Efficient charge transfer induced organic/inorganic based hybrid heterojunction of Ppy/GaN nanorods for high-performance self-powered UV photodetection
Dr. Jim Hwang presents an overview of his program, GHz-THz Electronics, at the AFOSR 2013 Spring Review. At this review, Program Officers from AFOSR Technical Divisions will present briefings that highlight basic research programs beneficial to the Air Force.
Dr. Mitat A. Birkan presents an overview of his program, Space Propulsion and Power, at the AFOSR 2013 Spring Review. At this review, Program Officers from AFOSR Technical Divisions will present briefings that highlight basic research programs beneficial to the Air Force.
Dr. Jim Hwang presents an overview of his program, GHz-THz Electronics, at the AFOSR 2013 Spring Review. At this review, Program Officers from AFOSR Technical Divisions will present briefings that highlight basic research programs beneficial to the Air Force.
Dr. Mitat A. Birkan presents an overview of his program, Space Propulsion and Power, at the AFOSR 2013 Spring Review. At this review, Program Officers from AFOSR Technical Divisions will present briefings that highlight basic research programs beneficial to the Air Force.
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efficiency and stability. The power conversion efficiency (PCE) reached 20.1% late last year. The key disquiet
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measured in thousands of hours. These improvements have been achieved through the application of
different materials, interfaces and device architecture optimizations, especially after the investigation of hole
conductor free mesoporous devices incorporating carbon electrodes, which promise stable, low cost
and easy device fabrication methods. However, this work is still far from complete.
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Organometal halide perovskite solar cells have evolved in an exponential manner in the two key areas of
efficiency and stability. The power conversion efficiency (PCE) reached 20.1% late last year. The key disquiet
was stability, which has been limiting practical application, but now the state of the art is promising, being
measured in thousands of hours. These improvements have been achieved through the application of
different materials, interfaces and device architecture optimizations, especially after the investigation of hole
conductor free mesoporous devices incorporating carbon electrodes, which promise stable, low cost
and easy device fabrication methods. However, this work is still far from complete.
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We present a potential solution to the problem of extraction of photogenerated holes from CdS nanocrystals and nanowires. The nanosheet form of C3N5 is a low-band-gap (Eg = 2.03 eV), azo-linked graphenic carbon nitride framework formed by the polymerization of melem hydrazine (MHP). C3N5 nanosheets were either wrapped around CdS nanorods (NRs) following the synthesis of pristine chalcogenide or intercalated among them by an in situ synthesis protocol to form two kinds of heterostructures, CdS-MHP and CdS-MHPINS, respectively. CdS-MHP improved the photocatalytic degradation rate of 4-nitrophenol by nearly an order of magnitude in comparison to bare CdS NRs. CdS-MHP also enhanced the sunlight-driven photocatalytic activity of bare CdS NWs for the decolorization of rhodamine B (RhB) by a remarkable 300% through the improved extraction and utilization of photogenerated holes due to surface passivation. More interestingly, CdS-MHP provided reaction pathway control over RhB degradation. In the absence of scavengers, CdS-MHP degraded RhB through the N-deethylation pathway. When either hole scavenger or electron scavenger was added to the RhB solution, the photocatalytic activity of CdS-MHP remained mostly unchanged, while the degradation mechanism shifted to the chromophore cleavage (cycloreversion) pathway. We investigated the optoelectronic properties of CdS-C3N5 heterojunctions using density functional theory (DFT) simulations, finite difference time domain (FDTD) simulations, time-resolved terahertz spectroscopy (TRTS), and photoconductivity measurements. TRTS indicated high carrier mobilities >450 cm2 V–1 s–1 and carrier relaxation times >60 ps for CdS-MHP, while CdS-MHPINS exhibited much lower mobilities <150 cm2 V–1 s–1 and short carrier relaxation times <20 ps. Hysteresis in the photoconductive J–V characteristics of CdS NWs disappeared in CdS-MHP, confirming surface passivation. Dispersion-corrected DFT simulations indicated a delocalized HOMO and a LUMO localized on C3N5 in CdS-MHP. C3N5, with its extended π-conjugation and low band gap, can function as a shuttle to extract carriers and excitons in nanostructured heterojunctions, and enhance performance in optoelectronic devices. Our results demonstrate how carrier dynamics in core–shell heterostructures can be manipulated to achieve control over the reaction mechanism in photocatalysis.
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Conjugated polymer nanoparticles (CPNs) are a model system for the study of complex, nanoscale, multichromophoric interactions. Here, we are focused on furthering our understanding of the physical picture, processes, length scales, and time scales of energy transport in conjugated polymers. In particular, we are interested in determining how parameters related to the nanoscale structure and composition of CPs affect energy transport, which is investigated using steady-state and time-resolved fluorescence spectroscopy in conjunction with Monte Carlo simulation methods. Such information could prove useful for optimizing the structure and composition of device layers (e.g., in photovoltaic devices). We additionally seek to develop brighter, red-emitting CPNs through Förster Resonance Energy Transfer (FRET) for their use in biomedical imaging applications. Analysis of dye-doped and polymer blended CPNs shows that the doped CPNs exhibit bright, red-shifted emission, owing to the highly efficient energy transfer from the host polymer PFBT to the respective dopants (the fluorescent dye perylene red in dye-doped CPNs, and the polymer MEH-PPV in blended CPNs). An exciton diffusion energy transfer model was employed to simulate exciton dynamics in doped CPNs, and additionally to determine the intrinsic exciton diffusion length for PFBT in the absence of quenching defects. Solvent-induced swelling methods were utilized to study how swelling affects the multiple energy transfer cascade to intrinsic defects and/or aggregate species in CPNs, which modulates the exciton dynamics and fluorescence properties of CPNs. Changes in the rate of exciton transport over a range of solvent compositions were measured using picosecond
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1. Efficient charge transfer induced organic/inorganic
based hybrid heterojunction of Ppy/GaN nanorods for
high performance self-powered UV photodetection
15-01-2021
Presented by
P. Kedhareswara Sairam, Prof. Moon-Deock Kim*
Department of Physics, Chungnam National University, South Korea.
3. I. Introduction
Self powered-Photodetectors:
Basically also called photosensor, are sensors of light or other electromagnetic radiation. Typically,
the photo detector that converts optical signals (photons) into electrical signals (current/voltage).
Self-powered can be described as the device which can be operate without any external power source (0
bias).
UV photodetection
4. Material properties GaN
Structure Wurtzite
Lattice constant (Å) a = 3.18 c = 5.18
Band gap Direct (3.4 eV)
Dielectric constant 10.4
Thermal conductivity
(cm2 /V-s)
2000
Saturation velocity (107 cm/s) 2.5
I. Introduction
GaN
Issues with pristine GaN nanostructures:
The surface states, poor carrier life, and other native defects in GaN nanorods (NRs) limit their
utilization in high-speed and large-gain ultraviolet (UV) photodetection applications.
Strategies to improve GaN nanostructures to improve UV photodetection:
GaN PDs designed with a Schottky junction, p-n junction organic –inorganic and p-i-n.
5. I. Introduction
Polypyrrole (Ppy)
A typical organic polymer.
Polypyrrole (Ppy) is one of the typical p-type intrinsic
conductive polymer with a strong interactive possible cross
linking chains which helps to maintain a healthy bonding to the
other compounds which includes high environmental stability
and possess high electrical conductivity.
6. II. Motivation
GaN nanorods were functionalized with Ppy. The amine functional groups present in
Ppy can effectively passivate the surface states in GaN nanorods.
Thereby, p-n junction will form in the hybrid heterojunction.
The effect of passivation showed a significant influence on optical, electrical, structural
properties on GaN nanorods PD.
Thereby, the charge transformation would exists in between the heterojunction that it
could generate a built-in-potential at the interface, which further offers the self-driving
force to move the photo-generated carriers across the junction without external power
supply.
Thus, it can effectively enhances the optoelectrical properties of the device [1].
[1] N. Prakash. et.al, Appl. Phys. Lett. 109, 242102 (2016).
7. III. Experiments
Growth
• Plasma-assisted molecular beam epitaxy
• GaN nanorods on /Si(111)
Device fabrication
• Ppy was spin coated with speed of 3000
rpm on patterned GaN NRS followed by
organic cleaning.
Metal deposition
• Electron beam evaporation
• Top(Au:100 nm)-bottom(In) contact
Characterizations
• SEM, FTIR, XPS, UV-Visible
spectroscopy, characterizations and I-V,
and Photodetection properties.
8. IV. Results and discussions
SEM UV-Visible FTIR
[2] S. Nongthombam.et.al, J. VLSI DCS (2020), pp. 171-175.
[3] S. Munusamy.et.al, Arab. J. Chem (2019) 12, 3565-3575
The cross sectional SEM image of the Ppy/GaN NRs hybrid device,.
The characteristic absorption peaks of UV-Visible spectra positioned at 275 nm and a weak peak at 420
nm endorse the presence of Ppy and the optical band gap of Ppy was estimated as 3.1 eV from Tauc
plot (inset figure) [2, 3].
The band at 557 cm-1 (C-N) and others evaluates the existence of related functional groups and their
vibrational bands in Ppy and the peak at 669 cm-1 corresponds to Ga-O that confirms the successful
deposition of Ppy into the GaN [2].
1.2 1.8 2.4 3.0 3.6 4.2 4.8
Ppy
(h)
2
(eV/cm)
2
h (eV)
3.1eV
9. IV. Results and discuss
XPS
[3] S. Munusamy.et.al, Arab. J. Chem (2019) 12, 3565-3575.
10. IV. Results and discuss
∆Ev = E 𝐶1𝑠
𝑃1
− EVBM
𝑃1
+ (EGa2p3
2
𝑃1/GaN
−E 𝐶1𝑠
𝑃1/GaN
) − (EGa2p3
2
GaN
−EVBM
GaN
) (1)
∆Ec = ∆Ev + Eg 𝑃1 − Eg GaN (2)
XPS-band offsets
[4] E. A. Kraut.et.al, Phys. Rev. Lett., (1980), 44, 1620-1623.
12. IV. Results and discuss
(a) (b)
Photoresponse properties
𝑅 𝜆 =
∆𝐼
𝐴∗𝑃
−−−−− −(3)
𝐷∗
=
𝐴
1
2 𝑅 𝜆
2𝑒𝐼 𝑑
−−−− −(4)
𝐸𝑄𝐸 =
ℎ𝑐
𝑒𝜆
𝑅 𝜆 −−− −(5)
The estimated detectivity, responsivity and EQE by using the above standard formula, under 382 nm (1.32 mW/cm2) were
found in the range of5.0×1012 Jones, 102 A/W and 29.8×103 (%), and 25.×106 % respectively.
The Rλ and EQE of hybrid device was found to be decreased with increasing the power densities varying from 1.32
mW/cm2 to 6.56 mW/cm2, were ascribed to the carriers (mainly holes) trapping saturation resulting in larger quantum
efficiency [1, 5].
[1] N. Prakash. et.al, Appl. Phys. Lett. 109, 242102 (2016).
[5] N. Prakash. et.al, Adv. Optical Mater. (2018), 6, 1800191.
13. IV. Results and discuss
Band diagram
On UV absorption the hybrid PD stimulates the electrons from valence band to the conduction band in GaN and highest
occupied molecular orbit (HOMO) to lowest unoccupied molecular orbit (LUMO) in Ppy to produce excitons and can
diffused through the depletion region formed at interface [5].
As a result of built-in-potential at the interface, the excitons were being separated into the free holes and electrons
moving towards the p-Ppy and n-GaN layers respectively, resulting to the high photodetector properties at zero bias.
[5] N. Prakash. et.al, Adv. Optical Mater. (2018), 6, 1800191.
14. V. Conclusion
Self-powered UV photodetection optoelectrical properties of the Ppy/GaN nanorods hybrid
device was successfully investigated.
The surface trap states of the pristine GaN nanorods were effective passivated by the
amine functional groups of Ppy.
The charge transformation between the p-n junction interface of hybrid device would be the
reason for the excellent photo current properties.
Under UV light, the hybrid device exhibited the high photocurrent properties as compared to
the pristine device.
The high photoresponse characteristics was due to the formation of built-in potential at the
interface junction, that it would helps to separating the generated holes and electrons
moving towards the p-Ppy and n-GaN layers respectively, resulting to the high
photodetector properties at zero bias.