This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in ACS Nano, copyright © American Chemical Society after peer review. To access the final edited and published work see http://pubs.acs.org/doi/full/10.1021/acsnano.7b03148 High Photovoltaic Quantum Efficiency in Ultrathin van der Waals Heterostructures Joeson Wong1ǂ, Deep Jariwala1,2ǂ, Giulia Tagliabue1,4, Kevin Tat1, Artur R. Davoyan1,2,3, Michelle C. Sherrott1,2 and Harry A. Atwater1,2,3,4* 1Department of Applied Physics and Materials Science, California Institute of Technology, Pasadena, CA-91125, USA 2Resnick Sustainability Institute, California Institute of Technology, Pasadena, CA-91125, USA 3Kavli Nanoscience Institute, California Institute of Technology, Pasadena, CA-91125, USA 4Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, CA-91125, USA * Corresponding author: Harry A Atwater (
[email protected]) ǂ These authors contributed equally ABSTRACT: We report experimental measurements for ultrathin (< 15 nm) van der Waals heterostructures exhibiting external quantum efficiencies exceeding 50%, and show that these structures can achieve experimental absorbance > 90%. By coupling electromagnetic simulations and experimental measurements, we show that pn WSe2/MoS2 heterojunctions with vertical carrier collection can have internal photocarrier collection efficiencies exceeding 70%. GRAPHICAL TABLE OF CONTENTS: KEYWORDS: van der Waals, heterojunction, photovoltaics, quantum efficiency,