, in spite of their zinc blende (ZB) structure. This polarization response, which is unusual for ZB NWs, is attributed to the local strain in the vicinity of the N-related centers participating in the radiative recombination and to their preferential alignment along the growth direction, presumably caused by the presence of planar defects. Our findings therefore show that defect engineering via alloying with nitrogen provides an additional degree of freedom to control the polarization anisotropy of III-V nanowires, advantageous for their applications as a nanoscale source of polarized light.

Structural and optical properties of novel coaxial GaAs/Ga(N)As NWs grown on Si substrates, were evaluated in papers 2-4. In paper 2 we show by using -Raman spectroscopy that, though nitrogen incorporation shortens a phonon correlation length, the GaNAs shell with [N]<0.6% has a low degree of alloy disorder and weak residual strain. Additionally, Raman scattering by the GaAs-like and GaNlike phonons is found to be enhanced when the excitation energy approaches the E+ transition energy. This effect was attributed the involvement of intermediate states that were created by N-related clusters in proximity to the E+ subband. Recombination processes in these structures were studied in paper 3 by means of μ-PL, μ-PL excitation (μ-PLE), and time-resolved PL spectroscopies. At low temperatures, the alloy disorder is found to localize photo-excited carriers leading to predominance of localized exciton (LE) transitions in the PL spectra. Some of the local fluctuations in N composition are suggested to create three-dimensional confining potentials equivalent to that for QDs, based on the observation of sharp PL lines within the LE contour. In paper 4 we show that the formation of these QD-like confinement potentials is somewhat facilitated in spatial regions of the NWs with a high density of structural defects, based on correlative spatially-resolved structural and optical studies. It is also concluded the principal axis of these QD-like local potentials is mainly oriented along the growth direction and emit light that is linearly polarized in the direction orthogonal to the NW axis. At room temperature, the PL emission is found to be dominated by recombination of free carriers/excitons and their lifetime is governed by non-radiative recombination via surface states. The surface recombination is found to become less severe upon N incorporation due to N-induced modification of the surface states, possibly due to partial surface nitridation. All these findings suggest that the GaNAs/GaAs hetero-structures with the onedimensional geometry are promising for fabrication of novel optoelectronic devices on foreign substrates (e.g. Si).

Fine-structure splitting (FSS) of excitons in semiconductor nanostructures has significant implications in photon entanglement, relevant to quantum information technology and spintronics. In paper 5 we study FSS in various laterally-arranged single quantum molecular structures (QMSs), including double QDs (DQDs), quantum rings (QRs), and QD-clusters (QCs), by means of polarization resolved μ-PL spectroscopy. It is found that FSS strongly depends on the geometric arrangements of the QMSs, which can effectively tune the degree of asymmetry in the lateral confinement potential of the excitons and can reduce FSS even in a strained QD system to a limit similar to strain-free QDs.

Fabrication of nanostructured ZnO-based devices involves, as a compulsory step, deposition of thin metallic layers. In paper 6 we investigate impact of metallization by Ni on structural quality of ZnO NWs by means of Raman spectroscopy. We show that Ni coating of ZnO NWs causes passivation of surface states responsible for the enhanced intensity of the A1(LO) in the bare ZnO NWs. From the resonant Raman studies, strong enhancement of the multiline Raman signal involving A1(LO) in the ZnO/Ni NWs is revealed and is attributed to the combined effects of the Fröhlich interaction and plasmonic coupling. The latter effect is also suggested to allow detection of carbon-related species absorbed at the surface of a single ZnO/Ni NW, promising for utilizing such structures as efficient nano-sized gas sensors.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2015. p. 55
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1731
National Category
Physical Sciences Nano Technology
Identifiers
urn:nbn:se:liu:diva-123939 (URN)10.3384/diss.diva-123939 (DOI)978-91-7685-877-6 (ISBN)
Public defence
2016-02-05, Planck, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2016-01-14 Created: 2016-01-14 Last updated: 2017-03-27Bibliographically approved
2. Spin generation and detection in low-dimensional semiconductors
Open this publication in new window or tab >>Spin generation and detection in low-dimensional semiconductors
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Semiconductor spintronics and opto-spintronics have intrigued intense attention as they promise great advance of contemporary semiconductor information technology with integrated spin functionalities. Over the last few decades, the development of growth techniques and discovery of topological band structures have led to the explosion of a wide range of low-dimensional semiconductor materials, many of which have superior properties compared to their bulk ancestors. The limited dimension of materials imposes constraint on the motion of charge carriers and causes spin interactions of various forms, which have profound influence on the spin properties that are important for various spintronic and/or opto-spintronic applications.

In this context, semiconductor quantum dot (QD) structures (QDS) and 3D topological insulator (TI) have emerged as promising material systems that exhibit distinct spin properties: In QDS, carriers are restricted in all three dimensions. The 3D confinement quenches the spin-orbit interaction (SOI) mediated spin depolarization/dephasing processes and, as a consequence, leads to a prolonged spin relaxation time, which can be used for non-volatile storage or quantum bits in quantum information technology; Whereas, the surface state of 3D TI, on the contrary, has the electronic structure that is dominated by SOI such that the orientation of the electron spin is tied to its momentum. The strong SOI limits the spin relaxation time but can be utilized to generate spin polarized current that is free from backscattering. This thesis work focuses on these two prototypical materials to provide an in-depth understanding of the spin phenomena as well as to tailor their spin properties such that novel spintronic and/or opto-spintronic devices can be built on.

To employ QDS for storage of spin information, first and foremost is to be able to generate and detect spin polarization effectively and efficiently. For this purpose, we have carefully inspected both the spin injection and spin detection processes in various QDS. In this thesis work, spin polarized carriers or excitons are generated via optical orientation that converts the angular momentum of the absorbed photons to the photo-generated carriers or excitons. The as-generated spin polarized carriers/excitons then need to relax their energy before getting injected to the QDS. We have found that the spin injection process is influenced by the interactions with phonons (Paper 1) and disordered environment associated with the injection path (Paper 2). In the former case, we show that the longitudinal optical (LO) phonon contributes to accelerated relaxation of the carrier/exciton energy to the QDS ground state, which preserves the spin polarization. By engineering the energy of the QDS, we can take advantage of such LO-phonon assisted process and can avoid the spin injection loss due to the commonly observed phonon bottleneck effect. In the latter case, we discover that the surrounding media of the QDS is generally disordered, distributed by potential fluctuations caused by alloying or strain randomness. Exciton injection via such localized potential undergoes spin relaxation caused by an anisotropic exchange interaction (AEI), which leads to appreciable spin injection loss at low temperatures.

The AEI is also found to be responsible for the low spin detection efficiency observed in the undoped QDS reported in Paper 3. The AEI causes mixing and splitting of exciton spin states, which leads to not only a low PL polarization degree of the QDS but also a serious issue in generation of entangled photon pairs utilizing QDS. We show that the aforementioned spin injection (Paper 2) and spin detection (Paper 3) loss associated with the AEI can be effectively tuned in the QDS by the arrangement of the constituting QDs. The effect originates from the modification of the strain and shape anisotropy both inside and outside the QDS due to the collective interaction with the neighboring QDs, which introduces a new degree of freedom in electronic-structure engineering of the QDS.

In the doped QDS, we have found that the spin detection efficiency can additionally be affected by the exciton charge states and a hyperfine interaction (HFI) with the nuclear-spin bath. In Paper 4, we discover a dynamic charging process that the charged states of an InGaAs QD ensemble are altered with different excitation power densities and excitation photon energies. The charging effect leads to an anomalous spectral dependence of PL polarization such that the copolarized emission can be dynamically converted to the counter-polarized one. This finding thus calls for caution in the correlation between the optical and spin polarization in QDS with a complex charging environment. The effect of the HFI depends on the condition of nuclear spin polarization. In QDS with an unpolarized nuclear-spin bath, the HFI is a primary electron/exciton spin depolarization/dephasing source in QDS at low temperatures. In Paper 5, we show that the ensemble spin dephasing time of QDs at a cryogenic temperature correlates with the averaged size of QDs. The behavior can be accounted for by electron spin dephasing in a fluctuating nuclear field, which is experimentally verified for the first time. The results thus highlight the important role of the HFI in the electron spin dephasing in the QDs. On the other hand, finite nuclear spin polarization can be achieved through the dynamic nuclear polarization (DNP) process that transfers the angular momentum from the spin-polarized electron to nuclei. DNP is recognized to be important for spintronics and quantum information in nuclear spin-rich nanostructures. This is not only because of its role in suppressing the aforementioned electron spin dephasing, but also because it is behind the idea of exploring the long coherent nuclear spin as a quantum computing qubit. In Paper 6, we have investigated the effect of DNP in a series of QDS, where the strength and orientation of the nuclear field resulted from the DNP are identified and measured. We find that the DNP is built along a tilted axis that deviates from the commonly observed orientation along the QD growth axis and the nuclear field develops a substantial transverse component. This anomalous behavior of the DNP is found to arise from the nuclear quadrupole interaction with an oblique principal axis. The resulting tilting nuclear field can further lead to dephasing and depolarization of the electron spin that has previously been overlooked. The results uncover the detrimental effect rooted in the complex electrostatic environment of the nuclei inside the QDS and call for special care of the strain and alloying engineering of the nanostructures.

In the case of 3D TI, we aim at providing both the experimental and theoretical understanding of the surface spin photocurrent as well as innovations in future opto-spintronic applications utilizing the semiconductor-TI interface. As has been shown earlier, the circular polarized excitation light creates a spin photocurrent that is resistant to moderate scattering. In Paper 7, we present detailed studies of the dependence of the spin photocurrent on the incident angle of the excitation light in a prototypical 3D TI, Bi2Te3. We point out that the spin photocurrent, as a result of spin-selective optical transitions, is associated with both the in-plane and out-of-plane spin texture of the topological surface states. We focus on the contribution of the out-of-plane spin texture, which is less explored, and demonstrate, for the first time, spin injection from a conventional semiconductor, GaAs, to a 3D TI. In favor of this hybrid system, we show that the spin photocurrent contributed by the spin injection exceeds that from the TI alone and the magnitude and direction of the current can be controlled by applying a transverse magnetic field. In Paper 8, we give a tight-binding description of the microscopic origin of the spin photocurrent in Bi2Te3, where we have provided theoretical calculations of the spin photocurrent as a function of the excitation incidence angle, Fermi energy and different scattering potentials. The results explain the observation of the out-of-plane spin texture contribution reported in Paper 7, which should have been forbidden by symmetry, and provide a pathway for opto-spintronic applications based on a TI-semiconductor hybrid system.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2018. p. 58
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1946
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-150938 (URN)9789176852576 (ISBN)
Public defence
2018-09-28, Planck, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2018-09-06 Created: 2018-09-05 Last updated: 2018-09-06Bibliographically approved

Open Access in DiVA

fulltext(935 kB)126 downloads
File information
File name FULLTEXT01.pdfFile size 935 kBChecksum SHA-512
ea5333dd4fb77e929bb62322bf51f7164d9128c81dce1ba632a41cc756c80a3a34789f573f4f247bb014c6a3efd475df6eef430a14b95a14d0399350db4fbe8c
Type fulltextMimetype application/pdf

Other links

Publisher's full textPubMed

Authority records BETA

Filippov, StanislavPuttisong, YuttapoomHuang, YuqingBuyanova, Irina AChen, Weimin

Search in DiVA

By author/editor
Filippov, StanislavPuttisong, YuttapoomHuang, YuqingBuyanova, Irina AChen, Weimin
By organisation
Functional Electronic MaterialsFaculty of Science & Engineering
In the same journal
ACS Nano
Condensed Matter Physics

Search outside of DiVA

GoogleGoogle Scholar
Total: 126 downloads
The number of downloads is the sum of all downloads of full texts. It may include eg previous versions that are now no longer available

doi
pubmed
urn-nbn

Altmetric score

doi
pubmed
urn-nbn
Total: 168 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • harvard1
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • oxford
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf