Thomas Unold

ORCID: 0000-0002-5750-0693
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About
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Research Areas
  • Chalcogenide Semiconductor Thin Films
  • Quantum Dots Synthesis And Properties
  • Copper-based nanomaterials and applications
  • Perovskite Materials and Applications
  • Semiconductor materials and interfaces
  • Silicon and Solar Cell Technologies
  • Thin-Film Transistor Technologies
  • Conducting polymers and applications
  • Silicon Nanostructures and Photoluminescence
  • Advanced Semiconductor Detectors and Materials
  • Semiconductor Quantum Structures and Devices
  • Electronic and Structural Properties of Oxides
  • solar cell performance optimization
  • Phase-change materials and chalcogenides
  • ZnO doping and properties
  • Advanced Thermoelectric Materials and Devices
  • Crystal Structures and Properties
  • Solid-state spectroscopy and crystallography
  • Organic Electronics and Photovoltaics
  • nanoparticles nucleation surface interactions
  • Machine Learning in Materials Science
  • 2D Materials and Applications
  • Surface and Thin Film Phenomena
  • Magnetic and transport properties of perovskites and related materials
  • Semiconductor Lasers and Optical Devices

Helmholtz-Zentrum Berlin für Materialien und Energie
2016-2025

University of Cambridge
2024

Duke University
2021

Shinshu University
2014

University of Limerick
2013

German Orient Foundation
2005-2009

Fraunhofer Institute for Telecommunications, Heinrich Hertz Institute
2004-2008

National Renewable Energy Laboratory
1995-2008

Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy
2003-2005

Carl von Ossietzky Universität Oldenburg
1999-2004

Tandem solar cells that pair silicon with a metal halide perovskite are promising option for surpassing the single-cell efficiency limit. We report monolithic perovskite/silicon tandem certified power conversion of 29.15%. The absorber, bandgap 1.68 electron volts, remained phase-stable under illumination through combination fast hole extraction and minimized nonradiative recombination at hole-selective interface. These features were made possible by self-assembled, methyl-substituted...

10.1126/science.abd4016 article EN Science 2020-12-10

Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V_OC) cell. In order to realize full thermodynamic potential absorber, both electron and hole layer (ETL/HTL) need be as selective possible. By measuring quasi-Fermi level splitting (QFLS) perovskite/CTL heterojunctions, we quantify interfacial current for a wide range commonly used...

10.1039/c9ee02020a article EN Energy & Environmental Science 2019-01-01

Abstract Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell particular. It can give direct information on the recombination kinetics processes as well internal electrochemical potential of free charge carriers single layers, layer stacks with transport complete cells. The correct evaluation interpretation photoluminescence requires consideration proper excitation conditions, calibration...

10.1002/aenm.201904134 article EN cc-by Advanced Energy Materials 2020-05-06

Abstract Today's perovskite solar cells (PSCs) are limited mainly by their open‐circuit voltage ( V OC ) due to nonradiative recombination. Therefore, a comprehensive understanding of the relevant recombination pathways is needed. Here, intensity‐dependent measurements quasi‐Fermi level splitting (QFLS) and on very same devices, including pin‐type PSCs with efficiencies above 20%, performed. It found that QFLS in lies significantly below its radiative limit for all intensities but also...

10.1002/aenm.201901631 article EN cc-by Advanced Energy Materials 2019-07-25

We demonstrate open-circuit voltages exceeding 1.26 V for inverted planar CH3NH3PbI3 solar cells fabricated using a combination of lead acetate and PbCl2 precursors leading to smooth films large grain sizes. Surface recombination is suppressed by careful optimization the PTAA hole transport PCBM electron layers. Suppression bulk surface verified absolute photoluminescence measurements with external quantum efficiencies ∼5% in complete cells. In addition, we find exceptionally long lifetimes...

10.1021/acsenergylett.8b01906 article EN ACS Energy Letters 2018-12-06

Abstract Solar cells based on kesterite‐type Cu 2 ZnSnS 4 (CZTS) were fabricated molybdenum coated soda lime glass by evaporation using ZnS, Sn, Cu, and S sources. The coevaporation process was performed at a nominal substrate temperature of 550°C sulfur partial pressure 2–3 × 10 −3 Pa leading to polycrystalline CZTS thin films with promising electronic properties. absorber layers grown copper‐rich, requiring KCN etch step remove excess copper sulfide. compositional ratios as determined...

10.1002/pip.976 article EN Progress in Photovoltaics Research and Applications 2010-05-31

Identification of electronic processes at buried interfaces charge-selective contacts is crucial for photovoltaic and photocatalysis research. Here, transient surface photovoltage (SPV) used to study the passivation different hole-selective carbazole-based SAMs. It shown that SPV photoluminescence provide complementary information on charge transfer kinetics trapping/de-trapping mechanisms, trap-assisted non-radiative recombination losses originate from electron trapping SAM-modified...

10.1016/j.joule.2021.07.016 article EN cc-by Joule 2021-08-18

A series of Cu(In,Ga)Se2 (CIGS) thin film solar cells with differently prepared heterojunctions has been investigated by admittance spectroscopy, capacitance-voltage (CV) profiling, and temperature dependent current-voltage (IVT) measurements. The devices different CdS buffer layer thicknesses, an In2S3 or a Schottky barrier junction, all show the characteristic step at shallow energies between 40 160 meV, which often referred to as N1 defect. No correlation thickness capacitance is found....

10.1063/1.3277043 article EN Journal of Applied Physics 2010-02-01

In the quest for better solar panels, we continue to refine our understanding of physics photovoltaic absorbers, such as hybrid metal-organic perovskites. By scrutinizing photoluminescence transients, authors explain how determine fundamental semiconductor properties and estimate potential open-circuit voltage perovskite thin films. Additionally, they highlight impacts photon recycling, doping, bulk surface recombination charge carriers on device performance.

10.1103/physrevapplied.6.044017 article EN Physical Review Applied 2016-10-26
T. Jesper Jacobsson Adam Hultqvist Alberto García‐Fernández Aman Anand Amran Al‐Ashouri and 89 more Anders Hagfeldt Andrea Crovetto Antonio Abate Antonio Gaetano Ricciardulli Anuja Vijayan Ashish Kulkarni Assaf Y. Anderson Barbara Primera Darwich Bowen Yang Brendan L. Coles Carlo A. R. Perini Carolin Rehermann Daniel Ramírez David Fairen‐Jimenez Diego Di Girolamo Donglin Jia Elena Avila Emilio J. Juárez‐Pérez Fanny Baumann Florian Mathies G. S. Anaya González Gerrit Boschloo Giuseppe Nasti Gopinath Paramasivam Guillermo Martínez‐Denegri Hampus Näsström Hannes Michaels Hans Köbler Hua Wu Iacopo Benesperi M. Ibrahim Dar İlknur Bayrak Pehlivan Isaac E. Gould Jacob N. Vagott Janardan Dagar Jeff Kettle Jie Yang Jinzhao Li Joel A. Smith Jorge Pascual José J. Jerónimo-Rendón Juan Felipe Montoya Juan‐Pablo Correa‐Baena Junming Qiu Junxin Wang Kári Sveinbjörnsson Katrin Hirselandt Krishanu Dey Kyle Frohna Lena Mathies Luigi Angelo Castriotta Mahmoud H. Aldamasy Manuel Vásquez-Montoya Marco A. Ruiz‐Preciado Marion A. Flatken Mark Khenkin Max Grischek Mayank Kedia Michael Saliba Miguel Anaya M. Veldhoen Neha Arora Oleksandra Shargaieva Oliver Maus Onkar S. Game Ori Yudilevich Paul Faßl Qisen Zhou Rafael Betancur Rahim Munir Rahul Patidar Samuel D. Stranks Shahidul Alam Shaoni Kar Thomas Unold Tobias Abzieher Tomas Edvinsson Tudur Wyn David Ulrich W. Paetzold Waqas Zia Weifei Fu Weiwei Zuo Vincent Schröder Wolfgang Tress Xiaoliang Zhang Yu‐Hsien Chiang Zafar Iqbal Zhiqiang Xie Eva Unger

Abstract Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all meaningful device peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in database. We collect over 42,400 photovoltaic devices with up 100 parameters per device. then develop...

10.1038/s41560-021-00941-3 article EN cc-by Nature Energy 2021-12-13

Abstract Nanocrystal‐based Cu 2 Zn(Sn y Ge 1‐y )(S x Se 4‐x ) (CZTGeSSe) thin‐film solar cell absorbers with tunable band gap have been prepared. Maximum solar‐conversion total area efficiencies of up to 9.4% are achieved a content 30 at.%. Improved performance compared similarly processed films ZnSn(S (CZTSSe, 8.4% efficiency) is through controlling loss from the bulk absorber film during high‐temperature selenization treatment, although some surface still observed following this step....

10.1002/pip.2442 article EN Progress in Photovoltaics Research and Applications 2013-12-04

Perovskite-based tandem solar cells can increase the power conversion efficiency (PCE) of conventional single-junction photovoltaic devices. Here, we present monolithic perovskite/CIGSe with a perovskite top cell fabricated directly on an as-grown, rough CIGSe bottom cell. To prevent potential shunting due to surface, thin NiOx layer is conformally deposited via atomic deposition front contact The performance further improved by additional polymer PTAA at NiOx/perovskite interface. This hole...

10.1021/acsenergylett.9b00135 article EN ACS Energy Letters 2019-01-24

Tuning the energy levels of halide perovskite by controlling deposition dipolar self-assembled monolayers.

10.1039/d0ee02216k article EN cc-by Energy & Environmental Science 2020-12-16

Abstract Perovskite semiconductors are an attractive option to overcome the limitations of established silicon based photovoltaic (PV) technologies due their exceptional opto‐electronic properties and successful integration into multijunction cells. However, performance single‐ cells is largely limited by significant nonradiative recombination at perovskite/organic electron transport layer junctions. In this work, cause interfacial perovskite/C 60 interface revealed via a combination...

10.1002/aenm.202103567 article EN cc-by Advanced Energy Materials 2022-02-09

Halide perovskites are a strong candidate for the next generation of photovoltaics. Chemical doping halide is an established strategy to prepare highest efficiency and most stable perovskite-based solar cells. In this study, we unveil mechanism using series alkaline earth metals. We find that low levels enable incorporation dopant within perovskite lattice, whereas high concentrations induce surface segregation. The threshold from regime correlates size element. show results in more n-type...

10.1021/jacs.9b11637 article EN Journal of the American Chemical Society 2020-01-09

An approach is proposed to predict the impact of point defects on solar cell performance.

10.1039/d0ee00291g article EN cc-by Energy & Environmental Science 2020-01-01

Abstract Understanding carrier loss mechanisms at microscopic regions is imperative for the development of high-performance polycrystalline inorganic thin-film solar cells. Despite progress achieved kesterite, a promising environmentally benign and earth-abundant photovoltaic material, their impact on device performance remain largely unknown. Herein, we unveil these in state-of-the-art Cu 2 ZnSnSe 4 (CZTSe) cells using framework that integrates multiple macroscopic characterizations with...

10.1038/s41560-022-01078-7 article EN cc-by Nature Energy 2022-07-21

Abstract The next technological step in the exploration of metal‐halide perovskite solar cells is demonstration larger‐area device prototypes under outdoor operating conditions. authors here demonstrate that when slot‐die coating halide layers on large areas, ribbing effects may occur but can be prevented by adjusting precursor ink's rheological properties. For formamidinium lead triiodide (FAPbI 3 ) inks based 2‐methoxyethanol, ink viscosity adjusted adding acetonitrile (ACN) as a...

10.1002/aenm.202203898 article EN cc-by Advanced Energy Materials 2023-03-04

We demonstrate coherent nonlinear-optical control of excitons in a pair quantum dots (QDs) coupled via dipolar interaction. The single-exciton population the first QD is controlled by resonant picosecond excitation, giving rise to Rabi oscillations. As result, exciton transition second spectrally shifted and concomitant oscillations are observed. identify coupling between permanent excitonic dipole moments as dominant interaction mechanism, whereas quasiresonant (Förster) energy transfer...

10.1103/physrevlett.94.137404 article EN Physical Review Letters 2005-04-08

The electronic structure of the CdS/Cu2ZnSnS4 (CZTS) heterojunction was investigated by direct and inverse photoemission. effects a KCN etch CZTS absorber prior to CdS deposition on band alignment at respective interface were studied. We find “cliff”-like conduction offset CdS/CZTS independent pretreatment significant etch-induced enhancement energetic barrier for charge carrier recombination across interface.

10.1063/1.3663327 article EN Applied Physics Letters 2011-11-28

Thin film solar cells with Al/ITO/ZnO/CdS/CZTSSe/Mo‐glass structure are fabricated employing a fast and low‐cost preparation procedure using an aqueous ink deposited by nonpyrolytic spray, followed high temperature crystallization selenization steps. Capacitance–voltage measurements on previously reported devices >8% efficiency under 1 sun irradiation show charge carrier density of the order 10 17 cm −3 . Moreover, admittance spectroscopy indicates presence mid‐bandgap defects that...

10.1002/aenm.201501404 article EN Advanced Energy Materials 2015-10-15

Abstract The performance of many emerging compound semiconductors for thin‐film solar cells is considerably lower than the Shockley–Queisser limit, and one main reasons this presence various deleterious defects. A partial or complete substitution cations presents a viable strategy to alter characteristics detrimental defects defect clusters. Particularly, it hypothesized that double cation could be feasible mitigate negative effects different types In study, on pure‐sulfide Cu 2 ZnSnS 4...

10.1002/aenm.201802540 article EN Advanced Energy Materials 2018-10-04
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