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result(s) for
"Ardalan Armin"
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Accurate characterization of next-generation thin-film photodetectors
2019
The performance of photodetectors fabricated from emerging semiconductors such as perovskites, quantum dots, two-dimensional materials or organics, for example, can be prone to misinterpretation. This Comment exposes the problems and proposes some guidelines for accurate characterization.
Journal Article
A universal Urbach rule for disordered organic semiconductors
by
Li, Wei
,
Sandberg, Oskar J.
,
Kaiser, Christina
in
639/301/119/995
,
639/4077/909/4101/4096/946
,
Absorption
2021
In crystalline semiconductors, absorption onset sharpness is characterized by temperature-dependent Urbach energies. These energies quantify the static, structural disorder causing localized exponential-tail states, and dynamic disorder from electron-phonon scattering. Applicability of this exponential-tail model to disordered solids has been long debated. Nonetheless, exponential fittings are routinely applied to sub-gap absorption analysis of organic semiconductors. Herein, we elucidate the sub-gap spectral line-shapes of organic semiconductors and their blends by temperature-dependent quantum efficiency measurements. We find that sub-gap absorption due to singlet excitons is universally dominated by thermal broadening at low photon energies and the associated Urbach energy equals the thermal energy, regardless of static disorder. This is consistent with absorptions obtained from a convolution of Gaussian density of excitonic states weighted by Boltzmann-like thermally activated optical transitions. A simple model is presented that explains absorption line-shapes of disordered systems, and we also provide a strategy to determine the excitonic disorder energy. Our findings elaborate the meaning of the Urbach energy in molecular solids and relate the photo-physics to static disorder, crucial for optimizing organic solar cells for which we present a revisited radiative open-circuit voltage limit.
The sub-gap absorption coefficient in organic semiconductors is often characterized by Urbach energies, which quantify both structural and dynamic disorders, yet the fundamental is not well-understood. Here, the authors provide a strategy to determine excitonic disorder energy, and reveal that absorption at energies well below the gap is universally dominated by thermal broadening.
Journal Article
Direct observation of trap-assisted recombination in organic photovoltaic devices
by
Li, Wei
,
Sandberg, Oskar J.
,
Armin, Ardalan
in
639/301/119/995
,
639/301/299/946
,
639/925/357/995
2021
Trap-assisted recombination caused by localised sub-gap states is one of the most important first-order loss mechanism limiting the power-conversion efficiency of all solar cells. The presence and relevance of trap-assisted recombination in organic photovoltaic devices is still a matter of some considerable ambiguity and debate, hindering the field as it seeks to deliver ever higher efficiencies and ultimately a viable new solar photovoltaic technology. In this work, we show that trap-assisted recombination loss of photocurrent is universally present under operational conditions in a wide variety of organic solar cell materials including the new non-fullerene electron acceptor systems currently breaking all efficiency records. The trap-assisted recombination is found to be induced by states lying 0.35-0.6 eV below the transport edge, acting as deep trap states at light intensities equivalent to 1 sun. Apart from limiting the photocurrent, we show that the associated trap-assisted recombination via these comparatively deep traps is also responsible for ideality factors between 1 and 2, shedding further light on another open and important question as to the fundamental working principles of organic solar cells. Our results also provide insights for avoiding trap-induced losses in related indoor photovoltaic and photodetector applications.
Trap-assisted recombination caused by localised sub-gap states is one of the factors limiting power-conversion efficiency in solar cells, yet the presence and relevance is still under debate in organic solar cells. Here, the authors reveal that this recombination loss is universally present under operational conditions in these devices.
Journal Article
Precision ultrasound sensing on a chip
by
Basiri-Esfahani, Sahar
,
Armin, Ardalan
,
Bowen, Warwick P.
in
639/624/1107/510
,
639/766/1130/2800
,
639/766/400/1113
2019
Ultrasound sensors have wide applications across science and technology. However, improved sensitivity is required for both miniaturisation and increased spatial resolution. Here, we introduce cavity optomechanical ultrasound sensing, where dual optical and mechanical resonances enhance the ultrasound signal. We achieve noise equivalent pressures of 8–300 μPa H
z
−1/2
at kilohertz to megahertz frequencies in a microscale silicon-chip-based sensor with >120 dB dynamic range. The sensitivity far exceeds similar sensors that use an optical resonance alone and, normalised to the sensing area, surpasses previous air-coupled ultrasound sensors by several orders of magnitude. The noise floor is dominated by collisions from molecules in the gas within which the acoustic wave propagates. This approach to acoustic sensing could find applications ranging from biomedical diagnostics, to autonomous navigation, trace gas sensing, and scientific exploration of the metabolism-induced-vibrations of single cells.
With the wide adoption of ultrasound methods in biomedical and technological diagnostics, sensitive probes are in demand. Here, the authors employ cavity optomechanics where optical and mechanical resonances are coupled, both enhancing the sensitivity of the device and allowing its chip-integration.
Journal Article
Scaling of next generation solution processed organic and perovskite solar cells
2018
Why, despite considerable R&D efforts and significant translational investment over the past 20 years, has the technology of solution-processed thin film solar cells not become a commercial reality? The manufacturing cost-to-power conversion efficiency ratio seems persuasive, as do the energy payback and embodied energy metrics. As new perovskite-based semiconductors achieve impressive efficiencies and organic semiconductors enjoy a resurgence, the lab-to-manufacturing translation and scaling questions require urgent attention. This comment addresses the challenges in solution processable photovoltaic technologies faced by scientists and engineers in addressing these questions, and highlights the concept of thick junctions as a promising solution.
Journal Article
Charge-generating mid-gap trap states define the thermodynamic limit of organic photovoltaic devices
by
Sandberg, Oskar J.
,
Zarrabi, Nasim
,
Riley, Drew B.
in
639/301/119/1000
,
639/301/923/3931
,
639/4077/909/4101/4096/946
2020
Detailed balance is a cornerstone of our understanding of artificial light-harvesting systems. For next generation organic solar cells, this involves intermolecular charge-transfer (CT) states whose energies set the maximum open circuit voltage
V
OC
. We have directly observed sub-gap states significantly lower in energy than the CT states in the external quantum efficiency spectra of a significant number of organic semiconductor blends. Taking these states into account and using the principle of reciprocity between emission and absorption results in non-physical radiative limits for the
V
OC
. We propose and provide compelling evidence for these states being non-equilibrium mid-gap traps which contribute to photocurrent by a non-linear process of optical release, upconverting them to the CT state. This motivates the implementation of a two-diode model which is often used in emissive inorganic semiconductors. The model accurately describes the dark current,
V
OC
and the long-debated ideality factor in organic solar cells. Additionally, the charge-generating mid-gap traps have important consequences for our current understanding of both solar cells and photodiodes – in the latter case defining a detectivity limit several orders of magnitude lower than previously thought.
The inability to accurately measure the charge-generating energy states in organic solar cells makes elucidating the photovoltaic effect in these devices difficult. Here, the authors report charge-generating mid-gap trap states in organic solar cells via ultra-sensitive photovoltaic measurements.
Journal Article
Narrowband light detection via internal quantum efficiency manipulation of organic photodiodes
by
Jansen-van Vuuren, Ross D.
,
Kopidakis, Nikos
,
Armin, Ardalan
in
132/122
,
639/301/119/1000
,
639/624/400
2015
Spectrally selective light detection is vital for full-colour and near-infrared (NIR) imaging and machine vision. This is not possible with traditional broadband-absorbing inorganic semiconductors without input filtering, and is yet to be achieved for narrowband absorbing organic semiconductors. We demonstrate the first sub-100 nm full-width-at-half-maximum visible-blind red and NIR photodetectors with state-of-the-art performance across critical response metrics. These devices are based on organic photodiodes with optically thick junctions. Paradoxically, we use broadband-absorbing organic semiconductors and utilize the electro-optical properties of the junction to create the narrowest NIR-band photoresponses yet demonstrated. In this context, these photodiodes outperform the encumbent technology (input filtered inorganic semiconductor diodes) and emerging technologies such as narrow absorber organic semiconductors or quantum nanocrystals. The design concept allows for response tuning and is generic for other spectral windows. Furthermore, it is material-agnostic and applicable to other disordered and polycrystalline semiconductors.
There is a growing interest in the development of narrowband photodiodes for full-color imaging and visible-blind near-infrared detection. Armin
et al.
show a sub-100 nm response by tuning the spectral bandwidth through regulating the charge collection efficiency in a thick organic bulk heterojunction.
Journal Article
Ligand-assisted cation-exchange engineering for high-efficiency colloidal Cs1−xFAxPbI3 quantum dot solar cells with reduced phase segregation
by
Liu, Gang
,
Cheng, Hui-Ming
,
Ren, Long
in
639/301/299/946
,
639/4077/4072/4062
,
Cation exchanging
2020
The mixed caesium and formamidinium lead triiodide perovskite system (Cs
1
−
x
FA
x
PbI
3
) in the form of quantum dots (QDs) offers a pathway towards stable perovskite-based photovoltaics and optoelectronics. However, it remains challenging to synthesize such multinary QDs with desirable properties for high-performance QD solar cells (QDSCs). Here we report an effective oleic acid (OA) ligand-assisted cation-exchange strategy that allows controllable synthesis of Cs
1
−
x
FA
x
PbI
3
QDs across the whole composition range (
x
=
0–1), which is inaccessible in large-grain polycrystalline thin films. In an OA-rich environment, the cross-exchange of cations is facilitated, enabling rapid formation of Cs
1
−
x
FA
x
PbI
3
QDs with reduced defect density. The hero Cs
0.5
FA
0.5
PbI
3
QDSC achieves a certified record power conversion efficiency (PCE) of 16.6% with negligible hysteresis. We further demonstrate that the QD devices exhibit substantially enhanced photostability compared with their thin-film counterparts because of suppressed phase segregation, and they retain 94% of the original PCE under continuous 1-sun illumination for 600 h.
Mixed-cation perovskite quantum dot solar cells possess decent phase stability but considerably low efficiency. Here Hao et al. show that ligands are key to the formation of quantum dots with lower defect density and demonstrate devices that are more stable and efficient than their bulk counterparts.
Journal Article
Electron-donating amine-interlayer induced n-type doping of polymer:nonfullerene blends for efficient narrowband near-infrared photo-detection
by
Shanivarasanthe, Rachith
,
Vandewal, Koen
,
Zeiske, Stefan
in
147/3
,
639/301/1005/1009
,
639/766/400/1021
2022
Inherently narrowband near-infrared organic photodetectors are highly desired for many applications, including biological imaging and surveillance. However, they suffer from a low photon-to-charge conversion efficiencies and utilize spectral narrowing techniques which strongly rely on the used material or on a nano-photonic device architecture. Here, we demonstrate a general and facile approach towards wavelength-selective near-infrared phtotodetection through intentionally n-doping 500–600 nm-thick nonfullerene blends. We show that an electron-donating amine-interlayer can induce n-doping, resulting in a localized electric field near the anode and selective collection of photo-generated carriers in this region. As only weakly absorbed photons reach this region, the devices have a narrowband response at wavelengths close to the absorption onset of the blends with a high spectral rejection ratio. These spectrally selective photodetectors exhibit zero-bias external quantum efficiencies of ~20–30% at wavelengths of 900–1100 nm, with a full-width-at-half-maximum of ≤50 nm, as well as detectivities of >10
12
Jones.
Fabrication of efficient narrowband near-infrared photodetectors remains a challenge. Here, Liu
et al
. show a facile and general approach for achieving a sub-50 nm response by intentionally
n
-doping an optically-thick nonfullerene photodiode using an electron-donating amine-interlayer.
Journal Article
Slower carriers limit charge generation in organic semiconductor light-harvesting systems
2016
Blends of electron-donating and -accepting organic semiconductors are widely used as photoactive materials in next-generation solar cells and photodetectors. The yield of free charges in these systems is often determined by the separation of interfacial electron–hole pairs, which is expected to depend on the ability of the faster carrier to escape the Coulomb potential. Here we show, by measuring geminate and non-geminate losses and key transport parameters in a series of bulk-heterojunction solar cells, that the charge-generation yield increases with increasing slower carrier mobility. This is in direct contrast with the well-established Braun model where the dissociation rate is proportional to the mobility sum, and recent models that underscore the importance of fullerene aggregation for coherent electron propagation. The behaviour is attributed to the restriction of opposite charges to different phases, and to an entropic contribution that favours the joint separation of both charge carriers.
In organic solar cells, the photogeneration of free charge carriers is limited by the dissociation of interfacial charge transfer states. Here, the authors study the impact of charge carrier mobilities in operational devices and show that the slowest charge carriers limit the dissociation of charge transfer states.
Journal Article