Table of contents Chapter 1 Introduction 7 Chapter 2 Which cocoa bean traits persist when eating chocolate? 31 Real-time nosespace analysis by PTR-QiToF-MS Chapter 3 Factors contributing to the variation in the volatile composition of chocolate: 63 Botanical and geographical origins of the cocoa beans, and brand-related formulation and processing Chapter 4 Making cocoa origin traceable: 85 Fingerprints of chocolates using Flow Infusion-Electro Spray Ionization-Mass Spectrometry Chapter 5 Sniffing out cocoa bean traits that persist in chocolates by PTR-MS, ICP-MS 103 and IR-MS Chapter 6 PTR-QiToF-MS and HSI for the characterisation of fermented cocoa beans 133 from different origins Chapter 7 Discussion 161 Summary 175 Acknowledgements 179 List of publications 183 Overview of completed training activities 184 About the author 185 Acknowledgements of financial support 186 Within the group of MS techniques, Isotope Ratio-MS (IR-MS) for the measurements of stable isotope abundance and Inductively Coupled Plasma-MS (ICP-MS) for the detection of macro, micro-or trace-elements have been used to develop methods for the geographical assessment of several foodstuffs. These are within the most used analytical techniques for tracing foods (Kelly, Heaton, & Hoogewerff, 2005). What makes the isotope abundance a good geographical indication is that the isotope fraction is related to physico-chemical phenomena happening in nature. For example, the isotopic fractionation can occur with absorption and desorption, crystallisation and melting, evaporation and condensation. The natural variation that occurs in the isotopic ratio of hydrogen, carbon, nitrogen and oxygen and the heavy element strontium can be used for the geographical detection of food origin (Kelly et al., 2005). Moreover, the isotopic composition of the constituents of agricultural products (proteins, carbohydrates, fats, minerals) is depending on several factors both indicative of the geographical origin and some production steps. These factors include seasonal and geological variation such as altitude, soil composition etc.